Spin-Induced Linear Polarization of Excitonic Emission in Antiferromagnetic van der Waals Crystals

Abstract

Antiferromagnets display enormous potential in spintronics owing to its intrinsic nature, including terahertz resonance, multilevel states, and absence of stray fields. Combining with the layered nature, van der Waals (vdW) antiferromagnets hold the promise in providing new insights and new designs in two-dimensional (2D) spintronics. The zero net magnetic moments of vdW antiferromagnets strengthens the spin stability, however, impedes the correlation between spin and other excitation elements, like excitons. Such coupling is urgently anticipated for fundamental magneto-optical studies and potential opto-spintronic devices. Here, we report an ultra-sharp excitonic emission with excellent monochromaticity in antiferromagnetic nickel phosphorus trisulfides (NiPS3) from bulk to atomically thin flakes. We prove that the linear polarization of the excitonic luminescence is perpendicular to the ordered spin orientation in NiPS3. By applying an in-plane magnetic field to alter the spin orientation, we further manipulate the excitonic emission polarization. Such strong correlation between exciton and spins provides new insights for the study of magneto-optics in 2D materials, and hence opens a path for developing opto-spintronic devices and antiferromagnet-based quantum information technologies.

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• Magnetically brightened dark electron-phonon bound states in a van der Waals antiferromagnet
• Direct imaging of antiferromagnetic domains and anomalous layer-dependent mirror symmetry breaking in atomically thin MnPS${}_3$
• Spin Photovoltaic Effect in Magnetic van der Waals Heterostructures
• Magnetically propagating Hund's exciton in van der Waals antiferromagnet NiPS3
• Progress and Prospects in Two-Dimensional Magnetism of van der Waals Materials
• Vibrational properties of CuInP2S6 across the ferroelectric transition
• Dimensionality crossover to 2D vestigial nematicity from 3D zigzag antiferromagnetism in an XY-type honeycomb van der Waals magnet
• All van der Waals three-terminal SOT-MRAM realized by topological ferromagnet Fe3GeTe2
• Observation of three-state nematicity and domain evolution in atomically-thin antiferromagnetic NiPS3
• Tunable Strong Magnetic Anisotropy in Two-Dimensional van der Waals Antiferromagnets
• Direct Observation and Analysis of Low-Energy Magnons with Raman Spectroscopy in Atomically Thin NiPS3
• Exciton-magnon splitting in van der Waals antiferromagnet MnPS${}_3$ unveiled by second-harmonic generation
• Magnetoelectric effect in van der Waals magnets
• Giant Magneto-Optical Schäfer-Hubert Effect in Two-Dimensional van der Waals Antiferromagnets \textit{M}PS${}_3$ (\textit{M}=Mn, Fe, Ni)
• Distinct Optical Excitation Mechanisms of a Coherent Magnon in a van der Waals Antiferromagnet
• Field-induced spin polarization in lightly Cr-substituted layered antiferromagnet NiPS3
• Brightened Optical Transition as Indicator of Multiferroicity in a Layered Antiferromagnet
• Long-lived population inversion in resonantly driven excitonic antiferromagnet
• Characteristic exciton energy scales in antiferromagnetic NiPS${}_3$
• Enhanced Magnetization by Defect-Assisted Exciton Recombination in Atomically Thin CrCl${}_3$
• Deconstruction of the anisotropic magnetic interactions from spin-entangled optical excitations in van der Waals antiferromagnets
• Revealing the Electronic Structure of van der Waals Antiferromagnetic NiPS${}_3$ through Synchrotron-Based $\mu$-ARPES and Alkali Metal Dosing
• Magnetic-field tuning of the spin dynamics in the quasi-2D van der Waals antiferromagnet CuCrP${}_2$S${}_6$
• Unconventional magnon transport in antiferromagnet NiPS${}_3$ induced by an anisotropic spin-flop transition
• Exciton-spin interactions in antiferromagnetic charge-transfer insulators
• Probing the band structure of the strongly correlated antiferromagnet NiPS3 across its phase transition
• Absence of magnetic order in epitaxial RuO2 revealed by X-ray linear dichroism
• Spin-flip optical excitations in van der Waals antiferromagnet CrPS${}_4$
• Spin Wave Dispersion of the van der Waals Antiferromagnet NiPS${}_3$
• Crystal field tuned spin-flip luminescence in NiPS3
• Ultrafast Dynamics of Spin-Orbit Entangled Excitons Coupled to Magnetic Ordering in van der Waals Antiferromagnet NiPS3
• Magnetic Field-Tunable Repulsive Exciton-Exciton Interaction in the van der Waals Antiferromagnet NiPS${}_3$
• Crucial role of magnetic dipole and anomalous field dependence in $\mathrm{NiP}{\mathrm{S}}_3$