Showing 1–50 of 131 results for author: Jozwiak, C

Spin-Valley Locking in 2H-TaS2 and Its Co-Intercalated Counterpart: Roles of Surface Domains and Co Intercalation

Authors: Hai-Lan Luo, Josue Rodriguez, Maximilian Huber, Haoyue Jiang, Luca Moreschini, Pranav Thekke Madathil, Catherine Xu, Chris Jozwiak, Aaron Bostwick, Alexei Fedorov, James G. Analytis, Dung-Hai Lee, Alessandra Lanzara

Abstract: Tuning and probing spin-valley coupling is key to understanding correlated ground states in 2$\it{H}$-TaS$_2$. Its magnetically intercalated analogue, Co$_{1/3}$TaS$_2$, introduces additional degrees of freedom, including modified interlayer coupling and magnetism, to modulate spin-valley physics. Surface-sensitive probes like ARPES are essential for accessing surface spin texture, yet previous st… ▽ More Tuning and probing spin-valley coupling is key to understanding correlated ground states in 2$\it{H}$-TaS$_2$. Its magnetically intercalated analogue, Co$_{1/3}$TaS$_2$, introduces additional degrees of freedom, including modified interlayer coupling and magnetism, to modulate spin-valley physics. Surface-sensitive probes like ARPES are essential for accessing surface spin texture, yet previous studies on 2$\it{H}$-TMDs have reported conflicting results regarding spin-polarized bands, leaving open whether these discrepancies are intrinsic or extrinsic. Here we performed spatially resolved spin-ARPES measurements on 2$\it{H}$-TaS$_2$ and Co$_{1/3}$TaS$_2$. Our results reveal robust spin-valley locking on both compounds. Importantly, Co intercalation enhances interlayer hybridization and introduces magnetism while preserving the TaS$_2$-derived spin texture. We further observe a spatial reversal of the out-of-plane spin polarization, which we attribute to different surface domains. This effect complicates quantifying spin textures and may underlie prior inconsistent observations. Our findings provide microscopic insight into how interlayer interactions and surface domains together govern spin-valley phenomena in layered TMDs. △ Less

Submitted 16 January, 2026; originally announced January 2026.

Comments: 9 pages, 5 figures

Discovery of Van Hove Singularities: Electronic Fingerprints of 3Q Magnetic Order in a van der Waals Quantum Magnet

Authors: Hai-Lan Luo, Josue Rodriguez, Debasis Dutta, Maximilian Huber, Haoyue Jiang, Luca Moreschini, Catherine Xu, Alexei Fedorov, Chris Jozwiak, Aaron Bostwick, Guoqing Chang, James G. Analytis, Dung-Hai Lee, Alessandra Lanzara

Abstract: Magnetically intercalated transition metal dichalcogenides are emerging as a rich platform for exploring exotic quantum states in van der Waals magnets. Among them, CoxTaS2 has attracted intense interest following the recent discovery of a distinctive 3Q magnetic ground state and a pronounced topological Hall effect below a critical doping of x=1/3, both intimately tied to cobalt concentration. To… ▽ More Magnetically intercalated transition metal dichalcogenides are emerging as a rich platform for exploring exotic quantum states in van der Waals magnets. Among them, CoxTaS2 has attracted intense interest following the recent discovery of a distinctive 3Q magnetic ground state and a pronounced topological Hall effect below a critical doping of x=1/3, both intimately tied to cobalt concentration. To date, direct signatures of this enigmatic 3Q magnetic order in the electronic structure remain elusive. Here we report a comprehensive doping dependent angle resolved photoemission spectroscopy study that unveils these long-sought fingerprints. Our data reveal an unexpected "inverse Mexican hat" dispersion along the K-M-K direction, accompanied by two van Hove singularities. These features are consistent with theoretical predictions for a 3Q magnetic order near three-quarters band filling on a cobalt triangular lattice. These results provide evidence of 3Q magnetic order in the electronic structure, establishing TMD van der Waals magnets as tunable materials to explore the interplay between magnetism and topology. △ Less

Submitted 7 March, 2026; v1 submitted 16 January, 2026; originally announced January 2026.

Comments: 23 pages, 4 figures. Accepted in Nature Communications

Journal ref: Nature Communications (2026)

Visualization of Tunable Electronic Structure of Monolayer TaIrTe$_4$

Authors: Sandy Adhitia Ekahana, Aalok Tiwari, Souvik Sasmal, Zefeng Cai, Ravi Kumar Bandapelli, I-Hsuan Kao, Jian Tang, Chenbo Min, Tiema Qian, Kenji Watanabe, Takashi Taniguchi, Ni Ni, Qiong Ma, Chris Jozwiak, Eli Rotenberg, Aaron Bostwick, Simranjeet Singh, Noa Marom, Jyoti Katoch

Abstract: Monolayer TaIrTe$_4$ has emerged as an attractive material platform to study intriguing phenomena related to topology and strong electron correlations. Recently, strong interactions have been demonstrated to induce strain and dielectric screening tunable topological phases such as quantum spin Hall insulator (QSHI), trivial insulator, higher-order topological insulator, and metallic phase, in the… ▽ More Monolayer TaIrTe$_4$ has emerged as an attractive material platform to study intriguing phenomena related to topology and strong electron correlations. Recently, strong interactions have been demonstrated to induce strain and dielectric screening tunable topological phases such as quantum spin Hall insulator (QSHI), trivial insulator, higher-order topological insulator, and metallic phase, in the ground state of monolayer TaIrTe$_4$. Moreover, charge dosing has been demonstrated to convert the QSHI into a dual QSHI state. Although the band structure of monolayer TaIrTe$_4$ is central to interpreting its topological phases in transport experiments, direct experimental access to its intrinsic electronic structure has so far remained elusive. Here we report direct measurements of the monolayer TaIrTe$_4$ band structure using spatially resolved micro-angle-resolved photoemission spectroscopy (microARPES) with micrometre-scale resolution. The observed dispersions show quantitative agreement with density functional theory calculations using the Heyd-Scuseria-Ernzerhof hybrid functional, establishing the insulating ground state and revealing no evidence for strong electronic correlations. We further uncover a pronounced electron-hole asymmetry in the doping response. Whereas hole doping is readily induced by electrostatic gating, attempts to introduce electrons via gating or alkali metal deposition do not yield a rigid upward shift of the Fermi level. Fractional charge calculations demonstrate that added electrons instead drive band renormalization and shrink the band gap. Taken together, our experimental and theoretical results identify the microscopic mechanism by which induced charges reshape the band topology of monolayer TaIrTe$_4$, showing that doping can fundamentally alter the electronic structure beyond the rigid band behaviour that is typically assumed. △ Less

Submitted 16 January, 2026; originally announced January 2026.

Influence of Bi Alloying on GaAs Valence Band Structure

Authors: Joshua J. P. Cooper, Jared W. Mitchell, Shane Smolenski, Ming Wen, Eoghan Downey, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, Kai Sun, Dominika Zgid, Na Hyun Jo, Rachel S. Goldman

Abstract: Bi alloying is predicted to transform GaAs from a semiconductor to a topological insulator or semi-metal. To date, studies of the GaAs$_{1-x}$Bi$_x$ alloy band structure have been limited, and the origins of Bi-induced enhancement of the spin-orbit splitting energy, $Δ_\mathrm{SO}$, are unresolved. Here, we present high-resolution angle-resolved photoemission spectroscopy (ARPES) of droplet-free e… ▽ More Bi alloying is predicted to transform GaAs from a semiconductor to a topological insulator or semi-metal. To date, studies of the GaAs$_{1-x}$Bi$_x$ alloy band structure have been limited, and the origins of Bi-induced enhancement of the spin-orbit splitting energy, $Δ_\mathrm{SO}$, are unresolved. Here, we present high-resolution angle-resolved photoemission spectroscopy (ARPES) of droplet-free epitaxial GaAs$_{1-x}$Bi$_x$ films with $x_{\mathrm{Bi}}$ = 0.06. In addition to quantifying the Bi-induced shifts of the light-hole and heavy-hole valence bands, we probe the origins of the Bi-enhanced $Δ_\mathrm{SO}$. Using exact-two-component density functional theory calculations, we identify the key role of Bi p-orbitals in the upward shift of the light-hole and heavy-hole bands that results in the Bi-enhanced $Δ_\mathrm{SO}$. △ Less

Submitted 7 November, 2025; originally announced November 2025.

Direct visualization of gate-tunable flat bands in twisted double bilayer graphene

Authors: Souvik Sasmal, Ryan Muzzio, Ahmed Khalifa, Paulina Majchrzak, Alfred J. H. Jones, I-Hsuan Kao, Kenji Watanabe, Takashi Taniguchi, Simranjeet Singh, Eli Rotenberg, Aaron Bostwick, Chris Jozwiak, Søren Ulstrup, Shubhayu Chatterjee, Jyoti Katoch

Abstract: The symmetry-broken correlated states in twisted double bilayer graphene (TDBG) can be tuned via several external knobs, including twist angle, displacement field, and carrier density. However, a direct, momentum-resolved characterization of how these parameters reshape the flat-band structure remains limited. In this study, we employ micro focused angle-resolved photoemission spectroscopy to inve… ▽ More The symmetry-broken correlated states in twisted double bilayer graphene (TDBG) can be tuned via several external knobs, including twist angle, displacement field, and carrier density. However, a direct, momentum-resolved characterization of how these parameters reshape the flat-band structure remains limited. In this study, we employ micro focused angle-resolved photoemission spectroscopy to investigate the flat-band dispersion of TDBG at a twist angle of 1.6, systematically varying the displacement field and carrier density via electrostatic gating. We directly observe multiple flat moir'e minibands near charge neutrality, including a flat remote valence band residing below the low-energy flat-band manifold. Furthermore, the dominant Coulomb repulsive energy over the flat- band bandwidth suggests favorable conditions for the emergence of interaction-driven correlated phenomena in TDBG. These findings establish that the formation and evolution of flat bands in TDBG arises from the interplay between the electron filling and the displacement field. △ Less

Submitted 22 October, 2025; originally announced October 2025.

Strain-tunability of the multipolar Berry curvature in altermagnet MnTe

Authors: Shane Smolenski, Ning Mao, Dechen Zhang, Yucheng Guo, A. K. M. Ashiquzzaman Shawon, Mingyu Xu, Eoghan Downey, Trisha Musall, Ming Yi, Weiwei Xie, Chris Jozwiak, Aaron Bostwick, Nobumichi Tamura, Eli Rotenberg, Lu Li, Kai Sun, Yang Zhang, Na Hyun Jo

Abstract: The anomalous Hall effect describes the generation of a transverse voltage by a longitudinal current even in the absence of an external magnetic field. While typically observed in ferromagnets, it has also been predicted to arise in altermagnets, materials characterized by rotational symmetries that enable broken time reversal symmetry despite compensated collinear magnetic ordering. These symmetr… ▽ More The anomalous Hall effect describes the generation of a transverse voltage by a longitudinal current even in the absence of an external magnetic field. While typically observed in ferromagnets, it has also been predicted to arise in altermagnets, materials characterized by rotational symmetries that enable broken time reversal symmetry despite compensated collinear magnetic ordering. These symmetries enforce band (anti)crossings that can generate significant contributions to the Berry curvature that drives the anomalous Hall effect. This Berry curvature is predicted to exhibit a characteristic multipolar order, resulting in a symmetry-enforced distribution at or near net compensation which is highly sensitive to perturbations that distort this balance. However, exploring the predicted multipolar Berry curvature of altermagnets and its reversible manipulation remains challenging. Here, we demonstrate evidence for the multipolar nature of the altermagnetic Berry curvature in MnTe by tuning the anomalous Hall effect via uniaxial stress. Upon straining, the magnitude of the anomalous Hall conductivity changes and, at a critical strain of 0.14%, the sign is reversed. Symmetry analysis and density functional theory calculations reveal that this tunability is a direct consequence of the altermagnetic multipolar Berry curvature. Our results provide insight into the role of crystal and magnetic symmetries in the realization of higher-order Berry curvature distributions and their unique tunability. △ Less

Submitted 25 September, 2025; originally announced September 2025.

