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arXiv:quant-ph/0305006 · Physical Review A

Eliminating ground-state dipole moments in quantum optics via canonical transformation

Gediminas Juzeliūnas, Luciana C. Dávila Romero, Davıd L. Andrews

Published Oct 9, 2003• 12 citations
arXivHTMLPDF

Abstract

By means of a canonical transformation it is shown how it is possible to recast the equations for molecular nonlinear optics to completely eliminate ground-state static dipole coupling terms. Such dipoles can certainly play a highly important role in nonlinear optical response---but equations derived by standard methods, in which these dipoles emerge only as special cases of transition moments, prove unnecessarily complex. It has been shown that the elimination of ground-state static dipoles in favor of dipole shifts results in a considerable simplification in form of the nonlinear optical susceptibilities. In a fully quantum theoretical treatment the validity of such a procedure has previously been verified using an expedient algorithm, whose defense was afforded only by a highly intricate proof. In this paper it is shown how a canonical transformation method entirely circumvents such an approach; it also affords insights into the formulation of quantum field interactions.

DOI
10.1103/physreva.68.043811

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By means of a canonical transformation it is shown how it is possible to recast the equations for molecular nonlinear optics to completely eliminate ground-state static dipole coupling terms. Such dipoles can certainly play a highly important role in nonlinear optical response---but equations derived by standard methods, in which these dipoles emerge only as special cases of transition moments, prove unnecessarily complex. It has been shown that the elimination of ground-state static dipoles in favor of dipole shifts results in a considerable simplification in form of the nonlinear optical susceptibilities. In a fully quantum theoretical treatment the validity of such a procedure has previously been verified using an expedient algorithm, whose defense was afforded only by a highly intricate proof. In this paper it is shown how a canonical transformation method entirely circumvents such an approach; it also affords insights into the formulation of quantum field interactions.
It is well known that a simple transformation of the electric dipole interaction provides a convenient means for ascertaining the effects of permanent dipoles on the optical behaviour of systems with a response dominated by two energy levels. By establishing the general validity of the procedure for parametric processes such as harmonic generation, it is shown how the detailed structure of the optical susceptibilities associated with arbitrary forms of optical nonlinearity can be ascertained by an algorithmic method, based on a novel interpretation of the relevant quantum electrodynamical Feynman diagrams. Application of the algorithm to second and third harmonic generation illustrates its usefulness and simplicity, whilst also providing new results and revealing features, related to the role of permanent dipoles, which have not hitherto been apparent.
Abstract In reporting and explaining the interactions of light with atoms and molecules, a photon-based description is not only appropriate but clearly essential when electronic or other kinds of quantum transition ensue. However, textbook treatments frequently go no further than the Planck relation, in representing the quantum nature of the light itself—often resorting to classical principles when discussing mechanism. Complete consistency and rigour can be achieved by treating both the matter and the radiation in a fully quantised form, which requires the electromagnetic fields to be cast in a quantum field representation. It proves possible to develop a rigorous approach to this theory that is simple to convey and apply, and which lends itself to a significantly enhanced level of appreciation of mechanism. This paper lays a concise foundation and exemplifies the application in three specific cases: absorption, emission and scattering. It is also shown how this formulation affords a basis for applications in higher-order, multiphoton and nonlinear optical processes.
Absorptive and dispersive nonlinear optical properties have been studied considering a two-level molecular system with permanent dipole moments immersed in a thermal reservoir interacting with a classical electromagnetic field. Our model is based in a stochastic description, where the system–solvent interaction induces random shifts in the Bohr frequency (ω0) that transforms ω0 into a stochastic variable ξ(t). Our results show that it is necessary to neglect the rotating-wave approximation in order to measure the effect of the permanent dipole moments. The two-photon transitions over those with one-photon are favored when the permanent dipole moments are considered.
The classical theory of nonlinear optics is well established, owing to the seminal work of Bloembergen and others. In this theory, nonlinear coefficients are used to express dielectric properties in a unified way. A quantum-mechanical theory of this type is obviously desirable, allowing the calculation of quantum effects, without requiring a detailed electronic and molecular model of the dielectric. In current research that encompasses such effects as squeezing and photon antibunching, a coherent quantum theory is essential. This should include nonlinearities, inhomogeneity, and dispersion to be relevant to physical dielectric media.
In a gauge invariant formulation of the molecular electric dipole-photon interaction, the rigorous coupling is strictly linear in the photon creation and photon annihilation operators. The linear coupling allows for a super-radiant phase transition as in the Hepp-Lieb formulation. A previous notion of a quadratic-coupling ``no-go theorem'' for super-radiance is incorrect. Also incorrect is a previous assertion that the dipole-photon coupling has absolutely no effect on the thermal equations of state. These dubious assertions were based on incorrect canonical transformations which eliminated the electric field (and thereby eliminated the dipole-photon interaction) which is neither mathematically nor physically consistent. The correct form of the canonical transformations are given in this work which allows for the physical reality of super-radiant condensed matter phases.
Quantum canonical transformations are defined algebraically outside of a Hilbert space context. This generalizes the quantum canonical transformations of Weyl and Dirac to include non-unitary transformations. The importance of non-unitary transformations for constructing solutions of the Schr\\"odinger equation is discussed. Three elementary canonical transformations are shown both to have quantum implementations as finite transformations and to generate, classically and infinitesimally, the full canonical algebra. A general canonical transformation can be realized quantum mechanically as a product of these transformations. Each transformation corresponds to a familiar tool used in solving differential equations, and the procedure of solving a differential equation is systematized by the use of the canonical transformations. Several examples are done to illustrate the use of the canonical transformations. [This is an extensively revised version of hep-th-9205080: the first third of the paper is new material; the notation has been simplified, and further discussion has been added to the remainder.]