Showing 1–50 of 202 results for author: Xu, K

Spin-mediated hysteretic switching of unidirectional charge density waves by rotating magnetic fields

Authors: Zichao Chen, Shiyu Zhu, Kailin Xu, Ruwen Wang, Ningning Wang, Jianfeng Guo, Yunhao Wang, Xianghe Han, Zhongyi Cao, Jianping Sun, Hui Chen, Haitao Yang, Jinguang Cheng, Ziqiang Wang, Hong-Jun Gao

Abstract: Charge density waves (CDWs) are a widespread collective electronic order in quantum materials, furnishing key insights into symmetry breaking and competing phases. However, their dynamic control with external fields remains a pivotal challenge. Here, we report deterministic and hysteretic switching of unidirectional CDW orientation via in-plane magnetic field rotation in magnetic kagome metal GdTi… ▽ More Charge density waves (CDWs) are a widespread collective electronic order in quantum materials, furnishing key insights into symmetry breaking and competing phases. However, their dynamic control with external fields remains a pivotal challenge. Here, we report deterministic and hysteretic switching of unidirectional CDW orientation via in-plane magnetic field rotation in magnetic kagome metal GdTi3Bi4. Atomically resolved spectroscopy shows two types of 3a0*1a0 CDW domains, Q1 and Q2 oriented 60 degree apart along two distinct crystallographic directions and separated by atomically sharp domain walls. Rotating the magnetic field drives reversible transitions between these CDW configurations, exhibiting a robust C2-symmetric phase diagram with pronounced hysteresis. This hysteretic switching is mediated by a field-dependent reorientation of underlying antiferromagnetic spins, revealing a tunable energy landscape with stable and metastable states and modulates the electronic charge order via spin-lattice coupling. Our findings not only demonstrate the switching of CDW configurations by in-plane magnetic field but also reveal the mechanism of coupling between CDW and magnetic fields, offering new insights into CDW manipulation and versatile platform for developing a spin-mediated multistate spin-charge coupling memory and programmable quantum devices. △ Less

Submitted 15 April, 2026; originally announced April 2026.

Strain-Mediated Lattice Reconstruction Enhances Ferromagnetism in Cr2Ge2Te6/WTe2 van der Waals Heterobilayers

Authors: Franz Herling, Mireia Torres-Sala, Dorye L. Esteras, Charlotte Evason, Motomi Aoki, Marcos Rosado, Kapil Gupta, Bernat Mundet, Kai Xu, J. Sebastián Reparaz, Kenji Watanabe, Takashi Taniguchi, Dimitre Dimitrov, Vera Marinova, Ivan A. Verzhbitskiy, Goki Eda, José H. Garcia, Stephan Roche, Juan. F. Sierra, Sergio O. Valenzuela

Abstract: Van der Waals (vdW) heterostructures enable tailored electronic and magnetic phases by stacking atomically thin layers with pristine interfaces. Here, we investigate fully 2D Cr2Ge2Te6/WTe2 heterostructures and identify a strong enhancement of ferromagnetism in Cr2Ge2Te6 (CGT). Magnetotransport measurements across multiple devices with WTe2 thicknesses ranging from monolayer to bulk reveal a robus… ▽ More Van der Waals (vdW) heterostructures enable tailored electronic and magnetic phases by stacking atomically thin layers with pristine interfaces. Here, we investigate fully 2D Cr2Ge2Te6/WTe2 heterostructures and identify a strong enhancement of ferromagnetism in Cr2Ge2Te6 (CGT). Magnetotransport measurements across multiple devices with WTe2 thicknesses ranging from monolayer to bulk reveal a robust anomalous Hall effect together with a more than twofold increase of the Curie temperature and substantially enhanced coercive fields. Interface microscopy confirms chemically abrupt vdW interfaces with no detectable interdiffusion, while control experiments rule out processing- or stray-field-induced artifacts. Our experiments and theoretical calculations demonstrate that interfacial charge transfer renders CGT conductive and that proximity-induced lattice distortions in CGT enhance exchange and magnetocrystalline anisotropy. These results establish strain-mediated lattice reconstruction as a strategy for engineering high-temperature magnetic order in 2D heterostructures and clarify that modifications within the magnetic layer itself can govern proximity effects in vdW stacks. △ Less

Submitted 15 April, 2026; originally announced April 2026.

Comments: 23 pages, 5 figures, 1 table

Limits of Statistical Models of Ultracold Complex Lifetimes

Authors: Kevin B. Xu, John L. Bohn

Abstract: The puzzle of "sticky collisions," in which molecular collision complexes exhibit long lifetimes, remains an unresolved mystery. A central challenge is that traditional close-coupling calculations remain limited by the vast computational cost needed to take into account all the degrees of freedom involved in the collision. In this work, we propose a statistical model designed to simulate close-cou… ▽ More The puzzle of "sticky collisions," in which molecular collision complexes exhibit long lifetimes, remains an unresolved mystery. A central challenge is that traditional close-coupling calculations remain limited by the vast computational cost needed to take into account all the degrees of freedom involved in the collision. In this work, we propose a statistical model designed to simulate close-coupling calculations, with the goal of collecting statistics about reasonable lifetimes of collision complexes. To do so, we numerically sample resonances using random matrix theory and utilize results from quantum defect theory to calculate scattering properties and lifetimes. We find that in the limit of dense resonances, our theory agrees well with the Rice-Ramsperger-Kassel-Markus (RRKM) prediction, whereas in the limit of sparse resonances, the physics is governed by threshold behavior rather than resonant effects. By comparing these predictions to experimental results in two limits, we argue that close-coupling calculations alone may be insufficient to resolve the issue of long lifetimes. △ Less

Submitted 13 April, 2026; originally announced April 2026.

Comments: 14 pages, 9 figures

Observation of glueball excitations and string breaking in a $2+1$D $\mathbb{Z}_2$ lattice gauge theory on a trapped-ion quantum computer

Authors: Kaidi Xu, Umberto Borla, Kevin Hemery, Rohan Joshi, Henrik Dreyer, Enrico Rinaldi, Jad C. Halimeh

Abstract: A major goal of the quantum simulation of high-energy physics (HEP) is to probe real-time nonperturbative far-from-equilibrium quantum processes underlying phenomena such as hadronization in quantum chromodynamics (QCD). The quantum simulation of the dynamics of confining strings and glueballs, both essential aspects of quark confinement, in a controllable first-principles way is an important step… ▽ More A major goal of the quantum simulation of high-energy physics (HEP) is to probe real-time nonperturbative far-from-equilibrium quantum processes underlying phenomena such as hadronization in quantum chromodynamics (QCD). The quantum simulation of the dynamics of confining strings and glueballs, both essential aspects of quark confinement, in a controllable first-principles way is an important step towards this goal. Here, we realize a $\mathbb{Z}_2$ lattice gauge theory in $2+1$D with a tunable plaquette term on a \texttt{Quantinuum System Model H2} trapped-ion quantum computer. We implement a shallow depth-6 Trotter circuit on a $6 \times 5$ matter-site square lattice utilizing all $56$ available qubits to execute over $1000$ entangling gates. We prepare far-from-equilibrium initial string configurations that we quench across a range of parameters to observe rich dynamical phenomena, such as the formation of gauge-invariant closed-loop excitations reminiscent of glueballs in QCD and multi-order string breaking accompanied by spontaneous matter creation. We further demonstrate experimentally that the system displays genuine $2+1$D dynamics, as evidenced by string snapshots over time that cannot be trivially mapped to $1+1$D physics. Our results demonstrate digital quantum simulations of nonequilibrium dynamics in a higher-dimensional lattice gauge theory and provide an experimentally accessible setting for phenomena related to confinement physics. △ Less

Submitted 8 April, 2026; originally announced April 2026.

Comments: $12+7$ pages, $4+6$ figures, $0+1$ table. See parallel submission by R. Joshi et al., "Observation of genuine $2+1$D string dynamics in a U$(1)$ lattice gauge theory with a tunable plaquette term on a trapped-ion quantum computer''

GPUMDkit: A User-Friendly Toolkit for GPUMD and NEP

Authors: Zihan Yan, Denan Li, Xin Wu, Zhoulin Liu, Chen Hua, Boyi Situ, Hao Yang, Shengjie Tang, Benrui Tang, Ziyang Wang, Shangzhao Yi, Huan Wang, Dian Huang, Ke Li, Qilin Guo, Zherui Chen, Ke Xu, Yanzhou Wang, Ziliang Wang, Gang Tang, Shi Liu, Zheyong Fan, Yizhou Zhu

Abstract: Machine-learned interatomic potentials have revolutionized molecular dynamics simulations by providing quantum-mechanical accuracy at empirical-potential speeds. The graphics processing unit molecular dynamics (GPUMD) package, featuring the highly efficient neuroevolution potential (NEP) framework, has emerged as a powerful tool in this domain. However, the complexity of force field development, a… ▽ More Machine-learned interatomic potentials have revolutionized molecular dynamics simulations by providing quantum-mechanical accuracy at empirical-potential speeds. The graphics processing unit molecular dynamics (GPUMD) package, featuring the highly efficient neuroevolution potential (NEP) framework, has emerged as a powerful tool in this domain. However, the complexity of force field development, active learning, and trajectory post-processing often requires extensive manual scripting, imposing a steep learning curve on new users. To address this, we present GPUMDkit, a comprehensive and user-friendly toolkit that streamlines the entire simulation workflow for GPUMD and NEP. GPUMDkit integrates a suite of essential functionalities, including format conversion, structure sampling, property calculation, and data visualization, accessible through both interactive and command-line interfaces. Its modular, extensible architecture ensures accessibility for users of all experience levels while allowing seamless integration of new features. By automating complex tasks and enhancing productivity, GPUMDkit substantially lowers the barrier to using GPUMD and NEP programs. This article describes the program architecture and demonstrates its capabilities through practical applications. △ Less

Submitted 18 March, 2026; originally announced March 2026.

Comments: 17 pages, 7 figures

NEP-CG and NEP-AACG: Efficient coarse-grained and multiscale all-atom-coarse-grained neuroevolution potentials

Authors: Zheyong Fan, Wenjun Zhang, Zhenhao Zhang, Ke Xu, Xuecheng Shao, Haikuan Dong

Abstract: Machine-learned coarse-grained (CG) models often suffer from noisy training data, limiting their accuracy and transferability. We propose a method to generate low-noise training data based on the potential of mean force by constraining CG beads during atomistic simulations and accumulating time-averaged forces. Implemented within the neuroevolution potential (NEP) framework, our approach achieves… ▽ More Machine-learned coarse-grained (CG) models often suffer from noisy training data, limiting their accuracy and transferability. We propose a method to generate low-noise training data based on the potential of mean force by constraining CG beads during atomistic simulations and accumulating time-averaged forces. Implemented within the neuroevolution potential (NEP) framework, our approach achieves training accuracy comparable to atomistic models trained on density functional theory data. For liquid water, the NEP-CG model accurately reproduces densities from 1 bar to 1 GPa, successfully extrapolating beyond the 0.5 GPa training limit, with a virial correction essential for the correct equation of state. For an anisotropic C$_{60}$ monolayer, distinguishing crystallographically distinct bead types reduces stress errors by an order of magnitude and captures directional thermal conductivity. We further introduce a multiscale NEP-AACG model integrating all-atom (AA) and CG degrees of freedom, demonstrated for gold nanowire fracture at an experimentally relevant strain rate. Computational speeds for NEP-CG models reach hundreds to thousands of ns/day using a single consumer-grade GPU. This work provides a robust framework for constructing accurate, transferable, and efficient CG models across diverse systems. △ Less

Submitted 1 March, 2026; originally announced March 2026.

