-
Oxygen stoichiometry directs rutile-anatase phase selection through kinetic control of nucleation
Authors:
Han Uk Lee,
Hyeon Woo Kim,
Ji Min Kim,
Dong Won Jeon,
Rohan Mishra,
Sung Beom Cho
Abstract:
Synthesis of a target polymorph remains more empirical than predictive because crystallization often selects the most accessible nucleation pathway rather than the thermodynamically most stable phase. Here, we show that oxygen stoichiometry converts this empirical synthesis variable into a kinetic control parameter for anatase-rutile selection in TiO$_{2-x}$. Enhanced-sampling simulations reveal t…
▽ More
Synthesis of a target polymorph remains more empirical than predictive because crystallization often selects the most accessible nucleation pathway rather than the thermodynamically most stable phase. Here, we show that oxygen stoichiometry converts this empirical synthesis variable into a kinetic control parameter for anatase-rutile selection in TiO$_{2-x}$. Enhanced-sampling simulations reveal that oxygen content alters the nucleation-barrier landscape, switching the relative accessibility of anatase and rutile, even while rutile remains thermodynamically favored. Molecular dynamics simulations show the presence of a diffuse intermediate shell around the nucleus, where oxygen deficiency alters Ti-O coordination and connectivity and drives shell-local motif evolution from anatase-like toward rutile-like environments. A coupled-flux model that integrates barrier competition with shell-mediated attachment/exchange yields a relative nucleation-rate map consistent with reported oxygen-dependent synthesis trends. These results establish stoichiometry-controlled intermediate-shell motif evolution as a kinetic origin of polymorph selection and provide a framework for predicting target phases in composition-coupled crystallization.
△ Less
Submitted 23 August, 2026;
originally announced August 2026.
-
Physics-guided machine learning for sim-to-real calibration of NV diamond magnetometers
Authors:
Jonathan Daniel,
Martin Y. Kim,
Jesse Hernandez,
Emanuel Suarez,
Sangwoo Lee,
Jinhee Lee,
Je-Hyung Kim
Abstract:
Ensemble nitrogen-vacancy (NV) centers in diamond enable robust vector magnetometry in unshielded environments, yet deployment remains bottlenecked by complex calibration and a reliance on external data references. Conventional statistical machine learning requires an exorbitantly large volume of training data and suffers from severe simulation-to-reality mismatches. To address this, we introduce…
▽ More
Ensemble nitrogen-vacancy (NV) centers in diamond enable robust vector magnetometry in unshielded environments, yet deployment remains bottlenecked by complex calibration and a reliance on external data references. Conventional statistical machine learning requires an exorbitantly large volume of training data and suffers from severe simulation-to-reality mismatches. To address this, we introduce a physics-guided hybrid machine learning framework that embeds the Zeeman splitting directly into the learning pipeline. Our physics-guided model significantly reduces the average tracking error demonstrating a 372-fold precision improvement over purely statistical baselines. Furthermore, our hybrid architecture pairs a sparse physical measurement with scalable synthetic data generation, seamlessly incorporating real-world hardware non-idealities. When deployed to decode uncalibrated, raw experimental ODMR data, our framework delivers exceptional predictive accuracy for the scalar magnetic field. This work paves the way toward self-calibrated sensors while establishing a machine learning training method applicable to other data-scarce physical systems
△ Less
Submitted 19 August, 2026;
originally announced August 2026.
-
Antiferromagnetic order and lattice response in DyCuAs$_2$
Authors:
M. G. Kim,
J. -W. Kim,
P. Ryan,
D. Evans,
E. D. Mun
Abstract:
We report high-resolution synchrotron X-ray diffraction and X-ray resonant magnetic scattering (XRMS) studies of the low-temperature crystal and magnetic structures of DyCuAs$_2$, a member of the \RE{}CuAs$_2$ family exhibiting a resistivity minimum above the antiferromagnetic transition temperature. Synchrotron diffraction measurements reveal that DyCuAs$_2$ preserves tetragonal symmetry down to…
▽ More
We report high-resolution synchrotron X-ray diffraction and X-ray resonant magnetic scattering (XRMS) studies of the low-temperature crystal and magnetic structures of DyCuAs$_2$, a member of the \RE{}CuAs$_2$ family exhibiting a resistivity minimum above the antiferromagnetic transition temperature. Synchrotron diffraction measurements reveal that DyCuAs$_2$ preserves tetragonal symmetry down to low temperature within the experimental resolution, although pronounced anomalies in both lattice parameters $a$ and $c$ are observed near the antiferromagnetic transition temperature, $T_{\mathrm N}\approx7$~K, indicating strong magnetoelastic coupling. XRMS measurements at the Dy $L_3$ edge establish commensurate antiferromagnetic ordering below $T_{\mathrm N}$ with AFM Bragg peaks at \qq{} = (0, 0, 0.5). Representation analysis and calculations of the AFM Bragg peak intensities identify the magnetic structure as the $Γ_{10}$ representation, consisting of in-plane Dy moments stacked along the \cc{} axis in a $++--$ sequence. The magnetic structure is therefore identical to that previously reported for SmCuAs$_2$. Comparison among DyCuAs$_2$, SmCuAs$_2$, and GdCuAs$_2$ suggests that in-plane AFM order and the associated magnetic frustration on the tetragonal lattice are closely connected to the emergence of the resistivity minimum in the \RE{}CuAs$_2$ family. At the same time, the enhanced lattice response and stronger magnetic-field sensitivity observed in DyCuAs$_2$ imply that magnetoelastic and spin-orbit interactions additionally play important roles in determining the robustness of this anomalous transport behavior.
△ Less
Submitted 19 August, 2026;
originally announced August 2026.
-
Fresnel diffraction imaging of surface nanostructure using coherent resonant X-ray scattering
Authors:
L. Burgard,
C. Neupane,
A. Balodhi,
S. Bista,
S. Butun,
R. Jangid,
A. Barbour,
N. Basit,
D. F. Agterberg,
M. Weinert,
C. Mazzoli,
M. G. Kim
Abstract:
We investigated surface nanostructures on an antiferromagnet MnBi$_2$Te$_4$ using a novel imaging technique, direct (real)-space and real time coherent X-ray imaging (direct-CXI). This technique has provided new insights into antiferromagnetic textures, including the formation of anti-phase antiferromagnetic (AFM) domains and thermal dynamics of AFM domains and domain walls. While this method prod…
▽ More
We investigated surface nanostructures on an antiferromagnet MnBi$_2$Te$_4$ using a novel imaging technique, direct (real)-space and real time coherent X-ray imaging (direct-CXI). This technique has provided new insights into antiferromagnetic textures, including the formation of anti-phase antiferromagnetic (AFM) domains and thermal dynamics of AFM domains and domain walls. While this method produces real-space images of AFM textures without requiring a complex imaging retrieval process, its underlying imaging mechanism has not been fully understood, limiting a deep understanding of AFM textures and the information they contain. By investigating the well-defined structural characteristics of the nanostructures fabricated on MnBi$_2$Te$_4$, we elucidate the imaging principle of this novel technique. We find that the observed images can be well explained by Fresnel diffraction integral. Using a simple model from classical optics, our calculations successfully reproduce the experimentally observed images of the nanostructures. This demonstrates that direct-CXI not only provides straightforward real-space imaging but also contains phase information through its Fresnel diffraction integral.
△ Less
Submitted 18 August, 2026;
originally announced August 2026.
-
Low temperature magnetic structure and lattice response in SmCuAs$_2$
Authors:
M. G. Kim,
C. Neupane,
Y. Yu,
R. Acevedo-Esteves,
C. Nelson,
D. Evans,
E. D. Mun,
D. F. Agterberg,
J. -W. Kim
Abstract:
We investigated the structural and magnetic properties of single-crystalline SmCuAs$_2$ using high-resolution synchrotron X-ray diffraction and X-ray resonant magnetic scattering (XRMS) at the Sm $L_2$ and $L_3$ edges. Temperature-dependent diffraction measurements confirm that SmCuAs$_2$ maintains its tetragonal symmetry from room temperature down to 8 K, with lattice parameters showing anomalous…
▽ More
We investigated the structural and magnetic properties of single-crystalline SmCuAs$_2$ using high-resolution synchrotron X-ray diffraction and X-ray resonant magnetic scattering (XRMS) at the Sm $L_2$ and $L_3$ edges. Temperature-dependent diffraction measurements confirm that SmCuAs$_2$ maintains its tetragonal symmetry from room temperature down to 8 K, with lattice parameters showing anomalous behavior below the resistivity minimum ($T \approx$ 30 K). Notably, the \textbf{c}-axis lattice parameter exhibits a plateau and subsequent increase near the Néel temperature, indicating magnetoelastic coupling. XRMS measurements reveal a commensurate antiferromagnetic structure with a propagation vector \textbf{\textit{q}} = (0, 0, 0.5). Our measurement shows that the Sm moments are aligned within the \textbf{\textit{ab}} plane and arranged in a $++--$ stacking along the \textbf{\textit{c}}-axis. Comparison with related \textit{RE}CuAs$_2$ compounds (\textit{RE} = Pr, Nd, and Gd) suggests that in-plane moment orientation and associated magnetic frustration play a key role in the emergence of the resistivity minimum. Differences in spin-orbit and magnetoelastic coupling across the series highlight their importance in governing low-temperature transport behavior.
△ Less
Submitted 14 August, 2026;
originally announced August 2026.
-
Shape of Wigner Crystals and Hole Self-Doping in a Mexican-Hat Dispersion
Authors:
Minho Luke Kim,
Xiao-Gang Wen
Abstract:
We study Wigner crystals (WCs) induced by a strong Coulomb interaction from the ring-like Fermi surface of a Mexican-hat dispersion $ε_k= c_2k^2+c_4k^4$. We design orbital shape in order to minimize the energy of the WC, and find that a low ground-state energy requires an orbital shape with a depletion of electrons near $k=0$. To capture the Coulomb-induced correlations, we include a Jastrow facto…
▽ More
We study Wigner crystals (WCs) induced by a strong Coulomb interaction from the ring-like Fermi surface of a Mexican-hat dispersion $ε_k= c_2k^2+c_4k^4$. We design orbital shape in order to minimize the energy of the WC, and find that a low ground-state energy requires an orbital shape with a depletion of electrons near $k=0$. To capture the Coulomb-induced correlations, we include a Jastrow factor as well as a factor describing the correlation between electrons and doped vacancies. Using variational Monte Carlo calculations, we calibrate the effective band parameters $c_2$ and $c_4$ to reproduce the two transitions observed experimentally as the electron density is lowered: from a spin-valley-polarized Fermi liquid with a disk-like Fermi surface, to one with a ring-like Fermi surface, and finally to a WC. We find that, even with an optimized orbital shape that depletes electrons near $k=0$, a WC with hole self-doping near $k=0$ can still be energetically favorable near the WC transition, provided that the electron-vacancy correlation is included. We also estimate the dispersion of the doped hole.
△ Less
Submitted 31 July, 2026;
originally announced August 2026.
