We present first-principles calculations of the thermal conductivity, ${\bm κ}$, of monolayer CrSBr, a van der Waals magnetic 2D material. We find a considerable thermal anisotropy, with a ratio $κ_{xx}/κ_{yy}$ of around 1.8. The anisotropy stems from a combined effect of phonon velocities and lifetimes and can be tuned by controlling the flake size by suppressing long mean path phonons.
Understanding the stability limitations and defect formation mechanisms in 2D magnets is essential for their utilization in spintronic and memory technologies. Here, we correlate defects in mono- to multilayer CrSBr with their structural, vibrational and magnetic properties. We use resonant Raman scattering to reveal distinct vibrational defect signatures. In pristine CrSBr, we show that bromine atoms mediate vibrational interlayer coupling, allowing for distinguishing between surface and bulk defect modes. We show that environmental exposure causes drastic degradation in monolayers, with the …
The recent discovery of two-dimensional (2D) magnets offers unique opportunities for the experimental exploration of low-dimensional magnetism4 and the magnetic proximity effects, and for the development of novel magnetoelectric, magnetooptic and spintronic devices. These advancements call for 2D materials with diverse magnetic structures as well as effective probes for their magnetic symmetries, which is key to understanding intralayer magnetic order and interlayer magnetic coupling. Here we apply second harmonic generation (SHG), a technique acutely sensitive to symmetry breaking, to probe t…
Two-dimensional (2D) ferromagnets have recently drawn extensive attention, and here we study the electronic structure and magnetic properties of the bulk and monolayer of CrSBr, using first-principles calculations and Monte Carlo simulations. Our results show that bulk CrSBr is a magnetic semiconductor and has the easy magnetization b-axis, hard c-axis, and intermediate a-axis. Thus, the experimental triaxial magnetic anisotropy (MA) is well reproduced here, and it is identified to be the joint effects of spin-orbit coupling (SOC) and magnetic dipole-dipole interaction. We find that bulk CrSBr…
Element-Specific Visualization of Layer-Parity and Twist-Dependent Magnetism in CrSBr
Carnegie Mellon University（卡内基梅隆大学）；Helmholtz-Zentrum Berlin für Materialien und Energie（柏林亥姆霍兹材料与能源中心）；Indian Institute of Technology Ropar（印度理工学院罗帕尔分校）；The University of Texas at Dallas（德克萨斯大学达拉斯分校）
研究 CrSBr 中层奇偶性和扭曲相关磁性，利用 X 射线磁圆二色性和线性二色性结合光发射电子显微镜解析其磁序，揭示纳米尺度磁结构及相关依赖性，还发现正交扭曲双层结构磁易轴的不同，为莫尔磁性开辟新途径。
Bulk and surface excitons in the van der Waals magnet CrSBr: Magneto-optical studies to 55 tesla
National High Magnetic Field Laboratory, Los Alamos National Laboratory（国家强磁场实验室，洛斯阿拉莫斯国家实验室）；Kyung Hee University（庆熙大学）；University of Chemistry and Technology Prague（布拉格化工大学）；Graduate Center of the City University of New York（纽约市立大学研究生院）
Magnetic excitations in layered magnetic materials that can be thinned down the two-dimensional (2D) monolayer limit are of high interest from a fundamental point of view and for applications perspectives. Raman scattering has played a crucial role in exploring the properties of magnetic layered materials and, even-though it is essentially a probe of lattice vibrations, it can reflect magnetic ordering in solids through the spin-phonon interaction or through the observation of magnon excitations. In bulk CrSBr, a layered A type antiferromagnet (AF), we show that the magnetic ordering can be di…
Layer-Dependent Phonons, Excitons, and Magneto-Optical Phenomena in CrSBr: A Mini Review
National Center for Nanoscience and Technology（中国科学院国家纳米科学中心）；University of Chinese Academy of Sciences（中国科学院大学）；University of Warsaw（华沙大学）；CNRS–UGA–UPS–INSA–EMFL（法国国家科学研究中心-格勒诺布尔阿尔卑斯大学-图卢兹第三大学-INSA图卢兹-东洛林大学）；University of Sapienza（罗马第一大学）
Layer- and Field-Dependent Magnetic Order in 2D CrSBr Revealed by Pulsed Nanocalorimetry
Catalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and BIST（加泰罗尼亚纳米科学和纳米技术研究所）；Universitat Autònoma de Barcelona（巴塞罗那自治大学）；Université Catholique de Louvain (UCLouvain)（天主教鲁汶大学）；Institut de Microelectrònica de Barcelona (IMB-CNM-CSIC)（巴塞罗那微电子研究所）；Columbia University（哥伦比亚大学）；WEL Research Institute（WEL研究所）；National Institute for Materials Science（日本国立材料研究所）