Spin-polarised surface fermiology of ohmic WSe$_2$/NbSe$_2$ interfaces

Authors: Oliver J. Clark, Thi-Hai-Yen Vu, Ben A. Chambers, Federico Mazzola, Sadhana Sridhar, Geetha Balakrishnan, Aaron Bostwick, Chris Jozwiak, Eli Rotenberg, Sarah L. Harmer, Michael S. Fuhrer, Mark T. Edmonds

Abstract: Discovering and engineering spin-polarised surface states in the electronic structures of condensed matter systems is a crucial first step in development of spintronic devices, wherein spin-polarised bands crossing the Fermi level can facilitate information transfer. Here, we show how the spin-orbit split K-point valleys of monolayer WSe$_2$ can be made potentially suitable for this purpose, despi… ▽ More Discovering and engineering spin-polarised surface states in the electronic structures of condensed matter systems is a crucial first step in development of spintronic devices, wherein spin-polarised bands crossing the Fermi level can facilitate information transfer. Here, we show how the spin-orbit split K-point valleys of monolayer WSe$_2$ can be made potentially suitable for this purpose, despite the semiconducting ground state. By interfacing with metallic 2H-NbSe$_2$, these valence band extrema are shifted by $\sim$800~meV to produce a surface-localised Fermi surface populated only by spin-polarised carriers. By increasing the WSe$_2$ thickness, the Fermi pockets can be moved from K to $Γ$, demonstrating tunability of novel semi-metallic phases that exist atop a substrate additionally possessing charge density wave and superconducting transitions. Together, this study provides spectroscopic understanding into $p$-type, Schottky barrier-free interfaces, which are of urgent interest for bypassing the limitations of current-generation vertical field effect transistors, in addition to longer-term spintronics development. △ Less

Submitted 18 September, 2025; originally announced September 2025.

Comments: 7 pages, 4 figures

Visualizing Electronic Structure of Twisted Bilayer MoTe2 in Devices

Authors: Cheng Chen, William Holtzmann, Xiao-Wei Zhang, Eric Anderson, Shanmei He, Yuzhou Zhao, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, Kenji Watanabe, Takashi Taniguchi, Ting Cao, Di Xiao, Xiaodong Xu, Yulin Chen

Abstract: The pursuit of emergent quantum phenomena lies at the forefront of modern condensed matter physics. A recent breakthrough in this arena is the discovery of the fractional quantum anomalous Hall effect (FQAHE) in twisted bilayer MoTe2 (tbMoTe2), marking a paradigm shift and establishing a versatile platform for exploring the intricate interplay among topology, magnetism, and electron correlations.… ▽ More The pursuit of emergent quantum phenomena lies at the forefront of modern condensed matter physics. A recent breakthrough in this arena is the discovery of the fractional quantum anomalous Hall effect (FQAHE) in twisted bilayer MoTe2 (tbMoTe2), marking a paradigm shift and establishing a versatile platform for exploring the intricate interplay among topology, magnetism, and electron correlations. While significant progress has been made through both optical and electrical transport measurements, direct experimental insights into the electronic structure - crucial for understanding and modeling this system - have remained elusive. Here, using spatially and angle-resolved photoemission spectroscopy (μ-ARPES), we directly map the electronic band structure of tbMoTe2. We identify the valence band maximum, whose partial filling underlies the FQAHE, at the K points, situated approximately 150 meV above the Γ valley. By fine-tuning the doping level via in-situ alkali metal deposition, we also resolve the conduction band minimum at the K point, providing direct evidence that tbMoTe2 exhibits a direct band gap - distinct from all previously known moire bilayer transition metal dichalcogenide systems. These results offer critical insights for theoretical modeling and advance our understanding of fractionalized excitations and correlated topological phases in this emergent quantum material. △ Less

Submitted 10 September, 2025; originally announced September 2025.

Comments: 13 pages, 4 figures

Non-monotonic band flattening near the magic angle of twisted bilayer MoTe$_2$

Authors: Yujun Deng, William Holtzmann, Ziyan Zhu, Timothy Zaklama, Paulina Majchrzak, Takashi Taniguchi, Kenji Watanabe, Makoto Hashimoto, Donghui Lu, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, Liang Fu, Thomas P. Devereaux, Xiaodong Xu, Zhi-Xun Shen

Abstract: Twisted bilayer MoTe$_2$ (tMoTe$_2$) is an emergent platform for exploring exotic quantum phases driven by the interplay between nontrivial band topology and strong electron correlations. Direct experimental access to its momentum-resolved electronic structure is essential for uncovering the microscopic origins of the correlated topological phases therein. Here, we report angle-resolved photoemiss… ▽ More Twisted bilayer MoTe$_2$ (tMoTe$_2$) is an emergent platform for exploring exotic quantum phases driven by the interplay between nontrivial band topology and strong electron correlations. Direct experimental access to its momentum-resolved electronic structure is essential for uncovering the microscopic origins of the correlated topological phases therein. Here, we report angle-resolved photoemission spectroscopy (ARPES) measurements of tMoTe$_2$, revealing pronounced twist-angle-dependent band reconstruction shaped by orbital character, interlayer coupling, and moiré potential modulation. Density functional theory (DFT) captures the qualitative evolution, yet underestimates key energy scales across twist angles, highlighting the importance of electronic correlations. Notably, the hole effective mass at the K point exhibits a non-monotonic dependence on twist angle, peaking near 2°, consistent with band flattening at the magic angle predicted by continuum models. Via electrostatic gating and surface dosing, we further visualize the evolution of electronic structure versus doping, enabling direct observation of the conduction band minimum and confirm tMoTe$_2$ as a direct band gap semiconductor. These results establish a spectroscopic foundation for modeling and engineering emergent quantum phases in this moiré platform. △ Less

Submitted 10 September, 2025; originally announced September 2025.

Comments: 11 pages, 4 figures

Investigating the Electrical Transport Properties and Electronic Structure of Zr2CuSb3

Authors: Eoghan Downey, Soumya S. Bhat, Shane Smolenski, Ruiqi Tang, Carly Mistick, Aaron Bostwick, Chris Jozwiak, Eli Rotenberg, Demet Usanmaz, Na Hyun Jo

Abstract: The checkerboard lattice has been proposed to host topological flat bands as a result of destructive interference among its various electronic hopping terms. However, it has proven challenging to realize experimentally due to the difficulty of isolating this structure from any significant out-of-plane bonding while maintaining structural integrity. Here, single crystals of Zr2CuSb3, a potential ca… ▽ More The checkerboard lattice has been proposed to host topological flat bands as a result of destructive interference among its various electronic hopping terms. However, it has proven challenging to realize experimentally due to the difficulty of isolating this structure from any significant out-of-plane bonding while maintaining structural integrity. Here, single crystals of Zr2CuSb3, a potential candidate for the checkerboard lattice, were synthesized using the solution (self-flux) method, and their structure was confirmed via X-ray diffraction. Electrical transport measurements indicate metallic behavior with electron-dominated carriers. Angle-resolved photoemission spectroscopy reveals multiple electron pockets and significant kz broadening due to its large c-axis and low dispersion features in k z. Density functional theory calculations further disentangle the contributions from each high-symmetry plane, providing a comprehensive characterization of electronic behavior. △ Less

Submitted 25 August, 2025; originally announced August 2025.

Journal ref: Phys. Rev. Materials 10, 025001 (2026)

Mesoscale variations of chemical and electronic landscape on the surface of Weyl semimetal Co$_3$Sn$_2$S$_2$ visualized by ARPES and XPS

Authors: Sudheer Anand Sreedhar, Matthew Staab, Mingkun Chen, Robert Prater, Zihao Shen, Giuseppina Conti, Ittai Sidilkover, Zhenghong Wu, Eli Rotenberg, Aaron Bostwick, Chris Jozwiak, Hadas Soifer, Slavomir Nemsak, Sergey Y. Savrasov, Vsevolod Ivanov, Valentin Taufour, Inna M. Vishik

Abstract: The multiple crystalline terminations in magnetic Weyl semimetal Co$_3$Sn$_2$S$_2$ display distinct topological and trivial surface states, which have successfully been distinguished experimentally. However, a model of pure terminations is known to be inadequate because these surfaces exhibit a high degree of spatial heterogeneity and point disorder. Here we perform a spectromicroscopy study of th… ▽ More The multiple crystalline terminations in magnetic Weyl semimetal Co$_3$Sn$_2$S$_2$ display distinct topological and trivial surface states, which have successfully been distinguished experimentally. However, a model of pure terminations is known to be inadequate because these surfaces exhibit a high degree of spatial heterogeneity and point disorder. Here we perform a spectromicroscopy study of the surface chemistry and surface electronic structure using photoemission measurements in combination with first-principles calculations of core levels. We identify an intermediate region with properties distinct from both the sulfur and tin terminations, and demonstrate that the spectral features in this region can be associated with a disordered termination with a varying density of surface tin vacancies. This work establishes heuristics for identifying variable surface disorder using photoemission, an important prerequisite to experimentally establishing the behavior of momentum-space topological surface features subject to variable surface disorder on a single cleave. △ Less

Submitted 22 October, 2025; v1 submitted 3 August, 2025; originally announced August 2025.

Journal ref: Phys. Rev. B 112, 245154 (2025)

Local interface effects modulate global charge order and optical properties of 1T-TaS$_2$/1H-WSe$_2$ heterostructures

Authors: Samra Husremović, Valerie S. McGraw, Medha Dandu, Lilia S. Xie, Sae Hee Ryu, Oscar Gonzalez, Shannon S. Fender, Madeline Van Winkle, Karen C. Bustillo, Takashi Taniguchi, Kenji Watanabe, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, Archana Raja, Katherine Inzani, D. Kwabena Bediako

Abstract: 1T-TaS$_2$ is a layered charge density wave (CDW) crystal exhibiting sharp phase transitions and associated resistance changes. These resistance steps could be exploited for information storage, underscoring the importance of controlling and tuning CDW states. Given the importance of out-of-plane interactions in 1T-TaS$_2$, modulating interlayer interactions by heterostructuring is a promising met… ▽ More 1T-TaS$_2$ is a layered charge density wave (CDW) crystal exhibiting sharp phase transitions and associated resistance changes. These resistance steps could be exploited for information storage, underscoring the importance of controlling and tuning CDW states. Given the importance of out-of-plane interactions in 1T-TaS$_2$, modulating interlayer interactions by heterostructuring is a promising method for tailoring CDW phase transitions. In this work, we investigate the optical and electronic properties of heterostructures comprising 1T-TaS$_2$ and monolayer 1H-WSe$_2$. By systematically varying the thickness of 1T-TaS$_2$ and its azimuthal alignment with 1H-WSe$_2$, we find that intrinsic moiré strain and interfacial charge transfer introduce CDW disorder in 1T-TaS$_2$ and modify the CDW ordering temperature. Furthermore, our studies reveal that the interlayer alignment impacts the exciton dynamics in 1H-WSe$_2$, indicating that heterostructuring can concurrently tailor the electronic phases in 1T-TaS$_2$ and the optical properties of 1H-WSe$_2$. This work presents a promising approach for engineering optoelectronic behavior of heterostructures that integrate CDW materials and semiconductors. △ Less

Submitted 2 August, 2025; originally announced August 2025.

Single domain spectroscopic signatures of a magnetic Kagome metal

Authors: L. Plucinski, G. Bihlmayer, Y. Mokrousov, Yishui Zhou, Yixi Su, A. Bostwick, C. Jozwiak, E. Rotenberg, D. Usachov, C. M. Schneider

Abstract: Spin- and orbital-resolved access to the electronic bands is necessary to establish key properties of quantum materials such as the quantum-geometric tensor. Despite recent revival on magnetic Kagome compounds, no spectroscopic access to their magnetic properties has been available so far due to small domain sizes and lack of appropriate techniques. Furthermore, their real space magnetic texture i… ▽ More Spin- and orbital-resolved access to the electronic bands is necessary to establish key properties of quantum materials such as the quantum-geometric tensor. Despite recent revival on magnetic Kagome compounds, no spectroscopic access to their magnetic properties has been available so far due to small domain sizes and lack of appropriate techniques. Furthermore, their real space magnetic texture is often complex and temperature-dependent. We investigate the magnetic Kagome metal DyMn$_6$Sn$_6$ using high-resolution micro-focused circular-dichroic angle-resolved photoemission ($μ$-CD-ARPES) to probe its magnetic and electronic properties. By tuning the kinetic energy to various features of the Dy $4f$ multiplet, we resolve magnetic domains in samples cryo-cooled down to 20 K. Smaller, but clear signatures are detected in the Mn $3p$ levels. The behavior of both Dy $4f$ and Mn $3p$ features are in remarkable agreement with our modeling based on the Hartree-Fock method, revealing ferrimagnetic alignment of Dy and Mn local moments, and further strengthening our interpretation. Adjusting the energy to the Mn $3d$-dominated valence bands reveals signatures which we relate to the orbital magnetization through a comparison to {\it ab initio} electronic structure calculations. Our study establishes the spectroscopic access to a single magnetic domain in a Kagome metal, paving the way for further research into imaging magnetic phases of novel magnetic materials using $μ$-CD-ARPES. △ Less

Submitted 16 July, 2025; originally announced July 2025.

