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Physical Review Letters

Photon-Echo Spectroscopy of Organic Mixed Crystals

Thijs J. Aartsma, Douwe A. Wiersma

Published Jun 7, 1976• 72 citations
Publisher

Abstract

We report the first observation of photon echoes in an organic mixed crystal. The echo was observed after excitation with a nitrogen-laser-pumped dye laser in the $^{1}B_{2\mathrm{u}}\ensuremath{\leftarrow}^{1}A_{g}$ electronic transition at 3739.9 \AA{} of pyrene in biphenyl at 2 K. The photon-echo excitation spectrum of the origin (zero-phonon line) region shows that drastic variations occur in the coherence lifetime of sites which, qua incoherent (fluorescent) decay, are indistinguishable.

DOI
10.1103/physrevlett.36.1360

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We report the first observation of photon echoes in an organic mixed crystal. The echo was observed after excitation with a nitrogen-laser-pumped dye laser in the 1B2u\ensuremath←1Ag^{1}B_{2\mathrm{u}}\ensuremath{\leftarrow}^{1}A_{g}1B2u​\ensuremath←1Ag​ electronic transition at 3739.9 \AA{} of pyrene in biphenyl at 2 K. The photon-echo excitation spectrum of the origin (zero-phonon line) region shows that drastic variations occur in the coherence lifetime of sites which, qua incoherent (fluorescent) decay, are indistinguishable.
The signals of both primary and stimulated femtosecond photon echoes are observed and investigated in a dye-doped polymer film at room temperature using a modernized femtosecond echo-spectrometer. It should be noted that stimulated photon echo in the solid-state sample is observed for the first time at such a high temperature. Experimentally obtained decay curves of these signals have a nonexponential character. The spectra of these echo signals are also measured. It is found that the spectrum of the primary photon echo is short-wave shifted with respect to the spectrum of excitation. This can be used for the coherent laser cooling of a sample. The spectrum of the stimulated photon echo is also shifted to the short-wave range relative to the spectrum of excitation, but its shift is much less than that of the primary photon echo. The experiment shows that the femtosecond echo signals at room temperature are excited via the phonon-side band of the absorption line.
The first observation is reported of the primary and stimulated femtosecond photon echoes at liquid nitrogen and room temperatures in a dye-doped polymer film at a wavelength of 780 nm. Echo signals were generated by pulses with the duration of 130 fs. The primary echo signal decay at a liquid nitrogen temperature can not be described by a simple exponential function. There is a fast decay region below 250-300 fs and a slow decay region at longer time intervals. The decay of primary echo signal at room temperature demonstrates complex behavior caused by the presence of the phonon-side band in the optical band of impurity centers. There were also detected signals of the self-diffraction of exciting pulses on a nonequilibrium population difference grating, induced in resonant medium by these pulses.
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.
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.
We have used the phenomenon of laser-induced molecular photodissociation to determine the homogeneous linewidth at 2 K of the origin (zero-phonon line) and a vibronic transition in the mixed-crystal absorption spectrum of dimethyl sss-tetrazine in durene. From the measured 55-MHz (upper limit) homogeneous width of the origin we conclude that in the vibrationless excited state coherence persists at least during the 6-nsec lifetime. The 29-GHz homogeneous vibronic linewidth is ascribed to vibrational relaxation.
The first observation is reported of the primary femtosecond photon echo at a liquid nitrogen temperature in a dye-doped polymer film at a wavelength of 780 nm. Echo signals were generated by pulses with the duration of 130 fs. The echo signal decay can not be described by a simple exponential function. There is a fast decay region below 250-300 fs and a slow decay region at longer time intervals. There were also detected signals of the self-diffraction of exciting pulses on a nonequilibrium population difference grating, induced in resonant medium by these pulses.