-
Unconventional and Fragile Magnetic Exciton in a van der Waals Quantum Magnet
Authors:
Kai-Xuan Zhang,
Min Zhang,
Minjae Kim,
Yong-Hyun Kim,
Junghyun Kim,
Heejun Yang,
Pyeongjae Park,
Chaebin Kim,
Mangesh Diware,
Junik Hwang,
Youjin Lee,
Byeong-Gwan Cho,
Hyeong-Do Kim,
Tae-Yeong Koo,
Chunhua Chen,
Mingtao Li,
Xujie Lü,
Wenge Yang,
Kee-Hoon Kim,
Seung-Ho Baek,
Hyeonsik Cheong,
Sung-Keun Lee,
Beom Hyun Kim,
Christopher Lane,
Jian-Xin Zhu
, et al. (3 additional authors not shown)
Abstract:
The recently discovered magnetic exciton in the van der Waals (vdW) antiferromagnet NiPS3 exemplifies these phenomena, exhibiting several distinctive characteristics. Despite extensive investigation, much of its physics remains unresolved, with key questions about why the NiPS3 magnetic exciton is so sharp and optically bright despite the nominally spin-forbidden transition, posing significant cha…
▽ More
The recently discovered magnetic exciton in the van der Waals (vdW) antiferromagnet NiPS3 exemplifies these phenomena, exhibiting several distinctive characteristics. Despite extensive investigation, much of its physics remains unresolved, with key questions about why the NiPS3 magnetic exciton is so sharp and optically bright despite the nominally spin-forbidden transition, posing significant challenges to a proper understanding and practical manipulation of the exciton. An urgent question is to what extent it is due to chemical disorder, magnetic weakening, lattice modification, or intrinsic instability of the bright exciton itself: answers to which will put stringent constraints on possible theoretical models. Here we address these questions using hydrostatic pressure as a clean, continuous, reversible, and in-situ tuning parameter. We find that the sharp photoluminescence peak is drastically suppressed by as little as 0.4 GPa and completely quenched by 1.5 GPa, with demonstrating its reversibility. Crucially, this bright-to-dark conversion occurs without magnetic, crystallographic, or electronic reconstruction despite an increase in the Neel temperature, as established by Raman, X-ray absorption, nuclear magnetic resonance spectroscopy, and first-principles many-body calculations. Our results demonstrate that the optical brightness of the magnetic exciton is independent of chemical disorder, lattice expansion, and weakening of magnetic order, indicating that a higher-order correlated mechanism governs the bright exciton. We further propose experimentally constrained microscopic scenarios involving exciton pairing, crystal-field-controlled spin-orbit mixing, and symmetry breaking, providing a framework for future tests of entangled magnetic exciton in correlated quantum magnets.
△ Less
Submitted 30 July, 2026;
originally announced July 2026.
-
Role of $p$-$d$ Hybridization on Optical Properties of Chalcopyrite Semiconductors
Authors:
Neunghee Han,
Harang Kim,
Minjae Kim,
Woonhyuk Baek
Abstract:
Designing quantum materials for coherent optical properties is a central agenda in quantum technology. Semiconductor quantum dots are an emerging approach for controlling coherent optical properties via confinement effects, tunable band gaps, and exciton binding energies, yet their inherent structural and compositional inhomogeneity degrades the coherence of the optical spectra, posing a major obs…
▽ More
Designing quantum materials for coherent optical properties is a central agenda in quantum technology. Semiconductor quantum dots are an emerging approach for controlling coherent optical properties via confinement effects, tunable band gaps, and exciton binding energies, yet their inherent structural and compositional inhomogeneity degrades the coherence of the optical spectra, posing a major obstacle. We show that, for chalcopyrite semiconductors, hybridization between transition-metal $d$ and ligand $p$ electrons in the valence band is key to the coherence of the quantum dot optical spectrum. We demonstrate this using first-principles electronic-structure calculations and optical spectroscopy. The strong $p$-$d$ hybridization in CuInS$_{2}$ induces the Cu($d$) Coulomb scattering channel, giving rise to the incoherent photodoped hole carrier, while the weak $p$-$d$ hybridization in AgInS$_{2}$ induces the delocalized photodoped hole carrier having a predominant S($p$) orbital character. Our experimental results on optical spectra suggest that when the Cu ratio is enhanced in the Ag$_{1-x}$Cu$_{x}$In$_{1-y}$Ga$_{y}$S$_{2}$ quantum dot, Cu atoms at both Ag sites and defect sites experience enhanced $p$-$d$ hybridization, and a coupling begins to develop between the electrons in the quantum dot and the defect electrons at a small Cu ratio. This coupling activates Cu($d$) Coulomb scattering for photodoped holes traversing the defect sites, producing an incoherent optical response that naturally explains the long-standing absence of band-edge spectral signatures in CuIn$_{1-y}$Ga$_y$S$_2$ quantum dots. These results serve as a guideline for designing semiconductor quantum dots. To achieve a coherent optical spectrum, avoid $p$-$d$-hybridized orbital character in the photo-doped carrier.
△ Less
Submitted 24 July, 2026;
originally announced July 2026.
-
Complete measurement of tunnel- and valley-coupling parameters in a silicon double quantum dot
Authors:
Daniel J. King,
Minyoung Kim,
J. Reily,
Jonathan C. Marcks,
Mark Friesen,
Benjamin D. Woods,
M. A. Eriksson
Abstract:
Tunneling is essential in the initialization, measurement, and control of quantum dot qubits. In silicon, such tunneling connects not only the qubit states but also valley minima in the conduction band on opposite sides of the Brillouin zone, with large consequences for the quantum dot behavior. Here we present a full characterization of the intravalley and intervalley tunnel couplings, including…
▽ More
Tunneling is essential in the initialization, measurement, and control of quantum dot qubits. In silicon, such tunneling connects not only the qubit states but also valley minima in the conduction band on opposite sides of the Brillouin zone, with large consequences for the quantum dot behavior. Here we present a full characterization of the intravalley and intervalley tunnel couplings, including their complex phases -- the valley phases. These phases are shown to control measurable parameters, including the ratios of the gaps at anticrossings between quantum states of a double quantum dot. The valley phases themselves evolve as a function of the quantum dot gate voltages and depend on the underlying atomic structure of the quantum well. Knowledge of the valley phases completes the picture and fills a key gap in our understanding of sample-wide variations of valley couplings and the physical parameters that depend on them, including spin-orbit coupling, valley-orbit mixing, and Landé $g$-factors.
△ Less
Submitted 22 July, 2026; v1 submitted 10 July, 2026;
originally announced July 2026.
-
Engineering Disordered Many-particle Plasmonic Nanoclusters for Wafer-scale Uniform and Giant Electromagnetic Field Enhancement
Authors:
Minjun Kim,
Vasanthan Devaraj,
Hyeon-Seok Seo,
Seongjae Eom,
Jeong-Su Lee,
Donghan Lee,
Min Yong Jeon,
Thomas Zentgraf,
Jong-Min Lee
Abstract:
Scalable plasmonic technologies face a critical trade-off: few-body architectures offer high enhancement but are sensitive to fabrication flaws, while scalable methods like solid-state dewetting yield large, low-enhancement gaps. We introduce a paradigm shift using a many-body plasmonic architecture inspired by statistical mechanics. By moving toward the continuum limit (N>>1), local geometric var…
▽ More
Scalable plasmonic technologies face a critical trade-off: few-body architectures offer high enhancement but are sensitive to fabrication flaws, while scalable methods like solid-state dewetting yield large, low-enhancement gaps. We introduce a paradigm shift using a many-body plasmonic architecture inspired by statistical mechanics. By moving toward the continuum limit (N>>1), local geometric variations are statistically averaged out, effectively decoupling optical performance from microscopic disorder. We implement this concept via a lithography- and etching-free, multi-step dewetting strategy, creating wafer-scale nanoclusters. This process strategically forms a robust many-body system by introducing numerous small satellite nanoparticles between larger particles. Crucially, this design achieves a high collective enhancement that surpasses even optimized few-body systems, despite having larger individual gaps. Under optimized conditions, these substrates exhibit a surface-enhanced Raman scattering enhancement factor approaching 4 x 108 with unprecedented reproducibility (RSD of ~10%). This scalable, low-cost concept establishes a practical route toward reproducible wafer-scale nanophotonic platforms for sensing, spectroscopy, and quantum technologies.
△ Less
Submitted 7 July, 2026;
originally announced July 2026.
-
Disentangling Haldane Phase by Generalized Clifford Circuits
Authors:
Minsoo Kim,
Changhun Oh,
Donghoon Kim
Abstract:
Disentangling transformations play a central role in the classical simulation of quantum many-body systems, yet their analytic structure and underlying mechanism remain largely unexplored. Here, we study the structure of the disentangler in the Haldane phase of spin-1 systems using generalized Clifford circuits. To this end, we extend the Clifford-circuit-augmented matrix product states (CAMPS)-ba…
▽ More
Disentangling transformations play a central role in the classical simulation of quantum many-body systems, yet their analytic structure and underlying mechanism remain largely unexplored. Here, we study the structure of the disentangler in the Haldane phase of spin-1 systems using generalized Clifford circuits. To this end, we extend the Clifford-circuit-augmented matrix product states (CAMPS)-based density-matrix renormalization group (DMRG) method to spin-1 systems. Within this framework, we find that the local disentanglers optimized for the Haldane phase implement the generalized Kramers--Wannier (KW) transformation, and we analytically verify its optimality for the Affleck--Kennedy--Lieb--Tasaki (AKLT) state. Beyond reducing entanglement, the KW transformation maps the Haldane phase to a phase with spontaneously broken $\mathbb{Z}_{2}$ symmetry. This mapping is distinct from the Kennedy--Tasaki transformation and provides a new unitary route from symmetry-protected topological order to symmetry breaking.
△ Less
Submitted 4 July, 2026;
originally announced July 2026.
-
Electrically tunable interfacial thermal conduction via electronic structure engineering in ${Au}$/$Bi_{1-x}$$Sb_{x}$ topological insulators
Authors:
Min Young Kim,
Joon Sang Kang,
Jangwoo Ha,
Hyungyu Jin,
Sandy A. Ekahana,
Pratik Saud,
Chris Jozwiak,
Eli Rotenberg,
Aaron Bostwick,
Jyoti Katoch,
Joseph P. Heremans
Abstract:
This work provides direct experimental evidence for the role of topological interface states in thermal conduction across a metal/topological insulator junction. It also shows that this conduction can be reversibly modulated by electrical current injection, offering a new approach toward active control of heat flow at solid-state interfaces. Specifically, the interfacial thermal conductance of…
▽ More
This work provides direct experimental evidence for the role of topological interface states in thermal conduction across a metal/topological insulator junction. It also shows that this conduction can be reversibly modulated by electrical current injection, offering a new approach toward active control of heat flow at solid-state interfaces. Specifically, the interfacial thermal conductance of ${Au}$/$Bi_{89}$$Sb_{11}$ and ${Au}$/$Bi_{87}$$Sb_{13}$ junctions demonstrates distinct temperature- and bias-dependent behavior. Both responses are attributed to carrier redistribution between topological interface and bulk band states, driven thermally by Fermi-Dirac broadening and electrically by quasi-Fermi-level shifts and WKB tunneling into nearby bulk bands. Control experiments using trivial semimetals and insulating interlayers further confirm the topological specificity of the effect. Such electrically tunable interfacial heat conduction positions interface electronic structure engineering as a promising route for active thermal management. In doing so, it lays the groundwork for a mechanically robust alternative to conventional structure-driven thermal control compatible with increasingly dense, high-power solid-state devices.
△ Less
Submitted 2 July, 2026;
originally announced July 2026.
