A Three-Stage Magnetic Phase Transition Revealed in Ultrahigh-Quality van der Waals Bulk Magnet CrSBr

Abstract

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. The high crystalline quality of vdW magnets is the key to maintaining intrinsic magnetic and electronic properties, especially when exfoliated down to the two-dimensional limit. Here, ultrahigh-quality air-stable vdW CrSBr crystals are synthesized using the direct solid–vapor synthesis method. The high single crystallinity and spatial homogeneity have been thoroughly evidenced at length scales from submm to atomic resolution by X-ray diffraction, second harmonic generation, and scanning transmission electron microscopy. More importantly, specific heat measurements of ultrahigh-quality CrSBr crystals show three thermodynamic anomalies at 185, 156, and 132 K, revealing a stage-by-stage development of the magnetic order upon cooling, which is also corroborated with the magnetization and transport results. Our ultrahigh-quality CrSBr can further be exfoliated down to monolayers and bilayers easily, providing the building blocks of heterostructures for spintronic and magneto-optoelectronic applications.

Origin and regulation of triaxial magnetic anisotropy in the ferromagnetic semiconductor CrSBr monolayer

“…Motivated by these burgeoning developments, we focus on the recently observed 2D air-stable FMS CrSBr monolayer. 25,43 First, using the first-principles calculations, the triaxial magnetic MA of bulk CrSBr, which was confirmed experimentally, was well reproduced. 36,45,49 Interestingly, the CrSBr monolayer also exhibits triaxial MA, which originates from the coexistence of spin–orbit coupling and dipole–dipole interactions.…”

“…Recently, a promising 2D van der Waals semiconducting magnet, CrSBr, is of great interest owing to its exotic properties. 12,25,[36][37][38][39][40][41][42][43][44][45][46][47][48][49][50] Bulk CrSBr is a layered A-type antiferromagnetic semiconductor with the Néel temperature T N ≈ 140 K, and it exhibits triaxial magnetic anisotropy (intermediate magnetization x axis, easy magnetization y axis, and hard magnetization z axis) with a band gap of about 1.5 eV. 25,44,49 More importantly, CrSBr exhibits air stability and gate-tunable conductivity, which reinforces its potential application as a spintronic device.…”

Correlation-Driven Topological Transition in Janus Two-Dimensional Vanadates

“…Since the observation of intrinsic ferromagnetism in two-dimensional layered materials (2D) such as CrGeTe 3 [ 1 ] and CrI 3 [ 2 ], the fields of magnetism and spintronics have received tremendous research attention in the 2D limit [ 3 , 4 , 5 , 6 , 7 , 8 , 9 , 10 , 11 , 12 , 13 , 14 ]. The atomically thin 2D magnetic materials are considered ideal systems, where the magnetic and spin-related features can effectively be controlled and modulated via proximity effects, electric field, magnetic field, strain, defects and optical doping [ 15 , 16 , 17 , 18 , 19 , 20 , 21 , 22 ].…”

Significantly anisotropic Raman response of the (110) surface in quasi-one-dimensional system (TaSe4)2I by polarized Raman spectroscopy

“…Low-dimensional systems exhibit a rich phenomenology due to strong electron-phonon interaction or electron-electron scattering; among them, the charge density wave (CDW) state is one of the most fundamental orderings and has been discovered in various low dimensional materials. [1][2][3][4][5][6][7][8][9] It is reported that quasi-onedimensional and quasi-two-dimensional features in the unusual layered ZrTe 3 structure are respectively conducive to the formation of a charge density wave at 63 K and superconductivity up to 4 K, which suggests a new induction route of the superconductivity in layered compounds with competitive orderings. 10 In layered compound TaS 2 , a commensurate CDW phase has been treated as a quasi-two-dimensional phenomenon, however, band structure calculations and angle-resolved photoemission spectroscopy (ARPES) show that perpendicular to the crystal planes, CDW coexists with a one-dimensional metallic dispersion, which implies that the notion of viewing the layered transitionmetal dichalcogenide CDW materials as quasi-two-dimensional is an oversimplification.…”