Comments: 7 pages, 4 figures

Dark states of electrons in a quantum system with two pairs of sublattices

Authors: Yoonah Chung, Minsu Kim, Yeryn Kim, Seyeong Cha, Joon Woo Park, Jeehong Park, Yeonjin Yi, Dongjoon Song, Jung Hyun Ryu, Kimoon Lee, Timur K. Kim, Cephise Cacho, Jonathan Denlinger, Chris Jozwiak, Eli Rotenberg, Aaron Bostwick, Keun Su Kim

Abstract: A quantum state of matter that is forbidden to interact with photons and is therefore undetectable by spectroscopic means is called a dark state. This basic concept can be applied to condensed matter where it suggests that a whole band of quantum states could be undetectable across a full Brillouin zone. Here we report the discovery of such condensed matter dark states in palladium diselenide as a… ▽ More A quantum state of matter that is forbidden to interact with photons and is therefore undetectable by spectroscopic means is called a dark state. This basic concept can be applied to condensed matter where it suggests that a whole band of quantum states could be undetectable across a full Brillouin zone. Here we report the discovery of such condensed matter dark states in palladium diselenide as a model system that has two pairs of sublattices in the primitive cell. By using angle-resolved photoemission spectroscopy, we find valence bands that are practically unobservable over the whole Brillouin zone at any photon energy, polarisation, and scattering plane. Our model shows that two pairs of sublattices located at half-translation positions and related by multiple glide-mirror symmetries make their relative quantum phases polarised into only four kinds, three of which become dark due to double destructive interference. This mechanism is generic to other systems with two pairs of sublattices, and we show how the phenomena observed in cuprates, lead-halide perovskites, and density wave systems can be resolved by the mechanism of dark states. Our results suggest that the sublattice degree of freedom, which has been overlooked so far, should be considered in the study of correlated phenomena and optoelectronic characteristics. △ Less

Submitted 10 July, 2025; originally announced July 2025.

Journal ref: Nature Physics 20, 1582-1588 (2024)

Electronic rotons and Wigner crystallites in a two-dimensional dipole liquid

Authors: Soobin Park, Minjae Huh, Chris Jozwiak, Eli Rotenberg, Aaron Bostwick, Keun Su Kim

Abstract: A key concept proposed by Landau to explain superfluid liquid helium is the elementary excitation of quantum particles called rotons. The irregular arrangement of atoms in a liquid forms the aperiodic dispersion of rotons that played a pivotal role in understanding fractional quantum Hall liquid (magneto-rotons) and the supersolidity of Bose-Einstein condensates. Even for a two-dimensional electro… ▽ More A key concept proposed by Landau to explain superfluid liquid helium is the elementary excitation of quantum particles called rotons. The irregular arrangement of atoms in a liquid forms the aperiodic dispersion of rotons that played a pivotal role in understanding fractional quantum Hall liquid (magneto-rotons) and the supersolidity of Bose-Einstein condensates. Even for a two-dimensional electron or dipole liquid in the absence of a magnetic field, their repulsive interactions were predicted to form a roton minimum that can be used to trace the transition to Wigner crystals and superconductivity, but it has not been observed. Here, we report the observation of such electronic rotons in a two-dimensional dipole liquid of alkali-metal ions doping charges to surface layers of black phosphorus. Our data reveal a striking aperiodic dispersion of rotons characterized by a local minimum of energy at a finite momentum. As the density of dipoles decreases, where interactions dominate over kinetic energy, the roton gap reduces to 0 as in crystals, signalling Wigner crystallisation. Our model shows the importance of short-range order arising from repulsion between dipoles, which can be viewed as the formation of Wigner crystallites (bubbles or stripes) floating in the sea of Fermi liquids. Our results reveal that the primary origin of electronic rotons (and the pseudogap) is strong correlations. △ Less

Submitted 10 July, 2025; originally announced July 2025.

Journal ref: Nature 634, 813-817 (2024)

Pseudogap in a crystalline insulator doped by disordered metals

Authors: Sae Hee Ryu, Minjae Huh, Do Yun Park, Chris Jozwiak, Eli Rotenberg, Aaron Bostwick, Keun Su Kim

Abstract: A key to understand how electrons behave in crystalline solids is the band structure that connects the energy of electron waves to their wavenumber (k). Even in the phase of matter with only short-range order (liquid or amorphous solid), the coherent part of electron waves still possesses a band structure. Theoretical models for the band structure of liquid metals were formulated more than 5 decad… ▽ More A key to understand how electrons behave in crystalline solids is the band structure that connects the energy of electron waves to their wavenumber (k). Even in the phase of matter with only short-range order (liquid or amorphous solid), the coherent part of electron waves still possesses a band structure. Theoretical models for the band structure of liquid metals were formulated more than 5 decades ago, but thus far, bandstructure renormalization and pseudogap induced by resonance scattering have remained unobserved. Here, we report the observation of this unusual band structure at the interface of a crystalline insulator (black phosphorus) and disordered dopants (alkali metals). We find that a conventional parabolic band structure of free electrons bends back towards zero k with the pseudogap of 30-240 meV from the Fermi level. This is k renormalization caused by resonance scattering that leads to the formation of quasi-bound states in the scattering potential of alkali-metal ions. The depth of this potential tuned by different kinds of alkali metal (Na, K, Rb, and Cs) allows to classify the pseudogap of p-wave and d-wave resonance. Our results may provide a clue to the puzzling spectrum of various crystalline insulators doped by disordered dopants, such as the waterfall dispersion in cuprates. △ Less

Submitted 10 July, 2025; originally announced July 2025.

Journal ref: Nature 596, 68-73 (2021)

Designer three-dimensional electronic bands in asymmetric transition metal dichalcogenide heterostructures

Authors: Oliver J. Clark, Anugrah Azhar, Ben A. Chambers, Daniel McEwen, Thi-Hai-Yen Vu, M. Tofajjol H. Bhuiyan, Rodion V. Belosludov, Aaron Bostwick, Chris Jozwiak, Eli Rotenberg, Seng Huat Lee, Zhiqiang Mao, Geetha Balakrishnan, Federico Mazzola, Sarah L. Harmer, Michael S. Fuhrer, M. Saeed Bahramy, Mark. T. Edmonds

Abstract: Van der Waals materials enable the construction of atomically sharp interfaces between compounds with distinct crystal and electronic properties. This is dramatically exploited in moiré systems, where a lattice mismatch or twist between monolayers generates an emergent in-plane periodicity, giving rise to electronic properties absent in the constituent materials. In contrast, vertical superlattice… ▽ More Van der Waals materials enable the construction of atomically sharp interfaces between compounds with distinct crystal and electronic properties. This is dramatically exploited in moiré systems, where a lattice mismatch or twist between monolayers generates an emergent in-plane periodicity, giving rise to electronic properties absent in the constituent materials. In contrast, vertical superlattices, formed by stacking dissimilar materials in the out-of-plane direction on the nanometer scale, have received far less attention despite their potential to realize analogous emergent phenomena in three dimensions. Through angle-resolved photoemission spectroscopy and density functional theory, we investigate six-to-eight-layer transition metal dichalcogenide (TMD) heterostructures constructed from pairs of stacked few-layer materials. Counterintuitively, we find that even these single superlattice units can host fully-delocalised bands, evidencing a robust coherent interlayer coupling across lattice-mismatched interfaces over extended spatial scales. We show how uncompensated semimetallic phases and energetically-mismatched topological surface states are readily and exclusively stabilized within such asymmetrical architectures. These findings establish two-component heterostructures in the intermediate layer-regime as platforms to invoke and control unprecedented combinations and instances of the diverse quantum phases native to many-layer TMDs. △ Less

Submitted 16 September, 2025; v1 submitted 23 March, 2025; originally announced March 2025.

Comments: 23 pages, 14 Figures including SI

Journal ref: Newton 100401 (2026)

Hund flat band in a frustrated spinel oxide

Authors: Dongjin Oh, Alexander Hampel, Joshua P. Wakefield, Peter Moen, Steef Smit, Xiangyu Luo, Marta Zonno, Sergey Gorovikov, Mats Leandersson, Craig Polley, Asish K. Kundu, Anil Rajapitamahuni, Elio Vescovo, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, Masahiko Isobe, Manish Verma, Matteo Crispino, Martin Grundner, Fabian B. Kugler, Olivier Parcollet, Ulrich Schollwöck, Hidenori Takagi, Andrea Damascelli , et al. (4 additional authors not shown)

Abstract: Electronic flat bands associated with quenched kinetic energy and heavy electron mass have attracted great interest for promoting strong electronic correlations and emergent phenomena such as high-temperature charge fractionalization and superconductivity. Intense experimental and theoretical research has been devoted to establishing the rich non-trivial metallic and heavy fermion phases intertwin… ▽ More Electronic flat bands associated with quenched kinetic energy and heavy electron mass have attracted great interest for promoting strong electronic correlations and emergent phenomena such as high-temperature charge fractionalization and superconductivity. Intense experimental and theoretical research has been devoted to establishing the rich non-trivial metallic and heavy fermion phases intertwined with such localized electronic states. Here, we investigate the transition metal oxide spinel LiV2O4, an enigmatic heavy fermion compound lacking localized f orbital states. We use angle-resolved photoemission spectroscopy and dynamical mean field theory to reveal a new kind of correlation-induced flat band with suppressed inter-atomic electron hopping arising from intra-atomic Hund coupling. The appearance of heavy quasiparticles is ascribed to a proximate orbital-selective Mott state characterized by fluctuating local moments as evidenced by complementary magnetotransport measurements. The spectroscopic fingerprints of long-lived quasiparticles and their disappearance with increasing temperature further support the emergence of a high-temperature bad metal state observed in transport data. This work resolves a long-standing puzzle on the origin of heavy fermion behavior and unconventional transport in LiV2O4. Simultaneously, it opens a new path to achieving flat bands through electronic interactions in d-orbital systems with geometrical frustration, potentially enabling the realization of exotic phases of matter such as the fractionalized Fermi liquids. △ Less

Submitted 16 February, 2025; v1 submitted 10 February, 2025; originally announced February 2025.

Comments: 21 pages, 4 figures

Journal ref: Proc. Natl. Acad. Sci. U.S.A. 122 (45) e2518213122 (2025)

Mapping the three-dimensional fermiology of the triangular lattice magnet EuAg$_4$Sb$_2$

Authors: J. Green, Harry W. T. Morgan, Morgaine Mandigo-Stoba, William T. Laderer, Kuan-Yu Wey, Asari G. Prado, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, Christopher Gutiérrez, Anastassia N. Alexandrova, Ni Ni

Abstract: In this paper, we report the temperature-field phase diagram as well as present a comprehensive study of the electronic structure and three-dimensional fermiology of the triangular-lattice magnet EuAg$_4$Sb$_2$, utilizing quantum oscillation measurements, angle-resolved photoemission spectroscopy and first-principles calculations. The complex magnetic phase diagram of EuAg$_4$Sb$_2$ highlights man… ▽ More In this paper, we report the temperature-field phase diagram as well as present a comprehensive study of the electronic structure and three-dimensional fermiology of the triangular-lattice magnet EuAg$_4$Sb$_2$, utilizing quantum oscillation measurements, angle-resolved photoemission spectroscopy and first-principles calculations. The complex magnetic phase diagram of EuAg$_4$Sb$_2$ highlights many transitions through nontrivial AFM states. Shubnikov-de Haas and de Haas-van Alphen oscillations were observed in the polarized ferromagnetic state of EuAg$_4$Sb$_2$, revealing three pairs of distinct spin-split frequency branches with small effective masses. A comparison of the angle-dependent oscillation data with first-principles calculations in the ferromagnetic state and angle-resolved photoemission spectra shows good agreement, identifying tubular hole pockets and hourglass-shaped hole pockets at the Brillouin zone center, as well as diamond-shaped electron pockets at the zone boundary. As the temperature increases, the frequency branches of the tiny hourglass pockets evolve into a more cylindrical shape, while the larger pockets remain unchanged. This highlights that variations in exchange splitting, driven by changes in the magnetic moment, primarily impact the small Fermi pockets without significantly altering the overall band structure. This is consistent with first-principles calculations, which show minimal changes near the Fermi level across ferromagnetic and simple antiferromagnetic states or under varying on-site Coulomb repulsion. △ Less

Submitted 17 January, 2025; originally announced January 2025.