-
Helicity-Resolved Spatiotemporal Mapping of Chiral Plexcitons in Helicoids
Authors:
Jeong Hyun Han,
Sankaran Ramesh,
Jaeyeon Jo,
Pavel Chabera,
Ryeong Myeong Kim,
Sung Hoon Cho,
In Han Ha,
Amitav Sahu,
Yoonsang Tak,
Jiawei Lv,
Miyoung Kim,
Ki Tae Nam,
Tönu Pullerits
Abstract:
Plasmon-exciton hybrids, or plexcitons, offer deeply subwavelength light-matter interactions with versatile pathways for energy redistribution. Incorporating chirality into such systems is particularly compelling, enabling spin-sensitive optical functionality that can operate on ultrafast timescales and within ultracompact volumes. Despite recent progress in chiral plexcitonic systems, how structu…
▽ More
Plasmon-exciton hybrids, or plexcitons, offer deeply subwavelength light-matter interactions with versatile pathways for energy redistribution. Incorporating chirality into such systems is particularly compelling, enabling spin-sensitive optical functionality that can operate on ultrafast timescales and within ultracompact volumes. Despite recent progress in chiral plexcitonic systems, how structural chirality and plasmon-exciton coupling determine chiroptical spectra and ultrafast energy flow remains elusive. Here we realize chiral plexcitons by functionalizing intrinsically chiral gold helicoid nanoparticles with molecular J-aggregates. Within a non-Hermitian framework, we trace the microscopic origin of the helicoid chiroptical response and its coupling to the excitonic transition, revealing how the helicity of light selectively addresses distinct hybrid responses. At the spatiotemporal extreme, we find that the gap-localized response not only enhances polarization-sensitive contrast but also strengthens the local hybrid interaction, leading to accelerated ultrafast relaxation. Together, these space-, time-, and polarization-resolved measurements provide a physically grounded and experimentally benchmarked picture of chiral plexcitonic coupling, identifying chirality as a practical control parameter for selectively steering nanoscale energy pathways and dynamics.
△ Less
Submitted 8 June, 2026;
originally announced June 2026.
-
Polymer-Regulated Freezing of Water Droplets Revealed by Synchrotron X-ray Imaging and Raman Spectroscopy
Authors:
Hyeonjun An,
Bomi Kim,
Jae Kwan Im,
Min Woo Kim,
Seob-Gu Kim,
Jae-Hong Lim,
Kitae Kim,
Joonwoo Jeong
Abstract:
Adding a polymer to a sessile water droplet not only lowers its freezing point but also suppresses the tip singularity that forms during its freezing on cold substrates. Here, we employ synchrotron X-ray and Raman imaging to elucidate the spatiotemporal mechanism underlying tip suppression in an aqueous polyvinyl alcohol (PVA) solution, a model polymer solution. As the polymer concentration increa…
▽ More
Adding a polymer to a sessile water droplet not only lowers its freezing point but also suppresses the tip singularity that forms during its freezing on cold substrates. Here, we employ synchrotron X-ray and Raman imaging to elucidate the spatiotemporal mechanism underlying tip suppression in an aqueous polyvinyl alcohol (PVA) solution, a model polymer solution. As the polymer concentration increases, we observe slower propagation of the freezing front, reduced bubble entrapment, and a progressively more rounded apex across the volumes and molecular weights examined. X-ray tomography reveals that frozen PVA droplets retain low X-ray transmittance domains in their interiors and at the surface, and Raman spectral mapping confirms that these domains correspond to PVA-enriched regions, providing direct evidence of freeze-induced polymer segregation. These findings indicate that PVA is redistributed heterogeneously during water solidification rather than shifting bulk properties homogeneously, providing a spatially resolved framework for interpreting the observed tip blunting and the suppression of discrete bubble entrapment. Our work identifies freeze-induced polymer segregation as a pathway by which a dissolved polymer regulates both the external shape and the internal structure of a freezing droplet, and these findings shed light on potential applications in freezing-based processes such as freeze-casting and cryopreservation.
△ Less
Submitted 31 May, 2026;
originally announced June 2026.
-
Autonomous scanning electrochemical cell microscopy enables rapid exploration of large compositionally complex material spaces
Authors:
Felix Thelen,
Moonjoo Kim,
Geovane Arruda de Oliveira,
Jan Lukas Buergel,
Wolfgang Schuhmann,
Alfred Ludwig
Abstract:
Alloying is a central strategy in electrocatalysis, enabling fine-tuning of electronic structure. In particular, compositionally complex solid solutions (CCSS) often called high-entropy alloys are of high interest as they allow active site design. However, the "combinatorial explosion" in the number of possible compositions poses a critical bottleneck for the discovery of active CCSS electrocataly…
▽ More
Alloying is a central strategy in electrocatalysis, enabling fine-tuning of electronic structure. In particular, compositionally complex solid solutions (CCSS) often called high-entropy alloys are of high interest as they allow active site design. However, the "combinatorial explosion" in the number of possible compositions poses a critical bottleneck for the discovery of active CCSS electrocatalysts. We present an autonomous scanning electrochemical cell microscopy (SECCM) system for ultrahigh-throughput and large-scale CCSS activity screening. The platform rapidly establishes composition-electrocatalytic activity relationships for large compositional spaces across multiple thin-film CCSS materials libraries via active learning and automated library exchange. Embedding analytical expressions of voltammetry in the algorithm enables the learning of whole voltammograms rather than a single selected metric. As a demonstration, we investigated hydrogen evolution reaction (HER) activities of Au-Ir-Rh, where Ir and Rh exhibit strong metal-hydrogen binding and Au exhibits relatively weak binding as derived from the HER volcano plot. The composition-activity trend was accurately predicted after measuring only 15% of all 966 measurement areas. Au30Ir20Rh50 and Au10Ir35Rh55 exhibit highest activities with standard rate constants of about 0.012 cm/s, demonstrating positive synergistic contributions from elemental mixing. The autonomous robotic SECCM platform is broadly applicable to a wide range of electrocatalytic reactions, providing a general pathway for accelerating CCSS electrocatalyst discovery and optimization.
△ Less
Submitted 30 May, 2026;
originally announced June 2026.
-
Non-local low energy neutral excitations in a strongly disordered triangular Mott magnet Cr$_3$Se$_2$Br$_5$
Authors:
Wenhao Liu,
Dechen Zhang,
Yuanqi Lyu,
Lebing Chen,
Lifang Hu,
Keith M. Teddei,
Yuting Zhang,
Steve Shelton,
Moon Kim,
Xiqu Wang,
Michael A. Susner,
James G. Analytis,
Dung-Hai Lee,
Lu Li,
Bing Lv,
Robert J. Birgeneau
Abstract:
Understanding if low-energy excitations can remain itinerant in the presence of strong disorder remains a central challenge in frustrated quantum magnets, where disorder is generally expected to localize excitations through Anderson-like mechanisms. Here we report the emergence of charge-neutral itinerant excitations in a van der Waals compound Cr$_3$Se$_2$Br$_5$, a strongly disordered $S = 3/2$ M…
▽ More
Understanding if low-energy excitations can remain itinerant in the presence of strong disorder remains a central challenge in frustrated quantum magnets, where disorder is generally expected to localize excitations through Anderson-like mechanisms. Here we report the emergence of charge-neutral itinerant excitations in a van der Waals compound Cr$_3$Se$_2$Br$_5$, a strongly disordered $S = 3/2$ Mott insulator with a frustrated triangular lattice. Structural analysis reveals substantial intrinsic disorder arising from Cr-site deficiency and Se/Br-site mixing, which appear to be fixed and cannot be readily tuned. No long-range magnetic order or conventional glassy behavior is observed. In addition to its highly insulating nature, the magnetic specific heat C_mag/T and thermal conductivity \k{appa}_xx/T both exhibit linear temperature dependencies with substantial finite intercepts. In particular, a sizeable field-independent residual term $κ/T \approx 0.03~\mathrm{W\,m^{-1}\,K^{-2}}$ is observed, providing compelling evidence of itinerant low-energy excitations that carry entropy without charge. These findings conceptually advance our understanding of quantum matter by demonstrating a rare regime where the interplay of disorder, frustration, and electronic correlations actively reshapes the nature of low-energy excitations, allowing itinerant neutral excitations to coexist with strong intrinsic disorder.
△ Less
Submitted 24 May, 2026;
originally announced May 2026.
-
High-fidelity EDSR in Si/SiGe Wiggle Wells
Authors:
Hudaiba Soomro,
Minyoung Kim,
Avani Vivrekar,
M. A. Eriksson,
Benjamin D. Woods,
Mark Friesen
Abstract:
Si/SiGe quantum wells that incorporate Ge concentration oscillations, known as long-period Wiggle Wells, have been shown to enhance the Dresselhaus spin-orbit coupling of conduction-band electrons. Such intrinsic spin-orbit coupling is desirable when performing spin-qubit gate operations based on electric dipole spin resonance (EDSR) because it eliminates the need for external micromagnets. Howeve…
▽ More
Si/SiGe quantum wells that incorporate Ge concentration oscillations, known as long-period Wiggle Wells, have been shown to enhance the Dresselhaus spin-orbit coupling of conduction-band electrons. Such intrinsic spin-orbit coupling is desirable when performing spin-qubit gate operations based on electric dipole spin resonance (EDSR) because it eliminates the need for external micromagnets. However, random-alloy disorder plays a key role in this materials system by spatially randomizing the valley splitting and the valley phase $φ_{s,s}$, and it has not been fully accounted for in recent EDSR analyses. Here, we show that alloy disorder affects EDSR in two main ways. First, the Rabi frequency $Ω$ acquires a dependence on the valley phase, given by $\cosφ_{s,s}$, which causes spatial randomization of $Ω$. Despite this variability, we show that fast EDSR can be achieved at most locations across a given sample. Second, a new Rabi driving mechanism emerges, enabled by valley dipoles and the hybridization of ground and excited valley states, which arise from alloy disorder and EDSR driving, respectively. This mechanism is dominant in regions of low valley splitting. Alloy disorder can therefore strengthen EDSR, but it can also cause gradients in $Ω$ that lead to dephasing in the rotating frame. We explore this problem by first locating "sweet spots," where EDSR is relatively insensitive to electric-field fluctuations. We then show that high-fidelity Rabi oscillations can be achieved in the presence of realistic charge noise. These results suggest that Wiggle Wells are a promising platform for high-quality, micromagnet-free gate operations.
△ Less
Submitted 1 June, 2026; v1 submitted 23 May, 2026;
originally announced May 2026.
-
Order-Disorder Tricriticality in $\mathrm{A}_n \mathrm{B}_n$ Star Polymer Melts
Authors:
Minhoon Kim,
Wonjun Kang,
Daeseong Yong,
Junhan Cho,
Jaeup U. Kim
Abstract:
Tricriticality usually requires tuning an additional thermodynamic parameter. Here we show that, in symmetric $\mathrm{A}_n\mathrm{B}_n$ star-polymer melts, the arm number $n$ itself plays this role and drives the order--disorder transition (ODT) from second order to first order. By developing a sixth-order free-energy expansion within the random phase approximation and comparing it with self-cons…
▽ More
Tricriticality usually requires tuning an additional thermodynamic parameter. Here we show that, in symmetric $\mathrm{A}_n\mathrm{B}_n$ star-polymer melts, the arm number $n$ itself plays this role and drives the order--disorder transition (ODT) from second order to first order. By developing a sixth-order free-energy expansion within the random phase approximation and comparing it with self-consistent field theory (SCFT) calculations, we analytically identify a tricritical arm number, $n_{\mathrm{tc}}\approx 5.4475$. For $n<n_{\mathrm{tc}}$, the lamellar ordering transition remains continuous and occurs at the spinodal point, $(χN)_{\mathrm{s}}\approx 10.495$. For $n>n_{\mathrm{tc}}$, the transition becomes first order, and $(χN)_{\mathrm{ODT}}$ shifts below $(χN)_{\mathrm{s}}$ with a quadratic dependence near the tricritical point. SCFT calculations confirm the predicted transition character and phase-boundary shift. The origin of this behavior is traced to inter-arm correlations generated by the common junction. We further show that the noninteger tricritical arm number can be effectively realized in binary mixtures of star polymers. This provides a rare analytically tractable example of architecture-induced tricriticality in a microphase-separating polymer system.
