Measuring Time-Dependent Induced Quantum Coherences via Two-Dimensional Coherence Spectroscopy

TL;DR

This paper introduces a two-dimensional spectroscopic method to measure how quantum coherences evolve over time in systems affected by environment interactions, providing insights into exciton dynamics in polymers.

Contribution

It presents a novel protocol for probing time-dependent quantum coherences and their environmental interactions using a combination of analytical and numerical approaches.

Findings

Protocol successfully measures induced quantum coherences.

Temporal noise effects on coherence dephasing are characterized.

Application demonstrated on exciton dynamics in conjugated polymers.

Abstract

We propose a two-dimensional spectroscopic protocol for measuring the time-dependent coherences between the stationary states of a system induced by a time-dependent system-bath interaction. We also investigate the role of temporally-correlated noise on coherence dephasing. This protocol enables dynamical information about the system and its coupling to the environment to be determined. Our results are based on the quantum-trajectory method, and are obtained from both approximate, analytical and exact, numerical solutions of the time-dependent Schroedinger equation. As an example, we show how this protocol can be used to investigate exciton dynameds in conjugated polymers induced by the coupling of their torsional modes with the environment.