arXiv subjects

Lixin He

Publications and source records attributed to Lixin He.

At least 19 recordsLinked to original sources

arXiv2026

Interface-Controlled Phase Stability in Polymorphic HfO$_2$ Revealed by Machine-Learning Atomistic Simulations

HfO$_2$ exhibits rich polymorphism, and competition among different phases underpins many of its functional properties. Yet bulk free-energy relations alone cannot explain phase selection at mixed-phase boundaries, where interface orientation and structural continuity constrain collective rearrangements. Here, using machine-learning atomistic simulations and a Hf-centered local phase classification scheme, we show that crystallographic interface matching redirects phase competition and accessible transformation pathways. The M(100)/T(100) interface remains pinned as an M/T mixture throughout 3 ns simulations from 300 to 1800 K. M/PO, M/AO, and PO/AO interfaces retain two-phase coexistence up to 900 K, whereas all T/PO interfaces become PO-dominant. At 1800 K, all non-M interfaces become T-dominant, while M-containing interfaces retain a monoclinic majority. Nudged elastic band calculations reveal lower-barrier routes through interface states. For M(100)$\rightarrow$T(100), the interface-mediated route in a long cell ($\sim$12 nm) yields a barrier of 136.03 meV/f.u., 29.2 % lower than the direct route in a short cell ($\sim$3 nm). This difference is associated with sequential phase-front motion absent from the short cell. These results identify phase boundaries as active participants in phase stability and transformation and establish interface orientation and crystallographic matching as variables for stabilizing metastable polymorphs and directing phase conversion in HfO$_2$.

cond-mat.mtrl-sci↗

arXiv2026

Cartesian tensor equivariant machine-learning force field for spin-dependent atomistic simulations

Magnetic materials exhibit an intricate coupling between atomic structure and spin degrees of freedom, posing a fundamental challenge for atomistic simulations across experimentally relevant length and time scales. Here we introduce HotPP-Spin, a spin-dependent extension of HotPP for magnetic machine learning interatomic potentials, built on Cartesian tensor equivariant message passing. Atomic magnetic moments are treated as explicit axial-vector degrees of freedom, while spatial-inversion and time-reversal parities are propagated through the tensor couplings. This construction provides a unified representation of exchange-dominated and spin-orbit-induced interactions without imposing predefined analytical interaction forms. A scalar spin-dependent potential energy surface yields energy-conserving atomic forces and magnetic effective fields through differentiation. Benchmarks spanning collinear magnetism, noncollinear magnetism, and spin-orbit-coupling-induced magnetic anisotropy show that HotPP-Spin accurately describes magnetic energy landscapes, magnetic forces, and magnetic-order-dependent energy-volume relations within the same general framework. For H-phase monolayer VSe$_2$, stochastic spin-dynamics simulations using the learned magnetic effective fields locate the finite-size magnetic ordering crossover at 415--435~K, in close numerical agreement with the reported experimental value of $418.5\pm7.8$~K. These results establish Cartesian tensor message passing as a general route for connecting first-principles magnetic energetics with large-scale atomistic simulations of coupled structural and spin phenomena.

physics.comp-ph↗

arXiv2026

Optically Active Fractional Wannier-Center Displacement Drives Giant Second-Harmonic Generation

Electric polarization is a static ground-state Berry-phase property, whereas second-harmonic generation (SHG) and shift current are dynamical optical responses. Their connection is encoded in the shift vector, whose Brillouin-zone average is governed by the band-resolved Berry-phase polarization difference between the optically connected initial and final states. Here we exploit this geometric relation in quantized formal polarization (QFP) crystals, where symmetry-quantized formal-polarization branches correspond to fractional Wannier-center sectors. First-principles screening identifies noncentrosymmetric QFP materials with giant SHG responses, including $\mathrm{InNbBr}_6$ and $\mathrm{InPS}_3$. Band-resolved Berry-phase analysis shows that their dominant optical transitions connect occupied and low-lying unoccupied states whose Wannier centers lie at distinct fractional Wyckoff positions, producing a large transition-resolved Wannier-center displacement. This displacement gives rise to a large shift vector and a dominant shift-vector-related intraband contribution to the static SHG susceptibility. Our results show that symmetry-quantized formal polarization can become optically active through transitions between fractional Wannier-center sectors, providing a symmetry-guided route to giant SHG and shift-current responses.