△ Less
Submitted 22 May, 2026;
originally announced May 2026.
-
Finite-temperature spin diffusion in the two-dimensional XY model
Authors:
Erik Fitzner,
Byungjin Lee,
Junhyeok Hur,
Minseok Kim,
Benedikt Schneider,
Jae-yoon Choi,
Björn Sbierski
Abstract:
We present a combined theory-experiment study to quantify spin diffusion in the square lattice quantum spin-1/2 XY model at finite temperature. On the theory side, we leverage a recently developed dynamical high-temperature expansion method to faithfully capture the long spatiotemporal scales of the hydrodynamic regime. Experimental results are obtained from an optical lattice hard-core boson quan…
▽ More
We present a combined theory-experiment study to quantify spin diffusion in the square lattice quantum spin-1/2 XY model at finite temperature. On the theory side, we leverage a recently developed dynamical high-temperature expansion method to faithfully capture the long spatiotemporal scales of the hydrodynamic regime. Experimental results are obtained from an optical lattice hard-core boson quantum simulator. The excellent agreement of spin diffusion constants marks a breakthrough in spin-transport beyond one dimension and for the quantitative validation of state-of-the-art quantum simulation platforms. We also provide theory predictions for future experiments on dynamic spin conductivity or anisotropy-induced integrability breaking.
△ Less
Submitted 19 May, 2026;
originally announced May 2026.
-
Strong electron correlations and ligand hybridization for altermagnetism
Authors:
Byungkyun Kang,
Anderson Janotti,
Dai Q. Ho,
Myoung-Hwan Kim,
Chul Hong Park,
Sangkook Choi,
Mark R. Pederson,
Eunja Kim
Abstract:
Spin-band splitting is a hallmark of altermagnetism, intrinsically linked to magnetic ordering driven by electron correlations. However, recent inconsistencies in the detection of altermagnetism in strongly correlated altermagnet candidates have cast doubt on the robustness of this phenomenon and its dependence on many-body effects. Here, using state-of-the-art quantum many-body frameworks, we dis…
▽ More
Spin-band splitting is a hallmark of altermagnetism, intrinsically linked to magnetic ordering driven by electron correlations. However, recent inconsistencies in the detection of altermagnetism in strongly correlated altermagnet candidates have cast doubt on the robustness of this phenomenon and its dependence on many-body effects. Here, using state-of-the-art quantum many-body frameworks, we dissect the electronic origins of altermagnetism in three prototypical candidates: MnF$_2$, MnTe, and RuO$_2$. In MnF$_2$, we identify pronounced local electron correlations within Mn-3$d$ states and uncover a distinct Mott gap in the visible range, rooted in nonlocal screening effects. The strong correlations markedly localize the Mn-3$d$ electrons, leading to a narrowing of the spin-resolved bandwidth and, consequently, a suppression of spin-band splitting. By contrast, MnTe provides an ideal platform for altermagnetism, exhibiting substantial local Mn-3$d$ magnetic moments due to the strong correlations and pronounced spin-band splitting, enabled by robust Mn 3$d$--Te-5$p$ orbital hybridization. RuO$_2$ manifests as a Pauli paramagnet with vanishing local moments, even in its antiferromagnetic phase. Nonetheless, it exhibits significant spin-band splitting, indicative of itinerant altermagnetic behavior. Our results reveal that both strong local electron correlations and judicious ligand selection to promote orbital hybridization are key prerequisites to realizing altermagnetism in strongly correlated systems. These insights pave the way for the rational design and discovery of novel altermagnetic materials.
△ Less
Submitted 13 May, 2026;
originally announced May 2026.
-
A Hardware-aware Hopfield Network with a Nonlinear Memristor Array for Robust Associative Memory with Superlinear Capacity
Authors:
Younghyun Lee,
Hakseung Rhee,
Unhyeon Kang,
Seungmin Oh,
Kyungmin Lee,
Hyun Jae Jang,
Seongsik Park,
YeonJoo Jeong,
Inho Kim,
Jong Keuk Park,
Kyung Min Kim,
Suyoun Lee
Abstract:
Associative memory retrieves complete patterns from partial or corrupted inputs and constitutes a primitive form of generative inference. Classical Hopfield networks (CHN) provide a canonical framework for associative memory but suffer from limited memory capacity. Recently, modern Hopfield networks (MHN) were introduced to achieve higher capacity by using explicit pattern-wise storage and neurons…
▽ More
Associative memory retrieves complete patterns from partial or corrupted inputs and constitutes a primitive form of generative inference. Classical Hopfield networks (CHN) provide a canonical framework for associative memory but suffer from limited memory capacity. Recently, modern Hopfield networks (MHN) were introduced to achieve higher capacity by using explicit pattern-wise storage and neurons with the softmax activation function, which makes the MHN vulnerable to noise and the hardware implementation complicated due to its network size varying with the number of stored patterns. Here, we introduce a hardware-aware Hopfield network (HHN), in which the intrinsic nonlinear current-voltage characteristics of a charge-trap memristor are leveraged to engineer the energy landscape of the HN, increasing the memory capacity. Using a 25 x 25 nonlinear memristor array, we demonstrate reliable reconstruction of corrupted patterns with memory capacity far exceeding the classical limit (K ~ 0.14N, where N is the number of neurons). The HHN preserves Hopfield-type energy-minimization dynamics and remains robust to synaptic conductance noise. Large-scale simulations on high-dimensional image data reveal an empirical memory capacity scaling of K ~ 0.3 x N^1.2 under a fixed synaptic budget. These results establish HHN as a scalable hardware-native architecture for low-power associative memory and generative inference.
△ Less
Submitted 8 May, 2026;
originally announced May 2026.
-
Density diversity in training data governs thermodynamic transferability of machine learning interatomic potentials
Authors:
Minwoo Kim,
Seungtae Kim,
Je-Yeon Jung,
Min Young Ha,
Won Bo Lee
Abstract:
Machine learning interatomic potentials (MLIPs) offer first-principles accuracy with reduced computational cost, but their transferability across different thermodynamic states remains questionable, particularly for fluid systems where molecules experience local environments far from crystalline equilibrium. Here, we demonstrate that diversifying the density of training configurations, rather than…
▽ More
Machine learning interatomic potentials (MLIPs) offer first-principles accuracy with reduced computational cost, but their transferability across different thermodynamic states remains questionable, particularly for fluid systems where molecules experience local environments far from crystalline equilibrium. Here, we demonstrate that diversifying the density of training configurations, rather than temperature, is the most effective strategy for building thermodynamically transferable MLIPs within a fixed computational budget. We first show that foundation MLIPs trained on solid-state databases accurately describe liquid-like densities but fail at gas-like conditions, while molecular-database-trained models exhibit the opposite behavior. Controlled from-scratch training and distillation experiments confirm that density-diverse datasets resolve both failure modes, whereas temperature-diverse datasets cannot compensate for missing density regimes. Coordination number analysis reveals the physical origin of this behavior: local coordination topology is more susceptible to density than temperature, leading to further structural diversity. These results establish density diversity as a design principle for thermodynamically transferable MLIPs and provide a validation framework for assessing the thermodynamic coverage of both foundation and from-scratch models, enabling reliable atomistic simulation of fluid-phase processes across diverse operating conditions.
△ Less
Submitted 7 May, 2026;
originally announced May 2026.
-
On the complementary roles of anisotropic crack density and anisotropic crack driving force in phase-field modeling of mixed-mode fracture
Authors:
Guk Heon Kim,
Minseo Kim,
Kwangsan Chun,
Jaemin Kim
Abstract:
Phase-field models for anisotropic fracture employ two complementary mechanisms: (i) the anisotropic crack density function, controlling direction-dependent fracture resistance, and (ii) the anisotropic strain energy, governing the fracture driving force. Although the unified framework was presented in Pranavi et al.[Comput. Mech., 73 (2024)], the distinct roles of these mechanisms and their inter…
▽ More
Phase-field models for anisotropic fracture employ two complementary mechanisms: (i) the anisotropic crack density function, controlling direction-dependent fracture resistance, and (ii) the anisotropic strain energy, governing the fracture driving force. Although the unified framework was presented in Pranavi et al.[Comput. Mech., 73 (2024)], the distinct roles of these mechanisms and their interaction remain uninvestigated. This work addresses this gap by first validating the formulation against mixed-mode fracture experiments on a soft elastomer (Lu et al. [Extreme Mech. Lett., 48 (2021)]), and then conducting systematic parametric studies on single-edge-notched (SEN) and open-hole tension (OHT) specimens to isolate each mechanism. The SEN studies show that the crack density anisotropy controls the crack path and toughness while leaving the elastic response unchanged, whereas the anisotropic strain energy deflects the crack but saturates rapidly. The OHT studies reveal a geometry-dependent role expansion: the anisotropic strain energy governs fiber-orientation-dependent stiffness, peak force, and fracture displacement. When both mechanisms act together, the combined response exhibits nonlinear synergistic interaction exceeding the linear sum of the individual contributions. These results establish that the crack density anisotropy governs the crack path (fracture resistance), while the anisotropic strain energy governs the driving force and, in stress-concentration geometries, additionally controls the elastic strain energy distribution around the stress concentrator.
△ Less
Submitted 18 April, 2026;
originally announced April 2026.
-
Continuous correlated states and dual-flatness in a moiré heterostructure
Authors:
Mohammed M. Al Ezzi,
Na Xin,
Yanmeng Shi,
Shuigang Xu,
Julien Barrier,
Alexey Berdyugin,
Shubhadeep Bhattacharjee,
Angelika Knothe,
Kenji Watanabe,
Takashi Taniguchi,
Vladimir Falko,
Giovanni Vignale,
Andre K. Geim,
Shaffique Adam,
Kostya S. Novoselov,
Minsoo Kim
Abstract:
Many-body effects in condensed matter yield novel quantum states when the electronic density of states is enhanced. A vivid example is flat bands, which suppress kinetic energy and let interactions dominate, when they are filled with an integer number of electrons in moire systems. Yet flat bands and commensurate fillings are not the only conditions for correlated phenomena. Situations may occur w…
▽ More
Many-body effects in condensed matter yield novel quantum states when the electronic density of states is enhanced. A vivid example is flat bands, which suppress kinetic energy and let interactions dominate, when they are filled with an integer number of electrons in moire systems. Yet flat bands and commensurate fillings are not the only conditions for correlated phenomena. Situations may occur where the band structure develops locally enhanced density of states, leading to strong correlations even at non-integer fillings, although such cases often yield pseudogaps that make detection elusive. Here we demonstrate that small-angle twisted monolayer-bilayer graphene combines moire-induced global flat band and additional local band flattening. Their coexistence allows direct comparison of correlated effects. The global route stabilizes commensurate states, while the local mechanism produces nearly flat bands, lifting degeneracy and generating symmetry breaking at non-integer fillings, yet without opening a global gap. Because there is no global gapped signature, the system remains metallic, but the effect reveals itself in anomalous Hall responses, signaling time-reversal symmetry breaking and valley polarization. Our results demonstrate dual-flatness as a guiding principle, extending moire physics beyond commensurate fillings and identifying topological transport as a probe of gapless correlated metals.
△ Less
Submitted 15 April, 2026;
originally announced April 2026.
