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Physical Review A

Kinetic Equations for Optical Pumping

C. R. Willis

Published Feb 1, 1970• 11 citations
Publisher

Abstract

We derive quantum-mechanical kinetic equations for the matter density $\ensuremath{\rho}$ and radiation density matrix $R$, which describe optical pumping phenomena. The resultant kinetic equations are a set of coupled nonlinear equations for $\ensuremath{\rho}$ and $R$. With appropriate linearizations, we can obtain the present theories of optical pumping. The nonlinear equations describe multiple scattering and line narrowing due to imprisonment of resonant radiation. We show that the coupled equations for $\ensuremath{\rho}$ and $R$ are equivalent to coupled equations for $\ensuremath{\rho}$ and a generalized polarization matrix II, whose matrix elements are the second moments of $R$. The polarization matrix II constitutes a complete description of linear phenomena in the same manner as present theories describe optical pumping phenomena by using the matter density matrix $\ensuremath{\rho}$ alone. As a consequence of our nonphenomenological treatment of radiation, we can provide a completely microscopic treatment of the externally modulated light-beam experiment of Bell and Bloom. We show that the atom absorbs the modulation envelope directly from the external thermal light beam in the same way that the atom absorbs transverse polarization directly from the light beam in optical pumping experiments.

DOI
10.1103/physreva.1.467

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Journal of Physics A Mathematical Nuclear and General•Mar 21, 1974•96 citations
We derive quantum-mechanical kinetic equations for the matter density \ensuremathρ\ensuremath{\rho}\ensuremathρ and radiation density matrix RRR, which describe optical pumping phenomena. The resultant kinetic equations are a set of coupled nonlinear equations for \ensuremathρ\ensuremath{\rho}\ensuremathρ and RRR. With appropriate linearizations, we can obtain the present theories of optical pumping. The nonlinear equations describe multiple scattering and line narrowing due to imprisonment of resonant radiation. We show that the coupled equations for \ensuremathρ\ensuremath{\rho}\ensuremathρ and RRR are equivalent to coupled equations for \ensuremathρ\ensuremath{\rho}\ensuremathρ and a generalized polarization matrix II, whose matrix elements are the second moments of RRR. The polarization matrix II constitutes a complete description of linear phenomena in the same manner as present theories describe optical pumping phenomena by using the matter density matrix \ensuremathρ\ensuremath{\rho}\ensuremathρ alone. As a consequence of our nonphenomenological treatment of radiation, we can provide a completely microscopic treatment of the externally modulated light-beam experiment of Bell and Bloom. We show that the atom absorbs the modulation envelope directly from the external thermal light beam in the same way that the atom absorbs transverse polarization directly from the light beam in optical pumping experiments.
Classical, semi-classical, and quantum-field descriptions for the interaction of light with matter are systematically discussed. Applications of interest include precise determinations of the linear and the non-linear electromagnetic response relevant to resonant pump-probe optical phenomena, such as electromagnetically induced transparency. In the quantum-mechanical description of matter systems, we introduce a general reduced-density-matrix framework. Time-domain (equation-of-motion) and frequency-domain (resolvent-operator) formulations are developed in a unified and self-consistent manner, using a Liouville-space operator representation. A preliminary semi-classical perturbation treatment of the electromagnetic interaction is adopted, in which the electromagnetic field is described as a classical field satisfying the Maxwell equations. Compact Liouville-space operator expressions are derived for the linear and the general (nth order) non-linear electromagnetic-response tensors describing moving many-electron systems. The tetradic matrix elements of the Liouville-space self-energy operators, which are introduced in the time-domain and frequency-domain formulations, are evaluated for environmental collisional and radiative interactions, in order to provide explicit forms for the quantum kinetic equations and the spectral-line shape formulas. It is emphasized that a quantized-field approach is essential for a fully self-consistent quantum-mechanical description of the interacting light-matter system.
