arXiv subjects

Zeyuan Sun

Publications and source records attributed to Zeyuan Sun.

12 recordsLinked to original sources

arXiv2026

Unveiling the impact of anti-site defects in magnetic transitions of few-layer MnBi2Te4 by operando heating

As the first experimentally discovered intrinsic magnetic topological insulator, MnBi2Te4 has attracted widespread attentions, providing a unique platform for the exploration of topological quantum phases, such as quantum anomalous Hall effect and axion insulator state. Despite the increasing number of potential factors affecting samples being identified, obtaining the high-quality device performance with desired topological quantum phases remains a challenge. In this work, by comparing the reflective magnetic circular dichroism (RMCD) of crystals with different defect densities that are characterized by atomically resolved scanning tunneling microscopy, we demonstrate that anti-site defects play an essential role in achieving ideal magnetic states. By measuring RMCD hysteresis loops with operando heating, we find that MnBi2Te4 few-layer samples are highly susceptible to thermal impact, even at temperature as low as 45{\deg}C. The magnetic behavior of heating-treated samples is akin to that of samples fabricated into devices, revealing the thermal impact on devices as well. Starting from few-layers with ideal layer-dependent magnetic order, thermal heating leads to the convergence of magnetization and transition fields between odd- and even-layers. The observed heating-induced magnetic evolution can serve as a valuable reference for assessing the sample quality or the density of anti-site defects. Our findings not only point out the long-standing hidden factor that arose controversies in MnBi2Te4, but also pave the way for controllably engineering the topological quantum phenomena.

cond-mat.mtrl-sci↗

arXiv2025

pH Regulates Ion Dynamics in Carboxylated Mixed Conductors

Coupled ionic and electronic transport underpins processes as diverse as electrochemical energy conversion, biological signaling, and soft adaptive electronics. Yet, how chemical environments such as pH modulate this coupling at the molecular scale remains poorly understood. Here, we show that the protonation state of carboxylated polythiophenes provides precise chemical control over ion dynamics, doping efficiency, solvent uptake and mechanical response. The findings establish molecular acidity as a general strategy to program ionic preference and mechanical stability, offering design principles for pH-responsive mixed conductors and soft electronic materials that couple ionic, electronic, and mechanical functionality.

cond-mat.mtrl-sci↗

arXiv2025

Roadmap for Photonics with 2D Materials

Triggered by the development of exfoliation and the identification of a wide range of extraordinary physical properties in self-standing films consisting of one or few atomic layers, two-dimensional (2D) materials such as graphene, transition metal dichalcogenides (TMDs), and other van der Waals (vdW) crystals currently constitute a wide research field protruding in multiple directions in combination with layer stacking and twisting, nanofabrication, surface-science methods, and integration into nanostructured environments. Photonics encompasses a multidisciplinary collection of those directions, where 2D materials contribute with polaritons of unique characteristics such as strong spatial confinement, large optical-field enhancement, long lifetimes, high sensitivity to external stimuli (e.g., electric and magnetic fields, heating, and strain), a broad spectral range from the far infrared to the ultraviolet, and hybridization with spin and momentum textures of electronic band structures. The explosion of photonics with 2D materials as a vibrant research area is producing breakthroughs, including the discovery and design of new materials and metasurfaces with unprecedented properties as well as applications in integrated photonics, light emission, optical sensing, and exciting prospects for applications in quantum information, and nanoscale thermal transport. This Roadmap summarizes the state of the art in the field, identifies challenges and opportunities, and discusses future goals and how to meet them through a wide collection of topical sections prepared by leading practitioners.

cond-mat.mtrl-sci↗

arXiv2024

Resolving and routing the magnetic polymorphs in 2D layered antiferromagnet

Polymorphism, commonly denoting the variety of molecular or crystal structures, is a vital element in many natural science disciplines. In van der Waals layered antiferromagnets, a new type of magnetic polymorphism is allowed by having multiple layer-selective magnetic structures with the same total magnetization. However, resolving and manipulating such magnetic polymorphs remain a great challenge. Here we use the phase-resolved magnetic second-harmonic generation microscopy to elucidate such magnetic polymorphism in the 2D semiconducting layered antiferromagnet chromium sulfur bromide (CrSBr), and demonstrate how the magnetic polymorphs can be deterministically switched in an unprecedented layer-selective manner. With the nonlinear magneto-optical technique unveiling the magnetic symmetry information through the amplitude and phase of light, we could unambiguously resolve the polymorphic spin-flip transitions in CrSBr bilayers and tetralayers. Remarkably, the deterministic routing of polymorphic transitions originates from the breaking of energy degeneracy via a magnetic layer-sharing effect: the spin-flip transitions in a tetralayer are governed by the laterally extended bilayer, which acts as a control bit. We envision such controllable magnetic polymorphism to be ubiquitous for van der Waals layered antiferromagnets, and could lead to conceptually new design and construction of spintronic and opto-spintronic devices for probabilistic computation and neuromorphic engineering.

