SearcharxivSearch

arXiv subjects

Liuyan Zhao

Publications and source records attributed to Liuyan Zhao.

At least 19 recordsLinked to original sources

Observation and Control of the Magnetic Photogalvanic Effect from Strongly Bound Excitons

Photogalvanic effects arising from the quantum geometry of noncentrosymmetric materials are promising for next-generation light-harvesting devices that do not require a built-in electric field. Recent theories predict photogalvanic currents generated in magnetic systems with spin-dependent symmetry breaking as well as by bound exciton states, allowing for potential magnetic field control of the photoresponse and enhanced detection of deep sub-gap signals, respectively. We demonstrate the magnetic photogalvanic effect in a bilayer CrI3 tunnel junction with both magnetic field switching and electric field tuning of interlayer symmetry. By controlling for the polarization and energy of light illumination, we disentangle the shift and injection current contributions and find that the peak response occurs under resonant excitation of strongly bound excitons in CrI3. Our results can be captured within a many-body framework of the photogalvanic effect, while our devices function as tunable, multispectral helicity- and polarization-sensitive detectors that highlight the potential of 2D magnets for future optoelectronic applications.

cond-mat.mtrl-sci

Magneto-Moiré Excitons in Twisted Bilayer CrSBr

Moiré superlattices in van der Waals materials have revolutionized the study of electronic and excitonic systems by creating periodic electrostatic potentials. Extending this concept to magnetic materials promises new pathways in merging spintronics with photonics. While moiré magnetism has been revealed with near-field probes and nonlinear optical techniques, the coupling of these magnetic textures to optical excitations - magneto-moiré excitons - remains unexplored. Here, we report the observation of magneto-moiré excitons in twisted bilayer CrSBr, correlated with moiré spin textures that emerge below a critical twist angle of ~2°. The nanoscale moiré spin texture imprints distinct signatures onto the optical spectrum, shifting the exciton energy via a periodic magnetic exchange field. First-principles calculations corroborate that these signatures arise from one-dimensional spin textures governed by the balance of exchange interactions and domain wall energy. Our results demonstrate that moiré magnetism can be used to engineer nanoscale excitonic energy landscapes, providing a new platform for magneto-optical sensing, quantum transduction, and control of non-collinear magnetism and topology through light.

cond-mat.mes-hall

Domain wall induced topological Hall effect in the chiral-lattice ferromagnet Fe$_x$TaS$_2$

Magnetic topology and its associated emergent phenomena are central to realizing intriguing quantum states and spintronics functionalities. Designing spin textures to achieve strong and distinct electrical responses remains a significant challenge. Layered transition metal dichalcogenides offer a versatile platform for tailoring structural and magnetic properties, enabling access to a wide spectrum of topological magnetic states. Here, we report a domain-wall-driven, large, and tunable topological Hall effect (THE) in a non-centrosymmetric intercalated transition metal dichalcogenides series Fe$_x$TaS$_2$. By systematically varying the Fe intercalation level, we exert precise control over the magnetic ground states, allowing manipulation of the topological Hall effect. Real-space magnetic force microscopy (MFM) provides direct evidence of periodic magnetic stripe domain formation, confirming the microscopic origin of the observed topological transport phenomena. Our findings establish a promising way for tuning the topology of domains to generate substantial electromagnetic responses in layered magnetic materials.

cond-mat.mtrl-sci

Emergent Atomic Scale Polarisation Vortices in BaTiS3

Topological defects, such as vortices and skyrmions in magnetic and dipolar systems, can give rise to properties that are not observed in typical magnets and dielectrics. Here, we report the discovery of long-range ordered periodic dipole arrays of atomic-scale vortices and antivortices in the unconventional charge-density-wave (CDW) phase of BaTiS3, a quasi-1D chalcogenide. Synchrotron X-ray diffraction (XRD) reveals the presence of a multi-q ordering in BaTiS3 that confines vortex-vortex-antivortex polarisation triplets to the a-b plane with alternating handedness along the c-axis. The multi-q displacive distortions are characterised by three distinctive off-centre TiS6 configurations, whose ratios are independently confirmed by 47/49Ti solid-state nuclear magnetic resonance (SSNMR). Using first-principles calculations and phenomenological modelling, we show that the dipolar vortex unit cell in BaTiS3 arises from the coupling between multiple lattice instabilities arising from flat, soft phonon bands. This mechanism contrasts with classical dipolar textures in ferroelectric heterostructures that emerge from the competition between electrostatic and strain energies. The observation of dipolar vortices in BaTiS3 brings the ultimate scaling limit for real-space dipolar topological structures down to about a nanometre and unveils the intimate connection between crystal symmetry and real-space topology. Our work sets up zero-filling semiconducting materials with competing structural instabilities as a playground for realising and understanding quantum polarisation topologies.

