Showing 1–50 of 89 results for author: Wang, E

Emergent Chiral Spin Crystal Phase in (111) SrRuO3 Thin Films

Authors: Zhaoqing Ding, Yongjie Xie, Xuejiao Chen, Sheng Wang, Zhen Wang, Zeguo Lin, Enling Wang, Xiaofeng Wu, Mingyu Yang, Yuelong Xiong, Meng Meng, Fang Yang, Jiandi Zhang, Xianggang Qiu, XIaoran Liu, Jiandong Guo

Abstract: Perovskite ruthenates are fascinating playgrounds for exploring topological spin textures, but generally rely on extrinsic mechanisms to trigger the noncoplanar states. Here we report the discovery of an emergent chiral spin crystal phase in (111) SrRuO3 epitaxial films, characterized by a significant topological Hall effect and noncoplanar spin arrangements with different propagation vectors alon… ▽ More Perovskite ruthenates are fascinating playgrounds for exploring topological spin textures, but generally rely on extrinsic mechanisms to trigger the noncoplanar states. Here we report the discovery of an emergent chiral spin crystal phase in (111) SrRuO3 epitaxial films, characterized by a significant topological Hall effect and noncoplanar spin arrangements with different propagation vectors along two orthogonal directions. Instead of driven by the enhanced Dzyaloshinskii-Moriya interaction due to broken inversion symmetry at heterointerfaces, this emergent state arises intrinsically from the interplay of dipolar interactions and magnetic frustration, leading to the stabilization of topological phases in much thicker films. These findings open a new pathway for creating and controlling the topological spin states in perovskites, with broad implications for spintronic device design. △ Less

Submitted 2 December, 2025; originally announced December 2025.

Elucidating the Inter-system Crossing of the Nitrogen-Vacancy Center up to Megabar Pressures

Authors: Benchen Huang, Srinivas V. Mandyam, Weijie Wu, Bryce Kobrin, Prabudhya Bhattacharyya, Yu Jin, Bijuan Chen, Max Block, Esther Wang, Zhipan Wang, Satcher Hsieh, Chong Zu, Christopher R. Laumann, Norman Y. Yao, Giulia Galli

Abstract: The integration of Nitrogen-Vacancy color centers into diamond anvil cells has opened the door to quantum sensing at megabar pressures. Despite a multitude of experimental demonstrations and applications ranging from quantum materials to geophysics, a detailed microscopic understanding of how stress affects the NV center remains lacking. In this work, using a combination of first principles calcul… ▽ More The integration of Nitrogen-Vacancy color centers into diamond anvil cells has opened the door to quantum sensing at megabar pressures. Despite a multitude of experimental demonstrations and applications ranging from quantum materials to geophysics, a detailed microscopic understanding of how stress affects the NV center remains lacking. In this work, using a combination of first principles calculations as well as high-pressure NV experiments, we develop a complete description of the NV's optical properties under general stress conditions. In particular, our ab initio calculations reveal the complex behavior of the NV's inter-system crossing rates under stresses that both preserve and break the defect's symmetry. Crucially, our proposed framework immediately resolves a number of open questions in the field, including: (i) the microscopic origin of the observed contrast-enhancement in (111)-oriented anvils, and (ii) the surprising observation of NV contrast-inversion in certain high-pressure regimes. Our work lays the foundation for optimizing the performance of NV high-pressure sensors by controlling the local stress environment, and more generally, suggests that symmetry-breaking stresses can be utilized as a novel tuning knob for generic solid-state spin defects. △ Less

Submitted 25 November, 2025; originally announced November 2025.

Structure and stability of 7:3 rare earth oxide-phosphates: a combined ab initio and experimental study

Authors: Ligen Wang, Konrad Burkmann, Sergey V. Ushakov, Edric X. Wang, Jared Matteucci, Mara Scheuermann, Erik Melnitschuk, Robert Glaum, Hongwu Xu, Elizabeth J. Opila, Alexandra Navrotsky, Qi-Jun Hong

Abstract: Rare earth oxide-phosphates (REOPs) form a largely unexplored family of refractory lanthanides and yttrium compounds with general formula RExOy(PO4)z. They are of interest for applications ranging from thermal barrier coatings to catalysts and magnetic materials. At least four REOPs phases were experimentally identified with RE/P ratios from 7:3 to 6:1, however the structures were solved only for… ▽ More Rare earth oxide-phosphates (REOPs) form a largely unexplored family of refractory lanthanides and yttrium compounds with general formula RExOy(PO4)z. They are of interest for applications ranging from thermal barrier coatings to catalysts and magnetic materials. At least four REOPs phases were experimentally identified with RE/P ratios from 7:3 to 6:1, however the structures were solved only for 3:1 phases (RE3O3(PO4)). In this work we report the structure for the 7:3 phases (RE7O6(PO4)3) derived by ab initio analysis of models based on previously reported oxide-vanadate analogues. The most stable structures for all 7:3 REOPs were found to be isotypic, adopting monoclinic symmetry with space group P21/c. The structures were validated by comparison of their powder X-ray diffraction patterns to those of synthesized La, Pr, Nd, Sm, Eu, Gd and Tb 7:3 phases (Rietveld refinement for all except Tb). Ab initio analysis of thermodynamic stability showed that all 7:3 REOPs are unstable at 0 K toward decomposition to REPO4 and RE3PO7 or RE2O3. The entropy contribution stabilizes RE7O6(PO4)3 phases for light rare earth elements above 1000 K, however, starting with Dy, computationally predicted stabilization temperature is higher than estimated melting points of RE7O6(PO4)3, which is consistent with observed synthesis pattern. △ Less

Submitted 21 October, 2025; v1 submitted 18 October, 2025; originally announced October 2025.

Uncovering origins of heterogeneous superconductivity in La$_3$Ni$_2$O$_7$ using quantum sensors

Authors: Srinivas V. Mandyam, Esther Wang, Zhipan Wang, Bijuan Chen, Nishan C. Jayarama, Anmay Gupta, Eric A. Riesel, Valery I. Levitas, Christopher R. Laumann, Norman Y. Yao

Abstract: The family of nickelate superconductors have long been explored as analogs of the high temperature cuprates. Nonetheless, the recent discovery that certain stoichiometric nickelates superconduct up to high $T_c$ under pressure came as a surprise. The mechanisms underlying the superconducting state remain experimentally unclear. In addition to the practical challenges posed by working in a high pre… ▽ More The family of nickelate superconductors have long been explored as analogs of the high temperature cuprates. Nonetheless, the recent discovery that certain stoichiometric nickelates superconduct up to high $T_c$ under pressure came as a surprise. The mechanisms underlying the superconducting state remain experimentally unclear. In addition to the practical challenges posed by working in a high pressure environment, typical samples exhibit anomalously weak diamagnetic responses, which have been conjectured to reflect inhomogeneous `filamentary' superconducting states. We perform wide-field, high-pressure, optically detected magnetic resonance spectroscopy to image the local diamagnetic responses of as grown La$_3$Ni$_2$O$_7$ samples \emph{in situ}, using nitrogen vacancy quantum sensors embedded in the diamond anvil cell. These maps confirm significant inhomogeneity of the functional superconducting responses at the few micron scale. By spatially correlating the diamagnetic Meissner response with both the local tensorial stress environment, also imaged \emph{in situ}, and stoichiometric composition, we unravel the dominant mechanisms suppressing and enhancing superconductivity. Our wide-field technique simultaneously provides a broad view of sample behavior and excellent local sensitivity, enabling the rapid construction of multi-parameter phase diagrams from the local structure-function correlations observed at the sub-micron pixel scale. △ Less

Submitted 16 December, 2025; v1 submitted 2 October, 2025; originally announced October 2025.

Quantifying the reactivity of isolated LixSi domains in Si anodes using operando NMR

Authors: Evelyna Wang, Marco-Tulio F. Rodrigues, Baris Key

Abstract: The use of Si anodes can greatly improve the energy density of Li-ion batteries. However, understanding and mitigation of calendar aging remains a barrier to commercialization. In this short report, we utilize operando Nuclear Magnetic Resonance (NMR) spectroscopy to detect and quantify lithium silicides (LixSi) as they form and react within Si anodes in pouch cells during calendar aging. We provi… ▽ More The use of Si anodes can greatly improve the energy density of Li-ion batteries. However, understanding and mitigation of calendar aging remains a barrier to commercialization. In this short report, we utilize operando Nuclear Magnetic Resonance (NMR) spectroscopy to detect and quantify lithium silicides (LixSi) as they form and react within Si anodes in pouch cells during calendar aging. We provide direct experimental evidence of complex aging phenomena in the Si anodes, including both SEI growth and dissolution during storage. Formation of electrochemically isolated LixSi is also observed, as indicated by the partial persistence of highly lithiated phases after the cell is discharged. Remarkably, we show that these isolated domains can themselves self-discharge over time, suggesting that their detection can be challenging in post-mortem studies. Finally, we show that aging outcomes depend heavily on the type of silicon particles contained within the electrode, and that certain surface coatings can help decrease the reactivity between lithium silicides and the electrolyte. △ Less

Submitted 22 September, 2025; originally announced September 2025.

Building high-energy silicon-containing batteries using off-the-shelf materials

Authors: Marco-Tulio F. Rodrigues, Stephen E. Trask, Alison R. Dunlop, Yi-Chen Lan, Joseph Kubal, Devashish Salpekar, Andressa Y. R. Prado, Evelyna Wang, Charles McDaniel, Eliot F. Woods, Lily A. Robertson, Ryan J. Tancin, Maxwell C. Schulze, Nicolas Folastre, Baris Key, Zhengcheng Zhang, Wenquan Lu, Daniel P. Abraham, Andrew N. Jansen

Abstract: The technology of silicon anodes appears to be reaching maturity, with high-energy Si cells already in pilot-scale production. However, the performance of these systems can be difficult to replicate in academic settings, making it challenging to translate research findings into solutions that can be implemented by the battery industry. Part of this difficulty arises from the lack of access to engi… ▽ More The technology of silicon anodes appears to be reaching maturity, with high-energy Si cells already in pilot-scale production. However, the performance of these systems can be difficult to replicate in academic settings, making it challenging to translate research findings into solutions that can be implemented by the battery industry. Part of this difficulty arises from the lack of access to engineered Si particles and anodes, as electrode formulations and the materials themselves have become valuable intellectual property for emerging companies. Here, we summarize the efforts by Argonne's Cell Analysis, Modeling, and Prototyping (CAMP) Facility in developing Si-based prototypes made entirely from commercially available materials. We describe the many challenges we encountered when testing high-loading electrodes (> 5 mAh/cm2) and discuss strategies to mitigate them. With the right electrode and electrolyte design, we show that our pouch cells containing > 70 wt% SiOx can achieve 600-1,000 cycles at C/3 and meet projected energy targets of 700 Wh/L and 350 Wh/kg. These results provide a practical reference for research teams seeking to advance silicon-anode development using accessible materials. △ Less

Submitted 18 September, 2025; originally announced September 2025.

