Nonperturbative approach to the nonlinear photon echo of V-type system

TL;DR

This paper introduces a nonperturbative quantum dynamical approach to analyze nonlinear photon echo signals in V-type systems, capturing higher-order effects neglected in traditional perturbative methods.

Contribution

It develops a nonperturbative response formalism for nonlinear spectroscopy, extending analysis beyond third-order perturbation to include higher-order contributions.

Findings

Higher-order terms significantly affect the photon echo signals.

The method accounts for environmental dephasing effects.

Demonstrates applicability to quantum optical systems.

Abstract

The analysis of nonlinear spectroscopy, widely used to study the dynamics and structures of condensed-phase matter, typically employs a perturbative approach noticing the weak interaction between the laser and the matter of interest. However, such perturbative approach is no longer applicable once the interaction between the laser and the matter is strong. We adapt the method of quantum dynamical evolution into the calculation of signal and present the response formalism of the nonlinear spectroscopy in a nonperturbative approach. In this new approach, we demonstrate that in addition to the third-order term in the perturbative method, the higher-order terms have essential contributions to the nonlinear signal of the two-pulse and three-pulse photon echo (2PPE and 3PPE). The detailed calculations are demonstrated with the example of a three-level V-type system, which is widely used in the studies of quantum optics. We consider the effect of the environment via a pure dephasing mechanism with both the localized modes of each molecule and the shared modes between molecules.