Comments: 12 pages, 8 figures

qNEP: A highly efficient neuroevolution potential with dynamic charges for large-scale atomistic simulations

Authors: Zheyong Fan, Benrui Tang, Esmée Berger, Ethan Berger, Erik Fransson, Ke Xu, Zihan Yan, Zhoulin Liu, Zichen Song, Haikuan Dong, Shunda Chen, Lei Li, Ziliang Wang, Yizhou Zhu, Julia Wiktor, Paul Erhart

Abstract: Although electrostatics can be incorporated into machine-learned interatomic potentials, existing approaches are computationally very demanding, limiting large-scale, long-time simulations of electrostatics-driven phenomena such as dielectric response, infrared activity, and field-matter coupling. Here, we extend the neuroevolution potential (NEP), a highly efficient machine-learned interatomic po… ▽ More Although electrostatics can be incorporated into machine-learned interatomic potentials, existing approaches are computationally very demanding, limiting large-scale, long-time simulations of electrostatics-driven phenomena such as dielectric response, infrared activity, and field-matter coupling. Here, we extend the neuroevolution potential (NEP), a highly efficient machine-learned interatomic potential, to a charge-aware framework (qNEP) by introducing explicit, environment-dependent partial charges. Each ionic partial charge is represented by a neural network as a function of the local descriptor vector, analogous to the NEP site-energy model. This formulation enables the direct prediction of the Born effective charge tensor for each ion and, consequently, the polarization. As a result, dielectric properties, infrared spectra, and coupling to external electric fields can be evaluated within a unified framework. We derive consistent expressions for the forces and virials that explicitly account for the position dependence of the partial charges. The qNEP method has been implemented in the free-and-open-source GPUMD package, with support for both Ewald summation and particle-particle particle-mesh treatments of electrostatics. We demonstrate the accuracy and efficiency of the qNEP approach through representative applications to water, Li7La3Zr2O12, BaTiO3, and a magnesium-water interface. These results show that qNEP enables accurate atomistic simulations with explicit long-range electrostatics, scalable to million-atom systems on nanosecond time scales using consumer-grade GPUs. △ Less

Submitted 26 January, 2026; originally announced January 2026.

Comments: 17 pages, 7 figures

Erbium Probes of Magnetic Order in a Layered van der Waals Material

Authors: Guadalupe García-Arellano, Kang Xu, Arun Ramanathan, Jiayi Li, Gabriel I. López-Morales, Xavier Roy, Cyrus E. Dreyer, Carlos A. Meriles

Abstract: There is growing interest in characterizing magnetic order and dynamics in two-dimensional magnets, yet most efforts to date rely on external probes that interrogate the sample from tens of nanometers away and inevitably average over that length scale. Here we use internal, lattice-embedded Er3+ defects in CrSBr as atomic-scale probes, accessing their telecom-band photoluminescence with spectrosco… ▽ More There is growing interest in characterizing magnetic order and dynamics in two-dimensional magnets, yet most efforts to date rely on external probes that interrogate the sample from tens of nanometers away and inevitably average over that length scale. Here we use internal, lattice-embedded Er3+ defects in CrSBr as atomic-scale probes, accessing their telecom-band photoluminescence with spectroscopy and temperature-dependent confocal imaging to read out magnetism from within the material. At room temperature we observe narrow, long-lived photoluminescence (PL) lines in the telecom band, characteristic of erbium emitters. Upon cooling to 3 K and reheating, the Er3+ PL intensity and excited-state lifetime display pronounced thermal hysteresis with a minimum near 132 K, at the reported antiferromagnetic (AFM) transition of CrSBr. Remarkably, we observe magnetic signatures persisting over a broader temperature range than expected from bulk benchmarks, suggesting nanoscale magnetic order that locally survives beyond the nominal phase boundary. Further, a moderate in-plane field of 0.3 T shifts the PL minimum by +8 K, which we tentatively associate to field-biased ferromagnetic correlations. △ Less

Submitted 24 January, 2026; originally announced January 2026.

Data-driven active learning approaches for accelerating materials discovery

Authors: Jiaxin Chen, Tianjiao Wan, Hui Geng, Liang Xiong, Guohong Wang, Yihan Zhao, Longxiang Deng, Zijian Gao, Susu Fang, Zheng Luo, Huaimin Wang, Shanshan Wang, Kele Xu

Abstract: Materials discovery is a cornerstone of modern technological advancement, yet it remains constrained by traditional trial-and-error paradigms and the inherent bias of human intuition. Artificial intelligence (AI) has emerged as a transformative tool in materials science by effectively modeling structure-property relationships. Despite substantial efforts to enhance model expressiveness, data effic… ▽ More Materials discovery is a cornerstone of modern technological advancement, yet it remains constrained by traditional trial-and-error paradigms and the inherent bias of human intuition. Artificial intelligence (AI) has emerged as a transformative tool in materials science by effectively modeling structure-property relationships. Despite substantial efforts to enhance model expressiveness, data efficiency remains an equally critical challenge, given the limited availability of experimental and computational resources. Active learning (AL), as a data-driven machine learning paradigm, has shown great promise for discovering novel materials and enabling the efficient navigation of vast materials spaces. In this review, we follow the evolution of sampling strategy design techniques in AL, from Bayesian optimization to advanced deep learning-based strategies. We then highlight how AL enhances data efficiency across various data regimes, ranging from task-specific settings with limited data to the development of general-purpose datasets and large-scale models. We further provide a systematic overview of AL applications throughout the materials research pipeline, including computational simulation, composition and structural design, process optimization, and self-driving laboratory systems. Finally, we pinpoint key challenges and future perspectives of AL in materials discovery. △ Less

Submitted 1 February, 2026; v1 submitted 11 January, 2026; originally announced January 2026.

Electric field switching of altermagnetic spin-splitting in multiferroic skyrmions

Authors: Gui Wang, Yuhang Li, Bin Li, Xianzhe Chen, Jianting Dong, Weizhao Chen, Xiaobing Chen, Naifu Zheng, Maosen Guo, Aomei Tong, Hua Bai, Hongrui Zhang, Yifan Gao, Kaiwen Shen, Jiangyuan Zhu, Jiahao Han, Yingfen Wei, Hao Jiang, Xumeng Zhang, Ming Wang, Kebiao Xu, Wu Shi, Pengfei Wang, Jia Zhang, Qihang Liu , et al. (4 additional authors not shown)

Abstract: Magnetic skyrmions are localized magnetic structures that retain their shape and stability over time, thanks to their topological nature. Recent theoretical and experimental progress has laid the groundwork for understanding magnetic skyrmions characterized by negligible net magnetization and ultrafast dynamics. Notably, skyrmions emerging in materials with altermagnetism, a novel magnetic phase f… ▽ More Magnetic skyrmions are localized magnetic structures that retain their shape and stability over time, thanks to their topological nature. Recent theoretical and experimental progress has laid the groundwork for understanding magnetic skyrmions characterized by negligible net magnetization and ultrafast dynamics. Notably, skyrmions emerging in materials with altermagnetism, a novel magnetic phase featuring lifted Kramers degeneracy-have remained unreported until now. In this study, we demonstrate that BiFeO3, a multiferroic renowned for its strong coupling between ferroelectricity and magnetism, can transit from a spin cycloid to a Neel-type skyrmion under antidamping spin-orbit torque at room temperature. Strikingly, the altermagnetic spin splitting within BiFeO3 skyrmion can be reversed through the application of an electric field, revealed via the Circular photogalvanic effect. This quasiparticle, which possesses a neutral topological charge, holds substantial promise for diverse applications-most notably, enabling the development of unconventional computing systems with low power consumption and magnetoelectric controllability. △ Less

Submitted 10 January, 2026; originally announced January 2026.

Interference-Induced Suppression of Doublon Transport and Prethermalization in the Extended Bose-Hubbard Model

Authors: Zhen-Ting Bao, Kai Xu, Heng Fan

Abstract: The coherent mobility of doublons, arising from second-order virtual dissociation-recombination processes, fundamentally limits their use as information carriers in the strongly interacting Bose-Hubbard model. We propose a disorder-free suppression mechanism by introducing an optimized nearest-neighbor pair-hopping term that destructively interferes with the dominant virtual hopping channel. Using… ▽ More The coherent mobility of doublons, arising from second-order virtual dissociation-recombination processes, fundamentally limits their use as information carriers in the strongly interacting Bose-Hubbard model. We propose a disorder-free suppression mechanism by introducing an optimized nearest-neighbor pair-hopping term that destructively interferes with the dominant virtual hopping channel. Using the third-order Schrieffer-Wolff transformation, we derive an analytical optimal condition that accounts for lattice geometry corrections. Exact numerical simulations demonstrate that this optimized scheme achieves near-complete dynamical arrest and entanglement preservation in one-dimensional chains, while in two-dimensional square lattices, it significantly suppresses ballistic spreading yet permits a slow residual expansion. Furthermore, in the many-body regime, finite-size scaling analysis identifies the observed long-lived density-wave order as a prethermal plateau emerging from the dramatic separation of microscopic and thermalization timescales. △ Less

Submitted 29 March, 2026; v1 submitted 7 January, 2026; originally announced January 2026.

Exceptional Alkaline Methanol Electrooxidation on Bi-modified Pt3M Intermetallics: Kinetic Origins and an OH Binding Energy Descriptor

Authors: Lecheng Liang, Hengyu Li, Shao Ye, Peng Li, Kaiyang Xu, Jinhui Liang, Binwen Zeng, Bo Shen, Taisuke Ozaki, Zhiming Cui

Abstract: The exploration of advanced CO-free catalysts and clarifying the ambiguous kinetic origins and governing factors would undoubtedly open up opportunities to overcome the sluggish kinetics of methanol electrooxidation and promote the development of direct methanol fuel cells. Herein, we constructed a family of Bi-modified Pt3M intermetallic catalysts (Bi-Pt3M/C, M=Cr, Mn, Co, Zn, In, Ga, and Sn) tha… ▽ More The exploration of advanced CO-free catalysts and clarifying the ambiguous kinetic origins and governing factors would undoubtedly open up opportunities to overcome the sluggish kinetics of methanol electrooxidation and promote the development of direct methanol fuel cells. Herein, we constructed a family of Bi-modified Pt3M intermetallic catalysts (Bi-Pt3M/C, M=Cr, Mn, Co, Zn, In, Ga, and Sn) that follow CO-free dominated pathway and exhibit exceptional catalytic activity. More significantly, leveraging this platform, we have identified the pivotal factor governing the reaction kinetics in CO-free pathway, namely OH binding energy (OHBE). This arises because the rate-determining step (RDS) encompasses both C-H bond activation and water dissociation, whose respective barriers can be reflected by the OHBE. Accordingly, OHBE can act as an activity descriptor. Specifically, Bi-Pt3In/C stands out from other Bi-Pt3M/C and delivers the unprecedented mass activity of 36.7 A mgPt-1 at peak potential, far exceeding state-of-the-art Pt-based catalysts reported to date. Taking Bi-Pt3In/C as a proof of concept, we clearly elucidate the origin of enhanced MOR activity by combining theoretical calculations, kinetic isotope effects, and formaldehyde electrooxidation. Moreover, there exhibits a volcano-type trend between OHBE and the activity of Bi-Pt3M/C. Beyond the discovery of ultrahigh-performance catalysts, these findings provide a detailed mechanistic picture of RDS and offer an innovative design principle for advanced catalysts. △ Less

Submitted 12 December, 2025; originally announced December 2025.

