Ultrafast Collective Excited-State Dynamics of a Virus-Supported Fluorophore Antenna

Joseph Holmes; Arathi Anil Sushma; Irina B. Tsvetkova; William L. Schaich; Richard D. Schaller; Bogdan Dragnea

doi:10.1021/acs.jpclett.2c00262

Ultrafast Collective Excited-State Dynamics of a Virus-Supported Fluorophore Antenna

Joseph Holmes, Arathi Anil Sushma, Irina B. Tsvetkova, William L. Schaich, Richard D. Schaller, Bogdan Dragnea

Chemistry

Research output: Contribution to journal › Article › peer-review

2 Scopus citations

Abstract

Radiation brightening was recently observed in a multifluorophore-conjugated brome mosaic virus (BMV) particle at room temperature under pulsed excitation. On the basis of its nonlinear dependence on the number of chromophores, the origins of the phenomenon were attributed to a collective relaxation. However, the mechanism remains unknown. We present ultrafast transient absorption and fluorescence spectroscopic studies which shed new light on the collective nature of the relaxation dynamics in such radiation-brightened, multifluorophore particles. Our findings indicate that the emission dynamics is consistent with a superradiance mechanism. The ratio between the rates of competing radiative and nonradiative relaxation pathways depends on the number of chromophores per virus. The findings suggest that small icosahedral virus shells provide a unique biological scaffold for developing nonclassical, deep subwavelength light sources and may open new avenues for the development of photonic probes for medical imaging applications.

Original language	English (US)
Pages (from-to)	3237-3243
Number of pages	7
Journal	Journal of Physical Chemistry Letters
Volume	13
Issue number	14
DOIs	https://doi.org/10.1021/acs.jpclett.2c00262
State	Published - Apr 14 2022

Funding

The work was supported by the Army Research Office, under Awards W911NF2010072 and W911NF2010071, and by the National Science Foundation, under Award CBET-1803440. This work was performed, in part, at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, and supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. We are grateful to the Center for Bioanalytical Metrology (CBM), an NSF Industry-University Cooperative Research Center, for providing funding for this project under Grant NSF IIP 1916645, and to members of the industry advisory board of the CBM for valuable discussions and feedback.

ASJC Scopus subject areas

General Materials Science
Physical and Theoretical Chemistry

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10.1021/acs.jpclett.2c00262

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title = "Ultrafast Collective Excited-State Dynamics of a Virus-Supported Fluorophore Antenna",

abstract = "Radiation brightening was recently observed in a multifluorophore-conjugated brome mosaic virus (BMV) particle at room temperature under pulsed excitation. On the basis of its nonlinear dependence on the number of chromophores, the origins of the phenomenon were attributed to a collective relaxation. However, the mechanism remains unknown. We present ultrafast transient absorption and fluorescence spectroscopic studies which shed new light on the collective nature of the relaxation dynamics in such radiation-brightened, multifluorophore particles. Our findings indicate that the emission dynamics is consistent with a superradiance mechanism. The ratio between the rates of competing radiative and nonradiative relaxation pathways depends on the number of chromophores per virus. The findings suggest that small icosahedral virus shells provide a unique biological scaffold for developing nonclassical, deep subwavelength light sources and may open new avenues for the development of photonic probes for medical imaging applications.",

author = "Joseph Holmes and Sushma, {Arathi Anil} and Tsvetkova, {Irina B.} and Schaich, {William L.} and Schaller, {Richard D.} and Bogdan Dragnea",

note = "Funding Information: The work was supported by the Army Research Office, under Awards W911NF2010072 and W911NF2010071, and by the National Science Foundation, under Award CBET-1803440. This work was performed, in part, at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, and supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. We are grateful to the Center for Bioanalytical Metrology (CBM), an NSF Industry-University Cooperative Research Center, for providing funding for this project under Grant NSF IIP 1916645, and to members of the industry advisory board of the CBM for valuable discussions and feedback. Publisher Copyright: {\textcopyright} 2022 American Chemical Society. All rights reserved.",

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AU - Schaller, Richard D.

AU - Dragnea, Bogdan

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PY - 2022/4/14

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N2 - Radiation brightening was recently observed in a multifluorophore-conjugated brome mosaic virus (BMV) particle at room temperature under pulsed excitation. On the basis of its nonlinear dependence on the number of chromophores, the origins of the phenomenon were attributed to a collective relaxation. However, the mechanism remains unknown. We present ultrafast transient absorption and fluorescence spectroscopic studies which shed new light on the collective nature of the relaxation dynamics in such radiation-brightened, multifluorophore particles. Our findings indicate that the emission dynamics is consistent with a superradiance mechanism. The ratio between the rates of competing radiative and nonradiative relaxation pathways depends on the number of chromophores per virus. The findings suggest that small icosahedral virus shells provide a unique biological scaffold for developing nonclassical, deep subwavelength light sources and may open new avenues for the development of photonic probes for medical imaging applications.

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Ultrafast Collective Excited-State Dynamics of a Virus-Supported Fluorophore Antenna

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