Super-resolved time–frequency measurements of coupled phonon dynamics in a 2D quantum material
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...
| Main Authors: | , , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2022-11-01
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| Series: | Scientific Reports |
| Online Access: | https://doi.org/10.1038/s41598-022-22055-w |
| _version_ | 1797784704248709120 |
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| author | Christian Gentry Chen-Ting Liao Wenjing You Sinéad A. Ryan Baldwin Akin Varner Xun Shi Meng-Xue Guan Thomas Gray Doyle Temple Sheng Meng Markus Raschke Kai Rossnagel Henry C. Kapteyn Margaret M. Murnane Emma Cating-Subramanian |
| author_facet | Christian Gentry Chen-Ting Liao Wenjing You Sinéad A. Ryan Baldwin Akin Varner Xun Shi Meng-Xue Guan Thomas Gray Doyle Temple Sheng Meng Markus Raschke Kai Rossnagel Henry C. Kapteyn Margaret M. Murnane Emma Cating-Subramanian |
| author_sort | Christian Gentry |
| collection | DOAJ |
| description | 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, 1T-TaSe2, 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. |
| first_indexed | 2024-03-13T00:43:41Z |
| format | Article |
| id | doaj.art-834a6b1951fc4d9b827ba4431bcfc603 |
| institution | Directory Open Access Journal |
| issn | 2045-2322 |
| language | English |
| last_indexed | 2024-03-13T00:43:41Z |
| publishDate | 2022-11-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Scientific Reports |
| spelling | doaj.art-834a6b1951fc4d9b827ba4431bcfc6032023-07-09T11:10:14ZengNature PortfolioScientific Reports2045-23222022-11-011211810.1038/s41598-022-22055-wSuper-resolved time–frequency measurements of coupled phonon dynamics in a 2D quantum materialChristian Gentry0Chen-Ting Liao1Wenjing You2Sinéad A. Ryan3Baldwin Akin Varner4Xun Shi5Meng-Xue Guan6Thomas Gray7Doyle Temple8Sheng Meng9Markus Raschke10Kai Rossnagel11Henry C. Kapteyn12Margaret M. Murnane13Emma Cating-Subramanian14JILA, University of Colorado and NISTJILA, University of Colorado and NISTJILA, University of Colorado and NISTJILA, University of Colorado and NISTSTROBE Science and Technology CenterJILA, University of Colorado and NISTInstitute of Physics, Chinese Academy of SciencesJILA, University of Colorado and NISTDepartment of Physics, Norfolk State UniversityInstitute of Physics, Chinese Academy of SciencesJILA, University of Colorado and NISTInstitute of Experimental and Applied Physics and KiNSIS, Kiel UniversityJILA, University of Colorado and NISTJILA, University of Colorado and NISTJILA, University of Colorado and NISTAbstract 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, 1T-TaSe2, 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.https://doi.org/10.1038/s41598-022-22055-w |
| spellingShingle | Christian Gentry Chen-Ting Liao Wenjing You Sinéad A. Ryan Baldwin Akin Varner Xun Shi Meng-Xue Guan Thomas Gray Doyle Temple Sheng Meng Markus Raschke Kai Rossnagel Henry C. Kapteyn Margaret M. Murnane Emma Cating-Subramanian Super-resolved time–frequency measurements of coupled phonon dynamics in a 2D quantum material Scientific Reports |
| title | Super-resolved time–frequency measurements of coupled phonon dynamics in a 2D quantum material |
| title_full | Super-resolved time–frequency measurements of coupled phonon dynamics in a 2D quantum material |
| title_fullStr | Super-resolved time–frequency measurements of coupled phonon dynamics in a 2D quantum material |
| title_full_unstemmed | Super-resolved time–frequency measurements of coupled phonon dynamics in a 2D quantum material |
| title_short | Super-resolved time–frequency measurements of coupled phonon dynamics in a 2D quantum material |
| title_sort | super resolved time frequency measurements of coupled phonon dynamics in a 2d quantum material |
| url | https://doi.org/10.1038/s41598-022-22055-w |
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