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Physical Review A

Populating Excited States of Incoherent Atoms Using Coherent Light

Thomas J. Mcilrath, John L. Carlsten

Published Sep 1, 1972• 43 citations
Publisher

Abstract

This paper deals with the equations of motion of the density matrix of a two-level atom in the presence of an intense multimode radiation field characterizing a multimode laser. Using a simplified treatment of line broadening which does not include correlations between momentum-changing collisions and pressure-broadening collisions, we obtain expressions which show the effect of pressure, laser-pulse length, and intensity on the excitation. We obtain analytic expressions in limiting cases of the pressure which allow prediction of the degree of excitation from a given laser pulse. In our treatment the phase relaxation time of the atoms is assumed to be fast enough so that coherence effects among the atoms can be ignored. Treating the velocity of the atoms statistically, we solve for three cases: constant velocity, velocity changes that are fast compared to the excitation time but slow compared to the dephasing time, and velocity changes that are fast compared to all other processes. The three cases yield the same formal equation for the two-body process of absorption of photons by incoherent atoms; however, the cross sections differ and are calculated explicitly for each case. Also discussed are the range of laboratory conditions and the relationship between these laboratory conditions and the various cases considered to demonstrate that under most circumstances this simple photon-absorption picture is applicable, provided the cross section is calculated correctly.

DOI
10.1103/physreva.6.1091

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Application of state-multipole Heisenberg equations to Raman excitation dynamics

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Description of detailed temporal excitation dyanmics for coherent excitation, such as is produced by idealized laser radiation, contrasts with evaluation of rate coefficients by means of generalized Golden Rule procedures; it requires an appropriate time-dependent Schroedinger equation. When the atom undergoing excitation is also affected by incoherent processes, such as collisions, this equation no longer suffices. The Heisenberg equations, or equivalent density-matrix equations, permit treatment in which coherence and incoherence play comparable roles in the excitation dynamics. Unlike rate equations, such equations must incorporate complexities that originate in the orientation degeneracy expressed by magnetic quantum numbers. In simple cases of coherent excitation, both for single-photon and multiphoton excitation, the sublevels merely require an average of 2J+1 independent Schroedinger equations. Relaxation couples the independent equations. It has been known for some time that appropriate state-multipole operators can simplify the description of many phenomena connected with optical pumping. This memo discusses application of these multipole operators to the description of Raman (or more general multiphoton) coherent excitation. In some simple limiting cases the equations simplify, but in general one has a hierarchy of coupled multipole polarizations and coherences in place of the populations and coherences that occur as variables in nondegenerate systems. 28 refs., 4 figs.

