arXiv subjects

Jia-Xin Li

Publications and source records attributed to Jia-Xin Li.

9 recordsLinked to original sources

arXiv2026

Ai2-Kit: Streamlining AI-Accelerated Ab Initio Workflows for Complex Chemical Systems

Molecular simulations of complex chemical systems, such as catalysis, electrochemistry, and energy storage, often need to capture the interplay of effects such as electronic structure, finite-temperature fluctuations, and electric-field response. Such complexity is difficult to address with traditional ab initio calculations, which are limited by the time and length scales they can reach. AI-accelerated ab initio (AI2) methods use machine learning potentials trained on first-principles data to replace expensive electronic-structure calculations, extending ab initio accuracy to these regimes, but their routine application requires reliable workflows that connect first-principles calculations, model training, molecular dynamics, enhanced sampling, trajectory analysis, and HPC orchestration. Here we present ai2-kit, a software toolkit for developing accessible, reproducible, and extensible AI2 workflows. ai2-kit provides high-semantic-density command-line interfaces and Python APIs for structure and dataset conversion, batch task generation, active-learning screening, job orchestration, and workflow recovery. We demonstrate ai2-kit in four representative applications: active-learning-based machine learning potential construction, free-energy perturbation for redox and acid-base processes, electrochemical machine learning potentials for electrified interfaces, and spectroscopies from machine learning molecular dynamics. ai2-kit also provides AI-agent skills that help users adapt these use cases into customized workflows for their own chemical systems and computational software stacks. Together, ai2-kit helps turn AI2 methods from bespoke computational protocols into reusable and extensible workflows for complex chemical systems, from model construction to property prediction.

physics.chem-ph↗

arXiv2026

Steering Selective Formation and 2D Crystallization of [4]Radialenes on Au(111) via [1+1+1+1] Cycloaddition of Isocyanides and Enantioselective Molecular Recognition

Conjugated carbon rings are fundamental skeletons of organic functional materials, and their selective formation is of paramount importance in molecular materials engineering. However, steering the formation and 2D crystallization of conjugated carbon rings on the surface with high chemo- and stereoselectivities remains a great challenge. Here, we report a highly chemoselective [1+1+1+1] cycloaddition of isocyanides on the Au(111) surface, which affords the stereospecific tetraaza[4]radialene products and further enables their long-range-ordered 2D crystallization via enantioselective molecular recognition. Using the progressive annealing method, we found that at room temperature, isocyanides undergo a coordination reaction with Au adatoms to form two-fold symmetric isocyanide-Au-isocyanide complexes. In contrast, gradually increasing the annealing temperature induces the transformation of these complexes and subsequent covalent polymerization, leading to the selective generation of tetraaza[4]radialenes with homotactic configurations. The tetraaza[4]radialenes further assemble into 2D homochiral molecular crystals through enantioselective molecular recognition driven by multiple C-H -- Cl hydrogen-bonding interactions. By combining scanning tunneling microscopy/spectroscopy and non-contact atomic force microscopy, we determined the atomic structure and molecular orbitals of tetraaza[4]radialene, confirming that its four-membered ring adopts a planar geometry with a localized lowest unoccupied molecular orbital. Density functional theory calculations suggest that the [1+1+1+1] cycloaddition process involves stepwise formation of C-C bonds and its high selectivity arises from the spatial steric hindrance. Our findings provide new insights into the selective formation of conjugated rings on surfaces and have implications for engineering 2D homochiral molecular crystallization.

cond-mat.mtrl-sci↗

arXiv2026

Tomonaga-Luttinger liquid and charge-density wave in a quasi-one-dimensional material