Gradient-based search of quantum phases: discovering unconventional fractional Chern insulators

Authors: André Grossi Fonseca, Eric Wang, Sachin Vaidya, Patrick J. Ledwith, Ashvin Vishwanath, Marin Soljačić

Abstract: The discovery and understanding of new quantum phases has time and again transformed both fundamental physics and technology, yet progress often relies on slow, intuition-based theoretical considerations or experimental serendipity. Here, we introduce a general gradient-based framework for targeted phase discovery. We define a differentiable function, dubbed "target-phase loss function", which enc… ▽ More The discovery and understanding of new quantum phases has time and again transformed both fundamental physics and technology, yet progress often relies on slow, intuition-based theoretical considerations or experimental serendipity. Here, we introduce a general gradient-based framework for targeted phase discovery. We define a differentiable function, dubbed "target-phase loss function", which encodes spectral fingerprints of a quantum state, thereby recasting phase search as a tractable optimization problem in Hamiltonian space. The method is broadly applicable to phases characterized by ground-state degeneracy and can be extended to a wide range of symmetry-broken and topological orders. As a demonstration, we apply it to spinless fermions on the kagome lattice and discover two distinctive fractional Chern insulators (FCIs), verified through detailed exact diagonalization: (i) at filling $ν= 1/3$, a "non-ideal" Abelian FCI whose band geometry lies far beyond the Landau-level mimicry paradigm and all recent generalizations; and (ii) at $ν= 1/2$, a non-Abelian FCI stabilized purely by finite-range two-body interactions. These results provide the first explicit realization of such types of FCIs and establish a versatile paradigm for systematic quantum-phase discovery. △ Less

Submitted 12 September, 2025; originally announced September 2025.

Phase-matching of high harmonic generation in twisted solids

Authors: Chenjun Ma, Chen Huang, Yilong You, Huazhan Liu, Zhitong Ding, Mingchao Ding, Jin Zhang, Guixin Li, Zhipei Sun, Shiwei Wu, Chaojie Ma, Enge Wang, Hao Hong, Kaihui Liu

Abstract: High harmonic generation (HHG) in solids could enable attosecond and ultraviolet light sources with high compactness, great controllability and rich functions. However, the HHG process is accompanied by a quite large wavevector mismatch that is uncompensated by any traditional phase-matching method, directly limiting its energy conversion efficiency. Here, we propose an effective strategy for phas… ▽ More High harmonic generation (HHG) in solids could enable attosecond and ultraviolet light sources with high compactness, great controllability and rich functions. However, the HHG process is accompanied by a quite large wavevector mismatch that is uncompensated by any traditional phase-matching method, directly limiting its energy conversion efficiency. Here, we propose an effective strategy for phase-matching of HHG with arbitrary harmonic orders in solids. Two flakes of solids with an interlayer twist induce a nonlinear optical phase that depends on the crystal symmetry, twist angle and harmonic order, which can be accurately designed to compensate for the phase mismatch in HHG. Guided by the twist-phase-matching theory, we achieved a record-high conversion efficiency of $~1.5\times10^{-5}$ for the fifth HHG in twisted hexagonal boron nitride crystals with a total thickness of only 1 $μm$. Our work establishes a foundation for developing ultrashort-wavelength and ultrafast-pulse laser sources in compact solid-state tabletop systems for fundamental and applied sciences. △ Less

Submitted 11 March, 2025; originally announced March 2025.

Observation of liquid-solid transition of nanoconfined water at ambient temperature

Authors: Wentian Zheng, Shichen Zhang, Jian Jiang, Yipeng He, Rainer Stöhr, Andrej Denisenko, Jörg Wrachtrup, Xiao Cheng Zeng, Ke Bian, En-Ge Wang, Ying Jiang

Abstract: Nanoconfined water plays an indispensable role in various phenomena in biology, chemistry, and engineering. It exhibits many abnormal properties compared to bulk water, especially under strong confinement. However, the origin of those anomalies is still elusive due to the lack of structural information on hydrogen-bonding networks. Considering the inhomogeneity of the nanocavity and the tiny amoun… ▽ More Nanoconfined water plays an indispensable role in various phenomena in biology, chemistry, and engineering. It exhibits many abnormal properties compared to bulk water, especially under strong confinement. However, the origin of those anomalies is still elusive due to the lack of structural information on hydrogen-bonding networks. Considering the inhomogeneity of the nanocavity and the tiny amount of water molecules, conventional optical spectroscopies and nuclear magnetic resonance (NMR) fail to realize the structure analysis of nanoconfined water. Here, we addressed this issue by combining scanning probe microscopy (SPM) with advanced quantum sensing(QS) based on an atomic-size quantum sensor like nitrogen-vacancy (NV) center in diamond, which can apply the nanoscale-NMR for characterizing both the dynamics and structure of confined water at ambient conditions. We built a two-dimensional (2D) nanoconfined water system with a hexagonal-boron nitride (hBN) flake and a hydrophilic diamond surface. By using the SPM tip to measure the confinement size precisely, we observed a critical confinement size of ~2 nm, below which the water diffusion was significantly suppressed and the hydrogen-bonding network of water showed an ordered structure. Meanwhile, molecular dynamics (MD) simulation revealed a solid-like water contact layer on the diamond surface under strong confinement, which also reproduced the measured nanoscale-NMR spectra and confirmed the liquid-solid phase transition observed in the experiments. Notably, with this new SPM-QS platform, our results showed a promising way to elucidate the abnormal properties of nanoconfined water in future applications. △ Less

Submitted 19 December, 2024; originally announced December 2024.

Computational investigation of formation enthalpies and phase stability for rare earth oxyphosphates

Authors: Edric X. Wang, Ligen Wang, Qi-Jun Hong

Abstract: Rare earth phosphates have garnered significant interest due to their versatile properties, including high chemical stability, thermal resistance, luminescence, and the ability to adopt various crystalline structures. Density functional theory (DFT)-based ab initio methods have become essential tools for complementing experimental studies. In this paper, we performed DFT calculations on rare earth… ▽ More Rare earth phosphates have garnered significant interest due to their versatile properties, including high chemical stability, thermal resistance, luminescence, and the ability to adopt various crystalline structures. Density functional theory (DFT)-based ab initio methods have become essential tools for complementing experimental studies. In this paper, we performed DFT calculations on rare earth (RE; here considered as lanthanides + Y) oxyphosphates to examine their formation enthalpies and phase stability. The calculations were conducted using the GGA-PBE and r2SCAN exchange-correlation functionals. Our results indicate that both functionals predict similar phase stabilities for REPO4 and RE3PO7. However, the r2SCAN functional provides significantly more accurate formation enthalpies for the monazite and xenotime REPO4, aligning closely with experimental data. Furthermore, the inclusion of lattice vibrational entropy enhances the free energy predictions, leading to improved agreement with experimental observations on phase stability. △ Less

Submitted 1 November, 2024; originally announced November 2024.

Higher-Order Van Hove Singularities in Kagome Topological Bands

Authors: Edrick Wang, Lakshmi Pullasseri, Luiz H. Santos

Abstract: Motivated by the growing interest in band structures featuring higher-order Van Hove singularities (HOVHS), we investigate a spinless fermion kagome system characterized by nearest-neighbor (NN) and next-nearest-neighbor (NNN) hopping amplitudes. While NN hopping preserves time-reversal symmetry, NNN hopping, akin to chiral hopping on the Haldane lattice, breaks time-reversal symmetry and leads to… ▽ More Motivated by the growing interest in band structures featuring higher-order Van Hove singularities (HOVHS), we investigate a spinless fermion kagome system characterized by nearest-neighbor (NN) and next-nearest-neighbor (NNN) hopping amplitudes. While NN hopping preserves time-reversal symmetry, NNN hopping, akin to chiral hopping on the Haldane lattice, breaks time-reversal symmetry and leads to the formation of topological bands with Chern numbers ranging from $C = \pm 1$ to $ \pm 4$. We perform analytical and numerical analysis of the energy bands near the high-symmetry points $\boldsymbolΓ$, $\pm \boldsymbol{K}$, and $\boldsymbol{M_i}$ ($i=1,2,$ and $3$), which uncover a rich and complex landscape of HOVHS, controlled by the magnitude and phase of the NNN hopping. We observe power-law divergences in the density of states (DOS), $ρ(ε) \sim |ε|^{-ν}$, with exponents $ν= 1/2, 1/3, 1/4$, which can significantly affect the anomalous Hall response at low temperatures when the Fermi level crosses the HOVHS. Additionally, the NNN hopping induces the formation of higher Chern number bands $C = \pm 2, \pm 4$ in the middle of the spectrum obeying a sublattice interference whereupon electronic states are maximally localized in each of the sublattices when the momentum approaches the three high-symmetry points $\boldsymbol{M_i}$ ($i=1,2,$ and $3$) on the Brillouin zone boundary. This classification of HOVHS in kagome systems provides a platform to explore unconventional electronic orders induced by electronic correlations. △ Less

Submitted 8 February, 2025; v1 submitted 9 October, 2024; originally announced October 2024.

Comments: 11 pages, 7 figures

Journal ref: E. Wang, L. Pullasseri, and L. H. Santos, Higher-order Van-Hove singularities in kagome topological bands, Phys. Rev. B 111, 075114 (2025)

Intrinsic Orbital Origin for the Chirality-Dependent Nonlinear Planar Hall Effect of Topological Nodal Fermions in Chiral Crystals

Authors: Mingxiang Pan, Hui Zeng, Erqing Wang, Huaqing Huang

Abstract: Topological semimetals in chiral crystals, which possess both structural handedness and band crossings (or nodes) with topological chiral charge, exhibit many exotic physical properties. Here we demonstrate that the structural and electronic chirality of these systems can endow them with another fascinating phenomenon -- the intrinsic nonlinear planar Hall effect (INPHE), which is prominent around… ▽ More Topological semimetals in chiral crystals, which possess both structural handedness and band crossings (or nodes) with topological chiral charge, exhibit many exotic physical properties. Here we demonstrate that the structural and electronic chirality of these systems can endow them with another fascinating phenomenon -- the intrinsic nonlinear planar Hall effect (INPHE), which is prominent around the nodes and reverses sign upon chirality reversal in opposite enantiomers. Taking chiral tellurium as an example, we reveal an intrinsic orbital mechanism, which manifests diverging orbital magnetic moments with hedgehog-like textures around nodes and, therefore, generates a dominant contribution to the INPHE that is proportional to the topological charge. Furthermore, we show that multifold fermions in topological chiral semimetals with B20 structures (e.g., CoSi and PtAl) induce a giant INPHE conductivity reaching the order of $1\sim 10\; \mathrm{A}\cdot\mathrm{V}^{-2}\cdot\mathrm{T}^{-1}$, which is detectable in experiments. Our study not only relates nonlinear transport to band topology and enantiomer recognition but also offers a new way to explore the exotic physical properties associated with unconventional chiral fermions. △ Less

Submitted 13 May, 2024; originally announced May 2024.

