Mesoscale interplay between phonons and crystal electric field excitations in quantum spin liquid candidate CsYbSe2. Issue 11 (2nd March 2022)

• Record Type: Journal Article
• Authors: Pai, Yun-Yi; Marvinney, Claire E.; Liang, Liangbo; Xing, Jie; Scheie, Allen; Puretzky, Alexander A.; Halász, Gábor B.; Li, Xun; Juneja, Rinkle; Sefat, Athena S.; Parker, David; Lindsay, Lucas; Lawrie, Benjamin J.
• Is Part Of: Journal of materials chemistry. Volume 10:Issue 11(2022)
• Page Start: 4148
• Page End: 4156
• Publication Date: 2022-03-02
• Subjects: Materials -- Periodicals; Chemistry, Analytic -- Periodicals; Optical materials -- Research -- Periodicals; Electronics -- Materials -- Research -- Periodicals; 543.0284
• DOI: 10.1039/d1tc05934c
• Languages: English
• ISSNs: 2050-7526

Abstract

Abstract : In quantum spin liquid candidate CsYbSe2, phonon coupling to a crystal electric field mode results in a vibronic bound state, and complex, mesoscale interplay between phonon modes and CEF modes is observed. 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.