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 ...

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

Spectral diffusion and individual two-level systems probed by fluorescence of single terrylene molecules in a polyethylene matrix

Coherent Transient and Holeburning Spectroscopy of Rare Earth Ions in Solids

Experimental data describing the time evolution of photochemical holes in organic glasses are reported. The photochemical system is 1,4‐dihydroxyanthraquinone (quinizarin) in ethanol/methanol glasses; its photochemistry is based on proton or deuteron transfer processes. The experiments show a logarithmic increase of the hole widths in a time domain between minutes and about 104 min. The experimental results yield a pronounced deuteration effect and little variation with temperature between 1.35 and 4.2 K. The data are interpreted in a semiquantitative way using current theories of spectral diffusion in amorphous solids. The fastest measured photochemical rates are on the order of seconds, leaving a ‘‘time independent’’ linewidth of about 0.4 cm−1 at 1.35 K.

Spectral diffusion of a photochemical proton transfer system in an amorphous organic host: Quinizarin in alcohol glass

Optical spectroscopy provides a useful tool for probing the structure and dynamics of solids. Over the years, optical methods have evolved from absorption spectroscopy to more complex methods such as spectral hole burning, photon echoes, and luminescence line narrowing. The absorption spectrum provides information about inhomogeneous broadening, while the latter approaches provide information about the systematics of the homogeneous line shapeinformation that is often obscured by inhomogeneous broadening. When external perturbations such as strain or electric fields are applied, details of the local site can be obtained. Recently, the ultimate limit of optical spectroscopy has been attained, in which the spectral properties of individual single impurity molecules in a solid can be measured, with all ensemble averaging removed. This novel regime has provided additional, previously unobtainable, information on a highly local scale, such as the direct observation of the spectral shifting of a single molecule...

Structure and Dynamics in Solids As Probed by Optical Spectroscopy

Experiences de «hole burning» photochimique sur la dihydroxy-1,4 anthraquinone dans un verre alcoolique perdeuterie (Et OD/Me OD)=3:1)

W. Breinl

Papers

Spectral diffusion of a photochemical proton transfer system in an amorphous organic host: Quinizarin in alcohol glass

Ground state tunneling and optical spectral diffusion in organic glasses