Abstract
A novel barochromic technique to study solvation of molecular electronic states is introduced using chlorophyll and carotenoids as probes. Nonpolar carotenoids in nonpolar solvent demonstrate an excess barochromic shift over solvatochromic shifts of absorption at high pressures as a result of solute cavity compression. The dependence of weakly polar bacteriochlorophyll a absorption and emission spectra, responsible for the Qy electronic transition, on pressure in weakly polar solvents demonstrates a breakdown of linear relationship between the squared bandwidths and the Stokes shift suggested by the standard model. This is a result of solvent-induced non-adiabatic coupling of solute electronic states. The Stokes shift as a function of pressure passes through a minimum due to suppression of dispersion interactions by polar interactions at high densities.
Published Version
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