•Sep 10, 1987•0 citations
This paper deals with the equations of motion of the density matrix of a two-level atom in the presence of an intense multimode radiation field characterizing a multimode laser. Using a simplified treatment of line broadening which does not include correlations between momentum-changing collisions and pressure-broadening collisions, we obtain expressions which show the effect of pressure, laser-pulse length, and intensity on the excitation. We obtain analytic expressions in limiting cases of the pressure which allow prediction of the degree of excitation from a given laser pulse. In our treatment the phase relaxation time of the atoms is assumed to be fast enough so that coherence effects among the atoms can be ignored. Treating the velocity of the atoms statistically, we solve for three cases: constant velocity, velocity changes that are fast compared to the excitation time but slow compared to the dephasing time, and velocity changes that are fast compared to all other processes. The three cases yield the same formal equation for the two-body process of absorption of photons by incoherent atoms; however, the cross sections differ and are calculated explicitly for each case. Also discussed are the range of laboratory conditions and the relationship between these laboratory conditions and the various cases considered to demonstrate that under most circumstances this simple photon-absorption picture is applicable, provided the cross section is calculated correctly.
Abstract The treatment of transient excitation of transitions between two atomic or molecular energy levels by monochromatic laser radiation under conditions in which phase-destroying collisions predominate is treated by means of numerical and approximate analytical solutions of the equations giving the rate of change of a modified density matrix. The analytical solutions are then used to obtain the transient values of the population of the excited state when Doppler broadening is taken into account. Numerical calculations are carried out for the ratio γ'/γ = 10, where 2γ is the damping constant for diagonal and γ' for non-diagonal elements of the density matrix. This extends the treatm ent given in two previous papers for the situation when γ' = γ, corresponding to very low pressures for which phase-destroying collisions are relatively unimportant.
The present paper includes the influence of collisions in the high-intensity laser theory by Stenholm and Lamb. The history of an atom is divided into field- and collision-dominated intervals. The collisions are treated as instantaneous independent events (impact approximation). The equation of motion for the density matrix of an ensemble of atoms undergoing collisions is derived. The collisions manifest themselves as an integral operator in the equation of motion. As a model, collisions which do not change the populations of the atomic levels are treated. Physical conditions on the kernel matrix of the collision integral are used to construct a simple nontrivial model. To simplify the treatment, the phase and velocity changes are assumed to take place in different collisions. This model is used to solve the problem of a high-intensity laser with collisions. Only the lowest nonvanishing terms in the Fourier expansion of the density matrix elements are used. Typical numerical results are evaluated and shown in the figures. Connections with other papers and generalizations are discussed.
Coherent manipulations of atoms using laser light The internal structure of a particle - an atom or other quantum system in which the excitation energies are discrete - undergoes change when exposed to pulses of near-resonant laser light. This tutorial review presents basic concepts of quantum states, of laser radiation and of the Hilbert-space statevector that provides the theoretical portrait of probability amplitudes - the tools for quantifying quantum properties not only of individual atoms and molecules but also of artificial atoms and other quantum systems. It discusses the equations of motion that describe the laser-induced changes (coherent excitation), and gives examples of laser-pulse effects, with particular emphasis on two-state and three-state adiabatic time evolution within the rotating-wave approximation. It provides pictorial descriptions of excitation based on the Bloch equations that allow visualization of two-state excitation as motion of a three-dimensional vector (the Bloch vector). Other visualization techniques allow portrayal of more elaborate systems, particularly the Hilbert-space motion of adiabatic states subject to various pulse sequences. Various more general multilevel systems receive treatment that includes degeneracies, chains and loop linkages. The concluding sections discuss techniques for creating arbitrary pre-assigned quantum states, for manipulating them into alternative coherent superpositions and for analyzing an unknown superposition. Appendices review some basic mathematical concepts and provide further details of the theoretical formalism, including photons, pulse propagation, statistical averages, analytic solutions to the equations of motion, exact solutions of periodic Hamiltonians, and population-trapping "dark" states.
The interaction between an intense radiation field and atoms that undergo collisions in an atomic vapor is studied. With the assumption that velocity-changing collisions are state independent and weak, we obtain an analytic expression for the time-dependent density-matrix elements by solving a quantum-mechanical transport equation using a dressed-state approach. Our analytical calculation is used to predict the form of the signal in an extended-pulse photon echo. The results show good agreement with an experiment carried out by Yodh et al. [Phys. Rev. Lett. 53, 659 (1984)]. It is found that the decay rate of the echo signal decreases rapidly with increasing duration of the second pulse in the pulse excitation sequence. A comparison between theory and experiment is presented and a physical interpretation of the results is given.
We investigate coherent accumulation processes in three-level atoms excited by a train of ultrashort pulses in the case where the atomic relaxation times are greater than the laser repetition period. In this situation the resonances of the laser field with the atomic system are determined by the laser frequency comb rather than by the spectrum of a single pulse. Using the density matrix formalism, we develop a perturbative theory that is valid for arbitrary pulse shapes. The excitation of a Doppler-broadened atomic vapor by hyperbolic-secant pulses and $0\ensuremath{\pi}$ pulses is analyzed. It is shown that pulse shape has a great influence on the accumulation process and can change the spectral periodicity of the pattern impressed on the Doppler profile of the medium due to the two-photon absorption process. The effect of interpulse phases is also investigated, and we show that the atomic populations can vary by more than one order of magnitude with small variations of the laser repetition rate, while being insensitive to variations of the laser offset. Finally, the theory is adapted for the temporal-coherent-control technique, and its results are compared with previously reported experimental data.
Description of detailed temporal excitation dyanmics for coherent excitation, such as is produced by idealized laser radiation, contrasts with evaluation of rate coefficients by means of generalized Golden Rule procedures; it requires an appropriate time-dependent Schroedinger equation. When the atom undergoing excitation is also affected by incoherent processes, such as collisions, this equation no longer suffices. The Heisenberg equations, or equivalent density-matrix equations, permit treatment in which coherence and incoherence play comparable roles in the excitation dynamics. Unlike rate equations, such equations must incorporate complexities that originate in the orientation degeneracy expressed by magnetic quantum numbers. In simple cases of coherent excitation, both for single-photon and multiphoton excitation, the sublevels merely require an average of 2J+1 independent Schroedinger equations. Relaxation couples the independent equations. It has been known for some time that appropriate state-multipole operators can simplify the description of many phenomena connected with optical pumping. This memo discusses application of these multipole operators to the description of Raman (or more general multiphoton) coherent excitation. In some simple limiting cases the equations simplify, but in general one has a hierarchy of coupled multipole polarizations and coherences in place of the populations and coherences that occur as variables in nondegenerate systems. 28 refs., 4 figs.