Correlated spectral fluctuations quantified by line shape analysis of fifth-order two-dimensional electronic spectra

Constantin Heshmatpour, Jürgen Hauer, František Šanda

Research output: Contribution to journalArticlepeer-review

3 Scopus citations

Abstract

Correlated spectral fluctuations were suggested to coordinate excitation transport inside natural light harvesting complexes. We demonstrate the capacities of 2D line shapes from fifth-order coherent electronic signals (R5-2D) to report on such fluctuations in molecular aggregates and present a stochastic approach to fluctuations in correlated site and bi-exciton binding energies in the optical dynamics of Frenkel excitons. The model is applied to R5-2D line shapes of a homodimer, and we show that the peak tilt dynamics are a measure for site energy disorder, inter-site correlation, and the strength of bi-exciton binding energy fluctuations.

Original languageEnglish
Article number084114
JournalJournal of Chemical Physics
Volume156
Issue number8
DOIs
StatePublished - 28 Feb 2022

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