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arXiv:1709.05875 · New Journal of Physics

A master equation for strongly interacting dipoles

Adam Stokes, Ahsan Nazir

Published Feb 27, 2018• 25 citations
arXivHTMLPDF

Abstract

We consider a pair of dipoles such as Rydberg atoms for which direct electrostatic dipole–dipole interactions may be significantly larger than the coupling to transverse radiation. We derive a master equation using the Coulomb gauge, which naturally enables us to include the inter-dipole Coulomb energy within the system Hamiltonian rather than the interaction. In contrast, the standard master equation for a two-dipole system, which depends entirely on well-known gauge-invariant S -matrix elements, is usually derived using the multipolar gauge, wherein there is no explicit inter-dipole Coulomb interaction. We show using a generalised arbitrary-gauge light-matter Hamiltonian that this master equation is obtained in other gauges only if the inter-dipole Coulomb interaction is kept within the interaction Hamiltonian rather than the unperturbed part as in our derivation. Thus, our master equation depends on different S -matrix elements, which give separation-dependent corrections to the standard matrix elements describing resonant energy transfer and collective decay. The two master equations coincide in the large separation limit where static couplings are negligible. We provide an application of our master equation by finding separation-dependent corrections to the natural emission spectrum of the two-dipole system.

DOI
10.1088/1367-2630/aab29d

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We consider a pair of dipoles such as Rydberg atoms for which direct electrostatic dipole–dipole interactions may be significantly larger than the coupling to transverse radiation. We derive a master equation using the Coulomb gauge, which naturally enables us to include the inter-dipole Coulomb energy within the system Hamiltonian rather than the interaction. In contrast, the standard master equation for a two-dipole system, which depends entirely on well-known gauge-invariant S -matrix elements, is usually derived using the multipolar gauge, wherein there is no explicit inter-dipole Coulomb interaction. We show using a generalised arbitrary-gauge light-matter Hamiltonian that this master equation is obtained in other gauges only if the inter-dipole Coulomb interaction is kept within the interaction Hamiltonian rather than the unperturbed part as in our derivation. Thus, our master equation depends on different S -matrix elements, which give separation-dependent corrections to the standard matrix elements describing resonant energy transfer and collective decay. The two master equations coincide in the large separation limit where static couplings are negligible. We provide an application of our master equation by finding separation-dependent corrections to the natural emission spectrum of the two-dipole system.
A quantum dipole interacting with an optical cavity is one of the key models in cavity quantum electrodynamics (cavity-QED). To treat this system theoretically, the typical approach is to truncate the dipole to two levels. However, it has been shown that in the ultrastrong-coupling regime, this truncation naively destroys gauge invariance. By truncating in a manner consistent with the gauge principle, we introduce master equations to compute gauge-invariant emission spectra and quantum correlation functions which show significant disagreement with previous results obtained using the standard quantum Rabi model, with quantitative differences already present in the strong coupling regime. Explicit examples are shown using both the dipole gauge and the Coulomb gauge.
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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.
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We revisit the derivation of Rabi- and Dicke-type models, which are commonly used for the study of quantum light-matter interactions in cavity and circuit QED. We demonstrate that the validity of the two-level approximation, which is an essential step in this derivation, depends explicitly on the choice of gauge once the system enters the ultrastrong-coupling regime. In particular, while in the electric dipole gauge the two-level approximation can be performed as long as the Rabi frequency remains much smaller than the energies of all higher-lying levels, it can dramatically fail in the Coulomb gauge, even for systems with an extremely anharmonic spectrum. We extensively investigate this phenomenon both in the single-dipole (Rabi) and multidipole (Dicke) case, and consider the specific examples of dipoles confined by double-well and square-well potentials, and of circuit QED systems with flux qubits coupled to an LC resonator.
The calculation of the natural lineshape of an excited two-level system (TLS) has long been known to be gauge dependent, with experiments and classical predictions in better agreement with the lineshape calculated with the dipole gauge ($\ensuremath{-}\mathbf{r}\ifmmode\cdot\else\textperiodcentered\fi{}\mathbf{E}$ coupling). We show that by using a Coulomb-gauge ($\mathbf{p}\ifmmode\cdot\else\textperiodcentered\fi{}\mathbf{A}$ coupling) Hamiltonian truncated in a manner consistent with the gauge principle, the correct output spectrum can, in fact, be obtained. For TLSs undergoing dynamics arising from additional Hamiltonian couplings, we also show that the master equation is gauge invariant under the same conditions of validity as the Markov approximation, despite different gauges having different spectral densities. These results highlight the importance of using correctly truncated gauge-invariant Hamiltonians in input-output theory for accurate frequency-dependent spectra, even in weak-coupling regimes.