A quantum theory of nonlinear phenomena is considered in which account is taken of all contributions from electric and magnetic multipoles, without any multipolar approximation. Exact closed analytical expressions for the multipoles are first obtained from quantum electrodynamics by applying a generalization of the Power-Zienau transformation. The standard procedure is invoked to calculate general electromagnetic susceptibility tensors ${\ensuremath{\chi}}_{\ensuremath{\mu}\ensuremath{\nu}{\ensuremath{\alpha}}_{1}{\ensuremath{\beta}}_{1}\ensuremath{\cdots}{\ensuremath{\alpha}}_{n}{\ensuremath{\beta}}_{n}}^{[n]}$ (${\ensuremath{\omega}}_{1}, \dots{}, {\ensuremath{\omega}}_{n}$). Such a tensor is a shorthand for the electric and magnetic susceptibilities as well as mixed susceptibilities. By considering a relativistic theory based on the Dirac equation, the spin susceptibilities are automatically included. The formalism in this way allows for the computation of a wide range of electro- and magneto-optical effects to any order of perturbation and to any order of multipolar approximation.
A quantum theory of nonlinear phenomena is considered in which account is taken of all contributions from electric and magnetic multipoles, without any multipolar approximation. Exact closed analytical expressions for the multipoles are first obtained from quantum electrodynamics by applying a generalization of the Power-Zienau transformation. The standard procedure is invoked to calculate general electromagnetic susceptibility tensors \ensuremathχ\ensuremathμ\ensuremathν\ensuremathα1\ensuremathβ1\ensuremath⋯\ensuremathαn\ensuremathβn[n] (\ensuremathω1,…,\ensuremathωn). Such a tensor is a shorthand for the electric and magnetic susceptibilities as well as mixed susceptibilities. By considering a relativistic theory based on the Dirac equation, the spin susceptibilities are automatically included. The formalism in this way allows for the computation of a wide range of electro- and magneto-optical effects to any order of perturbation and to any order of multipolar approximation.
Abstract This book is unique in covering phenomena in photon- matter interactions in a unified way over a range of many orders in energy. The quantum field theoretic approach to the fully relativistic theory of quantum electrodynamics (QED) is presented together with the non- relativistic theory in both confined and unconfined geometries. The predictions of QED have been verified to a greater accuracy than any other physical theory. Moreover QED is a paradigm for other gauge theories and is presented in such a way that the generalisation to other gauge theories is natural. Gauge and Poincare symmetry properties and the non-existence of a photon wave function are thoroughly discussed. Starting from the Dirac equation the non-relativistic interaction of the electron with the electromagnetic field is derived as an effective Hamiltonian of multipole expansions. Much of quantum optics is based on the lowest order dipole approximation. From this point on the treatment of fully relativistic QED and quantum optics is done in parallel. Applications of perturbation theory such as Compton and Moller scattering and the theory photdetection are given. After the impressive successes of QED, the limitation of the theory and the necessity of electroweak theory and quantumchromodynamics are discussed. The remaining chapters are devoted to quantum optics inside cavaties. Various approaches to open systems such as master equations are discussed within the context of active systems (e.g. the laser) and passive systems. Semi- classical approximarions are shown to imply a rich non- linear dynamics including chaos for certain parameter regimes. The effect of fluctuations on such non-linear dynamics is also studied. The final chapter is devoted to highly non- classical states of the light field such as photon number, squeezed and two photon entangled states. The latter are studied for the important system of parametric down conversion and the localisation properties of photons are characterised in terms of asympotic tails in photodetection probabilities as a function of time delay. The range of the book has wider benefits. Workers in quantum optics will gain a deeper understanding of the foundations of their subject and field theorists will see concrete examples of open systems, which are beginning to impinge on fundamental theories.
In earlier chapters we have considered in detail the susceptibility formalism of nonlinear optics, which is perhaps the most familiar approach and has a wide range of application. Starting from the constitutive relations of Chapter 2, the susceptibility formalism is quite general. In many practical applications, a particular phenomenon can be described accurately by a single order of nonlinearity, and the susceptibility then provides a useful and convenient description. However, this is not always the case. Some of the most interesting phenomena in nonlinear optics involve close resonance with the transition frequencies of the medium, and perhaps also the use of very intense optical fields. As remarked in §4.5, in these circumstances the resonant susceptibilities display mathematical divergences which are clearly unphysical. Strictly, these divergences occur only because higher-order nonlinearities have been neglected. Successive orders of nonlinearity take into account such effects as saturation, power broadening and level shifts (optical Stark effect). For intense fields or very close resonance, the contributions from several orders of nonlinearity may be comparable in magnitude. Therefore, despite its generality, the susceptibility formalism does not necessarily provide the most practical approach for the description of resonant processes. This chapter is concerned with the problem of deriving alternative and more manageable descriptions of resonant nonlinear processes, illustrated by examples. For much of the chapter, the nonlinear medium is treated as a two-level system (described in §6.2).
Starting with well known formulae for nth-order atomic susceptibilities, irreducible spherical tensor techniques and Racah algebra are used to put these in a form suitable for the treatment of complex nonlinear processes, e.g. where fine and hyperfine interactions can be included and the interacting fields can have quite general polarizations. By way of illustration the susceptibilities are calculated in detail for third harmonic generation and Raman scattering in alkali vapours, taking into account the effect of spin-orbit coupling.
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.
A generalization of Dirac's transformation of the off-resonance single-photon scattering amplitude that leads to the Kramers-Heisenberg dispersion formula is described. The amplitude is first calculated to order e2 in perturbation theory with the minimal-coupling interaction Hamiltonian as perturbing energy, and is then transformed so that the effects of multipole transition moments of all orders and types (electric, magnetic, and diamagnetic) readily become manifest. No appeal is made to any multipolar expansions, however, as exact integral expressions are used for the summed series. It is shown that the same dispersion formula is obtained by using the multipolar Hamiltonian partitioned in the usual way, and this despite the fact that the unperturbed Hamiltonians are different in the two calculations.
In this paper, we derive a quantum optics model in a non-inertial rotating ring cavity from first principles. We begin with the Dirac equation in curved spacetime, add minimal coupling to the electromagnetic field, and then find the Dirac Hamiltonian for the generalized Born metric. We then formally take the non-relativistic limit by way of Foldy-Wouthuysen transformations and project onto a fermionic Fock space for the atoms' electrons, protons, and neutrons. Focusing on a protium atom, we next move from a minimal coupling gauge to a multipole expansion gauge by taking a Power-Zienau-Woolley transformation under the dipole and long-wavelength approximations. Here, we find additional terms from the rotation of the system including a rotation-induced hyperfine shift of the atomic transition which could possibly be observed experimentally even for small rotation rates. Making the electric dipole, two-level, and rotating-wave approximations, we arrive at a Jaynes-Cummings-like Hamiltonian which also accounts for rotational effects, such as the rotation-induced hyperfine shift and the Sagnac shift for the cavity's counterpropagating modes.