Correlated quantum phenomena in one-dimensional (1D) systems that exhibit competing electronic and magnetic order are of strong interest for studying fundamental interactions and excitations, such as Tomonaga-Luttinger liquids and topological orders and defects with properties completely different from the quasiparticles expected in their higher-dimensional counterparts. However, clean 1D electronic systems are difficult to realize experimentally, particularly magnetically ordered systems. Here, we show that the van der Waals layered magnetic semiconductor CrSBr behaves like a quasi-1D materia…
The recent isolation of two-dimensional (2D) magnets offers tantalizing opportunities for spintronics and magnonics at the limit of miniaturization. One of the key advantages of atomically-thin materials is their outstanding deformation capacity, which provides an exciting avenue to control their properties by strain engineering. Herein, we investigate the magnetic properties, magnon dispersion and spin dynamics of the air-stable 2D magnetic semiconductor CrSBr ($T_C$ = 146 K) under mechanical strain using first-principles calculations. Our results provide a deep microscopic analysis of the co…
Using first-principles full-potential density functional calculations, we predict that mechanically tunable band-gap is realizable in ZnS monolayer in graphene-like honeycomb structure by application of in-plane homogeneous biaxial strain. A transition point from direct-to-indirect gap-phase is predicted to exist for biaxial tensile strain lying in the interval (2.645%, 3.171%). In the two gap-phases, the band gap decreases with increasing strain and varies linearly with strain.
The recent advent of two-dimensional monolayer materials with tunable optoelectronic properties and high carrier mobility offers renewed opportunities for efficient, ultra-thin excitonic solar cells alternative to those based on conjugated polymer and small molecule donors. Using first-principles density functional theory and many-body calculations, we demonstrate that monolayers of hexagonal BN and graphene (CBN) combined with commonly used acceptors such as PCBM fullerene or semiconducting carbon nanotubes can provide excitonic solar cells with tunable absorber gap, donor-acceptor interface …
van der Waals (vdW) magnets are receiving ever-growing attention nowadays due to their significance in both fundamental research on low-dimensional magnetism and potential applications in spintronic devices. High crystalline quality of vdW magnets is key for maintaining intrinsic magnetic and electronic properties, especially when exfoliated down to the 2D limit. Here, ultrahigh-quality air-stable vdW CrSBr crystals are synthesized using the direct vapor-solid synthesis method. The high single crystallinity and spatial homogeneity have been thoroughly evidenced at length scales from sub-mm to …
Although much effort has been made to explore quantum anomalous Hall effect (QAHE) in both theory and experiment, the QAHE systems with tunable Chern numbers are yet limited. Here, we theoretically propose that NiAsO$_3$ and PdSbO$_3$, monolayer transitional metal oxides, can realize QAHE with tunable Chern numbers via manipulating their magnetization orientations. When the magnetization lies in the \textit{x-y} plane and all mirror symmetries are broken, the low-Chern-number (i.e., $\mathcal{C}=\pm1$) phase emerges. When the magnetization exhibits non-zero \textit{z}-direction component, the …
We present ab initio calculations which show that the direct-band-gap, effective masses and Fermi velocities of charge carriers in ZnO monolayer (ML-ZnO) in graphene-like honeycomb structure are all tunable by application of in-plane homogeneous biaxial strain. Within our simulated strain limit of $\pm 10$%, the band gap remains direct and shows a strong non-linear variation with strain. Moreover, the average Fermi velocity of electrons in unstrained ML-ZnO is of the same order of magnitude as that in graphene. The results promise potential applications of ML-ZnO in mechatronics/straintronics …
The van der Waals material CrSBr stands out as a promising two-dimensional magnet. Especially, its high magnetic ordering temperature and versatile magneto-transport properties make CrSBr an important candidate for new devices in the emergent field of two-dimensional magnetic materials. To date, the magnetic and structural properties of CrSBr have not been fully elucidated. Here, we report on the detailed temperature-dependent magnetic and structural properties of this material, by comprehensively combining neutron scattering, muon spin relaxation spectroscopy, synchrotron X-ray diffraction, a…
Spin-Chirality-Driven Bulk Photovoltaic Effect in van der Waals Magnet CrSBr