Journal ref: Phys. Rev. B 111, 075145 (2025)

Surface termination effect of SrTiO3 substrate on ultrathin SrRuO3

Authors: Huiyu Wang, Zhen Wang, Zeeshan Ali, Enling Wang, Mohammad Saghayezhian, Jiandong Guo, Yimei Zhu, Jing Tao, Jiandi Zhang

Abstract: A uniform one-unit-cell-high step on the SrTiO3 substrate is a prerequisite for growing high-quality epitaxial oxide heterostructures. However, it is inevitable that defects induced by mixed substrate surface termination exist at the interface, significantly impacting the properties of ultrathin films. In this study, we microscopically identify the origin for the lateral inhomogeneity in the growt… ▽ More A uniform one-unit-cell-high step on the SrTiO3 substrate is a prerequisite for growing high-quality epitaxial oxide heterostructures. However, it is inevitable that defects induced by mixed substrate surface termination exist at the interface, significantly impacting the properties of ultrathin films. In this study, we microscopically identify the origin for the lateral inhomogeneity in the growth of ultrathin SrRuO3 films due to the step effects of SrTiO3(001). By using atomic-resolved scanning transmission electron microscopy, we observe two distinct types of step propagation along the [011] and [0-11]crystallographic direction in SrTiO3-SrRuO3 heterostructures, respectively. In particular, the type-II [0-11] step results in lateral discontinuity of monolayer SrRuO3 and originates from the SrO-terminated regions along the TiO2-terminated step edge. Such an induced lateral discontinuity should be responsible for the distinct electronic and magnetic properties of monolayer SrRuO3. Our findings underscore the critical importance of using single termination STO substrate to achieve high-quality termination selective films and to unveil the intrinsic properties of epitaxial films in the atomic limit. △ Less

Submitted 6 December, 2023; originally announced December 2023.

Comments: 19 pages, 10 figures, 30 references

Probing photo-induced granular superconductivity in K$_{3}$C$_{60}$ thin films with an ultrafast on-chip voltmeter

Authors: Joseph D. Adelinia, Eryin Wang, Mariana Chavez-Cervantes, Toru Matsuyama, Michael Fechner, Michele Buzzi, Guido Meier, Andrea Cavalleri

Abstract: The physics of optically-induced superconductivity remains poorly understood, with questions that range from the underlying microscopic mechanism to the macroscopic electrical response of the non-equilibrium phase. In this paper, we study optically-induced superconductivity in K$_{3}$C$_{60}$ thin films, which display signatures of granularity both in the equilibrium state below T$_{c}$ and in the… ▽ More The physics of optically-induced superconductivity remains poorly understood, with questions that range from the underlying microscopic mechanism to the macroscopic electrical response of the non-equilibrium phase. In this paper, we study optically-induced superconductivity in K$_{3}$C$_{60}$ thin films, which display signatures of granularity both in the equilibrium state below T$_{c}$ and in the nonequilibrium photo-induced phase above T$_{c}$. Photo-conductive switches are used to measure the ultrafast voltage drop across a K$_{3}$C$_{60}$ film as a function of time after irradiation, both below and above T$_{c}$. These measurements reveal fast changes associated with the kinetic inductance of in-grain superconductivity, and a slower response attributed to the Josephson dynamics at the weak links. Fits to the data yield estimates of the in-grain photo-induced superfluid density after the drive and the dynamics of phase slips at the weak links. This work underscores the increasing ability to make electrical measurements at ultrafast speeds in optically-driven quantum materials, and demonstrates a striking new platform for optoelectronic device applications. △ Less

Submitted 11 December, 2023; originally announced December 2023.

Observing periodic gap variations in cuprates

Authors: Riju Banerjee, Emily L. Wang, Eric W. Hudson

Abstract: Central to the enigma of the cuprates is ubiquitous electronic inhomogeneity arising from a variety of electronic orders that coexist with superconductivity, the individual signatures of which have been impossible to disentangle despite four decades of intense research. This strong nanoscale inhomogeneity complicates interpretation of measurements both by probes which average over this inhomogenei… ▽ More Central to the enigma of the cuprates is ubiquitous electronic inhomogeneity arising from a variety of electronic orders that coexist with superconductivity, the individual signatures of which have been impossible to disentangle despite four decades of intense research. This strong nanoscale inhomogeneity complicates interpretation of measurements both by probes which average over this inhomogeneity and those, like scanning tunneling microscopy (STM), which should be able to spatially resolve variations driven by both order and inhomogeneity. Here, we develop a novel technique that directly acknowledges this electronic inhomogeneity and extracts statistically significant features from scanning tunneling spectroscopic data. Applying our novel technique to single and bilayer Bi-based cuprates spanning a large doping range, we peer through local inhomogeneities and find that the gap breaks translational and rotational symmetries and varies periodically in a four-fold pattern. Our direct observation of a symmetry breaking gap in the single particle tunneling spectra adds strong credence to the pair density wave hypotheses supposed to exist in these materials. We also discuss various implications of our observations and, in particular, how they can explain the origin of the low energy checkerboard pattern. △ Less

Submitted 31 October, 2023; originally announced November 2023.

Comments: 9 pages, 4 figures and supplementary sections

Giant nonlinear optical wave mixing in van der Waals compound MnPSe3

Authors: Li Yue, Chang Liu, Shanshan Han, Hao Hong, Yijun Wang, Qiaomei Liu, Jiajie Qi, Yuan Li, Dong Wu, Kaihui Liu, Enge Wang, Tao Dong, Nanlin Wang

Abstract: Optical nonlinearities, one of the most fascinating properties of two-dimensional (2D) materials, are essential for exploring novel physics in 2D systems and developing next-generation nonlinear optical applications. While tremendous efforts have been made to discover and optimize second-order nonlinear optical responses in various 2D materials, higher odd-order nonlinear processes, which are in g… ▽ More Optical nonlinearities, one of the most fascinating properties of two-dimensional (2D) materials, are essential for exploring novel physics in 2D systems and developing next-generation nonlinear optical applications. While tremendous efforts have been made to discover and optimize second-order nonlinear optical responses in various 2D materials, higher odd-order nonlinear processes, which are in general much less efficient than second order ones, have been paid less attention despite their scientific and applicational significance. Here we report giant odd-order nonlinear optical wave mixing in a correlated van der Waals insulator MnPSe3 at room temperature. Illuminated by two near-infrared femtosecond lasers simultaneously, it generates a series of degenerate and non-degenerate four- and six-wave mixing outputs, with conversion efficiencies up to the order of $10^{-4}$ and $10^{-6}$ for the four- and six-wave mixing processes, respectively, far exceeding the efficiencies of several prototypical nonlinear optical materials (GaSe, LiNbO3). This work highlights the intriguing prospect of transition metal phosphorous trichalcogenides for future research of the nonlinear light matter interactions in 2D systems and for potential nonlinear photonic applications. △ Less

Submitted 28 September, 2023; originally announced October 2023.

Comments: 17 pages, 4 figures

Imaging the Meissner effect and flux trapping in a hydride superconductor at megabar pressures using a nanoscale quantum sensor

Authors: Prabudhya Bhattacharyya, Wuhao Chen, Xiaoli Huang, Shubhayu Chatterjee, Benchen Huang, Bryce Kobrin, Yuanqi Lyu, Thomas J. Smart, Maxwell Block, Esther Wang, Zhipan Wang, Weijie Wu, Satcher Hsieh, He Ma, Srinivas Mandyam, Bijuan Chen, Emily Davis, Zachary M. Geballe, Chong Zu, Viktor Struzhkin, Raymond Jeanloz, Joel E. Moore, Tian Cui, Giulia Galli, Bertrand I. Halperin , et al. (2 additional authors not shown)

Abstract: By directly altering microscopic interactions, pressure provides a powerful tuning knob for the exploration of condensed phases and geophysical phenomena. The megabar regime represents an exciting frontier, where recent discoveries include novel high-temperature superconductors, as well as structural and valence phase transitions. However, at such high pressures, many conventional measurement tech… ▽ More By directly altering microscopic interactions, pressure provides a powerful tuning knob for the exploration of condensed phases and geophysical phenomena. The megabar regime represents an exciting frontier, where recent discoveries include novel high-temperature superconductors, as well as structural and valence phase transitions. However, at such high pressures, many conventional measurement techniques fail. Here, we demonstrate the ability to perform local magnetometry inside of a diamond anvil cell with sub-micron spatial resolution at megabar pressures. Our approach utilizes a shallow layer of Nitrogen-Vacancy (NV) color centers implanted directly within the anvil; crucially, we choose a crystal cut compatible with the intrinsic symmetries of the NV center to enable functionality at megabar pressures. We apply our technique to characterize a recently discovered hydride superconductor, CeH$_9$. By performing simultaneous magnetometry and electrical transport measurements, we observe the dual signatures of superconductivity: local diamagnetism characteristic of the Meissner effect and a sharp drop of the resistance to near zero. By locally mapping the Meissner effect and flux trapping, we directly image the geometry of superconducting regions, revealing significant inhomogeneities at the micron scale. Our work brings quantum sensing to the megabar frontier and enables the closed loop optimization of superhydride materials synthesis. △ Less

Submitted 5 June, 2023; originally announced June 2023.

Journal ref: Nature 627, 73-79 (2024)

Comment on arXiv:2210.01114: Optical Saturation Produces Spurious Evidence for Photoinduced Superconductivity in K$_3$C$_{60}$

Authors: M. Buzzi, D. Nicoletti, E. Rowe, E. Wang, A. Cavalleri

Abstract: In the manuscript arXiv:2210.01114, Dodge and co-authors discuss the influence of pump-probe profile deformations on the reconstructed non-equilibrium optical conductivity of K$_3$C$_{60}$. They state that when pump-induced saturation of the probe response is taken into account, the reconstructed optical properties are not superconducting-like, as was claimed in a number of experimental reports by… ▽ More In the manuscript arXiv:2210.01114, Dodge and co-authors discuss the influence of pump-probe profile deformations on the reconstructed non-equilibrium optical conductivity of K$_3$C$_{60}$. They state that when pump-induced saturation of the probe response is taken into account, the reconstructed optical properties are not superconducting-like, as was claimed in a number of experimental reports by our group. We show here that the conclusion reached by Dodge et al. is unjustified. In fact, independent of the specific model, including the problematic saturation profile proposed by the authors, the reconstructed optical properties are those of a finite temperature superconductor. The true fingerprint of superconductivity, which is the $1/ω$ divergence of the imaginary conductivity, $σ_{2}(ω)$, is retained and is virtually independent of the chosen model. The only model-dependent feature is the degree of gapping in $σ_{1}(ω)$. In all cases the extracted optical properties reflect the presence of residual quasiparticles, which at finite temperatures are inevitably present alongside the superfluid. △ Less

Submitted 17 March, 2023; originally announced March 2023.

