Cryogenic fluorescence spectroscopy of ionic fluorones in gaseous and condensed phases: New light on their intrinsic photophysics

Ashworth, Eleanor K., Langeland, Jeppe, Stockett, Mark H., Lindkvist, Thomas Toft, Kjær, Christina, Bull, James N. ORCID: https://orcid.org/0000-0003-0953-1716 and Nielsen, Steen Brøndsted (2022) Cryogenic fluorescence spectroscopy of ionic fluorones in gaseous and condensed phases: New light on their intrinsic photophysics. The Journal of Physical Chemistry A, 126 (51). 9553–9563. ISSN 1089-5639

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Abstract

Fluorescence spectroscopy of gas-phase ions generated through electrospray ionization is an emerging technique able to probe intrinsic molecular photophysics directly without perturbations from solvent interactions. While there is ample scope for the ongoing development of gas-phase fluorescence techniques, the recent expansion into low-temperature operating conditions accesses a wealth of data on intrinsic fluorophore photophysics, offering enhanced spectral resolution compared with room-temperature measurements, without matrix effects hindering the excited-state dynamics. This perspective reviews current progress on understanding the photophysics of anionic fluorone dyes, which exhibit an unusually large Stokes shift in the gas phase, and discusses how comparison of gas- and condensed-phase fluorescence spectra can fingerprint structural dynamics. The capacity for temperature-dependent measurements of both fluorescence emission and excitation spectra helps establish the foundation for the use of fluorone dyes as fluorescent tags in macromolecular structure determination. We suggest ideas for technique development.

Item Type: Article
Additional Information: The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpca.2c07231. Funding information: Funding was provided by the Swedish Foundation for International Cooperation in Research and Higher Education (STINT, Grant No. PT2017-7328 to M.H.S. and J.N.B.) and an EPSRC New Investigator Award (EP/W018691 to J.N.B.). E.K.A. thanks the University of East Anglia for a doctoral studentship. S.B.N. acknowledges support from the NOVO Nordisk Foundation (Grant No. NNF20OC0064958) and Carlsbergfondet (Grant No. CF20-0097). Electronic structure calculations were carried out on the High Performance Computing Cluster supported by the Research and Specialist Computing Support service at the University of East Anglia.
Uncontrolled Keywords: physical and theoretical chemistry ,/dk/atira/pure/subjectarea/asjc/1600/1606
Faculty \ School: Faculty of Science > School of Chemistry
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Depositing User: LivePure Connector
Date Deposited: 20 Dec 2022 17:33
Last Modified: 05 Jan 2023 09:32
URI: https://ueaeprints.uea.ac.uk/id/eprint/90342
DOI: 10.1021/acs.jpca.2c07231

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