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Low-temperature dynamics in a dye-doped polymer: correspondence between the data obtained by photon echo and single molecule spectroscopy

Каримуллин Камиль Равкатович, А. В. Наумов

Published Jan 1, 2018• 0 citations
Publisher

Abstract

Low temperature dynamics (tunneling and vibrational relaxation) in doped polyisobutylene film has been reinvestigated using 2-pulse incoherent photon echo (2IPE) and compared with single-molecule spectroscopy (SMS) data. It has been shown that in a very wide range of low temperatures the 2IPE gives optical dephasing times which correspond to the narrowest zero-phonon lines of single dye molecules.

DOI
10.1051/epjconf/201819004008

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Low temperature dynamics (tunneling and vibrational relaxation) in doped polyisobutylene film has been reinvestigated using 2-pulse incoherent photon echo (2IPE) and compared with single-molecule spectroscopy (SMS) data. It has been shown that in a very wide range of low temperatures the 2IPE gives optical dephasing times which correspond to the narrowest zero-phonon lines of single dye molecules.
The photon echo (PE) spectroscopy and single-molecule spectroscopy (SMS) may be combined to give a very powerful tool for comprehensive study of low-temperature dynamics in dye-doped disordered solids (polymers, glasses). At the same time, this type of studies are likely to reveal discrepancies when comparing characteristic times of optical dephasing T2 and single-molecule zero-phonon spectral lines (ZPL) broadening obtained from PE and SMS, correspondingly, for tetra-tert-butylterrylene in polyisobutylene in the temperature range of a few–dozen of Kelvins [see Phys. Status Solidi B 241, 3480 and 3487 (2004)]. Inexplicably, PE-experiments demonstrated T2-times to be much shorter than it is sufficient to cause the corresponding ZPL broadening. Here we experimentally solve this problem and show that at T = 4.5–15 K the incoherent PE gives T2-times which correspond to the narrowest SM ZPL. On the SM-level there is a pronounced additional ZPL-broadening due to spectral diffusion processes which are strongly dependent on the characteristics time of the measurement (tens of nanoseconds for PE and seconds for SMS). There is also a broad distribution of ZPL spectral widths for different SMs due to different local environments, that contribute differently to both the optical dephasing and the spectral diffusion processes, but always in addition to the value of inverse optical dephasing times measured using a PE technique.
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.
The temperature-dependent femtosecond dephasing of vibronic lines of a dye, Nile blue, doped in a polymer (polyvinyl alcohol) was studied by using an incoherent-photon-echo technique. It is, to our knowledge, the first detailed study on temperature-dependent dephasing for vibronic lines in a dye-doped polymer system. Photon echoes for the vibronic lines displayed an exponential decay with the dephasing times less than 100 fs, and the temperature dependence of the dephasing was found to follow a power law of T1.5{\mathit{T}}^{1.5}T1.5 in the temperature range from 9.5 to 130 K. By comparing the results with the behavior of the zero-phonon line, we discuss the effect of the interactions with so-called two-level tunneling system and phonons in the polymer host on the femtosecond dephasing of the vibronic lines.
Fourier-transform spectroscopy using the technique of femtosecond accumulated photon echo with incoherent light has been performed in dye-doped polymers. Several types of interference effect or quantum beat between the zero-phonon line and other spectral components including the phonon sideband, the vibronic lines, and the photoproduct state have been observed. Based on the density matrix incorporating the transition-frequency modulation, it is pointed out that the factorization approximation for the relaxation function holds rigorously in the accumulated photon echo. We also clarified that the Fourier cosine transform of the heterodyne-detected echo signal provides the hole-burning spectrum.
Subpicosecond photon echo quantum beats were studied in a dye, Rhodamine 800, doped in a polymer (polyvinyl alcohol) by using an incoherent photon echo technique. At the long-wavelength tail of absorption, photon echo quantum beats were observed as the sinusoidal modulation with the frequency of about 100 cm-1, which resulted from the interference between a single vibronic line and the zero-phonon line. The dephasing time of the vibronic line and its temperature dependence were briefly studied. At nearly the peak of absorption, the quantum beats appeared as more complicated modulation, indicating the contribution from multiple vibronic lines.