Robust Paramagnon and Acoustic Plasmon in a Photo-excited Electron-doped Cuprate Superconductor

Authors: Daniel Jost, Jiarui Li, Jordyn Hales, Jonathan Sobota, Giacomo Merzoni, Leonardo Martinelli, Shuhan Ding, Kejun Xu, Justine Schlappa, Andreas Scherz, Robert Carley, Benjamin E. Van Kuiken, Teguh C. Asmara, Le Phuong Hoang, Laurent Mercadier, Sergii Parchenko, Martin Teichmann, Patrick S. Kirchmann, Giacomo Ghiringhelli, Brian Moritz, Zhi-Xun Shen, Thomas P. Devereaux, Yao Wang, Wei-Sheng Lee

Abstract: Characterizing the spin and charge degrees of freedom in high-temperature superconducting cuprates under non-equilibrium conditions provides new insights into their electronic correlations. However, their collective dynamics have been largely unexplored due to experimental challenges. Here, we use time-resolved resonant inelastic X-ray scattering (trRIXS) at the Cu $L_3$-edge to simultaneously tra… ▽ More Characterizing the spin and charge degrees of freedom in high-temperature superconducting cuprates under non-equilibrium conditions provides new insights into their electronic correlations. However, their collective dynamics have been largely unexplored due to experimental challenges. Here, we use time-resolved resonant inelastic X-ray scattering (trRIXS) at the Cu $L_3$-edge to simultaneously track the collective spin (paramagnon) and charge (acoustic plasmon) dynamics in an optimally electron-doped cuprate driven out-of-equilibrium by a femtosecond pump laser pulse. Upon pumping, we observed an anti-Stokes signal associated with paramagnon generation, which modifies the paramagnon dispersion near the zone center, though the bandwidth remained unchanged, suggesting no significant alteration to spin exchange interactions. Simultaneously, in the charge sector, the acoustic plasmon's energy and spectral weight decreased, suggesting a light-induced redistribution of charge carriers. The variations of both the paramagnon and the plasmon were locked in time, demonstrating a robust intertwining between the spin and charge degrees of freedom on a femtosecond timescale, even in this non-equilibrium state. △ Less

Submitted 26 November, 2025; originally announced November 2025.

Device-Scale Atomistic Simulations of Heat Transport in Advanced Field-Effect Transistors

Authors: Ke Xu, Gang Wang, Ting Liang, Yang Xiao, Dongliang Ding, Haichang Guo, Xiang Gao, Lei Tong, Xi Wan, Gang Zhang, Jianbin Xu

Abstract: Self-heating in next-generation, high-power-density field-effect transistor limits performance and complicates fabrication. Here, we introduce NEP-FET, a machine-learned framework for device-scale heat transport simulations of field-effect transistors. Built upon the neuroevolution potential, the model extends a subset of the OMat24 dataset through an active-learning workflow to generate a chemica… ▽ More Self-heating in next-generation, high-power-density field-effect transistor limits performance and complicates fabrication. Here, we introduce NEP-FET, a machine-learned framework for device-scale heat transport simulations of field-effect transistors. Built upon the neuroevolution potential, the model extends a subset of the OMat24 dataset through an active-learning workflow to generate a chemically diverse, interface-rich reference set. Coupled with the FETMOD structure generator module, NEP-FET can simulate realistic field-effect transistor geometries at sub-micrometer scales containing millions of atoms, and delivers atomistic predictions of temperature fields, per-atom heat flux, and thermal stress in device structures with high fidelity. This framework enables rapid estimation of device-level metrics, including heat-flux density and effective thermal conductivity. Our results reveal pronounced differences in temperature distribution between fin-type and gate-all-around transistor architectures. The framework closes a key gap in multiscale device modeling by combining near-quantum-mechanical accuracy with device-scale throughput, providing a systematic route to explore heat transport and thermo-mechanical coupling in advanced transistors. △ Less

Submitted 25 November, 2025; v1 submitted 24 November, 2025; originally announced November 2025.

Comments: 10 pages, 4 figures, 46 conferences

Defect Engineered Hexagonal-Boron Nitride Enables Ionic Conduction for Lithium Metal Batteries

Authors: Yecun Wu, Yan-Kai Tzeng, Hao Chen, Kun Xu, Gangbin Yan, Takashi Taniguchi, Kenji Watanabe, Arun Majumdar, Yi Cui, Steven Chu

Abstract: The practical implementation of lithium-metal anodes has been hindered by uncontrollable dendrite formation and interfacial instability. This study presents a defect-engineering approach of a chemically stable and electrically insulating interfacial layer of hexagonal boron nitride (h-BN) that markedly enhances ionic conductivity through argon ion irradiation. Initially, the electrochemical perfor… ▽ More The practical implementation of lithium-metal anodes has been hindered by uncontrollable dendrite formation and interfacial instability. This study presents a defect-engineering approach of a chemically stable and electrically insulating interfacial layer of hexagonal boron nitride (h-BN) that markedly enhances ionic conductivity through argon ion irradiation. Initially, the electrochemical performance from commercially available, large-area chemical vapor deposition (CVD)-grown h-BN films with industrial-scale argon ion implantation motivated our subsequent detailed investigations using lab-scale exfoliated single-crystal h-BN flakes. Integration of these exfoliated flakes into a hybrid microfluidic-microelectronic chip provided direct evidence that controlled vacancy defects transform h-BN into an efficient lithium-ion conductor while preserving its intrinsic electrical insulation. Experimental validation confirmed improved lithium-metal anode stability, achieving dendrite-free cycling with Li plating/stripping Coulombic efficiencies exceeding 99.5% about 1000 cycles. Further assemble of irradiated h-BN in lithium-sulfur batteries effectively mitigates the polysulfide shuttle effect, sustaining over 97% specific capacity around 300 cycles. These results establish a robust, scalable interface-engineering route for next-generation lithium-metal batteries that combine high ionic transport with excellent electrical insulation. △ Less

Submitted 30 October, 2025; originally announced October 2025.

Repulsively Bound Hadrons in a $\mathbb{Z}_2$ Lattice Gauge Theory

Authors: Sayak Guha Roy, Vaibhav Sharma, Kaidi Xu, Umberto Borla, Jad C. Halimeh, Kaden R. A. Hazzard

Abstract: The $\mathbb{Z}_2$ lattice gauge theory is a paradigmatic model that exhibits gauge-field-mediated-confinement of pairs of particles into mesons, drawing connections to quantum chromodynamics. In the absence of any additional attractive interactions between particles, mesons are not known to bind in this model. Here, we show that resonant pair-production terms give rise to two separate mechanisms… ▽ More The $\mathbb{Z}_2$ lattice gauge theory is a paradigmatic model that exhibits gauge-field-mediated-confinement of pairs of particles into mesons, drawing connections to quantum chromodynamics. In the absence of any additional attractive interactions between particles, mesons are not known to bind in this model. Here, we show that resonant pair-production terms give rise to two separate mechanisms to form stable ``hadron'' bound states of two mesons: either induced by an effective attractive interaction, or a new dynamical binding mechanism induced by an effective repulsion. The repulsively bound hadron is a high-energy state stabilized by being energetically separated from the two-meson continuum through quantum fluctuations of the gauge fields. We study the dynamical formation of this bound state starting from local excitations. We use matrix product state techniques based on the time-evolving block decimation algorithm to perform our numerical simulations and analyze the effect of model parameters on hadron formation. Furthermore, we derive an effective model that explains its formation. Our findings are amenable to experimental observation on modern quantum hardware such as superconducting qubits, trapped ions, and Rydberg atom arrays. △ Less

Submitted 11 February, 2026; v1 submitted 21 October, 2025; originally announced October 2025.

Comments: 10 + 12 pages, 3 + 13 figures

Two-Dimensional Na2LiAlP2 Crystal for High-Performance Field-Effect Transistors

Authors: Run-Jie Peng, Xing-Yu Wang, Jun-Hui Yuan, Nian-Nian Yu, Kan-Hao Xue, Jiafu Wang, Pan Zhang

Abstract: High-performance, low-power transistors are core components of advanced integrated circuits, and the ultimate limitation of Moore's law has made the search for new alternative pathways an urgent priority. Two-dimensional (2D) materials have become the most promising exploration target due to their exceptional electronic properties and scalability. In this work, we conducted device transport resear… ▽ More High-performance, low-power transistors are core components of advanced integrated circuits, and the ultimate limitation of Moore's law has made the search for new alternative pathways an urgent priority. Two-dimensional (2D) materials have become the most promising exploration target due to their exceptional electronic properties and scalability. In this work, we conducted device transport research on the previously proposed 2D quaternary semiconductor Na2LiAlP2 using the non-equilibrium Green's function method. The results demonstrate that even with a channel length of 5 nm, Na2LiAlP2 still exhibits excellent n-type transistor characteristics, fully meeting and surpassing the technical specifications outlined in the International Roadmap for Devices and Systems (IRDS). Encouragingly, the device can easily achieve the required on-state current of 900 μA/μm under low operating voltages of 0.1 V and 0.2 V. Moreover, at 0.1 V operating voltage, the device's subthreshold swing breaks through the theoretical limit of 60 mV/dec, reaching an astonishing value 30.33 mV/dec. Additionally, its p-type transistor performance also stands out with a subthreshold swing of ~50 mV/dec when the channel length is 7 nm. Our research not only showcases the exceptional transistor properties of Na2LiAlP2 but also further expands the research scope of 2D high-performance transistors. △ Less

Submitted 23 October, 2025; v1 submitted 14 October, 2025; originally announced October 2025.

Comments: 22 pages, 5 figures, 2 tables

High-current p-type transistors from precursor-engineered synthetic monolayer WSe$_2$

Authors: Anh Tuan Hoang, Kathryn Neilson, Kaikui Xu, Yucheng Yang, Stephanie M. Ribet, Tara Peña, Giulio D'Acunto, Young Suh Song, Anton E. O. Persson, William Millsaps, Colin Ophus, Matthew R. Rosenberger, Eric Pop, Andrew J. Mannix

Abstract: Monolayer tungsten diselenide (WSe$_2$) is a leading candidate for nanoscale complementary logic. However, high defect densities introduced during thin-film growth and device fabrication have limited p-type transistor performance. Here, we report a combined strategy of precursor-engineered chemical vapor deposition and damage-minimizing fabrication to overcome this limitation. By converting tungst… ▽ More Monolayer tungsten diselenide (WSe$_2$) is a leading candidate for nanoscale complementary logic. However, high defect densities introduced during thin-film growth and device fabrication have limited p-type transistor performance. Here, we report a combined strategy of precursor-engineered chemical vapor deposition and damage-minimizing fabrication to overcome this limitation. By converting tungsten trioxide and residual oxyselenides into reactive suboxides before growth, and precisely regulating selenium delivery during deposition, we synthesize uniform, centimeter-scale monolayer WSe$_2$ films with charged defect densities as low as $5 \times 10^{9}$ cm$^{-2}$. Transistors fabricated from these films achieve record p-type on-state current up to $888 μ$A$\cdotμ$m$^{-1}$ at $V_{\mathrm{DS}}=-1$ V, matching leading n-type devices. This leap in material quality closes the p-type performance gap without exotic doping or contact materials, marking a critical step towards complementary two-dimensional semiconductor circuits. △ Less

Submitted 8 September, 2025; originally announced September 2025.