The absorption of light by optically pumped atoms undergoing magnetic resonance is calculated from expressions based on a simplification of Barrat and Cohen-Tannoudji's theory of optical pumping. The density matrix for the system is first derived in orders of approximation which correspond to successive cycles of pumping. The off-diagonal elements of the matrix, and consequently the absorption of light, are modulated. The amplitudes of modulation are resonance functions which are, in general, more complicated than solutions of the Bloch equations. The selection rules for electric dipole radiation limit the possible frequencies of modulation to ω0 and 2ω0 for primary interactions (ω0 is the applied frequency), but modulation at higher frequencies can arise through the circulation of coherence in optical pumping cycles. The functions which represent the amplitude of modulation at 4ω0 are derived in first and second order, for comparison with experiment.
We generalize the method of deriving a kinetic equation for a gas laser developed in the first paper of this series to include radiation-matter correlations. As a consequence, we are able to show that the first Born approximation with asymptotic conditions which contain radiation-matter correlations is sufficient to explain the nonthermal photon distribution observed in photon-counting experiments. Our derivation includes the spatial and velocity effects of the motion of the gas atoms. After adiabatically eliminating the matter variables, we obtain a master equation for the radiation density matrix RRR with nonlinear coefficients. Our radiation master equation for stationary atoms without spatial effects is the same as the generalized Fokker-Planck equation of the Langevin-noise-equation treatment of lasers. We show that the generalized Fokker-Planck equation is the result of the first-Born-approximation treatment of the j\ifmmode\cdot\else\textperiodcentered\fi{}A interaction and is not dependent upon the microscopic structure of the reservoirs. In the first Born approximation, the diagonal and off-diagonal matrix elements of RRR do not interact with each other. Consequently, an initially diagonal radiation density matrix remains diagonal. However, we show that even though the stationary state is diagonal it is necessary to know the propagator of the off-diagonal part of RRR to answer time-dependent questions about quantities, such as the line shape, that depend on phase.
Linear and nonlinear (especially coherent) electromagnetic interactions of moving many-electron atoms are investigated using a reduced-density-matrix description, which is applied to electromagnetically induced transparency and related resonant pump-probe optical phenomena. External magnetic fields are included on an equal footing with the electromagnetic fields and spin-Zeeman interactions are taken into account. Complimentary time-domain (equation-of-motion) and frequency-domain (resolvent-operator) formulations of the reduced-density-matrix description are self-consistently developed. The general nonperturbative and non-Markovian formulations provide a fundamental framework for systematic evaluations of corrections to the standard Born (lowest-order-perturbation) and Markov (short-memory-time) approximations. The macroscopic electromagnetic response is described semiclassically, employing a perturbation expansion of the reduced-density operator in powers of the classical electromagnetic field. Our primary results are compact Liouville-space operator expressions for the linear and general (nthn\text{th}nth-order) nonlinear macroscopic electromagnetic-response tensors, which can be evaluated for nonlocal and nonstationary optical media described by multilevel atomic-system representations. Interactions among atoms and with environmental photons are treated as line-broadening effects by means of a general Liouville-space self-energy operator, for which the tetradic-matrix elements are explicitly evaluated in the diagonal, lowest-order, and Markov approximations. The compact Liouville-space operator expressions that are derived for the macroscopic electromagnetic-response tensors are introduced into the dynamical description of the electromagnetic-field propagation. It is pointed out that a quantized-electromagnetic-field approach will be required for a fully self-consistent quantum-mechanical treatment of local-field effects and radiative corrections.
The theory of optical birefringence is discussed from the point of view of the scattering of polarized photons by molecules using the framework of formal scattering theory and quantum electrodynamics. In Part One, those features from noncovariant quantum electrodynamics relevant to the molecular scattering of photons are reviewed. Chapter One contains an outline of classical electrodynamics in the Coulomb gauge, including the Stokes parameter and density matrix formulations of polarization. Chapter Two deals with the quantization of the radiation field, and the occupation number representation is defined. The quantum mechanical description of polarized light is outlined in Chapter Three: operator equivalents of the density matrix and Stokes parameters are invoked, the parameters themselves being obtained from the expectation values of the Stokes operators with