Magnetic field-induced quantum phase transitions in a van der Waals magnet

Abstract

Exploring new parameter regimes to realize and control novel phases of matter has been a main theme in modern condensed matter physics research. The recent discovery of 2D magnetism in nearly freestanding monolayer atomic crystals has already led to observations of a number of novel magnetic phenomena absent in bulk counterparts. Such intricate interplays between magnetism and crystalline structures provide ample opportunities for exploring quantum phase transitions in this new 2D parameter regime. Here, using magnetic field and temperature dependent circularly polarized Raman spectroscopy of phonons and magnons, we map out the phase diagram of CrI3 that has been known to be a layered AFM in its 2D films and a FM in its 3D bulk. We, however, reveal a novel mixed state of layered AFM and FM in 3D CrI3 bulk crystals where the layered AFM survives in the surface layers and the FM appears in deeper bulk layers. We then show that the surface layered AFM transits into the FM at a critical magnetic field of 2 T, similar to what was found in the few layer case. Interestingly, concurrent with this magnetic phase transition, we discover a first-order structural phase transition that alters the crystallographic point group from C3i to C2h and thus, from a symmetry perspective, this monoclinic structural phase belongs to the 3D nematic order universality class. Our result not only unveils the complex single magnon behavior in 3D CrI3, but also settles down the puzzle of how CrI3 transits from a bulk FM to a thin layered AFM semiconductor, despite recent efforts in understanding the origin of layered AFM in CrI3 thin layer, and reveals the intimate relationship between the layered AFM-to-FM and the crystalline rhombohedral-to-monoclinic phase transitions. These findings further open up opportunities for future 2D magnet-based magneto-mechanical devices.

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• Magnetic Dipole Interactions in Crystals
• Lattice dynamics and phase transition in CrI${}_3$ single crystals
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Cited by in corpus (28)

• Direct observation of 2D magnons in atomically thin CrI${}_3$
• Twist engineering of the two-dimensional magnetism in double bilayer chromium triiodide homostructures
• Magnon-phonon hybridization in quasi-2D antiferromagnet MnPSe${}_3$
• Interaction-stabilized topological magnon insulator in ferromagnets
• Distinct magneto-Raman signatures of spin-flip phase transitions in CrI3
• Magnetic field effect on topological spin excitations in CrI${}_3$
• Evidence of Noncollinear Spin Texture in Magnetic Moiré Superlattices
• Observation of the polaronic character of excitons in a two-dimensional semiconducting magnet $\mathrm{Cr}{\mathrm{I}}_3$
• Opportunities in Electrically Tunable 2D Materials Beyond Graphene: Recent Progress and Future Outlook
• Spin Dynamics in van der Waals Magnetic Systems
• Quantum rescaling, domain metastability and hybrid domain-walls in two-dimensional CrI3 magnets
• Coherent Helicity-Dependent Spin-Phonon Oscillations in the Ferromagnetic van der Waals Crystal CrI3
• Progress and Prospects in Two-Dimensional Magnetism of van der Waals Materials
• Tunable layered-magnetism-assisted magneto-Raman effect in a two-dimensional magnet $\mathrm{Cr}{\mathrm{I}}_3$
• Structural Monoclinicity and Its Coupling to Layered Magnetism in Few-Layer $\mathrm{Cr}{\mathrm{I}}_3$
• Light-induced topological magnons in two-dimensional van der Waals magnets
• Whirling interlayer fields as a source of stable topological order in moiré CrI3
• Magnetism and stability of all primitive stacking patterns in bilayer chromium trihalides
• Uniaxial pressure effects in the two-dimensional van-der-Waals ferromagnet CrI${}_3$
• 2D correlations in the van der Waals ferromagnet CrBr${}_3$ using high frequency electron spin resonance spectroscopy
• Resonant Raman Scattering of Few Layers CrBr${}_3$
• Superexchange and spin-orbit coupling in monolayer and bilayer chromium trihalides
• Antiferromagnetic-ferromagnetic homostructures with Dirac magnons in van der Waals magnet CrI${}_3$
• Observation of intrinsic crystal phase in bare CrI3 ferromagnetism
• Large cross-polarized Raman signal in CrI${}_3$: A first-principles study
• Spontaneously formed phonon frequency combs in van der Waals solid CrXTe${}_3$ (X=Ge,Si)
• Magnetic Field Induced Quantum Metric Dipole in Dirac Semimetal Cd3As2
• Raman spectroscopy of van der Waals topological magnet GdGaI