Room-temperature anisotropic in-plane spin dynamics in graphene induced by PdSe$_2$ proximity

Authors: Juan F. Sierra, Josef Světlík, Williams Savero Torres, Lorenzo Camosi, Franz Herling, Thomas Guillet, Kai Xu, Juan Sebastián Reparaz, Vera Marinova, Dimitre Dimitrov, Sergio O. Valenzuela

Abstract: Van der Waals heterostructures offer a versatile platform for tailoring electrical, magnetic, optical, and spin transport properties of materials through proximity effects. Notably, hexagonal transition metal dichalcogenides have been shown to induce valley-Zeeman spin-orbit coupling (SOC) in graphene, resulting in significant spin lifetime anisotropy between in-plane and out-of-plane spin orienta… ▽ More Van der Waals heterostructures offer a versatile platform for tailoring electrical, magnetic, optical, and spin transport properties of materials through proximity effects. Notably, hexagonal transition metal dichalcogenides have been shown to induce valley-Zeeman spin-orbit coupling (SOC) in graphene, resulting in significant spin lifetime anisotropy between in-plane and out-of-plane spin orientations. However, in-plane lifetimes remain isotropic due to the inherent threefold symmetry of the heterostructure. Here, we demonstrate that pentagonal PdSe$_2$, characterised by unique in-plane anisotropy, induces an unprecedented gate-tunable SOC in graphene. Our measurements reveal a remarkable 10-fold modulation of the spin lifetime for spins oriented within the graphene plane at room temperature. Moreover, the directional dependence of the spin lifetimes, along the three spatial directions, suggests the existence of a persistent in-plane spin texture component that dominates the spin dynamics. These findings deepen our understanding of spin dynamics in van der Waals heterostructures and open avenues for designing and engineering novel topological phases in graphene-based heterostructures within the strong SOC regime. △ Less

Submitted 25 August, 2025; originally announced August 2025.

Journal ref: Nature Materials 24, 876-882 (2025)

Observation and Modulation of the Quantum Mpemba Effect on a Superconducting Quantum Processor

Authors: Yueshan Xu, Cai-Ping Fang, Bing-Jie Chen, Ming-Chuan Wang, Zi-Yong Ge, Yun-Hao Shi, Yu Liu, Cheng-Lin Deng, Kui Zhao, Zheng-He Liu, Tian-Ming Li, Hao Li, Ziting Wang, Gui-Han Liang, Da'er Feng, Xueyi Guo, Xu-Yang Gu, Yang He, Hao-Tian Liu, Zheng-Yang Mei, Yongxi Xiao, Yu Yan, Yi-Han Yu, Wei-Ping Yuan, Jia-Chi Zhang , et al. (11 additional authors not shown)

Abstract: In non-equilibrium quantum many-body systems, the quantum Mpemba effect (QME) emerges as a counterintuitive phenomenon: systems exhibiting greater initial symmetry breaking restore symmetry faster than those with less. While theoretical exploration of QME has surged, experimental studies on its multidimensional modulation remain limited. Here, we report the observation and control of QME using a s… ▽ More In non-equilibrium quantum many-body systems, the quantum Mpemba effect (QME) emerges as a counterintuitive phenomenon: systems exhibiting greater initial symmetry breaking restore symmetry faster than those with less. While theoretical exploration of QME has surged, experimental studies on its multidimensional modulation remain limited. Here, we report the observation and control of QME using a superconducting processor featuring a unique fully connected, tunable-coupling architecture that enables precise modulation from short- to long-range interactions. This platform allows independent manipulation of coupling regimes, on-site potentials, and initial states, elucidating their roles in QME. To quantify symmetry restoration, we employ entanglement asymmetry (EA) -- the relative entropy between a subsystem reduced density matrix and its symmetric projection -- as a sensitive probe of symmetry breaking. In strong short-range coupling regimes, EA crossovers during quenches from tilted Néel states confirm the presence of QME. In contrast, in intermediate coupling regimes, synchronized EA and entanglement entropy dynamics reveal the suppression of QME. Remarkably, QME reemerges with the introduction of on-site linear potentials or quenches from tilted ferromagnetic states, the latter proving robust against on-site disorder. Our study provides the first demonstration of flexible QME modulation on a superconducting platform with multiple controllable parameters, shedding light on quantum many-body non-equilibrium dynamics and opening avenues for quantum information applications. △ Less

Submitted 11 August, 2025; originally announced August 2025.

Role of Plaquette Term in Genuine $2+1$D String Dynamics on Quantum Simulators

Authors: Yizhuo Tian, N. S. Srivatsa, Kaidi Xu, Jesse J. Osborne, Umberto Borla, Jad C. Halimeh

Abstract: With the advent of quantum simulators of $2+1$D lattice gauge theories (LGTs), a fundamental open question is under what circumstances the observed physics is genuinely $2+1$D rather than effectively $1+1$D. Here, we address this question in the ongoing strong effort to quantum-simulate string dynamics in $2+1$D LGTs on state-of-the-art quantum hardware. Through tensor network simulations and anal… ▽ More With the advent of quantum simulators of $2+1$D lattice gauge theories (LGTs), a fundamental open question is under what circumstances the observed physics is genuinely $2+1$D rather than effectively $1+1$D. Here, we address this question in the ongoing strong effort to quantum-simulate string dynamics in $2+1$D LGTs on state-of-the-art quantum hardware. Through tensor network simulations and analytic derivations, we show that the plaquette term, which represents a magnetic field and only emerges in $d>1$ spatial dimensions, plays a crucial role in \textit{genuine} $2+1$D string dynamics deep in the confined regime. In its absence and for minimal-length (Manhattan-distance) strings, we demonstrate how string breaking, although on a lattice in $d=2$ spatial dimensions, can be effectively mapped to a $1+1$D dynamical process independently of lattice geometry. Our findings not only answer the question of what qualifies as genuine $2+1$D string dynamics, but also serve as a clear guide for future quantum simulation experiments of $2+1$D LGTs. △ Less

Submitted 7 August, 2025; originally announced August 2025.

Comments: $10+9$ pages, $4+12$ figures

Single-shot optical precessional magnetization switching of Pt/Co/Pt ferromagnetic trilayers

Authors: Rui Xu, Chen Xiao, Xiangyu Zheng, Renyou Xu, Xiaobai Ning, Tianyi Zhu, Dinghao Ma, Kangning Xu, Fei Xu, Youguang Zhang, Boyu Zhang, Jiaqi Wei

Abstract: Ultra-fast magnetization switching triggered by a single femtosecond laser pulse has gained significant attention over the last decade for its potential in low-power consumption, high-speed memory applications. However, this phenomenon has been primarily observed in Gd-based ferrimagnetic materials, which are unsuitable for storage due to their weak perpendicular magnetic anisotropy (PMA). In this… ▽ More Ultra-fast magnetization switching triggered by a single femtosecond laser pulse has gained significant attention over the last decade for its potential in low-power consumption, high-speed memory applications. However, this phenomenon has been primarily observed in Gd-based ferrimagnetic materials, which are unsuitable for storage due to their weak perpendicular magnetic anisotropy (PMA). In this work, we demonstrated that applying a single laser pulse and an in-plane magnetic field can facilitate magnetic switching in a Pt/Co/Pt ferromagnetic trilayers stack within a specific laser power window. To further understand this phenomenon, we introduce a Cu layer to accelerates the re-establishment time of the anisotropy field of Pt/Co/Pt trilayers, which leads to bullseye-patterned magnetic switching. We have mapped state diagrams for these phenomena, and through micromagnetic simulations, we have determined that these switchings are influenced by thermal anisotropy torque, which can be modulated through PMA. These findings indicate that single-shot optical precessional magnetization reversal is feasible in a broader range of materials, opening avenues for the development of optical-magnetic memory devices. △ Less

Submitted 7 August, 2025; originally announced August 2025.

Many-body delocalization with a two-dimensional 70-qubit superconducting quantum simulator

Authors: Tian-Ming Li, Zheng-Hang Sun, Yun-Hao Shi, Zhen-Ting Bao, Yong-Yi Wang, Jia-Chi Zhang, Yu Liu, Cheng-Lin Deng, Yi-Han Yu, Zheng-He Liu, Chi-Tong Chen, Li Li, Hao Li, Hao-Tian Liu, Si-Yun Zhou, Zhen-Yu Peng, Yan-Jun Liu, Ziting Wang, Yue-Shan Xu, Kui Zhao, Yang He, Da'er Feng, Jia-Cheng Song, Cai-Ping Fang, Junrui Deng , et al. (13 additional authors not shown)

Abstract: Quantum many-body systems with sufficiently strong disorder can exhibit a non-equilibrium phenomenon, known as the many-body localization (MBL), which is distinct from conventional thermalization. While the MBL regime has been extensively studied in one dimension, its existence in higher dimensions remains elusive, challenged by the avalanche instability. Here, using a 70-qubit two-dimensional (2D… ▽ More Quantum many-body systems with sufficiently strong disorder can exhibit a non-equilibrium phenomenon, known as the many-body localization (MBL), which is distinct from conventional thermalization. While the MBL regime has been extensively studied in one dimension, its existence in higher dimensions remains elusive, challenged by the avalanche instability. Here, using a 70-qubit two-dimensional (2D) superconducting quantum simulator, we experimentally explore the robustness of the MBL regime in controlled finite-size 2D systems. We observe that the decay of imbalance becomes more pronounced with increasing system sizes, scaling up from 21, 42 to 70 qubits, with a relatively large disorder strength, and for the first time, provide an evidence for the many-body delocalization in 2D disordered systems. Our experimental results are consistent with the avalanche theory that predicts the instability of MBL regime beyond one spatial dimension. This work establishes a scalable platform for probing high-dimensional non-equilibrium phases of matter and their finite-size effects using superconducting quantum circuits. △ Less

Submitted 22 July, 2025; originally announced July 2025.

Comments: main text: 7 pages, 3 figures; supplementary information: 19 pages, 17 figures

The occupation dependent DFT-1/2 method

Authors: Shengxin Yang, Jiangzhen Shi, Kan-Hao Xue, Jun-Hui Yuan, Xiangshui Miao

Abstract: There has been a high demand in rectifying the band gap under-estimation problem in density functional theory (DFT), while keeping the computational load at the same level as local density approximation. DFT-1/2 and shell DFT-1/2 are useful attempts, as they correct the spurious electron self-interaction through the application of self-energy potentials, which pull down the valence band. Neverthel… ▽ More There has been a high demand in rectifying the band gap under-estimation problem in density functional theory (DFT), while keeping the computational load at the same level as local density approximation. DFT-1/2 and shell DFT-1/2 are useful attempts, as they correct the spurious electron self-interaction through the application of self-energy potentials, which pull down the valence band. Nevertheless, the self-energy potential inevitably disturbs the conduction band, and these two methods fail for semiconductors whose hole and electron are entangled in the same shell-like regions. In this work, we introduce the occupation-dependent DFT-1/2 method, where conduction band states are not subject to the additional self-energy potential disturbance. This methodology works for difficult cases such as $\text{Li}_2\text{O}_2$, $\text{Cu}_2\text{O}$ and two-dimensional semiconductors. Using a shell-like region for the self-energy potential, and allowing for downscaling of the atomic self-energy potential (with an $A$ < 1 factor), the occupation-dependent shell DFT+$A$-1/2 method yields more accurate conduction band and valence band edge levels for monolayer $\text{MoS}_2$, compared with the computationally demanding hybrid functional approach. △ Less

Submitted 7 July, 2025; originally announced July 2025.