-
Epitaxial MgSnN2 on 4H-SiC (0001): An Earth-Abundant Nitride for Green Optoelectronics and Photovoltaics
Authors:
D. Gogova,
D. Tran,
V. Stanishev,
D. Shafizadeh,
C. -L. Hsiao,
M. Kim,
B. Pécz,
A. Kovács,
K. Frey,
A. Sulyok,
N. K. Singh,
A. Le Febvrier,
P. Eklund,
V. Darakchieva
Abstract:
Group II-IV nitrides have recently emerged as a novel class of semiconductors composed of earth-abundant elements. Owing to their tunable bandgaps, comparable to those of III-nitrides, these materials are attractive candidates for replacing expensive Ga-based alloys in photovoltaics and green-gap optoelectronics. In this work, epitaxial growth of MgSnN2 layers on 4H-SiC(0001) substrates by direct…
▽ More
Group II-IV nitrides have recently emerged as a novel class of semiconductors composed of earth-abundant elements. Owing to their tunable bandgaps, comparable to those of III-nitrides, these materials are attractive candidates for replacing expensive Ga-based alloys in photovoltaics and green-gap optoelectronics. In this work, epitaxial growth of MgSnN2 layers on 4H-SiC(0001) substrates by direct current magnetron sputtering is demonstrated. Mg and Sn metal targets have been co-sputtered in nitrogen-containing atmosphere at growth temperatures up to 500 °C. X-ray diffraction and cross-sectional transmission electron microscopy confirm the MgSnN2 layers grow epitaxially in a wurtzite crystal structure, exhibiting the epitaxial relationships with the substrate: MgSnN2 [0001]//4H-SiC [0001] and MgSnN2 [10-10]//4H-SiC[10-10]. Improved crystalline quality is observed for higher deposition temperatures and near-stoichiometric composition, as evidenced by the narrowing of rocking curve linewidths. Optical characterization reveals high absorption coefficients (1e5 cm-1) in the visible spectrum, comparable to that of GaAs, highlighting the suitability of MgSnN2 for photovoltaic applications. A photoluminescence emission band at ~2.4 eV is detected, highly desirable for optoelectronic devices operating in the challenging green spectral region. These results establish MgSnN2 as an earth-abundant, environmentally friendly material, structurally compatible with III-nitrides, with potential for cost-efficient components in sustainable optoelectronics and photovoltaics.
△ Less
Submitted 6 April, 2026;
originally announced April 2026.
-
A Solid-Based Approach for Modeling Simple Yield-Stress Fluids: Rheological Transitions, Overshoot and Relaxation
Authors:
Jehyeok Choi,
Ju Min Kim,
Kwang Soo Cho
Abstract:
Yield-stress fluids are ubiquitous and encountered in diverse fields ranging from natural muddy flows to industrial applications such as secondary battery electrode slurries and direct ink writing. Despite the proposal of various constitutive equations, few models have been shown to successfully predict both steady and transient rheological behaviors in yield-stress fluids. In this study, a consti…
▽ More
Yield-stress fluids are ubiquitous and encountered in diverse fields ranging from natural muddy flows to industrial applications such as secondary battery electrode slurries and direct ink writing. Despite the proposal of various constitutive equations, few models have been shown to successfully predict both steady and transient rheological behaviors in yield-stress fluids. In this study, a constitutive equation is hereby proposed, offering a comprehensive description of the rheological characteristics observed in simple yield-stress fluids, excluding thixotropy, such as the Carbopol dispersion. The constitutive equation is derived from a Zener-type viscoelastic solid element combined with an additional linear dashpot connected in parallel, together with a nonlinear viscosity model, a flow rule, an evolution equation for the back stress, and the Kroner-Lee decomposition. This combination satisfies the principle of material frame invariance. The proposed model successfully reproduces the rheological characteristics qualitatively in a manner consistent with experimental observations conducted during start-up shear, creep, and stress relaxation tests. In particular, the present viscoelastic solid-based constitutive equation is shown to accurately predict stress overshoot during start-up shear. Importantly, the overshoot is found to originate from a homogeneous mechanism in which normal stress difference enhances the stress invariant and thereby accelerates the plastic response, rather than from isotropic hardening or spatially heterogeneous microstructural evolution. This study is expected to facilitate a deeper understanding of the intricate dynamics governing the flow of yield-stress fluids.
△ Less
Submitted 4 June, 2026; v1 submitted 3 April, 2026;
originally announced April 2026.
-
Visualizing Millisecond Atomic Dynamics of Nanocrystals in Liquid
Authors:
Sungsu Kang,
Jinho Rhee,
Joodeok Kim,
Sam Oaks-Leaf,
Minwoo Kim,
Shengsong Yang,
Chang Liu,
Dongsu Kim,
Sungin Kim,
Binyu Wu,
Won Bo Lee,
David T. Limmer,
A. Paul Alivisatos,
Peter Ercius Jungwon Park
Abstract:
Atomic structures of nanomaterials are inherently dynamic, continuously reshaped through interactions with chemical species and external stimuli. Such dynamics are further amplified as the size and dimensionality of nanomaterials are reduced. Despite advances in analytical methods, it remains challenging to capture structural dynamics of nanomaterials in reactive environments with both atomic spat…
▽ More
Atomic structures of nanomaterials are inherently dynamic, continuously reshaped through interactions with chemical species and external stimuli. Such dynamics are further amplified as the size and dimensionality of nanomaterials are reduced. Despite advances in analytical methods, it remains challenging to capture structural dynamics of nanomaterials in reactive environments with both atomic spatial resolution and commensurate temporal resolution. Here, we directly visualize atomic-scale dynamics of gold (Au) nanocrystals in reactive liquid environments with millisecond-speed liquid cell electron microscopy (EM) and deep-learning denoising. We uncover reversible fluctuations in local crystallinity of Au nanocrystals dependent on the surrounding chemical environment. These transient fluctuations, driven by interactions at nanocrystal-liquid interfaces, critically influence dissolution kinetics and grain boundary relaxation. By overcoming the spatiotemporal limitations in conventional liquid cell EM, our findings provide insights into how transient nanoscale structures dictate the stability and reactivity of nanomaterials.
△ Less
Submitted 25 March, 2026;
originally announced March 2026.
-
Density-Dependent Transition in Bacterial Self-Organization Driven by Confinement and Aerotaxis
Authors:
Minjun Kim,
Joonwoo Jeong
Abstract:
We experimentally investigate how aerotactic bacteria, confined within a thin liquid film between two solid substrates, respond to a controlled oxygen gradient. We find that the total bacterial number density dictates which mechanism dominates the steady-state spatial distribution: wall accumulation or aerotaxis. At low densities, despite receiving oxygen only from one substrate, motile bacteria a…
▽ More
We experimentally investigate how aerotactic bacteria, confined within a thin liquid film between two solid substrates, respond to a controlled oxygen gradient. We find that the total bacterial number density dictates which mechanism dominates the steady-state spatial distribution: wall accumulation or aerotaxis. At low densities, despite receiving oxygen only from one substrate, motile bacteria accumulate at both walls, forming a symmetric distribution. In contrast, pronounced aerotactic migration toward the oxygen-supplying wall emerges as the density increases. Analyzing the temporal evolution of this bacterial distribution reveals that the aerotactic response is driven by a self-generated oxygen gradient induced by collective respiration. Our diffusion-advection model of bacteria and oxygen, accounting for aerotactic migration, hydrodynamic attraction to the walls, and respiration, quantitatively reproduces our experimental observations and provides valuable insights into bacterial self-organization within complex environments.
△ Less
Submitted 5 April, 2026; v1 submitted 15 March, 2026;
originally announced March 2026.
-
Plasmonic polaron in self-intercalated 1T-TiS2
Authors:
Byoung Ki Choi,
Woojin Choi,
Zhiyu Tao,
Ji-Eun Lee,
Sae Hee Ryu,
Seungrok Mun,
Hyobeom Lee,
Kyoungree Park,
Seha Lee,
Hayoon Im,
Yong Zhong,
Hyejin Ryu,
Min Jae Kim,
Sue Hyeon Hwang,
Xuetao Zhu,
Jiandong Guo,
Jong Mok Ok,
Jaekwang Lee,
Haeyong Kang,
Sungkyun Park,
Jonathan D. Denlinger,
Heung-Sik Kim,
Aaron Bostwick,
Zhi-Xun Shen,
Choongyu Hwang
, et al. (2 additional authors not shown)
Abstract:
Electron-boson coupling is central to a comprehensive understanding of the diverse physical phenomena emerging from many-body interactions. Yet less attention has been paid to how plasmons, collective bosonic modes of electron density oscillation, interact with conduction electrons and how external parameters can tune this interaction. Here, we present a clear display of composite quasiparticles s…
▽ More
Electron-boson coupling is central to a comprehensive understanding of the diverse physical phenomena emerging from many-body interactions. Yet less attention has been paid to how plasmons, collective bosonic modes of electron density oscillation, interact with conduction electrons and how external parameters can tune this interaction. Here, we present a clear display of composite quasiparticles stemming from electron-plasmon coupling, known as the plasmonic polaron, in self-intercalated 1T-TiS2, by using angle-resolved photoemission spectroscopy (ARPES), high-resolution electron energy loss spectroscopy (HR-EELS) and first-principles calculations. The single particle spectral function exhibits a distinctive plasmon-loss satellite with the same characteristic energy scale determined by HR-EELS measurements. The bosonic energy scale of plasmonic polaron is tunable by controlling charge carrier density and temperature, distinguishing itself from conventional polarons arising from electron-phonon interactions. Furthermore, we find that the dielectric screening strongly affects the formation of the plasmonic polaron states. Our findings provide direct spectroscopic evidence of plasmonic polarons and establish self-intercalated layered materials as a promising platform for studying, controlling, and harnessing plasmonic interactions in quantum materials.
△ Less
Submitted 3 March, 2026;
originally announced March 2026.
-
Self-avoiding tethered surfaces are always flat
Authors:
A. D. Chen,
M. C. Gandikota,
M. J. Kim,
A. Cacciuto
Abstract:
The scaling behavior of fully flexible elastic tethered surfaces has been debated for decades. Some theories predict that self-avoiding surfaces would crumple in the absence of bending rigidity, while most simulations suggested that they would remain flat. Recent simulations on ideal membranes with lattice perforations suggest that systematically removing surface area from a membrane may provide a…
▽ More
The scaling behavior of fully flexible elastic tethered surfaces has been debated for decades. Some theories predict that self-avoiding surfaces would crumple in the absence of bending rigidity, while most simulations suggested that they would remain flat. Recent simulations on ideal membranes with lattice perforations suggest that systematically removing surface area from a membrane may provide an alternative way to crumpling self-avoiding surfaces. We perform extensive numerical simulations of two models of fully flexible elastic tethered surfaces in which self-avoidance can be systematically and continuously tuned to the ideal limit. We show that in the thermodynamic limit, these surfaces remain flat with a size exponent $ν=1$ for any finite degree of self-avoidance, with or without membrane perforations.
△ Less
Submitted 25 February, 2026;
originally announced February 2026.