In one-dimensional (1D) electron systems, the Fermi liquid state breaks down due either to electron interactions, which results in a Tomonaga-Luttinger liquid (TLL) state, or to Peierls instability, which leads to an insulating charge-density-wave (CDW) phase. In general, these two phenomena are mutually exclusive, and their coexistence remains elusive in real materials. Here, we report the discovery of a new quasi-1D material, Cs$_{1-δ}$Cr$_3$S$_3$, which unexpectedly exhibits coexistence of the antithetical CDW and TLL states. The CDW state is evidenced by the intra-unit-cell dimerization, and the opening of an optical band gap of $\sim$250 meV. Meanwhile, TLL behaviour is unambiguously demonstrated by the measurements of electrical transport and angle-resolved photoemission spectroscopy, which reveal a power-law scaling with temperature, bias voltage and electron energy. Band structure calculations reveal isolated, linearly dispersive, 1D bands around the Fermi level. For the dimerized CDW phase, the 1D Fermi-surface sheets located at the boundary of the Brillouin zone are gapped from intra-unit-cell bond symmetry breaking. Experimentally, subtle Cs vacancies shift the Fermi level into the linearly dispersive valence band, enabling the observation of TLL behaviour without interrupting the CDW order. This work establishes Cs$_{1-δ}$Cr$_3$S$_3$ as a rare material platform in which the antagonistic Fermi-liquid instabilities coexist and intertwine, opening new avenues for studying emergent quantum phenomena in 1D systems.

cond-mat.str-el↗

arXiv2026

Entropy stabilization and effect of A-site ionic size in bilayer nickelates

The discovery of high-temperature superconductivity in La$_3$Ni$_2$O$_7$ under high pressure has sparked a surge of research into Ruddlesden-Popper (RP) nickelates. Currently, stabilizing the bilayer RP phases with smaller $A$-site ions remains a significant challenge. In this work, we have successfully synthesized medium- and high-entropy bilayer nickelates, La$_{1.2}$Pr$_{0.6}$Nd$_{0.6}$Sm$_{0.6}$Ni$_2$O$_{7-δ}$ and La$_{0.67}$Pr$_{0.67}$Nd$_{0.67}$Sm$_{0.33}$Eu$_{0.33}$Gd$_{0.33}$Ni$_2$O$_{7-δ}$, by utilizing the concept of configuration entropy stabilization. The high-entropy nickelate exhibits the smallest unit-cell volume and the largest orthorhombic distortion reported to date. The chemical pressure induced by the smaller A-site ions significantly enhances the NiO$_6$ octahedral rotation/distortion and shortens the interlayer Ni-Ni interatomic spacing. Physical property measurements reveal bad electrical conductivity alongside a markedly elevated density-wave transition temperature. Notably, the superconducting transition temperature extrapolated from structural correlations is projected to exceed 100 K. Our work not only demonstrates entropy stabilization of bilayer nickelates, but also reveals the effect of $A$-site-ion size on the crystal structure and physical properties, opening a new pathway for developing nickelate superconductors and tuning their electronic properties.

cond-mat.supr-con↗

arXiv2025

Stabilization of Tetragonal Phase and Aluminum-Doping Effect in a Bilayer Nickelate

Recent studies suggest that the tetragonal phase of the Ruddlesden-Popper (RP) bilayer nickelate, La$_3$Ni$_2$O$_7$ or La$_2$PrNi$_2$O$_7$, which is stabilized under high pressures, is responsible for high-temperature superconductivity (HTSC). In this context, realization of the tetragonal phase at ambient pressure could be a rational step to achieve the goal of ambient-pressure HTSC in the nickelate system. By employing the concept of Goldschmidt tolerance factor, we succeed in stabilizing the tetragonal phase by aluminum doping together with post annealing under moderately high oxygen pressure. X-ray and neutron diffractions verify the tetragonal $I4/mmm$ structure for the post-annealed samples La$_3$Ni$_{2-x}$Al$_x$O$_{7-δ}$ (0.3 $\leq x \leq$ 0.5). The Al-doped samples, including the tetragonal ones, show semiconducting properties, carry localized magnetic moments, and exhibit spin-glass-like behaviors at low temperatures, all of which can be explained in terms of charge carrier localization. Furthermore, high-pressure resistance measurements on post-annealed samples reveal that even a low Al doping ($x$ = 0.05) suppresses superconductivity almost completely. This work gives information about the effect of nonmagnetic impurity on metallicity as well as superconductivity in bilayer nickelates, which would contribute to understanding the superconducting mechanism in RP nickelates.

