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The Journal of Physical Chemistry A

Transient Phenomena in Time- and Frequency-Gated Spontaneous Emission

Maxim F. Gelin, Dassia Egorova, Andrei V. Pisliakov, Wolfgang Domcke

Published Apr 1, 2005• 8 citations
Publisher

Abstract

The effect of overlapping pump and gate pulses on time- and frequency-gated spontaneous emission spectra is explored for a model of material dynamics that accounts for strong nonadiabatic and electron-vibrational coupling effects, vibrational relaxation, and optical dephasing, thus representing characteristic features of photoinduced excited-state dynamics in large molecules in the gas phase or in condensed phases. The behaviors of the sequential, coherent, and doorway-window contributions to the spontaneous emission spectrum are studied separately. The interrelation between the sequential and coherent contributions is demonstrated to be sensitive to the carrier frequencies of the pump and gate pulses and also to the optical dephasing rate, opening the possibility of an experimental determination of the latter. The coherent contribution is shown to dominate the spectrum at specific emission frequencies.

DOI
10.1021/jp044463t

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The effect of overlapping pump and gate pulses on time- and frequency-gated spontaneous emission spectra is explored for a model of material dynamics that accounts for strong nonadiabatic and electron-vibrational coupling effects, vibrational relaxation, and optical dephasing, thus representing characteristic features of photoinduced excited-state dynamics in large molecules in the gas phase or in condensed phases. The behaviors of the sequential, coherent, and doorway-window contributions to the spontaneous emission spectrum are studied separately. The interrelation between the sequential and coherent contributions is demonstrated to be sensitive to the carrier frequencies of the pump and gate pulses and also to the optical dephasing rate, opening the possibility of an experimental determination of the latter. The coherent contribution is shown to dominate the spectrum at specific emission frequencies.
The theory of time- and frequency-gated (TFG) spontaneous emission (SE) spectra is elaborated. The present formulation generalizes previous derivations, clarifies the interrelations between different existing expressions, and establishes the validity of certain commonly assumed approximations. We obtain various explicit expressions for TFG SE spectra, which are suitable for performing actual calculations for nontrivial systems and which allow us to establish generic (that is, model-independent) properties of TFG spectra. The doorway-window picture of temporally and spectrally resolved spectra is further developed. It is shown that, to the leading order in the pump and probe pulses, the TFG SE signal is equivalent to the stimulated-emission contribution to the integral pump-probe spectrum in the case of nonoverlapping pulses. The theory is illustrated for the example of an electronic two-level system with a single Condon-active harmonic vibrational mode that is coupled to a thermal bath. The effect of imperfect time and frequency resolution is studied. It is pointed out that the TFG SE spectrum carries information not only on the strength of the system-bath coupling, but also on the relative magnitude of the bath correlation time.
Several nonlinear optical phenomena are described exactly for two-level electronic systems with a Gaussian frequency modulation under a pump field of arbitrary strength. We discuss the emission spectrum and the absorption spectrum of weak probe field under pumping in the frequency region, and the free induction decay (FID) and the optical nutation (ON) as examples of the coherent optical transients in the time region. It is shown that the relaxation behavior depends upon the pumping field intensity, i.e., the effect of the frequency modulations is reduced when the Rabi frequency increases beyond the amplitude or the inverse correlation time of the frequency modulation. We further show that the relaxation behavior depends upon the particular nonlinear optical phenomena, i.e., the vertex correction due to the frequency modulation works in the FID but does not in the ON.
Abstract The quantum dynamics of a system of Rb atoms, modeled by a V -type three-level system interacting with intense probe and pump pulses, are studied. The time-delay-dependent transient-absorption spectrum of an intense probe pulse is thus predicted, simulating pump-probe experiments in which this is preceded or followed by a strong pump pulse. Numerical results are interpreted in terms of an analytical model based on interaction operators , which quantify the transformation undergone by the system under the action of an intense pulse. The oscillating features of the resulting transient-absorption spectra, due to the coupling of several excited states, are thus interpreted in terms of the atomic population and phase changes imposed by the pump and probe pulses. Strong-field-induced phases and their influence on the resulting transient-absorption spectra are thereby investigated for different values of pump and probe intensities and frequencies, focusing on the atomic properties which are encoded in the absorption line shapes for positive and negative time delays.
We have extended the doorway-window representation of optical pump-probe spectroscopy with weak pulses toward N-wave-mixing spectroscopy with temporally well-separated pulses of arbitrary strength. The expressions for the signals in the strong-pulse doorway-window representation are derived in the framework of the nonperturbative theory of N-wave-mixing spectroscopy. The strong-pulse doorway-window representation is complementary to the equation-of-motion phase-matching approach. The latter fully accounts for pulse-overlap effects in signals induced by weak pulses but is computationally more expensive. The performance of the doorway-window approximation for temporally well-separated strong pulses is illustrated for an electronic two-level system with an underdamped Condon-active vibrational mode.
The spectra of spontaneous emission accompanying the generation of femtosecond superradiant pulses in GaAs/AlGaAs heterostructures are studied. It is clearly demonstrated that spontaneous emission spectra of electron–hole pairs, which have been left in the semiconductor after the formation of a coherent collective e–h state, correspond to the strong overheating of carriers. This phenomenon can be explained by the effect of dynamic cooling and nonequilibrium condensation of collectively paired carriers at the bottoms of the bands during the superradiant emission, which was observed earlier.