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Photocalorimetric spectroscopy is demonstrated as a sensitive technique for recording the vibrational and electronic spectra of weakly absorbing films on surfaces. The method employs a low‐temperature microcalorimeter which may also be used to monitor enthalpy changes associated with processes in surface films. The calorimeter is sufficiently sensitive to determine growth rates during film deposition, enthalpies of surface adsorption, and the heat capacity of the surface film. Therefore, it becomes possible to correlate spectroscopic data from surface films with thermodynamic information from the same sample. Preliminary results from studies of pyridine films on evaporated metal films are reported

Photocalorimetric spectroscopy and ac calorimetry of thin surface films