Jahn-Teller distortion and spin-phonon coupling in the lacunar spinel <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mi>GaM</mml:mi> <mml:msub> <mml:mi mathvariant="normal">o</mml:mi> <mml:mn>4</mml:mn> </mml:msub> <mml:msu

Lacunar spinels $\mathrm{A}{\mathrm{M}}_{4}{\mathrm{X}}_{8}$ ($\mathrm{A}=\mathrm{Ga}$, Ge, Al; $\mathrm{M}=\mathrm{V}$, Mo, Nb, Ta; $\mathrm{X}=\mathrm{S}$, Se) have garnered significant attention due to their remarkable properties, including multiferroicity, Mott-Hubbard gaps, and skyrmion phases. In this study, we present temperature-dependent Raman spectroscopy measurements of $\mathrm{GaM}{\mathrm{o}}_{4}{\mathrm{S}}_{8}$, spanning the Jahn-Teller (JT) distortion and spin ordering transitions. Using group theory analysis and first-principles calculations, we identified and assigned ten Raman-active modes, among which the two lowest-energy modes, ${A}_{1}^{1}\phantom{\rule{4pt}{0ex}}({T}_{2}^{1})$ and ${A}_{1}^{2}\phantom{\rule{4pt}{0ex}}({T}_{2}^{2})$, were confirmed as JT active modes. The ${A}_{1}^{2}\phantom{\rule{4pt}{0ex}}({T}_{2}^{2})$ mode exhibits a redshift as the temperature approaches 50 K from both sides, indicative of a soft mode and suggesting a displacive nature for the ferroelectric transition. Additionally, anomalies observed in the ${A}_{1}$ and $E$ modes near 50 K and 25 K correlate with the JT transition and subsequent magnetic ordering, pointing to significant electron-phonon and spin-phonon coupling in $\mathrm{GaM}{\mathrm{o}}_{4}{\mathrm{S}}_{8}$. These findings deepen our understanding of the mechanisms of the phase transition and the orbital-spin-lattice interactions in $\mathrm{GaM}{\mathrm{o}}_{4}{\mathrm{S}}_{8}$, while highlighting the crucial role of phonon dynamics in the $\mathrm{A}{\mathrm{M}}_{4}{\mathrm{X}}_{8}$ family.

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Publication Details

Journal
Physical review. B./Physical review. B
Published
2025-11-12
DOI
https://doi.org/10.1103/52zx-jhvr
Primary Topic
Multiferroics and related materials
Type
article
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Jahn-Teller distortion and spin-phonon coupling in the lacunar spinel <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mi>GaM</mml:mi> <mml:msub> <mml:mi mathvariant="normal">o</mml:mi> <mml:mn>4</mml:mn> </mml:msub> <mml:msu

Yonghui Zhou, Zhaorong Yang, Min Zhang, Jian Zhou et al.
Physical review. B./Physical review. B
Multiferroics and related materials
article

Jahn-Teller distortion and spin-phonon coupling in the lacunar spinel <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mi>GaM</mml:mi> <mml:msub> <mml:mi mathvariant="normal">o</mml:mi> <mml:mn>4</mml:mn> </mml:msub> <mml:msu

Yonghui Zhou, Zhaorong Yang, Min Zhang, Jian Zhou, Ruijing Liang, Yichi Li, Ying Zhou, Chao An, Shuyang Wang, Xia Fan
article en

Abstract

Lacunar spinels $\mathrm{A}{\mathrm{M}}_{4}{\mathrm{X}}_{8}$ ($\mathrm{A}=\mathrm{Ga}$, Ge, Al; $\mathrm{M}=\mathrm{V}$, Mo, Nb, Ta; $\mathrm{X}=\mathrm{S}$, Se) have garnered significant attention due to their remarkable properties, including multiferroicity, Mott-Hubbard gaps, and skyrmion phases. In this study, we present temperature-dependent Raman spectroscopy measurements of $\mathrm{GaM}{\mathrm{o}}_{4}{\mathrm{S}}_{8}$, spanning the Jahn-Teller (JT) distortion and spin ordering transitions. Using group theory analysis and first-principles calculations, we identified and assigned ten Raman-active modes, among which the two lowest-energy modes, ${A}_{1}^{1}\phantom{\rule{4pt}{0ex}}({T}_{2}^{1})$ and ${A}_{1}^{2}\phantom{\rule{4pt}{0ex}}({T}_{2}^{2})$, were confirmed as JT active modes. The ${A}_{1}^{2}\phantom{\rule{4pt}{0ex}}({T}_{2}^{2})$ mode exhibits a redshift as the temperature approaches 50 K from both sides, indicative of a soft mode and suggesting a displacive nature for the ferroelectric transition. Additionally, anomalies observed in the ${A}_{1}$ and $E$ modes near 50 K and 25 K correlate with the JT transition and subsequent magnetic ordering, pointing to significant electron-phonon and spin-phonon coupling in $\mathrm{GaM}{\mathrm{o}}_{4}{\mathrm{S}}_{8}$. These findings deepen our understanding of the mechanisms of the phase transition and the orbital-spin-lattice interactions in $\mathrm{GaM}{\mathrm{o}}_{4}{\mathrm{S}}_{8}$, while highlighting the crucial role of phonon dynamics in the $\mathrm{A}{\mathrm{M}}_{4}{\mathrm{X}}_{8}$ family.

Physical review. B./Physical review. BVol. 112(22)
Anhui University (CN), Chinese Academy of Sciences (CN), Hefei Institutes of Physical Science (CN), High Magnetic Field Laboratory (CN), Collaborative Innovation Center of Advanced Microstructures (CN), Nanjing University (CN)
Openalex Percentile: Top 72%
Multiferroics and related materials
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