cond-mat.supr-con↗

arXiv2025

Quantum Criticality by Interaction Frustration in a Square-Planar Lattice

We report experimental and theoretical investigations on ThCr$_2$Ge$_2$C, a metallic compound in which Cr$_2$C planes form a square-planar lattice. Neutron powder diffraction, magnetization, and specific heat measurements reveal no evidence of long-range magnetic order or short-range spin freezing down to 70~mK. Quantum critical behavior was indicated through logarithmic divergences in both the magnetic susceptibility and the specific heat divided by temperature. Resistivity measurements exhibit non-Fermi-liquid behavior, with a Fermi liquid recovered under magnetic fields or high pressures. First-principles calculations identify competing nearest-neighbor ($J_1$) and next-nearest-neighbor ($J_2$) exchange interactions, with $J_2/J_1 \sim -0.5$, pointing to strong magnetic frustration. The interaction frustration is reduced, and magnetically ordered phases are stabilized upon the application of negative or positive pressures. This work offers a rare example of zero-field, ambient pressure quantum criticality mainly driven by interaction frustration in a square lattice.

cond-mat.str-el↗

arXiv2024

Absence of itinerant ferromagnetism in a cobalt-based oxypnictide

We report a layered transition-metal-ordered oxypnictide Sr$_{2}$CrCoAsO$_{3}$. The new material was synthesized by solid-state reactions under vacuum. It has an intergrowth structure with a perovskite-like Sr$_3$Cr$_2$O$_6$ unit and ThCr$_2$Si$_2$-type SrCo$_2$As$_2$ block stacking coherently along the crystallographic $c$ axis. The measurements of electrical resistivity, magnetic susceptibility, and specific heat indicate metallic conductivity from the CoAs layers and short-range antiferromagnetic ordering in the CrO$_{2}$ planes. No itinerant-electron ferromagnetism expected in CoAs layers is observed. This result, combined with the first-principles calculations and the previous reports of other CoAs-layer-based materials, suggests that the Co$-$Co bondlength plays a crucial role in the emergence of itinerant ferromagnetism.

cond-mat.mtrl-sci↗

arXiv2022

Van der Waals heterostructure mid-infrared emitters with electrically controllable polarization states and spectral characteristics

Modern infrared (IR) microscopy, communication, and sensing systems demand control of the spectral characteristics and polarization states of light. Typically, these systems require the cascading of multiple filters, polarization optics and rotating components to manipulate light, inevitably increasing their sizes and complexities. Here, we report two-terminal mid-infrared (mid-IR) emitters with electrically controllable spectral and polarization properties. Our devices are composed of two back-to-back p-n junctions formed by stacking anisotropic light-emitting materials, black phosphorus and black arsenic-phosphorus with MoS2. By controlling the crystallographic orientations and engineering the band profile of heterostructures, the emissions of two junctions exhibit distinct spectral ranges and polarization directions; more importantly, these two electroluminescence (EL) units can be independently activated, depending on the polarity of the applied bias. Furthermore, we show that when operating our emitter under the polarity-switched pulse mode, its EL exhibits the characteristics of broad spectral coverage, encompassing the entire first mid-IR atmospheric window, and electrically tunable spectral shapes. Our results provide the basis for developing groundbreaking technology in the field of light emitters.

physics.optics↗

arXiv2020

Black phosphorus van der Waals heterostructures light emitting diodes for mid-infrared silicon photonics

Light-emitting diodes (LEDs) based on III-V/II-VI materials have delivered a compelling performance in the mid-infrared (mid-IR) region, which enabled wide-ranging applications, including environmental monitoring, defense and medical diagnostics. Continued efforts are underway to realize on-chip sensors via heterogeneous integration of mid-IR emitters on a silicon photonic chip. But the uptake of such approach is limited by the high costs and interfacial strains, associated with the process of heterogeneous integrations. Here, the black phosphorus (BP)-based van der Waals (vdW) heterostructures are exploited as room temperature LEDs. The demonstrated devices can emit linearly polarized light, and their spectra cover the technologically important mid-IR atmospheric window (3-4 um). Additionally, the BP LEDs exhibit fast modulation speed as well as exceptional stability, and its peak extrinsic quantum efficiency (QE~0.9%) is comparable to the III-V/II-VI mid-IR LEDs. By leveraging the integrability of vdW heterostructures, we further demonstrate a silicon photonic waveguide-integrated BP LED. The reported hybrid platform holds great promise for mid-IR silicon photonics.

physics.app-ph↗