Comments: 19 pages, 10 figures, 1 table

String Breaking Dynamics and Glueball Formation in a $2+1$D Lattice Gauge Theory

Authors: Kaidi Xu, Umberto Borla, Sergej Moroz, Jad C. Halimeh

Abstract: With the advent of advanced quantum processors capable of probing lattice gauge theories (LGTs) in higher spatial dimensions, it is crucial to understand string dynamics in such models to guide upcoming experiments and to make connections to high-energy physics (HEP). Using tensor network methods, we study the far-from-equilibrium quench dynamics of electric flux strings between two static charges… ▽ More With the advent of advanced quantum processors capable of probing lattice gauge theories (LGTs) in higher spatial dimensions, it is crucial to understand string dynamics in such models to guide upcoming experiments and to make connections to high-energy physics (HEP). Using tensor network methods, we study the far-from-equilibrium quench dynamics of electric flux strings between two static charges in the $2+1$D $\mathbb{Z}_2$ LGT with dynamical matter. We calculate the probabilities of finding the time-evolved wave function in string configurations of the same length as the initial string. At resonances determined by the the electric field strength and the mass, we identify various string breaking processes accompanied with matter creation. Away from resonance strings exhibit intriguing confined dynamics which, for strong electric fields, we fully characterize through effective perturbative models. Starting in maximal-length strings, we find that the wave function enters a dynamical regime where it splits into shorter strings and disconnected loops, with the latter bearing qualitative resemblance to glueballs in quantum chromodynamics (QCD). Our findings can be probed on state-of-the-art superconducting-qubit and trapped-ion quantum processors. △ Less

Submitted 2 July, 2025; originally announced July 2025.

Comments: $9+7$ pages, $4+8$ figures, $0+1$ table

Electron-magnon coupling at the interface of a "twin-twisted" antiferromagnet

Authors: Yue Sun, Fanhao Meng, Sijia Ke, Kun Xu, Hongrui Zhang, Aljoscha Soll, Zdeněk Sofer, Arun Majumdar, Ramamoorthy Ramesh, Jeffrey B. Neaton, Jie Yao, Joseph Orenstein

Abstract: We identify a "twin-twist" angle in orthorhombic two-dimensional magnets that maximizes interlayer orbital overlap and enables strong interfacial coupling. Focusing on the van der Waals antiferromagnet CrSBr, we show that this twist angle, near 72 deg, aligns diagonal lattice vectors across the layers, enhancing the interlayer hopping that is spin-forbidden in pristine systems and orbital-forbidde… ▽ More We identify a "twin-twist" angle in orthorhombic two-dimensional magnets that maximizes interlayer orbital overlap and enables strong interfacial coupling. Focusing on the van der Waals antiferromagnet CrSBr, we show that this twist angle, near 72 deg, aligns diagonal lattice vectors across the layers, enhancing the interlayer hopping that is spin-forbidden in pristine systems and orbital-forbidden in 90-deg-twisted samples. The enhanced hopping modifies the electronic structure and activates a novel mechanism for excitation of interfacial magnons. Using optical probes we discover that excitons on one side of the interface selectively excite magnons localized on the opposite side. We show that this cross-coupling phenomenon can be understood as a consequence of the spin-transfer torque as that arises as electrons tunnel across the twin-twisted interface. Our findings demonstrate that large-angle twisting in anisotropic 2D materials offers a powerful tool for engineering spin and charge transport through controlled interlayer hybridization, opening new avenues for twisted magnetism and strongly correlated moiré physics. △ Less

Submitted 11 June, 2025; originally announced June 2025.

Comments: 21+10 pages, 6+8 figures

Statistical Mechanics and Categorical Entropy

Authors: Haiqi Wu, Kai Xu

Abstract: This paper investigates the relationship between categorical entropy and von Neumann entropy of quantum lattices. We begin by studying the von Neumann entropy, proving that the average von Neumann entropy per site converges to the logarithm of an algebraic integer in the low-temperature and thermodynamic limits. Next, we turn to categorical entropy. Given an endofunctor of a saturated A-infinity-c… ▽ More This paper investigates the relationship between categorical entropy and von Neumann entropy of quantum lattices. We begin by studying the von Neumann entropy, proving that the average von Neumann entropy per site converges to the logarithm of an algebraic integer in the low-temperature and thermodynamic limits. Next, we turn to categorical entropy. Given an endofunctor of a saturated A-infinity-category, we construct a corresponding lattice model, through which the categorical entropy can be understood in terms of the information encoded in the model. Finally, by introducing a gauged lattice framework, we unify these two notions of entropy. This unification leads naturally to a sufficient condition for a conjectural algebraicity property of categorical entropy, suggesting a deeper structural connection between A-infinity-categories and statistical mechanics. △ Less

Submitted 24 May, 2025; originally announced May 2025.

Electronic origin of reorganization energy in interfacial electron transfer

Authors: Sonal Maroo, Leonardo Coello Escalante, Yizhe Wang, Matthew P. Erodici, Jonathon N. Nessralla, Ayana Tabo, Takashi Taniguchi, Kenji Watanabe, Ke Xu, David T. Limmer, D. Kwabena Bediako

Abstract: Electron transfer (ET) reactions underpin energy conversion and chemical transformations in both biological and abiological systems. The efficiency of any ET process relies on achieving a desired ET rate within an optimal driving force range. Marcus theory provides a microscopic framework for understanding the activation free energy, and thus the rate, of ET in terms of a key parameter: the reorga… ▽ More Electron transfer (ET) reactions underpin energy conversion and chemical transformations in both biological and abiological systems. The efficiency of any ET process relies on achieving a desired ET rate within an optimal driving force range. Marcus theory provides a microscopic framework for understanding the activation free energy, and thus the rate, of ET in terms of a key parameter: the reorganization energy. For electrified solid-liquid interfaces, it has long been conventionally understood that only factors in the electrolyte phase are responsible for determining the reorganization energy and the electronic density of states (DOS) of the electrode serves only to dictate the number of thermally accessible channels for ET. Here we show instead that the electrode DOS plays a central role in governing the reorganization energy, far outweighing its conventionally assumed role. Using atomically layered heterostructures, we tune the DOS of graphene and measure outer-sphere ET kinetics. We find the ensuing variation in ET rate arises from strong modulation in a reorganization energy associated with image potential localization in the electrode. This work redefines the traditional paradigm of heterogeneous ET kinetics, revealing a deeper role of the electrode electronic structure in interfacial reactivity. △ Less

Submitted 6 October, 2025; v1 submitted 16 May, 2025; originally announced May 2025.

Microwave-activated high-fidelity three-qubit gate scheme for fixed-frequency superconducting qubits

Authors: Kui Zhao, Wei-Guo Ma, Ziting Wang, Hao Li, Kaixuan Huang, Yun-Hao Shi, Kai Xu, Heng Fan

Abstract: Scalable superconducting quantum processors require balancing critical constraints in coherence, control complexity, and spectral crowding. Fixed-frequency architectures suppress flux noise and simplify control via all-microwave operations but remain limited by residual ZZ crosstalk. Here we propose a microwave-activated three-qubit gate protocol for fixed-frequency transmon qubits in the large-de… ▽ More Scalable superconducting quantum processors require balancing critical constraints in coherence, control complexity, and spectral crowding. Fixed-frequency architectures suppress flux noise and simplify control via all-microwave operations but remain limited by residual ZZ crosstalk. Here we propose a microwave-activated three-qubit gate protocol for fixed-frequency transmon qubits in the large-detuning regime ($|Δ| \gg g$), leveraging the third-order nonlinear interaction to coherently exchange $\ket{001} \leftrightarrow \ket{110}$ states. By incorporating a phase-compensated optimization protocol, numerical simulations demonstrate a high average gate fidelity exceeding $99.9\%$. Systematic error analysis identifies static long-range ZZ coupling as the dominant error source in multi-qubit systems, which can be suppressed via operations in the large-detuning regime ($\sim 1$ GHz). The protocol maintains process fidelities exceeding $98\%$ under decoherence, while demonstrating intrinsic robustness to fabrication-induced parameter variations and compatibility with existing all-microwave two-qubit gate architectures. This hardware-efficient strategy advances scalable quantum computing systems by improving coherence properties, reducing spectral congestion, and expanding the experimental toolkit for error-resilient quantum operations in the noisy intermediate-scale quantum era. △ Less

Submitted 16 October, 2025; v1 submitted 30 April, 2025; originally announced April 2025.

Comments: 16 pages, 11 figures

Journal ref: Phys. Rev. Applied 24, 034064 (2025)

NEP89: Universal neuroevolution potential for inorganic and organic materials across 89 elements

Authors: Ting Liang, Ke Xu, Eric Lindgren, Zherui Chen, Rui Zhao, Jiahui Liu, Esmée Berger, Benrui Tang, Bohan Zhang, Yanzhou Wang, Keke Song, Penghua Ying, Nan Xu, Haikuan Dong, Shunda Chen, Paul Erhart, Zheyong Fan, Tapio Ala-Nissila, Jianbin Xu

Abstract: While machine-learned interatomic potentials offer near-quantum-mechanical accuracy for atomistic simulations, many are material-specific or computationally intensive, limiting their broader use. Here we introduce NEP89, a foundation model based on neuroevolution potential architecture, delivering empirical-potential-like speed and high accuracy across 89 elements. A compact yet comprehensive trai… ▽ More While machine-learned interatomic potentials offer near-quantum-mechanical accuracy for atomistic simulations, many are material-specific or computationally intensive, limiting their broader use. Here we introduce NEP89, a foundation model based on neuroevolution potential architecture, delivering empirical-potential-like speed and high accuracy across 89 elements. A compact yet comprehensive training dataset covering inorganic and organic materials was curated through descriptor-space subsampling and iterative refinement across multiple datasets. NEP89 achieves competitive accuracy compared to representative foundation models while being three to four orders of magnitude more computationally efficient, enabling previously impractical large-scale atomistic simulations of inorganic and organic systems. In addition to its out-of-the-box applicability to diverse scenarios, including million-atom-scale compression of compositionally complex alloys, ion diffusion in solid-state electrolytes and water, rocksalt dissolution, methane combustion, and protein-ligand dynamics, NEP89 also supports fine-tuning for rapid adaptation to user-specific applications, such as mechanical, thermal, structural, and spectral properties of two-dimensional materials, metallic glasses, and organic crystals. △ Less

Submitted 10 June, 2025; v1 submitted 29 April, 2025; originally announced April 2025.

Comments: 14 pages, 5 figures in the main text; 1 supplementary table, 11 supplementary figures in the SI

Monitoring charge separation of individual cells in perovskite/silicon tandems via transient surface photovoltage spectroscopy

Authors: Maxim Simmonds, Ke Xu, Steve Albrecht, Lars Korte, Igal Levine

Abstract: Identification of charge carrier separation processes in perovskite/silicon tandem solar cells and recombination at buried interfaces of charge selective contacts is crucial for photovoltaic research. Here, intensity- and wavelength- dependent transient surface photovoltage (tr-SPV) is used to investigate slot-die-coated perovskite top layers deposited on n-type Heterojunction Silicon bottom cells… ▽ More Identification of charge carrier separation processes in perovskite/silicon tandem solar cells and recombination at buried interfaces of charge selective contacts is crucial for photovoltaic research. Here, intensity- and wavelength- dependent transient surface photovoltage (tr-SPV) is used to investigate slot-die-coated perovskite top layers deposited on n-type Heterojunction Silicon bottom cells. We show that using an appropriate combination of photon energy and/or bottom cell polarity, one can individually probe the buried interfaces of the bottom silicon cell or the perovskite`s buried interfaces of a tandem solar cell: For excitation with higher energy photons, time delays before the onset of a strong SPV signal indicate significant hole minority drift before separation in the silicon bottom cells. Furthermore, symmetric bottom Si heterojunction solar cell stacks can serve to investigate the top perovskite stack including its junction to the bottom cell, unhampered by photovoltages from the silicon substrate. Thus, investigation of the buried interfaces in tandem devices using time-resolved surface photovoltage is found to yield valuable information on charge carrier extraction at buried interfaces and demonstrates its unique potential compared to more conventional approaches that rely on photoluminescence decay kinetics. △ Less

Submitted 25 April, 2025; originally announced April 2025.