-
Accelerated Markov Chain Monte Carlo Simulation via Neural Network-Driven Importance Sampling
Authors:
Michael Kim,
Wei Cai
Abstract:
Atomistic simulations provide valuable insights into the physical processes governing material behavior. However, their applicability is fundamentally constrained by the limited time scales accessible to brute-force simulations. This bottleneck often stems from complex energy landscapes where the systems stay trapped in metastable states for long periods of time. Yet, the long-term evolution is co…
▽ More
Atomistic simulations provide valuable insights into the physical processes governing material behavior. However, their applicability is fundamentally constrained by the limited time scales accessible to brute-force simulations. This bottleneck often stems from complex energy landscapes where the systems stay trapped in metastable states for long periods of time. Yet, the long-term evolution is controlled by the transitions between the metastable states, which are rare events and difficult to observe. We present an importance sampling method designed to accelerate the time scale of Markov chain Monte Carlo (MCMC) simulations. By employing a bias potential, our approach enhances the sampling of rare transition events while preserving the relative probabilities of distinct transition pathways. The bias potential is represented by a neural network which enables the flexibility needed for high-dimensional systems. We propose a rigorous formulation to obtain the original transition rates between metastable states using transition paths obtained from the biased simulation. We further use a branching random walk (BRW) technique to enhance efficiency and to reduce variance. The proposed methodology is validated on 2-dimensional and 14-dimensional systems, demonstrating its accuracy and scalability.
△ Less
Submitted 31 January, 2026;
originally announced February 2026.
-
AtomMOF: All-Atom Flow Matching for MOF-Adsorbate Structure Prediction
Authors:
Nayoung Kim,
Honghui Kim,
Sihyun Yu,
Minkyu Kim,
Seongsu Kim,
Sungsoo Ahn
Abstract:
Deep generative models have shown promise for modeling metal-organic frameworks (MOFs), but existing approaches (1) rely on coarse-grained representations that assume fixed bond lengths and angles, and (2) neglect the MOF-adsorbate interactions, which are critical for downstream applications. We introduce AtomMOF, a scalable flow-based model built on an all-atom Diffusion Transformer that maps 2D…
▽ More
Deep generative models have shown promise for modeling metal-organic frameworks (MOFs), but existing approaches (1) rely on coarse-grained representations that assume fixed bond lengths and angles, and (2) neglect the MOF-adsorbate interactions, which are critical for downstream applications. We introduce AtomMOF, a scalable flow-based model built on an all-atom Diffusion Transformer that maps 2D molecular graphs of building blocks and adsorbates directly to equilibrium 3D structures without imposing structural constraints. We further present scaling laws for porous crystal generation, indicating predictable performance gains with increased model capacity, and introduce Feynman-Kac steering guided by machine-learned interatomic potentials to improve geometric validity and sampling stability. On the (MOF-only) BW dataset, AtomMOF increases the match rate by 35.00% and reduces RMSD by 32.64%. On the ODAC25 dataset (MOF-adsorbate), AtomMOF is substantially more sample-efficient than grand canonical Monte Carlo in recovering adsorption configurations and can identify candidates with lower adsorption energies than the reference dataset. Code is available at https://github.com/nayoung10/AtomMOF.
△ Less
Submitted 6 February, 2026;
originally announced February 2026.
-
Superconductivity in Isolated Single Copper Oxygen Plane
Authors:
Youngdo Kim,
Byeongjun Gil,
Sehoon Kim,
Yeonjae Lee,
Donghan Kim,
Jaeung Lee,
Jinyoung Kim,
Younsik Kim,
Miyoung Kim,
Changyoung Kim
Abstract:
One of the central questions in cuprate superconductivity is if superconductivity can exist in an isolated single CuO$_2$ plane without any interlayer coupling. There have been numerous experimental efforts to answer this question, but it still has not been clearly resolved. Here we present a heterostructure system with an isolated half-unit-cell La$_{2-x}$Sr$_x$CuO$_4$ which has a single CuO$_2$…
▽ More
One of the central questions in cuprate superconductivity is if superconductivity can exist in an isolated single CuO$_2$ plane without any interlayer coupling. There have been numerous experimental efforts to answer this question, but it still has not been clearly resolved. Here we present a heterostructure system with an isolated half-unit-cell La$_{2-x}$Sr$_x$CuO$_4$ which has a single CuO$_2$ plane. Using in-situ angle-resolved photoemission spectroscopy, we measured the electronic and gap structures of a single CuO$_2$ plane. We observed a \textit{d}-wave-like gap which closes somewhat above the bulk T$_c$. Moreover, almost identical gap properties are seen for both single CuO$_2$ plane and bulk. These observations lead us to the conclusion that the d-wave superconductivity of cuprates also exists in a single CuO$_2$ plane. Our results demonstrate that cuprate superconductivity is essentially a two-dimensional phenomenon and provide a platform to study cuprate superconductivity in a purely two-dimensional system.
△ Less
Submitted 5 February, 2026;
originally announced February 2026.
-
CatFlow: Co-generation of Slab-Adsorbate Systems via Flow Matching
Authors:
Minkyu Kim,
Nayoung Kim,
Honghui Kim,
Sungsoo Ahn
Abstract:
Discovering heterogeneous catalysts tailored for specific reaction intermediates remains a fundamental bottleneck in materials science. While traditional trial-and-error methods and recent generative models have shown promise, they struggle to capture the intrinsic coupling between surface geometry and adsorbate interactions. To address this limitation, we propose CatFlow, a flow matching-based fr…
▽ More
Discovering heterogeneous catalysts tailored for specific reaction intermediates remains a fundamental bottleneck in materials science. While traditional trial-and-error methods and recent generative models have shown promise, they struggle to capture the intrinsic coupling between surface geometry and adsorbate interactions. To address this limitation, we propose CatFlow, a flow matching-based framework for de novo design and structure prediction of heterogeneous catalysts. Our model operates on a primitive cell-based factorized representation of the slab-adsorbate complex, reducing the number of learnable variables by an average of 9.2x while explicitly encoding the surface orientation of the slab-adsorbate interface. Experiments on the Open Catalyst 2020 dataset demonstrate that CatFlow significantly improves the structural fidelity of generated catalysts compared to autoregressive and sequential baselines. Further experiments show that the generated structures accurately capture the adsorption energy distributions of physically plausible interfaces and lie closer to thermodynamic local minima.
△ Less
Submitted 18 May, 2026; v1 submitted 5 February, 2026;
originally announced February 2026.
-
Transient Pauli blocking in a InN film as a mechanism for broadband ultrafast optical switching
Authors:
Junjun Jia,
Minseok Kim,
Yuzo Shigesato,
Ryotaro Nakazawa,
Keisuke Fukutani,
Satoshi Kera,
Toshiki Makimoto,
Takashi Yagi
Abstract:
The transient Pauli blocking effect offers a promising route for achieving ultrafast optical switching in semiconductors, enabling a rapid switching from an initially opaque state to a relatively transparent state upon photoexcitation. Herein, we demonstrate broadband ultrafast optical switching in degenerate InN thin films, spanning the visible to near-infrared spectral range, using pump-probe tr…
▽ More
The transient Pauli blocking effect offers a promising route for achieving ultrafast optical switching in semiconductors, enabling a rapid switching from an initially opaque state to a relatively transparent state upon photoexcitation. Herein, we demonstrate broadband ultrafast optical switching in degenerate InN thin films, spanning the visible to near-infrared spectral range, using pump-probe transient transmittance measurements. To elucidate the underlying physical mechanism, we perform probe-energy-resolved analysis for ultrafast dynamics, and develop a theoretical model based on a quasi-equilibrium Fermi-Dirac distribution. The model successfully captures the experimental transients and yields an electron-phonon coupling constant of $1.0\times10^{17}\,\mathrm{W\,m^{-3}\,K^{-1}}$, along with an electronic specific heat coefficient ranging from 1.52 to 2.02 $\mathrm{mJ\,mol^{-1}\,K^{-2}}$, which allow direct prediction of the spectral switching window. Notably, we demonstrate that the Pauli blocking effect can be induced solely by a laser-excitation driven rise in electronic temperature, without requiring significant carrier injection into the conduction band in degenerate semiconductors. These findings offer new insights for designing ultrafast optical modulators, shutters, and photonic devices for next-generation communication and computing technologies.
△ Less
Submitted 21 January, 2026;
originally announced January 2026.
-
Low-dimensionality-induced tunable ferromagnetism in SrRuO$_3$ ultrathin films
Authors:
Jinyoung Kim,
Minjae Kim,
Donghan Kim,
Sungsoo Hahn,
Younsik Kim,
Minsoo Kim,
Byungmin Sohn,
Changyoung Kim
Abstract:
Quantum materials near electronic or magnetic phase boundaries exhibit enhanced tunability, as their emergent properties become highly sensitive to external perturbations. Here, we demonstrate precise control of ferromagnetism in a SrRuO$_3$ ultrathin film, where a high density of states (DOS), arising from low-dimensional quantum states, places the system at the crossover between a non-magnetic a…
▽ More
Quantum materials near electronic or magnetic phase boundaries exhibit enhanced tunability, as their emergent properties become highly sensitive to external perturbations. Here, we demonstrate precise control of ferromagnetism in a SrRuO$_3$ ultrathin film, where a high density of states (DOS), arising from low-dimensional quantum states, places the system at the crossover between a non-magnetic and bulk ferromagnetic state. Using spin- and angle-resolved photoemission spectroscopy (SRPES/ARPES), transport measurements, and theoretical calculations, we systematically tune the Fermi level via electron doping across the high-DOS point. We directly visualize the spin-split band structure and reveal its influence on both magnetic and transport properties. Our findings provide compelling evidence that magnetism can be engineered through DOS control at a phase crossover, establishing a pathway for the rational design of tunable quantum materials.
△ Less
Submitted 10 December, 2025;
originally announced December 2025.
-
Improving 2D-ness to enhance thermopower in oxide superlattices
Authors:
Dongwon Shin,
Inseo Kim,
Min-Su Kim,
Yu-Qiao Zhang,
Woo Tack Lim,
Si-Young Choi,
Minseok Choi,
Hiromichi Ohta,
Woo Seok Choi
Abstract:
The transport dynamics of itinerant charge carriers and their interactions with the environment. For two-dimensional oxide thermoelectrics, predominantly represented by doped SrTiO3-based superlattices, reduced spatial dimensions and increased effective mass are known to enhance thermopower (S). However, because of their large effective Bohr radius resulting from their high dielectric constant, Sr…
▽ More
The transport dynamics of itinerant charge carriers and their interactions with the environment. For two-dimensional oxide thermoelectrics, predominantly represented by doped SrTiO3-based superlattices, reduced spatial dimensions and increased effective mass are known to enhance thermopower (S). However, because of their large effective Bohr radius resulting from their high dielectric constant, SrTiO3-based systems have limitations in exhibiting the 2D characteristic. Here, we focus on EuTiO3 as an alternative perovskite platform in which fractional LaxEu1-xTiO3/EuTiO3 artificial superlattices demonstrate the improvement in 2D nature for the dimensionality-induced improvement of S. We observed a quasi-2D thermopower S2D of -950 uV K-1 and S2D/S3D of ~20 resulting from the improved 2D confinement. Thermopower measurements, combined with hybrid density functional theory calculations, show the enhanced S originates from the confinement of Ti 3dxy-states within the LaxEu1-xTiO3 layers and the associated increase in the 2D density of states. In detail, a smaller effective Bohr radius and modified electronic band structures, in conjunction with the presence of the Eu 4f-states in EuTiO3 which modified the local electronic potential and strengthened the spatial confinement of Ti 3d-states. This approach to improving the dimensional confinement establishes a small effective Bohr radius and Eu 4f-state assisted 2D confinement provides valuable insights into the design of high-performance applications in artificial oxide superlattices.
△ Less
Submitted 5 December, 2025;
originally announced December 2025.