cond-mat.mtrl-sci↗

arXiv2026

$G^0W^0$ implementation based on the pseudopotential and numerical-atomic-orbital basis-set framework: Algorithms and benchmarks

The $GW$ method delivers substantially improved accuracy in electronic band structure calculations over conventional Kohn-Sham density functional theory (KS-DFT) by explicitly incorporating the electron self-energy effect beyond mean-field approximations. Despite many existing implementations, a periodic $GW$ implementation within the framework of numerical atomic orbitals (NAO) combined with the pseudopotential (PP) scheme has not been reported. This is urgently needed given the increasing popularity of the NAO-PP framework in KS-DFT calculations and its importance for the development of machine-learning electronic-structure approaches. In this work, we present an efficient NAO-PP-based $G^0W^0$ computational framework by interfacing the first-principles software package ABACUS with LibRPA -- a library for performing low-scaling random-phase approximation and $GW$ calculations based on NAOs. Our approach employs the localized resolution of identity (LRI) technique with a novel compression scheme, significantly improving both computational efficiency and numerical stability. In addition, an analytic treatment of the small-q limit of the microscopic dielectric function reduces the need for dense q-point sampling. Furthermore, we propose a practical strategy to select a suitable KS-DFT pseudopotential prior to $G^0W^0$ calculations by examining the frequency-dependent macroscopic dielectric function. Systematic benchmarks validate the effectiveness of our compression scheme and real-space tensor filtering strategies, demonstrating both high accuracy and significant computational efficiency gains. Comparisons with established $G^0W^0$ implementations show excellent agreement in band structures and band gaps, confirming ABACUS+LibRPA as a reliable and efficient platform for large-scale $G^0W^0$ simulations.

cond-mat.mtrl-sci↗

arXiv2026

6.2-GW tabletop attosecond light source

The generation of attosecond pulses (1 as=10-18 s) has enabled real-time observation and manipulation of coherent electron dynamics, yet their low peak power has hindered the development of advanced attosecond pump-probe spectroscopy and attosecond nonlinear metrology. Here we overcome this limitation by generating 1.64 uJ, 263 as isolated attosecond pulses with a peak power of 6.2 GW, the highest pulse energy and peak power reported for a tabletop isolated attosecond source. This is achieved by combining a 2.1 TW, few-cycle (8.3 fs) two-color synthesizer with a loose focusing geometry that enables macroscopic phase-matching. The synthesizer features a stabilized carrier-envelope phase and an actively synchronized relative time delay between the two-color channels, ensuring high stability and reproducibility. This robust tabletop attosecond source enables nonlinear effect experiments that were previously inaccessible with lower-power IAPs, establishing a foundation for advanced attosecond spectroscopy and nonlinear metrology.

physics.optics↗

arXiv2026

Nonvolatile single-ion memory with picosecond switching

The rapid development of artificial intelligence (AI), Internet of Things (IoT), and edge computing applications has posed severe challenges to conventional memory technologies in terms of density, speed, and energy consumption. Herein, a single-ion transport mechanism is proposed to achieve picosecond (ps) switching capability. For monolayer hexagonal boron nitride (h-BN) with single-atom vacancy defects, first-principles calculations reveal that single-ion penetration across the BN plane dominates the resistive switching. The trapping and release of a single ion correspond to different states of the memory device for one bit of information. Experimentally fabricated single-ion memory exhibits nonvolatile resistive switching with ultra-fast switching speed of 20 ps and ultra-low energy consumption of 310 aJ/bit. This high performance is attributed to the extremely short distance for the single ion to travel through. Such devices pave the way for the realization of high-performance nonvolatile memory with ultra-fast speed, ultra-low energy consumption, and high storage density, that is called the "Unified Memory" long desired by the whole industry.

physics.app-ph↗

arXiv2026

Insulator-to-Metal Transitions Driven by Quantized Formal Polarization Mismatch

We propose a mechanism for insulator-to-metal (IM) transitions driven by the mismatch of quantized formal polarization (QFP), a symmetry-protected bulk invariant. For a material with a low-symmetry insulating phase and a high-symmetry phase that allow distinct QFPs, any continuous path connecting them while preserving the symmetry of the low-symmetry phase must inevitably pass through an IM transition. The reason is that QFP remains invariant along any gapped symmetry-preserving evolution, whereas the high-symmetry phase requires a different QFP, which can only be accommodated by gap closing. First-principles calculations on two representative systems, two-dimensional InPS$_3$ and three-dimensional CdBiO$_3$, confirm this mechanism. Our results establish QFP mismatch as a general symmetry constraint on phase evolution and reveal a new route to symmetry-driven IM transitions in high-symmetry materials.