cond-mat.mes-hall↗

arXiv2024

Magnetostatic effect on spin dynamics properties in antiferromagnetic Van der Waals material CrSBr

Van der Waals (vdW) antiferromagnets are exceptional platforms for exploring the spin dynamics of antiferromagnetic materials owing to their weak interlayer exchange coupling. In this study, we examined the antiferromagnetic resonance spectra of anisotropic Van der Waals antiferromagnet CrSBr. In addition to the ordinary resonance modes, we observed a dipolar spin wave mode when the microwave field was oriented perpendicular to the in-plane easy axis of CrSBr. Furthermore, our results uncovered a pronounced dependency of various resonant modes on the orientation of the microwave field, which is pivotal for the accurate determination of exchange coupling constants. Numerical simulations have elucidated this orientation dependence of spin dynamics arises from the magnetostatic effect. This discovery underscores the previously underappreciated significance of dipolar interactions in shaping the dynamical properties of two-dimensional AFM materials, thereby enhancing our understanding of the intrinsic dynamic properties of vdW magnets.

cond-mat.mtrl-sci↗

arXiv2024

Spin texture and tunneling magnetoresistance in atomically thin CrSBr

The exploration of spin configurations and magnetoresistance in van der Waals magnetic semiconductors, particularly in the realm of thin-layer structures, is of paramount significance for the development of two-dimensional spintronic nanodevices. In this letter, we present detailed magneto-transport and photoluminescence studies on few-layer CrSBr flakes utilizing a vertical tunneling device configuration. Our investigations revealed complex magnetic states along the evolutionary path of few-layer CrSBr. We observed intermediate states exhibiting identical net magnetization demonstrate rectification properties, reminiscent of a diode-like behavior at positive and negative bias voltages. Notably, in devices with 5-layer CrSBr, we detected an intriguing positive magnetoresistive state when subjected to an in-plane magnetic field along the b-axis. The implementation of the Mott two-current model successfully calculated the tunneling resistance of different magnetic states, thereby elucidating the spin configurations responsible for the observed transport phenomena. These insights not only provide new perspectives on the intricate spin textures of two-dimensional CrSBr but also highlight the efficacy of tunneling measurements as a sensitive method for probing magnetic order in van der Waals materials.

cond-mat.mes-hall↗

arXiv2024

Balancing Rigor and Utility: Mitigating Cognitive Biases in Large Language Models for Multiple-Choice Questions

This paper examines the role of cognitive biases in the decision-making processes of large language models (LLMs), challenging the conventional goal of eliminating all biases. When properly balanced, we show that certain cognitive biases can enhance decision-making efficiency through rational deviations and heuristic shortcuts. By introducing heuristic moderation and an abstention option, which allows LLMs to withhold responses when uncertain, we reduce error rates, improve decision accuracy, and optimize decision rates. Using the Balance Rigor and Utility (BRU) dataset, developed through expert collaboration, our findings demonstrate that targeted inspection of cognitive biases aligns LLM decisions more closely with human reasoning, enhancing reliability and suggesting strategies for future improvements. This approach offers a novel way to leverage cognitive biases to improve the practical utility of LLMs across various applications.

cs.CL↗

arXiv2023

Extrinsic nonlinear Kerr rotation in topological materials under a magnetic field

Topological properties in quantum materials are often governed by symmetry and tuned by crystal structure and external fields, and hence symmetry-sensitive nonlinear optical measurements in a magnetic field are a valuable probe. Here we report nonlinear magneto-optical second harmonic generation (SHG) studies of non-magnetic topological materials including bilayer WTe2, monolayer WSe2 and bulk TaAs. The polarization-resolved patterns of optical SHG under magnetic field show nonlinear Kerr rotation in these time-reversal symmetric materials. For materials with three-fold rotational symmetric lattice structure, the SHG polarization pattern rotates just slightly in a magnetic field, whereas in those with mirror or two-fold rotational symmetry the SHG polarization pattern rotates greatly and distorts. These different magneto-SHG characters can be understood by considering the superposition of the magnetic field-induced time-noninvariant nonlinear optical tensor and the crystal-structure-based time-invariant counterpart. The situation is further clarified by scrutinizing the Faraday rotation, whose subtle interplay with crystal symmetry accounts for the diverse behavior of the extrinsic nonlinear Kerr rotation in different materials. Our work illustrates the application of magneto-SHG techniques to directly probe nontrivial topological properties, and underlines the importance of minimizing extrinsic nonlinear Kerr rotation in polarization-resolved magneto-optical studies.

