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AIP conference proceedings

Incoherent photon echoes with femtosecond time resolution: Principles and applications for studies of low temperature dynamics in amorphous solids

Yu. G. Vainer, Roman I. Personov

Published Jan 1, 1996• 0 citations
Publisher

Abstract

The principles of incoherent photon echoes (IPE) are shortly recalled. The results on dynamics in doped organic glasses and polymers (resorufin in d‐ and d6‐ethanol and terrylene in polyethylene) studied by IPE are presented. In all cases the fast dephasing processes are related to coupling with both two‐level systems (TLS) and pseudolocal mode. The nanosecond spectral diffusion (SD) processes has been observed. The IPE‐results are compared with hole‐burning and single molecule spectroscopy (SMS) data.

DOI
10.1063/1.50185

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Ultrafast Dephasing of Organic Glasses in Wide Temperature Region Investigated by Incoherent Photon-Echo: Resorufin/D- and D6-Ethanol.

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Until now, in spite of a great number of experimental and theoretical works in study of organic amorphous solids, the basic features of the low temperature dynamics of these mediums are poorly understood. One of the main reason of this is the lack of experimental information about these dynamical processes. In particular, it’s necessary to learn more about optical dephasing in doped organic glasses and polymers for wider temperature interval. It will allow to test the existent theories more correctly and to create new conceptions.

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PHOTON-ECHO STUDY OF ULTRAFAST DEPHASING IN AMORPHOUS SOLIDS IN WIDE TEMPERATURE REGION WITH INCOHERENT LIGHT

N.V. Gruzdev, Силькис Эммануил Гершович, V. D. Titov +1 more

The temperature-dependence of the electronic dephasing for resorufin in d-ethanol glass was measured from 1.7 to 35 K by incoherent photon echo. The difference between two-pulse picosecond photon echo and incoherent photon echo results was obtained and attributed to spectral diffusion in nanosecond time scale.

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Picosecond photon echo (PE) experiments are used to examine the optical dephasing and intermolecular interactions of organic chromophores in a variety of glassy organic and polymer hosts. The inherent disorder in these systems leads to dynamics which span times from picoseconds to hours and longer. The temperature dependent optical dephasing as measured by the PE follows a power law characteristic of tunnelling twolevel systems (TLS) at low temperatures (1 °K to 4 °K) and is exponentially activated at higher temperatures due to dephasing by additional modes. The nature of these modes will be addressed. These data and those from other line narrowing experiments such as hole burning allow the study both of fast dephasing processes and spectral diffusion due to slow fluctuations in the host. The observed lineshapes and holewidths require dipolar coupling between the chromophore and TLS and offer information on the distribution of relaxation rates. Furthermore, techniques sensitive to different timescales are used to examine host dynamics by removing the guest-host coupling from consideration. The data are discussed in conjunction with recently developed theoretical treatments of dephasing in disordered systems.

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Revisiting the combined photon echo and single-molecule studies of low-temperature dynamics in a dye-doped polymer

Mikhail Knyazev, Каримуллин Камиль Равкатович, А. В. Наумов

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.

physica status solidi (RRL) - Rapid Research Letters•Feb 14, 2017•25 citations
The principles of incoherent photon echoes (IPE) are shortly recalled. The results on dynamics in doped organic glasses and polymers (resorufin in d‐ and d6‐ethanol and terrylene in polyethylene) studied by IPE are presented. In all cases the fast dephasing processes are related to coupling with both two‐level systems (TLS) and pseudolocal mode. The nanosecond spectral diffusion (SD) processes has been observed. The IPE‐results are compared with hole‐burning and single molecule spectroscopy (SMS) data.
Until now, in spite of a great number of experimental and theoretical works in study of organic amorphous solids, the basic features of the low temperature dynamics of these mediums are poorly understood. One of the main reason of this is the lack of experimental information about these dynamical processes. In particular, it’s necessary to learn more about optical dephasing in doped organic glasses and polymers for wider temperature interval. It will allow to test the existent theories more correctly and to create new conceptions.
The temperature dependence of the electronic dephasing of Resorufin in d-ethanol glass was measured from 1.7 to 40 K by incoherent photon echo (IPE) techniques. At T = 8–11 K good agreement between IPE and two-pulse picosecond photon echo (PPE) results was observed. For T < 8 K, PPE and IPE results differed; the difference is attributed to spectral diffusion on a nanosecond time scale. IPE results for T > 11 K confirm the hypothesis that high-temperature dephasing in this system is due mainly to interaction with a pseudolocal mode.
The long-lived stimulated photon echo is put forward as a powerful technique to probe structural dynamics in glasses and other amorphous solids. We present results of optical dephasing measurements on several doped organic glasses (deuterated ethanol, toluene, and triethylamine) and polymers (polystyrene, polyvinylbutyral, and polymethylmethacrylate). Using a stochastic analysis within the so-called two-level-system model, we can extract from these measurements the distribution function of fluctuation rates over a huge range of time scales, varying from picoseconds to hundreds of milliseconds. We show that the dynamics, which lies at the origin of spectral diffusion, is very dependent on the glass structure and can be described by two separate hyperbolic distribution functions of fluctuation rates. From longitudinal photon echo measurements in the population dimension, we find evidence for structural dynamics which is not accounted for in the standard two-level-system model and which is related to a spatially inhomogeneous distribution of fluctuation centers.
Picosecond photon echo (PE) experiments are used to examine the optical dephasing and intermolecular interactions of organic chromophores in a variety of glassy organic and polymer hosts. The inherent disorder in these systems leads to dynamics which span times from picoseconds to hours and longer. The temperature dependent optical dephasing as measured by the PE follows a power law characteristic of tunnelling twolevel systems (TLS) at low temperatures (1 °K to 4 °K) and is exponentially activated at higher temperatures due to dephasing by additional modes. The nature of these modes will be addressed. These data and those from other line narrowing experiments such as hole burning allow the study both of fast dephasing processes and spectral diffusion due to slow fluctuations in the host. The observed lineshapes and holewidths require dipolar coupling between the chromophore and TLS and offer information on the distribution of relaxation rates. Furthermore, techniques sensitive to different timescales are used to examine host dynamics by removing the guest-host coupling from consideration. The data are discussed in conjunction with recently developed theoretical treatments of dephasing in disordered systems.
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.