Comments: 10 pages, 5 figures

Measurements of the quantum geometric tensor in solids

Authors: Mingu Kang, Sunje Kim, Yuting Qian, Paul M. Neves, Linda Ye, Junseo Jung, Denny Puntel, Federico Mazzola, Shiang Fang, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, Jun Fuji, Ivana Vobornik, Jae-Hoon Park, Joseph G. Checkelsky, Bohm-Jung Yang, Riccardo Comin

Abstract: Understanding the geometric properties of quantum states and their implications in fundamental physical phenomena is at the core of modern physics. The Quantum Geometric Tensor (QGT) is a central physical object in this regard, encoding complete information about the geometry of the quantum state. The imaginary part of the QGT is the well-known Berry curvature, which plays a fundamental role in th… ▽ More Understanding the geometric properties of quantum states and their implications in fundamental physical phenomena is at the core of modern physics. The Quantum Geometric Tensor (QGT) is a central physical object in this regard, encoding complete information about the geometry of the quantum state. The imaginary part of the QGT is the well-known Berry curvature, which plays a fundamental role in the topological magnetoelectric and optoelectronic phenomena. The real part of the QGT is the quantum metric, whose importance has come to prominence very recently, giving rise to a new set of quantum geometric phenomena, such as anomalous Landau levels, flat band superfluidity, excitonic Lamb shifts, and nonlinear Hall effect. Despite the central importance of the QGT, its experimental measurements have been restricted only to artificial two-level systems. In this work, we develop a framework to measure the QGT (both quantum metric and Berry curvature) in crystalline solids using polarization-, spin-, and angle-resolved photoemission spectroscopy. Using this framework, we demonstrate the effective reconstruction of the QGT in solids in the archetype kagome metal CoSn, which hosts topological flat bands. The key idea is to introduce another geometrical tensor, the quasi-QGT, whose components, the band Drude weight and orbital angular momentum, are experimentally accessible and can be used for extracting the QGT. Establishing such a momentum- and energy-resolved spectroscopic probe of the QGT is poised to significantly advance our understanding of quantum geometric responses in a wide range of crystalline systems. △ Less

Submitted 23 December, 2024; originally announced December 2024.

Journal ref: Nat. Phys. (2024)

Insulator to Metal Transition under High Pressure in FeNb$_3$Se$_{10}$

Authors: Haozhe Wang, Shuyuan Huyan, Eoghan Downey, Yang Wang, Shane Smolenski, Du Li, Li Yang, Aaron Bostwick, Chris Jozwiak, Eli Rotenberg, Sergey L. Bud'ko, Paul C. Canfield, R. J. Cava, Na Hyun Jo, Weiwei Xie

Abstract: Non-magnetic FeNb$_3$Se$_{10}$ has been demonstrated to be an insulator at ambient pressure through both theoretical calculations and experimental measurements and it does not host topological surface states. Here we show that on the application of pressure, FeNb$_3$Se$_{10}$ transitions to a metallic state at around 3.0 GPa. With a further increase in pressure, its resistivity becomes independent… ▽ More Non-magnetic FeNb$_3$Se$_{10}$ has been demonstrated to be an insulator at ambient pressure through both theoretical calculations and experimental measurements and it does not host topological surface states. Here we show that on the application of pressure, FeNb$_3$Se$_{10}$ transitions to a metallic state at around 3.0 GPa. With a further increase in pressure, its resistivity becomes independent of both temperature and pressure. Its crystal structure is maintained to at least 4.4 GPa. △ Less

Submitted 10 September, 2024; originally announced September 2024.

Comments: 20 pages, 5 figures

Ultrafast creation of a light induced semimetallic state in strongly excited 1T-TiSe$_2$

Authors: Maximilian Huber, Yi Lin, Giovanni Marini, Luca Moreschini, Chris Jozwiak, Aaron Bostwick, Matteo Calandra, Alessandra Lanzara

Abstract: Screening, a ubiquitous phenomenon associated with the shielding of electric fields by surrounding charges, has been widely adopted as a means to modify a material's properties. While so far most studies have relied on static changes of screening through doping or gating, here we demonstrate that screening can also drive the onset of distinct quantum states on the ultrafast timescale. By using tim… ▽ More Screening, a ubiquitous phenomenon associated with the shielding of electric fields by surrounding charges, has been widely adopted as a means to modify a material's properties. While so far most studies have relied on static changes of screening through doping or gating, here we demonstrate that screening can also drive the onset of distinct quantum states on the ultrafast timescale. By using time and angle-resolved photoemission spectroscopy we show that intense optical excitation can drive 1T-TiSe$_2$, a prototypical charge density wave material, almost instantly from a gapped into a semimetallic state. By systematically comparing changes in bandstructure over time and excitation strength with theoretical calculations we find that the appearance of this state is likely caused by a dramatic reduction of the screening length. In summary, this work showcases how optical excitation enables the screening driven design of a non-equilibrium semimetallic phase in TiSe$_2$, possibly providing a general pathway into highly screened phases in other strongly correlated materials. △ Less

Submitted 16 August, 2024; originally announced August 2024.

Journal ref: Science Advances 10 (2024)

Revealing the Electronic Structure of van der Waals Antiferromagnetic NiPS$_3$ through Synchrotron-Based $μ$-ARPES and Alkali Metal Dosing

Authors: Yifeng Cao, Qishuo Tan, Yucheng Guo, Clóvis Guerim Vieira, Mário S. C. Mazzon, Jude Laverock, Nicholas Russo, Hongze Gao, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, Jinghua Guo, Ming Yi, Matheus J. S. Matos, Xi Ling, Kevin E. Smith

Abstract: This study presents a comprehensive analysis of the band structure in NiPS$_3$, a van der Waals layered antiferromagnet, utilizing high-resolution synchrotron-based angle-resolved photoemission spectroscopy (ARPES) and corroborative density functional theory (DFT) calculations. By tuning the parameters of the light source, we obtained a very clear and wide energy range band structure of NiPS$_3$.… ▽ More This study presents a comprehensive analysis of the band structure in NiPS$_3$, a van der Waals layered antiferromagnet, utilizing high-resolution synchrotron-based angle-resolved photoemission spectroscopy (ARPES) and corroborative density functional theory (DFT) calculations. By tuning the parameters of the light source, we obtained a very clear and wide energy range band structure of NiPS$_3$. Comparison with DFT calculations allows for the identification of the orbital character of the observed bands. Our DFT calculations perfectly match the experimental results, and no adaptations were made to the calculations based on the experimental outcomes. The appearance of novel electronic structure upon alkali metal dosing (AMD) were also obtained in this ARPES study. Above valence band maximum, structure of conduction bands and bands from defect states were firstly observed in NiPS$_3$. We provide the direct determination of the band gap of NiPS$_3$ as 1.3 eV from the band structure by AMD. In addition, detailed temperature dependent ARPES spectra were obtained across a range that spans both below and above the Néel transition temperature of NiPS$_3$. We found that the paramagnetic and antiferromagnetic states have almost identical spectra, indicating the highly localized nature of Ni $d$ states. △ Less

Submitted 22 December, 2025; v1 submitted 2 July, 2024; originally announced July 2024.

Comments: 8 figures

Tailored topotactic chemistry unlocks heterostructures of magnetic intercalation compounds

Authors: Samra Husremović, Oscar Gonzalez, Berit H. Goodge, Lilia S. Xie, Zhizhi Kong, Wanlin Zhang, Sae Hee Ryu, Stephanie M. Ribet, Karen C. Bustillo, Chengyu Song, Jim Ciston, Takashi Taniguchi, Kenji Watanabe, Colin Ophus, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, D. Kwabena Bediako

Abstract: The construction of thin film heterostructures has been a widely successful archetype for fabricating materials with emergent physical properties. This strategy is of particular importance for the design of multilayer magnetic architectures in which direct interfacial spin--spin interactions between magnetic phases in dissimilar layers lead to emergent and controllable magnetic behavior. However,… ▽ More The construction of thin film heterostructures has been a widely successful archetype for fabricating materials with emergent physical properties. This strategy is of particular importance for the design of multilayer magnetic architectures in which direct interfacial spin--spin interactions between magnetic phases in dissimilar layers lead to emergent and controllable magnetic behavior. However, crystallographic incommensurability and atomic-scale interfacial disorder can severely limit the types of materials amenable to this strategy, as well as the performance of these systems. Here, we demonstrate a method for synthesizing heterostructures comprising magnetic intercalation compounds of transition metal dichalcogenides (TMDs), through directed topotactic reaction of the TMD with a metal oxide. The mechanism of the intercalation reaction enables thermally initiated intercalation of the TMD from lithographically patterned oxide films, giving access to a new family of multi-component magnetic architectures through the combination of deterministic van der Waals assembly and directed intercalation chemistry. △ Less

Submitted 21 June, 2024; originally announced June 2024.

Spin Excitations and Flat Electronic Bands in a Cr-based Kagome Superconductor

Authors: Zehao Wang, Yucheng Guo, Hsiao Yu Huang, Fang Xie, Yuefei Huang, Bin Gao, Ji Seop Oh, Han Wu, Jun Okamoto, Ganesha Channagowdra, Chien Te Chen, Feng Ye, Xingye Lu, Zhaoyu Liu, Zheng Ren, Yuan Fang, Yiming Wang, Ananya Biswas, Yichen Zhang, Ziqin Yue, Cheng Hu, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, Makoto Hashimoto , et al. (11 additional authors not shown)

Abstract: In the quest for topology- and correlation-driven quantum states, kagome lattice materials have garnered significant interest for their band structures, featuring flat bands (FBs) from the quantum destructive interference of the electronic wavefunction. Tuning an FB to the chemical potential could induce electronic instabilities and emergent orders. Despite extensive studies, direct evidence of FB… ▽ More In the quest for topology- and correlation-driven quantum states, kagome lattice materials have garnered significant interest for their band structures, featuring flat bands (FBs) from the quantum destructive interference of the electronic wavefunction. Tuning an FB to the chemical potential could induce electronic instabilities and emergent orders. Despite extensive studies, direct evidence of FBs tuned to the chemical potential and their role in emergent orders in bulk materials remains lacking. Using angle-resolved photoemission spectroscopy, resonant inelastic X-ray scattering, and density functional theory, we show that the low-energy structure of the Cr-based kagome metal superconductor {\Cr} is dominated by FBs at the Fermi level. We also observe low-energy magnetic excitations evolving across the low-temperature transition, largely consistent with the FB shift. Our results suggest that the low-temperature order contains a magnetic origin and that the kagome FBs may play a role in the emergence of this order. △ Less

Submitted 24 November, 2025; v1 submitted 7 June, 2024; originally announced June 2024.

Comments: Published in Nature Communications 16, 7573 (2025). 11 pages, 4 main figures, 13 supplementary figures

Journal ref: Nat Commun 16, 7573 (2025)

Large Exciton Binding Energy in the Bulk van der Waals Magnet CrSBr

Authors: Shane Smolenski, Ming Wen, Qiuyang Li, Eoghan Downey, Adam Alfrey, Wenhao Liu, Aswin L. N. Kondusamy, Aaron Bostwick, Chris Jozwiak, Eli Rotenberg, Liuyan Zhao, Hui Deng, Bing Lv, Dominika Zgid, Emanuel Gull, Na Hyun Jo

Abstract: Excitons, bound electron-hole pairs, influence the optical properties in strongly interacting solid state systems. Excitons and their associated many-body physics are typically most stable and pronounced in monolayer materials. Bulk systems with large exciton binding energies, on the other hand, are rare and the mechanisms driving their stability are still relatively unexplored. Here, we report an… ▽ More Excitons, bound electron-hole pairs, influence the optical properties in strongly interacting solid state systems. Excitons and their associated many-body physics are typically most stable and pronounced in monolayer materials. Bulk systems with large exciton binding energies, on the other hand, are rare and the mechanisms driving their stability are still relatively unexplored. Here, we report an exceptionally large exciton binding energy in single crystals of the bulk van der Waals antiferromagnet CrSBr. Utilizing state-of-the-art angle-resolved photoemission spectroscopy and self-consistent ab-initio GW calculations, we present direct spectroscopic evidence that robust electronic and structural anisotropy can significantly amplify the exciton binding energy within bulk crystals. Furthermore, the application of a vertical electric field enables broad tunability of the optical and electronic properties. Our results indicate that CrSBr is a promising material for the study of the role of anisotropy in strongly interacting bulk systems and for the development of exciton-based optoelectronics. △ Less

Submitted 20 March, 2024; originally announced March 2024.

