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Soviet Journal of Quantum Electronics

Two-photon transition in a colliding particle system

Pavel A Apanasevich, Alexander P. Nizovtsev

Published Mar 31, 1979• 1 citation
Publisher

Abstract

The first analysis is made of stimulated Raman scattering and two-photon absorption (emission) processes resulting in a change in the states of two colliding particles. These processes are caused the by interaction between dipole moments induced as a result of polarization of the particles by the radiation. Equations are derived to describe multiphoton transitions during a collision between two particles in a radiation field. Using the approximation of rectilinear trajectories, expressions are derived and analyzed for the cross section of collisional two-photon transitions in weak and strong fields. It is shown that in fields of ≈103 cgs esu, the cross section of these transitions may reach 10–4 cm2

DOI
10.1070/qe1979v009n03abeh008852

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The first analysis is made of stimulated Raman scattering and two-photon absorption (emission) processes resulting in a change in the states of two colliding particles. These processes are caused the by interaction between dipole moments induced as a result of polarization of the particles by the radiation. Equations are derived to describe multiphoton transitions during a collision between two particles in a radiation field. Using the approximation of rectilinear trajectories, expressions are derived and analyzed for the cross section of collisional two-photon transitions in weak and strong fields. It is shown that in fields of ≈103 cgs esu, the cross section of these transitions may reach 10–4 cm2
Semiclassical expressions of two-photon ionization of atoms induced by radiative collisions are derived. The dependence of the ionization yield on the atomic forces, field intensity, and energy gap is derived. Although absorption tends to decrease as the field intensity rises due to stimulated emission at the second crossing, the two-photon ionization yield can be nearly saturated at the first crossing, thus enhancing the absorption. Both regions, ionization in single collisions and ionization between collisions, are treated. In the latter we find that saturation of the ionization can be achieved at much reduced intensities. This process promises an extremely sensitive method for studying radiative collisions, especially when absorption or fluorescence becomes extremely weak.
A set of coupled equations for the particle scattering by a two level atom in a strong near resonant radiation field is derived from the time dependent Schrodinger equation. This set of equations is discussed in a first and second order approximation. The result can be visualized in terms of a scheme in which the two well separated (nondegenerate) atomic states split, each into two energy levels. The splitting depends on the strength of the field and on the difference between the resonance frequency and the frequency of the incident light and is typically a few meV. In this scheme all possible elastic, quasielastic, inelastic and superelastic transitions between the four levels can be induced by collision processes. In addition, multiphoton processes may occur if the scattered particle remains long enough in the interaction region. Estimates of the two photon gain process for electron and heavy particle scattering by sodium atoms in a dye laser field are given. It is suggested that the superelastic processes may play an important role in laser induced gas breakdown, even if the laser frequency does not coincide with any atomic transition. Spontaneous emission of atoms in laser fields is also treated. The results are similar to the particle scattering processes.
The collision-induced absorption and emission coefficients for electric-dipole forbidden atomic transitions are calculated for weak radiation fields. The approximations used are valid for $\ensuremath{\hbar}\ensuremath{\omega}$ near $\ensuremath{\hbar}{\ensuremath{\omega}}_{0}$, the atomic energy differences. The example case of $S\ensuremath{-}D$ transitions induced by a spherically symmetric perturber (e.g., a noble-gas atom) is treated in detail and compared to measurements. The case of "radiative collisions," in which both colliding atoms change their state, is included in the theory and is also compared to experiment.
Radiation can change the energy state of matter via three optical processes: spontaneous emission, absorption and stimulated emission. In spontaneous emission, an excited atomic or molecular state decays to a lower energy state with the emission of a photon of energy equal to the difference in the quantum state energies. Photon absorption is the reverse process, with a photon causing excitation from a lower to an excited quantum state. Stimulated emission was first proposed by Einstein in a paper published in 1917. He attempted to balance spontaneous emission and photon absorption, but could not get the correct balance without the postulated process of stimulated emission (see Section 4.2). With stimulated emission, an excited quantum state is stimulated to decay to a lower quantum state by an impinging photon. The existing photon survives with another identical photon being created (so that energy is conserved). The rates at which radiative transitions occur can be calculated using quantum mechanics. The time-dependent Schrodinger equation is used with the system wavefunction comprising time-varying linear combinations of the two wavefunctions for the lower and upper quantum states. In semi-classical treatments, an atom is treated quantum mechanically with the radiation field treated classically. There is a perturbation in energy associated with, say, the electric field of the radiation interacting with the electric dipole of the atom, though other interactions can be significant if the electric dipole interaction energy is small. In absorption, for example, a differential equation representing the change in ‘weighting’ of the wavefunction from the lower to upper state is obtained. A ‘time constant’ for the speed of change represents the rate of the radiative process. We examine the quantum mechanical nature of radiation absorption in Section 10.1 before discussing (Section 10.3) another important parameter arising with radiative transitions between discrete bound quantum states: the lineshape function. Quantum Theory of the Atom–Radiation Interaction An expression for the Einstein B-coefficient for photo-absorption is derived using quantum mechanics in this section. Einstein determined the detailed balance relationship between the rates of spontaneous emission, photo-absorption and stimulated emission when light interacts with an atom by considering an atomic system of two energy levels which are in equilibrium with a black-body radiation field. We use a semi-classical treatment where the atom is treated quantum mechanically and the radiation field is treated as a classical oscillating electric field.
Investigates theoretically a new aspect of radiative collisions on two-photon ionisation of colliding atoms of different species A and B. The authors derive the main characteristics of the resonance appearing in the two-photon ionisation cross section of atom B when the laser frequency is tuned on a resonance transition of atom A which cannot itself be ionised by two-photon absorption. Under some realistic conditions and for reasonable values of the light energy density flux F ( approximately 1 MW cm -2 ), the cross section of the process considered varies as F 2/5 while its width varies as F 1/2 . These predictions are in reasonable agreement with a recent observation on the mixture Sr(A)-Cs(B) by Brechignac et al. (1980).
Abstract The quantum electrodynamic theory, based on the quantization of the electromagnetic field, introduces the concept of photon and the related photon creation operator, photon annihilation operator, and photon number operator. It is used to describe stimulated Raman scattering, stimulated Kerr scattering, and various multiphoton excitation processes. Within this theoretical regime the light (as a photon field) and molecules are treated as a combined quantum mechanical system. The light emission or absorption is always accompanied by the quantum transition of the whole system from its initial eigenstate to the final eigenstate. The molecular emission or absorption probability rate is determined by the corresponding transition matrix elements of the interaction Hamiltonian operator.