Dynamic Magnetic Crossover at the Origin of the Hidden-Order in van der Waals Antiferromagnet CrSBr

Abstract

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, and magnetization measurements. We evidence that this material undergoes a transition to an A-type antiferromagnetic state below $T_{\mathrm{N}}\approx$ 140 K, with a pronounced two-dimensional character as deduced from the determined critical exponent of $\beta \approx$ 0.18. In our analysis of the field-induced metamagnetic transition, we find that the ferromagnetic correlations within the monolayers persist clearly above the Néel temperature in this material. Furthermore, we unravel the low-temperature (i.e. $T<T_{\mathrm{N}}$) magnetic hidden order within the long-range magnetically ordered state. We find that it is associated to a slowing down of the magnetic fluctuations, accompanied by a continuous reorientation of the internal magnetic field. These take place upon cooling below $T_s$ $\approx$ 100 K, until a spin freezing process occurs at $T$* $\approx$ 40 K. We argue this complex dynamic behavior to reflect a magnetic crossover driven by the in-plane uniaxial anisotropy, which is ultimately caused by the mixed-anion character of the material. Our findings indicate that the magnetic and structural properties of CrSBr widen its potential application as a component for spin-based electronic devices.

References in corpus (8)

• Magnetic 2D materials and heterostructures
• Negative Thermal Expansion Coefficient of Graphene Measured by Raman Spectroscopy
• Van der Waals heterostructures for spintronics and opto-spintronics
• Direct photoluminescence probing of ferromagnetism in monolayer two-dimensional CrBr3
• Strain-tunable magnetic and electronic properties of monolayer CrI3
• Triaxial magnetic anisotropy in the two-dimensional ferromagnetic semiconductor CrSBr
• Distinctive magnetic properties of CrI3 and CrBr3 monolayers caused by spin-orbit coupling
• Hidden, entangled and resonating order

Cited by in corpus (41)

• Magneto-optics in a van der Waals magnet tuned by self-hybridized polaritons
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• Spin waves and magnetic exchange Hamiltonian in CrSBr
• Probing defects and spin-phonon coupling in CrSBr via resonant Raman scattering
• Magnon straintronics in the 2D van der Waals ferromagnet CrSBr from first-principles
• Sensing the local magnetic environment through optically active defects in a layered magnetic semiconductor
• Strong Exciton-Phonon Coupling as a Fingerprint of Magnetic Ordering in van der Waals Layered CrSBr
• Raman scattering signatures of the strong spin-phonon coupling in the bulk magnetic van der Waals material CrSBr
• Nanoscale magnetism and magnetic phase transitions in atomically thin CrSBr
• Paramagnetic Electronic Structure of CrSBr: Comparison between Ab Initio GW Theory and Angle-Resolved Photoemission Spectroscopy
• Magnetic imaging and domain nucleation in CrSBr down to the 2D limit
• Giant exchange splitting in the electronic structure of A-type 2D antiferromagnet CrSBr
• Magneto-optical sensing of the pressure driven magnetic ground states in bulk CrSBr
• Charge transfer and asymmetric coupling of MoSe${}_2$ valleys to the magnetic order of CrSBr
• Ferromagnetic interlayer coupling in CrSBr crystals irradiated by ions
• Charge Density Wave and Ferromagnetism in Intercalated CrSBr
• Intrinsic magnetic properties of the layered antiferromagnet CrSBr
• Programmable Magnetic Hysteresis in Orthogonally-Twisted Two-Dimensional CrSBr Magnets via Stacking Engineering
• Spin-mechanical coupling in 2D antiferromagnet CrSBr
• Evaluating SCAN and r${}^2$SCAN meta-GGA functionals for predicting transition temperatures in antiferromagnetic materials
• Synthesis and Anisotropic Magnetic Properties of LiCrTe${}_2$ Single Crystals with a Triangular-Lattice Antiferromagnetic Structure
• Interplay of energy and charge transfer in WSe2/CrSBr heterostructures
• Engineering of a Layered Ferromagnet via Graphitization: An Overlooked Polymorph of GdAlSi
• Efficient Soft-Chemical Synthesis of Large van-der-Waals Crystals of the Room-Temperature Ferromagnet 1T-CrTe2
• Surface-Dominated Quantum Metric-Induced Nonlinear Transport in the Layered Antiferromagnet CrSBr
• Resonance Raman Scattering and Anomalous Anti-Stokes Phenomena in CrSBr
• Probing Short-Range Correlations in the van der Waals Magnet CrSBr by Small-Angle Neutron Scattering
• Magnetically Modulated Electrical Switching in an Antiferromagnetic Transistor
• Controlling the Magnetic Properties of the van der Waals Multiferroic Crystals Co${}_{1-x}$Ni${}_x$I${}_2$
• Magnon sensing of NO, NO${}_2$ and NH${}_3$ gas capture on CrSBr monolayer
• Van der Waals CrSBr alloys with tunable magnetic and optical properties
• Resonant X-ray spectroscopies on Chromium $3\text{d}$ orbitals in CrSBr
• Theory of interaction-induced charge order in CrSBr
• Light-induced ultrafast magnetization dynamics in van der Waals antiferromagnetic CrSBr
• Magneto-Excitonic Duality From Monolayer to Trilayer CrSBr
• Growth of Large Crystals of Janus Phase RhSeCl Using Self-Selecting Vapour Growth
• Magnetism of kagome metals $\left({\text{Fe}}_{1-x}{\text{Co}}_x\right)\text{Sn}$ studied by $\mu$SR
• Excitonic optical absorption in strained monolayer CrSBr
• Crystallographic Orientation-Dependent Magnetotransport in the Layered Antiferromagnet -- CrSBr
• Creation of Depth-Confined, Shallow Nitrogen-Vacancy Centers in Diamond With Tunable Density