A joint analysis of spectroscopic data obtained at liquid–helium temperatures by three line-narrowing techniques, photon echo (PE), persistent hole burning (HB), and single molecule spectroscopy (SMS), is presented. Two polymer systems, polyisobutylene (PIB) and polymethylmethacrylate (PMMA), doped with tetra-tert-butylterrylene (TBT) were studied via PE and HB techniques and the results are compared with literature data [R. Kettner et al., J. Phys. Chem. 98, 6671 (1994); B. Kozankiewicz et al., J. Chem. Phys. 101, 9377 (1994)] obtained by SMS. Both systems behave quite differently. In TBT/PIB a rather strong influence of a dispersion of the dephasing time T2 was found which plays only a minor role in TBT/PMMA. We have also measured the temperature dependence of T2 for both systems in a broad temperature range (0.4–22 K). Using these data we separated the two different contributions to the optical dephasing — due to an interaction with two-level systems and due to coupling with local low-frequency modes. The data are compared with calculations using a numerical and a semianalytical model in the presence of a large dispersion of the single molecule parameters. Furthermore, we discuss the differences of the linewidths as measured by different experimental methods.

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We have measured the temperature dependence of the homogeneous width of spectral holes in the incommensurate phase III of chlorin-doped biphenyl from 60 mK to 10 K. Below 2 K a power law (∼ T α , α = 1.36, 1.74 for different spectral peaks) prevails. Above 2 K a strong coupling to low-energy (5 and 9 cm −1 ) vibrational modes dominates. No indication of a low-temperature lock-in transition was found.

The dependence of frequency, width, and area of spectral holes on pressure were measured at 1.6 K in the pressure range up to 2.5 MPa for dimethyl-s-tetrazine (DMST) doped n-hexane (Shpol’skii system), and as reference systems, for DMST-doped durene (“hard” molecular crystal) and ethanol:methanol glass. For the Shpol’skii system, in addition the inhomogenous fluorescence spectra were measured for normal and high (200 MPa) pressures. The main observations were the following: (i) spectral holes in the Shpol’skii system exhibit very large pressure-induced broadening (up to 65 GHz/MPa) depending essentially on the prehistory (freezing pressure) and exceeding the corresponding values for durene (by far) and glass; (ii) spectral holes in the Shpol’skii system exhibit strong, and to a large extent, reversible, area reduction with applied pressure; and (iii) the inhomogeneous fluorescence lines show quite a moderate (as compared to holes) pressure broadening of about several GHz/MPa. The results for the Shpol’skii system are shown to be inconsistent with existing theories. They are qualitatively explained by pressure-induced dynamics of vacancy defects in the frozen n-alkanes.