Direct imaging of antiferromagnetic domains and anomalous layer-dependent mirror symmetry breaking in atomically thin MnPS${}_3$

Abstract

We have developed a sensitive cryogenic second-harmonic generation microscopy to study a van der Waals antiferromagnet MnPS${}_3$. We find that long-range Néel antiferromagnetic order develops from the bulk crystal down to the bilayer, while it is absent in the monolayer. Before entering the long-range antiferromagnetic ordered phase in all samples, an upturn of the second harmonic generation below 200 K indicates the formation of the short-range order and magneto-elastic coupling. We also directly image the two antiphase (180${}^{\circ }$) antiferromagnetic domains and thermally-induced domain switching down to bilayer. An anomalous mirror symmetry breaking shows up in samples thinner than ten layers for the temperature both above and below the Néel temperature, which indicates a structural change in few-layer samples. Minimal change of the second harmonic generation polar patterns in strain tuning experiments indicate that the symmetry crossover at ten layers is most likely an intrinsic property of MnPS${}_3$ instead of an extrinsic origin of substrate-induced strain. Our results show that second harmonic generation microscopy is a direct tool for studying antiferromagnetic domains in atomically thin materials, and opens a new way to study two-dimensional antiferromagnets.

arXiv commentTo appear in Phys. Rev. Lett

References in corpus (30)

• 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${}_2$
• Magnetic 2D materials and heterostructures
• Electrical Control of 2D Magnetism in Bilayer CrI3
• Giant Tunneling Magnetoresistance in Spin-Filter van der Waals Heterostructures
• Ising-Type Magnetic Ordering in Atomically Thin FePS3
• Probing magnetism in 2D van der Waals crystalline insulators via electron tunneling
• Direct observation of van der Waals stacking dependent interlayer magnetism
• Probing magnetism in 2D materials at the nanoscale with single spin microscopy
• Giant and nonreciprocal second harmonic generation from layered antiferromagnetism in bilayer CrI3
• Giant anisotropic nonlinear optical response in transition metal monopnictide Weyl semimetals
• Suppression of magnetic ordering in XXZ-type antiferromagnetic monolayer NiPS3
• Optical imaging of strain in two-dimensional crystals
• Charge-spin correlation in van der Waals antiferromagenet NiPS3
• Spin-flop transition in atomically thin MnPS${}_3$ crystals
• Magnon transport in quasi-two-dimensional van der Waals antiferromagnets
• Imaging the Néel vector switching in the monolayer antiferromagnet MnPSe${}_3$ with strain-controlled Ising order
• Antiferromagnetic ordering in van der Waals two-dimensional magnetic material MnPS3 probed by Raman spectroscopy
• Highly Anisotropic Excitons and Multiple Phonon Bound States in a Van der Waals Antiferromagnetic Insulator
• Magnetoelectric MnPS3 thiophosphate as a new candidate for ferrotoroidicity
• Spin-Induced Linear Polarization of Excitonic Emission in Antiferromagnetic van der Waals Crystals
• Linear magneto-electric phase in ultrathin MnPS${}_3$ probed by optical second harmonic generation
• Controlling the anisotropy of a van der Waals antiferromagnet with light
• Magnetic and electronic phase transitions probed by nanomechanical resonance
• Quasi-Two-Dimensional Magnon Identification in Antiferromagnetic FePS3 via Magneto-Raman Spectroscopy
• Tunneling transport of mono- and few-layers magnetic van der Waals MnPS${}_3$
• Magnetoelastic interaction in the two-dimensional magnetic material MnPS${}_3$ studied by first principles calculations and Raman experiments
• A Microscopic Model of Non-Reciprocal Optical Effects in Cr_2 O_3
• Dimensional crossover in a layered ferromagnet detected by spin correlation driven distortions

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• Magnetic Anisotropy in Two-dimensional van der Waals Magnetic Materials and Their Heterostructures: Importance, Mechanisms, and Opportunities
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• Observation of three-state nematicity and domain evolution in atomically-thin antiferromagnetic NiPS3
• Observation of terahertz second harmonic generation from Dirac surface states in the topological insulator Bi${}_2$Se${}_3$
• Exciton-magnon splitting in van der Waals antiferromagnet MnPS${}_3$ unveiled by second-harmonic generation
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• Electric-field-enhanced second-harmonic domain contrast and nonreciprocity in a van der Waals antiferromagnet
• Nonreciprocal magnons in layered antiferromagnets VPX3(X =S,Se,Te)
• Two-Dimensional Magnetic Materials from Ferromagnetism to Altermagnetism: Fabrication, Symmetry, Evidence, and Device Readiness