Nonperturbative modeling of fifth-order coherent multidimensional spectroscopy in light harvesting antennas

Exciton–vibrational coupling in the dynamics and spectroscopy of Frenkel excitons in molecular aggregates

“…The local oscillator is significantly weaker than the other pulses and usually comes first (adapted from Ref. [285]). (b) Double-sided Feynman diagrams for two Liouville space pathways for a system consisting of a ground state |g and an excited state |e following the notation of Ref.…”

“…Even though some 2D spectroscopy studies have addressed higher-order signals [285][286][287], usually the third order is considered which corresponds to a four-wave mixing experiment. Upon expansion of the polarization up to third order with respect to the incoming fields, one obtains eight four-time correlation functions of the dipole operator, which can be interpreted in terms of doublesided Feynman diagrams corresponding to distinct paths in Liouville space.…”

Mapping of exciton–exciton annihilation in a molecular dimer via fifth-order femtosecond two-dimensional spectroscopy

“…4,5,14 In a theoretical study, Brüggemann and Pullerits have simulated a fifth-order signal in the Fenna-Matthews-Olson complex numerically that carries information on EEA. 15 Recently, it was shown that it is possible to detect exciton-exciton interactions and to extract diffusion time constants from coherent two-dimensional (2D) spectra. 16 The EEA is connected to an appearance of spectral peaks during a pulse delay time (population time) and it becomes more effective if the laser fields interacting with a sample are of high intensity.…”

Two-dimensional action spectroscopy of excitonic systems: Explicit simulation using a phase-modulation technique

“…Previously, simulation of 2D spectra based on the explicit calculations of the nonlinear coherent response from an ensemble of systems have been carried out [38,39]. However, such calculations cannot be used to simulate 2D spectra from a single excitonic system.…”