arXiv subjects

Changsong Xu

Publications and source records attributed to Changsong Xu.

At least 19 recordsLinked to original sources

arXiv2026

Dimensional crossover and local strain induced deflection of the spin spiral state in multiferroic NiI2

Low-dimensional multiferroics hold great promise for integrated magnetoelectric devices. Spin spiral state has recently been shown to induce ferroelectricity in single-layer van der Waals (vdW) material NiI2. However, how this state evolves and can be tuned towards the two-dimensional limit remain unclear. Here, we combine spin-polarized scanning tunneling microscopy, layer-by-layer film growth, and multi-scale theoretical modeling to investigate the spin spirals in NiI2 thin films. As the film thickness increases from 1 to 7 monolayers, we observed a continuous increase of spin-spiral wavelength and a rotation of wavevector from near [110] to [1-10] direction, which evidences a dimensional crossover primarily driven by enhanced interlayer exchange energy. Moreover, we find that the film wrinkles can cause deflection of the spin spiral wavevector, which is caused by local curvature induced modification of exchange interactions. Our findings establish thickness and local strain as two tuning methods for engineering non-collinear helical magnetism and accompanied electric polarization in vdW multiferroics.

cond-mat.mes-hall↗

arXiv2026

Sizable Ligand-Mediated Bond-Dependent Interactions in a Spin-1 Triangular Antiferromagnet NiI$_2$

The bond-dependent anisotropic Kitaev interactions are the key for the Kitaev model, which has attracted intense interest for its potential to host quantum-spin-liquid states and fractional excitations. However, experimental realizations of such interactions remain scarce. Here, we investigate the magnetic excitations of NiI$_2$, a van der Waals magnet with spin $S=1$. By combining inelastic neutron scattering, magnetization measurements, magnetic structure analysis, first-principles calculations, and linear-spin-wave simulations, we identify a minimal model that features substantial Kitaev and off-diagonal $\Gamma$ interactions, which together stabilize the canted magnetic ground state and open a gap in the spin-wave spectrum. Notably, these interactions arise from strong spin-orbit coupling on the ligand ions, despite the quenched orbital moment of the magnetic Ni$^{2+}$ ions. Our results provide compelling experimental evidence for the ligand-driven Kitaev mechanism. This demonstrates a concrete pathway to generating strong bond-dependent anisotropy in systems where the magnetic ions themselves have weak spin-orbit coupling, thereby substantially broadening the range of potential Kitaev materials.

cond-mat.str-el↗

arXiv2026

Microscopic evidence of spin-driven multiferroicity and topological spin textures in monolayer NiI2

In type II multiferroics, noncollinear spin textures are expected to induce electric polarization directly, leading to strong magnetoelectric coupling. Realizing such spin driven multiferroicity in two-dimensional systems, and elucidating the interplay between local spins and electric polarization, are of both fundamental and technological importance. Here, using vectorial spin polarized scanning tunneling microscopy, we investigated the spin-driven multiferroicity in monolayer NiI2 at atomic scale. We identify a canted spin-spiral state with fully determined spin rotation plane, accompanied by a 2Q charge modulation. At spin spiral domain walls, we discover topological spin textures that composed of meron/antimeron pairs. These textures are associated with distinct charge pattern and notable band shifts, indicating local bound charges induced by variations of ferroelectricity at domain wall. Our observations are well captured by a realistic spin model incorporating Kitaev interactions and generalized spin-current model of type II multiferroicity. The findings provide microscopic evidence of spin-driven multiferroicity in an extreme 2D system and establish a platform for low-dissipation, electric-field control of topological spin textures.

cond-mat.mes-hall↗

arXiv2025

Lessons from $\alpha$-RuCl3 for pursuing quantum spin liquid physics in atomically thin materials

Quantum spin liquids can arise from Kitaev magnetic interactions, and exhibit fractionalized excitations with the potential for a topological form of quantum computation. This review surveys recent experimental and theoretical progress on the pursuit of phenomena related to Kitaev magnetism in layered and exfoliatable materials, which offer numerous opportunities to apply powerful techniques from the field of atomically thin materials. We primarily focus on the antiferromagnetic Mott insulator $\alpha$-RuCl3, which exhibits Kitaev couplings and is readily exfoliated to single- or few-layer sheets, and thus serves as a test bed for developing probes of Kitaev phenomena in atomically thin materials and devices. We introduce the Kitaev model and how it is realized in $\alpha$-RuCl3 and other material candidates; and cover $\alpha$-RuCl3 synthesis and fabrication into van der Waals heterostructure devices. A key discovery is a work-function-mediated charge transfer that heavily dopes both the $\alpha$-RuCl3 and proximate materials, and can enhance Kitaev interactions by up to 50%. We further discuss a wide range of recent results in electronic transport and optical and tunneling spectroscopies of $\alpha$-RuCl3 devices. The experimental techniques and theoretical insights developed for $\alpha$-RuCl3 establish a framework for discovering and engineering superior two-dimensional Kitaev materials that may ultimately realize elusive quantum spin liquid phases.