cond-mat.mtrl-sci

Tuning Coupled Toroidic and Polar Orders in a Bilayer Antiferromagnet

Magnetic toroidal order features a loop-like arrangement of magnetic dipole moments, thus breaking both spatial inversion (P) and time-reversal (T) symmetries while preserving their combined PT sym-metry. This PT symmetry enables a linear magnetoelectric effect, allowing the coupling between magnetic toroidicity and electric polarity. However, the detection and control of two-dimensional (2D) magnetic toroidal order and the investigation of its linear magnetoelectric response remain largely unexplored. Here, using bilayer CrSBr as a platform, which hosts an in-plane layer-antiferromagnetic (AFM) order and simultaneously exhibits a magnetic toroidal order, we show compelling evidence for tuning this 2D magnetic toroidicity and its induced electric polarity through magnetic-field-depend-ent second harmonic generation (SHG). Under an out-of-plane magnetic field, we decompose the SHG signal into a time-reversal-odd component that scales with the magnetic toroidal moment and a time-reversal-even component that is proportional to the electric polarization. When sweeping the magnetic field from positive to negative values, we observe that the magnetic toroidicity retains its sign but diminishes in magnitude at higher fields while the electric polarity flips its sign and increases in strength at increasing fields below a critical threshold. When applying an in-plane electric field along the Néel vector direction, together with an out-of-plane field, we find that the magnetic toroidal and electric polar domains are moved in a locked fashion. These findings underscore the promise of 2D magnetic toroidal order in realizing giant linear magnetoelectric effects, opening exciting possi-bilities for next-generation electronic, magnetic, optical, and photonic devices enabled by 2D mag-netoelectrics.

cond-mat.mtrl-sci

Intertwined polar, chiral, and ferro-rotational orders in a rotation-only insulator

Intertwined orders refer to strongly coupled and mutually dependent orders that coexist in correlated electron systems, often underpinning key physical properties of the host materials. Among them, polar, chiral, and ferro-rotational orders have been theoretically known to form a closed set of intertwined orders. However, experimental investigation into their mutual coupling and physical consequences has remained elusive. In this work, we employ the polar-chiral insulator Ni$_3$TeO$_6$ as a platform and utilize a multimodal optical approach to directly probe and reveal the intertwining among polarity, chirality, and ferro-rotational order. We demonstrate how their coupling governs the formation of domains and dictates the nature of domain walls. Within the domains, we identify spatial inversion symmetry as the operation connecting two domain states of opposite polarity and chirality, with a common ferro-rotational state serving as the prerequisite for these interlocked configurations. At the domain walls, we observe a pronounced enhancement of in-plane polarization accompanied by a suppression of chirality. By combining with Ginzburg-Landau theory within the framework of a pre-existing ferro-rotational background, we uncover the emergence of mixed N\'eel- and Bloch-type domain walls. Our findings highlight the critical role of intertwined orders in defining domain and domain wall characteristics and open pathways for domain switching and domain wall control via intertwined order parameters.

cond-mat.mtrl-sci

Direct observation of distinct bulk and edge nonequilibrium spin accumulation in ultrathin MoTe$_2$

Low-symmetry two-dimensional (2D) topological materials such as MoTe$_2$ host efficient charge-to-spin conversion (CSC) mechanisms that can be harnessed for novel electronic and spintronic devices. However, the nature of the various CSC mechanisms and their correlation with underlying crystal symmetries remain unsettled. In this work, we use local spin-sensitive electrochemical potential measurements to directly probe the spatially dependent nonequilibrium spin accumulation in MoTe$_2$ flakes down to four atomic layers. We are able to clearly disentangle contributions originating from the spin Hall and Rashba-Edelstein effects and uncover an abundance of unconventional spin polarizations that develop uniquely in the sample bulk and edges with decreasing thickness. Using ab-initio calculations, we construct a unified understanding of all the observed CSC components in relation to the material dimensionality and stacking arrangement. Our findings not only illuminate previous CSC results on MoTe$_2$ but also have important ramifications for future devices that can exploit the local and layer-dependent spin properties of this 2D topological material.

