Issue 11, 2022

Mesoscale interplay between phonons and crystal electric field excitations in quantum spin liquid candidate CsYbSe2

Abstract

CsYbSe2, a recently identified quantum spin liquid (QSL) candidate, exhibits strong crystal electric field (CEF) excitations. Here, we identify phonon and CEF modes with Raman spectroscopy and observe strong CEF-phonon coupling resulting in a vibronic bound state. Complex, mesoscale interplay between phonon modes and CEF modes is observed in real space. Additionally, an unexpected resonant Raman excitation condition is satisfied, yielding up to third-order combination modes, with a total of 17 modes identified in the spectra. This study paves the way to coherent control of possible QSL ground states with optically accessible CEF-phonon manifolds and mesoscale engineering of CEF-phonon interactions.

Graphical abstract: Mesoscale interplay between phonons and crystal electric field excitations in quantum spin liquid candidate CsYbSe2

Supplementary files

Article information

Article type
Paper
Submitted
11 Dec 2021
Accepted
19 Feb 2022
First published
24 Feb 2022

J. Mater. Chem. C, 2022,10, 4148-4156

Mesoscale interplay between phonons and crystal electric field excitations in quantum spin liquid candidate CsYbSe2

Y. Pai, C. E. Marvinney, L. Liang, J. Xing, A. Scheie, A. A. Puretzky, G. B. Halász, X. Li, R. Juneja, A. S. Sefat, D. Parker, L. Lindsay and B. J. Lawrie, J. Mater. Chem. C, 2022, 10, 4148 DOI: 10.1039/D1TC05934C

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