cond-mat.str-el↗

arXiv2025

Defect-Charge-Driven 90{\deg} Switching in HfO2

Hafnium dioxide (HfO2) is a CMOS-compatible ferroelectric showing both 180{\deg} and 90{\deg} switching, yet the microscopic nature of the 90{\deg} pathway remains unresolved. We show that the 90{\deg} rotation pathway, negligible in pristine HfO2, becomes dominant under E// [111] when induced by charged oxygen vacancies. This pathway is more fatigue-resistant than the 180{\deg} reversal pathway, while delivering the same polarization change along [111] (2Pr=60 {\mu}C/cm^2 ). This charge-driven switching arises from two factors: the crystal geometry of HfO2 and the intrinsic nature of rotational pathways, the latter suggesting a possible general tendency for defect charge to bias rotation over reversal in ferroelectrics. Together these findings reveal a pathway-level origin of fatigue resistance and establish defect charge as a general control parameter for polarization dynamics.

cond-mat.mtrl-sci↗

arXiv2025

Moir\'e-Induced Magnetoelectricity in Twisted Bilayer NiI2

Twisted magnetic van der Waals (vdW) materials offer a promising route for multiferroic engineering, yet modeling large-scale moir\'e superlattices remains challenging. Leveraging a newly developed SpinGNN++ framework that effectively handles spin-lattice coupled systems, we develop a comprehensive interatomic machine learning (ML) potential and apply it to twisted bilayer NiI2 (TBN). Structural relaxation introduces moir\'e-periodic "bumps" that modulate the interlayer spacing by about 0.55~\AA{} and in-plane ionic shifts up to 0.48~\AA{}. Concurrently, our ML potential, which faithfully captures all key spin interactions, produces reliable magnetic configurations; combined with the generalized KNB mechanism, it yields accurate spin-driven polarization. For twist angles 1.89^{\circ} \leq \theta \leq 2.45^{\circ}, both mechanisms become prominent, yielding rich polarization textures that combine ionic out-of-plane dipoles with purely electronic in-plane domains. In the rigid (unrelaxed) bilayer, skyrmions are absent; lattice relaxation is essential for generating polar-magnetic topologies. In contrast, near {\theta} \approx 60^{\circ}, stacking-dependent ferroelectric displacements dominate, giving rise to polar meron-antimeron networks. These results reveal cooperative ionic and spin-driven ferroelectricity in TBN, positioning twisted vdW magnets as adaptable platforms for tunable multiferroic devices.

cond-mat.mtrl-sci↗

arXiv2025

Efficient construction of effective Hamiltonians with a hybrid machine learning method

The effective Hamiltonian method is a powerful tool for simulating large-scale systems across a wide range of temperatures. However, previous methods for constructing effective Hamiltonian models suffer from key limitations: some require to manually predefine interaction terms limited flexibility in capturing complex systems, while others lack efficiency in selecting optimal interactions. In this work, we introduce the Lasso-GA Hybrid Method (LGHM), a novel approach that combines Lasso regression and genetic algorithms to rapidly construct effective Hamiltonian models. Such method is broadly applicable to both magnetic systems (e.g., spin Hamiltonians) and atomic displacement models. To verify the reliability and usefulness of LGHM, we take monolayer CrI_3 and Fe_3 GaTe_2 as examples. In both cases, LGHM not only successfully identifies key interaction terms with high fitting accuracy, but also reproduces experimental magnetic ground states and Curie temperatures with further Monte Carlo simulations. Notable, our analysis of monolayer Fe_3 GaTe_2 reveals that the single-ion anisotropy and Heisenberg interaction lead to an out-of-plane ferromagnetic ground state, while the fourth-order interactions contribute significantly to the high Curie temperature. Our method is general so it can be applied to construct other effective Hamiltonian models.

