Selective Vibronic Excitation for Coherent Energy Transport in Photosynthetic and Agrivoltaic Systems

Abstract

Partitioning the photonic environment into resonant and off-resonant modes provides a mechanism for dephasing suppression in photosynthetic energy transfer. Aligning the excitation spectrum with underdamped vibronic resonances in the Fenna-Matthews-Olson (FMO) complex prepares vibronically dressed states with reduced coupling to dissipative fluctuations, inducing a biexponential coherence decay: a rapid initial dephasing (τfast {\approx} 37fs) followed by persistent inter-band coherences extending beyond 1ps-a > 3x extension of the effective coherence window relative to broadband excitation (τc = 280fs). This improves forward transfer yields by 39% at 295K. PT-HOPS/SBD simulations establish that dual-band filtering at 750nm and 820nm targets vibronic resonances while bypassing dephasing-dominated noise. This enhancement is robust against static disorder (σ = 50 cm-1), with an ensemble-averaged increase of η = 0.39 {\pm} 0.04. These results identify selective vibronic excitation as a foundational design principle for coherence-assisted transport. This framework extends to symbiotic agrivoltaic systems, where organic photovoltaics function as active spectral filters to co-optimize excitonic transport alongside the photosynthetic requirements of underlying crops.