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

Research output: Contribution to journalArticlepeer-review

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 languageEnglish (US)
Pages (from-to)3237-3243
Number of pages7
JournalJournal of Physical Chemistry Letters
Volume13
Issue number14
DOIs
StatePublished - Apr 14 2022
Externally publishedYes

ASJC Scopus subject areas

  • Materials Science(all)
  • Physical and Theoretical Chemistry

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