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Dephasing dynamics across different local vibrational modes and crystalline environments
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Keat, T. J., Coxon, D. J. L., Staniforth, M., Dale, M. W., Stavros, V. G., Newton, M. E. and Lloyd-Hughes, J. (2022) Dephasing dynamics across different local vibrational modes and crystalline environments. Physical Review Letters, 129 (23). 237401. doi:10.1103/physrevlett.129.237401 ISSN 1079-7114.
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Official URL: https://doi.org/10.1103/PhysRevLett.129.237401
Abstract
The perturbed free induction decay (PFID) observed in ultrafast infrared spectroscopy was used to unveil the rates at which different vibrational modes of the same atomic-scale defect can interact with their environment. The N3VH0 defect in diamond provided a model system, allowing a comparison of stretch and bend vibrational modes within different crystal lattice environments. The observed bend mode (first overtone) exhibited dephasing times T2=2.8(1) ps, while the fundamental stretch mode had surprisingly faster dynamics T2<1.7 ps driven by its more direct perturbation of the crystal lattice, with increased phonon coupling. Further, at high defect concentrations the stretch mode’s dephasing rate was enhanced. The ability to reliably measure T2 via PFID provides vital insights into how vibrational systems interact with their local environment.
Item Type: | Journal Article | ||||||||||||
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Subjects: | Q Science > QC Physics | ||||||||||||
Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry Faculty of Science, Engineering and Medicine > Science > Physics |
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SWORD Depositor: | Library Publications Router | ||||||||||||
Library of Congress Subject Headings (LCSH): | Infrared spectroscopy, Crystallography, Crystals -- Defects, Phonons | ||||||||||||
Journal or Publication Title: | Physical Review Letters | ||||||||||||
Publisher: | American Physical Society | ||||||||||||
ISSN: | 1079-7114 | ||||||||||||
Official Date: | 29 November 2022 | ||||||||||||
Dates: |
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Volume: | 129 | ||||||||||||
Number: | 23 | ||||||||||||
Number of Pages: | 6 | ||||||||||||
Article Number: | 237401 | ||||||||||||
DOI: | 10.1103/physrevlett.129.237401 | ||||||||||||
Status: | Peer Reviewed | ||||||||||||
Publication Status: | Published | ||||||||||||
Access rights to Published version: | Restricted or Subscription Access | ||||||||||||
Copyright Holders: | American Physical Society | ||||||||||||
Date of first compliant deposit: | 9 January 2023 | ||||||||||||
Date of first compliant Open Access: | 10 January 2023 | ||||||||||||
RIOXX Funder/Project Grant: |
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