Journal ref: Nat Commun 16, 1134 (2025)

Revealing the EuCd_{2}As_{2} Semiconducting Band Gap via n-type La-Doping

Authors: Ryan A. Nelson, Jesaiah King, Shuyu Cheng, Archibald J. Williams, Christopher Jozwiak, Aaron Bostwick, Eli Rotenberg, Souvik Sasmal, I-Hsuan Kao, Aalok Tiwari, Natalie R. Jones, Chuting Cai, Emma Martin, Andrei Dolocan, Li Shi, Roland Kawakami, Joseph P. Heremans, Jyoti Katoch, Joshua E. Goldberger

Abstract: EuCd_{2}As_{2} has attracted considerable interest as one of the few magnetic Weyl semimetal candidate materials, although recently there have been emerging reports that claim it to have a semiconducting electronic structure. To resolve this debate, we established the growth of n-type EuCd_{2}As_{2} crystals, to directly visualize the nature of the conduction band using angle resolve photoemission… ▽ More EuCd_{2}As_{2} has attracted considerable interest as one of the few magnetic Weyl semimetal candidate materials, although recently there have been emerging reports that claim it to have a semiconducting electronic structure. To resolve this debate, we established the growth of n-type EuCd_{2}As_{2} crystals, to directly visualize the nature of the conduction band using angle resolve photoemission spectroscopy (ARPES). We show that La-doping leads to n-type transport signatures in both the thermopower and Hall effect measurements, in crystals with doping levels at 2 - 6 x 10^{17} e^{-} cm^{-3}. Both p-type and n-type doped samples exhibit antiferromagnetic ordering at 9 K. ARPES experiments at 6 K clearly show the presence of the conduction band minimum at 0.8 eV above the valence band maximum, which is further corroborated by the observation of a 0.71 - 0.72 eV band gap in room temperature diffuse reflectance absorbance measurements. Together these findings unambiguously show that EuCd_{2}As_{2} is indeed a semiconductor with a substantial band gap and not a topological semimetal. △ Less

Submitted 4 March, 2024; originally announced March 2024.

Nodal fermions in a strongly spin-orbit coupled frustrated pyrochlore superconductor

Authors: Dongjin Oh, Junha Kang, Yuting Qian, Shiang Fang, Mingu Kang, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, Joseph G. Checkelsky, Liang Fu, Tomasz Klimczuk, Michal J. Winiarski, Bohm-Jung Yang, Riccardo Comin

Abstract: The pyrochlore lattice, a three-dimensional network of corner-sharing tetrahedra, is a promising material playground for correlated topological phases arising from the interplay between spin-orbit coupling (SOC) and electron-electron interactions. Due to its geometrically frustrated lattice structure, exotic correlated states on the pyrochlore lattice have been extensively studied using various sp… ▽ More The pyrochlore lattice, a three-dimensional network of corner-sharing tetrahedra, is a promising material playground for correlated topological phases arising from the interplay between spin-orbit coupling (SOC) and electron-electron interactions. Due to its geometrically frustrated lattice structure, exotic correlated states on the pyrochlore lattice have been extensively studied using various spin Hamiltonians in the localized limit. On the other hand, the topological properties of the electronic structure in the pyrochlore lattice have rarely been explored, due to the scarcity of pyrochlore materials in the itinerant paramagnetic limit. Here, we explore the topological electronic band structure of pyrochlore superconductor RbBi$_{2}$ using angle-resolved photoemission spectroscopy. Thanks to the strong SOC of the Bi pyrochlore network, we experimentally confirm the existence of three-dimensional (3D) massless Dirac fermions enforced by nonsymmorphic symmetry, as well as a 3D quadratic band crossing protected by cubic crystalline symmetry. Furthermore, we identify an additional 3D linear Dirac dispersion associated with band inversion protected by threefold rotation symmetry. These observations reveal the rich non-trivial band topology of itinerant pyrochlore lattice systems in the strong SOC regime. Through manipulation of electron correlations and SOC of the frustrated pyrochlore lattices, this material platform is a natural host for exotic phases of matter, including the fractionalized quantum spin Hall effect in the topological Mott insulator phase, as well as axion electrodynamics in the axion insulator phase. △ Less

Submitted 6 February, 2024; originally announced February 2024.

Comments: 18 pages, 4 figures

Flat Bands at the Fermi Level in Unconventional Superconductor YFe2Ge2

Authors: R. Kurleto, C. -H. Wu, S. Acharya, D. M. Narayan, B. S. Berggren, P. Hao, A. Shackelford, H. R. Whitelock, Z. Sierzega, M. Hashimoto, D. Lu, C. Jozwiak, R. P. Cline, D. Pashov, J. Chen, M. van Schilfgaarde, F. M. Grosche, D. S. Dessau

Abstract: We report heavy electron behavior in unconventional superconductor YFe$_2$Ge$_2$ ($T_C \,{=}\, 1.2$ K). We directly observe very heavy bands ($m_\mathrm{eff}\sim 25 m_e$) within $\sim$10 meV of the Fermi level $E_{F}$ using angle-resolved photoelectron spectroscopy (ARPES). The flat bands reside at the X points of the Brillouin zone and are composed principally of $d_{xz}$ and $d_{yz}$ orbitals. W… ▽ More We report heavy electron behavior in unconventional superconductor YFe$_2$Ge$_2$ ($T_C \,{=}\, 1.2$ K). We directly observe very heavy bands ($m_\mathrm{eff}\sim 25 m_e$) within $\sim$10 meV of the Fermi level $E_{F}$ using angle-resolved photoelectron spectroscopy (ARPES). The flat bands reside at the X points of the Brillouin zone and are composed principally of $d_{xz}$ and $d_{yz}$ orbitals. We utilize many-body perturbative theory, GW, to calculate the electronic structure of this material, obtaining excellent agreement with the ARPES data with relatively minor band renormalizations and band shifting required. We obtain further agreement at the Dynamical Mean Field Theory (DMFT) level, highlighting the emergence of the many-body physics at low energies (near $E_F$) and temperatures. △ Less

Submitted 15 November, 2023; originally announced November 2023.

Comments: 5 figures, 10 pages

Controlling spin-orbit coupling to tailor type-II Dirac bands

Authors: Nguyen Huu Lam, Phuong Lien Nguyen, Byoung Ki Choi, Trinh Thi Ly, Ganbat Duvjir, Tae Gyu Rhee, Yong Jin Jo, Tae Heon Kim, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, Younghun Hwang, Young Jun Chang, Jaekwang Lee, Jungdae Kim

Abstract: NiTe2, a type-II Dirac semimetal with strongly tilted Dirac band, has been explored extensively to understand its intriguing topological properties. Here, using density-functional theory (DFT) calculations, we report that the strength of spin-orbit coupling (SOC) in NiTe2 can be tuned by Se substitution. This results in negative shifts of the bulk Dirac point (BDP) while preserving the type-II Dir… ▽ More NiTe2, a type-II Dirac semimetal with strongly tilted Dirac band, has been explored extensively to understand its intriguing topological properties. Here, using density-functional theory (DFT) calculations, we report that the strength of spin-orbit coupling (SOC) in NiTe2 can be tuned by Se substitution. This results in negative shifts of the bulk Dirac point (BDP) while preserving the type-II Dirac band. Indeed, combined studies using scanning tunneling spectroscopy (STS) and angle-resolved photoemission spectroscopy (ARPES) confirm that the BDP in the NiTe2-xSex alloy moves from +0.1 eV (NiTe2) to -0.3 eV (NiTeSe) depending on the Se concentrations, indicating the effective tunability of type-II Dirac fermions. Our results demonstrate an approach to tailor the type-II Dirac band in NiTe2 by controlling the SOC strength via chalcogen substitution. This approach can be applicable to different types of topological materials. △ Less

Submitted 22 October, 2023; originally announced October 2023.

Comments: 25 pages, 4 figures

Journal ref: ACS Nano 16, 11227 (2022)

Orbital-selective metal skin induced by alkali-metal-dosing Mott-insulating Ca$_2$RuO$_4$

Authors: M. Horio, F. Forte, D. Sutter, M. Kim, C. G. Fatuzzo, C. E. Matt, S. Moser, T. Wada, V. Granata, R. Fittipaldi, Y. Sassa, G. Gatti, H. M. Rønnow, M. Hoesch, T. K. Kim, C. Jozwiak, A. Bostwick, Eli Rotenberg, I. Matsuda, A. Georges, G. Sangiovanni, A. Vecchione, M. Cuoco, J. Chang

Abstract: Doped Mott insulators are the starting point for interesting physics such as high temperature superconductivity and quantum spin liquids. For multi-band Mott insulators, orbital selective ground states have been envisioned. However, orbital selective metals and Mott insulators have been difficult to realize experimentally. Here we demonstrate by photoemission spectroscopy how Ca$_2$RuO$_4$, upon a… ▽ More Doped Mott insulators are the starting point for interesting physics such as high temperature superconductivity and quantum spin liquids. For multi-band Mott insulators, orbital selective ground states have been envisioned. However, orbital selective metals and Mott insulators have been difficult to realize experimentally. Here we demonstrate by photoemission spectroscopy how Ca$_2$RuO$_4$, upon alkali-metal surface doping, develops a single-band metal skin. Our dynamical mean field theory calculations reveal that homogeneous electron doping of Ca$_2$RuO$_4$ results in a multi-band metal. All together, our results provide compelling evidence for an orbital-selective Mott insulator breakdown, which is unachievable via simple electron doping. Supported by a cluster model and cluster perturbation theory calculations, we demonstrate a novel type of skin metal-insulator transition induced by surface dopants that orbital-selectively hybridize with the bulk Mott state and in turn produce coherent in-gap states. △ Less

Submitted 19 October, 2023; originally announced October 2023.

Comments: A revised version of this manuscript will appear in Communications Physics

Journal ref: Commun. Phys. 6, 323 (2023)

Anomalous excitonic phase diagram in band-gap-tuned Ta2Ni(Se,S)5

Authors: Cheng Chen, Weichen Tang, Xiang Chen, Zhibo Kang, Shuhan Ding, Kirsty Scott, Siqi Wang, Zhenglu Li, Jacob P. C. Ruff, Makoto Hashimoto, Dong-Hui Lu, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, Eduardo H. da Silva Neto, Robert J. Birgeneau, Yulin Chen, Steven G. Louie, Yao Wang, Yu He

Abstract: During a band-gap-tuned semimetal-to-semiconductor transition, Coulomb attraction between electrons and holes can cause spontaneously formed excitons near the zero-band-gap point, or the Lifshitz transition point. This has become an important route to realize bulk excitonic insulators -- an insulating ground state distinct from single-particle band insulators. How this route manifests from weak to… ▽ More During a band-gap-tuned semimetal-to-semiconductor transition, Coulomb attraction between electrons and holes can cause spontaneously formed excitons near the zero-band-gap point, or the Lifshitz transition point. This has become an important route to realize bulk excitonic insulators -- an insulating ground state distinct from single-particle band insulators. How this route manifests from weak to strong coupling is not clear. In this work, using angle-resolved photoemission spectroscopy (ARPES) and high-resolution synchrotron x-ray diffraction (XRD), we investigate the broken symmetry state across the semimetal-to-semiconductor transition in a leading bulk excitonic insulator candidate system Ta2Ni(Se,S)5. A broken symmetry phase is found to be continuously suppressed from the semimetal side to the semiconductor side, contradicting the anticipated maximal excitonic instability around the Lifshitz transition. Bolstered by first-principles and model calculations, we find strong interband electron-phonon coupling to play a crucial role in the enhanced symmetry breaking on the semimetal side of the phase diagram. Our results not only provide insight into the longstanding debate of the nature of intertwined orders in Ta2NiSe5, but also establish a basis for exploring band-gap-tuned structural and electronic instabilities in strongly coupled systems. △ Less

Submitted 13 September, 2023; originally announced September 2023.