cond-mat.mes-hall

Tunable symmetry breaking in a hexagonal-stacked moiré magnet

Symmetry plays a central role in defining magnetic phases, making tunable symmetry breaking across magnetic transitions highly desirable for discovering non-trivial magnetism. Magnetic moiré superlattices, formed by twisting two-dimensional (2D) magnetic crystals, have been theoretically proposed and experimentally explored as platforms for unconventional magnetic states. However, despite recent advances, tuning symmetry breaking in moiré magnetism remains limited, as twisted 2D magnets, such as rhombohedral (R)-stacked twisted CrI_3, largely inherit the magnetic properties and symmetries of their constituent layers. Here, in hexagonal-stacked twisted double bilayer (H-tDB) CrI_3, we demonstrate clear symmetry evolution as the twist angle increases from 180^{\circ} to 190^{\circ}. While the net magnetization remains zero across this twist angle range, the magnetic phase breaks only the three-fold rotational symmetry at 180^{\circ}, but it breaks all of the rotational, mirror, and time-reversal symmetries at intermediate twist angles between 181^{\circ} and 185^{\circ}, and all broken symmetries are recovered at 190^{\circ}. These pronounced symmetry breakings at intermediate twist angles are accompanied by metamagnetic behaviors, evidenced by symmetric double hysteresis loops around zero magnetic field. Together, these results reveal that H-tDB CrI_3 at intermediate twist angles host a distinct moiré magnetic phase, featuring periodic in-plane spin textures with broken rotational, mirror, and time-reversal symmetries, which is markedly different from the out-of-plane layered antiferromagnetism in bilayer CrI_3 and the predominantly out-of-plane moiré magnetism in R-tDB CrI_3. Our work establishes H-stacked CrI_3 moiré magnets as a versatile platform for engineering magnetic properties, including and likely beyond complex spin textures.

cond-mat.mtrl-sci

The Future of the Correlated Electron Problem

A central problem in modern condensed matter physics is the understanding of materials with strong electron correlations. Despite extensive work, the essential physics of many of these systems is not understood and there is very little ability to make predictions in this class of materials. In this manuscript we share our personal views on the major open problems in the field of correlated electron systems. We discuss some possible routes to make progress in this rich and fascinating field. This manuscript is the result of the vigorous discussions and deliberations that took place at Johns Hopkins University during a three-day workshop January 27, 28, and 29, 2020 that brought together six senior scientists and 46 more junior scientists. Our hope, is that the topics we have presented will provide inspiration for others working in this field and motivation for the idea that significant progress can be made on very hard problems if we focus our collective energies.

cond-mat.str-el

Nanoscale quantum imaging of field-free deterministic switching of a chiral antiferromagnet

Recently, unconventional spin-orbit torques (SOTs) with tunable spin generation open new pathways for designing novel magnetization control for cutting-edge spintronics innovations. A leading research thrust is to develop field-free deterministic magnetization switching for implementing scalable and energy favorable magnetic recording and storage applications, which have been demonstrated in conventional ferromagnetic and antiferromagnetic material systems. Here we extend this advanced magnetization control strategy to chiral antiferromagnet Mn3Sn using spin currents with out-of-plane canted polarization generated from low-symmetry van der Waals (vdW) material WTe2. Numerical calculations suggest that damping-like SOT of spins injected perpendicular to the kagome plane of Mn3Sn serves as a driving force to rotate the chiral magnetic order, while the field-like SOT of spin currents with polarization parallel to the kagome plane provides the bipolar deterministicity to the magnetic switching. We further introduce scanning quantum microscopy to visualize nanoscale evolutions of Mn3Sn magnetic domains during the field-free switching process, corroborating the exceptionally large magnetic switching ratio up to 90%. Our results highlight the opportunities provided by hybrid SOT material platforms consisting of noncollinear antiferromagnets and low-symmetry vdW spin source materials for developing next-generation, transformative spintronic logic devices.

cond-mat.mtrl-sci

Melting of Charge Density Waves in Low Dimensions

Charge density waves (CDWs) are collective electronic states that can reshape and melt, even while confined within a rigid atomic crystal. In two dimensions, melting is predicted to be distinct, proceeding through partially ordered nematic and hexatic states that are neither liquid nor crystal. Here we measure and explain how continuous, hexatic melting of incommensurate CDWs occurs in low-dimensional materials. As a CDW is thermally excited, disorder emerges progressively$\unicode{x2013}$initially through smooth elastic deformations that modulate the local wavelength, and subsequently via the nucleation of topological defects. Experimentally, we track three hallmark signatures of CDW melting$\unicode{x2013}$azimuthal superlattice peak broadening, wavevector contraction, and integrated intensity decay.