physics.comp-ph↗

arXiv2025

Long-Range Spin-Orbit-Coupled Magnetoelectricity in Type-II Multiferroic NiI$_2$

Type-II multiferroics, where spin order induces ferroelectricity, exhibit strong magnetoelectric coupling. However, for the typical 2D type-II multiferroic NiI$_2$, the underlying magnetoelectric mechanism remains unclear. Here, applying generalized spin-current model, together with first-principles calculations and a tight-binding approach, we build a comprehensive magnetoelectric model for spin-induced polarization. Such model reveals that the spin-orbit coupling extends its influence to the third-nearest neighbors, whose contribution to polarization rivals that of the first-nearest neighbors. By analyzing the orbital-resolved contributions to polarization, our tight-binding model reveals that the long-range magnetoelectric coupling is enabled by the strong $e_g$-$p$ hopping of NiI$_2$. Monte Carlo simulations further predict a Bloch-type magnetic skyrmion lattice at moderate magnetic fields, accompanied by polar vortex arrays. These findings can guide the discovery and design of strongly magnetoelectric multiferroics.

cond-mat.mtrl-sci↗

arXiv2024

Role of Domain Walls on Imprint and Fatigue in HfO2-Based Ferroelectrics

HfO2-based ferroelectric materials are promising for the next generation of memory devices, attracting significant attention. However, their potential applications are significantly limited by fatigue and imprint phenomena, which affect device lifetime and memory capabilities. Here, to accurately describe the dynamics and field effects of HfO2, we adopt our newly developed DREAM-Allegro network scheme and develop a comprehensive machine-learning model for HfO2. Such model can not only predict the interatomic potential, but also predict Born effective charges. Applying such model, we explore the role of domain dynamics in HfO2 and find that the fatigue and imprint phenomena are closely related to the so-called E-path and T-path switching pathways. Based on the different atomic motions in the two paths, we propose that an inclined electric field can sufficiently suppress fatigue and enhancing the performance of HfO2-based ferroelectric devices.

cond-mat.mtrl-sci↗

arXiv2024

Emergent spin-charge-orbital order in superconductor La$_3$Ni$_2$O$_7$

The bilayer nickelate La$_3$Ni$_2$O$_7$ (LNO) exhibits a remarkably high-temperature superconductivity of approximately 80 K under pressure, sparking considerable attentions. However, the nature of the spin, charge, and orbital order in LNO remains unknown, hindering the exploration of the mechanism of superconductivity. Here, supported by symmetry analysis and density functional theory calculations, we unravel a double strip ground state of LNO with alternating magnetic moments arrangements. Interestingly, a charge density wave emerges under this determined magnetic order. Such CDW phase exhibits a Pmnm space group with breathing deformation of the NiO$_6$ octahedra, where the stretching and shrinking of the octahedra correspond to the formation of \emph{d}$_{z^2}^1$\emph{d}$_{x^2-y^2}^1$ and \emph{d}$_{z^2}^1$ orbital order. Moreover, we build a first-principles-based Hamiltonian for LNO, which provides deeper insight into its peculiar magnetic order. Our work thus reveals a systematic spin-charge-orbital picture for LNO, which can be extended to other nickelate-based superconductors, paving the way for determining the mechanism of superconductivity.

cond-mat.supr-con↗

arXiv2024

Mechanism of Type-II Multiferroicity in Pure and Al-Doped CuFeO$_2$

Type-II multiferroicity, where electric polarization is induced by specific spin patterns, is crucial in fundamental physics and advanced spintronics. However, the spin model and magnetoelectric coupling mechanisms in prototypical type-II multiferroic CuFeO$_2$ and Al-doped CuFeO$_2$ remain unclear. Here, by considering both spin and alloy degrees of freedom, we develop a magnetic cluster expansion method, which considers all symmetry allowed interactions. Applying such method, we not only obtain realistic spin model that can correctly reproduce observations for both CuFeO$_2$ and CuFe$_{1-x}$Al$_x$O$_2$, but also revisit well-known theories of the original spin-current (SC) model and $p$-$d$ hybridization model. Specifically, we find that (i) a previously overlooked biquadratic interaction is critical to reproduce the $\uparrow\uparrow\downarrow\downarrow$ ground state and excited states of CuFeO$_2$; (ii) the combination of absent biquadratic interaction and increased magnetic frustration around Al dopants stabilizes the proper screw state; and (iii) it is the generalized spin-current (GSC) model that can correctly characterize the multiferroicity of CuFeO$_2$. These findings have broader implications for understanding novel magnetoelectric couplings in, e.g., monolayer multiferroic NiI$_2$.

