Observation of Ultrafast Coherence Transfer and Degenerate States with Polarization-Controlled Two-Dimensional Electronic Spectroscopy

Overview

Journal J Phys Chem B

Publisher American Chemical Society

Specialty Chemistry

Date 2020 Sep 29

PMID 32990439

Citations 9

Authors

Andy S Sardjan

Floris P Westerman

Jennifer P Ogilvie

Thomas L C Jansen

Affiliations

Soon will be listed here.

Abstract

Optical spectroscopy is a powerful tool to interrogate quantum states of matter. We present simulation results for the cross-polarized two-dimensional electronic spectra of the light-harvesting system LH2 of purple bacteria. We identify a spectral feature on the diagonal, which we assign to ultrafast coherence transfer between degenerate states. The implication for the interpretation of previous experiments on different systems and the potential use of this feature are discussed. In particular, we foresee that this kind of feature will be useful for identifying mixed degenerate states and for identifying the origin of symmetry breaking disorder in systems like LH2. Furthermore, this may help identify both vibrational and electronic states in biological systems such as proteins and solid-state materials such as hybrid perovskites.

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