Air pollution and greenhouse emissions are a significant problem across various sectors, urging the need for advanced technologies to detect and capture harmful gases. In recent years, two-dimensional (2D) materials have attracted an increasing attention due to their large surface-to-volume ratio and reactivity. Herein, we investigate the potential of single-layer CrSBr for gas sensing and capturing by means of first-principles calculations. We explore the adsorption behaviour of different pollutant gases (H$_2$S, NH$_3$, NO, NO$_2$, CO and CO$_2$) on this 2D ferromagnet and the impact of intrinsic defects on its magnetic properties. Interestingly, we find that Br vacancies enhance the adsorption of NH$_3$, NO and NO$_2$ and induces a selective frequency shift on the magnon dispersion. This work motivates the creation of novel magnonic gas sensing devices based on 2D van der Waals magnetic materials.
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…
CrSBr is an air-stable 2D van der Waals semiconducting magnet with great technological promise, but its atomic-scale magnetic interactions -- crucial information for high-frequency switching -- are poorly understood. We present an experimental study to determine the CrSBr magnetic exchange Hamiltonian and bulk magnon spectrum. We confirm the $A$-type antiferromagnetic order using single crystal neutron diffraction. We also measure the magnon dispersions using inelastic neutron scattering and rigorously fit the excitation modes to a spin wave model. The magnon spectrum is well described by an i…
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…
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…
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。
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…
Magnon softening in a ferromagnetic monolayer: a first-principles spin dynamics study
我们采用第一性原理计算和原子自旋动力学模拟相结合的方法研究了Fe/W（110）单层系统。我们主要研究平行于[001]方向的自旋波的色散。我们的研究结果与Prokop等人的实验数据[Phys. Rev. Lett. 102，177206]，并正确地捕捉到一个急剧软化的磁振子谱，相对于体心立方铁。反驳了巡游电子模型，特别是密度泛函理论给出的巡游电子模型的缺点。我们还表明，有限的温度效应是显着的，原子自旋动力学模拟代表了一个强大的工具，其中包括这些。
We present first principles calculations of the two-particle excitation spectrum of CrI$_3$ using many-body perturbation theory including spin-orbit coupling. Specifically, we solve the Bethe-Salpeter equation, which is equivalent to summing up all ladder diagrams with static screening and it is shown that excitons as well as magnons can be extracted seamlessly from the calculations. The resulting optical absorption spectrum as well as the magnon dispersion agree very well with recent measurements and we extract the amplitude for optical excitation of magnons resulting from spin-orbit interact…
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 …
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…
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）
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）
The strong coupling between photons and matter excitations such as excitons, phonons, and magnons is of central importance in the study of light-matter interactions. Bridging the flying and stationary quantum states, the strong light-matter coupling enables the coherent transmission, storage, and processing of quantum information, which is essential for building photonic quantum networks. Over the past few decades, exciton-polaritons have attracted substantial research interest due to their half-light-half-matter bosonic nature. Coupling exciton-polaritons with magnetic orders grants access to…
Monolayer chromium trihalides, the archetypal two dimensional (2D) magnetic materials, are readily suggested as a promising platform for high frequency magnonics. Here we detail the spin wave properties of monolayer CrBr$_3$ and CrI$_3$, using spin dynamics simulations parametrized from the first principles. We reveal that spin wave dispersion can be tuned in a broad range of frequencies by strain, paving the way towards flexo magnonic applications. We further show that ever present halide vacancies in these monolayers host sufficiently strong Dzyaloshinskii Moriya interaction to scatter spin …
Strongly Magnetically Tuned Coupling Strength and Nonlinearity in CrSBr Exciton-Polaritons
Peking University（北京大学）；Institute of Semiconductors, Chinese Academy of Sciences（中国科学院半导体研究所）；University of Chinese Academy of Sciences（中国科学院大学）；Paderborn University（帕德博恩大学）；National Center for Nanoscience and Technology（国家纳米科学中心）；Shandong University（山东大学）；Xi’an Jiaotong University（西安交通大学）
Temperature and field dependence of collective spin excitations or magnon in monolayer honeycomb spin lattices is investigated using an anisotropic exchange XZ-Heisenberg model in an external field. Magnetic phase transition in the presence of the transverse field is the spin reorientation (SR) transition with magnon intensity existing above the SR temperature. The transverse field either decreases or sustains the spin-wave intensity in the temperature region below or above the SR temperature, respectively. The gap of the zero-momentum low-energy magnon branch closes at the SR transverse field…
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）
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…
Two-dimensional van der Waals Janus materials and their heterostructures offer fertile platforms for designing fascinating functionalities. Here, by means of systematic first-principles studies on van der Waals Janus monolayer Cr-based dichalcogenide halides CrYX (Y=S, Se, Te; X=Cl, Br, I), we find that CrSX (X=Cl, Br, I) are the very desirable high TC ferromagnetic semiconductors with an out-of-plane magnetization. Excitingly, by the benefit of the large magnetic moments on ligand S2- anions, the sought-after large-gap quantum anomalous Hall effect and sizable valley splitting can be achieved…
We explore possibilities for control of magnons in two-dimensional heterostructures by an external electric field acting across a dielectric barrier. By performing ab-initio calculations for a Fe monolayer and a Fe bilayer, both suspended in vacuum and deposited on Cu(001), we demonstrate that external electric field can significantly modify magnon lifetimes and that these changes can be related to field-induced changes in the layer-resolved Bloch spectral functions. For systems with more magnon dispersion branches, the gap between high- and low-energy eigenmodes varies with the external field…
Exfoliated chromium triiodide (CrI$_3$) is a layered van der Waals (vdW) magnetic insulator that consists of ferromagnetic layers coupled through antiferromagnetic interlayer exchange. The resulting permutations of magnetic configurations combined with the underlying crystal symmetry produces tunable magneto-optical phenomena that is unique to the two-dimensional (2D) limit. Here, we report the direct observation of 2D magnons through magneto-Raman spectroscopy with optical selection rules that are strictly determined by the honeycomb lattice and magnetic states of atomically thin CrI$_3$. In …
It has been predicted theoretically and indirectly confirmed experimentally that single-layer CrX$_3$ (X=Cl, Br, I) might be the prototypes of topological magnetic insulators (TMI). In this work, by using first-principles calculations combined with atomistic spin dynamics we provide a complete picture of the magnetic interactions and magnetic excitations in CrX$_3$. The focus is here on the two most important aspects for the actual realization of TMI, namely the relativistic magnetic interactions and the finite-size (edge) effects. We compute the full interaction tensor, which includes both Ki…
