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Journal of Physics A Mathematical and General

Quantum theory of nonlinear optical phenomena

Miguel Orszag

Published Nov 1, 1979• 4 citations
Publisher

Abstract

The equivalence between the Hamiltonians representing nonlinear optical phenomena and N two-level atoms interacting via the electromagnetic field is exploited to find a solution to a parametric amplifier, a frequency converter and to the problems of Brillouin and Raman scattering. The n-photon probability and average number of photons as a function of time are obtained for all these cases. The results of the parametric amplifier can be readily applied to the Brillouin and Raman effects. In particular the results obtained for spontaneous fluorescence are applicable to the Stokes line of the stimulated Raman effect. Other nonlinear effects are discussed in the context of the present theory.

DOI
10.1088/0305-4470/12/11/031

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Proceedings of the Royal Society of London A Mathematical and Physical Sciences•Apr 23, 1968•62 citations
The equivalence between the Hamiltonians representing nonlinear optical phenomena and N two-level atoms interacting via the electromagnetic field is exploited to find a solution to a parametric amplifier, a frequency converter and to the problems of Brillouin and Raman scattering. The n-photon probability and average number of photons as a function of time are obtained for all these cases. The results of the parametric amplifier can be readily applied to the Brillouin and Raman effects. In particular the results obtained for spontaneous fluorescence are applicable to the Stokes line of the stimulated Raman effect. Other nonlinear effects are discussed in the context of the present theory.
A description of the parametric amplifier and frequency converter is presented without introducing the classical (i.e., parametric) approximation for the pumping field. Constants of the motion are found which reduce the solution of the Schr\"odinger equation to the diagonalization of a matrix. This diagonalization is accomplished numerically, and the eigenvalues and eigen-functions of a system with fixed energy are calculated. The time-dependent behavior of the mean number of photons in the amplified or frequency up-converted field is presented. The time evolution of the probability distributions is illustrated. The technique is extended to the problem of coherent spontaneous emission from a system of NNN two-level atoms interacting with the radiation field where both the atomic system and the radiation field are quantized.
The nonlinear process of the stimulated Raman effect is treated theoretically. Simple expressions are derived for the initial rates of change and limiting steady state values of the first two moments, the degrees of second-order coherence and the correlation function of the pump and Stokes beams. An analytical solution for the time dependence of the joint photon probability distribution of the two light beams is obtained and then employed to calculate some numerical results for various special cases of interest, and the significance of these results is discussed in physical terms. Simpler approximate expressions are also derived for the case where the pump beam is much more intense than the Stokes beam.
Partial table of contents: PART I: GENERAL CONCEPTS AND METHODS OF NONLINEAR OPTICS. Electromagnetic Fields. Classical Description. The Quantized Free Radiation Field. Interaction Between Radiation and Matter. Semiclassical Description of Nonlinear Optics. Statistical and Coherence Properties of the Radiation Field and Their Measurement. Nonstationary Processes. PART II: EFFECTS AND PROCESSES OF NONLINEAR OPTICS. Nonlinear One--photon Processes in Lasers. Nonlinearities in Transient One--photon Processes. Nonlinearities and Qunatum Phenomena in Transient One--photon Processes. Multiphoton Absorption and Emission. Generation of Harmonics and Sum and Difference Frequencies. Parametric Amplification and Oscillation. Stimulated Raman Scattering. Optical Bistability. APPENDIX A: Compilation of Quantum--Theoretical Definitions and Relations. General References. Index.
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.
Abstract A general approach to the discussion of optical birefringence phenomena is presented. It is based on the S-matrix approach to photon scattering in a nonrelativistic quantum field theoretical formalism and the Stokes operator description of polarization. The use of a canonically transformed interaction Hamiltonian in combination with diagrammatic perturbation theory enables the response of a system to electromagnetic radiation to be calculated in a straightforward and consistent manner to any order in the perturbation, and the effect of static fields is included easily. As an illustration, the angle of rotation of a beam of plane-polarized light by a solution of optically active molecules is calculated and the intensity dependence of the angle determined. The latter phenomenon should become apparent at high photon flux densities particularly when ω, the frequency of the incident light, or 2ω are similar to electronic excitation frequencies in the optically active molecules.