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Optics and Spectroscopy

Infinite motion of a wave packet in a system of crossing electronic terms upon pulsed resonance excitation

И. М. Уманский, L. D. Ievleva

Published Jul 1, 1995• 0 citations
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Journal of Experimental and Theoretical Physics•Sep 1, 1975•0 citations
The resonance secondary emission (RSE) in femtosecond laser excitation is discussed in reference to the motion of the created wave packet moving on the excited state potential surface. The density matrix of emitted light for the multi-intermediate-level system is outlined, from which the emission correlation function is derived. The correlation function is put into the theoretical expression of the time-dependent ‘‘physical spectrum’’ for the Fabry–Perot interferometer (which is used in order to consider temporal and energetic resolution inherent in detection). The compact and practical expressions obtained connect the time- and frequency-resolved spectrum with the time evolution of the wave packet. Numerical results for a displaced harmonic oscillator model indicate that the time- and frequency-resolved spectrum can reveal how the wave packet created by a fs laser pulse travels on the excited potential surface if the response time 1/Γd of the photodetector satisfies the relation that Ω<Γd <∼ the Stokes shift (where Ω is the vibrational frequency). It is shown that the excited state wave function can be split into two terms, the one that adiabatically follows the temporal change in incident light (the adiabatic term) and the one that represents the effect of spectral broadening of light (the Fourier broadening term). It is only the Fourier broadening term that survives after the termination of incident light and reflects the motion of the created wave packet on the excited potential surface. In off-resonance excitation, the adiabatic term produces Raman-like emission and the Fourier broadening one produces fluorescence-like emission. In resonance excitation, these two terms are indistinguishable from each other with respect to emission frequency: for the duration of incident light, the adiabatic term offsets the Fourier broadening one, leading to a slow buildup of intensity in the time- and frequency-resolved spectrum (which is slower than the initial rise of the incident pulse profile).
Quantum wave packet engineering is demonstrated using a phase-programmable femtosecond optical source. This paper describes development of a programmable phase modulator and coherent control of quantum wave packets. Wave packet motion in a cyanine dye molecule is observed to be dependent on the chirp direction and rate of excitation pulses. Strong reduction in excited state population is efficient for negatively chirped pulses in the cyanine dye molecule, which is explained in terms of a pump-dump process. We discuss a possibility of mutual conversion between the optical and electronic phase information by means of nonlinear light-matter interaction.
The paper first discusses theoretically the off-resonance selective excitation method that is dependent on the atomic internal states and used to generate approximately a standard coherent state of harmonic oscillator. The coherent average method then is proposed to construct the state-selective trigger pulse. A state-selective trigger pulse can keep Gaussian shape unchanged but change in an internal-state-dependent form the center-of-mass position and/or momentum of an atomic Gaussian wave-packet motional state. A Gaussian wave-packet state is one of the simplest wave-packet states that can be easily manipulated and controlled in time and space. The paper also investigates how to manipulate in time and space an atomic Gaussian wave-packet motional state by a generalized quadratic potential field. A general quadratic Hamiltonian can affect not only the center-of-mass position and momentum but also the complex linewidth of a Gaussian wave-packet motional state while keep Gaussian shape of the motional state unchanged. It is shown that generally quadratic terms of a quadratic Hamiltonian can control directly the complex linewidth, while linear terms of a quadratic Hamiltonian can affect only the center-of-mass position and momentum of a Gaussian wave-packet motional state.