Spin-orbital excitations encoding the magnetic phase transition in the van der Waals antiferromagnet FePS$_{3}$

Fuente: arXiv
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Autores principales: Wei, Yuan, Tseng, Yi, Elnaggar, Hebatalla, Zhang, Wenliang, Asmara, Teguh Citra, Paris, Eugenio, Domaine, Gabriele, Strocov, Vladimir N., Testa, Luc, Favre, Virgile, Di Luca, Mario, Banerjee, Mitali, Wildes, Andrew R., de Groot, Frank M. F., Ronnow, Henrik M., Schmitt, Thorsten
Formato: Preprint
Publicado: 2024
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author Wei, Yuan
Tseng, Yi
Elnaggar, Hebatalla
Zhang, Wenliang
Asmara, Teguh Citra
Paris, Eugenio
Domaine, Gabriele
Strocov, Vladimir N.
Testa, Luc
Favre, Virgile
Di Luca, Mario
Banerjee, Mitali
Wildes, Andrew R.
de Groot, Frank M. F.
Ronnow, Henrik M.
Schmitt, Thorsten
author_facet Wei, Yuan
Tseng, Yi
Elnaggar, Hebatalla
Zhang, Wenliang
Asmara, Teguh Citra
Paris, Eugenio
Domaine, Gabriele
Strocov, Vladimir N.
Testa, Luc
Favre, Virgile
Di Luca, Mario
Banerjee, Mitali
Wildes, Andrew R.
de Groot, Frank M. F.
Ronnow, Henrik M.
Schmitt, Thorsten
contents In the rich phases of van der Waals (vdW) materials featuring intertwined electronic order and collective phenomena, characterizing elementary dynamics that entail the low-energy Hamiltonian and electronic degrees of freedom is of paramount importance. Here we performed resonant inelastic X-ray scattering (RIXS) to elaborate the spin-orbital ground and excited states of the vdW antiferromagnetic insulator FePS$_{3}$, as well as their relation to magnetism. We observed the spectral enhancement of spin-orbital multiplet transitions about $\sim$ 100 and $\sim$ 220 meV, as well as quasielastic response, when entering the zig-zag antiferromagnetic phase, where the spectral changes develop an order-parameter-like evolution with temperature. By comparing with ligand field theory calculations, we discovered the essential role of trigonal lattice distortion and negative metal-ligand charge-transfer to account for these emergent excitations. Such spectral profiles are further examined upon confinement by mechanical exfoliation. We reveal their spectral robustness down to the few atomic layer limit, in accordance with the persistent antiferromagnetic state previously reported in optical measurements. Our study demonstrates the versatile RIXS capability that resolves magneto-crystalline anisotropy and charge-transfer energetics. These provide the crucial insight to understand how the spontaneous magnetic symmetry-breaking stabilizes in the quasi-two-dimensional limit for the vdW magnet FePS$_{3}$.
format Preprint
id arxiv_https___arxiv_org_abs_2405_13720
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Spin-orbital excitations encoding the magnetic phase transition in the van der Waals antiferromagnet FePS$_{3}$
Wei, Yuan
Tseng, Yi
Elnaggar, Hebatalla
Zhang, Wenliang
Asmara, Teguh Citra
Paris, Eugenio
Domaine, Gabriele
Strocov, Vladimir N.
Testa, Luc
Favre, Virgile
Di Luca, Mario
Banerjee, Mitali
Wildes, Andrew R.
de Groot, Frank M. F.
Ronnow, Henrik M.
Schmitt, Thorsten
Strongly Correlated Electrons
In the rich phases of van der Waals (vdW) materials featuring intertwined electronic order and collective phenomena, characterizing elementary dynamics that entail the low-energy Hamiltonian and electronic degrees of freedom is of paramount importance. Here we performed resonant inelastic X-ray scattering (RIXS) to elaborate the spin-orbital ground and excited states of the vdW antiferromagnetic insulator FePS$_{3}$, as well as their relation to magnetism. We observed the spectral enhancement of spin-orbital multiplet transitions about $\sim$ 100 and $\sim$ 220 meV, as well as quasielastic response, when entering the zig-zag antiferromagnetic phase, where the spectral changes develop an order-parameter-like evolution with temperature. By comparing with ligand field theory calculations, we discovered the essential role of trigonal lattice distortion and negative metal-ligand charge-transfer to account for these emergent excitations. Such spectral profiles are further examined upon confinement by mechanical exfoliation. We reveal their spectral robustness down to the few atomic layer limit, in accordance with the persistent antiferromagnetic state previously reported in optical measurements. Our study demonstrates the versatile RIXS capability that resolves magneto-crystalline anisotropy and charge-transfer energetics. These provide the crucial insight to understand how the spontaneous magnetic symmetry-breaking stabilizes in the quasi-two-dimensional limit for the vdW magnet FePS$_{3}$.
title Spin-orbital excitations encoding the magnetic phase transition in the van der Waals antiferromagnet FePS$_{3}$
topic Strongly Correlated Electrons
url https://arxiv.org/abs/2405.13720