Vibration-rotational overtones absorption of solid hydrogens using optoacoustic spectroscopy technique

Vibrational-rotational overtones absorption solid hydrogens (H2, D2, HD) is studied using pulsed laser piezoeletric transducer (PULPIT) optoacoustic spectroscopy is studied. A general downward shift in energy from isolated molecular energies is observed. Studying normal-hydrogen it was observed that the phonon excitations associated with double-molecular transitions are predominantly transverse-optical phonons, whereas the excitations associated with single-molecular transitions are predominantly longitudinal - optical phonons. Multiplet structures were observed for certain double transitions in parahydrogen and orthodeuterium. The HD spectrum, besides presenting the sharp zero-phonon lines and the associated phonon side bands, like H2 and D2, showed also two different features. This observation was common to all the transitions involving pure rotational excitation in H2 and D2, which showed broad linewidths. This, together with some other facts (fluorescence lifetime *approx*105 sec; weak internal vibration and lattice coupling), led to the proposition of a mechanism for the fast nonradiative relaxation in solid hydrogens, implied from some observed experimental evidences. This relaxation, due to strong coupling, would happen in two steps: the internal vibration modes would relax to the rotational modes of the molecules, and then this rotational modes would relax to the lattice vibration modes. (Author)