Fifth-order electronically non-resonant Raman scattering: two-dimensional Fourier deconvolution

This paper presents an analytical Fourier deconvolution procedure for homod yne detected electronically non-resonant fifth-order signal that reveals th e bare nuclear response function free from the influence of the electronic (hyperpolarizability) responses generated by the five potentially overlappi ng finite duration pulses used in the experiment. In developing the fifth-o rder deconvolution procedure, an analogous procedure for homodyne detected third-order responses is elaborated. The potential implementation problems with the homodyne deconvolution procedure are evaluated through comparison of the third-order homodyne deconvolution result with that of the well-know n third-order heterodyne deconvolution. Then, the homodyne deconvolution is extended to fifth-order where it is used on several measured tenser elemen ts of the direct fifth-order signal. Suggestions are given for improving im plementation of the procedure in fifth order so that more information on th e direct fifth-order nuclear response as well as the hyperpolarizability re sponses can be recovered via the deconvolution procedure. (C) 2001 Elsevier Science B.V. All rights reserved.