Optimizing thermoelectric performance of graphene antidot lattices via quantum transport and machine-learning molecular dynamics simulations

Authors: Yang Xiao, Yuqi Liu, Zihan Tan Bohan Zhang, Ke Xu, Zheyong Fan, Shunda Chen, Shiyun Xiong, Haikuan Dong

Abstract: Thermoelectric materials, which can convert waste heat to electricity or be utilized as solid-state coolers, hold promise for sustainable energy applications. However, optimizing thermoelectric performance remains a significant challenge due to the complex interplay between electronic and thermal transport properties. In this work, we systematically optimize $ZT$ in graphene antidot lattices (GALs… ▽ More Thermoelectric materials, which can convert waste heat to electricity or be utilized as solid-state coolers, hold promise for sustainable energy applications. However, optimizing thermoelectric performance remains a significant challenge due to the complex interplay between electronic and thermal transport properties. In this work, we systematically optimize $ZT$ in graphene antidot lattices (GALs), nanostructured graphene sheets with periodic nanopores characterized by two geometric parameters: the hexagonal unit cell side length $L$ and the antidot radius $R$. The lattice thermal conductivity is determined through machine-learned potential-driven molecular dynamics (MD) simulations, while electronic transport properties are computed using linear-scaling quantum transport in combination with MD trajectories based on a bond-length-dependent tight-binding model. This method is able to account for electron-phonon scattering, allowing access to diffusive transport in large-scale systems, overcoming limitations of previous methods based on nonequilibrium Green function formalism. Our results show that the introduction of the antidots effectively decouples lattice and electronic transport and lead to a favorable and significant violation of the Wiedemann-Franz law. We find that optimal $ZT$ values occur in GALs with intermediate $L$ and $R$, closely correlated with peak power factor values. Notably, thermoelectric performance peaks near room temperature, with maximal $ZT$ values approaching 2, highlighting GALs as promising candidates for high-performance thermoelectric energy conversion. △ Less

Submitted 24 April, 2025; originally announced April 2025.

Comments: 10 pages, 7 figures

Prethermalization by Random Multipolar Driving on a 78-Qubit Superconducting Processor

Authors: Zheng-He Liu, Yu Liu, Gui-Han Liang, Cheng-Lin Deng, Keyang Chen, Yun-Hao Shi, Tian-Ming Li, Lv Zhang, Bing-Jie Chen, Cai-Ping Fang, Da'er Feng, Xu-Yang Gu, Yang He, Kaixuan Huang, Hao Li, Hao-Tian Liu, Li Li, Zheng-Yang Mei, Zhen-Yu Peng, Jia-Cheng Song, Ming-Chuan Wang, Shuai-Li Wang, Ziting Wang, Yongxi Xiao, Minke Xu , et al. (21 additional authors not shown)

Abstract: Time-dependent drives hold the promise of realizing non-equilibrium many-body phenomena that are absent in undriven systems. Yet, drive-induced heating normally destabilizes the systems, which can be parametrically suppressed in the high-frequency regime by using periodic (Floquet) drives. It remains largely unknown to what extent highly controllable quantum simulators can suppress heating in non-… ▽ More Time-dependent drives hold the promise of realizing non-equilibrium many-body phenomena that are absent in undriven systems. Yet, drive-induced heating normally destabilizes the systems, which can be parametrically suppressed in the high-frequency regime by using periodic (Floquet) drives. It remains largely unknown to what extent highly controllable quantum simulators can suppress heating in non-periodically driven systems. Using the 78-qubit superconducting quantum processor, Chuang-tzu 2.0, we report the experimental observation of long-lived prethermal phases in many-body systems with tunable heating rates, driven by structured random protocols, characterized by $n$-multipolar temporal correlations. By measuring both the particle imbalance and subsystem entanglement entropy, we monitor the entire heating process over 1,000 driving cycles and observe the existence of the prethermal plateau. The prethermal lifetime is `doubly tunable': one way by driving frequency, the other by multipolar order; it grows algebraically with the frequency with the universal scaling exponent $2n{+}1$. Using quantum state tomography on different subsystems, we demonstrate a non-uniform spatial entanglement distribution and observe a crossover from area-law to volume-law entanglement scaling. With 78 qubits and 137 couplers in a 2D configuration, the entire far-from-equilibrium heating dynamics are beyond the reach of simulation using tensor-network numerical techniques. Our work highlights superconducting quantum processors as a powerful platform for exploring universal scaling laws and non-equilibrium phases of matter in driven systems in regimes where classical simulation faces formidable challenges. △ Less

Submitted 1 April, 2025; v1 submitted 27 March, 2025; originally announced March 2025.

Journal ref: Nature 650, 79-85 (2026)

Acceleration of shell DFT-1/2 in high-throughput calculations via cutoff radii prediction

Authors: Shanzhong Xie, Kan-Hao Xue, Zijian Zhou, Xiangshui Miao

Abstract: Shell DFT-1/2 is a fast band gap rectification method that is versatile for semiconductor supercell and superlattice calculations, which involves two cutoff radii that have to be optimized. Although such optimization is trivial in terms of time cost for a primitive cell, in high-throughput calculations this can be a big concern because most materials are themselves in small unit cells. The numerou… ▽ More Shell DFT-1/2 is a fast band gap rectification method that is versatile for semiconductor supercell and superlattice calculations, which involves two cutoff radii that have to be optimized. Although such optimization is trivial in terms of time cost for a primitive cell, in high-throughput calculations this can be a big concern because most materials are themselves in small unit cells. The numerous optimization trials increase the computational cost to orders of magnitudes higher. In this work, we construct a regression model for the prediction of the two cutoff radii based on chemical composition and primitive cell structure. Moreover, a model for metal and insulator classification is also given, with 95.2% accuracy. △ Less

Submitted 25 March, 2025; originally announced March 2025.

Comments: 15 pages, 4 figures, 2 tables, and with Supplementary Information

High-efficiency computational methodologies for electronic properties and structural characterization of Ge-Sb-Te based phase change materials

Authors: Shanzhong Xie, Kan-Hao Xue, Shaojie Yuan, Shengxin Yang, Heng Yu, Rongchuan Gu, Ming Xu, Xiangshui Miao

Abstract: Theoretical simulation to phase change materials such as Ge-Sb-Te has suffered from two methodology issues. On the one hand, there is a lack of efficient band gap correction method for density functional theory, which is suitable for these materials in both crystalline and amorphous phases, though the computational complexity should be kept at the local density approximation level. On the other ha… ▽ More Theoretical simulation to phase change materials such as Ge-Sb-Te has suffered from two methodology issues. On the one hand, there is a lack of efficient band gap correction method for density functional theory, which is suitable for these materials in both crystalline and amorphous phases, though the computational complexity should be kept at the local density approximation level. On the other hand, analysis of the coordination number in amorphous phases relies on an integration involving the radial distribution function, which adds to the complexity. In this work, we find that the shell DFT-1/2 method offers an overall band gap accuracy for phase change materials comparable to HSE06 hybrid functional, though its computational cost is around three orders of magnitude lower. Moreover, the mixed length-angle coordination number theory enables calculating the coordination numbers in the amorphous phase directly from the structure, with definite outcomes. The two methodologies could be helpful for high throughput simulation of phase change materials. △ Less

Submitted 18 March, 2025; originally announced March 2025.

Comments: 26 pages, 7 figures, 6 tables, and with Supplementary Information

Probing the ideal limit of interfacial thermal conductance in two-dimensional van der Waals heterostructures

Authors: Ting Liang, Ke Xu, Penghua Ying, Wenwu Jiang, Meng Han, Xin Wu, Wengen Ouyang, Yimin Yao, Xiaoliang Zeng, Zhenqiang Ye, Zheyong Fan, Jianbin Xu

Abstract: Probing the ideal limit of interfacial thermal conductance (ITC) in two-dimensional (2D) heterointerfaces is of paramount importance for assessing heat dissipation in 2D-based nanoelectronics. Using graphene/hexagonal boron nitride (Gr/$h$-BN), a structurally isomorphous heterostructure with minimal mass contrast, as a prototype, we develop an accurate yet highly efficient machine-learned potentia… ▽ More Probing the ideal limit of interfacial thermal conductance (ITC) in two-dimensional (2D) heterointerfaces is of paramount importance for assessing heat dissipation in 2D-based nanoelectronics. Using graphene/hexagonal boron nitride (Gr/$h$-BN), a structurally isomorphous heterostructure with minimal mass contrast, as a prototype, we develop an accurate yet highly efficient machine-learned potential (MLP) model, which drives nonequilibrium molecular dynamics (NEMD) simulations on a realistically large system with over 300,000 atoms, enabling us to report the ideal limit range of ITC for 2D heterostructures at room temperature. We further unveil an intriguing stacking-sequence-dependent ITC hierarchy in the Gr/$h$-BN heterostructure, which can be connected to moiré patterns and is likely universal in van der Waals layered materials. The underlying atomic-level mechanisms can be succinctly summarized as energy-favorable stacking sequences facilitating out-of-plane phonon energy transmission. This work demonstrates that MLP-driven MD simulations can serve as a new paradigm for probing and understanding thermal transport mechanisms in 2D heterostructures and other layered materials. △ Less

Submitted 19 February, 2025; originally announced February 2025.

Comments: 13 pages, 6 figures in the main text; 20 figures in the SI

Report number: 1-12

Journal ref: npj Computational Materials 2025

Quantum Avalanches in $\mathbb{Z}_2$-preserving Interacting Ising Majorana Chain

Authors: Lv Zhang, Kai Xu, Heng Fan

Abstract: Recent numerical works have revealed the instability of many-body localized (MBL) phase in disordered quantum many-body systems with finite system sizes and over finite timescales. This instability arises from Griffith regions that occur at the thermodynamic limit, which rapidly thermalize and affect the surrounding typical MBL regions, introducing an avalanche mechanism into the system. Here, we… ▽ More Recent numerical works have revealed the instability of many-body localized (MBL) phase in disordered quantum many-body systems with finite system sizes and over finite timescales. This instability arises from Griffith regions that occur at the thermodynamic limit, which rapidly thermalize and affect the surrounding typical MBL regions, introducing an avalanche mechanism into the system. Here, we consider the $\mathbb{Z}_2$-preserving interacting Ising Majorana chain model, which exhibits a more complex phase diagram, where an ergodic phase emerges between two MBL phases with different long-range order properties. We calculate the dynamic characteristics of the model when coupled to an infinite bath under perturbation, and through scaling behavior of the slowest thermalization rate, we find how critical disorder strengths in finite-size systems are affected by the avalanche mechanism. We also employe the embedded inclusion model and use the time evolution of mutual information between each spin and the artificial Griffith region to probe the diffusion of the thermal bubble. We observe that in finite-sized systems, the critical disorder strength gradually drifts away from the central. Our work demonstrate that both MBL paramagnetic phase and MBL spin-glass phase are unstable at finite sizes. △ Less

Submitted 10 January, 2025; originally announced January 2025.

Slow water in engineered nano-channels revealed by color-center-enabled sensing

Authors: Daniela Pagliero, Rohma Khan, Kapila Elkaduwe, Ankit Bhardwaj, Kang Xu, Abraham Wolcott, Gustavo López, Boya Radha, Nicolas Giovambattista, Carlos A. Meriles

Abstract: Nanoscale confinement of molecules in a fluid can result in enhanced viscosity, local fluidic order, or collective motion. Confinement also affects ion transport and/or the rate and equilibrium concentration in a chemical reaction, all of which makes it the subject of broad interest. Studying these effects, however, is notoriously difficult, mainly due to the lack of experimental methods with the… ▽ More Nanoscale confinement of molecules in a fluid can result in enhanced viscosity, local fluidic order, or collective motion. Confinement also affects ion transport and/or the rate and equilibrium concentration in a chemical reaction, all of which makes it the subject of broad interest. Studying these effects, however, is notoriously difficult, mainly due to the lack of experimental methods with the required sensitivity and spatial or time resolution. Here we leverage shallow nitrogen-vacancy (NV) centers in diamond to probe the dynamics of room-temperature water molecules entrapped within ~6-nm-tall channels formed between the diamond crystal and a suspended hexagonal boron nitride (hBN) flake. NV-enabled nuclear magnetic resonance measurements of confined water protons reveal a much reduced H2O self-diffusivity, orders of magnitude lower than in bulk water. We posit the slow dynamics stem from the accumulation of photogenerated carriers at the interface and trapped fluid, a notion we support with the help of molecular dynamics modeling. Our results provide feedback for theories describing interfacial water, and lay out a route for investigating other fluids under confinement. △ Less

Submitted 25 December, 2024; originally announced December 2024.