cond-mat.mtrl-sci↗

arXiv2024

Deterministic and Efficient Switching of Sliding Ferroelectrics

Recent studies highlight the scientific importance and broad application prospects of two-dimensional (2D) sliding ferroelectrics, which prevalently exhibit vertical polarization with suitable stackings. It is crucial to understand the mechanisms of sliding ferroelectricity and to deterministically and efficiently switch the polarization with optimized electric fields. Here, applying our newly developed DREAM-Allegro multi-task equivariant neural network, which simultaneously predicts interatomic potentials and Born effective charges, we construct a comprehensive potential for boron nitride ($\mathrm{BN}$) bilayer. The molecular dynamics simulations reveal a remarkably high Curie temperature of up to 1500K, facilitated by robust intralayer chemical bonds and delicate interlayer van der Waals(vdW) interactions. More importantly, it is found that, compared to the out-of-plane electric field, the inclined field not only leads to deterministic switching of electric polarization, but also largely lower the critical strength of field, due to the presence of the in-plane polarization in the transition state. This strategy of an inclined field is demonstrated to be universal for other sliding ferroelectric systems with monolayer structures belonging to the symmetry group $p \bar{6} m 2$, such as transition metal dichalcogenides (TMDs).

cond-mat.mtrl-sci↗

arXiv2024

Effects of Kitaev Interaction on Magnetic Orders and Anisotropy

We systematically investigate the effects of Kitaev interaction on magnetic orders and anisotropy in both triangular and honeycomb lattices. Our study highlights the critical role of the Kitaev interaction in modulating phase boundaries and predicting new phases, e.g., zigzag phase in triangular lattice and AABB phase in honeycomb lattice, which are absent with pure Heisenberg interactions. Moreover, we reveal the special state-dependent anisotropy of Kitaev interaction, and develop a general method that can determine the presence of Kitaev interaction in different magnets. It is found that the Kitaev interaction does not induce anisotropy in some magnetic orders such as ferromagnetic order, while can cause different anisotropy in other magnetic orders. Furthermore, we emphasize that the off-diagonal $\Gamma$ interaction also contributes to anisotropy, competing with the Kitaev interaction to reorient spin arrangements. Our work establishes a framework for comprehensive understanding the impact of Kitaev interaction on ordered magnetism.

cond-mat.str-el↗

arXiv2024

Strength of Kitaev Interaction in Na$_3$Co$_2$SbO$_6$ and Na$_3$Ni$_2$BiO$_6$

Kitaev spin liquid is proposed to be promisingly realized in low spin-orbit coupling $3d$ systems, represented by Na$_3$Co$_2$SbO$_6$ and Na$_3$Ni$_2$BiO$_6$. However, the existence of Kitaev interaction is still debatable among experiments, and obtaining the strength of Kitaev interaction from first-principles calculations is also challenging. Here, we report the state-dependent anisotropy of Kitaev interaction, based on which a convenient method is developed to rapidly determine the strength of Kitaev interaction. Applying such method and density functional theory calculations, it is found that Na$_3$Co$_2$SbO$_6$ with $3d^7$ configuration exhibits considerable ferromagnetic Kitaev interaction. Moreover, by further applying the symmetry-adapted cluster expansion method, a realistic spin model is determined for Na$_3$Ni$_2$BiO$_6$ with $3d^8$ configuration. Such model indicates negligible small Kitaev interaction, but it predicts many properties, such as ground states and field effects, which are well consistent with measurements. Furthermore, we demonstrate that the heavy elements, Sb or Bi, located at the hollow sites of honeycomb lattice, do not contribute to emergence of Kitaev interaction through proximity, contradictory to common belief. The presently developed anisotropy method will be beneficial not only for computations but also for measurements.

cond-mat.str-el↗

arXiv2024

Memristive switching in the surface of a charge-density-wave topological semimetal

Owing to the outstanding properties provided by nontrivial band topology, topological phases of matter are considered as a promising platform towards low-dissipation electronics, efficient spin-charge conversion, and topological quantum computation. Achieving ferroelectricity in topological materials enables the non-volatile control of the quantum states, which could greatly facilitate topological electronic research. However, ferroelectricity is generally incompatible with systems featuring metallicity due to the screening effect of free carriers. In this study, we report the observation of memristive switching based on the ferroelectric surface state of a topological semimetal (TaSe4)2I. We find that the surface state of (TaSe4)2I presents out-of-plane ferroelectric polarization due to surface reconstruction. With the combination of ferroelectric surface and charge-density-wave-gapped bulk states, an electric switchable barrier height can be achieved in (TaSe4)2I-metal contact. By employing a multi-terminal grounding design, we manage to construct a prototype ferroelectric memristor based on (TaSe4)2I with on/off ratio up to 10^3, endurance over 10^3 cycles, and good retention characteristics. The origin of the ferroelectric surface state is further investigated by first-principles calculations, which reveals an interplay between ferroelectricity and band topology. The emergence of ferroelectricity in (TaSe4)2I not only demonstrates it as a rare but essential case of ferroelectric topological materials, but also opens new routes towards the implementation of topological materials in functional electronic devices.

