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International Conference on Ultrafast Phenomena

Picosecond Photon Echo Studies of Mixed Molecular Solids at High Pressure

Eric L. Chronister

Published Jan 1, 1994• 0 citations
Publisher

Abstract

High pressure photon echo results are presented for pentacene doped naphthalene, pentacene doped (triclinic and monoclinic) p-terphenyl, and rhodamine doped PMMA. Figure 1 illustrates typical photon echo intensity decays in a high pressure diamond anvil cell at variable low temperatures. The effect of pressure and temperature on the homogeneous dephasing is used to characterize the interactions between the impurity molecule and the host crystal, as well as provide a unique probe of local polymorphic phase changes.

DOI
10.1364/up.1994.tud.28

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Optics and Spectroscopy•May 1, 2005•1 citation
High pressure photon echo results are presented for pentacene doped naphthalene, pentacene doped (triclinic and monoclinic) p-terphenyl, and rhodamine doped PMMA. Figure 1 illustrates typical photon echo intensity decays in a high pressure diamond anvil cell at variable low temperatures. The effect of pressure and temperature on the homogeneous dephasing is used to characterize the interactions between the impurity molecule and the host crystal, as well as provide a unique probe of local polymorphic phase changes.
Abstract Photon echo decay time is measured for pentacence molecules introduced in naphthalene and p-terphenyl crystals with rather high concentrations (10−6–105 mol/mol) at temperatures between 1.6 K and 4.1 K, using a tunable picosecond laser system consisting of a mode-locked YAG laser and a parametric oscillator. In naphthalene echo decay time increases with lowering temperature approaching a constant value below 2 K, but in p-terphenyl it is almost constant. The phase relaxation time at very low temperature is much shorter than twice the population relaxation time in both crystals, indicating that pure dephasing processes exist. Analyzing the results it turns out that there exsists a pure dephasing process which is temperature-independent and is very probably due to interactions between pentacene molecules, in addition to the temperature-dependent dephasing process due to the scattering of pseudolocalized phonons.
Pressure- and temperature-dependent photon echo results are obtained for pentacene doped polymethyl methacrylate (PMMA). A unique pressure effect is observed in which the optical dephasing rate increases as the pressure is increased from ambient pressure to 4 kbar, above which the optical dephasing rate is pressure independent up to 43 kbar. The present results are also compared with pressure- and temperature-dependent photon echo results for rhodamine 101 in PMMA, in which the optical dephasing rate was completely insensitive to pressure over the range 0 to 30 kbar. A negative correlation is also observed between the optical dephasing rate and the spectral hole burning efficiency. Line broadening due to pressure induced spectral diffusion may be responsible for both the increased dephasing rate and the reduced spectral hole-burning at high pressure.
Picosecond optical coherence techniques are employed to study dynamical intermolecular interactions in low concentration mixed molecular crystals, i.e., pentacene in naphthalene at 1.4 K. A concentration-dependent broadening of the optical homogeneous line is observed. Stimulated photon echo measurements rule out excited state transport as the broadening mechanism. The photon echo results exhibit a linear concentration dependence and a theory is proposed that accounts for the broadening in terms of phonon-induced fluctuations in guest–guest dipole–dipole interactions. Detailed considerations indicate that the system is best described in terms of localized excitations rather than delocalized impurity band states. In the low concentration limit, there is additional broadening of the homogeneous line beyond that produced by the lifetime. A model is presented describing this broadening in terms of phonon-induced modulation of the guest–host van der Waals interactions, i.e., in terms of a fluctuating crystal shift.
Picosecond photon echo experiments on pentacene in polymethylmethacrylate (PMMA) show that the homogeneous width exhibits a T1.3 temperature dependence. This behavior is ascribed to coupling of the pentacene transition to randomly distributed low-frequency excitations in the amorphous host. A calculation of the resulting homogeneous width is presented which uses optical Redfield theory as a starting point. From the results of this calculation we conclude that the coupling between the pentacene molecule and the host low frequency excitations is of static dipolar nature and that the density of states of these excitations varies as ω0.3. Results of nonphotochemical hole-burning experiments on the same system are also reported. Comparison of these results with the ones obtained by the photon echo method indicates, that in the hole-burning experiments, the hole width and its temperature-induced broadening are dominated by spectral diffusion.
The effects of optical density (OD) on photon echo experiments is examined both theoretically and experimentally. The theoretical treatment involves coupled Maxwell-Optical Bloch equations, and the experiments are picosecond photon echo studies of the mixed molecular crystal, pentacene in naphthalene. Under high power excitation (π/2, π) in high OD samples, the echo decays are predicted and observed to be faster than decays arising solely from the intrinsic molecular T2. The increase in the echo decay rate vanishes in the limit of low power or low OD, permitting the intrinsic molecular T2 to be measured. Previously reported concentration effects are shown to actually be optical density effects. The experimentally determined intrinsic molecular T2 of pentacene in naphthalene is shown to be independent of concentration and temperature (below ∼2 K) and T2≠2T1. It is suggested that the difference between T2 and 2T1 is due to the static multiplet level structure arising from the electronic state-phonon coupling.
A high-pressure photon echo study of the low-temperature dynamics of rhodamine 640 in a 2-methyltetrahydrofuran (2-MTHF) molecular glass is reported. High pressure is found to decrease the homogeneous dephasing rate comparably to the volume compression ratio. The pressured-induced line narrowing is also qualitatively similar to high-pressure hole burning results reported for a 2-MTHF glass doped with bacteriochlorophyll a . The results are consistent with a pressure-induced decrease in the number of tunneling two-level systems (TLSs) that may be associated with collapsible void space in the molecular glass. Comparable high-pressure photon echo studies of organic polymer glasses over the same low-temperature range do not show line narrowing at high pressure, suggesting an intrinsic difference in the nature of TLSs for molecular versus polymer glasses.