Spectrally-tunable femtosecond single-molecule pump-probe spectroscopy
Name
oe-29-18-28246.pdf
Description
Published version
Size
2.88 MB
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Unknown
Checksum (MD5)
92e7094f5796720723f010d1581ddf0d
Author(s)
Moya, Raymundo
Kondo, Toru
Norris, Audrey C.
Schlau-Cohen, Gabriela S.
Date Issued
August 2021
Journal
Optics Express
Publisher
The Optical Society
Citation
Moya, Raymundo, Kondo, Toru, Norris, Audrey C and Schlau-Cohen, Gabriela S. 2021. "Spectrally-tunable femtosecond single-molecule pump-probe spectroscopy." Optics Express, 29 (18).
Version
Final published version
Abstract
Single-molecule spectroscopy has been extensively used to investigate heterogeneity in static and dynamic behaviors on millisecond and second timescales. More recently, single-molecule pump-probe spectroscopy emerged as a method to access heterogeneity on the femtosecond and picosecond timescales. Here, we develop a single-molecule pump-probe apparatus that is easily tunable across the visible region and demonstrate its utility on the widely-used fluorescent dye, Atto647N. A spectrally-independent, bimodal distribution of energetic relaxation time constants is found, where one peak corresponds to electronic dephasing (∼ 100 fs) and the other to intravibrational relaxation (∼ 300 fs). The bimodal nature indicates that relaxation within each individual molecule is dominated by only one of these processes. Both peaks of the distribution are narrow, suggesting little heterogeneity is present for either process. As illustrated here, spectrally-tunable single-molecule pump-probe spectroscopy will enable investigation of the heterogeneity in a wide range of biological and material systems.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
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Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use.
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DOI of Published Version
https://doi.org/10.1364/oe.432995
