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Philosophical Transactions of the Royal Society A Mathematical Physical and Engineering Sciences

Gauge and unitary transformations in multipolar quantum optics

M. Babiker

Published Dec 24, 2024• 0 citations
Publisher

Abstract

Multipolar quantum optics deals with the interaction of light with matter as a many-body bound system of charged particles where the coupling to electromagnetic fields is in terms of the multipolar electric polarization and magnetization. We describe two transformations applied to the conventional non-relativistic formalism, namely a gauge transformation applied directly to the fields at the Lagrangian stage and a unitary transformation applied to the old Hamiltonian. We show how such transformations lead to the same Power-Zienau-Woolley (PZW) formulation of the quantum electrodynamics (QED) of an overall electrically neutral many-body bound system of charges, including the internal motion as well as the gross dynamics of the centre of mass. Besides highlighting the utility of the multipolar formalism as a reliable and convenient platform in dealing with optical processes in atomic and molecular physics, it is shown how the analysis can also lead to the identification of the Röntgen effect arising from the gross motion of an electric dipole moment in a magnetic field and the Aharonov-Casher effect due to the motion of a magnetic dipole moment in an electric field. The importance of the two effects is pointed out in both experimental and theoretical contexts.This article is part of the theme issue 'The quantum theory of light'.

DOI
10.1098/rsta.2023.0330

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Multipolar quantum optics deals with the interaction of light with matter as a many-body bound system of charged particles where the coupling to electromagnetic fields is in terms of the multipolar electric polarization and magnetization. We describe two transformations applied to the conventional non-relativistic formalism, namely a gauge transformation applied directly to the fields at the Lagrangian stage and a unitary transformation applied to the old Hamiltonian. We show how such transformations lead to the same Power-Zienau-Woolley (PZW) formulation of the quantum electrodynamics (QED) of an overall electrically neutral many-body bound system of charges, including the internal motion as well as the gross dynamics of the centre of mass. Besides highlighting the utility of the multipolar formalism as a reliable and convenient platform in dealing with optical processes in atomic and molecular physics, it is shown how the analysis can also lead to the identification of the Röntgen effect arising from the gross motion of an electric dipole moment in a magnetic field and the Aharonov-Casher effect due to the motion of a magnetic dipole moment in an electric field. The importance of the two effects is pointed out in both experimental and theoretical contexts.This article is part of the theme issue 'The quantum theory of light'.
This article deals with the fundamental problem of light-matter interaction in the quantum theory. Although it is described through the vector potential in quantum electrodynamics, it is believed by some that a hamiltonian involving only the electric and the magnetic fields is preferable. In the literature this hamiltonian is known as the Power-Zienau-Woolley hamiltonian. We question its validity and show that it is not equivalent to the minimal-coupling hamiltonian. In this article, we show that these two hamiltonians are not connected through a gauge transformation. We find that the gauge is not fixed in the Power-Zienau-Woolley hamiltonian. The interaction term is written in one gauge whereas the rest of the hamiltonian is written in another gauge. The Power-Zienau-Woolley hamiltonian and the minimal-coupling one are related through a unitary transformation that does not fulfill the gauge fixing constraints. Consequently, they predict different physical results. In this letter, we provide the correct quantum theory in the multipolar gauge with a hamiltonian involving only the physical fields.
A system of nonrelativistic charged particles and radiation is canonically quantized in the Coulomb gauge and Maxwell's equations in quantum electrodynamics are derived. By requiring form invariance of the Schrodinger equation under a space and time dependent unitary transformation, operator gauge transformations on the quantized electromagnetic potentials and state vectors are introduced. These gauge transformed potentials have the same form as gauge transformations in non-Abelian gauge field theories. A gauge-invariant method for solving the time-dependent Schrodinger equation in quantum electrodynamics is given. Maxwell's equations are written in a form which holds in all gauges and which has formal similarity to the equations of motion of non-Abelian gauge fields. A gauge-invariant derivation of conservation of energy in quantum electrodynamics is given. An operator gauge transformation is made to the multipolar gauge in which the potentials are expressed in terms of the electromagnetic fields. The multipolar Hamiltonian is shown to be the minimally coupled Hamiltonian with the electromagnetic potentials in the multipolar gauge. The model of a charged harmonic oscillator in a single-mode electromagnetic field is considered as an example. The gauge-invariant procedure for solving the time-dependent Schrodinger equation is used to obtain the gauge-invariant probabilities that the oscillator is in an energy eigenstate For comparison, the conventional approach is also used to solve the harmonic oscillator problem and is shown to give gauge-dependent amplitudes.
The equations of motion and the class of Hamiltonians for electrodynamics, both classical and quantal, are considered for the interaction of radiation with bound charges within the electric-dipole approximation. It is emphasized that, despite the uniqueness of the equations of motion for physical variables, the form of the Hamiltonian is not unique and that a physical system is associated with an equivalence class of Hamiltonians. Two of the members of this class are the minimal-coupling and multipolar forms extensively used in quantum optics. It is shown that although different choices of Hamiltonians lead to different first-order equations of motion that connect canonical coordinates and momenta, they lead to the same second-order equations of motion for the physical variables and physical electromagnetic fields. In the quantum theory of electrodynamics the role played by the choice of representation for the operators and for the states is analyzed with care. The choice of representation leads to a freedom additional to that provided by canonical transformations in classical electrodyamics, although the two lead to the same operator equations of motion.
We revisit the interaction of a first-quantized atomic system (consisting of two charged quantum particles) with the quantum electromagnetic field, pointing out the subtleties related to the gauge nature of electromagnetism and the effect of multipole approximations. We connect the full minimal-coupling model with the typical effective models used in quantum optics and relativistic quantum information such as the Unruh-DeWitt (UDW) model and the dipole coupling approximation. We point out in what regimes different degrees of approximation are reasonable and in what cases effective models need to be refined to capture the features of the light-matter interaction. This is particularly important when considering the center of mass (COM) of the atom as a quantum system that can be delocalized over multiple trajectories. For example, we show that the simplest UDW approximation with a quantum COM fails to capture crucial R\"ontgen terms coupling COM and internal atomic degrees of freedom with each other and the field. Finally we show how effective dipole interaction models can be covariantly prescribed for relativistically moving atoms.
A recent investigation of the interaction between the Maxwell radiation field and neutral atoms or molecules has led us to consider the relation between the straightforward interaction Hamiltonian between particle (k) and the radiation field, and the more physical, and explicitly gauge invariant, couplings of the form q. E and µ. H, etc., where q and µ are the electric and magnetic dipole moments of a system of particles. That these latter form of interaction energies follow from well-formulated approximations for atoms in external fields has been known for many years (Goeppert-Mayer(1); see also Rosenfeld(2)). When the Maxwell field is an internal and dynamical field further discussion is necessary, especially concerning the Coulomb interactions. Their advantage has recently been shown in dealing with dipole interactions in the long range Van der Waals force between two neutral systems where the complete coupling, in dipole approximation, is given by — q.ET for each neutral system, where ET is the transverse electric field. The short-range London limit is contained in this coupling despite the absence of longitudinal electric fields (Power and Zienau (3)). In this note we extend these arguments to higher electric multipoles and magnetic multipoles. We also demonstrate their use in the quantum theory of scattering of light, and in particular the derivations of Stephen (4) of the phase angle between emergent beams in optical double refraction phenomena are shown to follow immediately.
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.