Comments: 3 pages, 1 figure, comment on arXiv:2210.01114

Nonlinear transport in a photo-induced superconductor

Authors: E. Wang, J. D. Adelinia, M. Chavez-Cervantes, T. Matsuyama, M. Fechner, M. Buzzi, G. Meier, A. Cavalleri

Abstract: Optically driven quantum materials exhibit a variety of non-equilibrium functional phenomena [1-11], which are potentially associated with unique transport properties. However, these transient electrical responses have remained largely unexplored, primarily because of the challenges associated with integrating quantum materials into ultrafast electrical devices. Here, thin films of K3C60 grown by… ▽ More Optically driven quantum materials exhibit a variety of non-equilibrium functional phenomena [1-11], which are potentially associated with unique transport properties. However, these transient electrical responses have remained largely unexplored, primarily because of the challenges associated with integrating quantum materials into ultrafast electrical devices. Here, thin films of K3C60 grown by Molecular Beam Epitaxy were connected by coplanar terahertz waveguides to a series of photo-conductive switches. This geometry enabled ultrafast transport measurements at high current densities, providing new information on the photo-induced phase created in the high temperature metal by mid-infrared excitation [12-16]. Nonlinearities in the current-voltage charactersitics of the transient state validate the assignment of transient superconductivity, and point to an inhomogeneous phase in which superconducting regions of the sample are connected by resistive weak links [17-23]. This work opens up the possibility of systematic transport measurements in driven quantum materials, both to probe their properties and to integrate them into ultrafast optoelectronic platforms. △ Less

Submitted 16 January, 2023; originally announced January 2023.

H$_2$ + H$_2$O -> H$_4$O: Synthesizing Hyper-hydrogenated Water in Small-Sized Fullerenes?

Authors: Endong Wang, Yi Gao

Abstract: Nanoscale confinement provides an ideal platform to rouse some exceptional reactions which cannot happen in the open space. Intuitively, H2 and H$_2$O cannot react. Herein, through utilizing small-sized fullerenes (C$_{24}$, C$_{26}$, C$_{28}$, and C$_{30}$) as nanoreactors, we demonstrate that a hyperhydrogenated water species, H$_4$O, can be easily formed using H2 and H$_2$O under ambient condit… ▽ More Nanoscale confinement provides an ideal platform to rouse some exceptional reactions which cannot happen in the open space. Intuitively, H2 and H$_2$O cannot react. Herein, through utilizing small-sized fullerenes (C$_{24}$, C$_{26}$, C$_{28}$, and C$_{30}$) as nanoreactors, we demonstrate that a hyperhydrogenated water species, H$_4$O, can be easily formed using H2 and H$_2$O under ambient conditions by ab initio molecular dynamics simulations.The H$_4$O molecule rotates freely in the cavity of the cages and maintains its structure during the simulations. Further theoretical analysis indicates that H$_4$O in the fullerene possesses high stability thermodynamically and chemically, which can be rationalized by the electron transfer between H$_4$O and the fullerene. This work highlights the possibility of utilizing fullerene as a nanoreactor to provide confinement constraints for unexpected chemistry. △ Less

Submitted 9 February, 2023; v1 submitted 12 October, 2022; originally announced October 2022.

Comments: This work has been accepted by J. Phys. Chem. A (J. Phys. Chem. A 2023, 127, 5, 1190-1195)

Journal ref: J. Phys. Chem. A 2023, 127, 5, 1190-1195

Phonon transition across an isotopic interface

Authors: Ning Li, Ruochen Shi, Yifei Li, Ruishi Qi, Zhetong Liu, Fachen Liu, Yuehui Li, Xiaowen Zhang, Xiangdong Guo, Kaihui Liu, Ying Jiang, Xin-Zheng Li, Ji Chen, Lei Liu, En-Ge Wang, Peng Gao

Abstract: Natural materials usually consist of isotopic mixtures, for which different isotopic ratios can lead to distinct material properties such as thermal conductivity and nucleation process. However, the knowledge of isotopic interface remains largely unexplored mainly due to the challenges in isotopic identification and property measurement at an atomic scale. Here, by using monochromated electron ene… ▽ More Natural materials usually consist of isotopic mixtures, for which different isotopic ratios can lead to distinct material properties such as thermal conductivity and nucleation process. However, the knowledge of isotopic interface remains largely unexplored mainly due to the challenges in isotopic identification and property measurement at an atomic scale. Here, by using monochromated electron energy-loss spectroscopy in a scanning transmission electron microscope, we reveal momentum-transfer-dependent lattice vibration behavior at an artificial h-10BN/h-11BN heterostructure with sub-unit-cell resolution. We find the vibrational energy changes across the isotopic interface gradually, featuring a wide transition regime, which suggests strong delocalization of the out-of-plane optical phonons at the interface. In addition, we identify phonons near the Brillouin zone center have a transition regime ~3.34 nm (10 atomic layers), whereas phonons at the Brillouin zone boundary transition in ~1.66 nm (5 atomic layers). We propose that the isotope-induced charge effect at the interface accounts for the distinct delocalization behavior. Moreover, intra-atomic layer variation of vibration energy is also sensitive to the momentum transfer, thus at the interface it depends on both of momentum transfer and mass change. The revealed lattice vibration behavior at an isotopic interface provides new insights to understand the isotopic effects on properties in natural materials. △ Less

Submitted 25 September, 2022; originally announced September 2022.

Journal ref: Li, N., Shi, R., Li, Y. et al. Phonon transition across an isotopic interface. Nat Commun 14, 2382 (2023)

Layer-by-layer growth of bilayer graphene single-crystals enabled by self-transmitting catalytic activity

Authors: Zhihong Zhang, Linwei Zhou, Zhaoxi Chen, Antonín Jaroš, Miroslav Kolíbal, Petr Bábor, Quanzhen Zhang, Changlin Yan, Ruixi Qiao, Qing Zhang, Teng Zhang, Wei Wei, Yi Cui, Jingsi Qiao, Liwei Liu, Lihong Bao, Haitao Yang, Zhihai Cheng, Yeliang Wang, Enge Wang, Zhi Liu, Marc Willinger, Hong-Jun Gao, Kaihui Liu, Zhu-Jun Wang , et al. (1 additional authors not shown)

Abstract: Direct growth of large-area vertically stacked two-dimensional (2D) van der Waal (vdW) materials is a prerequisite for their high-end applications in integrated electronics, optoelectronics and photovoltaics. Currently, centimetre- to even metre-scale monolayers of single-crystal graphene (MLG) and hexagonal boron nitride (h-BN) have been achieved by epitaxial growth on various single-crystalline… ▽ More Direct growth of large-area vertically stacked two-dimensional (2D) van der Waal (vdW) materials is a prerequisite for their high-end applications in integrated electronics, optoelectronics and photovoltaics. Currently, centimetre- to even metre-scale monolayers of single-crystal graphene (MLG) and hexagonal boron nitride (h-BN) have been achieved by epitaxial growth on various single-crystalline substrates. However, in principle, this success in monolayer epitaxy seems extremely difficult to be replicated to bi- or few-layer growth, as the full coverage of the first layer was believed to terminate the reactivity of those adopting catalytic metal surfaces. Here, we report an exceptional layer-by-layer chemical vapour deposition (CVD) growth of large size bi-layer graphene single-crystals, enabled by self-transmitting catalytic activity from platinum (Pt) surfaces to the outermost graphene layers. In-situ growth and real-time surveillance experiments, under well-controlled environments, unambiguously verify that the growth does follow the layer-by-layer mode on open surfaces of MLG/Pt(111). First-principles calculations indicate that the transmittal of catalytic activity is allowed by an appreciable electronic hybridisation between graphene overlayers and Pt surfaces, enabling catalytic dissociation of hydrocarbons and subsequently direct graphitisation of their radicals on the outermost sp2 carbon surface. This self-transmitting catalytic activity is also proven to be robust for tube-furnace CVD in fabricating single-crystalline graphene bi-, tri- and tetra-layers, as well as h-BN few-layers. Our findings offer an exceptional strategy for potential controllable, layer-by-layer and wafer-scale growth of vertically stacked few-layered 2D single crystals. △ Less

Submitted 3 May, 2022; originally announced May 2022.

Comments: 5 figures and 9 extended figures

Thermodynamic descriptors to predict oxide formation in aqueous solutions

Authors: Lauren N. Walters, Emily L. Wang, James M. Rondinelli

Abstract: We formulate the maximum driving force (MDF) parameter as a descriptor to capture the thermodynamic stability of aqueous surface scale creation over a range of environmental conditions. We use formation free energies, $Δ_f G$s, sourced from high-throughput density functional theory (DFT) calculations and experimental databases to compute the maximum driving force for a wide variety of materials, i… ▽ More We formulate the maximum driving force (MDF) parameter as a descriptor to capture the thermodynamic stability of aqueous surface scale creation over a range of environmental conditions. We use formation free energies, $Δ_f G$s, sourced from high-throughput density functional theory (DFT) calculations and experimental databases to compute the maximum driving force for a wide variety of materials, including simple oxides, intermetallics, and alloys of varying compositions. We show how to use the MDF to describe trends in aqueous corrosion of nickel thin films determined from experimental linear-sweep-voltometry data. We also show how to account for subsurface oxidation behavior using depth-dependent effective chemical potentials. We anticipate this approach will increase overall understanding of oxide formation on chemically complex multielement alloys, where competing oxide phases can form during transient aqueous corrosion. △ Less

Submitted 21 March, 2022; originally announced March 2022.

Comments: 7 pages, 3 figures

Journal ref: J. Phys. Chem. Lett. 13, 6236-6243 (2022)

Heteroepitaxy of Large-Area, Monocrystalline Lead Halide Perovskite Films on Gallium Arsenide

Authors: Deying Kong, Yu Zhang, Dali Cheng, Enze Wang, Kaiyuan Zhang, Huachun Wang, Kai Liu, Lan Yin, Xing Sheng

Abstract: Lead halide perovskite materials have been emerging as promising candidates for high-performance optoelectronic devices. Significant efforts have sought to realize monocrystalline perovskite films at a large scale. Here, we epitaxially grow monocrystalline methylammonium lead tribromide (MAPbBr3) films on lattice-matched gallium arsenide (GaAs) substrates at a centimeter scale. In particular, a so… ▽ More Lead halide perovskite materials have been emerging as promising candidates for high-performance optoelectronic devices. Significant efforts have sought to realize monocrystalline perovskite films at a large scale. Here, we epitaxially grow monocrystalline methylammonium lead tribromide (MAPbBr3) films on lattice-matched gallium arsenide (GaAs) substrates at a centimeter scale. In particular, a solution-processed lead(II) sulfide (PbS) layer provides a lattice-matched and chemical protective interface for the solid-gas reaction to form MAPbBr3 films on GaAs. Structure characterizations identify the crystal orientations in the trilayer MAPbBr3/PbS/GaAs epi-structure and confirm the monocrystalline nature of MAPbBr3 on PbS/GaAs. The dynamic evolution of surface morphologies during the growth indicates a two-step epitaxial process. These fundamental understandings and practical growth techniques offer a viable guideline to approach high-quality perovskite films for previously inaccessible applications. △ Less

Submitted 3 February, 2022; originally announced February 2022.