Emergence of topological defects and spin liquid in a two-orbital spin-fermion model on the honeycomb lattice

Authors: Kaidi Xu, Shan-Shan Wang, Rong Yu, Shuai Dong

Abstract: Stabilizing exotic quantum phases of matter, e.g. spin liquid, is an attractive topic in condensed matter. Here, by a Monte Carlo study of a two-orbital spin-fermion model on a honeycomb lattice, we show the cooperative effects of the orbital degeneracy of itinerant electrons and the exchange interaction of localized spins can significantly suppress both ferromagnetic and antiferromagnetic orders… ▽ More Stabilizing exotic quantum phases of matter, e.g. spin liquid, is an attractive topic in condensed matter. Here, by a Monte Carlo study of a two-orbital spin-fermion model on a honeycomb lattice, we show the cooperative effects of the orbital degeneracy of itinerant electrons and the exchange interaction of localized spins can significantly suppress both ferromagnetic and antiferromagnetic orders by generating topological defects and give rise to an intermediate spin liquid state via continuous phase transitions. This phase competition can also be achieved by tuning the electron filling. These results shed new light on realizing spin liquids on geometrically non-frustrated lattices. △ Less

Submitted 23 December, 2024; originally announced December 2024.

Comments: 7 pages, 4 figures

Journal ref: Physical Review B 111, 014413 (2025)

Sign of the Gap Temperature Dependence in CsPb(Br,Cl)3 Nanocrystals Determined by Cs-Rattler Mediated Electron-Phonon Coupling

Authors: S. Fasahat, N. Fiuza-Maneiro, B. Schäfer, K. Xu, S. Gómez-Graña, M. I. Alonso, L. Polavarapu, A. R. Goñi

Abstract: So far, the striking sign reversal in the near-ambient slope of the gap temperature dependence of colloidal CsPbCl3 perovskite nanocrystals (NCs) compared to its Br counterpart, remains unresolved. Pure bromide NCs exhibit a linear gap increase with increasing temperature, to which thermal expansion and electron-phonon interaction equally contribute. In contrast, the temperature slope for the chlo… ▽ More So far, the striking sign reversal in the near-ambient slope of the gap temperature dependence of colloidal CsPbCl3 perovskite nanocrystals (NCs) compared to its Br counterpart, remains unresolved. Pure bromide NCs exhibit a linear gap increase with increasing temperature, to which thermal expansion and electron-phonon interaction equally contribute. In contrast, the temperature slope for the chlorine compound gap is outspoken negative. By combining temperature and pressure-dependent photoluminescence on a series of CsPb(Br1-xClx)3 NCs, we unravel the origin of such inversion. Responsible is solely the electron-phonon interaction, undergoing a sudden change in sign and magnitude due to activation of an anomalous electron-phonon coupling mechanism linked to vibrational modes characterized by synchronous octahedral tilting and Cs rattling. This takes place in the shrunken orthorhombic NC lattice for Cl concentrations exceeding ca. 40%. We have thus clarified a puzzling result directly impacting the optoelectronic properties of lead halide perovskite NCs. △ Less

Submitted 20 November, 2024; originally announced November 2024.

Comments: 18 pages, 4 figures, 1 table

MSC Class: 81-05; 78-05 ACM Class: F.2.2; I.7

Journal ref: S. Fasahat, N. Fiuza-Maneiro, B. Schäfer, K. Xu, S. Gómez-Graña, M. I. Alonso, L. Polavarapu, and A. R. Goñi, J. Phys. Chem. Lett. \textbf{16}, 1134-1141 (2025)

NEP-MB-pol: A unified machine-learned framework for fast and accurate prediction of water's thermodynamic and transport properties

Authors: Ke Xu, Ting Liang, Nan Xu, Penghua Ying, Shunda Chen, Ning Wei, Jianbin Xu, Zheyong Fan

Abstract: Water's unique hydrogen-bonding network and anomalous properties pose significant challenges for accurately modeling its structural, thermodynamic, and transport behavior across varied conditions. Although machine-learned potentials have advanced the prediction of individual properties, a unified computational framework capable of simultaneously capturing water's complex and subtle properties with… ▽ More Water's unique hydrogen-bonding network and anomalous properties pose significant challenges for accurately modeling its structural, thermodynamic, and transport behavior across varied conditions. Although machine-learned potentials have advanced the prediction of individual properties, a unified computational framework capable of simultaneously capturing water's complex and subtle properties with high accuracy has remained elusive. Here, we address this challenge by introducing NEP-MB-pol, a highly accurate and efficient neuroevolution potential (NEP) trained on extensive many-body polarization (MB-pol) reference data approaching coupled-cluster-level accuracy, combined with path-integral molecular dynamics and quantum-correction techniques to incorporate nuclear quantum effects. This NEP-MB-pol framework reproduces experimentally measured structural, thermodynamic, and transport properties of water across a broad temperature range, achieving simultaneous, fast, and accurate prediction of self-diffusion coefficient, viscosity, and thermal conductivity. Our approach provides a unified and robust tool for exploring thermodynamic and transport properties of water under diverse conditions, with significant potential for broader applications across research fields. △ Less

Submitted 19 November, 2024; v1 submitted 14 November, 2024; originally announced November 2024.

Comments: 12 pages, 4 figures in the main text; 8 figures in the SI

Journal ref: npj Computational Materials, 11, 279 (2025)

Quantum Interference and Optical Tuning of Self-Trapped Exciton State in Double Halide Perovskite

Authors: Kai-Xuan Xu, Xin-bao Liu, Simin Pang, Zhe Zhang, Yubin Wang, Jiajun Luo, Jiang Tang, Qihua Xiong, Sheng Meng, Shiwu Gao, Jun Zhang

Abstract: Self-trapped excitons (STEs), renowned for their unique radiative properties, have been harnessed in diverse photonic devices. Yet, a full comprehension and manipulation of STEs remain elusive. In this study, we present novel experimental and theoretical evidence of the hybrid nature and optical tuning of the STEs state in Cs2Ag0.4Na0.6InCl6. The detection of Fano resonance in the laser energy-dep… ▽ More Self-trapped excitons (STEs), renowned for their unique radiative properties, have been harnessed in diverse photonic devices. Yet, a full comprehension and manipulation of STEs remain elusive. In this study, we present novel experimental and theoretical evidence of the hybrid nature and optical tuning of the STEs state in Cs2Ag0.4Na0.6InCl6. The detection of Fano resonance in the laser energy-dependent Raman and photoluminescence spectra indicates the emergence of an exciton-phonon hybrid state, a result of the robust quantum interference between the discrete phonon and continuous exciton states. Moreover, we showcase the ability to continuously adjust this hybrid state with the energy and intensity of the laser field. These significant findings lay the foundation for a comprehensive understanding of the nature of STE and its potential for state control. △ Less

Submitted 27 October, 2024; originally announced October 2024.

Exploring structure diversity in atomic resolution microscopy with graph neural networks

Authors: Zheng Luo, Ming Feng, Zijian Gao, Jinyang Yu, Liang Hu, Tao Wang, Shenao Xue, Shen Zhou, Fangping Ouyang, Dawei Feng, Kele Xu, Shanshan Wang

Abstract: The emergence of deep learning (DL) has provided great opportunities for the high-throughput analysis of atomic-resolution micrographs. However, the DL models trained by image patches in fixed size generally lack efficiency and flexibility when processing micrographs containing diversified atomic configurations. Herein, inspired by the similarity between the atomic structures and graphs, we descri… ▽ More The emergence of deep learning (DL) has provided great opportunities for the high-throughput analysis of atomic-resolution micrographs. However, the DL models trained by image patches in fixed size generally lack efficiency and flexibility when processing micrographs containing diversified atomic configurations. Herein, inspired by the similarity between the atomic structures and graphs, we describe a few-shot learning framework based on an equivariant graph neural network (EGNN) to analyze a library of atomic structures (e.g., vacancies, phases, grain boundaries, doping, etc.), showing significantly promoted robustness and three orders of magnitude reduced computing parameters compared to the image-driven DL models, which is especially evident for those aggregated vacancy lines with flexible lattice distortion. Besides, the intuitiveness of graphs enables quantitative and straightforward extraction of the atomic-scale structural features in batches, thus statistically unveiling the self-assembly dynamics of vacancy lines under electron beam irradiation. A versatile model toolkit is established by integrating EGNN sub-models for single structure recognition to process images involving varied configurations in the form of a task chain, leading to the discovery of novel doping configurations with superior electrocatalytic properties for hydrogen evolution reactions. This work provides a powerful tool to explore structure diversity in a fast, accurate, and intelligent manner. △ Less

Submitted 23 October, 2024; originally announced October 2024.

On the material genome of wurtzite ferroelectrics

Authors: Zijian Zhou, Kan-Hao Xue, Jinhai Huang, Heng Yu, Shengxin Yang, Shujuan Liu, Yiqun Wang, Xiangshui Miao

Abstract: As the dielectric film thickness shrinks to ~10 nm, some traditional wurtzite piezoelectric materials demonstrate ferroelectricity through element doping. Among them, Sc doped AlN and Mg doped ZnO are the most famous examples. While it is widely acknowledged that the dopant atoms effectively reduce the coercive field, enabling ferroelectric polarization switching, the material genome of these wurt… ▽ More As the dielectric film thickness shrinks to ~10 nm, some traditional wurtzite piezoelectric materials demonstrate ferroelectricity through element doping. Among them, Sc doped AlN and Mg doped ZnO are the most famous examples. While it is widely acknowledged that the dopant atoms effectively reduce the coercive field, enabling ferroelectric polarization switching, the material genome of these wurtzite (WZ) ferroelectrics is still less understood. In this work, we analyze the features of WZ ferroelectrics, ascribing them to five-coordination (5C) ferroelectrics, which may be compared with 6C ferroelectrics (perovskite-type) and 7C ferroelectrics (hafnia-like). In particular, the exact reason for their adopting the hexagonal WZ structure instead of the zinc blende structure is studied. Emphasis is paid to the degree of ionicity in promoting the hexagonal arrangement, and the phenomenon of layer distance compression is discovered and explained in WZ ferroelectrics. The role of element doping in coercive field reduction is understood within this context. △ Less

Submitted 7 January, 2025; v1 submitted 3 October, 2024; originally announced October 2024.

