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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

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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
Subjects: Q Science > QC Physics
Divisions: Faculty of Science, Engineering and Medicine > Science > Chemistry
Faculty of Science, Engineering and Medicine > Science > Physics
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:
DateEvent
29 November 2022Published
20 October 2022Accepted
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:
Project/Grant IDRIOXX Funder NameFunder ID
UNSPECIFIEDDe Beers GroupUNSPECIFIED
UNSPECIFIEDWarwick Centre for Doctoral Training in Diamond Science and TechnologyUNSPECIFIED
UNSPECIFIED[RS] Royal Societyhttp://dx.doi.org/10.13039/501100000288

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