-
Symmetry-Enforced Fermi Surfaces
Authors:
Minho Luke Kim,
Salvatore D. Pace,
Shu-Heng Shao
Abstract:
We identify a symmetry that enforces every symmetric model to have a Fermi surface. These symmetry-enforced Fermi surfaces are realizations of a powerful form of symmetry-enforced gaplessness. The symmetry we construct exists in quantum lattice fermion models on a $d$-dimensional Bravais lattice, and is generated by the on-site U(1) fermion number symmetry and non-on-site Majorana translation symm…
▽ More
We identify a symmetry that enforces every symmetric model to have a Fermi surface. These symmetry-enforced Fermi surfaces are realizations of a powerful form of symmetry-enforced gaplessness. The symmetry we construct exists in quantum lattice fermion models on a $d$-dimensional Bravais lattice, and is generated by the on-site U(1) fermion number symmetry and non-on-site Majorana translation symmetry. The resulting symmetry group is a noncompact Lie group closely related to the Onsager algebra. For a symmetry-enforced Fermi surface $\cal{F}$, we show that this UV symmetry group always includes the subgroup of the ersatz Fermi liquid L$_{\cal{F}}$U(1) symmetry group formed by even functions ${f(\mathbf{k})\in\mathrm{U}(1)}$ with ${\mathbf{k}\in \cal{F}}$. Furthermore, we comment on the topology of these symmetry-enforced Fermi surfaces, proving they generically exhibit at least two noncontractible components (i.e., open orbits).
△ Less
Submitted 1 May, 2026; v1 submitted 3 December, 2025;
originally announced December 2025.
-
Microscopic origin of the spin-splitting in altermagnets
Authors:
Suyoung Lee,
Minjae Kim,
Changyoung Kim
Abstract:
Altermagnets, characterized by spin-split bands without net magnetization, have recently emerged as a promising platform for spintronics. However, their microscopic mechanisms remain elusive, often relying on abstract group theory. In this work, we present an intuitive and pedagogical framework to understand the origin of spin splitting in altermagnets. We identify two essential ingredients: (1) a…
▽ More
Altermagnets, characterized by spin-split bands without net magnetization, have recently emerged as a promising platform for spintronics. However, their microscopic mechanisms remain elusive, often relying on abstract group theory. In this work, we present an intuitive and pedagogical framework to understand the origin of spin splitting in altermagnets. We identify two essential ingredients: (1) alternating spin-polarized wavefunction localization on sublattices, and (2) broken translational symmetry caused by distortions in non-magnetic ion cages. We discuss a minimal model Hamiltonian based on an atomic exchange-driven spin splitting and anisotropic hopping that captures these effects and reproduces the hallmark features of altermagnetic band structures, including nodal spin degeneracies and large spin splittings. Our model is further validated by ab initio calculations on MnF2. By demystifying the microscopic origins of altermagnetism, our work bridges symmetry analysis and material realizations, shedding light on practical designs of altermagnetic spintronic devices.
△ Less
Submitted 30 November, 2025;
originally announced December 2025.
-
Universal Fabrication of Graphene/Perovskite Oxide Hybrid Heterostructures
Authors:
Yeongju Choi,
Seungjin Lee,
Dongwon Shin,
Sukhoon Sim,
Min-Hyoung Jung,
Dirk Wulferding,
Minjae Kim,
Jaesik Eom,
Myeesha Mostafa,
Wonhee Ko,
SeungNam Cha,
Jungseek Hwang,
Hu Young Jeong,
Ki Kang Kim,
Woo Seok Choi
Abstract:
Hybrid heterostructures composed of graphene and perovskite oxides provide a promising platform for exploiting synergetic interfacial functionalities. Conventional fabrication methods of the hybrid heterostructures rely on transferring graphene grown on metallic substrates-- a process that is time-consuming, labor-intensive, and prone to introducing numerous defects. In this study, we present a un…
▽ More
Hybrid heterostructures composed of graphene and perovskite oxides provide a promising platform for exploiting synergetic interfacial functionalities. Conventional fabrication methods of the hybrid heterostructures rely on transferring graphene grown on metallic substrates-- a process that is time-consuming, labor-intensive, and prone to introducing numerous defects. In this study, we present a universal, catalyst-free method for the direct growth of graphene on insulating substrates by employing three different perovskite oxide substrates (SrTiO$_3$, LaAlO$_3$, and (La$_{0.18}$Sr$_{0.82}$)(Al$_{0.59}$Ta$_{0.41}$)O$_3$) using atmospheric chemical vapor deposition. Comprehensive characterization via Raman spectroscopy, X-ray spectroscopy, scanning probe microscopy, and electron microscopy confirmed the formation of a uniform, continuous monolayer graphene on all substrates. We identified that growth temperature critically governs graphene quality, as excessive active species may lead to secondary nucleation and the formation of multilayer graphene. Notably, all substrates shared the same optimal growth conditions. Low-temperature Raman spectroscopy and scanning tunneling microscopy of the graphene/SrTiO$_3$ hybrid heterostructure revealed cooperative phenomena, including substrate-induced lattice-phonon and electron-phonon coupling. Our work establishes a reproducible, transfer-free fabrication route for graphene/perovskite oxide hybrid heterostructures and provides empirical support for the universal growth of graphene on insulating substrates.
△ Less
Submitted 30 November, 2025;
originally announced December 2025.
-
Non-magnetic spin splitting driven by spin-valley-layer coupling in multilayer WSe2
Authors:
Min-Gue Kim,
Min-Sik Kim,
Kenji Watanabe,
Takashi Taniguchi,
Ju-Jin Kim,
Myung-Ho Bae
Abstract:
Transition metal dichalcogenides provide a platform for exploring spin-valley physics, offering a promising approach to electric-field-driven spin control for low-power spintronic and quantum devices. Here, we demonstrate electric-field-induced spin splitting in the Q and Q' valleys of multilayer n-type WSe2 using quantum-point-contact spectroscopy. Systematic modulations in four distinct conducta…
▽ More
Transition metal dichalcogenides provide a platform for exploring spin-valley physics, offering a promising approach to electric-field-driven spin control for low-power spintronic and quantum devices. Here, we demonstrate electric-field-induced spin splitting in the Q and Q' valleys of multilayer n-type WSe2 using quantum-point-contact spectroscopy. Systematic modulations in four distinct conductance quantization steps, providing direct evidence of spin-valley-layer coupling-driven spin-resolved density of states, are achieved by tuning the out-of-plane gate voltage. Notably, the electric-field-induced spin splitting significantly dominate the magnetic-field-induced valley-Zeeman effect (i.e., ~7 meV for a displacement field change of ~0.08 V/nm vs. ~2 meV for a magnetic field of B = 9 T), demonstrating a powerful, non-magnetic manipulation of spin states. This ability to manipulate spin states by gate voltage is crucial for advancing next-generation low-power spintronic and quantum information technologies.
△ Less
Submitted 24 May, 2026; v1 submitted 28 November, 2025;
originally announced November 2025.
-
Broadband ultrafast self-heterodyned chiro-optical spectroscopy
Authors:
Francesco Gucci†,
Andrea Iudica†,
Andres Valladares Y Tacchi†,
Andrea Schirato,
Giulia Crotti,
Ryeong Myeong Kim,
Soo Min Lee,
Jeong Hyun Han,
Andrea Villa,
Dawar Ali,
Aurora Rizzo,
Margherita Maiuri,
Ki Tae Nam,
Giuseppe Della Valle,
Giulio Cerullo
Abstract:
Ultrafast chiro-optical spectroscopy provides unique access to the structural dynamics of molecules, spin-valley relaxation in semiconductors, and the non-equilibrium optical response of chiral nanophotonic systems. Yet, because chiral signals are intrinsically weak and time-resolved spectroscopy probes small photoinduced changes, transient chiro-optical responses are often difficult to isolate fr…
▽ More
Ultrafast chiro-optical spectroscopy provides unique access to the structural dynamics of molecules, spin-valley relaxation in semiconductors, and the non-equilibrium optical response of chiral nanophotonic systems. Yet, because chiral signals are intrinsically weak and time-resolved spectroscopy probes small photoinduced changes, transient chiro-optical responses are often difficult to isolate from parasitic achiral contributions. Here, we introduce a broadband ultrafast chiro-optical spectroscopy technique that integrates a birefringent common-path interferometer with an optical polarization bridge to sensitively detect photoinduced changes in the polarization state of light. Phase-sensitive self-heterodyned detection enables simultaneous measurement of transient circular dichroism and optical rotatory dispersion across a broad spectral range with ultrafast temporal resolution. Balanced detection suppresses excess laser noise, enabling exceptional sensitivity (<50 $μ$deg) close to shot-noise limit. We demonstrate this approach on an array of gold nano-helicoids, supported by a full-wave time-resolved model of the spatiotemporal dynamics of plasmonic non-equilibrium carriers and their associated optical nonlinearities. The model traces the system's transient chiro-optical response back to photoinduced modulations of the electric-magnetic dipole interaction in the nano-helicoid, elucidating the connection of near- and far-field dynamics in the non-equilibrium regime. We further investigate spin excitation, thermalization, and relaxation in a lead halide perovskite, establishing a novel approach to broadband time-resolved Faraday rotation. The simplicity, sensitivity, and wide applicability of this detection scheme provide a powerful platform for broadband ultrafast chiro-optical spectroscopy, opening new opportunities in biochemistry, solid-state physics, and nanophotonics.
△ Less
Submitted 13 November, 2025;
originally announced November 2025.
-
Role of Phase Fluctuation in Dynamic Competition Between Charge Order and Superconductivity in Cuprates
Authors:
Mingu Kang,
Pavel E. Dolgirev,
Chao C. Zhang,
Hoyoung Jang,
Byungjune Lee,
Minseok Kim,
Sang-Youn Park,
Ronny Sutarto,
Eugene Demler,
Jae-Hoon Park,
John Y. T. Wei,
Riccardo Comin
Abstract:
Phase fluctuations are a key factor distinguishing nonthermal (ultrafast) and thermal phase transitions. Charge order in cuprates is characterized by short-range coherence while competing with superconductivity, and as such, it provides a representative case to study the role of phase fluctuation in coupled order parameter dynamics. In this work, we investigated the intertwined evolution of charge…
▽ More
Phase fluctuations are a key factor distinguishing nonthermal (ultrafast) and thermal phase transitions. Charge order in cuprates is characterized by short-range coherence while competing with superconductivity, and as such, it provides a representative case to study the role of phase fluctuation in coupled order parameter dynamics. In this work, we investigated the intertwined evolution of charge order and superconductivity in cuprate/manganite heterostructures using time-resolved resonant X-ray scattering. The resulting dynamics are analyzed within a space- and time-dependent nonperturbative model capturing both amplitude and phase dynamics. At low fluence, photo-induced suppression of superconductivity results in a nonthermal enhancement of charge order, underscoring the dynamic competition between charge order and superconductivity. With increasing fluence, the slowing down of melting and recovery dynamics is observed, indicating a critical role of phase fluctuations. At high fluence, both charge order and superconductivity remain suppressed for an extended time window due to decoupling between amplitude and phase dynamics and the delayed recovery of phase coherence. Our work underscores the importance of phase fluctuation for understanding the dynamic competition between order parameters in cuprates.
△ Less
Submitted 30 October, 2025;
originally announced October 2025.
