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The Journal of Chemical Physics

Light absorption by interacting atomic gas in quantum optical regime

Андрій Сіжук, Konstantin E. Dorfman, C. H. Raymond Ooi

Published Jul 27, 2021• 0 citations
Publisher

Abstract

Quantum optical theory of absorption properties of interacting atoms is developed. The concept of local absorptance is introduced as a derivative of the logarithm of intensity with respect to the distance in the vicinity of a given spatial point and a moment of time. The intensity is represented by the quantum and statistically averaged normal product of creation and annihilation operators of the electromagnetic field. The development of an analytical method of the estimation for the kinetic and optical parameters for the system is proposed here. The calculation method of the absorption coefficient includes thermal atomic motion, Doppler effect, and the short-range interaction between atoms. The absorption coefficient explicitly takes into account the quantum nature of the optical field. The ability of the system to absorb or emit quanta is quantitatively expressed through the special form of interaction integrals. The specific form of integrals results from the structure of the quantum brackets. The interplay between the collective (virtual photon exchange) and binary (optically induced inter-particle bonding) processes determines the system behavior. The spectral profile of the local absorption coefficient for different atomic densities and time intervals is simulated for realistic parameters.

DOI
10.1063/5.0054189

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Quantum optical theory of absorption properties of interacting atoms is developed. The concept of local absorptance is introduced as a derivative of the logarithm of intensity with respect to the distance in the vicinity of a given spatial point and a moment of time. The intensity is represented by the quantum and statistically averaged normal product of creation and annihilation operators of the electromagnetic field. The development of an analytical method of the estimation for the kinetic and optical parameters for the system is proposed here. The calculation method of the absorption coefficient includes thermal atomic motion, Doppler effect, and the short-range interaction between atoms. The absorption coefficient explicitly takes into account the quantum nature of the optical field. The ability of the system to absorb or emit quanta is quantitatively expressed through the special form of interaction integrals. The specific form of integrals results from the structure of the quantum brackets. The interplay between the collective (virtual photon exchange) and binary (optically induced inter-particle bonding) processes determines the system behavior. The spectral profile of the local absorption coefficient for different atomic densities and time intervals is simulated for realistic parameters.
The quantum optical theory of absorption/reemission properties of a system of interacting atoms is discussed. The calculation method of the absorption coefficient is developed with regard for the quantization of field, thermal atomic motion, Doppler effect, and the model interaction between atoms. It is shown that the formulation of the absorption coefficient in the quantum optical context is based on the commutation relation between the operators of electric field and intensity. The revealed non-linear dependence of the absorption coefficient on the atomic density, even in the case of negligible binary interaction, can be referred to a certain kind of quantum-optic collective effects.
A method of calculation of the absorption coefficient in the terms of quantum optics with regard for the quantization of the electromagnetic field and the Doppler effect is presented. It is shown that the local value of the absorption coefficient non-linearly depends on the atomic density and initial intensity. The analytically derived results are demonstrated in graphs for the the local absorption coefficient as a function of the frequency. The relatively strong dependence of the absorptance on the path length of an optical light beam is caused by the interatomic coupling through the intermediary of an electromagnetic field. The splitting of the absorption line induced by the Doppler effect in the system placed between mirrors is demonstrated.
The dependence of the multiphoton absorption probability for an atomic system on the statistical properties of the incident light is investigated. It is shown, by means of nthn\mathrm{th}nth-order time-dependent perturbation theory, that the multiphoton absorption probability depends on the (n,n)th(n, n)\mathrm{th}(n,n)th normally ordered correlation functions of the electromagnetic field. For stationary fields, the transition probability per unit time is constant and is directly related to the reduced cross-spectral correlation function of the electromagnetic field. This expression for the transition probability is then analyzed under various conditions of coherence. Explicit calculations are carried out for thermal light and for laser light, and the transition rates are compared when each has a Lorentzian spectrum. In particular, when the width of the final atomic level is much larger than the bandwidth of the field, the transition rate for thermal light is nnn! times higher than with laser light of the same mean intensity. The other extreme case, i.e., when the width of the final atomic level is much smaller than the bandwidth of the field, is also considered in detail. An equation for the density operator of the field is derived; this equation governs the change in the statistical properties of the photon system in nnn-photon absorption processes. On the basis of this equation, the time-dependent properties of the photon system are then studied and some physical consequences of these equations are discussed. Some numerical solutions relating to the time dependence of the factorial moments in two-photon absorption processes are presented.
The spatial inhomogeneity of absorption coefficient of the space between mirrors, filled by an optically active gas, is analyzed in quantum optical terms. It was theoretically shown, that the quantization of electromagnetic field in a cavity (optical resonator) can reveal the spatial inhomogeneity of absorption or re-emission ability of the optically active medium. It appears from the analytical calculations, the inhomogeneity is caused by the Doppler frequency shifts (including recoil effects) during the atom-photon collisions and the non-zero initial frequency width of the scanning signal. The proposed analytical representation of the absorption coefficient through the additive quantum optical terms gives deeper insight into intrinsic processes in the interacting with light matter.
Two-photon absorption and emission for a collection of two level atoms from a single mode beam of light are considered and the statistical proper- ties of the field after the interaction are investigated without placing any restriction of the population of the atomic levels . The dynamical behaviour of the field is described by assuming the atomic levels maintained with a nearly fixed popula- tion distribution . By applying iteration methods the time development for the density operator of the field is written and an expression for the coherent component is obtained . This component appears to be present only when there is a coherent component in the field before the interaction . The statistical properties of the field after the interaction, when the mean photon number is large initially, are then discussed and explicit calculations are carried out for some special cases of initial fields . Finally, it is shown that two-photon spontaneous emission field can be expressed as a superposition of chaotic fields .
Sub-Doppler resonances observed in miniature cells (V≪1cm3V \ll 1 cm^3V≪1cm3) with Rb or Cs atoms in the field of counterpropagating bichromatic laser beams are of interest for the creation of a miniature quantum frequency standard (QFS) of the optical range. However, a theory of these resonances that takes into full account the real structure of energy levels in an atom has not yet been constructed, which would make it possible to obtain explicit analytical expressions for the absorption coefficient of the medium. This paper addresses this gap using the density matrix formalism and the algebra of irreducible tensor operators. Namely, we obtained an analytical expression for the absorption coefficient of the probe beam in the presence of a more intense counterpropagating beam (pump-probe regime). Moreover, the calculations were carried out for arbitrary parameters of laser beam polarization, arbitrary angular momenta of optical dipole transitions in the atom and various relaxation processes. The constructed theory allows us to correctly take into account the simultaneous action of various nonlinear optical effects, in contrast to the simplified three-level model of the atom, and also to investigate the partial contribution of each of them to the overall observed resonant circuit. The analysis performed, in particular, made it possible to predict an increase in the amplitude of the sub-Doppler resonance when using counterpropagating light beams with opposite circular polarizations in relation to the configuration of counterpropagating beams with orthogonal linear polarizations, which is often used in practice.