State Key Laboratory of Low Dimensional Quantum Physics and Department of Physics, Tsinghua University（清华大学物理系低维量子物理国家重点实验室）；Frontier Science Center for Quantum Information（量子信息前沿科学中心）；RIKEN Center for Emergent Matter Science (CEMS)（理化学会新兴物质科学中心）；Graduate School of China Academy of Engineering Physics（中国工程物理研究院研究生院）；Institute for Advanced Study, Tsinghua University（清华大学高等研究院）
Moiré excitons are emergent optical excitations in 2D semiconductors with deep moiré superlattice potentials. While these excitations have been realized in several platforms, a system with dynamically tunable moiré potential to tailor the moiré exciton properties is yet to be realized. Here, we present a continuously tunable moiré potential in a monolayer WSe2 that is enabled by its proximity to twisted bilayer graphene (TBG) near the magic-angle. Due to its flat electronic bands, charge distribution is highly localized and forms a triangular lattice in TBG. Tuning the local charge density via…
Tunable Magneto-Excitonic Coupling in Alloyed van der Waals Antiferromagnet
Wroclaw University of Science and Technology（弗罗茨瓦夫科技大学）；University of Warsaw（华沙大学）；Laboratoire National des Champs Magnétiques Intenses（强磁场国家实验室）；Université Grenoble Alpes（格勒诺布尔阿尔卑斯大学）；Université Toulouse（图卢兹大学）；King’s College London（伦敦国王学院）
We report the observation and gate manipulation of intrinsic dark trions in monolayer WSe$_2$. By using ultraclean WSe$_2$ devices encapsulated by boron nitride, we directly resolve the weak photoluminescence of dark trions. The dark trions can be tuned continuously between negative and positive charged trions with electrostatic gating. We also reveal their spin triplet configuration and distinct valley optical emission by their characteristic Zeeman splitting under magnetic field. The dark trions exhibit large binding energy (14-16 meV). Their lifetime (~1.3 ns) is two orders of magnitude lon…
We investigate the electric response of chiral phonons on the low-buckled group-IVA monolayers by performing first-principles calculations. The vertical electric field breaks the degeneracy of phonon modes at high-symmetry $\pm K$ points of the phonon Brillouin zone, and the size of the phononic gap is proportional to the strength of the electric field. The gapped phonon modes at $\pm K$ possess chiralities with considerable phonon circular polarizations and discrete phonon pseudoangular momenta. The chiralities of phonons are robust against the variation of the field strength, but reversed by…
One of the most fundamental devices for electronics and optoelectronics is the PN junction, which provides the functional element of diodes, bipolar transistors, photodetectors, LEDs, and solar cells, among many other devices. In conventional PN junctions, the adjacent p- and n-type regions of a semiconductor are formed by chemical doping. Materials with ambipolar conductance, however, allow for PN junctions to be configured and modified by electrostatic gating. This electrical control enables a single device to have multiple functionalities. Here we report ambipolar monolayer WSe2 devices in …
Three-dimensional confinement allows semiconductor quantum dots (QDs) to exhibit size-tunable electronic and optical properties that enable a wide range of opto-electronic applications from displays, solar cells and bio-medical imaging to single-electron devices. Additional modalities such as spin and valley properties can provide further degrees of freedom requisite for quantum information and spintronics. When seeking to combine these material features into QD structures, however, confinement can cause hybridization that inhibits the robustness of these emergent properties for insertion into…
The influence of triaxial in-plane strain on the electronic properties of a hexagonal boron-nitride sheet is investigated using density functional theory. Different from graphene, the triaxial strain localizes the molecular orbitals of the boron-nitride flake in its center depending on the direction of the applied strain. The proposed technique for localizing the molecular orbitals that are close to the Fermi level in the center of boron nitride flakes can be used to actualize engineered nanosensors, for instance, to selectively detect gas molecules. We show that the central part of the strain…
