This paper presents a theoretical framework for designing light-harvesting systems that achieve high efficiency through dark state engineering, including donor-acceptor architectures, non-Hermitian Hamiltonian engineering, and vibronic resonance-assisted transport mechanisms.
Key findings
A systematic protocol for constructing dark-state-protected donor-acceptor architectures is developed.
Non-Hermitian Hamiltonian engineering can recover and stabilize dark states under perturbations.
Vibronic resonance-assisted transport mechanisms can enhance transfer rates by 20-50%.
Optimized dark-state-engineered systems can achieve power conversion efficiencies exceeding 18%.
Limitations & open questions
The existence of dark states requires strict constraints, difficult to maintain in disordered molecular environments.
Dark state protection reduces radiative losses but can decrease absorption cross-section if not carefully engineered.
The influence of vibronic coupling on dark-state-mediated transport remains incompletely understood.