Intraband Exciton Transitions in Photosynthetic Complexes Revealed by Novel Five-Wave-Mixing Spectroscopy.
| Autor: | Kizmann M; Department of Chemistry, University of California, Irvine, California 92614, United States.; Department of Physics and Astronomy, University of California, Irvine, California 92614, United States., Yadalam HK; Department of Chemistry, University of California, Irvine, California 92614, United States.; Department of Physics and Astronomy, University of California, Irvine, California 92614, United States., Chernyak VY; Department of Chemistry, Wayne State University, 5101 Cass Avenue, Detroit, Michigan 48202, United States.; Department of Mathematics, Wayne State University, 656 W. Kirby, Detroit, Michigan 48202, United States., Mukamel S; Department of Chemistry, University of California, Irvine, California 92614, United States.; Department of Physics and Astronomy, University of California, Irvine, California 92614, United States. |
|---|---|
| Jazyk: | angličtina |
| Zdroj: | Journal of chemical theory and computation [J Chem Theory Comput] 2024 Jan 09; Vol. 20 (1), pp. 280-289. Date of Electronic Publication: 2023 Dec 21. |
| DOI: | 10.1021/acs.jctc.3c00919 |
| Abstrakt: | We calculate the χ (4) optical response of an oriented photosystem II reaction center of purple bacteria described by the Frenkel exciton model using nonlinear exciton equations (NEE). This approach treats each chromophore as an anharmonic oscillator and provides an intuitive quasiparticle picture of nonlinear spectroscopic signals of interacting excitons. It provides a computationally powerful description of nonlinear spectroscopic signals that avoids complete diagonalization of the total Hamiltonian. Expressions for the second- and the fourth-order nonlinear signals are derived. The NEE have been successfully employed in the past to describe even-order-wave-mixing. Here, we extend them to aggregates with broken inversion symmetries. Even-order susceptibilities require the introduction of permanent dipoles, which allow to directly probe low-frequency intraband transitions of excitons. |
| Databáze: | MEDLINE |
| Externí odkaz: |
|