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

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.