Coherent detection of hidden spin–lattice coupling in a van der Waals antiferromagnet

Emre Ergeçen; Batyr Ilyas; Junghyun Kim; Jaena Park; Mehmet Burak Yilmaz; Tianchuang Luo; Di Xiao; Satoshi Okamoto; Je Geun Park; Nuh Gedik

doi:10.1073/pnas.2208968120

Coherent detection of hidden spin–lattice coupling in a van der Waals antiferromagnet

Emre Ergeçen, Batyr Ilyas, Junghyun Kim, Jaena Park, Mehmet Burak Yilmaz, Tianchuang Luo, Di Xiao, Satoshi Okamoto, Je Geun Park, Nuh Gedik

Materials Theory

Research output: Contribution to journal › Article › peer-review

4 Scopus citations

Abstract

Strong interactions between different degrees of freedom lead to exotic phases of matter with complex order parameters and emergent collective excitations. Conventional techniques, such as scattering and transport, probe the amplitudes of these excitations, but they are typically insensitive to phase. Therefore, novel methods with phase sensitivity are required to understand ground states with phase modulations and interactions that couple to the phase of collective modes. Here, by performing phase-resolved coherent phonon spectroscopy (CPS), we reveal a hidden spin–lattice coupling in a vdW antiferromagnet FePS₃ that eluded other phase-insensitive conventional probes, such as Raman and X-ray scattering. With comparative analysis and analytical calculations, we directly show that the magnetic order in FePS₃ selectively couples to the trigonal distortions through partially filled t_2g orbitals. This magnetoelastic coupling is linear in magnetic order and lattice parameters, rendering these distortions inaccessible to inelastic scattering techniques. Our results not only capture the elusive spin–lattice coupling in FePS₃ but also establish phase-resolved CPS as a tool to investigate hidden interactions.

Original language	English
Article number	e2208968120
Journal	Proceedings of the National Academy of Sciences of the United States of America
Volume	120
Issue number	12
DOIs	https://doi.org/10.1073/pnas.2208968120
State	Published - Mar 21 2023

Funding

ACKNOWLEDGMENTS. We thank Riccardo Comin for fruitful discussions. We acknowledge the support from the US Department of Energy, Materials Science and Engineering Division, Office of Basic Energy Sciences (BES DMSE) (data taking and analysis), and Gordon and Betty Moore Foundation’s EPiQS Initiative grant GBMF9459 (instrumentation and manuscript writing). Work at the Center for Quantum Materials was supported by the Leading Researcher Program of the National Research Foundation of Korea (Grant No. 2020R1A3B2079375). The research of S.O. was supported by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division.

Funders	Funder number
BES DMSE
U.S. Department of Energy
Gordon and Betty Moore Foundation	GBMF9459
Office of Science
Basic Energy Sciences
Division of Materials Sciences and Engineering
National Research Foundation of Korea	2020R1A3B2079375

Keywords

spin-phonon coupling
ultrafast spectroscopy
van der Waals magnets

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abstract = "Strong interactions between different degrees of freedom lead to exotic phases of matter with complex order parameters and emergent collective excitations. Conventional techniques, such as scattering and transport, probe the amplitudes of these excitations, but they are typically insensitive to phase. Therefore, novel methods with phase sensitivity are required to understand ground states with phase modulations and interactions that couple to the phase of collective modes. Here, by performing phase-resolved coherent phonon spectroscopy (CPS), we reveal a hidden spin–lattice coupling in a vdW antiferromagnet FePS3 that eluded other phase-insensitive conventional probes, such as Raman and X-ray scattering. With comparative analysis and analytical calculations, we directly show that the magnetic order in FePS3 selectively couples to the trigonal distortions through partially filled t2g orbitals. This magnetoelastic coupling is linear in magnetic order and lattice parameters, rendering these distortions inaccessible to inelastic scattering techniques. Our results not only capture the elusive spin–lattice coupling in FePS3 but also establish phase-resolved CPS as a tool to investigate hidden interactions.",

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AU - Ilyas, Batyr

AU - Kim, Junghyun

AU - Park, Jaena

AU - Yilmaz, Mehmet Burak

AU - Luo, Tianchuang

AU - Xiao, Di

AU - Okamoto, Satoshi

AU - Park, Je Geun

AU - Gedik, Nuh

PY - 2023/3/21

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N2 - Strong interactions between different degrees of freedom lead to exotic phases of matter with complex order parameters and emergent collective excitations. Conventional techniques, such as scattering and transport, probe the amplitudes of these excitations, but they are typically insensitive to phase. Therefore, novel methods with phase sensitivity are required to understand ground states with phase modulations and interactions that couple to the phase of collective modes. Here, by performing phase-resolved coherent phonon spectroscopy (CPS), we reveal a hidden spin–lattice coupling in a vdW antiferromagnet FePS3 that eluded other phase-insensitive conventional probes, such as Raman and X-ray scattering. With comparative analysis and analytical calculations, we directly show that the magnetic order in FePS3 selectively couples to the trigonal distortions through partially filled t2g orbitals. This magnetoelastic coupling is linear in magnetic order and lattice parameters, rendering these distortions inaccessible to inelastic scattering techniques. Our results not only capture the elusive spin–lattice coupling in FePS3 but also establish phase-resolved CPS as a tool to investigate hidden interactions.

AB - Strong interactions between different degrees of freedom lead to exotic phases of matter with complex order parameters and emergent collective excitations. Conventional techniques, such as scattering and transport, probe the amplitudes of these excitations, but they are typically insensitive to phase. Therefore, novel methods with phase sensitivity are required to understand ground states with phase modulations and interactions that couple to the phase of collective modes. Here, by performing phase-resolved coherent phonon spectroscopy (CPS), we reveal a hidden spin–lattice coupling in a vdW antiferromagnet FePS3 that eluded other phase-insensitive conventional probes, such as Raman and X-ray scattering. With comparative analysis and analytical calculations, we directly show that the magnetic order in FePS3 selectively couples to the trigonal distortions through partially filled t2g orbitals. This magnetoelastic coupling is linear in magnetic order and lattice parameters, rendering these distortions inaccessible to inelastic scattering techniques. Our results not only capture the elusive spin–lattice coupling in FePS3 but also establish phase-resolved CPS as a tool to investigate hidden interactions.

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Coherent detection of hidden spin–lattice coupling in a van der Waals antiferromagnet

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