Electronic Raman scattering in the 2D antiferromagnet NiPS
            <sub>3</sub>

Wang, Xingzhi; Cao, Jun; Li, Hua; Lu, Zhengguang; Cohen, Arielle; Haldar, Anubhab; Kitadai, Hikari; Tan, Qishuo; Burch, Kenneth S.; Smirnov, Dmitry; Xu, Weigao; Sharifzadeh, Sahar; Liang, Liangbo; Ling, Xi

doi:10.1126/sciadv.abl7707

Cited by 25 publications

(17 citation statements)

References 55 publications

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“…In contrast, the 180 cm −1 Raman mode involving Ni atoms is coupled to the magnetic order and is found to rotate by 120° (Figure 2g,h), similar to the PL polar plot. Since phonon Raman intensity exhibits a fourfold symmetry, polarization‐resolved PL (or electronic Raman [ 21 ] ) is still preferred to reveal the local zigzag spin chain directions. In addition to the measurements presented in Figure 2 (indicating two different spin chain directions), the third spin chain direction allowed by the threefold symmetry is also observed on a separate flake (Figure , Supporting Information).…”

Section: Resultsmentioning

confidence: 99%

Anisotropic Excitons Reveal Local Spin Chain Directions in a van der Waals Antiferromagnet

et al. 2023

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A long‐standing pursuit in materials science is to identify suitable magnetic semiconductors for integrated information storage, processing, and transfer. Van der Waals magnets have brought forth new material candidates for this purpose. Recently, sharp exciton resonances in antiferromagnet NiPS3 have been reported to correlate with magnetic order, that is, the exciton photoluminescence intensity diminishes above the Néel temperature. Here, it is found that the polarization of maximal exciton emission rotates locally, revealing three possible spin chain directions. This discovery establishes a new understanding of the antiferromagnet order hidden in previous neutron scattering and optical experiments. Furthermore, defect‐bound states are suggested as an alternative exciton formation mechanism that has yet to be explored in NiPS3. The supporting evidence includes chemical analysis, excitation power, and thickness dependent photoluminescence and first‐principles calculations. This mechanism for exciton formation is also consistent with the presence of strong phonon side bands. This study shows that anisotropic exciton photoluminescence can be used to read out local spin chain directions in antiferromagnets and realize multi‐functional devices via spin‐photon transduction.

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Section: Resultsmentioning

confidence: 99%

Anisotropic Excitons Reveal Local Spin Chain Directions in a van der Waals Antiferromagnet

et al. 2023

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“…[17,22] The trigonal distortion introduces a D 3d symmetry which splits 3 T 2g → 3 A 1g + 3 E g (peaks B & C) and 3 T 1g → 3 A 2g + 3 E g (peaks E & F), in agreement with Raman and optical measurements. [22,23] Access 1 and in Supporting Information. [25] In (a,c), black and gray lines show energy levels calculated with and without SOC, respectively.…”

Section: Resultsmentioning

confidence: 99%

Elucidating the Role of Dimensionality on the Electronic Structure of the Van der Waals Antiferromagnet NiPS₃

DiScala,

Staros,

de la Torre

et al. 2024

Advanced Physics Research

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The sustained interest in investigating magnetism in the 2D limit of insulating antiferromagnets is driven by the possibilities of discovering, or engineering, novel magnetic phases through layer stacking. However, due to the difficulty of directly measuring magnetic interactions in 2D antiferromagnets, it is not yet understood how intralayer magnetic interactions in insulating, strongly correlated, materials can be modified through layer proximity. Herein, the impact of reduced dimensionality in the model van der Waals antiferromagnet NiPS3 is explored by measuring electronic excitations in exfoliated samples using Resonant Inelastic X‐ray Scattering (RIXS). The resulting spectra shows systematic broadening of NiS6 multiplet excitations with decreasing layer count from bulk down to three atomic layers (3L). It is shown that these trends originate from a decrease in transition metal‐ligand and ligand–ligand hopping integrals, and by charge‐transfer energy evolving from Δ = 0.83 eV in the bulk to 0.37 eV in 3L NiPS3. Relevant intralayer magnetic exchange integrals computed from the electronic parameters exhibit a decrease in the average interaction strength with thickness. This study underscores the influence of interlayer electronic interactions on intralayer ones in insulating magnets, indicating that magnetic Hamiltonians in few‐layer insulating magnets can greatly deviate from their bulk counterparts.