Comments: 5 figures

Structure evolution path of ferroelectric hafnium zirconium oxide nanocrystals under in-situ biasing

Authors: Yunzhe Zheng, Heng Yu, Tianjiao Xin, Kan-Hao Xue, Yilin Xu, Zhaomeng Gao, Cheng Liu, Qiwendong Zhao, Yonghui Zheng, Xiangshui Miao, Yan Cheng

Abstract: Fluorite-type $\mathrm{HfO_2}$-based ferroelectric (FE) oxides have rekindled interest in FE memories due to their compatibility with silicon processing and potential for high-density integration. The polarization characteristics of FE devices are governed by the dynamics of metastable domain structure evolution. Insightful design of FE devices for encoding and storage necessitates a comprehensive… ▽ More Fluorite-type $\mathrm{HfO_2}$-based ferroelectric (FE) oxides have rekindled interest in FE memories due to their compatibility with silicon processing and potential for high-density integration. The polarization characteristics of FE devices are governed by the dynamics of metastable domain structure evolution. Insightful design of FE devices for encoding and storage necessitates a comprehensive understanding of the internal structural evolution. Here, we demonstrate the evolution of domain structures through a transient polar orthorhombic (O)-$Pmn2_1$-like configuration via $in$-$situ$ biasing on $\mathrm{TiN/Hf_{0.5}Zr_{0.5}O_2/TiN}$ capacitors within spherical aberration-corrected transmission electron microscope, combined with theoretical calculations. Furthermore, it is directly evidenced that the non-FE O-$Pbca$ transforms into the FE O-$Pca2_1$ phase under electric field, with the polar axis of the FE-phase aligning towards the bias direction through ferroelastic transformation, thereby enhancing FE polarization. As cycling progresses further, however, the polar axis collapses, leading to FE degradation. These novel insights into the intricate structural evolution path under electrical field cycling facilitate optimization and design strategies for $\mathrm{HfO_2}$-based FE memory devices. △ Less

Submitted 17 September, 2024; originally announced September 2024.

Comments: 16 pages, 4 figures for the main text

Absence of Anomalous Electron-Phonon Coupling in the Temperature Renormalization of the Gap of CsPbBr$_3$ Nanocrystals

Authors: Shima Fasahat, Benedikt Schäfer, Kai Xu, Nadesh Fiuza-Maneiro, Sergio Gómez-Graña, M. Isabel Alonso, Lakshminarayana Polavarapu, Alejandro R. Goñi

Abstract: Metal halide perovskites exhibit a fairly linear increase of the bandgap with increasing temperature, when crystallized in a tetragonal or cubic phase. In general, both thermal expansion and electron-phonon interaction effects contribute equally to this variation of the gap with temperature. Herein, we have disentangled both contributions in the case of colloidal CsPbBr$_3$ nanocrystals (NCs) by m… ▽ More Metal halide perovskites exhibit a fairly linear increase of the bandgap with increasing temperature, when crystallized in a tetragonal or cubic phase. In general, both thermal expansion and electron-phonon interaction effects contribute equally to this variation of the gap with temperature. Herein, we have disentangled both contributions in the case of colloidal CsPbBr$_3$ nanocrystals (NCs) by means of photoluminescence (PL) measurements as a function of temperature (from 80 K to ambient) and hydrostatic pressure (from atmospheric to ca. 1 GPa). At around room temperature, CsPbBr$_3$ NCs also show a linear increase of the bandgap with temperature with a slope similar to that of the archetypal methylammonium lead iodide (MAPbI$_3$) perovskite. This is somehow unexpected in view of the recent observations in mixed-cation Cs$_x$MA$_{1-x}$PbI$_3$ single crystals with low Cs content, for which Cs incorporation caused a reduction by a factor of two in the temperature slope of the gap. This effect was ascribed to an anomalous electron-phonon interaction induced by the coupling with vibrational modes admixed with the Cs translational dynamics inside the cage voids. Thus, no trace of anomalous coupling is found in CsPbBr$_3$ NCs. In fact, we show that the linear temperature renormalization exhibited by the gap of CsPbBr$_3$ NCs is shared with most metal halide perovskites, due to a common bonding/antibonding and atomic orbital character of the electronic band-edge states. In this way, we provide a deeper understanding of the gap temperature dependence in the general case when the A-site cation dynamics is not involved in the electron-phonon interaction. △ Less

Submitted 10 September, 2024; originally announced September 2024.

Comments: 29 pages, including 4 figures, a long table and 2 pages of Supporting Information

Journal ref: S. Fasahat, B. Schäfer, K. Xu, N. Fiuza-Maneiro, S. Gómez-Graña, M. I. Alonso, L. Polavarapu, A. R. Goñi, J. Phys. Chem. C \textbf{129}, 453-463 (2025)

Highly efficient path-integral molecular dynamics simulations with GPUMD using neuroevolution potentials: Case studies on thermal properties of materials

Authors: Penghua Ying, Wenjiang Zhou, Lucas Svensson, Esmée Berger, Erik Fransson, Fredrik Eriksson, Ke Xu, Ting Liang, Jianbin Xu, Bai Song, Shunda Chen, Paul Erhart, Zheyong Fan

Abstract: Path-integral molecular dynamics (PIMD) simulations are crucial for accurately capturing nuclear quantum effects in materials. However, their computational intensity and reliance on multiple software packages often limit their applicability at large scales. Here, we present an integration of PIMD methods, including thermostatted ring-polymer molecular dynamics (TRPMD), into the open-source GPUMD p… ▽ More Path-integral molecular dynamics (PIMD) simulations are crucial for accurately capturing nuclear quantum effects in materials. However, their computational intensity and reliance on multiple software packages often limit their applicability at large scales. Here, we present an integration of PIMD methods, including thermostatted ring-polymer molecular dynamics (TRPMD), into the open-source GPUMD package, combined with highly accurate and efficient machine-learned neuroevolution potential (NEP) models. This approach achieves almost the accuracy of first-principles calculations with the computational efficiency of empirical potentials, enabling large-scale atomistic simulations that incorporate nuclear quantum effects. We demonstrate the efficacy of the combined NEP-PIMD approach by examining various thermal properties of diverse materials, including lithium hydride (LiH), three porous metal-organic frameworks (MOFs), liquid water, and elemental aluminum. For LiH, our NEP-PIMD simulations successfully capture the isotope effect, reproducing the experimentally observed dependence of the lattice parameter on the reduced mass. For MOFs, our results reveal that achieving good agreement with experimental data requires consideration of both nuclear quantum effects and dispersive interactions. For water, our PIMD simulations capture the significant impact of nuclear quantum effects on its microscopic structure. For aluminum, the TRPMD method effectively captures thermal expansion and phonon properties, aligning well with quantum mechanical predictions. This efficient NEP-PIMD approach opens new avenues for exploring complex material properties influenced by nuclear quantum effects, with potential applications across a broad range of materials. △ Less

Submitted 28 September, 2024; v1 submitted 6 September, 2024; originally announced September 2024.

Comments: 16 pages, 9 figures in the main text; 1 table and 8 figures in the SI

Journal ref: Journal of Chemical Physics 162, 064109 (2025)

Tailoring light holes in $β$-$Ga_{2}O_{3}$ via Anion-Anion Antibonding Coupling

Authors: Ke Xu, Qiaolin Yang, Wenhao Liu, Rong Zhang, Zhi Wang, Jiandong Ye

Abstract: A significant limitation of wide-bandgap materials is their low hole mobility related to localized holes with heavy effective masses ($m_h^*$). We identify in low-symmetric wide-bandgap compounds an anion-anion antibonding coupling (AAAC) effect as the intrinsic factor behind hole localization, which explains the extremely heavy $m_h^*$ and self-trapped hole (STH) formation observed in gallium oxi… ▽ More A significant limitation of wide-bandgap materials is their low hole mobility related to localized holes with heavy effective masses ($m_h^*$). We identify in low-symmetric wide-bandgap compounds an anion-anion antibonding coupling (AAAC) effect as the intrinsic factor behind hole localization, which explains the extremely heavy $m_h^*$ and self-trapped hole (STH) formation observed in gallium oxide ($β$-$Ga_{2}O_{3}$). We propose a design principle for achieving light holes by manipulating AAAC, demonstrating that specific strain conditions can reduce $m_h^*$ in $β$-$Ga_{2}O_{3}$ from 4.77 $m_0$ to 0.38 $m_0$, making it comparable to the electron mass (0.28 $m_0$), while also slightly suppresses the formation of self-trapped holes, evidenced by the reduction in the formation energy of hole polarons from -0.57 eV to -0.45 eV under tensile strain. The light holes show significant anisotropy, potentially enabling two-dimensional transport in bulk material. This study provides a fundamental understanding of hole mass enhancement and STH formation in novel wide-bandgap materials and suggest new pathways for engineering hole mobilities. △ Less

Submitted 13 January, 2025; v1 submitted 16 August, 2024; originally announced August 2024.

Comments: 23 pages, 1 table, 5 figures

Journal ref: Physical Review B 110, 235208 (2024)

Contrasting electron-phonon interaction between electron- and hole-doped cuprates

Authors: Qinda Guo, Ke-Jun Xu, Magnus H. Berntsen, Antonija Grubišić-Čabo, Maciej Dendzik, Thiagarajan Balasubramanian, Craig Polley, Su-Di Chen, Junfeng He, Yu He, Costel R. Rotundu, Young S. Lee, Makoto Hashimoto, Dong-Hui Lu, Thomas P. Devereaux, Dung-Hai Lee, Zhi-Xun Shen, Oscar Tjernberg

Abstract: Spin- and charge-lattice interactions are potential key factors in the microscopic mechanism of high-temperature superconductivity in cuprates. Although both interactions can dramatically shape the low-energy electronic structure, their phenomenological roles in superconductivity are usually investigated independently. Employing angle-resolved photoemission spectroscopy, we reveal the spectroscopi… ▽ More Spin- and charge-lattice interactions are potential key factors in the microscopic mechanism of high-temperature superconductivity in cuprates. Although both interactions can dramatically shape the low-energy electronic structure, their phenomenological roles in superconductivity are usually investigated independently. Employing angle-resolved photoemission spectroscopy, we reveal the spectroscopic fingerprint of short-range antiferromagnetic order in conjunction with enhanced electron-phonon interaction in the electron-doped cuprate superconductor $\mathrm{Nd_{1.85}Ce_{0.15}CuO_4}$. The observed mode coupling exhibits a strong momentum dependence that is in striking contrast to the node-antinode dichotomy previously observed in the hole-doped cuprates. Our results reveal an intimate relationship between electron-phonon coupling and antiferromagnetic fluctuations, which collectively sets the stage for unconventional superconductivity in the electron-doped cuprates. △ Less

Submitted 3 August, 2024; originally announced August 2024.

Photoinduced charge injection from shallow point defects in diamond into water

Authors: Kang Xu, Daniela Pagliero, Gabriel I. Lopez Morales, Johannes Flick, Abraham Wolcott, Carlos A. Meriles

Abstract: Thanks to its low or negative surface electron affinity and chemical inertness, diamond is attracting broad attention as a source material of solvated electrons produced by optical excitation of the solid-liquid interface. Unfortunately, its wide bandgap typically imposes the use of wavelengths in the ultra-violet range, hence complicating practical applications. Here we probe the photocurrent res… ▽ More Thanks to its low or negative surface electron affinity and chemical inertness, diamond is attracting broad attention as a source material of solvated electrons produced by optical excitation of the solid-liquid interface. Unfortunately, its wide bandgap typically imposes the use of wavelengths in the ultra-violet range, hence complicating practical applications. Here we probe the photocurrent response of water surrounded by single-crystal diamond surfaces engineered to host shallow nitrogen-vacancy (NV) centers. We observe clear signatures of diamond-induced photocurrent generation throughout the visible range and for wavelengths reaching up to 594 nm. Experiments as a function of laser power suggest that NV centers and other co-existing defects - likely in the form of surface traps - contribute to carrier injection, though we find that NVs dominate the system response in the limit of high illumination intensities. Given our growing understanding of near-surface NV centers and adjacent point defects, these results open new perspectives in the application of diamond-liquid interfaces to photo-carrier-initiated chemical and spin processes in fluids. △ Less

Submitted 20 July, 2024; originally announced July 2024.

Journal ref: ACS Appl. Mater. Interf. 16, 37226 (2024)