We explore the photocatalytic ability of honeycomb lattice of borocarbonitride, $BC_{6}N$, investigating its opto-electronic properties and band-edge alignment based on hybrid density functional theory. We observe that along with pronounced visible absorbance, $BC_{6}N$ exhibits a good reducing ability. It is capable of depositing heavy metal ions, hydrogen fuel generation and carbon dioxide sequestration through photoelectrocatalysis. To broaden its applicability we further tune its redox ability using biaxial strain. We observe even a slight expansion makes this material capable of performin…
Two-dimensional (2D) materials can host stable, long-range magnetic phases in the presence of underlying magnetic anisotropy. The ability to realize the full potential of 2D magnets necessitates systematic investigation of the role of individual atomic layers and nanoscale inhomogeneity ($\textit{i.e.}$, strain) on the emergence and stability of both intra- and interlayer magnetic phases. Here, we report multifaceted spatial-dependent magnetism in few-layer CrSBr using magnetic force microscopy (MFM) and Monte Carlo-based magnetic simulations. We perform nanoscale visualization of the magnetic…
A novel topological insulator with tunable edge states, called quantum spin-quantum anomalous Hall (QSQAH) insulator, is predicted in a heterostructure of a hydrogenated Sb (SbH) monolayer on a LaFeO3 substrate by using ab initio methods. The substrate induces a drastic staggered exchange field in the SbH film, which plays an important role to generate the QSQAH effect. A topologically nontrivial band gap (up to 35 meV) is opened by Rashba spin-orbit coupling, which can be enlarged by strain and electric field. To understand the underlying physical mechanism of the QSQAH effect, a tight-bindin…
We propose a new topological quantum state of matter---the two-dimensional (2D) Weyl half semimetal (WHS), which features 2D Weyl points at Fermi level belonging to a single spin channel, such that the low-energy electrons are described by fully spin-polarized 2D Weyl fermions. We predict its realization in the ground state of monolayer PtCl$_3$. We show that the material is a half metal with an in-plane magnetization, and its Fermi surface consists of a pair of fully spin-polarized Weyl points protected by a mirror symmetry, which are robust against spin-orbit coupling. Remarkably, we show th…
Light-emitting diodes are of importance for lighting, displays, optical interconnects, logic and sensors. Hence the development of new systems that allow improvements in their efficiency, spectral properties, compactness and integrability could have significant ramifications. Monolayer transition metal dichalcogenides have recently emerged as interesting candidates for optoelectronic applications due to their unique optical properties. Electroluminescence has already been observed from monolayer MoS2 devices. However, the electroluminescence efficiency was low and the linewidth broad due both …
The electronic topology is generally related to the Berry curvature, which can induce the anomalous Hall effect in time-reversal symmetry breaking systems. Intrinsic monolayer transition metal dichalcogenides possesses two nonequivalent K and K' valleys, having Berry curvatures with opposite signs, and thus vanishing anomalous Hall effect in this system. Here we report the experimental realization of asymmetrical distribution of Berry curvature in a single valley in monolayer WSe2 through applying uniaxial strain to break C3v symmetry. As a result, although the Berry curvature itself is still …
Exciton-polariton condensate in the van der Waals magnet CrSBr
Carl von Ossietzky University Oldenburg（奥尔登堡卡尔·冯·奥西茨基大学）；University of Exeter（埃克塞特大学）；Xiamen University Malaysia（厦门大学马来西亚分校）；Beijing University of Technology（北京工业大学）；Technion-Israel Institute of Technology（以色列理工学院）；Guangdong Technion-Israel Institute of Technology（广东以色列理工学院）；Friedrich Schiller University Jena（耶拿弗里德里希·席勒大学）；Fraunhofer-Institute for Applied Optics and Precision Engineering IOF（弗劳恩霍夫应用光学和精密工程研究所）；Max Planck School of Photonics（马克斯·普朗克光子学校）；University of Chemistry and Technology Prague（布拉格化学技术大学）；University of Sheffield（谢菲尔德大学）
We find, through first-principles calculations, that hole doping induces a ferromagnetic phase transition in monolayer GaSe. Upon increasing hole density, the average spin magnetic moment per carrier increases and reaches a plateau near 1.0 $μ_{\rm{B}}$/carrier in a range of $3\times 10^{13}$/cm$^{2}$-$1\times 10^{14}$/cm$^{2}$ with the system in a half-metal state before the moment starts to descend abruptly. The predicted magnetism originates from an exchange splitting of electronic states at the top of the valence band where the density of states exhibits a sharp van Hove singularity in thi…