Comments: 27 pages, 4 + 9 figures

Journal ref: Nat Commun 14, 7512 (2023)

Discovery of interlayer plasmon polaron in graphene/WS$_2$ heterostructures

Authors: Søren Ulstrup, Yann in 't Veld, Jill A. Miwa, Alfred J. H. Jones, Kathleen M. McCreary, Jeremy T. Robinson, Berend T. Jonker, Simranjeet Singh, Roland J. Koch, Eli Rotenberg, Aaron Bostwick, Chris Jozwiak, Malte Rösner, Jyoti Katoch

Abstract: Harnessing electronic excitations involving coherent coupling to bosonic modes is essential for the design and control of emergent phenomena in quantum materials [1]. In situations where charge carriers induce a lattice distortion due to the electron-phonon interaction, the conducting states get "dressed". This leads to the formation of polaronic quasiparticles that dramatically impact charge tran… ▽ More Harnessing electronic excitations involving coherent coupling to bosonic modes is essential for the design and control of emergent phenomena in quantum materials [1]. In situations where charge carriers induce a lattice distortion due to the electron-phonon interaction, the conducting states get "dressed". This leads to the formation of polaronic quasiparticles that dramatically impact charge transport, surface reactivity, thermoelectric and optical properties, as observed in a variety of crystals and interfaces composed of polar materials [2-6]. Similarly, when oscillations of the charge density couple to conduction electrons the more elusive plasmon polaron emerges [7], which has been detected in electron-doped semiconductors [8-10]. However, the exploration of polaronic effects on low energy excitations is still in its infancy in two-dimensional (2D) materials. Here, we present the discovery of an interlayer plasmon polaron in heterostructures composed of graphene on top of SL WS$_2$. By using micro-focused angle-resolved photoemission spectroscopy (microARPES) during in situ doping of the top graphene layer, we observe a strong quasiparticle peak accompanied by several carrier density-dependent shake-off replicas around the SL WS$_2$ conduction band minimum (CBM). Our results are explained by an effective many-body model in terms of a coupling between SL WS$_2$ conduction electrons and graphene plasmon modes. It is important to take into account the presence of such interlayer collective modes, as they have profound consequences for the electronic and optical properties of heterostructures that are routinely explored in many device architectures involving 2D transition metal dichalcogenides (TMDs) [11-15]. △ Less

Submitted 31 August, 2023; originally announced August 2023.

Comments: 25 pages, 9 figures including Supporting Information

Nature of the current-induced insulator-to-metal transition in Ca$_2$RuO$_4$ as revealed by transport-ARPES

Authors: Cissy T Suen, Igor Marković, Marta Zonno, Niclas Heinsdorf, Sergey Zhdanovich, Na-Hyun Jo, Michael Schmid, Philipp Hansmann, Pascal Puphal, Katrin Fürsich, Valentin Zimmerman, Steef Smit, Christine Au-Yeung, Berend Zwartsenberg, Maximilian Krautloher, Ilya S Elfimov, Roland Koch, Sergey Gorovikov, Chris Jozwiak, Aaron Bostwick, Marcel Franz, Eli Rotenberg, Bernhard Keimer, Andrea Damascelli

Abstract: The Mott insulator Ca$_2$RuO$_4$ exhibits a rare insulator-to-metal transition (IMT) induced by DC current. While structural changes associated with this transition have been tracked by neutron diffraction, Raman scattering, and x-ray spectroscopy, work on elucidating the response of the electronic degrees of freedom is still in progress. Here we unveil the current-induced modifications of the ele… ▽ More The Mott insulator Ca$_2$RuO$_4$ exhibits a rare insulator-to-metal transition (IMT) induced by DC current. While structural changes associated with this transition have been tracked by neutron diffraction, Raman scattering, and x-ray spectroscopy, work on elucidating the response of the electronic degrees of freedom is still in progress. Here we unveil the current-induced modifications of the electronic states of Ca$_2$RuO$_4$ by employing angle-resolved photoemission spectroscopy (ARPES) in conjunction with four-probe transport. Two main effects emerge: a clear reduction of the Mott gap and a modification in the dispersion of the Ru-bands. The changes in dispersion occur exclusively along the $XM$ high-symmetry direction, parallel to the $b$-axis where the greatest in-plane lattice change occurs. These experimental observations, together with dynamical mean-field theory (DMFT) calculations simulated from the current-induced structural distortions, indicate the intimate interplay of lattice and orbital-dependent electronic response in the current-driven IMT. Furthermore, based on a free energy analysis, we demonstrate that the current-induced phase, albeit thermodynamically equivalent, is electronically distinct from the high-temperature zero-current metallic phase. Our results provide insight into the elusive nature of the current-induced IMT of Ca$_2$RuO$_4$ and advance the challenging, yet powerful, technique of transport-ARPES. △ Less

Submitted 6 July, 2024; v1 submitted 10 August, 2023; originally announced August 2023.

Comments: 10 pages, 5 figures

Epitaxial Kagome Thin Films as a Platform for Topological Flat Bands

Authors: Shuyu Cheng, M. Nrisimhamurty, Tong Zhou, Nuria Bagues, Wenyi Zhou, Alexander J. Bishop, Igor Lyalin, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, David W. McComb, Igor Zutic, Roland K. Kawakami

Abstract: Systems with flat bands are ideal for studying strongly correlated electronic states and related phenomena. Among them, kagome-structured metals such as CoSn have been recognized as promising candidates due to the proximity between the flat bands and the Fermi level. A key next step will be to realize epitaxial kagome thin films with flat bands to enable tuning of the flat bands across the Fermi l… ▽ More Systems with flat bands are ideal for studying strongly correlated electronic states and related phenomena. Among them, kagome-structured metals such as CoSn have been recognized as promising candidates due to the proximity between the flat bands and the Fermi level. A key next step will be to realize epitaxial kagome thin films with flat bands to enable tuning of the flat bands across the Fermi level via electrostatic gating or strain. Here we report the band structures of epitaxial CoSn thin films grown directly on insulating substrates. Flat bands are observed using synchrotron-based angle-resolved photoemission spectroscopy (ARPES). The band structure is consistent with density functional theory (DFT) calculations, and the transport properties are quantitatively explained by the band structure and semiclassical transport theory. Our work paves the way to realize flat band-induced phenomena through fine-tuning of flat bands in kagome materials. △ Less

Submitted 28 July, 2023; originally announced July 2023.

Comments: 30 pages, 12 figures

Journal ref: Nano Lett. 23, 7107-7113 (2023)

Spectral Evidence for Local-Moment Ferromagnetism in van der Waals Metals Fe$_3$GaTe$_2$ and Fe$_3$GeTe$_2$

Authors: Han Wu, Chaowei Hu, Yaofeng Xie, Bo Gyu Jang, Jianwei Huang, Yucheng Guo, Shan Wu, Cheng Hu, Ziqin Yue, Yue Shi, Zheng Ren, T. Yilmaz, Elio Vescovo, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, Alexei Fedorov, Jonathan Denlinger, Christoph Klewe, Padraic Shafer, Donghui Lu, Makoto Hashimoto, Junichiro Kono, Robert J. Birgeneau, Xiaodong Xu , et al. (4 additional authors not shown)

Abstract: Magnetism in two-dimensional (2D) materials has attracted considerable attention recently for both fundamental understanding of magnetism and their tunability towards device applications. The isostructural Fe$_3$GeTe$_2$ and Fe$_3$GaTe$_2$ are two members of the Fe-based van der Waals (vdW) ferromagnet family, but exhibit very different Curie temperatures (T$_C$) of 210 K and 360 K, respectively.… ▽ More Magnetism in two-dimensional (2D) materials has attracted considerable attention recently for both fundamental understanding of magnetism and their tunability towards device applications. The isostructural Fe$_3$GeTe$_2$ and Fe$_3$GaTe$_2$ are two members of the Fe-based van der Waals (vdW) ferromagnet family, but exhibit very different Curie temperatures (T$_C$) of 210 K and 360 K, respectively. Here, by using angle-resolved photoemission spectroscopy and density functional theory, we systematically compare the electronic structures of the two compounds. Qualitative similarities in the Fermi surface can be found between the two compounds, with expanded hole pockets in Fe$_3$GaTe$_2$ suggesting additional hole carriers compared to Fe$_3$GeTe$_2$. Interestingly, we observe no band shift in Fe$_3$GaTe$_2$ across its T$_C$ of 360 K, compared to a small shift in Fe$_3$GeTe$_2$ across its T$_C$ of 210 K. The weak temperature-dependent evolution strongly deviates from the expectations of an itinerant Stoner mechanism. Our results suggest that itinerant electrons have minimal contributions to the enhancement of T$_C$ in Fe$_3$GaTe$_2$ compared to Fe$_3$GeTe$_2$, and that the nature of ferromagnetism in these Fe-based vdW ferromagnets must be understood with considerations of the electron correlations. △ Less

Submitted 2 December, 2023; v1 submitted 1 July, 2023; originally announced July 2023.

Journal ref: Physical Review B 109, 104410 (2024)

Direct visualization of the charge transfer in Graphene/$α$-RuCl$_3$ heterostructure

Authors: Antonio Rossi, Riccardo Dettori, Cameron Johnson, Jesse Balgley, John C. Thomas, Luca Francaviglia, Andreas K. Schmid, Kenji Watanabe, Takashi Taniguchi, Matthew Cothrine, David G. Mandrus, Chris Jozwiak, Aaron Bostwick, Erik A. Henriksen, Alexander Weber-Bargioni, Eli Rotenberg

Abstract: We investigate the electronic properties of a graphene and $α$-ruthenium trichloride (hereafter RuCl$_3$) heterostructure, using a combination of experimental and theoretical techniques. RuCl$_3$ is a Mott insulator and a Kitaev material, and its combination with graphene has gained increasing attention due to its potential applicability in novel electronic and optoelectronic devices. By using a c… ▽ More We investigate the electronic properties of a graphene and $α$-ruthenium trichloride (hereafter RuCl$_3$) heterostructure, using a combination of experimental and theoretical techniques. RuCl$_3$ is a Mott insulator and a Kitaev material, and its combination with graphene has gained increasing attention due to its potential applicability in novel electronic and optoelectronic devices. By using a combination of spatially resolved photoemission spectroscopy, low energy electron microscopy, and density functional theory (DFT) calculations we are able to provide a first direct visualization of the massive charge transfer from graphene to RuCl$_3$, which can modify the electronic properties of both materials, leading to novel electronic phenomena at their interface. The electronic band structure is compared to DFT calculations that confirm the occurrence of a Mott transition for RuCl$_3$. Finally, a measurement of spatially resolved work function allows for a direct estimate of the interface dipole between graphene and RuCl$_3$. The strong coupling between graphene and RuCl$_3$ could lead to new ways of manipulating electronic properties of two-dimensional lateral heterojunction. Understanding the electronic properties of this structure is pivotal for designing next generation low-power opto-electronics devices. △ Less

Submitted 29 May, 2023; v1 submitted 26 May, 2023; originally announced May 2023.

Comparative Electronic Structures of the Chiral Helimagnets Cr1/3NbS2 and Cr1/3TaS2

Authors: Lilia S. Xie, Oscar Gonzalez, Kejun Li, Matteo Michiardi, Sergey Gorovikov, Sae Hee Ryu, Shannon S. Fender, Marta Zonno, Na Hyun Jo, Sergey Zhdanovich, Chris Jozwiak, Aaron Bostwick, Samra Husremovic, Matthew P. Erodici, Cameron Mollazadeh, Andrea Damascelli, Eli Rotenberg, Yuan Ping, D. Kwabena Bediako

Abstract: Magnetic materials with noncollinear spin textures are promising for spintronic applications. To realize practical devices, control over the length and energy scales of such spin textures is imperative. The chiral helimagnets Cr1/3NbS2 and Cr1/3TaS2 exhibit analogous magnetic phase diagrams with different real-space periodicities and field dependence, positioning them as model systems for studying… ▽ More Magnetic materials with noncollinear spin textures are promising for spintronic applications. To realize practical devices, control over the length and energy scales of such spin textures is imperative. The chiral helimagnets Cr1/3NbS2 and Cr1/3TaS2 exhibit analogous magnetic phase diagrams with different real-space periodicities and field dependence, positioning them as model systems for studying the relative strengths of the microscopic mechanisms giving rise to exotic spin textures. Here, we carry out a comparative study of the electronic structures of Cr1/3NbS2 and Cr1/3TaS2 using angle-resolved photoemission spectroscopy and density functional theory. We show that bands in Cr1/3TaS2 are more dispersive than their counterparts in Cr1/3NbS2 and connect this result to bonding and orbital overlap in these materials. We also unambiguously distinguish exchange splitting from surface termination effects by studying the dependence of their photoemission spectra on polarization, temperature, and beam size. We find strong evidence that hybridization between intercalant and host lattice electronic states mediates the magnetic exchange interactions in these materials, suggesting that band engineering is a route toward tuning their spin textures. Overall, these results underscore how the modular nature of intercalated transition metal dichalcogenides translates variation in composition and electronic structure to complex magnetism. △ Less

Submitted 22 May, 2023; v1 submitted 15 May, 2023; originally announced May 2023.

