2012/11/19 by Aurélia Chenu, Niklas Christensson, Harald F. Kauffmann +2 · 1 citation
Biochemistry, Genetics and Molecular Biology · Chemistry · Physics and Astronomy · #Advanced Chemical Physics Studies #Atomic physics #Chemistry #Condensed matter physics #Dephasing #Excited state #Exciton #Ground state #Molecular physics #Molecular vibration #Molecule #Photosynthetic Processes and Mechanisms #Physics #Population #Quantum mechanics #Spectroscopy and Quantum Chemical Studies #Vibronic coupling #Vibronic spectroscopy #physics.chem-ph #quant-ph
paper · pdf · doi:10.1038/srep02029
published as Scientific Reports 3 (2013) 2029 · 16 pages, 6 figures
arxiv created 2012/11/19 · openalex publication_date 2013/06/19 · arxiv updated 2016/05/26 · openalex created_date 2025/10/10 · openalex updated_date 2026/08/06
A vibronic-exciton model is applied to investigate the recently proposed mechanism of enhancement of coherent oscillations due to mixing of electronic and nuclear degrees of freedom. We study a dimer system to elucidate the role of resonance coupling, site energies, vibrational frequency and energy disorder in the enhancement of vibronic-exciton and ground-state vibrational coherences, and to identify regimes where this enhancement is significant. For a heterodimer representing two coupled bachteriochloropylls of the FMO complex, long-lived vibronic coherences are found to be generated only when the frequency of the mode is in the vicinity of the electronic energy difference. Although the vibronic-exciton coherences exhibit a larger initial amplitude compared to the ground-state vibrational coherences, we conclude that, due to the dephasing of the former, both type of coherences have a similar magnitude at longer population time.