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“…Since 2D vdW magnets are typically produced as micrometer-scale thin flakes, macroscopic volumetric analysis tools such as superconducting quantum interference devices (SQUID) magnetometry and neutron scattering are generally not applicable. Optical spectroscopy and microscopy such as polarized micro-Raman scattering [60][61][62][63][64][65][66][67][68][69][70], magneto-optical Kerr effect (MOKE) [16,46] and magnetic circular dichroism (MCD) [47,71] have been widely used to study magnetic order parameters of 2D magnets. However, these techniques are highly sensitive to the wavelength of light and the choice of substrate since the magneto-optical response, as shown in CrI 3 and CrBr 3 , is dominated by excitonic effect [72][73][74].…”

Section: Introductionmentioning

confidence: 99%

Ferromagnetic Resonance in Two-dimensional van der Waals Magnets: A Probe for Spin Dynamics

Tang¹,

Alahmed²,

Mahdi³

et al. 2023

Preprint

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The discovery of atomic monolayer magnetic materials has stimulated intense research activities in the two-dimensional (2D) van der Waals (vdW) materials community. The field is growing rapidly and there has been a large class of 2D vdW magnetic compounds with unique properties, which provides an ideal platform to study magnetism in the atomically thin limit. In parallel, based on tunneling magnetoresistance and magneto-optical effect in 2D vdW magnets and their heterostructures, emerging concepts of spintronic and optoelectronic applications such as spin tunnel field-effect transistors and spin-filtering devices are explored. While the magnetic ground state has been extensively investigated, reliable characterization and control of spin dynamics play a crucial role in designing ultrafast spintronic devices. Ferromagnetic resonance (FMR) allows direct measurements of magnetic excitations, which provides insight into the key parameters of magnetic properties such as exchange interaction, magnetic anisotropy, gyromagnetic ratio, spin-orbit coupling, damping rate, and domain structure. In this review article, we present an overview of the essential progress in probing spin dynamics of 2D vdW magnets using FMR techniques. Given the dynamic nature of this field, we focus mainly on the broadband FMR, optical FMR, and spin-torque FMR, and their applications in studying prototypical 2D vdW magnets including CrX3 (X = Cl, Br, I), Fe5GeTe2, and Cr2Ge2Te6. We conclude with the recent advances in laboratory-and synchrotron-based FMR techniques and their opportunities to broaden the horizon of research pathways into atomically thin magnets.

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Electronic Raman scattering in the 2D antiferromagnet NiPS ₃

Abstract: Electronic Raman scattering activates the investigation of d-d excitations and electron-spin coupling in 2D antiferromagnets.

Cited by 25 publications

References 55 publications

Anisotropic Excitons Reveal Local Spin Chain Directions in a van der Waals Antiferromagnet

Anisotropic Excitons Reveal Local Spin Chain Directions in a van der Waals Antiferromagnet

Elucidating the Role of Dimensionality on the Electronic Structure of the Van der Waals Antiferromagnet NiPS₃

Ferromagnetic Resonance in Two-dimensional van der Waals Magnets: A Probe for Spin Dynamics

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Electronic Raman scattering in the 2D antiferromagnet NiPS 3

Abstract: Electronic Raman scattering activates the investigation of d-d excitations and electron-spin coupling in 2D antiferromagnets.

Cited by 25 publications

References 55 publications

Anisotropic Excitons Reveal Local Spin Chain Directions in a van der Waals Antiferromagnet

Anisotropic Excitons Reveal Local Spin Chain Directions in a van der Waals Antiferromagnet

Elucidating the Role of Dimensionality on the Electronic Structure of the Van der Waals Antiferromagnet NiPS3

Ferromagnetic Resonance in Two-dimensional van der Waals Magnets: A Probe for Spin Dynamics

Contact Info

Product

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Electronic Raman scattering in the 2D antiferromagnet NiPS ₃

Elucidating the Role of Dimensionality on the Electronic Structure of the Van der Waals Antiferromagnet NiPS₃