cond-mat.mes-hall↗

arXiv2023

Layer thickness crossover of type-II multiferroic magnetism in NiI2

The discovery of atomically thin van der Waals ferroelectric and magnetic materials encourages the exploration of 2D multiferroics, which holds the promise to understand fascinating magnetoelectric interactions and fabricate advanced spintronic devices. In addition to building a heterostructure consisting of ferroelectric and magnetic ingredients, thinning down layered multiferroics of spin origin such as NiI2 becomes a natural route to realize 2D multiferroicity. However, the layer-dependent behavior, widely known in the community of 2D materials, necessitates a rigorous scrutiny of the multiferroic order in the few-layer limit. Here, we interrogate the layer thickness crossover of helimagnetism in NiI2 that drives the ferroelectricity and thereby type-II multiferroicity. By using wavelength-dependent polarization-resolved optical second harmonic generation (SHG) to probe the ferroic symmetry, we find that the SHG arises from the inversion-symmetry-breaking magnetic order, not previously assumed ferroelectricity. This magnetism-induced SHG is only observed in bilayer or thicker layers, and vanishes in monolayer, suggesting the critical role of interlayer exchange interaction in breaking the degeneracy of geometrically frustrated spin structures in triangular lattice and stabilizing the type-II multiferroic magnetism in few-layers. While the helimagnetic transition temperature is layer dependent, the few-layer NiI2 exhibits another thickness evolution and reaches the bulk-like behavior in trilayer, indicated by the intermediate centrosymmetric antiferromagnetic state as revealed in Raman spectroscopy. Our work therefore highlights the magnetic contribution to SHG and Raman spectroscopy in reduced dimension and guides the optical study of 2D multiferroics.

cond-mat.mtrl-sci↗

arXiv2019

Direct observation of van der Waals stacking dependent interlayer magnetism

Controlling the crystal structure is a powerful approach for manipulating the fundamental properties of solids. Unique to two-dimensional (2D) van der Waals materials, the control can be achieved by modifying the stacking order through rotation and translation between the layers. Here, we report the first observation of stacking dependent interlayer magnetism in the 2D magnetic semiconductor, chromium tribromide (CrBr3), enabled by the successful growth of its monolayer and bilayer through molecular beam epitaxy. Using in situ spin-polarized scanning tunneling microscopy and spectroscopy, we directly correlated the atomic lattice structure with observed magnetic order. We demonstrated that while individual CrBr3 monolayer is ferromagnetic, the interlayer coupling in bilayer depends strongly on the stacking order and can be either ferromagnetic or antiferromagnetic. Our observations provide direct experimental evidence for exploring the stacking dependent layered magnetism, and pave the way for manipulating 2D magnetism with unique layer twist angle control.

cond-mat.mes-hall↗

arXiv2019

Giant and nonreciprocal second harmonic generation from layered antiferromagnetism in bilayer CrI3

Layered antiferromagnetism is the spatial arrangement of ferromagnetic layers with antiferromagnetic interlayer coupling. Recently, the van der Waals magnet, chromium triiodide (CrI3), emerged as the first layered antiferromagnetic insulator in its few-layer form, opening up ample opportunities for novel device functionalities. Here, we discovered an emergent nonreciprocal second order nonlinear optical effect in bilayer CrI3. The observed second harmonic generation (SHG) is giant: several orders of magnitude larger than known magnetization induced SHG and comparable to SHG in the best 2D nonlinear optical materials studied so far (e.g. MoS2). We showed that while the parent lattice of bilayer CrI3 is centrosymmetric and thus does not contribute to the SHG signal, the observed nonreciprocal SHG originates purely from the layered antiferromagnetic order, which breaks both spatial inversion and time reversal symmetries. Furthermore, polarization-resolved measurements revealed the underlying C2h symmetry, and thus monoclinic stacking order in CrI3 bilayers, providing crucial structural information for the microscopic origin of layered antiferromagnetism. Our results highlight SHG as a highly sensitive probe that can reveal subtle magnetic order and open novel nonlinear and nonreciprocal optical device possibilities based on 2D magnets.

cond-mat.mes-hall↗

arXiv2019

Pressure-controlled Structural Symmetry Transition in Layered InSe

Structural symmetry of crystals plays important roles in physical properties of two-dimensional (2D) materials, particularly in the nonlinear optics regime. It has been a long-term exploration on the physical properties in 2D materials with various stacking structures, which correspond to different structural symmetries. Usually, the manipulation of rotational alignment between layers in 2D heterostructures has been realized at the synthetic stage through artificial stacking like assembling Lego bricks. However, the reconfigurable control of translational symmetry of crystalline structure is still challenging. High pressure, as a powerful external control knob, provides a very promising route to circumvent this constraint. Here, we experimentally demonstrate a pressure-controlled symmetry transition in layered InSe. The continuous and reversible evolution of structural symmetries can be in-situ monitored by using the polarization-resolved second harmonic generation (SHG) spectroscopy. As pressure changes, the reconfigurable symmetry transition of the SHG pattern from three-fold rotational symmetry to mirror symmetry was experimentally observed in a layered InSe samples and was successfully explained by the proposed interlayer-translation model. This opens new routes towards potential applications of manipulating crystal symmetry of 2D materials.

physics.optics↗