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Annual Meeting Optical Society of America

Analysis of strong light-matter interaction using a dressed propagator approach

James G. Fujimoto, Ting K. Yee

Published Jan 1, 1985• 0 citations
Publisher

Abstract

A diagrammatic density matrix technique is developed and applied to study nonlinear optical processes involving responses from weak probe fields interacting with a system under strong excitation. These diagrams consist of lowest-order double-Feynman diagrams which represent the density matrix perturbation terms describing the system response to the weak probe fields1,2 combined with dressed propagators which represent the density matrix elements of the system under strong excitation. The dressed propagators are described by a set of linear equations which, in most cases, may be derived in inspection. The methodology is similar to the bare-atom approach.2 The advantages of using this diagrammatic technique are that (1) it allows one to select and express analytically the dominant and appropriate density matrix elements (diagrams and dressed propagators); (2) analytical expressions may be constructed directly from the diagrams and thus lengthy calculations needed to obtain closed-form solutions are greatly reduced; (3) it provides a physical interpretation for the density matrix solutions and nonlinear optical processes; and (4) it may be generalized to more complicated, multilevel systems. We demonstrate the application of this technique to describe gain saturation, Stark splitting, and Raman scattering.

DOI
10.1364/oam.1985.we6

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A diagrammatic density matrix technique is developed and applied to study nonlinear optical processes involving responses from weak probe fields interacting with a system under strong excitation. These diagrams consist of lowest-order double-Feynman diagrams which represent the density matrix perturbation terms describing the system response to the weak probe fields1,2 combined with dressed propagators which represent the density matrix elements of the system under strong excitation. The dressed propagators are described by a set of linear equations which, in most cases, may be derived in inspection. The methodology is similar to the bare-atom approach.2 The advantages of using this diagrammatic technique are that (1) it allows one to select and express analytically the dominant and appropriate density matrix elements (diagrams and dressed propagators); (2) analytical expressions may be constructed directly from the diagrams and thus lengthy calculations needed to obtain closed-form solutions are greatly reduced; (3) it provides a physical interpretation for the density matrix solutions and nonlinear optical processes; and (4) it may be generalized to more complicated, multilevel systems. We demonstrate the application of this technique to describe gain saturation, Stark splitting, and Raman scattering.
Diagrammatic methods for the calculation of the nonlinear response of a system that is dressed by resonant external fields are developed. The double-sided diagrams used earlier by Prior [IEEE J. Quantum Electron. QE-20, 37 (1984)] for the calculation of nonlinear susceptibilities in the presence of weak fields are generalized. Additional types of double-sided diagrams are given that incorporate explicitly (a) the relaxation-induced population transfers among the dressed levels and (b) the effects of the nonvanishing of the diagonal elements of the dipole operator in the dressed-state basis. The rules for the diagrams are worked out from the analytical structure of the nonlinear response. Applications of the diagrammatic techniques to several intense-field phenomena are discussed.
We apply a diagrammatic density matrix perturbation technique to analyze third order nonlinear optical processes. The diagrammatic approach is shown to yield a significant simplification in the computation of both steady state and transient response while including the effects of damping and linewidth. The topology of the diagrams is stressed in identifying and interpreting their associated perturbation terms as well as predicting frequency resonance and transient behavior. We demonstrate the practical utility of the technique by presenting a detailed analysis and discussion of the processes of stimulated Raman scattering, hot luminescence, and pressure induced resonances in four wave mixing.
The Liouville equation for the density matrix can be recast so that the external field terms which couple density matrix elements are second order in the field. This approach is shown to have a profound effect on the analysis of strong field resonant nonlinear optical problems. First, in the case where parity or appropriate field restrictions apply, there is a reduction of the number of coupled equations which must be solved by at least a factor of two. Second, this reformulation naturally leads to radiative renormalization terms which are directly related to saturation, Stark shifts and Rabi splittings. The renormalization is equivalent to a Dyson equation analysis. We use this simple formalism to obtain exact solutions to a number of nonlinear optical problems including cases where there are two or more strong, resonant fields. These problems include: 1) two levels, two strong fields, 2) three levels, two strong fields, and 3) four levels, three and four strong fields. Discussed in detail are the two level case and the three and four level cases where weak fields couple the ground state to other states. We use these results to discuss the physics of optically induced transparency, population beats, optical switching in quantum wells, and fully resonant coherent anti-Stokes Raman scattering (CARS).
A diagrammatic density matrix perturbation technique is applied to describe transient third-order nonlinear optical processes and their applications to the measurement of transient phenomena. Using this approach, pump probe, parametric scattering, and three-pulse scattering are analyzed in a computationally simple and unified manner. The density matrix allows the description of a wide variety of dynamical processes including population and dephasing relaxation as well as orientational randomization and spatial diffusion. In addition, the diagrams provide a physical interpretation for the density matrix terms that they represent, and the effect of varying experimental parameters for the measurement of transient behavior can often be determined directly from the diagrams. Finally, topological similarities between diagrams provide a unified description of several different transient four-wave mixing measurement techniques.
The Liouville equation for the density matrix can be recast so that the external-field terms which couple density-matrix elements are second order in the field. This approach is shown to have a profound effect on the steady-state analysis of strong-field resonant nonlinear optical problems. First, in the case where parity or appropriate field restrictions apply, there is a reduction of the number of coupled equations which must be solved by at least a factor of 2. Second, this reformulation naturally leads to radiative-renormalization terms which are directly related to saturation, Stark shifts, and Rabi splittings. We can use this simple formalism to obtain solutions to a number of resonant nonlinear problems including cases where there are two or more strong fields. The renormalization described here is equivalent to a Dyson-equation analysis.
Density-matrix calculations provide the steady-state conditions for probe amplification or lasing between atomic levels with an uninverted population, but additional insight into the underlying physics is given by a probability amplitude approach. In this paper we derive the gain coefficient from the Feynman diagrams for a probe-laser incident on a resonantly pumped, V-type system using time-dependent perturbation theory in a dressed basis. The connection is made to density-matrix calculations for this model, which have been used recently to describe experiments in Rb [A. S. Zibrov et al., Laser Phys. 5, 553 (1995); Phys. Rev. Lett. 75, 1499 (1995)]. In the density-matrix calculation the overall gain is possible because the pump-induced coherence of a strongly driven transition leads to probe amplification, despite the lack of inversion on the probe transition. In our amplitude approach we associate a specific physical process with each of the scattering channels for the probe and show how amplification without inversion can be achieved. The amplitude calculation reveals a distinction between stepwise and two-quantum processes. Interference is shown to result from the two-quantum processes, constructive for the amplification channels and destructive for the absorption. Terms appearing in the gain coefficient are traced to different sources in the amplitude and density-matrix approaches. The physical origin of each term is discussed and compared for both approaches. Terms that arise from coherences in the density-matrix approach are shown to correspond to noninterfering stepwise contributions in the amplitude approach. In deriving these results, we find that the Feynman rules that we construct for forming the probability amplitude for an arbitrary scattering process of the electromagnetic field from the coupled atom-strong pump system are consistent with Rayleigh-Schr\"odinger perturbation theory in the quantum dressed basis. In addition, the spontaneously emitted photons become entangled with the probe field, correlating the emission spectrum with specific scattering channels.