cond-mat.mtrl-sci

Twist Engineering of Anisotropic Excitonic and Optical Properties of a Two-Dimensional Magnetic Semiconductor

Two dimensional (2D) van der Waals (vdW) magnetic semiconductors are a new class of quantum materials for studying the emergent physics of excitons and spins in the 2D limit. Twist engineering provides a powerful tool to manipulate the fundamental properties of 2D vdW materials. Here, we show that twist engineering of the anisotropic ferromagnetic monolayer semiconductor, CrSBr, leads to bilayer magnetic semiconductors with continuously tunable magnetic moment, dielectric anisotropy, exciton energy and linear dichroism. We furthermore provide a model for exciton energy in the media with tunable anisotropy. These results advance fundamental studies on 2D vdW materials and open doors to applications to nano-optics, twistronics, and spintronics.

cond-mat.mes-hall

Emerging orthorhombic two-dimensional van der Waals magnets

Two-dimensional (2D) magnetism realized in van der Waals (vdW) materials has expanded to include a great variety of magnetic phases, over a short decade since its first discovery in 2016-2017. However, most of the investigated vdW magnets so far have highly symmetric crystal fields and isotropic in-plane lattice structures, making their 2D magnetism robust but often classical and expected. In this Perspective, we highlight a family of vdW magnets that have distorted crystal fields with low symmetries and orthorhombic crystal lattices with strong anisotropy, and furthermore, show their prospects for realizing a much richer landscape of magnetic phases and phase transitions. First, we introduce the classification of 2D vdW magnets based on their crystal fields and make a contrast between the orthorhombic vdW magnets of focus here and other popular honeycomb/hexagonal/kagome vdW magnets. We then discuss the material candidates, the emergent properties, and the designed controls for these orthorhombic 2D vdW magnets, using the representative CrSBr as an example and extending beyond it. Finally, we discuss a few existing challenges in orthorhombic 2D vdW magnets, overcome which would pave the way towards magneto-optical, opto-magnetic, and spintronic devices based on orthorhombic 2D vdW magnetism.

cond-mat.mtrl-sci

Altermagnetic Polar Metallic phase in Ultra-Thin Epitaxially-Strained RuO2 Films

Altermagnetism refers to a wide class of magnetic orders featuring magnetic sublattices with opposite spins related by rotational symmetries, resulting in non-trivial spin splitting and magnetic multipoles. However, the direct observation of the altermagnetic order parameter remains elusive. Here, by combining theoretical analysis, electrical transport, X-ray and optical spectroscopies, we establish a phase diagram in hybrid molecular beam epitaxy-grown RuO2/TiO2 (110) films, mapping symmetries along with altermagnetic/electronic/structural phase transitions as functions of film thickness and temperature. This features a novel altermagnetic metallic polar phase in epitaxially-strained 2 nm films, extending the concept of multiferroicity to altermagnets. Such a clear signature of a magnetic phase transition at ~500 K is observed exclusively in ultrathin strained films, unlike in bulk RuO2 single crystals. These results demonstrate the potential of epitaxial heterostructure design to induce altermagnetism, paving the way for emergent novel phases with multifunctional properties.

cond-mat.mtrl-sci

Visualizing Field-free Deterministic Magnetic Switching of all-van der Waals Spin-Orbit Torque System Using Spin Ensembles in Hexagonal Boron Nitride

Recently, optically active spin defects embedded in van der Waals (vdW) crystals have emerged as a transformative quantum sensing platform to explore cutting-edge materials science and quantum physics. Taking advantage of excellent solid-state integrability, this new class of spin defects can be arranged in controllable nanoscale proximity of target materials in vdW heterostructures, showing great promise for improving spatial resolution and field sensitivity of current sensing technologies. Building on this state-of-the-art measurement platform, here we report hexagonal boron nitride-based quantum imaging of field-free deterministic magnetic switching of room-temperature two-dimensional magnet Fe3GaTe2 in an all-vdW spin-orbit torque (SOT) system. By visualizing SOT-driven variations of nanoscale Fe3GaTe2 magnetic stray field profile under different conditions, we have revealed how the observed magnetic switching evolves from deterministic to indeterministic behavior due to the interplay between out-of-plane spins, in-plane spins and Joule heating. This understanding, which is otherwise difficult to access by conventional transport measurements, offers valuable insights on material design, testing, and evaluation of next-generation vdW spintronic devices.