-
Impact of AlN buffer thickness on electrical and thermal characteristics of AlGaN/GaN/AlN HEMTs
Authors:
Minho Kim,
Dat Q. Tran,
Plamen P. Paskov,
U. Choi,
O. Nam,
Vanya Darakchieva
Abstract:
We investigate the influence of AlN buffer thickness on the structural, electrical, and thermal properties of AlGaN/GaN high-electron mobility transistors (HEMTs) grown on semi-insulating SiC substrates by metal-organic chemical vapor deposition. X-ray diffraction and atomic force microscopy reveal that while thin AlN layers (120 nm) exhibit compressive strain and smooth step-flow surfaces, thicke…
▽ More
We investigate the influence of AlN buffer thickness on the structural, electrical, and thermal properties of AlGaN/GaN high-electron mobility transistors (HEMTs) grown on semi-insulating SiC substrates by metal-organic chemical vapor deposition. X-ray diffraction and atomic force microscopy reveal that while thin AlN layers (120 nm) exhibit compressive strain and smooth step-flow surfaces, thicker single-layer buffers (550 nm) develop tensile strain and increased surface roughness. Multi-layer buffer structures up to 2 μm alleviate strain and maintain surface integrity. Low-temperature Hall measurements confirm that electron mobility decreases with increasing interface roughness, with the highest mobility observed in the structure with a thin AlN buffer. Transient thermoreflectance measurements show that thermal conductivity (ThC) of the AlN buffer increases with the thickness, reaching 188 W/m.K at 300 K for the 2 μm buffer layer, which is approximately 60% of the bulk AlN ThC value. These results highlight the importance of optimizing AlN buffer design to balance strain relaxation, thermal management, and carrier transport for high-performance GaN-based HEMTs.
△ Less
Submitted 30 October, 2025;
originally announced October 2025.
-
Strain Engineering of van Hove Singularity and Coupled Itinerant Ferromagnetism in Quasi-2D Oxide Superlattices
Authors:
Seung Gyo Jeong,
Minjae Kim,
Jin Young Oh,
Youngeun Ham,
In Hyeok Choi,
Seong Won Cho,
Jihyun Kim,
Huimin Jeong,
Byungmin Sohn,
Tuson Park,
Suyoun Lee,
Jong Seok Lee,
Deok-Yong Cho,
Bongjae Kim,
Woo Seok Choi
Abstract:
Engineering van Hove singularities (vHss) near the Fermi level, if feasible, offers a powerful route to control exotic quantum phases in electronic and magnetic behaviors. However, conventional approaches, which rely primarily on chemical and electrical doping, focus mainly on local electrical or optical measurements, limiting their applicability to coupled functionalities. In this study, a vHs-in…
▽ More
Engineering van Hove singularities (vHss) near the Fermi level, if feasible, offers a powerful route to control exotic quantum phases in electronic and magnetic behaviors. However, conventional approaches, which rely primarily on chemical and electrical doping, focus mainly on local electrical or optical measurements, limiting their applicability to coupled functionalities. In this study, a vHs-induced insulator-metal transition coupled with a ferromagnetic phase transition was empirically achieved in atomically designed quasi-2D SrRuO3 (SRO) superlattices via epitaxial strain engineering, which has not been observed in conventional 3D SRO systems. Theoretical calculations revealed that epitaxial strain effectively modulates the strength and energy positions of vHs of specific Ru orbitals, driving correlated phase transitions in the electronic and magnetic ground states. X-ray absorption spectroscopy confirmed the anisotropic electronic structure of quasi-2D SRO modulated by epitaxial strain. Magneto-optic Kerr effect and electrical transport measurements demonstrated modulated magnetic and electronic phases. Furthermore, magneto-electrical measurements detected significant anomalous Hall effect signals and ferromagnetic magnetoresistance, indicating the presence of magnetically coupled charge carriers in the 2D metallic regime. This study establishes strain engineering as a promising platform for tuning vHss and resultant itinerant ferromagnetism of low-dimensional correlated quantum systems.
△ Less
Submitted 28 October, 2025;
originally announced October 2025.
-
Dynamics and formation of antiferromagnetic textures in MnBi$_2$Te$_4$ single crystal
Authors:
M. G. Kim,
S. Boney,
L. Burgard,
L. Rutowski,
C. Mazzoli
Abstract:
We report coherent X-ray imaging of antiferromagnetic (AFM) domains and domain walls in MnBi$_2$Te$_4$, an intrinsic AFM topological insulator. This technique enables direct visualization of domain morphology without reconstruction algorithms, allowing us to resolve antiphase domain walls as distinct dark lines arising from the A-type AFM structure. The wall width is determined to be 550(30) nm, i…
▽ More
We report coherent X-ray imaging of antiferromagnetic (AFM) domains and domain walls in MnBi$_2$Te$_4$, an intrinsic AFM topological insulator. This technique enables direct visualization of domain morphology without reconstruction algorithms, allowing us to resolve antiphase domain walls as distinct dark lines arising from the A-type AFM structure. The wall width is determined to be 550(30) nm, in good agreement with earlier magnetic force microscopy results. The temperature dependence of the AFM order parameter extracted from our images closely follows previous neutron scattering data. Remarkably, however, we find a pronounced hysteresis in the evolution of domains and domain walls: upon cooling, dynamic reorganizations occur within a narrow $\sim$1 K interval below $T_N$, whereas upon warming, the domain configuration remains largely unchanged until AFM order disappears. These findings reveal a complex energy landscape in MnBi$_2$Te$_4$, governed by the interplay of exchange, anisotropy, and domain-wall energies, and underscore the critical role of AFM domain-wall dynamics in shaping its physical properties.
△ Less
Submitted 24 October, 2025;
originally announced October 2025.
-
Chemical States and Local Structure in Cu-Deficient CuInSe2 Thin Films: Insights into Engineering and Bandgap Narrowing
Authors:
Ahmed Yousef Mohamed,
Byoung Gun Han,
Hyeonseo Jang,
Jun Oh Jeon,
Yejin Kim,
Haeseong Jang,
Min Gyu Kim,
Kug-Seung Lee,
Deok-Yong Cho
Abstract:
The Cu-deficient CuxInSe2 (x larger than 0.3) phase can be stabilized as a thin film. A uniform Cu-deficient composition with a chalcopyrite structure was obtained by the precision engineering of a two-step synthesis process involving electron-beam evaporation and Se vapor deposition. Detailed structural and chemical analyses were performed employing various X-ray and microscopic techniques to dem…
▽ More
The Cu-deficient CuxInSe2 (x larger than 0.3) phase can be stabilized as a thin film. A uniform Cu-deficient composition with a chalcopyrite structure was obtained by the precision engineering of a two-step synthesis process involving electron-beam evaporation and Se vapor deposition. Detailed structural and chemical analyses were performed employing various X-ray and microscopic techniques to demonstrate that the chemical states and local structure in the Cu-Se-In tetrahedral networks change with the loss of Cu, the In-Se bond becomes shorter, and the In ions become excessively oxidized without phase separation. Moreover, the results indicate that the bandgap narrowing is primarily attributed to the reconstruction of In3+d 5s orbital states. The bandgap narrows from 1.51 eV to 1.4 eV, which is optimal for the photon absorber. Therefore, cation-deficient selenide is promising for stable nontoxic photovoltaics with tunable bandgaps.
△ Less
Submitted 21 October, 2025;
originally announced October 2025.
-
Thermal transport in GaN/AlN HEMTs on 4H-SiC: Role of layer thickness and hetero-interfaces
Authors:
Dat Q. Tran,
Minho Kim,
Okhyun Nam,
Vanya Darakchieva,
Plamen P. Paskov
Abstract:
Thermal transport in high-electron-mobility-transistor (HEMT) structures grown on 4H-SiC substrates by metalorganic-vapour-phase epitaxy (MOCVD) is systematically investigated. The thermal conductivity of the GaN channel and AlN buffer layers is measured by thermoreflectance (TTR). A pronounced thickness dependence of thermal conductivity as a result of phonon-boundary scattering is observed at lo…
▽ More
Thermal transport in high-electron-mobility-transistor (HEMT) structures grown on 4H-SiC substrates by metalorganic-vapour-phase epitaxy (MOCVD) is systematically investigated. The thermal conductivity of the GaN channel and AlN buffer layers is measured by thermoreflectance (TTR). A pronounced thickness dependence of thermal conductivity as a result of phonon-boundary scattering is observed at low temperatures, while this effect becomes significantly weaker at elevated temperatures. The thermal boundary resistance (TBR) at the AlN/4H-SiC and GaN/AlN interfaces is also examined, showing a substantial reduction and eventual saturation with increasing temperature, indicating elastic phonon transport as the dominant mechanism. Reliable simulations of the temperature profile across the structures based on the measured thermal metrics highlight the critical role of TBR in thin-channel device and the advantage of thicker channel and buffer layers for efficient heat dissipation in the HEMTs.
△ Less
Submitted 13 October, 2025;
originally announced October 2025.
-
Co-evaporated Formamidinium tin triiodide with suppressed p-type self-doping
Authors:
Junhyoung Park,
Andrea Olivati,
Mirko Prato,
Min Kim,
Annamaria Petrozza
Abstract:
Co-evaporation of formamidinium tin triiodide (FASnI3) precursors, without any additives or reducing agents, leads to the growth of a highly crystalline thin film which shows a bandgap around 1.31 eV, closely matching the theoretical value predicted from the ideal single crystal structure of FASnI3. The polycrystalline thin film presents a lower tendency of Sn2+ to Sn4+ oxidation and highly reduce…
▽ More
Co-evaporation of formamidinium tin triiodide (FASnI3) precursors, without any additives or reducing agents, leads to the growth of a highly crystalline thin film which shows a bandgap around 1.31 eV, closely matching the theoretical value predicted from the ideal single crystal structure of FASnI3. The polycrystalline thin film presents a lower tendency of Sn2+ to Sn4+ oxidation and highly reduced tendency to self-doping, demonstrating, overall, an improved resistance to defects formation. These findings suggest solvent-free co-evaporation processes as a promising route for high quality Sn-based perovskite polycrystalline thin films.
△ Less
Submitted 7 October, 2025;
originally announced October 2025.
-
Layer controlled orbital selective Mott transition in monolayer nickelate
Authors:
Byungmin Sohn,
Minjae Kim,
Sangjae Lee,
Wenzheng Wei,
Juan Jiang,
Fengmiao Li,
Sergey Gorovikov,
Marta Zonno,
Tor Pedersen,
Sergey Zhdanovich,
Ying Liu,
Huikai Cheng,
Ke Zou,
Yu He,
Sohrab Ismail-Beigi,
Frederick J. Walker,
Charles H. Ahn
Abstract:
Dimensionality and electronic correlations are crucial elements of many quantum material properties. An example is the change of the electronic structure accompanied by the loss of quasiparticles when a metal is reduced from three dimensions to a lower dimension, where the Coulomb interaction between carriers becomes poorly screened. Here, using angle-resolved photoemission spectroscopy (ARPES), w…
▽ More
Dimensionality and electronic correlations are crucial elements of many quantum material properties. An example is the change of the electronic structure accompanied by the loss of quasiparticles when a metal is reduced from three dimensions to a lower dimension, where the Coulomb interaction between carriers becomes poorly screened. Here, using angle-resolved photoemission spectroscopy (ARPES), we report an orbital-selective decoherence of spectral density in the perovskite nickelate LaNiO3 towards the monolayer limit. The spectral weight of the dz2 band vanishes much faster than that of the dx2-y2 band as the thickness of the LaNiO3 layer is decreased to a single unit cell, indicating a stronger correlation effect for the former upon dimensional confinement. Dynamical mean-field theory (DMFT) calculations show an orbital-selective Mott transition largely due to the localization of dz2 electrons along the c axis in the monolayer limit. This orbital-selective correlation effect underpins many macroscopic properties of nickelates, such as metal-to-insulator transition and superconductivity, where most theories are built upon a dx2-y2-dz2 two-band model.
△ Less
Submitted 23 September, 2025;
originally announced September 2025.