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Title: Spatially-resolved fluorescence-detected two-dimensional electronic spectroscopy probes varying excitonic structure in photosynthetic bacteria

Abstract

Conventional implementations of two-dimensional electronic spectroscopy typically spatially average over ~10 10 chromophores spread over ~10 4 micron square area, limiting their ability to characterize spatially heterogeneous samples. Here we present a variation of two-dimensional electronic spectroscopy that is capable of mapping spatially varying differences in excitonic structure, with sensitivity orders of magnitude better than conventional spatially-averaged electronic spectroscopies. The approach performs fluorescence-detection-based fully collinear two-dimensional electronic spectroscopy in a microscope, combining femtosecond time-resolution, sub-micron spatial resolution, and the sensitivity of fluorescence detection. We demonstrate the approach on a mixture of photosynthetic bacteria that are known to exhibit variations in electronic structure with growth conditions. As a result, spatial variations in the constitution of mixed bacterial colonies manifests as spatially varying peak intensities in the measured two-dimensional contour maps, which exhibit distinct diagonal and cross-peaks that reflect differences in the excitonic structure of the bacterial proteins.

Authors:
ORCiD logo [1];  [2];  [3]; ORCiD logo [4]; ORCiD logo [3]; ORCiD logo [1]
  1. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Physics
  2. Univ. of Michigan, Ann Arbor, MI (United States). Applied Physics Program
  3. Univ. of Glasgow, Scotland (United Kingdom). Inst. of Molecular Biology
  4. Univ. of Groningen, Groningen (The Netherlands). Zernike Inst. for Advanced Materials
Publication Date:
Research Org.:
Washington Univ., St. Louis, MO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1483411
Grant/Contract Number:  
SC0001035
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
59 BASIC BIOLOGICAL SCIENCES

Citation Formats

Tiwari, Vivek, Matutes, Yassel Acosta, Gardiner, Alastair T., Jansen, Thomas L. C., Cogdell, Richard J., and Ogilvie, Jennifer P. Spatially-resolved fluorescence-detected two-dimensional electronic spectroscopy probes varying excitonic structure in photosynthetic bacteria. United States: N. p., 2018. Web. doi:10.1038/s41467-018-06619-x.
Tiwari, Vivek, Matutes, Yassel Acosta, Gardiner, Alastair T., Jansen, Thomas L. C., Cogdell, Richard J., & Ogilvie, Jennifer P. Spatially-resolved fluorescence-detected two-dimensional electronic spectroscopy probes varying excitonic structure in photosynthetic bacteria. United States. doi:10.1038/s41467-018-06619-x.
Tiwari, Vivek, Matutes, Yassel Acosta, Gardiner, Alastair T., Jansen, Thomas L. C., Cogdell, Richard J., and Ogilvie, Jennifer P. Thu . "Spatially-resolved fluorescence-detected two-dimensional electronic spectroscopy probes varying excitonic structure in photosynthetic bacteria". United States. doi:10.1038/s41467-018-06619-x. https://www.osti.gov/servlets/purl/1483411.
@article{osti_1483411,
title = {Spatially-resolved fluorescence-detected two-dimensional electronic spectroscopy probes varying excitonic structure in photosynthetic bacteria},
author = {Tiwari, Vivek and Matutes, Yassel Acosta and Gardiner, Alastair T. and Jansen, Thomas L. C. and Cogdell, Richard J. and Ogilvie, Jennifer P.},
abstractNote = {Conventional implementations of two-dimensional electronic spectroscopy typically spatially average over ~1010 chromophores spread over ~104 micron square area, limiting their ability to characterize spatially heterogeneous samples. Here we present a variation of two-dimensional electronic spectroscopy that is capable of mapping spatially varying differences in excitonic structure, with sensitivity orders of magnitude better than conventional spatially-averaged electronic spectroscopies. The approach performs fluorescence-detection-based fully collinear two-dimensional electronic spectroscopy in a microscope, combining femtosecond time-resolution, sub-micron spatial resolution, and the sensitivity of fluorescence detection. We demonstrate the approach on a mixture of photosynthetic bacteria that are known to exhibit variations in electronic structure with growth conditions. As a result, spatial variations in the constitution of mixed bacterial colonies manifests as spatially varying peak intensities in the measured two-dimensional contour maps, which exhibit distinct diagonal and cross-peaks that reflect differences in the excitonic structure of the bacterial proteins.},
doi = {10.1038/s41467-018-06619-x},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {Thu Oct 11 00:00:00 EDT 2018},
month = {Thu Oct 11 00:00:00 EDT 2018}
}

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