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Optics and Spectroscopy

Photon echo in amorphous media under conditions of significant dispersion of homogeneous linewidths of impurity centers

Yu. G. Vainer, Roman I. Personov

Published Nov 1, 1995• 2 citations
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The concept of the homogeneous spectral linewidth of an impurity center is more complicated in disordered media such as organic glasses and polymers than it is in crystals. In amorphous media the local environments for impurity centers are continuously changing with time. As a result transition frequencies of individual centers diffuse within the inhomogeneous broadened spectral contour, which is called spectral diffusion. When the timescale for spectral diffusion processes is much longer than the dephasing time, it is possible to distinguish homogeneous dephasing from spectral diffusion. On the other hand, when the timescales of spectral diffusion and dephasing processes are comparable these phenomena become indistinguishable.

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Soft-potential model and homogeneous width of spectral lines of impurity centers in molecular amorphous media

Yu. G. Vainer, M. A. Kol’chenko, Roman I. Personov

A study is made to analyze the possibility of using the soft-potential model in optical investigations of disordered molecular systems with impurities. A procedure is suggested for calculating the temperature dependence of the homogeneous width of a phononless line in amorphous media with impurities within the soft-potential model. A calculation is performed of the temperature dependence of the width of a phononless line (optical dephasing) in an amorphous system of polymethyl methacrylate (PMMA) with an addition of tetratert-butylterrylene (TBT) using the parameters of this system known from the literature. Calculations are performed of the contributions to the width of a phononless line due to the interaction of an impurity with tunneling two-level systems, with thermally activated barrier crossings in double-well potentials, and with quasilocal modes of the matrix. The model calculation results are compared with the experimental data on the photon echo for TBT/PMMA, measured by us in the temperature range from 0.3 to 20 K. It is found that the soft-potential model describes qualitatively correctly the temperature behavior of the homogeneous width of a phononless line. In the temperature range of T < 2 K, where the main contribution to optical dephasing is associated with tunneling two-level systems, the predicted values of phononless line width agree well with the experimental data. At higher temperatures, some difference is observed between the prediction and experimental data, which may be due to the effect of impurity on the formation of quasilocal oscillation of the matrix.

Journal of Experimental and Theoretical Physics•Apr 1, 2001•1 citation

Fast Dephasing in Glasses Induced by Tunneling States and Local Modes

Stephan J. Zilker, D. Haarer, Yuri G. Vainer +3 more

We present a comprehensive investigation of fast line broadening processes in two amorphous polymers, polymethylmethacrylate and polyisobutylene. Using a combination of two-pulse and incoherent photon echo spectroscopy, we have studied the homogeneous linewidth of embedded impurity molecules in a wide temperature range, namely 0.4–22 K. Thus, we are able to separate clearly between the two active dephasing mechanisms, two-level systems and low-frequency modes.

Molecular crystals and liquid crystals science technology. Section A, Molecular crystals and liquid crystals/Molecular crystals and liquid crystals science and technology. Section A, Molecular crystals and liquid crystals•May 1, 1998•0 citations
The concept of the homogeneous spectral linewidth of an impurity center is more complicated in disordered media such as organic glasses and polymers than it is in crystals. In amorphous media the local environments for impurity centers are continuously changing with time. As a result transition frequencies of individual centers diffuse within the inhomogeneous broadened spectral contour, which is called spectral diffusion. When the timescale for spectral diffusion processes is much longer than the dephasing time, it is possible to distinguish homogeneous dephasing from spectral diffusion. On the other hand, when the timescales of spectral diffusion and dephasing processes are comparable these phenomena become indistinguishable.
A study is made to analyze the possibility of using the soft-potential model in optical investigations of disordered molecular systems with impurities. A procedure is suggested for calculating the temperature dependence of the homogeneous width of a phononless line in amorphous media with impurities within the soft-potential model. A calculation is performed of the temperature dependence of the width of a phononless line (optical dephasing) in an amorphous system of polymethyl methacrylate (PMMA) with an addition of tetratert-butylterrylene (TBT) using the parameters of this system known from the literature. Calculations are performed of the contributions to the width of a phononless line due to the interaction of an impurity with tunneling two-level systems, with thermally activated barrier crossings in double-well potentials, and with quasilocal modes of the matrix. The model calculation results are compared with the experimental data on the photon echo for TBT/PMMA, measured by us in the temperature range from 0.3 to 20 K. It is found that the soft-potential model describes qualitatively correctly the temperature behavior of the homogeneous width of a phononless line. In the temperature range of T < 2 K, where the main contribution to optical dephasing is associated with tunneling two-level systems, the predicted values of phononless line width agree well with the experimental data. At higher temperatures, some difference is observed between the prediction and experimental data, which may be due to the effect of impurity on the formation of quasilocal oscillation of the matrix.