cond-mat.mtrl-sci↗

arXiv2024

Symmetry Strategy for Rapid Discovery of Abundant Fractional Quantum Ferroelectrics

Traditional ferroelectrics are limited by Neumann's principle, which confines exploration of ferroelectrics within polar point groups. Our recent work [Nat. Commun. 15, 135, (2024)] proposes the concept of fractional quantum ferroelectricity (FQFE) that extend the playground of ferroelectricity to non-polar point groups. Here, we apply group theory and introduce an efficient symmetry strategy to identify FQFE candidates. Integrated with a high-throughput screening scheme, we go through 171,527 materials and identify 202 potential FQFE candidates, which are already experimentally synthesized. In addition, we point out that the essence of FQFE is fractional atomic displacements with respect to lattice vectors, which can actually result in both fractional (type-I) and integer (type-II) quantized polarization, respectively. Through performing first-principles calculations, we verify the symmetry-predicted switchable FQFE properties in bulk AlAgS2 and monolayer HgI2. Notably, AlAgS2 exhibits an ultra-low switching barrier of 23 meV/f.u. and interlocked in-plane/out-of-plane polarization, while HgI2 demonstrates large spontaneous polarization of 42 {\mu}C/cm2. Our findings not only advance the understanding on FQFE, but also offer guidance for experimental exploration and design of novel ferroelectric materials.

cond-mat.mtrl-sci↗

arXiv2023

Evaluating Gilbert Damping in Magnetic Insulators from First Principles

Magnetic damping has a significant impact on the performance of various magnetic and spintronic devices, making it a long-standing focus of research. The strength of magnetic damping is usually quantified by the Gilbert damping constant in the Landau-Lifshitz-Gilbert equation. Here we propose a first-principles based approach to evaluate the Gilbert damping constant contributed by spin-lattice coupling in magnetic insulators. The approach involves effective Hamiltonian models and spin-lattice dynamics simulations. As a case study, we applied our method to Y$_3$Fe$_5$O$_{12}$, MnFe$_2$O$_4$ and Cr$_2$O$_3$. Their damping constants were calculated to be $0.8\times10^{-4}$, $0.2\times10^{-4}$, $2.2\times 10^{-4}$, respectively at a low temperature. The results for Y$_3$Fe$_5$O$_{12}$ and Cr$_2$O$_3$ are in good agreement with experimental measurements, while the discrepancy in MnFe$_2$O$_4$ can be attributed to the inhomogeneity and small band gap in real samples. The stronger damping observed in Cr$_2$O$_3$, compared to Y$_3$Fe$_5$O$_{12}$, essentially results from its stronger spin-lattice coupling. In addition, we confirmed a proportional relationship between damping constants and the temperature difference of subsystems, which had been reported in previous studies. These successful applications suggest that our approach serves as a promising candidate for estimating the Gilbert damping constant in magnetic insulators.

cond-mat.mtrl-sci↗

arXiv2023

Chiral magnetism in lithium-decorated monolayer CrTe$_{2}$: Interplay between Dzyaloshinskii-Moriya interaction and higher-order interactions

Chiral magnetic states in two-dimensional (2D) layered noncentrosymmetric magnets, which are promising advanced spintronic materials, are usually attributed to Dzyaloshinskii-Moriya interactions (DMI). However, the role of underlying higher-order spin couplings in determining the properties of chiral spin textures has much less reported. In this work, taking the lithium-decorated monolayer CrTe$_{2}$ (monolayer LiCrTe$_{2}$) as an example, we develop a first-principles-based comprehensive spin model constructed by using the symmetry-adapted cluster expansion method. Based on this spin model, we identify the ground state of monolayer LiCrTe$_{2}$ as a chiral spin spiral state, which can further assemble macroscopic chiral labyrinth domains (LD) under zero-field conditions as well as evolve into skyrmions under a finite magnetic field. Moreover, higher-order biquadratic and three-site interactions are identified to be responsible for modulating both the size and the field stability of the spin spiral state. Our study sheds light on complex magnetic couplings in 2D magnets.

cond-mat.mtrl-sci↗