cond-mat.mes-hall

Uncovering the Hidden Ferroaxial Density Wave as the Origin of the Axial Higgs Mode in RTe$_3$

The recent discovery of an axial amplitude (Higgs) mode in the long-studied charge density wave (CDW) systems GdTe$_3$ and LaTe$_3$ suggests a heretofore unidentified hidden order. A theoretical study proposed that the axial Higgs results from a hidden ferroaxial component of the CDW, which could arise from non-trivial orbital texture. Here, we report extensive experimental studies on ErTe$_3$ and HoTe$_3$ that possess a high-temperature CDW similar to other RTe$_3$ (R = rare earth), along with an additional low-temperature CDW with an orthogonal ordering vector. Combining Raman spectroscopy with large-angle convergent beam electron diffraction (LACBED), rotational anisotropy second-harmonic generation (RA-SHG), and muon-spin relaxation ($μ$SR), we provide unambiguous evidence that the high-temperature CDW breaks translation, rotation, and all vertical and diagonal mirror symmetries, but not time-reversal or inversion. In contrast, the low-temperature CDW only additionally breaks translation symmetry. Simultaneously, Raman scattering shows the high-temperature CDW produces an axial Higgs mode while the low-temperature mode is scalar. The weak monoclinic structural distortion and clear axial response in Raman and SHG are consistent with a ferroaxial phase in RTe$_3$ driven by coupled orbital and charge orders. Thus, our study provides a new standard for uncovering unconventional orders and confirms the power of Higgs modes to reveal them.

cond-mat.str-el

La$_2$O$_3$Mn$_2$Se$_2$: a correlated insulating layered d-wave altermagnet

Altermagnets represent a new class of magnetic phases without net magnetization that are invariant under a combination of rotation and time reversal. Unlike conventional collinear antiferromagnets (AFM), altermagnets could lead to new correlated states and important material properties deriving from their non-relativistic spin-split band structure. Indeed, they are the magnetic analogue of unconventional superconductors and can yield spin polarized electrical currents in the absence of external magnetic fields, making them promising candidates for next-generation spintronics. Here, we report altermagnetism in the correlated insulator, magnetically-ordered tetragonal oxychalcogenide, La$_2$O$_3$Mn$_2$Se$_2$. Symmetry analysis reveals a $\mathit{d}_{x^2 - y^2}$-wave type spin momentum locking, which is supported by density functional theory (DFT) calculations. Magnetic measurements confirm the AFM transition below $\sim$166 K while neutron pair distribution function analysis reveals a 2D short-range magnetic order that persists above the Néel temperature. Single crystals are grown and characterized using X-ray diffraction, optical and electron microscopy, and microRaman spectroscopy to confirm the crystal structure, stoichiometry, and uniformity.

cond-mat.mtrl-sci

Incommensurate Transverse Peierls Transition

In one-dimensional quantum materials, conducting electrons and the underlying lattices can undergo a spontaneous translational symmetry breaking, known as Peierls transition. For nearly a century, the Peierls transition has been understood within the paradigm of electron-electron interactions mediated by longitudinal acoustic phonons. This classical picture has recently been revised in topological semimetals, where transverse acoustic phonons can couple with conducting p-orbital electrons and give rise to an unconventional Fermi surface instability, dubbed the transverse Peierls transition (TPT). Most interestingly, the TPT induced lattice distortions can further break rotation or mirror/inversion symmetries, leading to nematic or chiral charge density waves (CDWs). Quantum materials that host the TPT, however, have not been experimentally established. Here, we report the experimental discovery of an incommensurate TPT in the tetragonal Dirac semimetal EuAl$_4$. Using inelastic x-ray scattering with meV resolution, we observe the complete softening of a transverse acoustic phonon at the CDW wavevector upon cooling, whereas the longitudinal acoustic phonon is nearly unchanged. Combining with first principles calculations, we show that the incommensurate CDW wavevector matches the calculated charge susceptibility peak and connects the nested Dirac bands with Al 3$p_{x}$ and 3$p_{y}$ orbitals. Supplemented by second harmonic generation measurements, we show that the CDW induced lattice distortions break all vertical and diagonal mirrors whereas the four-fold rotational symmetry is retained below the CDW transition. Our observations strongly suggest a chiral CDW in EuAl$_4$ and highlight the TPT as a new avenue for chiral quantum states.

cond-mat.str-el