2015/12/14 by Marco Merkli, G. P. Berman, Merkli, M. +11
Biochemistry, Genetics and Molecular Biology · Neuroscience · Physics and Astronomy · #Biological Physics (physics.bio-ph) #Chemical Physics (physics.chem-ph) #FOS: Physical sciences #Photoreceptor and optogenetics research #Photosynthetic Processes and Mechanisms #Quantum Physics (quant-ph) #Spectroscopy and Quantum Chemical Studies
paper · pdf · doi:10.48550/arxiv.1512.08810
openalex publication_date 2015/12/14 · openalex created_date 2025/10/10 · openalex updated_date 2026/08/01
We present a theoretical analysis of exciton transfer and decoherence effects in a photosynthetic dimer interacting with collective (correlated) and local (uncorrelated) protein-solvent environments. Our approach is based on the framework of the spin-boson model. We derive explicitly the thermal relaxation and decoherence rates of the exciton transfer process, valid for arbitrary temperatures and for arbitrary (in particular, large) interaction constants between the dimer and the environments. We establish a generalization of the Marcus formula, giving reaction rates for dimer levels possibly individually and asymmetrically coupled to environments. We identify rigorously parameter regimes for the validity of the generalized Marcus formula. The existence of long living quantum coherences at ambient temperatures emerges naturally from our approach.