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Springer series in chemical physics

On the Role of Quantum Interference in the Free-Induction Decay from Wave-Packet Systems

John N. Sweetser, Thomas J. Dunn, Ian A. Walmsley

Published Jan 1, 1994• 0 citations
Publisher
DOI
10.1007/978-3-642-85176-6_32

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It is well known that the application of a pulse to a molecular electronic transition leaves the molecules vibrational modes in different electronic states in well-localized states, or wave packets[1]. One method of detecting the wave packets is via the time-dependent spectra of spontaneous emission from the excited molecule[2]. The emission consists in general of two parts, an incoherent part that depends only on the wave packet in the excited state, and a coherent part, that depends on the wave packets in both excited and ground electronic states (of a two-state molecule). This can be seen from the following simple calculation.
We present a time- and phase-resolved, background-free scheme to study the extreme ultraviolet dipole emission of a bound electronic wave packet, without the use of any extreme ultraviolet exciting pulse. Using multiphoton transitions, we populate a superposition of quantum states which coherently emit extreme ultraviolet radiation through free induction decay. This emission is probed and controlled, both in amplitude and phase, by a time-delayed infrared femtosecond pulse. We directly measure the laser-induced dephasing of the emission by using a simple heterodyne detection scheme based on two-source interferometry. This technique provides rich information about the interplay between the laser field and the Coulombic potential on the excited electron dynamics. Its background-free nature enables us to use a large range of gas pressures and to reveal the influence of collisions in the relaxation process.
A model molecular system composed of an inhomogeneous distribution of homogeneous wave packets is presented in analogy with gain saturation in atomic systems. The numerically computed optical free-induction-decay pulse spectrum (as a representative picosecond-pulsed laser system) and other idealized pulse spectra are used as inputs to the molecular system to probe its absorption characteristics in the inhomogeneous limit. Various aspects of pulse spectral structure and their relative significance to the observed nonlinearity of the numerically computed 1/σ2-versus-I plot is discussed in detail. The relevance of such behavior in interpreting experimental data is also indicated.