Work

Enhancement of Vibronic and Ground-State Vibrational Coherences in 2D Spectra of Photosynthetic Complexes

Year: 2013

Type: article

Abstract: 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.

Source: Scientific Reports

DOI: 10.1038/srep02029

Authors: Aurélia Chenu, Niklas Christensson, Harald F. Kauffmann, Tomáš Mančal

Institutions: Charles University, University of Vienna

Language: English

Topic: Spectroscopy and Quantum Chemical Studies

Subfield: Atomic and Molecular Physics, and Optics

Field: Physics and Astronomy

Domain: Physical Sciences

Open Access status: gold

Estimated APC paid: $2,690

Funders: Ministerstvo Školství, Mládeže a Tělovýchovy, Grantová Agentura České Republiky, Austrian Science Fund