Comments: 46 pages, 18 figures, 5 tables

Journal ref: Chemistry of Materials, 2023, 35, 7239-7251

Nature of charge density wave in kagome metal ScV6Sn6

Authors: Seongyong Lee, Choongjae Won, Jimin Kim, Jonggyu Yoo, Sudong Park, Jonathan Denlinger, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, Riccardo Comin, Mingu Kang, Jae-Hoon Park

Abstract: Kagome lattice materials offer a fertile ground to discover novel quantum phases of matter, ranging from unconventional superconductivity and quantum spin liquids to charge orders of various profiles. However, understanding the genuine origin of the quantum phases in kagome materials is often challenging, owing to the intertwined atomic, electronic, and structural degrees of freedom. Here, we comb… ▽ More Kagome lattice materials offer a fertile ground to discover novel quantum phases of matter, ranging from unconventional superconductivity and quantum spin liquids to charge orders of various profiles. However, understanding the genuine origin of the quantum phases in kagome materials is often challenging, owing to the intertwined atomic, electronic, and structural degrees of freedom. Here, we combine angle-resolved photoemission spectroscopy, phonon mode calculation, and chemical doping to elucidate the driving mechanism of the root3*root3 charge order in a newly discovered kagome metal ScV6Sn6. In contrast to the case of the archetype kagome system AV3Sb5 (A= K, Rb, Cs), the van Hove singularities in ScV6Sn6 remain intact across the charge order transition, indicating a marginal role of the electronic instability from the V kagome lattice. Instead, we identified a three-dimensional band with dominant planar Sn character opening a large charge order gap of 260 meV and strongly reconstructing the Fermi surface. Our complementary phonon dispersion calculations further emphasize the role of the structural components other than the V kagome lattice by revealing the unstable planar Sn and Sc phonon modes associated to the root3*root3 phase. Finally, in the constructed phase diagram of Sc(V1-xCrx)6Sn6, the charge order remains robust in a wide doping range x = 0 ~ 0.10 against the Fermi level shift up to ~ 120 meV, further making the electronic scenarios such as Fermi surface or saddle point nesting unlikely. Our multimodal investigations demonstrate that the physics of ScV6Sn6 is fundamentally different from the canonical kagome metal AV3Sb5, uncovering a new mechanism to induce symmetry-breaking phase transition in kagome lattice materials. △ Less

Submitted 24 April, 2023; originally announced April 2023.

magnetoARPES: Angle Resolved Photoemission Spectroscopy with Magnetic Field Control

Authors: Sae Hee Ryu, Garett Reichenbach, Chris M. Jozwiak, Aaron Bostwick, Peter Richter, Thomas Seyller, Eli Rotenberg

Abstract: Angle-Resolved Photoemission Spectroscopy (ARPES) is a premier technique for understanding the electronic excitations in conductive, crystalline matter, in which the induced photocurrent is collected and dispersed in energy and angle of emission to reveal the energy- and momentum-dependent single particle spectral function $A(\mathbf{k},ω)$. So far, ARPES in a magnetic field has been precluded due… ▽ More Angle-Resolved Photoemission Spectroscopy (ARPES) is a premier technique for understanding the electronic excitations in conductive, crystalline matter, in which the induced photocurrent is collected and dispersed in energy and angle of emission to reveal the energy- and momentum-dependent single particle spectral function $A(\mathbf{k},ω)$. So far, ARPES in a magnetic field has been precluded due to the need to preserve the electron paths between the sample and detector. In this paper we report progress towards "magnetoARPES", a variant of ARPES that can be conducted in a magnetic field. It is achieved by applying a microscopic probe beam ($\lesssim$ 10 $μ$m ) to a thinned sample mounted upon a special sample holder that generates magnetic field confined to a thin layer near the sample surface. In this geometry we could produce ARPES in magnetic fields up to around $\pm$ 100 mT. The magnetic fields can be varied from purely in-plane to nearly purely out-of-plane, by scanning the probe beam across different parts of the device. We present experimental and simulated data for graphene to explore the aberrations induced by the magnetic field. These results demonstrate the viability of the magnetoARPES technique for exploring symmetry breaking effects in weak magnetic fields. △ Less

Submitted 14 April, 2023; originally announced April 2023.

Comments: 21 pages, 6 figures

Strong Inter-valley Electron-Phonon Coupling in Magic-Angle Twisted Bilayer Graphene

Authors: Cheng Chen, Kevin P. Nuckolls, Shuhan Ding, Wangqian Miao, Dillon Wong, Myungchul Oh, Ryan L. Lee, Shanmei He, Cheng Peng, Ding Pei, Yiwei Li, Chenyue Hao, Haoran Yan, Hanbo Xiao, Han Gao, Qiao Li, Shihao Zhang, Jianpeng Liu, Lin He, Kenji Watanabe, Takashi Taniguchi, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, Chu Li , et al. (9 additional authors not shown)

Abstract: The unusual properties of superconductivity in magic-angle twisted bilayer graphene (MATBG) have sparked enormous research interest. However, despite the dedication of intensive experimental efforts and the proposal of several possible pairing mechanisms, the origin of its superconductivity remains elusive. Here, utilizing angle-resolved photoemission spectroscopy with micrometer spatial resolutio… ▽ More The unusual properties of superconductivity in magic-angle twisted bilayer graphene (MATBG) have sparked enormous research interest. However, despite the dedication of intensive experimental efforts and the proposal of several possible pairing mechanisms, the origin of its superconductivity remains elusive. Here, utilizing angle-resolved photoemission spectroscopy with micrometer spatial resolution, we have revealed flat band replicas in superconducting MATBG, where MATBG is unaligned with its hexagonal boron nitride (hBN) substrate11. These replicas exhibit uniform energy spacing, approximately 150 +- 15 meV apart, indicative of strong electron-boson coupling. Strikingly, these replicas are absent in non-superconducting twisted bilayer graphene (TBG) systems, either when MATBG is aligned to hBN or when TBG deviates from the magic angle. Calculations suggest that the formation of these flat band replicas in superconducting MATBG are attributed to the strong coupling between flat band electrons and an optical phonon mode at the graphene K point, facilitated by inter-valley scattering. These findings, although do not necessarily put electron phonon coupling as the main driving force for the superconductivity in MATBG, unravel the unique electronic structure inherent in superconducting MATBG, thereby providing crucial information for understanding the unusual electronic landscape from which the superconductivity is derived. △ Less

Submitted 12 December, 2024; v1 submitted 26 March, 2023; originally announced March 2023.

Comments: 17 pages, 4 figures

Journal ref: Nature 636, 342 (2024)

On the effects of strain, defects, and interactions on the topological properties of HfTe5

Authors: Na Hyun Jo, Omar A. Ashour, Zhixue Shu, Chris Jozwiak, Aaron Bostwick, Sae Hee Ryu, Kai Sun, Tai Kong, Sinead M. Griffin, Eli Rotenberg

Abstract: Topological insulators are characterized by spin-momentum-locked massless surface states which are robust under various perturbations. Manipulating such surface states is a topic of vigorous research, as a possible route for the realization of emergent many-body physics in topological systems. Thus far, time-reversal symmetry breaking via Coulomb and magnetic perturbations has been a dominant appr… ▽ More Topological insulators are characterized by spin-momentum-locked massless surface states which are robust under various perturbations. Manipulating such surface states is a topic of vigorous research, as a possible route for the realization of emergent many-body physics in topological systems. Thus far, time-reversal symmetry breaking via Coulomb and magnetic perturbations has been a dominant approach for the tuning of topological states. However, the effect of the structural degrees of freedom on quasi-particle dynamics in topological materials remains elusive. In this work, we demonstrate a transition in HfTe5 between distinct topological phases as a function of either Te vacancy concentration or applied strain; these phases are characterized theoretically as a transition from strong to weak topological insulator and experimentally by a transition from sharp surface states and Dirac crossing to a Fermi-liquid-like quasiparticle state in which these surface-localized features are heavily suppressed. Although vacancies can result in various consequences such as scattering, doping, and structural distortions, we show that changes in the lattice constants play the foremost role in determining the electronic structure, self-energy, and topological states of HfTe5. Our results demonstrate the possibility of using both defect chemistry and strain as control parameters for topological phase transitions and associated many-body physics. △ Less

Submitted 19 March, 2023; originally announced March 2023.

Journal ref: Phys. Rev. B 109, 235122 (2024)

Small Fermi pockets intertwined with charge stripes and pair density wave order in a kagome superconductor

Authors: Hong Li, Dongjin Oh, Mingu Kang, He Zhao, Brenden R Ortiz, Yuzki Oey, Shiang Fang, Zheng Ren, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, Joseph G. Checkelsky, Ziqiang Wang, Stephen D. Wilson, Riccardo Comin, Ilija Zeljkovic

Abstract: The kagome superconductor family AV3Sb5 (A=Cs, K, Rb) emerged as an exciting platform to study exotic Fermi surface instabilities. Here we use spectroscopic-imaging scanning tunneling microscopy (SI-STM) and angle-resolved photoemission spectroscopy (ARPES) to reveal how the surprising cascade of higher and lower-dimensional density waves in CsV3Sb5 is intimately tied to a set of small reconstruct… ▽ More The kagome superconductor family AV3Sb5 (A=Cs, K, Rb) emerged as an exciting platform to study exotic Fermi surface instabilities. Here we use spectroscopic-imaging scanning tunneling microscopy (SI-STM) and angle-resolved photoemission spectroscopy (ARPES) to reveal how the surprising cascade of higher and lower-dimensional density waves in CsV3Sb5 is intimately tied to a set of small reconstructed Fermi pockets. ARPES measurements visualize the formation of these pockets generated by a 3D charge density wave transition. The pockets are connected by dispersive q* wave vectors observed in Fourier transforms of STM differential conductance maps. As the additional 1D charge order emerges at a lower temperature, q* wave vectors become substantially renormalized, signaling further reconstruction of the Fermi pockets. Remarkably, in the superconducting state, the superconducting gap modulations give rise to an in-plane Cooper pair-density-wave at the same q* wave vectors. Our work demonstrates the intrinsic origin of the charge-stripes and the pair-density-wave in CsV3Sb5 and their relationship to the Fermi pockets. These experiments uncover a unique scenario of how Fermi pockets generated by a parent charge density wave state can provide a favorable platform for the emergence of additional density waves. △ Less

Submitted 13 March, 2023; originally announced March 2023.

Journal ref: Phys. Rev. X 13, 031030 (2023)

Synthesis and physical properties of a new layered ferromagnet, Cr1.21Te2

Authors: Zhixue Shu, Haozhe Wang, Na Hyun Jo, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, Weiwei Xie, Tai Kong

Abstract: Single crystals of a new layered compound, Cr1.21Te2, was synthesized via a vapor transport method. The crystal structure and physical properties were characterized by single crystal and powder x-ray diffraction, temperature- and field-dependent magnetization, zero-field heat capacity and angle-resolved photoemission spectroscopy. Cr1.21Te2, containing two Cr sites, crystalizes in a trigonal struc… ▽ More Single crystals of a new layered compound, Cr1.21Te2, was synthesized via a vapor transport method. The crystal structure and physical properties were characterized by single crystal and powder x-ray diffraction, temperature- and field-dependent magnetization, zero-field heat capacity and angle-resolved photoemission spectroscopy. Cr1.21Te2, containing two Cr sites, crystalizes in a trigonal structure with a space group P-3 (No. 147). The Cr site in the interstitial layer is partially occupied. Physical property characterizations indicate that Cr1.21Te2 is metallic with hole pockets at the Fermi energy and undergoes a ferromagnetic phase transition at ~173 K. The magnetic moments align along the c-axis in the ferromagnetic state. Based on low temperature magnetization, the spin stiffness constant D and spin excitation gap $Δ$ were estimated according to Bloch's law to be D = 99 $\pm$ 24 meV $Å^2$ and $Δ$ = 0.46 $\pm$ 0.33 meV, suggesting its possible application as a low dimensional ferromagnet. △ Less

Submitted 1 March, 2023; originally announced March 2023.

