Super-resolved time–frequency measurements of coupled phonon dynamics in a 2D quantum material

Gentry, Christian; Liao, Chen-Ting; You, Wenjing; Ryan, Sinéad A.; Varner, Baldwin Akin; Shi, Xun; Guan, Meng-Xue; Gray, Thomas; Temple, Doyle; Meng, Sheng; Raschke, Markus; Rossnagel, Kai; Kapteyn, Henry C.; Murnane, Margaret M.; Cating-Subramanian, Emma

doi:10.1038/s41598-022-22055-w

Title: Super-resolved time–frequency measurements of coupled phonon dynamics in a 2D quantum material

Journal Article · 16 November 2022 · Scientific Reports

DOI: https://doi.org/10.1038/s41598-022-22055-w · OSTI ID:1898684

Gentry, Christian; Liao, Chen-Ting; You, Wenjing; Ryan, Sinéad A.; Varner, Baldwin Akin; Shi, Xun; Guan, Meng-Xue; Gray, Thomas; Temple, Doyle; Meng, Sheng; Raschke, Markus; Rossnagel, Kai; Kapteyn, Henry C.; Murnane, Margaret M.; Cating-Subramanian, Emma

Abstract Methods to probe and understand the dynamic response of materials following impulsive excitation are important for many fields, from materials and energy sciences to chemical and neuroscience. To design more efficient nano, energy, and quantum devices, new methods are needed to uncover the dominant excitations and reaction pathways. In this work, we implement a newly-developed superlet transform—a super-resolution time-frequency analytical method—to analyze and extract phonon dynamics in a laser-excited two-dimensional (2D) quantum material. This quasi-2D system, 1 T -TaSe ₂ , supports both equilibrium and metastable light-induced charge density wave (CDW) phases mediated by strongly coupled phonons. We compare the effectiveness of the superlet transform to standard time-frequency techniques. We find that the superlet transform is superior in both time and frequency resolution, and use it to observe and validate novel physics. In particular, we show fluence-dependent changes in the coupled dynamics of three phonon modes that are similar in frequency, including the CDW amplitude mode, that clearly demonstrate a change in the dominant charge-phonon couplings. More interestingly, the frequencies of the three phonon modes, including the strongly-coupled CDW amplitude mode, remain time- and fluence-independent, which is unusual compared to previously investigated materials. Our study opens a new avenue for capturing the coherent evolution and couplings of strongly-coupled materials and quantum systems.

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Research Organization:: Univ. of Colorado, Boulder, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: FG02-99ER14982

OSTI ID:: 1898684

Journal Information:: Scientific Reports, Journal Name: Scientific Reports Journal Issue: 1 Vol. 12; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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