Non-perturbative $ab$ $initio$ approach for calculating the electrical conductivity of a liquid metal

Authors: Xiao-Wei Zhang, Haoran Chen, En-Ge Wang, Junren Shi, Xin-Zheng Li

Abstract: We propose a non-perturbative $ab$ $initio$ approach to calculate the electrical conductivity of a liquid metal. Our approach is based on the Kubo formula and the theory of electron-phonon coupling (EPC), and unlike the conventional empirical approach based on the Kubo-Greenwood formula, fully takes into account the effect of coupling between electrons and moving ions. We show that the electrical… ▽ More We propose a non-perturbative $ab$ $initio$ approach to calculate the electrical conductivity of a liquid metal. Our approach is based on the Kubo formula and the theory of electron-phonon coupling (EPC), and unlike the conventional empirical approach based on the Kubo-Greenwood formula, fully takes into account the effect of coupling between electrons and moving ions. We show that the electrical conductivity at high temperature is determined by an EPC parameter $λ_{\mathrm{tr}}$, which can be inferred, non-perturbatively, from the correlation of electron scattering matrices induced by ions. The latter can be evaluated in a molecular dynamics simulation. Based on the density-functional theory and pseudopotential methods, we implement the approach in an $ab$ $initio$ manner. We apply it to liquid sodium and obtain results in good agreement with experiments. This approach is efficient and based on a rigorous theory, suitable for applying to general metallic liquid systems. △ Less

Submitted 16 January, 2022; originally announced January 2022.

Comments: 9 pages, 5 figures

Enhanced Planar Antenna Efficiency Through Magnetic Thin-Films

Authors: Zhi Yao, Sidhant Tiwari, Joseph Schneider, Robert N. Candler, Gregory P. Carman, Yuanxun Ethan Wang

Abstract: This work proposes to use magnetic material as the substrate of planar antennas to overcome the platform effect caused by the conducting ground plane. The upper bound of the radiation efficiency of an electric-current-driven low-profile antenna is theoretically derived, which is inversely proportional to the Gilbert damping factor of the magnetic material. Meanwhile, the improvement of radiation d… ▽ More This work proposes to use magnetic material as the substrate of planar antennas to overcome the platform effect caused by the conducting ground plane. The upper bound of the radiation efficiency of an electric-current-driven low-profile antenna is theoretically derived, which is inversely proportional to the Gilbert damping factor of the magnetic material. Meanwhile, the improvement of radiation due to the use of magnetic material is demonstrated by a three-dimensional (3D) multiphysics and multiscale time-domain model. The simulation results match the theoretical derivation, showing 25% radiation efficiency from a planar antenna backed by a FeGaB thin film with 2.56 um thickness. Furthermore, for conductive ferromagnetic materials, it is shown that the eddy current loss can be well suppressed by laminating the thin film into multiple layers. The radiation efficiency of the modeled antenna with a conductive ferromagnetic substrate is improved from 2.2% to 11.8% by dividing the substrate into 10 layers, with a ferromagnetic material fill factor of 93%. △ Less

Submitted 10 December, 2021; originally announced January 2022.

Onset of metallic transition in molecular liquid hydrogen

Authors: Jianqing Guo, Bingqing Cheng, Limei Xu, Enge Wang, Ji Chen

Abstract: Liquid-liquid phase transition of hydrogen is at the center of hydrogen phase diagram as a promising route towards emergent properties such as the Wigner-Huntington metallization, superconductivity, and superfluidity. Here we report a study on the liquid-liquid phase transition of hydrogen using the state-of-the-art diffusion quantum Monte Carlo and density functional theory calculations. Our resu… ▽ More Liquid-liquid phase transition of hydrogen is at the center of hydrogen phase diagram as a promising route towards emergent properties such as the Wigner-Huntington metallization, superconductivity, and superfluidity. Here we report a study on the liquid-liquid phase transition of hydrogen using the state-of-the-art diffusion quantum Monte Carlo and density functional theory calculations. Our results suggest that the metallization process happens at lower pressures and temperatures compared to the structural phase transition of molecular to atomic hydrogen. The consequence is that metallized molecular hydrogen is stable at a wide range of pressures and temperatures. Our study breaks the conventional assumption that metallization coinciding with dissociation of hydrogen molecule, and the molecular metallic hydrogen liquid phase is likely to become the frontier of studying hydrogen phase transitions. △ Less

Submitted 24 June, 2022; v1 submitted 9 January, 2022; originally announced January 2022.

Approaching the Purcell factor limit with whispering-gallery hyperbolic phonon polaritons in hBN nanotubes

Authors: Xiangdong Guo, Ning Li, Xiaoxia Yang, Ruishi Qi, Chenchen Wu, Ruochen Shi, Yuehui Li, Yang Huang, F. Javier García de Abajo, En-Ge Wang, Peng Gao, Qing Dai

Abstract: Enhanced light-matter interaction at the nanoscale is pivotal in the foundation of nonlinear optics, quantum optics, and nanophotonics, which are essential for a vast range of applications including single-photon sources, nanolasers, and nanosensors. In this context, the combination of strongly confined polaritons and low-loss nanocavities provides a promising way to enhance light-matter interacti… ▽ More Enhanced light-matter interaction at the nanoscale is pivotal in the foundation of nonlinear optics, quantum optics, and nanophotonics, which are essential for a vast range of applications including single-photon sources, nanolasers, and nanosensors. In this context, the combination of strongly confined polaritons and low-loss nanocavities provides a promising way to enhance light-matter interaction, thus giving rise to a high density of optical states, as quantified by the so-called Purcell factor - the ratio of the decay rate of an optical quantum emitter to its value in free space. Here, we exploit whispering-gallery hyperbolic-phonon-polariton (WG-HPhP) modes in hBN nanotubes (BNNTs) to demonstrate record-high Purcell factors (~10^12) driven by the deep-subwavelength confinement of phonon polaritons and the low intrinsic losses in these atomically smooth nanocavities. Furthermore, the measured Purcell factor increases with decreasing BNNT radius down to 5 nm, a result that extrapolates to ~10^14 in a single-walled BNNT. Our study supports WG-HPhP modes in one-dimensional nanotubes as a powerful platform for investigating ultrastrong light-matter interactions, which open exciting perspectives for applications in single-molecular sensors and nanolasers. △ Less

Submitted 22 December, 2021; originally announced December 2021.

Comments: 21 pages, 4 figures

Phonon-mediated exciton relaxation in two-dimensional semiconductors: selection rules and relaxation pathways

Authors: Xiao-Wei Zhang, Kaichen Xie, En-Ge Wang, Ting Cao, Xin-Zheng Li

Abstract: Exciton-phonon coupling (ExPC) is crucial for energy relaxation in semiconductors, yet the first-principles calculation of such coupling remains challenging, especially for low-dimensional systems. Here, an accurate algorithm for calculating ExPC is developed and applied in exciton relaxation problems in monolayer WSe2. Considering the interplay between the exciton wave functions and electron-phon… ▽ More Exciton-phonon coupling (ExPC) is crucial for energy relaxation in semiconductors, yet the first-principles calculation of such coupling remains challenging, especially for low-dimensional systems. Here, an accurate algorithm for calculating ExPC is developed and applied in exciton relaxation problems in monolayer WSe2. Considering the interplay between the exciton wave functions and electron-phonon coupling (EPC) matrix elements, we find that ExPC shows distinct selection rules from the ones of EPC. By employing the Wannier exciton model, we generalize these selection rules, which state that the angular quantum numbers of the exciton must match the winding numbers of the EPC matrix elements for the ExPC to be allowed. To verify our theory and algorithm, we calculate inter-valley exciton relaxation pathways, which agrees well with a recent experiment. △ Less

Submitted 19 October, 2021; v1 submitted 17 October, 2021; originally announced October 2021.

Comments: 6 pages, 4 figures

Journal ref: The Journal of Physical Chemistry Letters, 15, 7584 (2024)

Experimental evidence of plasmarons and effective fine structure constant in electron-doped graphene/h-BN heterostructure

Authors: Hongyun Zhang, Shuopei Wang, Eryin Wang, Xiaobo Lu, Qian Li, Changhua Bao, Ke Deng, Haoxiong Zhang, Wei Yao, Guorui Chen, Alexei V. Fedorov, Jonathan D. Denlinger, Kenji Watanabe, Takashi Taniguchi, Guangyu Zhang, Shuyun Zhou

Abstract: Electron-electron interaction is fundamental in condensed matter physics and can lead to composite quasiparticles called plasmarons, which strongly renormalize the dispersion and carry information of electron-electron coupling strength as defined by the effective fine structure constant $α_{ee}^*$. Although h-BN with unique dielectric properties has been widely used as an important substrate for g… ▽ More Electron-electron interaction is fundamental in condensed matter physics and can lead to composite quasiparticles called plasmarons, which strongly renormalize the dispersion and carry information of electron-electron coupling strength as defined by the effective fine structure constant $α_{ee}^*$. Although h-BN with unique dielectric properties has been widely used as an important substrate for graphene, so far there is no experimental report of plasmarons in graphene/h-BN yet. Here, we report direct experimental observation of plasmaron dispersion in graphene/h-BN heterostructures through angle-resolved photoemission spectroscopy (ARPES) measurements upon {\it in situ} electron doping. Characteristic diamond-shaped dispersion is observed near the Dirac cone in both 0$^\circ$ (aligned) and 13.5$^\circ$ (twisted) graphene/h-BN, and the electron-electron interaction strength $α_{ee}^*$ is extracted to be $α_{ee}^*\approx0.9\pm 0.1$, highlighting the important role of electron-electron interaction. Our results suggest graphene/h-BN as an ideal platform for investigating strong electron-electron interaction with weak dielectric screening, and lays fundamental physics for gate-tunable nano-electronics and nano-plasmonics. △ Less

Submitted 2 October, 2021; originally announced October 2021.

Journal ref: npj Quantum Mater. 6, 83 (2021)

Measuring phonon dispersion at an interface

Authors: Ruishi Qi, Ruochen Shi, Yuanwei Sun, Yuehui Li, Mei Wu, Ning Li, Jinlong Du, Kaihui Liu, Chunlin Chen, Dapeng Yu, En-Ge Wang, Peng Gao

Abstract: The breakdown of translational symmetry at heterointerfaces leads to the emergence of new phonon modes localized near the interface. These interface phonons play an essential role in thermal/electrical transport properties in devices especially in miniature ones wherein the interface may dominate the entire response of the device. Knowledge of phonon dispersion at interfaces is therefore highly de… ▽ More The breakdown of translational symmetry at heterointerfaces leads to the emergence of new phonon modes localized near the interface. These interface phonons play an essential role in thermal/electrical transport properties in devices especially in miniature ones wherein the interface may dominate the entire response of the device. Knowledge of phonon dispersion at interfaces is therefore highly desirable for device design and optimization. Although theoretical work has begun decades ago, experimental research is totally absent due to challenges in achieving combined spatial, momentum and spectral resolutions required to probe localized phonon modes. Here we use electron energy loss spectroscopy in an electron microscope to directly measure both the local phonon density of states and the interface phonon dispersion relation for an epitaxial cBN-diamond heterointerface. In addition to bulk phonon modes, we observe acoustic and optical phonon modes localized at the interface, and modes isolated away from the interface. These features only appear within ~ 1 nm around the interface. The experimental results can be nicely reproduced by ab initio calculations. Our findings provide insights into lattice dynamics at heterointerfaces and should be practically useful in thermal/electrical engineering. △ Less

Submitted 10 August, 2021; originally announced August 2021.