Comments: 6 figures

Journal ref: Phys. Rev. M 7, 044406 (2023)

Ideal Weak Topological Insulator and Protected Helical Saddle Points

Authors: Ji Seop Oh, Tianyi Xu, Nikhil Dhale, Sheng Li, Chao Lei, Chiho Yoon, Wenhao Liu, Jianwei Huang, Hanlin Wu, Makoto Hashimoto, Donghui Lu, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, Chun Ning Lau, Bing Lv, Fan Zhang, Robert Birgeneau, Ming Yi

Abstract: The paradigm of classifying three-dimensional (3D) topological insulators into strong and weak ones (STI and WTI) opens the door for the discovery of various topological phases of matter protected by different symmetries and defined in different dimensions. However, in contrast to the vast realization of STIs, very few materials have been experimentally identified as being close to WTI. Even among… ▽ More The paradigm of classifying three-dimensional (3D) topological insulators into strong and weak ones (STI and WTI) opens the door for the discovery of various topological phases of matter protected by different symmetries and defined in different dimensions. However, in contrast to the vast realization of STIs, very few materials have been experimentally identified as being close to WTI. Even amongst those identified, none exists with topological surface states (TSS) exposed in a global bulk band gap that is stable at all temperatures. Here we report the design and observation of an ideal WTI in a quasi-one-dimensional (quasi-1D) bismuth halide, Bi$_{4}$I$_{1.2}$Br$_{2.8}$ (BIB). Via angle-resolved photoemission spectroscopy (ARPES), we identify that BIB hosts TSS on the (100)$\prime$ side surface in the form of two anisotropic $π$-offset Dirac cones (DCs) separated in momentum while topologically dark on the (001) top surface. The ARPES data fully determine a unique side-surface Hamiltonian and thereby identify two pairs of non-degenerate helical saddle points and a series of four Lifshitz transitions. The fact that both the surface Dirac and saddle points are in the global bulk band gap of 195 meV, combined with the small Dirac velocities, nontrivial spin texture, and the near-gap chemical potential, qualifies BIB to be not only an ideal WTI but also a fertile ground for topological many-body physics. △ Less

Submitted 30 January, 2023; v1 submitted 29 January, 2023; originally announced January 2023.

Graphene-driven correlated electronic states in one dimensional defects within WS$_2$

Authors: Antonio Rossi, John C. Thomas, Johannes T. Küchle, Elyse Barré, Zhuohang Yu, Da Zhou, Shalini Kumari, Hsin-Zon Tsai, Ed Wong, Chris Jozwiak, Aaron Bostwick, Joshua A. Robinson, Mauricio Terrones, Archana Raja, Adam Schwartzberg, D. Frank Ogletree, Jeffrey B. Neaton, Michael F. Crommie, Francesco Allegretti, Willi Auwärter, Eli Rotenberg, Alexander Weber-Bargioni

Abstract: Tomonaga-Luttinger liquid (TLL) behavior in one-dimensional systems has been predicted and shown to occur at semiconductor-to-metal transitions within two-dimensional materials. Reports of one-dimensional defects hosting a Fermi liquid or a TLL have suggested a dependence on the underlying substrate, however, unveiling the physical details of electronic contributions from the substrate require cro… ▽ More Tomonaga-Luttinger liquid (TLL) behavior in one-dimensional systems has been predicted and shown to occur at semiconductor-to-metal transitions within two-dimensional materials. Reports of one-dimensional defects hosting a Fermi liquid or a TLL have suggested a dependence on the underlying substrate, however, unveiling the physical details of electronic contributions from the substrate require cross-correlative investigation. Here, we study TLL formation within defectively engineered WS$_2$ atop graphene, where band structure and the atomic environment is visualized with nano angle-resolved photoelectron spectroscopy, scanning tunneling microscopy and spectroscopy, and non-contact atomic force microscopy. Correlations between the local density of states and electronic band dispersion elucidated the electron transfer from graphene into a TLL hosted by one-dimensional metal (1DM) defects. It appears that the vertical heterostructure with graphene and the induced charge transfer from graphene into the 1DM is critical for the formation of a TLL. △ Less

Submitted 7 July, 2025; v1 submitted 6 January, 2023; originally announced January 2023.

Journal ref: Nature Communications, v. 16, n. 5809, July 2025

Nanoscale view of engineered massive Dirac quasiparticles in lithographic superstructures

Authors: Alfred J. H. Jones, Lene Gammelgaard, Mikkel O. Sauer, Deepnarayan Biswas, Roland J. Koch, Chris Jozwiak, Eli Rotenberg, Aaron Bostwick, Kenji Watanabe, Takashi Taniguchi, Cory R. Dean, Antti-Pekka Jauho, Peter Bøggild, Thomas G. Pedersen, Bjarke S. Jessen, Søren Ulstrup

Abstract: Massive Dirac fermions are low-energy electronic excitations characterized by a hyperbolic band dispersion. They play a central role in several emerging physical phenomena such as topological phase transitions, anomalous Hall effects and superconductivity. This work demonstrates that massive Dirac fermions can be controllably induced by lithographically patterning superstructures of nanoscale hole… ▽ More Massive Dirac fermions are low-energy electronic excitations characterized by a hyperbolic band dispersion. They play a central role in several emerging physical phenomena such as topological phase transitions, anomalous Hall effects and superconductivity. This work demonstrates that massive Dirac fermions can be controllably induced by lithographically patterning superstructures of nanoscale holes in a graphene device. Their band dispersion is systematically visualized using angle-resolved photoemission spectroscopy with nanoscale spatial resolution. A linear scaling of effective mass with feature sizes is discovered, underlining the Dirac nature of the superstructures. In situ electrostatic doping dramatically enhances the effective hole mass and leads to the direct observation of an electronic band gap that results in a peak-to-peak band separation of (0.64 $\pm$ 0.03) eV, which is shown via first-principles calculations to be strongly renormalized by carrier-induced screening. The presented methodology outlines a new approach for band structure engineering guided by directly viewing structurally- and electrically-tunable massive Dirac quasiparticles in lithographic superstructures at the nanoscale. △ Less

Submitted 17 December, 2022; originally announced December 2022.

Comments: 37 pages, 12 figures (includes supporting information). A revised version has been published in ACS Nano

Journal ref: ACS Nano 2022, 16, 11, 19354-19362

Topological band inversion in HgTe(001): surface and bulk signatures from photoemission

Authors: Raphael C. Vidal, Giovanni Marini, Lukas Lunczer, Simon Moser, Lena Fürst, Chris Jozwiak, Aaron Bostwick, Eli Rotenberg, Charles Gould, Hartmut Buhmann, Wouter Beugeling, Giorgio Sangiovanni, Domenico Di Sante, Gianni Profeta, Laurens W. Molenkamp, Hendrik Bentmann, Friedrich Reinert

Abstract: HgTe is a versatile topological material and has enabled the realization of a variety of topological states, including two- and three-dimensional (3D) topological insulators and topological semimetals. Nevertheless, a quantitative understanding of its electronic structure remains challenging, in particular due to coupling of the Te 5p-derived valence electrons to Hg 5d core states at shallow bindi… ▽ More HgTe is a versatile topological material and has enabled the realization of a variety of topological states, including two- and three-dimensional (3D) topological insulators and topological semimetals. Nevertheless, a quantitative understanding of its electronic structure remains challenging, in particular due to coupling of the Te 5p-derived valence electrons to Hg 5d core states at shallow binding energy. We present a joint experimental and theoretical study of the electronic structure in strained HgTe(001) films in the 3D topological-insulator regime, based on angle-resolved photoelectron spectroscopy and density functional theory. The results establish detailed agreement in terms of (i) electronic band dispersions and orbital symmetries, (ii) surface and bulk contributions to the electronic structure, and (iii) the importance of Hg 5d states in the valence-band formation. Supported by theory, our experiments directly image the paradigmatic band inversion in HgTe, underlying its non-trivial band topology. △ Less

Submitted 11 December, 2022; originally announced December 2022.

Antiferromagnetic metal phase in an electron-doped rare-earth nickelate

Authors: Qi Song, Spencer Doyle, Grace A. Pan, Ismail El Baggari, Dan Ferenc Segedin, Denisse Cordova Carrizales, Johanna Nordlander, Christian Tzschaschel, James R. Ehrets, Zubia Hasan, Hesham El-Sherif, Jyoti Krishna, Chase Hanson, Harrison LaBollita, Aaron Bostwick, Chris Jozwiak, Eli Rotenberg, Su-Yang Xu, Alessandra Lanzara, Alpha T. N'Diaye, Colin A. Heikes, Yaohua Liu, Hanjong Paik, Charles M. Brooks, Betul Pamuk , et al. (6 additional authors not shown)

Abstract: Long viewed as passive elements, antiferromagnetic materials have emerged as promising candidates for spintronic devices due to their insensitivity to external fields and potential for high-speed switching. Recent work exploiting spin and orbital effects has identified ways to electrically control and probe the spins in metallic antiferromagnets, especially in noncollinear or noncentrosymmetric sp… ▽ More Long viewed as passive elements, antiferromagnetic materials have emerged as promising candidates for spintronic devices due to their insensitivity to external fields and potential for high-speed switching. Recent work exploiting spin and orbital effects has identified ways to electrically control and probe the spins in metallic antiferromagnets, especially in noncollinear or noncentrosymmetric spin structures. The rare earth nickelate NdNiO3 is known to be a noncollinear antiferromagnet where the onset of antiferromagnetic ordering is concomitant with a transition to an insulating state. Here, we find that for low electron doping, the magnetic order on the nickel site is preserved while electronically a new metallic phase is induced. We show that this metallic phase has a Fermi surface that is mostly gapped by an electronic reconstruction driven by the bond disproportionation. Furthermore, we demonstrate the ability to write to and read from the spin structure via a large zero-field planar Hall effect. Our results expand the already rich phase diagram of the rare-earth nickelates and may enable spintronics applications in this family of correlated oxides. △ Less

Submitted 14 November, 2022; originally announced November 2022.

Comments: 25 pages, 4 figures

Electronic band structure changes across the antiferromagnetic phase transition of exfoliated MnPS$_3$ probed by $μ$-ARPES

Authors: Jeff Strasdas, Benjamin Pestka, Milosz Rybak, Adam K. Budniak, Niklas Leuth, Honey Boban, Vitaliy Feyer, Iulia Cojocariu, Daniel Baranowski, José Avila, Pavel Dudin, Aaron Bostwick, Chris Jozwiak, Eli Rotenberg, Carmine Autieri, Yaron Amouyal, Lukasz Plucinski, Efrat Lifshitz, Magdalena Birowska, Markus Morgenstern

Abstract: Exfoliated magnetic 2D materials enable versatile tuning of magnetization, e.g., by gating or providing proximity-induced exchange interaction. However, their electronic band structure after exfoliation has not been probed, most likely due to their photochemical sensitivity. Here, we provide micron-scale angle-resolved photoelectron spectroscopy of the exfoliated intralayer antiferromagnet MnPS… ▽ More Exfoliated magnetic 2D materials enable versatile tuning of magnetization, e.g., by gating or providing proximity-induced exchange interaction. However, their electronic band structure after exfoliation has not been probed, most likely due to their photochemical sensitivity. Here, we provide micron-scale angle-resolved photoelectron spectroscopy of the exfoliated intralayer antiferromagnet MnPS$_3$ above and below the Néel temperature down to one monolayer. The favorable comparison with density functional theory calculations enables to identify the orbital character of the observed bands. Consistently, we find pronounced changes across the Néel temperature for bands that consist of Mn 3d and 3p levels of adjacent S atoms. The deduced orbital mixture indicates that the superexchange is relevant for the magnetic interaction. There are only minor changes between monolayer and thicker films demonstrating the predominant 2D character of MnPS$_3$. The novel access is transferable to other MPX$_3$ materials (M: transition metal, P: phosphorus, X: chalcogenide) providing a multitude of antiferromagnetic arrangements. △ Less

Submitted 22 June, 2023; v1 submitted 10 November, 2022; originally announced November 2022.

Comments: 26 pages, 17 figures

ACM Class: J.2

Journal ref: Nano Lett. 2023, 23, 22, 10342-10349