cond-mat.mtrl-sci↗

arXiv2026

A Unified Heterogeneous Implementation of Numerical Atomic Orbitals-Based Real-Time TDDFT within the ABACUS Package

We present a unified heterogeneous computing framework for real-time time-dependent density functional theory (RT-TDDFT) based on numerical atomic orbitals (NAOs), implemented in the ABACUS package. We introduce three co-designed abstraction layers, including unified data containers, unified linear algebra operators, and unified grid integration interfaces. These layers collectively accelerate the two most demanding parts of NAO-based RT-TDDFT: explicit real-time wavefunction propagation and real-space grid operations such as Hamiltonian construction and force evaluation under external fields. We validate the method by computing optical properties for systems ranging from finite molecules to periodic solids, showing excellent agreement with standard benchmarks. Performance evaluations on bulk silicon demonstrate that a single GPU can achieve substantial wall-clock speedup over a fully utilized dual-socket CPU node. Furthermore, distributed multi-GPU strong-scaling tests confirm high parallel efficiency over tens of GPUs. This work establishes a high-performance, portable platform for large-scale first-principles simulations of ultrafast electron dynamics.

cond-mat.mtrl-sci↗

arXiv2026

NextCrystal: a Symmetry-Driven Generative Framework for Crystal Structure Prediction

Crystal structure prediction (CSP), which aims to predict the 3D atomic arrangement of a crystal from its composition, is central to materials discovery and mechanistic understanding. Crystal symmetry plays a crucial role in CSP, but given the composition in a unit cell, existing methods either struggle with the NP-hard combinatorial challenge of enforcing symmetry rigorously or rely on retrieving known templates, inherently limiting both physical fidelity and the discovery of genuinely new materials. To address this challenge, we introduce NextCrystal, a symmetry-driven generative framework that employs large language models to encode chemical semantics and directly generate fine-grained Wyckoff site patterns from atomic stoichiometry, eliminating reliance on database lookups. To overcome the combinatorial complexity of site assignments, we incorporate domain knowledge via an efficient, linear-complexity heuristic beam search, rigorously enforcing algebraic consistency between site multiplicities and atomic stoichiometry. By integrating this symmetry-consistent template into a diffusion backbone, the framework constrains the stochastic generative trajectory to a physically plausible geometric manifold. NextCrystal achieves state-of-the-art performance on stability, uniqueness, and novelty (SUN) benchmarks, as well as superior structural matching, establishing a rigorous paradigm for exploring previously unexplored crystallographic space without relying on prior structural templates. As a representative application, first-principles screening of HfO2 candidates generated by NextCrystal identifies a previously unreported dynamically stable Pnma phase, 0.056~eV/atom lower in energy than the conventional high-pressure Pnma phase.

cond-mat.mtrl-sci↗

arXiv2026

Quantum Trajectory Separation and Attosecond Mapping in Liquid High-Harmonic Generation

High-harmonic generation (HHG) from liquids offers a potential pathway to attosecond spectroscopy in chemically complex and disordered environments, yet fundamental questions remain open: whether liquid harmonic emission preserves well-defined attosecond synchronization, and whether harmonic emission can involve simultaneous contributions from multiple quantum trajectories with distinct excursion times despite strong disorder and scattering. Here, we address these issues experimentally by resolving the trajectory-dependent temporal structure of liquid HHG. By optimizing the laser focusing geometry, we achieve clear spatial discrimination of short- and long-trajectory contributions, providing direct evidence for the existence of multiple quantum trajectories in liquids. Using a phase-controlled two-color driving field, we independently retrieve the attochirp associated with each trajectory and demonstrate opposite energy-time correlations for short and long trajectories, establishing a trajectory-resolved energy-time mapping in liquid HHG. All observations are well reproduced by semiclassical recollision simulations. These results place liquid HHG on the same conceptual footing as gas- and solid-phase HHG and establish a robust foundation for attosecond-resolved spectroscopy of ultrafast electronic and chemical dynamics in liquid environments.

physics.optics↗

arXiv2025

Real-time time-dependent density functional theory simulations with range-separated hybrid functionals for periodic systems