the state vector of the photon. The Stokes parameter and density matrix are then applied to the polarization of a general beam containing an arbitrary number of photons, and some new methods are developed. The interaction of the electromagnetic field with bound electrons is formulated in Chapter Four in terms of a canonically transformed interaction Hamiltonian in which the multipole terms are explicit. Since each term is then gauge-invariant, this Hamiltonian is particularly suited to the application of diagrammatic perturbation theory which follows from the iteration of the scattering matrix in the interaction representation (Chapter Five). Also the extension of the theory to multiphoton processes is facilitated "because the field strength is explicit in the transformed Hamiltonian. The S-matrix connects the initial and final asymptotic states of the scattering system, and in Chapter Six the state vector and density operator of the scattered photon beam are obtained from those of the incident beam. Part Two contains the application of the above methods to a variety of linear and nonlinear optical birefringence effects in the absence or presence of external fields. In Chapter Seven, general equations are obtained for the polarization changes imposed on a forward scattered photon in terms of matrix elements of the reaction operator between plane polarized photon base states; whereas Chapter Eight extends this treatment to an n-photon beam, thereby encompassing the hyperpolarizability contributions to the polarization changes of the forward scattered beam. It is then demonstrated that the fundamental process in optical birefringence can be interpreted as an infinitesimal unitary transformation of the polarization spinor. Also the S-matrix approach to birefringence is compared with the methods used in crystal optics, and with the classical treatments of the scattering of polarized light by molecules. The general equations obtained for the polarization changes of the forward scattered beam are subsequently interpreted in the light of the physical circumstances appropriate to the bire- fringence effect of interest. In Chapters Nine, Ten, and Eleven, diagrammatic perturbation theory is used to obtain explicit expressions, in terms of molecular polarizability and rotation tensors, for the linear and nonlinear contributions to the polarization changes involved in natural optical activity, and in birefringence phenomena induced by static and optical electric and magnetic fields. The nonforward scattering of polarized photons by molecules is discussed in Part Three. General equations are calculated in Chapter Twelve for the azimuth, ellipticity, and depolarization ratio of the Rayleigh beam at any scattering angle and for any polarization of the incident beam. Explicit expressions in terms of molecular quantities are then obtained for the polarization at scattering angles of 90° and almost zero from both optically inactive and optically active molecules. It is demonstrated that a determination of the precise polarization state of the scattered beam can provide useful molecular information additional to that obtained from depolarization ratios alone. This is because the depolarization ratio depends on only the diagonal elements of the polarization density matrix and so does not convey all the information about the system. Raman scattering processes are contained in the formulation and the polarization of the Raman light at any scattering angle can be obtained. This is shown to be particularly useful for predicting the polarization of stimulated Raman light for any Raman-active liquid placed within a laser cavity. By extending the nonforward scattering formulation to incorporate multiphoton processes, equations are obtained in Chapter Thirteen for the ellipticity, azimuth, and depolarization ratio of the second harmonic wave at any scattering angle as a function of the incident polarization. Several specific situations are subsequently investigated. Finally, it is shown in Chapter Fourteen that the near-forw- ard Rayleigh and Raman scattering formulations provide an explanation for the observed polarization, as a function of the initial polarization, of the self-trapped filaments that arise from the self-focusing of an intense laser beam.
The nonlinear interaction of light with matter is described from a quantum-statistical point of view. The phenomena of two-photon emission and two-photon absorption including both the single- and two-mode cases and the Raman effect are discussed in detail. A master equation for the density operator of the light fields alone is derived. This operator equation is converted to a c number equation and analytic solutions are obtained for the diagonal matrix elements of the density operator in the Fock representation. No linearizing approximation is introduced. These solutions allow one to compute the moments of the photon distribution for the above nonlinear processes.