Accessing new magnetic regimes by tuning the ligand spin-orbit coupling in van der Waals magnets

Abstract

Van der Waals (VdW) materials have opened new directions in the study of low dimensional magnetism. A largely unexplored arena is the intrinsic tuning of VdW magnets toward new ground-states. The chromium trihalides provided the first such example with a change of inter-layer magnetic coupling emerging upon exfoliation. Here, we take a different approach to engineer new ground-states, not by exfoliation, but by tuning the spin-orbit coupling (SOC) of the non-magnetic ligand atoms (Cl,Br,I). We synthesize a three-halide series, CrCl${}_{3-x-y}$Br${}_x$I${}_y$, and map their magnetic properties as a function of Cl, Br, and I content. The resulting triangular phase diagrams unveil a frustrated regime near CrCl${}_3$. First-principles calculations confirm that the frustration is driven by a competition between the chromium and halide SOCs. Furthermore, we reveal a field-induced change of inter-layer coupling in the bulk of CrCl${}_{3-x-y}$Br${}_x$I${}_y$ crystals at the same field as in the exfoliation experiments.

arXiv comment22 pages, 6 figures

References in corpus (26)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Layer-dependent Ferromagnetism in a van der Waals Crystal down to the Monolayer Limit
• Discovery of intrinsic ferromagnetism in 2D van der Waals crystals
• Gate-tunable Room-temperature Ferromagnetism in Two-dimensional Fe${}_3$GeTe${}_2$
• Two-Dimensional Itinerant Ising Ferromagnetism in Atomically thin Fe3GeTe2
• Electrical Control of 2D Magnetism in Bilayer CrI3
• Giant Tunneling Magnetoresistance in Spin-Filter van der Waals Heterostructures
• Controlling magnetism in 2D CrI3 by electrostatic doping
• Ising-Type Magnetic Ordering in Atomically Thin FePS3
• Probing magnetism in 2D van der Waals crystalline insulators via electron tunneling
• Kitaev quantum spin liquid - concept and materialization
• On the origin of magnetic anisotropy in two dimensional CrI${}_3$
• Strain-tunable magnetic anisotropy in monolayer CrCl${}_3$, CrBr${}_3$, and CrI${}_3$
• Very Large Tunneling Magnetoresistance in Layered Magnetic Semiconductor CrI${}_3$
• Electric-field control of magnetism in few-layered van der Waals magnet
• Direct observation of van der Waals stacking dependent interlayer magnetism
• Pressure-controlled interlayer magnetism in atomically thin CrI3
• Crystal and Magnetic Structures in Layered, Transition Metal Dihalides and Trihalides
• Ligand-field helical luminescence in a 2D ferromagnetic insulator
• Interplay between Kitaev interaction and single ion anisotropy in ferromagnetic CrI${}_3$ and CrGeTe${}_3$ monolayers
• Magnon-assisted tunnelling in van der Waals heterostructures based on CrBr3
• One million percent tunnel magnetoresistance in a magnetic van der Waals heterostructure
• Fundamental Spin Interactions Underlying the Magnetic Anisotropy in the Kitaev Ferromagnet CrI${}_3$
• Calculating critical temperatures for ferromagnetic order in two-dimensional materials
• Bond disordered spin liquid and the honeycomb iridate H${}_3$LiIr${}_2$O${}_6$ $-$ abundant low energy density of states from random Majorana hopping
• Thermodynamic Evidence of Proximity to a Kitaev Spin-Liquid in Ag${}_3$LiIr${}_2$O${}_6$

Cited by in corpus (24)

• Atomistic spin textures on-demand in the van der Waals layered magnet CrSBr
• Controlling magnetic exchange and anisotropy by non-magnetic ligand substitution in layered MPX3 (M = Ni, Mn; X = S, Se)
• Microscopic origin of multiferroic order in monolayer NiI${}_2$
• Strain-tunable Dzyaloshinskii--Moriya interaction and skyrmions in two-dimensional Janus Cr${}_2$X${}_3$Y${}_3$ (X, Y = Cl, Br, I, X $\ne$ Y) trihalide monolayers
• Hybridized quadrupolar excitations in the spin-anisotropic frustrated magnet FeI2
• Spin-waves in 2D honeycomb lattice $XXZ$-type van der Waals antiferromagnet CoPS${}_3$
• Progress and Prospects in Two-Dimensional Magnetism of van der Waals Materials
• Monolayer CrCl${}_3$ as an ideal Test Bed for the Universality Classes of 2D Magnetism
• Moiré-driven multiferroic order in twisted CrCl${}_3$, CrBr${}_3$ and CrI${}_3$ bilayers
• Emergence of electric-field-tunable interfacial ferromagnetism in 2D antiferromagnet heterostructures
• AC susceptometry of 2D van der Waals magnets enabled by the coherent control of quantum sensors
• Enhanced Curie temperature and skyrmion stability in room temperature ferromagnetic semiconductor CrISe monolayer
• Visualization of moiré magnons in monolayer ferromagnet
• Intrinsic staggered spin-orbit torque for the electrical control of antiferromagnets -- application to CrI${}_3$
• 2D correlations in the van der Waals ferromagnet CrBr${}_3$ using high frequency electron spin resonance spectroscopy
• Controlling magnetism through Ising superconductivity in magnetic van der Waals heterostructures
• Impurity-induced excitations in a topological two-dimensional ferromagnet/superconductor van der Waals moiré heterostructure
• Large cross-polarized Raman signal in CrI${}_3$: A first-principles study
• Field-induced spin polarization in lightly Cr-substituted layered antiferromagnet NiPS3
• Helimagnetism in CrBr${}_2$ and CrIBr
• Self-doped flat band and spin-triplet superconductivity in monolayer 1T-TaSe${}_{2-x}$Te${}_x$
• Defect Engineered Room-Temperature Ferromagnetism in Quasi-Two-Dimensional Nitrided CoTa2O6
• Spin interactions and topological magnonics in chromium trihalide CrClBrI
• Deterministic Switching of Perpendicular Ferromagnets by Higher harmonics of Spin-orbit Torque in Noncentrosymmetric Weyl Semimetals