Real-time time-dependent density functional theory (RT-TDDFT) is a powerful approach for investigating various ultrafast phenomena in materials. However, most existing RT-TDDFT studies rely on adiabatic local or semi-local approximations, which suffer from several shortcomings, including the inability to accurately capture excitonic effects in periodic systems. Combining RT-TDDFT with range-separated hybrid (RSH) functionals has emerged as an effective strategy to overcome these limitations. The RT-TDDFT-RSH implementation for periodic systems requires careful treatment of the Coulomb singularity and choosing proper gauges for the incorporation of external fields. We benchmark two schemes for treating the Coulomb singularity - the truncated Coulomb potential and the auxiliary-function correction - and find that the latter shows better convergence behavior and numerical stability for long-range corrected hybrid functions. Additionally, we assess the impact of gauge choice in simulations using numerical atomic orbitals and show that the recently proposed hybrid gauge incorporating position-dependent phases provides a more accurate description of excitonic absorption than the conventional velocity gauge. Our implementation significantly improves the accuracy of RT-TDDFT-RSH for modeling ultrafast excitonic dynamics in periodic systems.

cond-mat.mtrl-sci↗

arXiv2025

Quantized Polarization Redefines Polar Interfaces

In crystalline solids, the electronic polarization follows the \emph{generalized Neumann's principle}, under which all crystallographic point groups can, in principle, support ferroelectric polarization. However, in high-symmetry structures, polarization is constrained by symmetry operations and becomes quantized into discrete values. We demonstrate that this quantized polarization (QP) is not a mathematical artifact but a \emph{symmetry-protected invariant} that encodes intrinsic information about a material's symmetry and electronic structure. Because of its discrete and non-continuous nature, when two materials with different QPs form an interface, their bulk polarization states cannot be connected adiabatically, compelling the system to develop pronounced interfacial responses: such as metallic states, bound charges, or strong lattice distortions. This theoretical framework provides a unified reinterpretation of classical systems such as the LaAlO$_3$/SrTiO$_3$ interface, revealing it as a prototypical case of QP mismatch. By establishing QP as a fundamental bulk invariant, our work uncovers a universal mechanism governing interfacial electronic phenomena and opens new pathways for the design of functional quantum materials through engineered polarization mismatch.

cond-mat.mtrl-sci↗

arXiv2025

Quantum Path Control in High-Order Harmonic Generation via Squeezed Lights

High-order harmonic generation (HHG), a robust tabletop source for producing attosecond pulses, has been extensively utilized in attosecond metrology. Traditionally, HHG driven by classical laser fields involves two typical quantum paths (short and long quantum paths) contributing to harmonic emission. Here, we demonstrate that these quantum paths in HHG can be selectively controlled using squeezed lights, a form of non-classical light. Our results indicate that the long (short) quantum path of HHG will be dramatically suppressed in the phase (amplitude)-squeezed fields. The time-frequency analysis reveals that this quantum path control stems from the quantum fluctuations in the squeezed light, which modify the phase matching of harmonic emission from different quantum states of the squeezed light. Such a quantum path selection can be achieved for the whole harmonic plateau, which has great potential to generate ultrashort isolated attosecond pulse with duration less than one atomic unit of time.

physics.optics↗

arXiv2025

Advancing Universal Deep Learning for Electronic-Structure Hamiltonian Prediction of Materials

Deep learning methods for electronic-structure Hamiltonian prediction has offered significant computational efficiency advantages over traditional DFT methods, yet the diversity of atomic types, structural patterns, and the high-dimensional complexity of Hamiltonians pose substantial challenges to the generalization performance. In this work, we contribute on both the methodology and dataset sides to advance universal deep learning paradigm for Hamiltonian prediction. On the method side, we propose NextHAM, a neural E(3)-symmetry and expressive correction method for efficient and generalizable materials electronic-structure Hamiltonian prediction. First, we introduce the zeroth-step Hamiltonians, which can be efficiently constructed by the initial charge density of DFT, as informative descriptors of neural regression model in the input level and initial estimates of the target Hamiltonian in the output level, so that the regression model directly predicts the correction terms to the target ground truths, thereby significantly simplifying the input-output mapping for learning. Second, we present a neural Transformer architecture with strict E(3)-Symmetry and high non-linear expressiveness for Hamiltonian prediction. Third, we propose a novel training objective to ensure the accuracy performance of Hamiltonians in both real space and reciprocal space, preventing error amplification and the occurrence of "ghost states" caused by the large condition number of the overlap matrix. On the dataset side, we curate a high-quality broad-coverage large benchmark, namely Materials-HAM-SOC, comprising 17,000 material structures spanning 68 elements from six rows of the periodic table and explicitly incorporating SOC effects. Experimental results on Materials-HAM-SOC demonstrate that NextHAM achieves excellent accuracy and efficiency in predicting Hamiltonians and band structures.

