Broadening and shifting of the Raman Q branch in D2 and D2–He mixtures, II: line shapes, fitting routines, and effects nonlinear in density

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Abstract
In the preceding paper we fitted the experimental profiles using a single Lorentzian line shape and assumed that the width and shift were proportional to the density. Here we discuss nonlinear contributions to widths and shifts and present a different spectral profile and analysis that allows us (i) to determine unbiased, binary collision, impact limit, broadening and shifting coefficients; (ii) to disentangle several effects nonlinear in the density; and, subsequently, (iii) to observe broadening and shifting arising purely from the correlation between perturbers and three-body interactions. This is a new avenue of research in molecular dynamics. In addition, measurements of the broadening of the depolarized part of the Q branch in D2 are reported for the first time.

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