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

TL;DR

This study investigates the ultrafast collective relaxation dynamics in virus-supported fluorophore assemblies, revealing superradiance behavior and coherent oscillations, with implications for biological light sources and medical imaging.

Contribution

It provides the first ultrafast spectroscopic evidence of superradiance and coherent oscillations in virus-supported fluorophore particles, advancing understanding of their collective emission mechanisms.

Findings

Emission dynamics consistent with superradiance

Rate ratios depend on fluorophore number

Evidence of room-temperature coherent oscillations

Abstract

Radiation brightening was recently observed in a multi-fluorophore-conjugated brome mosaic virus (BMV) particle, at room temperature under pulsed excitation. Based on its nonlinear dependence on the number of fluorophores, 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, multi-fluorophore particles. Our findings indicate that the emission dynamics is consistent with a superradiance mechanism. The ratio between the rates of competing radiative and non-radiative relaxation pathways depends on the number of fluorophores per virus. We also discuss the evidence of coherent oscillations in the transient absorption trace from multi-fluorophore conjugated which last for $\sim100$s of picoseconds, at room temperature. The findings suggest that small icosahedral virus shells provide a unique biological scaffold for developing non-classical, deep subwavelength light sources, and may open new realms for the development of photonic probes for medical imaging applications.