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Physical Review A

Summation of four-operator perturbation series: Application to atom-atom intensity-dependent correlations

Yves Gontier

Published Jan 1, 1985• 4 citations
Publisher

Abstract

It is shown how certain classes of problems dealing with the interaction of radiation with atoms can be formulated in terms of four-operator perturbation series. The case of an isolated atom coupled to a single-mode field is discussed in detail within the resolvent formalism. The process where no photon is effectively absorbed by the atom is described, to all orders, in terms of a series involving four operators which simultaneously increase and/or decrease the photon number and the orbital quantum number. This series is exactly summed and the summation technique is generalized to single-atom, two-field and to two-atom, single-field systems exhibiting zero, one, and two net photon absorptions or emissions. The theory is applied to induced emission of a single photon from a pair of two-level atoms coupled to a monomode radiation field. The energy diagrams, the time dependence of the probability, and the resonance curves are discussed for systems where (i) both atoms are in the upper state and (ii) atom 1 is in the upper state and atom 2 is in the lower state at t=0. In comparing these results to the ones obtained with a single atom, we find that the important intensity-dependent correlations give rise to trapping effects even when the atoms are initially in the upper state.

DOI
10.1103/physreva.31.279

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It is shown how certain classes of problems dealing with the interaction of radiation with atoms can be formulated in terms of four-operator perturbation series. The case of an isolated atom coupled to a single-mode field is discussed in detail within the resolvent formalism. The process where no photon is effectively absorbed by the atom is described, to all orders, in terms of a series involving four operators which simultaneously increase and/or decrease the photon number and the orbital quantum number. This series is exactly summed and the summation technique is generalized to single-atom, two-field and to two-atom, single-field systems exhibiting zero, one, and two net photon absorptions or emissions. The theory is applied to induced emission of a single photon from a pair of two-level atoms coupled to a monomode radiation field. The energy diagrams, the time dependence of the probability, and the resonance curves are discussed for systems where (i) both atoms are in the upper state and (ii) atom 1 is in the upper state and atom 2 is in the lower state at t=0. In comparing these results to the ones obtained with a single atom, we find that the important intensity-dependent correlations give rise to trapping effects even when the atoms are initially in the upper state.
The summation of all the higher-order contributions to multiphoton absorption in atoms is presented. The nonperturbative expressions for the transition amplitudes are expressed in terms of continued fractions. They account for the whole perturbation originated by the radiation field on the atom but do not exhibit explicit expression for the level shift. In the case of radiation fields of high intensity the only reliable determination of the level shift involves a careful location of the poles of the resolvent operator. The theory has been tested in considering a two-level atom. An extremely rapid convergence of the continued fractions has been observed, and accurate results concerning high-order resonance shifts have been obtained. The expressions for the transition amplitudes being nonperturbative with regard to the field strength, they can be considered as analytic continuations of the perturbation series. This provides a useful approach to the problem of ultraintense fields.
The interaction is considered between NNN stationary two-level atoms and a radiation field described by a single cavity mode. The state vector for the complete system of atoms plus radiation is expressed as a linear superposition of states constructed from a product of photon states in the nnn representation and products of Pauli spin eigenstates describing all combinations of atoms in the lower and upper energy levels. Equations for the corresponding probability amplitudes are derived by substituting this superposition into the Schr\"odinger equation. The resulting equations are combined into bilinear form and phenomenological damping contributions are added. After the neglect of certain of the bilinear quantities, a master equation is derived which governs the probability Pmn{{P}_{m}}^{n}Pm​n of having mmm atoms in the lower level and nnn photons in the mode. This master equation takes account of multiple single-quantum absorption and emission processes but not of simultaneous multiple processes involving two or more atoms at a time. The equation which governs the expected number of photons 〈n〉〈n〉〈n〉 derived from the master equation bears a close resemblance to a rate equation. The effect of radiation loss from the cavity is incorporated into the master equation. Numerical calculations for a QQQ-spoiled laser show that the statistics of the number of photons in the mode bear a qualitative resemblance to Poisson statistics.