Microscopic kinetics pathway of salt crystallization in graphene nanocapillaries

Authors: Lifen Wang, Ji Chen, Stephen J. Cox, Lei Liu, Gabriele C. Sosso, Ning Li, Peng Gao, Angelos Michaelides, Enge Wang, Xuedong Bai

Abstract: The fundamental understanding of crystallization, in terms of microscopic kinetic and thermodynamic details, remains a key challenge in the physical sciences. Here, by using in situ graphene liquid cell transmission electron microscopy, we reveal the atomistic mechanism of NaCl crystallization from solutions confined within graphene cells. We find that rock salt NaCl forms with a peculiar hexagona… ▽ More The fundamental understanding of crystallization, in terms of microscopic kinetic and thermodynamic details, remains a key challenge in the physical sciences. Here, by using in situ graphene liquid cell transmission electron microscopy, we reveal the atomistic mechanism of NaCl crystallization from solutions confined within graphene cells. We find that rock salt NaCl forms with a peculiar hexagonal morphology. We also see the emergence of a transitory graphite-like phase, which may act as an intermediate in a two-step pathway. With the aid of density functional theory calculations, we propose that these observations result from a delicate balance between the substrate-solute interaction and thermodynamics under confinement. Our results highlight the impact of confinement on both the kinetics and thermodynamics of crystallization, offering new insights into heterogeneous crystallization theory and a potential avenue for materials design. △ Less

Submitted 10 March, 2021; originally announced March 2021.

Comments: Main: 7 pages, 4 figures; Supplemental Material: 12 pages, 7 figures

A full configuration interaction quantum Monte Carlo study of ScO, TiO and VO molecules

Authors: Tonghuan Jiang, Yilin Chen, Nikolay Bogdanov, Enge Wang, Ali Alavi, Ji Chen

Abstract: Accurate ab initio calculations of 3d transition metal monoxide molecules have attracted extensive attention because of its relevance in physical and chemical science, as well as theoretical challenges in treating strong electron correlation. Meanwhile, recent years have witnessed the rapid development of full configuration interaction quantum Monte Carlo (FCIQMC) method to tackle electron correla… ▽ More Accurate ab initio calculations of 3d transition metal monoxide molecules have attracted extensive attention because of its relevance in physical and chemical science, as well as theoretical challenges in treating strong electron correlation. Meanwhile, recent years have witnessed the rapid development of full configuration interaction quantum Monte Carlo (FCIQMC) method to tackle electron correlation. In this study, we carry out FCIQMC simulations to ScO, TiO and VO molecules and obtain accurate descriptions of 13 low-lying electronic states (ScO $^2Σ^+$, $^2Δ$, $^2Π$; TiO $^3Δ$, $^1Δ$, $^1Σ^+$, $^3Π$, $^3Φ$; VO $^4Σ^-$, $^4Φ$, $^4Π$, $^2Γ$, $^2Δ$), including states that have significant multi-configurational character. The FCIQMC results are used to assess the performance of several other wave function theory and density functional theory methods. Our study highlights the challenging nature of electronic structure of transition metal oxides and demonstrates FCIQMC as a promising technique going forward to treat more complex transition metal oxide molecules and materials. △ Less

Submitted 24 January, 2021; originally announced January 2021.

Direct visualization of electromagnetic wave dynamics by laser-free ultrafast electron microscopy

Authors: Xuewen Fu, Erdong Wang, Yubin Zhao, Ao Liu, Eric Montgomery, Vikrant J. Gokhale, Jason J. Gorman, Chungguang Jing, June W. Lau, Yimei Zhu

Abstract: Integrating femtosecond (fs) lasers to electron microscopies has enabled direct imaging of transient structures and morphologies of materials in real time and space, namely, ultrafast electron microscopy (UEM). Here we report the development of a laser-free UEM offering the same capability of real-time imaging with high spatiotemporal resolutions but without requiring expensive fs lasers and intri… ▽ More Integrating femtosecond (fs) lasers to electron microscopies has enabled direct imaging of transient structures and morphologies of materials in real time and space, namely, ultrafast electron microscopy (UEM). Here we report the development of a laser-free UEM offering the same capability of real-time imaging with high spatiotemporal resolutions but without requiring expensive fs lasers and intricate instrumental modifications. We create picosecond electron pulses for probing dynamic events by chopping a continuous beam with a radiofrequency (RF)-driven pulser, where the repetition rate of the electron pulses is tunable from 100 MHz to 12 GHz. A same broadband of electromagnetic wave is enabled for sample excitation. As a first application, we studied the GHz electromagnetic wave propagation dynamics in an interdigitated comb structure which is one of the basic building blocks for RF micro-electromechanical systems. A series of pump-probe images reveals, on nanometer space and picosecond time scales, the transient oscillating electromagnetic field around the tines of the combs, and time-resolved polarization, amplitude, and nonlinear local field enhancement. The success of this study demonstrates the feasibility of the low-cost laser-free UEM in real-space visualizing of dynamics for many research fields, especially the electrodynamics in devices associated with information processing technology. △ Less

Submitted 4 June, 2020; originally announced June 2020.

Comments: 25 pages, 4 figures

Manipulating Weyl quasiparticles by orbital-selective photoexcitation in WTe2

Authors: Meng-Xue Guan, En Wang, Pei-Wei You, Jia-Tao Sun, Sheng Meng

Abstract: Optical control of structural and electronic properties of Weyl semimetals allows development of switchable and dissipationless topological devices at the ultrafast scale. An unexpected orbitial-selective photoexcitation in type-II Weyl material WTe2 is reported under linearly polarized light (LPL), inducing striking transitions among several topologically-distinct phases. The symmetry features of… ▽ More Optical control of structural and electronic properties of Weyl semimetals allows development of switchable and dissipationless topological devices at the ultrafast scale. An unexpected orbitial-selective photoexcitation in type-II Weyl material WTe2 is reported under linearly polarized light (LPL), inducing striking transitions among several topologically-distinct phases. The symmetry features of atomic orbitals comprising the Weyl bands result in asymmetric electronic transitions near the Weyl points, and in turn an anisotropic response of interlayer shear motion with respect to linear light polarization, when a near-infrared laser pulse is applied. Consequently, not only annihilation of Weyl quasiparticle pairs, but also increasing separation of Weyl points can be achieved, complementing existing experimental observations. Our results provide a new perspective on manipulating the singularity of Weyl nodes and coherent control of electron and lattice quantum dynamics simultaneously. △ Less

Submitted 25 April, 2020; originally announced April 2020.

The influence of high-energy local orbitals and electron-phonon interactions on the band gaps and optical spectra of hexagonal boron nitride

Authors: Tong Shen, Xiao-Wei Zhang, Honghui Shang, Min-Ye Zhang, Xinqiang Wang, En-Ge Wang, Hong Jiang, Xin-Zheng Li

Abstract: We report $ab$ $initio$ band diagram and optical absorption spectra of hexagonal boron nitride ($h$-BN), focusing on unravelling how the completeness of basis set for $GW$ calculations and how electron-phonon interactions (EPIs) impact on them. The completeness of basis set, an issue which was seldom discussed in previous optical spectra calculations of $h$-BN, is found crucial in providing conver… ▽ More We report $ab$ $initio$ band diagram and optical absorption spectra of hexagonal boron nitride ($h$-BN), focusing on unravelling how the completeness of basis set for $GW$ calculations and how electron-phonon interactions (EPIs) impact on them. The completeness of basis set, an issue which was seldom discussed in previous optical spectra calculations of $h$-BN, is found crucial in providing converged quasiparticle band gaps. In the comparison among three different codes, we demonstrate that by including high-energy local orbitals in the all-electron linearized augmented plane waves based $GW$ calculations, the quasiparticle direct and fundamental indirect band gaps are widened by $\sim$0.2 eV, giving values of 6.81 eV and 6.25 eV respectively at the $GW_0$ level. EPIs, on the other hand, reduce them to 6.62 eV and 6.03 eV respectively at 0 K, and 6.60 eV and 5.98 eV respectively at 300 K. With clamped crystal structure, the first peak of the absorption spectrum is at 6.07 eV, originating from the direct exciton contributed by electron transitions around $K$ in the Brillouin zone. After including the EPIs-renormalized quasiparticles in the Bethe-Salpeter equation, the exciton-phonon coupling shifts the first peak to 5.83 eV at 300 K, lower than the experimental value of $\sim$6.00 eV. This accuracy is acceptable to an $ab$ $initio$ description of excited states with no fitting parameter. △ Less

Submitted 23 May, 2020; v1 submitted 28 March, 2020; originally announced March 2020.

Journal ref: Phys. Rev. B 102, 045117 (2020)

Evidence for metastable photo-induced superconductivity in K$_3$C$_{60}$

Authors: M. Budden, T. Gebert, M. Buzzi, G. Jotzu, E. Wang, T. Matsuyama, G. Meier, Y. Laplace, D. Pontiroli, M. Riccò, F. Schlawin, D. Jaksch, A. Cavalleri

Abstract: Far and mid infrared optical pulses have been shown to induce non-equilibrium unconventional orders in complex materials, including photo-induced ferroelectricity in quantum paraelectrics, magnetic polarization in antiferromagnets and transient superconducting correlations in the normal state of cuprates and organic conductors. In the case of non-equilibrium superconductivity, femtosecond drives h… ▽ More Far and mid infrared optical pulses have been shown to induce non-equilibrium unconventional orders in complex materials, including photo-induced ferroelectricity in quantum paraelectrics, magnetic polarization in antiferromagnets and transient superconducting correlations in the normal state of cuprates and organic conductors. In the case of non-equilibrium superconductivity, femtosecond drives have generally resulted in electronic properties that disappear immediately after excitation, evidencing a state that lacks intrinsic rigidity. Here, we make use of a new optical device to drive metallic K$_3$C$_{60}$ with mid-infrared pulses of tunable duration, ranging between one picosecond and one nanosecond. The same superconducting-like optical properties observed over short time windows for femtosecond excitation are shown here to become metastable under sustained optical driving, with lifetimes in excess of ten nanoseconds. Direct electrical probing becomes possible at these timescales, yielding a vanishingly small resistance. Such a colossal positive photo-conductivity is highly unusual for a metal and, when taken together with the transient optical conductivities, it is rather suggestive of metastable light-induced superconductivity. △ Less

Submitted 28 February, 2020; originally announced February 2020.

Comments: 14 pages, 5 figures, supplementary materials

Anisotropic Moiré Optical Transitions in Twisted Monolayer/bilayer Phosphorene Heterostructures

Authors: Shilong Zhao, Erqing Wang, Ebru Alime Üzer, Shuaifei Guo, Kenji Watanabe, Takashi Taniguchi, Tom Nilges, Yuanbo Zhang, Bilu Liu, Xiaolong Zou, Feng Wang

Abstract: Moiré superlattices of van der Waals heterostructures provide a powerful new way to engineer the electronic structures of two-dimensional (2D) materials. Many novel quantum phenomena have emerged in different moiré heterostructures, such as correlated insulators, superconductors, and Chern insulators in graphene systems and moiré excitons in transition metal dichalcogenide (TMDC) systems. Twisted… ▽ More Moiré superlattices of van der Waals heterostructures provide a powerful new way to engineer the electronic structures of two-dimensional (2D) materials. Many novel quantum phenomena have emerged in different moiré heterostructures, such as correlated insulators, superconductors, and Chern insulators in graphene systems and moiré excitons in transition metal dichalcogenide (TMDC) systems. Twisted phosphorene offers another attractive system to explore moiré physics because phosphorene features an anisotropic rectangular lattice, different from the isotropic hexagonal lattice in graphene and TMDC. Here we report emerging anisotropic moiré optical transitions in twisted monolayer/bilayer phosphorene. The optical resonances in phosphorene moiré superlattice depend sensitively on the twist angle between the monolayer and bilayer. Surprisingly, even for a twist angle as large as 19° the moiré heterostructure exhibits optical resonances completely different from those in the constituent monolayer and bilayer phosphorene. The new moiré optical resonances exhibit strong linear polarization, with the principal axis lying close to but different from the optical axis of bilayer phosphorene. Our ab initio calculations reveal that the Γ-point direct bandgap and the rectangular lattice of phosphorene, unlike the K-point bandgap of hexagonal lattice in graphene and TMDC, give rise to the remarkably strong moiré physics in large-twist-angle phosphorene heterostructures. Our results highlight the exciting opportunities to explore moiré physics in phosphorene and other van der Waals heterostructures with different lattice configurations. △ Less

Submitted 8 December, 2019; originally announced December 2019.

