Dynamics in low temperature glasses: Theory and experiments on optical dephasing, spectral diffusion, and hydrogen tunneling

Abstract

Temperature dependent photon echo (PE) and nonphotochemical hole burning (NPHB) measurements are reported on resorufin in three organic glasses: ethanol (1.5–11 K), glycerol (1.1–25 K), and d-ethanol (1.5–11 K). In all cases, the NPHB results are broadened considerably from the PE results at low temperatures, but the two measurements coalesce at high temperatures. The temperature dependences are found to deviate from the power law dependence expected for two-level system dephasing, and the deviation is attributed to dephasing by a pseudolocal mode. The appropriate correlation functions for PE and hole burning experiments are shown to be different from each other. They also differ from the correlation function for the optical absorption (OA) experiment, which has been the basis for most calculations of optical dephasing in glasses. The broadening of hole widths beyond the PE result is shown to be a measure of the slow spectral diffusion processes in the glass. Other types of dephasing measurement are also analyzed and each measurement is shown to be sensitive to spectral diffusion to a different degree. By making standard assumptions about glass dynamics, the main experimental results can be accounted for. A long range chromophore–glass interaction and a 1/R distribution of relaxation rates R at short times are indicated.