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Journal of Physics B Atomic and Molecular Physics

On a model for multiphoton excitation of molecules in a strong laser field

J. Leo van Hemmen, Kazimierz Rza̧żewski

Published Dec 28, 1982• 1 citation
Publisher

Abstract

An exactly soluble model is presented for calculating the mean density matrix of a charged harmonic oscillator in the field of a multimode, high-power laser. Possible applications include multiphoton excitation of the vibrational degrees of freedom of a molecule, dissociation, and the excitation of optical modes in a crystal by chaotic laser light.

DOI
10.1088/0022-3700/15/24/005

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Journal of Physics B Atomic and Molecular Physics•Sep 4, 1982•38 citations
An exactly soluble model is presented for calculating the mean density matrix of a charged harmonic oscillator in the field of a multimode, high-power laser. Possible applications include multiphoton excitation of the vibrational degrees of freedom of a molecule, dissociation, and the excitation of optical modes in a crystal by chaotic laser light.
Harmonic-generation processes at high laser intensity are strongly affected by resonant multiphoton ionization. In this paper coexistence of these phenomena at low pressure and high intensity is taken into account with use of a mean-field theory. New consequences of this model are derived, especially for resonances strongly damped by ionization. Available experimental data on mercury agree qualitatively with this model. A second approach, called the quasistatic approximation, is used to get analytical solutions for mean-field equations, in good agreement with numerical results. Furthermore, possible applications of the quasistatic approximation to the study of harmonic generation at both high pressure and high laser intensity are mentioned.
We consider harmonics generation and wave mixing by two-color multiphoton resonant excitation of three-level atoms and molecules in strong laser fields. The coherent part of the spectra corresponding to multicolor harmonics generation is investigated. The obtained analytical results on the basis of a generalized rotating wave approximation are in a good agreement with numerical calculations. The results applied to the hydrogen atoms and homonuclear diatomic molecular ions show that one can achieve efficient generation of moderately high multicolor harmonics via multiphoton resonant excitation by appropriate laser pulses.
Multiphoton spectroscopy The subject of multiphoton excitation spectroscopy began in 1931 when Göppert-Mayer [450] wrote a theoretical paper in which she calculated the transition rate for an atom in the presence of two photons rather than just one. At the time, the process seemed rather exotic, and it was reassuring that the calculated rate was so low as to guarantee that it could not readily be observed in the laboratory with conventional sources. This conclusion was reassuring because it implies that a simple perturbative theory (one photon per transition is the weak-field limit) is adequate for most purposes. The subject came to life with the advent of lasers, when it became easy to create intense beams of light. Since the probability of excitation by two photons grows as the square of the photon density, whereas the probability of single-photon excitation grows only linearly with photon density, two-photon transitions gain in relative strength with increasing intensity despite the small value of the rate coefficient. The development of multiphoton spectroscopy has followed that of lasers: as the available power has increased, so has the number of photons involved in individual transitions. More significantly, it has become apparent that the physics of the interaction between radiation and matter is not the same at high laser powers as under weak illumination, i.e. that there is a qualitative change which sets in at strong laser fields. This is normally expressed by saying that perturbative approximations break down.
Multiphoton excitation and dissociation of large molecules under collisionless conditions is discussed in terms of an intercontinuum random coupling model. The mathematical approach described in a previous paper is used to obtain the general solution for a system of consecutively coupled discrete states, quasicontinuous manifolds, and continuous (dissociative) manifolds of molecular levels (eigenstates of the total molecular Hamiltonian), where the radiative coupling matrix elements are assumed to be given as a linear combination of smoothly varying and randomly varying (over level indices in the molecular manifolds) components. In the range of discrete molecular levels the time evolution is coherent and described in terms of the optical Bloch equation. In the quasicontinuous and continuous ranges the time evolution may be described in terms of Markoffian kinetic equations for the number of photons absorbed by the molecule, provided that the intramolecular vibrational relaxation widths associated with the optically active molecular modes is much larger than the Rabi frequency associated with the excitation of these modes. The kinetic evolution itself consists of direct multiphoton excitation processes (simultaneous transitions from the upper discrete levels to all higher energy molecular manifolds) resulting from the smooth component in the radiative coupling, and a consecutive excitation process described by the Pauli master equation with rates given by the golden rule expression. The interaction which enters into the golden rule expression is the variance in the radiative coupling. The direct excitation component contributes a negligible part of the overall excitation even if the random and smooth radiative coupling components are comparable. The resulting incoherent time evolution of the multiphoton excitation process is consistent with available experimental results. Coherent effects in the time evolution are expected for higher radiation field intensities, where the Rabi frequency becomes comparable to the intramolecular vibrational relaxation rate.
The author presents a theory of resonant multiphoton ionisation by multimode laser light. He investigates N photon resonant N+1 photon ionisation for a high order bound-bound transition with the resonance dominated by the Stark shift. Two aspects of the problem are considered. He studies the bandwidth dependence for the resonant ionisation probability, approximating the multimode laser light by a chaotic field. Secondly, he investigates the effects of finite mode numbers of the multimode laser. Finally, the theory is compared with the recent experimental results of Lompre et al (1981).