Comments: 34 pages, 11 figures

Decoupling of itinerant and localized $d$-orbital electrons in the compound Sc$_{0.5}$Zr$_{0.5}$Co

Authors: Jin Si, Xinwei Fan, Enyu Wang, Xiyu Zhu, Qing Li, Hai-Hu Wen

Abstract: By using the arc-melting method, we successfully synthesized the compound Sc$_{0.5}$Zr$_{0.5}$Co with the space group of $Pm$-$3m$. Both the resistivity and magnetic susceptibility measurements reveal a phase transition at about 86 K. This transition might be attributed to the establishment of an antiferromagnetic order. The magnetization hysteresis loop measurements in wide temperature region sho… ▽ More By using the arc-melting method, we successfully synthesized the compound Sc$_{0.5}$Zr$_{0.5}$Co with the space group of $Pm$-$3m$. Both the resistivity and magnetic susceptibility measurements reveal a phase transition at about 86 K. This transition might be attributed to the establishment of an antiferromagnetic order. The magnetization hysteresis loop measurements in wide temperature region show a weak ferromagnetic feature, which suggests a possible canted arrangement of the magnetic moments. Bounded by the phase transition temperature, the resistivity at ambient pressure shows a change from Fermi liquid behavior to a super-linear behavior as temperature increases. By applying pressures up to 32.1 GPa, the transition temperature does not show a clear change and no superconductivity is observed above 2 K. The density functional theory (DFT) calculations confirm the existence of the antiferromagnetic order and reveal a gap between the spin-up and spin-down $d$-orbital electrons. This kind of behavior may suggest that the antiferromagnetic order in this compound originates from the localized $d$-electrons which do not contribute to the conductance. Thus the itinerant and localized $d$-orbital electrons in the compound are decoupled. △ Less

Submitted 9 October, 2019; originally announced October 2019.

Comments: 6 pages, 6 figures

Journal ref: J. Phys.: Condens. Matter 32 40LT01 (2020)

Ideal type-II Weyl phonons in wurtzite CuI

Authors: Jian Liu, Wenjie Hou, En Wang, Shengjie Zhang, Jia-Tao Sun, Sheng Meng

Abstract: Weyl semimetals exhibitinging the topologically nontrivial touching points in electronic band dispersion of solids pave the wave way to novel electronic devices and functionalities. Here, we demonstrate the signature of topologically nontrivial Weyl points (WPs) in phonon dispersion of solids through a first-principles investigations. ofT noncentrosymmetric wurtzite CuI (cuprous iodide at high tem… ▽ More Weyl semimetals exhibitinging the topologically nontrivial touching points in electronic band dispersion of solids pave the wave way to novel electronic devices and functionalities. Here, we demonstrate the signature of topologically nontrivial Weyl points (WPs) in phonon dispersion of solids through a first-principles investigations. ofT noncentrosymmetric wurtzite CuI (cuprous iodide at high temperature). These type-II phononic WP in phonon dispersion of wurtzite CuI is manifested in noncentrosymmetric wurtzite CuI by six pairs of the nontrivial touching points in the k_z=0.0 plane. The ideal WPs in phonon dispersion are completely isolated from bulk phonon continuum, are different distinct from many type-II WPs in electronic band dispersion of solids associated with the overlapping band states. The opposite chirality of Weyl phonon nodes with quantized Berry curvature are utilized forproduces Weyl phonon Hall effect, in analogous analogy towith valley Hall effect of electrons. Such ideal type-II Weyl phonons are phase is readily observable in experiment, and could provideing a unique platform to study novel thermal transport properties different distinct from that in type-I Weyl phonons phase. △ Less

Submitted 29 April, 2019; originally announced April 2019.

Journal ref: Phys. Rev. B 100, 081204 (2019)

A New Cumulant Expansion Based Extraction for Higher Order Quantum Corrections in Equilibrium Wigner-Boltzmann Equation

Authors: Xiyue Li, Everett X. Wang

Abstract: A Cumulant based method has been introduced to extract quantum corrections in distribution function with the equilibrium Wigner-Boltzmann equation. It is shown that unlike the moment expansion used in hydrodynamic model, cumulant expansion converges much faster when distribution function is closed to Maxwellian with only first three cumulants are non-zero. In this case, quantum corrections higher… ▽ More A Cumulant based method has been introduced to extract quantum corrections in distribution function with the equilibrium Wigner-Boltzmann equation. It is shown that unlike the moment expansion used in hydrodynamic model, cumulant expansion converges much faster when distribution function is closed to Maxwellian with only first three cumulants are non-zero. In this case, quantum corrections higher than first order can be extracted mainly by lowest three cumulants and odd number derivatives of potential function. This method also provides a new way to determine the distribution function with Maxwellian form and study the role of potential function in quantum correction field. △ Less

Submitted 27 February, 2019; originally announced March 2019.

Comments: 6 pages, 1 figure

Synergy and competition between superconductivity and antiferromagnetism in FeSe under pressure

Authors: Guan-Yu Chen, Enyu Wang, Xiyu Zhu, Hai-Hu Wen

Abstract: Temperature dependence of resistivity under high pressures with magnetic fields parallel and perpendicular to the FeSe planes are measured in FeSe single crystals. It is found that the structural transition (nematic) temperature is suppressed by pressure and ends at around $P$ = 1.18 GPa. Below around 0.85 GPa, the superconducting transition shows a narrow width with no indication of antiferromagn… ▽ More Temperature dependence of resistivity under high pressures with magnetic fields parallel and perpendicular to the FeSe planes are measured in FeSe single crystals. It is found that the structural transition (nematic) temperature is suppressed by pressure and ends at around $P$ = 1.18 GPa. Below around 0.85 GPa, the superconducting transition shows a narrow width with no indication of antiferromagnetic order. While above this pressure, the superconducting transition temperature drops slightly forming a small dome of superconducting region with the maximum $T_c$ at around 0.825 GPa. Furthermore, just above this pressure, the superconducting transition exhibits an unusual large transition width which reaches about 6-8 K. This wide transition width is an intrinsic feature and does not change with magnetic field. In the high pressure region above 1.18 GPa, just accompanying the onset of superconducting transition, an upturn of resistivity immediately occurs, which is attributed to the formation of an antiferromagnetic order. This closely attached behavior of superconductivity and antiferromagnetic order indicates that these two orders have a synergy feature. Near the critical pressure 0.825 GPa and below, our data illustrate that an antiferromagnetic order emerges when superconductivity is suppressed. From the weak influence of magnetic field to the antiferromagnetic order, we conclude that it exists already below the small superconducting dome in the low pressure region. This shows a competing feature between superconductivity and antiferromagnetic order. Our results show duality features, namely synergy and competition between superconductivity and antiferromagnetic order under pressure in FeSe. △ Less

Submitted 28 November, 2018; originally announced November 2018.

Comments: 9 pages, 7 figures

Journal ref: Phys. Rev. B 99, 054517 (2019)

Towards the growth of single-crystal boron nitride monolayer on Cu

Authors: Li Wang, Xiaozhi Xu, Leining Zhang, Ruixi Qiao, Muhong Wu, Zhichang Wang, Shuai Zhang, Jing Liang, Zhihong Zhang, Yuwei Shan, Yi Guo, Marc Willinger, Hui Wu, Qunyang Li, Wenlong Wang, Peng Gao, Shiwei Wu, Ying Jiang, Dapeng Yu, Enge Wang, Xuedong Bai, Zhu-Jun Wang, Feng Ding, Kaihui Liu

Abstract: Atom-layered hexagonal boron nitride (hBN), with excellent stability, flat surface and large bandgap, has been reported to be the best 2D insulator to open up the great possibilities for exciting potential applications in electronics, optoelectronics and photovoltaics. The ability to grow high-quality large single crystals of hBN is at the heart for those applications, but the size of single-cryst… ▽ More Atom-layered hexagonal boron nitride (hBN), with excellent stability, flat surface and large bandgap, has been reported to be the best 2D insulator to open up the great possibilities for exciting potential applications in electronics, optoelectronics and photovoltaics. The ability to grow high-quality large single crystals of hBN is at the heart for those applications, but the size of single-crystal 2D BN is less than a millimetre till now. Here, we report the first epitaxial growth of a 10*10 cm2 single-crystal hBN monolayer on a low symmetry Cu(110) "vicinal surface". The growth kinetics, unidirectional alignment and seamless stitching of hBN domains are unambiguously illustrated using centimetre- to the atomic-scale characterization techniques. The findings in this work are expected to significantly boost the massive applications of 2D materials-based devices, and also pave the way for the epitaxial growth of broad non-centrosymmetric 2D materials. △ Less

Submitted 16 November, 2018; originally announced November 2018.

Towards Robust Deep Neural Networks

Authors: Timothy E. Wang, Yiming Gu, Dhagash Mehta, Xiaojun Zhao, Edgar A. Bernal

Abstract: We investigate the topics of sensitivity and robustness in feedforward and convolutional neural networks. Combining energy landscape techniques developed in computational chemistry with tools drawn from formal methods, we produce empirical evidence indicating that networks corresponding to lower-lying minima in the optimization landscape of the learning objective tend to be more robust. The robust… ▽ More We investigate the topics of sensitivity and robustness in feedforward and convolutional neural networks. Combining energy landscape techniques developed in computational chemistry with tools drawn from formal methods, we produce empirical evidence indicating that networks corresponding to lower-lying minima in the optimization landscape of the learning objective tend to be more robust. The robustness estimate used is the inverse of a proposed sensitivity measure, which we define as the volume of an over-approximation of the reachable set of network outputs under all additive $l_{\infty}$-bounded perturbations on the input data. We present a novel loss function which includes a sensitivity term in addition to the traditional task-oriented and regularization terms. In our experiments on standard machine learning and computer vision datasets, we show that the proposed loss function leads to networks which reliably optimize the robustness measure as well as other related metrics of adversarial robustness without significant degradation in the classification error. Experimental results indicate that the proposed method outperforms state-of-the-art sensitivity-based learning approaches with regards to robustness to adversarial attacks. We also show that although the introduced framework does not explicitly enforce an adversarial loss, it achieves competitive overall performance relative to methods that do. △ Less

Submitted 4 December, 2018; v1 submitted 27 October, 2018; originally announced October 2018.

