Diagonal Slice Four-Wave Mixing: Natural Separation of Coherent Broadening Mechanisms

TL;DR

This paper introduces a novel ultrafast spectroscopy method that efficiently separates homogeneous and inhomogeneous broadening effects in resonance lineshapes, enabling faster data collection and detailed analysis of broadening mechanisms.

Contribution

The authors develop a new slice-based spectroscopy technique with analytical lineshape expressions that distinguish broadening contributions, improving upon traditional methods.

Findings

Analytical lineshape formulas for separated broadening mechanisms

Faster data acquisition compared to full spectra

Applicable to slices from multidimensional spectra

Abstract

We present an ultrafast coherent spectroscopy data acquisition scheme that samples slices of the time domain used in multidimensional coherent spectroscopy to achieve faster data collection than full spectra. We derive analytical expressions for resonance lineshapes using this technique that completely separate homogeneous and inhomogeneous broadening contributions into separate projected lineshapes for arbitrary inhomogeneous broadening. These lineshape expressions are also valid for slices taken from full multidimensional spectra and allow direct measurement of the parameters contributing to the lineshapes in those spectra as well as our own.