Influence of a Weak Hydrogen Bond on Vibrational Coherence Probed by Photon Echoes in DCl Dimer Trapped in Solid Nitrogen

Abstract

The dynamics in the ground electronic state of the two intramolecular D-Cl stretching modes of (DCl)2 in nitrogen solid has been probed by degenerate four wave mixing experiments. Accumulated photon echoes on the "free" nu1 and "bonded" nu2 modes have been performed by means of the free electron laser of Orsay (CLIO). The analysis of the time-resolved signals provides information on the various processes responsible for the loss of vibrational coherence, in particular intra- and intermolecular vibrational energy transfer and pure dephasing. The influence of the weak hydrogen bond is clearly observed on the coherence times of the two stretching modes. Whatever the temperature, the homogeneous width of nu2 lines is almost twice that of nu1 lines. Contrary to the case of isolated DCl trapped in solid nitrogen, no obvious effect of the nitrogen lattice can be extracted from the temperature dependence of the coherence times.