Comments: Added further discussions, and supplementary material

Direct visualization of sign reversal s^+- superconducting gaps in FeTe0.55Se0.45

Authors: Mingyang Chen, Qingkun Tang, Xiaoyu Chen, Qiangqiang Gu, Huan Yang, Zengyi Du, Xiyu Zhu, Enyu Wang, Qiang-Hua Wang, Hai-Hu Wen

Abstract: In many unconventional superconductors, the pairing of electrons is driven by the repulsive interaction, which leads to the sign reversal of superconducting gaps along the Fermi surfaces (FS) or between them. However, to measure this sign change is not easy and straightforward. It is known that, in superconductors with sign reversal gaps, non-magnetic impurities can break Cooper pairs leading to t… ▽ More In many unconventional superconductors, the pairing of electrons is driven by the repulsive interaction, which leads to the sign reversal of superconducting gaps along the Fermi surfaces (FS) or between them. However, to measure this sign change is not easy and straightforward. It is known that, in superconductors with sign reversal gaps, non-magnetic impurities can break Cooper pairs leading to the quasiparticle density of states in the superconducting state. The standing waves of these quasiparticles will interfere each other leading to the quasiparticle interference (QPI) pattern which carries the phase message reflecting also the superconducting gap structure. Based on the recently proposed defect-bound-state QPI technique, we explore the applicability of this technique to a typical iron based superconductor FeTe$_{0.55}$Se$_{0.45}$ with roughly equivalent gap values on the electron and hole pockets connected by the wave vector q_2=(0,π). It is found that, on the negative energy side, with the energy slightly below the gap value, the phase reference quantity $|g(q,-E)|\cos(θ_{q,+E}-θ_{q,-E}) becomes negative and the amplitude is strongly enhanced with the scattering vector q_2, but that corresponding to the scattering between the electron-electron pockets, namely q_3=(π,π), keeps all positive. This is well consistent with the theoretical expectation of the s^+- pairing gap and thus serves as a direct visualization of the sign reversal gaps. This experimental observation is also supported by the theoretical calculations with the Fermi surface structure and s^+- pairing gap. △ Less

Submitted 15 October, 2018; originally announced October 2018.

Comments: 10 pages, 6 figures

Journal ref: Phys. Rev. B 99, 014507 (2019)

Ab initio investigation on the experimental observation of metallic hydrogen

Authors: Xiaowei Zhang, En-Ge Wang, Xin-Zheng Li

Abstract: The optical spectra of hydrogen at $\sim$500 GPa were studied theoretically using a combination of \emph{ab initio} methods. Among the four most competitive structures, i.e. C2/c-24, Cmca-12, Cmca-4, and I41/amd, only the atomic phase I41/amd can provide satisfactory interpretations of the recent experimental observation, and the electron-phonon interactions (EPIs) play a crucial role. Anharmonic… ▽ More The optical spectra of hydrogen at $\sim$500 GPa were studied theoretically using a combination of \emph{ab initio} methods. Among the four most competitive structures, i.e. C2/c-24, Cmca-12, Cmca-4, and I41/amd, only the atomic phase I41/amd can provide satisfactory interpretations of the recent experimental observation, and the electron-phonon interactions (EPIs) play a crucial role. Anharmonic effects (AHEs) due to lattice vibration are non-negligible but not sufficient to account for the experimentally observed temperature dependence of the reflectance. The drop of the reflectance at 2 eV is not caused by diamond's band gap reducing or interband plasmon, but very likely by defects absorptions in diamond. These results provide theoretical support for the recent experimental realization of metallic hydrogen. The strong EPIs and the non-negligible AHEs also emphasize the necessity for quantum treatments of both the electrons and the nuclei in future studies. △ Less

Submitted 4 May, 2018; originally announced May 2018.

Comments: 5 figures

Journal ref: Phys. Rev. B 98, 134110 (2018)

Quasicrystalline 30° Twisted Bilayer Graphene as an Incommensurate Superlattice with Strong Interlayer Coupling

Authors: Wei Yao, Eryin Wang, Changhua Bao, Yiou Zhang, Kenan Zhang, Kejie Bao, Chun Kai Chan, Chaoyu Chen, Jose Avila, Maria C. Asensio, Junyi Zhu, Shuyun Zhou

Abstract: The interlayer coupling can be used to engineer the electronic structure of van der Waals heterostructures (superlattices) to obtain properties that are not possible in a single material. So far research in heterostructures has been focused on commensurate superlattices with a long-ranged Moiré period. Incommensurate heterostructures with rotational symmetry but not translational symmetry (in anal… ▽ More The interlayer coupling can be used to engineer the electronic structure of van der Waals heterostructures (superlattices) to obtain properties that are not possible in a single material. So far research in heterostructures has been focused on commensurate superlattices with a long-ranged Moiré period. Incommensurate heterostructures with rotational symmetry but not translational symmetry (in analogy to quasicrystals) are not only rare in nature, but also the interlayer interaction has often been assumed to be negligible due to the lack of phase coherence. Here we report the successful growth of quasicrystalline 30° twisted bilayer graphene (30°-tBLG) which is stabilized by the Pt(111) substrate, and reveal its electronic structure. The 30°-tBLG is confirmed by low energy electron diffraction and the intervalley double-resonance Raman mode at 1383 cm$^{-1}$. Moreover, the emergence of mirrored Dirac cones inside the Brillouin zone of each graphene layer and a gap opening at the zone boundary suggest that these two graphene layers are coupled via a generalized Umklapp scattering mechanism, i.e. scattering of Dirac cone in one graphene layer by the reciprocal lattice vector of the other graphene layer. Our work highlights the important role of interlayer coupling in incommensurate quasicrystalline superlattices, thereby extending band structure engineering to incommensurate superstructures. △ Less

Submitted 19 June, 2018; v1 submitted 15 April, 2018; originally announced April 2018.

Comments: Evidences of quasicrystalline 30°-tBLG from LEED, Raman and ARPES (combined with regular and nano-size beam spot), submitted on December 1, 2017, has been accepted by PNAS

Pressure Induced Superconductivity in the New Compound ScZrCo1-$δ$

Authors: Enyu Wang, Jing Si, Xiyu Zhu, Guan-Yu Chen, Hai Lin, Hai-Hu Wen

Abstract: It is widely perceived that the correlation effect may play an important role in several unconventional superconducting families, such as cuprate, iron-based and heavy-fermion superconductors. The application of high pressure can tune the ground state properties and balance the localization and itineracy of electrons in correlated systems, which may trigger unconventional superconductivity. Moreov… ▽ More It is widely perceived that the correlation effect may play an important role in several unconventional superconducting families, such as cuprate, iron-based and heavy-fermion superconductors. The application of high pressure can tune the ground state properties and balance the localization and itineracy of electrons in correlated systems, which may trigger unconventional superconductivity. Moreover, non-centrosymmetric structure may induce the spin triplet pairing which is very rare in nature. Here, we report a new compound ScZrCo1-$δ$ crystallizing in the Ti2Ni structure with the space group of FD3-MS without a spatial inversion center. The resistivity of the material at ambient pressure shows a bad metal and weak semiconducting behavior. Furthermore, specific heat and magnetic susceptibility measurements yield a rather large value of Wilson ratio ~4.47. Both suggest a ground state with correlation effect. By applying pressure, the up-going behavior of resistivity in lowering temperature at ambient pressure is suppressed and gradually it becomes metallic. At a pressure of about 19.5 GPa superconductivity emerges. Up to 36.05 GPa, a superconducting transition at about 3.6 K with a quite high upper critical field is observed. Our discovery here provides a new platform for investigating the relationship between correlation effect and superconductivity. △ Less

Submitted 11 October, 2017; originally announced October 2017.

Comments: 23 pages, 6 figures, including Supplementary Information

Journal ref: New J. Phys. 20 (2018) 073036

Discrete energy levels of Caroli-de Gennes-Martricon states in quantum limit due to small Fermi energy in FeTe$_{0.55}$Se$_{0.45}$

Authors: Mingyang Chen, Xiaoyu Chen, Huan Yang, Zengyi Du, Xiyu Zhu, Enyu Wang, Hai-Hu Wen

Abstract: Caroli-de Gennes-Martricon (CdGM) states were predicted in 1964 as low energy excitations within vortex cores of type-II superconductors. In the quantum limit, namely $T/T_\mathrm{c} \ll Δ/E_\mathrm{F}$, the energy levels of these states were predicted to be discrete with the basic levels at $E_μ= \pm μΔ^2/E_\mathrm{F}$ ($μ= 1/2$, $3/2$, $5/2$, ...). However, due to the small ratio of… ▽ More Caroli-de Gennes-Martricon (CdGM) states were predicted in 1964 as low energy excitations within vortex cores of type-II superconductors. In the quantum limit, namely $T/T_\mathrm{c} \ll Δ/E_\mathrm{F}$, the energy levels of these states were predicted to be discrete with the basic levels at $E_μ= \pm μΔ^2/E_\mathrm{F}$ ($μ= 1/2$, $3/2$, $5/2$, ...). However, due to the small ratio of $Δ/E_\mathrm{F}$ in most type-II superconductors, it is very difficult to observe the discrete CdGM states, but rather a symmetric peak appears at zero-bias at the vortex center. Here we report the clear observation of these discrete energy levels of CdGM states in FeTe$_{0.55}$Se$_{0.45}$. The rather stable energies of these states versus space clearly validates our conclusion. Analysis based on the energies of these CdGM states indicates that the Fermi energy in the present system is very small. △ Less

Submitted 27 September, 2017; originally announced September 2017.

Comments: 26 pages, 9 figures

Journal ref: Nature Communications 9: 970 (2018)

Generalized Ensemble Theory with Non-extensive Statistics

Authors: Ke-Ming Shen, Ben-Wei Zhang, En-Ke Wang

Abstract: The non-extensive canonical ensemble theory is reconsidered with the method of Lagrange multipliers by maximizing Tsallis entropy, with the constraint that the normalized term of Tsallis' $q-$average of physical quantities, the sum $\sum p_j^q$, is independent of the probability $p_i$ for Tsallis parameter $q$. The self-referential problem in the deduced probability and thermal quantities in non-e… ▽ More The non-extensive canonical ensemble theory is reconsidered with the method of Lagrange multipliers by maximizing Tsallis entropy, with the constraint that the normalized term of Tsallis' $q-$average of physical quantities, the sum $\sum p_j^q$, is independent of the probability $p_i$ for Tsallis parameter $q$. The self-referential problem in the deduced probability and thermal quantities in non-extensive statistics is thus avoided, and thermodynamical relationships are obtained in a consistent and natural way. We also extend the study to the non-extensive grand canonical ensemble theory and obtain the $q$-deformed Bose-Einstein distribution as well as the $q$-deformed Fermi-Dirac distribution. The theory is further applied to the generalized Planck law to demonstrate the distinct behaviors of the various generalized $q$-distribution functions discussed in literature. △ Less

Submitted 11 July, 2017; originally announced July 2017.

Comments: 14 pages, 2 figures

Journal ref: Physica A 487C (2017) pp. 215-224