Quasi-localized low-frequency vibrational modes of disordered solids Ⅱ. Study by single-molecule spectroscopy

摘要

By means of single molecule (SM) spectroscopy we investigated elementary matrix excitations in a disordered solid, i.e., quasi-localized low-frequency vibrational modes (LFMs). To this end we recorded the spectra of single tetra-tert-butylterrylene molecules embedded in an amorphous polyisobutylene matrix in a temperature region, where the LFM contribution to line broadening dominates. The individual parameters of LFMs in a polymer glass can be determined from the temperature-dependent linewidths of single molecules. The magnitude of the LFM contribution to SM spectra was obtained by the statistical analysis of the distribution of linewidths of SMs. Pronounced distributions of LFM frequencies and SM-LFM coupling constants were found. This result can be regarded as the first direct experimental proof of the localized nature of LFMs.