A modified perturbation theory is developed for the calculation of the time-dependent wave function describing the propagation of an atom in a two-mode laser field. With the mode frequencies nearly equal, a first approximation is obtained that reproduces and extends known results, for both resonant and nonresonant transitions. This lowest-order solution sums terms that describe the absorption of a photon from one mode and emission into the other, leaving the total number of photons unchanged and shifting the momentum of the atom accordingly. Corrections are generated by expansion of a resolvent from which the nearly degenerate states have been projected out. These approximate solutions are used to construct asymptotic states in a formulation of atom-atom scattering in the two-mode field. In close analogy with the soft-photon approximation, a ``soft-pair'' approximation is developed based on the dominance of those asymptotic interactions in which the transfer of energy from the field to the atom is small, allowing one to relate the scattering amplitude in the presence of the field to the field-free amplitude. When the atomic ground state and an excited state are closely coupled by the field, the asymptotic wave function can have mixed parity allowing for long-range contributions to the effective potential. In addition to an enhancement of forward-scattering probabilities, this leads to a threshold anomaly that is analyzed here, in the resonant case, with the aid of a modified effective-range theory.
Using the formalism developed earlier, we treat spontaneous emission from a pair of identical two-level atoms A1{A}_{1}A1​, A2{A}_{2}A2​, whose separation r21{r}_{21}r21​ can be comparable to the wavelength $\ensuremath{\lambda}$. We obtain expressions for time-dependent intensities and damping rates with the initial conditions (a) both atoms inverted, (b) prior excitation by a short $\frac{1}{2}\ensuremath{\pi}$ pulse, and (c) only A1{A}_{1}A1​ inverted. The results in (a) are compared with those obtained for a model consisting of two initially excited harmonic oscillators O1{O}_{1}O1​, O2{O}_{2}O2​. The atoms exhibit superradiant behavior, whereas O1{O}_{1}O1​, O2{O}_{2}O2​ tend to trap radiation. In (a), the intensity pattern $\mathcal{R}(\ensuremath{\theta},t)$ develops lobes in different directions at different times, so that the spatial distribution of photons at time $t\ensuremath{\rightarrow}\ensuremath{\infty}$ is the same as in the independent-atom case ${r}_{21}\ensuremath{\gg}\ensuremath{\lambda}$. For the oscillators, the lobes of $\mathcal{R}(\ensuremath{\theta},t)$ do not change direction, but only become more pronounced as time increases. In (b) and (c), the lobes oscillate back and forth at frequency $2{\ensuremath{\Omega}}_{12}$ corresponding to the shifts $\ifmmode\pm\else\textpm\fi{}{\ensuremath{\Omega}}_{12}$ of the triplet and singlet states due to the ${A}_{1}\ensuremath{-}{A}_{2}$ interaction. The intensity can therefore have a sinusoidal component. Field correlation functions calculated for (a) and (c) show that A2{A}_{2}A2​ and A2{A}_{2}A2​ radiate simultaneously around the frequencies $\ensuremath{\epsilon}\ifmmode\pm\else\textpm\fi{}{\ensuremath{\Omega}}_{12}$, where $\ensuremath{\epsilon}$ is the single-atom resonant frequency. The spectrum is calculated for case (c), and shows the effects of coherent linewidth enhancement in addition to the frequency shifts.
A very large number of physical phenomena in the resonant interaction of atomic-molecular systems with the radiation fields can be studied by treating the atomic system as a two level system and by examining its response to the applied fields. Various perturbative results are well known. A number of recent experimental works require the knowledge of the nonperturbative response functions, when both the applied fields are strong. These include a variety of experiments on instabilities(1) in lasers involving the switching from a single mode to for example two mode operation. Similarly recent nonlinear mixing experiments, where not only four wave mixing but also higher mixing in saturating fields has been studied. Pump probe experiments have also been repeated with probes whose intensity could be large. The purpose of this paper is to formulate the general theory and use it to understand the experiments. The formulation we present is also well suited for studying the effect of collisions. Details of various collisional induced coherences in fourwave and six wave mixing etc. can be studied.
A theory of four-wave mixing is developed using an amplitude approach in the Schr\"odinger picture. It is shown that the four-wave mixing signal produced when three fields are incident on an ensemble of two-level atoms can be viewed as arising from constructive interference of the signals emitted at the various atomic sites. Fourteen distinct amplitudes contribute to the four-wave mixing signal. Some of these amplitudes involve final states in which one or two atoms are excited, and some involve final states in which photons are emitted into modes other than a phase-matched mode of interest. The amplitude approach has the advantage of clearly showing the atom-field correlations. It helps one to understand the underlying physical mechanisms responsible for creation of the four-wave mixing signal, as well as features in the line shape resulting from collisions and effects relating to atomic recoil on the absorption or emission of radiation. These so-called collision- and recoil-induced resonances are calculated explicitly using the amplitude approach, and an interpretation of the results in terms of the interference between different amplitudes is given. Our results, calculated for a finite interaction time between the atoms and the fields, are compared with analogous calculations in which an effective ground-state decay time is assumed. It is shown that the results differ if the atom-field interaction time is not the longest relevant time parameter in the problem.