Multidimensional spectroscopy with a single broadband phase-shaped laser pulse

TL;DR

This paper demonstrates how phase-shaped broadband laser pulses can control and manipulate nonlinear spectroscopic signals, specifically two-photon and Raman resonances, by adjusting phase profiles to suppress or enhance specific quantum pathways.

Contribution

It introduces a theoretical framework for calculating frequency-dispersed signals with phase-shaped pulses and shows how phase profiles influence quantum pathway selection in nonlinear spectroscopy.

Findings

Phase profiles can selectively enhance or suppress quantum pathways.

Two-dimensional signals reveal control over two-photon and Raman resonances.

Phase sign and shape significantly affect spectral features.

Abstract

We calculate the frequency-dispersed nonlinear transmission signal of a phase-shaped visible pulse to fourth order in the field. Two phase profiles, a phase-step and phase-pulse, are considered. Two dimensional signals obtained by varying the detected frequency and phase parameters are presented for a three electronic band model system. We demonstrate how two-photon and stimulated Raman resonances can be manipulated by the phase profile and sign, and selected quantum pathways can be suppressed.