Time-resolved infrared vibrational spectroscopy is a structurally sensitive probe of the excited-state properties of matter. The technique has found many applications in the study of molecules in dilute solution phase but has rarely been applied to crystalline samples. We report on the use of a sensitive pump–probe time-resolved infrared spectrometer and sample handling techniques for studies of the ultrafast excited-state dynamics of crystalline materials. The charge transfer excited states of crystalline metal carbonyls and the proton transfer of dihydroxyquinones are presented and compared with the solution phase.
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