cs.LG↗

arXiv2025

Topological Origin of Intrinsic High Chern Numbers in Two-Dimensional M$_2$X$_2$ Materials

Despite sharing a common lattice structure, monolayer M$_2$X$_2$ compounds realize quantum anomalous Hall phases with distinct Chern numbers, a striking phenomenon that has not been fully exploared. Combining first-principles calculations with symmetry analysis and tight-binding models, we identify two generic band-inversion mechanisms governed by the orbital composition and symmetry representations of 3$d$ states near the Fermi level. When $d_{xz}/d_{yz}$ orbtials dominate, a doubly degenerate $\Gamma$-point inversion yields $C=1$; otherwise, inversions occur along $\Gamma$-X and $\Gamma$-Y at four $C_4$-related momenta, whose Berry-curvature contributions add to give $C=2$, distinct from scenarios relying on multiple bands inversions at a single $\mathbf{k}$ point. The same mechanism consistently explains related two-dimensional systems, including LiFeSe, KTiSb, MgFeP, and Janus M$_2$X$_2$ derivatives. The mechanism provide practical guidance for screening and engineering tunable high-Chern-number insulators.

cond-mat.mtrl-sci↗

arXiv2025

Clean few-cycle blue soliton self-compressed pulses generation in hollow-core fibers

Blue pulses with few-cycle temporal durations hold significant value in attosecond science and ultrafast spectroscopy. In this work, we combine efficient broadband frequency doubling, multiplate continuum (MPC) post-compression and blue soliton self-compression in hollow-core fibers (HCF), experimentally demonstrating HCF-based 4.4 fs clean blue soliton self-compressed pulse. Our scheme offers three-fold advantages: (1) prevention of excessive dispersion accumulation by gradually suppressing dispersion through multi-stage design; (2) enhanced overall efficiency for self-compression-based ultrashort blue pulse generation; and (3) elimination of dispersion compensation components for the final spectral broadening stage compared to post-compression schemes. This work extends HCF-based self-compression soliton to the blue spectral region and paves the way for generating energetic ultrashort blue pulses.

physics.optics↗

arXiv2025

Constructing 3D Rotational Invariance and Equivariance with Symmetric Tensor Networks

Symmetry-aware architectures are central to geometric deep learning. We present a systematic approach for constructing continuous rotationally invariant and equivariant functions using symmetric tensor networks. The proposed framework supports inputs and outputs given as a tuple of Cartesian tensors of different rank as well as spherical tensors of different type. We introduce tensor network generators for invariant maps and obtain equivariant maps via differentiation. Specifically, we derive general continuous equivariant maps from vector inputs to Cartesian or spherical tensor output. Finally, we clarify how common equivariant primitives in geometric graph neural networks arise within our construction.

cs.LG↗

arXiv2025

Unveiling unique ultrafast nonlinearities in liquid-phase high-order harmonic generation

High-order harmonic generation (HHG) provides a powerful optical tool for probing ultrafast dynamics on the attosecond timescale. While its mechanisms in gases and solids are well-established, understanding nonlinear optical responses in liquids remains challenging. The absence of long-range order in liquids questions the applicability of the existing HHG models developed in other media. Through combined experimental and theoretical investigations, we identify unique characters of liquid-phase HHG -- spectral redshift and broadening, which are fundamentally distinct from both the gaseous and solid-state counterparts. Quantitative measurements and simulations of HHG in liquids illustrate a near linear dependence of harmonic redshift and broadening on the laser intensity, with the nonlinear response of water exceeding that of ethanol. The simulations reveal that these features arise from delocalized electronic states with energy loss in multiple scatterings and transient Stark shift during their transitions in laser fields. Meanwhile, we find that liquid polarity or hydrogen bond exerts decisive control over the transition dipole momentum distributions of delocalized states. Our findings establish a nonlinear spectral method for probing the internal network in liquids, paving the way for studying its role in chemical and biological processes.

physics.optics↗