Identification of Nonradiative Decay Pathways in Cy3
Name
Hart_jpcl_2020.pdf
Description
Accepted version
Size
4.39 MB
Format
Adobe PDF
Checksum (MD5)
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Author(s)
Hart, Stephanie M.
Banal, James L.
Bathe, Mark
Schlau-Cohen, Gabriela S
Date Issued
June 2020
Journal
Journal of Physical Chemistry Letters
Publisher
American Chemical Society (ACS)
Citation
Hart, Stephanie M. et al. "Identification of Nonradiative Decay Pathways in Cy3." Journal of Physical Chemistry Letters
11, 13 (June 2020): 5000-5007. © 2020 American Chemical Society
Version
Author's final manuscript
Abstract
Photoexcited fluorescent markers are extensively used in spectroscopy, imaging, and analysis of biological systems. The performance of fluorescent markers depends on high levels of emission, which are limited by competing nonradiative decay pathways. Small-molecule fluorescent dyes have been increasingly used as markers due to their high and stable emission. Despite their prevalence, the nonradiative decay pathways of these dyes have not been determined. Here, we investigate these pathways for a widely used indocarbocyanine dye, Cy3, using transient grating spectroscopy. We identify a nonradiative decay pathway via a previously unknown dark state formed within ∼1 ps of photoexcitation. Our experiments, in combination with electronic structure calculations, suggest that the generation of the dark state is mediated by picosecond vibrational mode coupling, likely via a conical intersection. We further identify the vibrational modes, and thus structural elements, responsible for the formation and dynamics of the dark state, providing insight into suppressing nonradiative decay pathways in fluorescent markers such as Cy3.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
Massachusetts Institute of Technology. Department of Biological Engineering
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Creative Commons Attribution-Noncommercial-Share Alike
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DOI of Published Version
https://doi.org/10.1021/acs.jpclett.0c01201
