Abstract The Thomas–Reiche–Kuhn (TRK) sum rule is a fundamental consequence of the position–momentum commutation relation for an atomic electron, and it provides an important constraint on the transition matrix elements for an atom. Here, we propose a TRK sum rule for electromagnetic fields which is valid even in the presence of very strong light–matter interactions and/or optical nonlinearities. While the standard TRK sum rule involves dipole matrix moments calculated between atomic energy levels (in the absence of interaction with the field), the sum rule here proposed involves expectation values of field operators calculated between general eigenstates of the interacting light–matter system. This sum rule provides constraints and guidance for the analysis of strongly interacting light–matter systems and can be used to test the validity of approximate effective Hamiltonians often used in quantum optics.
Abstract The Thomas–Reiche–Kuhn (TRK) sum rule is a fundamental consequence of the position–momentum commutation relation for an atomic electron, and it provides an important constraint on the transition matrix elements for an atom. Here, we propose a TRK sum rule for electromagnetic fields which is valid even in the presence of very strong light–matter interactions and/or optical nonlinearities. While the standard TRK sum rule involves dipole matrix moments calculated between atomic energy levels (in the absence of interaction with the field), the sum rule here proposed involves expectation values of field operators calculated between general eigenstates of the interacting light–matter system. This sum rule provides constraints and guidance for the analysis of strongly interacting light–matter systems and can be used to test the validity of approximate effective Hamiltonians often used in quantum optics.
The Thomas-Reiche-Kuhn (TRK) sum rule is a fundamental consequence of the position-momentum commutation relation for an atomic electron, and it provides an important constraint on the transitionmatrix elements for an atom. Here, we propose a TRK sum rule for electromagnetic fields which is valid even in the presence of very strong light- matter interactions and/or optical nonlinearities. While the standard TRK sum rule involves dipole matrix moments calculated between atomic energy levels (in the absence of interaction with the field), the sum rule here proposed involves expectation values of field operators calculated between general eigenstates of the interacting light-matter system. This sum rule provides constraints and guidance for the analysis of strongly interacting light-matter systems and can be used to test the validity of approximate effective Hamiltonians often used in quantum optics.
Some new sum rules for atomic transition probabilities are developed; they are similar to the well-known rule of Kuhn, Reiche, and Thomas. They give, if unpolarized light is incident on any gaseous element in any given discrete energy level, the total absorption, excitation plus ionization, with various types of frequency weighting. The results are similar to those of Dirac and Harding, but are more general in that they apply to any discrete state of any atom, rather than to the ground state of hydrogen only. The method differs from that of Dirac and Harding.
Spontaneous light emission is central to a vast range of physical systems and is a founding pillar for the theory of light–matter interactions. In the presence of complex photonic media, the description of spontaneous light emission usually requires advanced theoretical quantum optics tools such as macroscopic quantum electrodynamics, involving quantized electromagnetic fields. Although rigorous and comprehensive, the complexity of such models can obscure the intuitive understanding of many quantum-optical phenomena. Here, we review a method for calculating spontaneous emission and other quantum-optical processes without making explicit use of quantized electromagnetic fields. Instead, we introduce the concept of transition currents, comprising charges in matter that undergo transitions between initial and final quantum states. We show how predictions that usually demand advanced methods in quantum electrodynamics or quantum optics can be reproduced by feeding these transition currents as sources to the classical Maxwell equations. One then obtains the relevant quantum observables from the resulting classical field amplitudes, without washing out quantum optical effects. We show that this procedure allows for a straightforward description of quantum phenomena, even when going beyond the dipole approximation and single emitters. As illustrative examples, we calculate emission patterns and Purcell-enhanced emission rates in both bound-electron and free-electron systems. For the latter, we derive cathodoluminescence emission and energy-loss probabilities of free electrons interacting with nanostructured samples. In addition, we calculate quantum-beat phenomena in bound-electron systems and wave function-dependent optical coherence in free-electron systems. Remarkably, the transition-current formalism captures more complex phenomena, such as many-body interference effects and super-radiance of both bound- and free-electron systems, second-order processes such as two-photon emission, and quantum recoil corrections to free-electron radiation. We review a variety of light–matter interactions in fields ranging from electron microscopy to nanophotonics and quantum optics, for which the transition-current theoretical formalism facilitates practical simulations and a deeper understanding of novel applications.
Spatially-structured laser beams, eventually carrying orbital angular momentum, affect electronic transitions of atoms and their motional states in a complex way. We present a general framework, based on the spherical tensor decomposition of the interaction Hamiltonian, for computing atomic transition matrix elements for light fields of arbitrary spatial mode and polarization structures. We study both the bare electronic matrix elements, corresponding to transitions with no coupling to the atomic center-of-mass motion, as well as the matrix elements describing the coupling to the quantized atomic motion in the resolved side-band regime. We calculate the spatial dependence of electronic and motional matrix elements for tightly focused Hermite-Gaussian, Laguerre-Gaussian and for radially and azimuthally polarized beams. We show that near the diffraction limit, all these beams exhibit longitudinal fields and field gradients, which strongly affect the selection rules and could be used to tailor the light-matter interaction. The presented framework is useful for describing trapped atoms or ions in spatially-structured light fields and therefore for designing new protocols and setups in quantum optics, -sensing and -information processing. We provide open code to reproduce our results or to evaluate interaction matrix elements for different transition types, beam structures and interaction geometries.
Theoretical concepts and framework for describing nonlinear light-matter interactions are the subject of this chapter. A density matrix approach is introduced for describing the nonlinear optical response of quantum systems to an electromagnetic field. Starting with the full description, different approximations are introduced and their limitations discussed from the viewpoint of physics. Basic concepts such as quantum coherences in multi-level systems, nonlinear currents, and nonperturbative light-matter interactions are explained and illustrated by model calculations.
This chapter discusses light–matter interactions from a semiclassical point of view. By expanding the electromagnetic field into a Taylor series we derive the multipolar interaction potential and particle-field Hamiltonian. Then, using the Green function formalism, we calculate the fields of an oscillating dipole and, based on Poynting’s theorem, derive a general expression for the rate of energy dissipation in an arbitrary environment. This expression leads to the concept of local density of states (LDOS) and provides a direct link to spontaneous emission and atomic decay rates. The rate of energy dissipation of an oscillating dipole is also used to derive the absorption cross-section in terms of the polarizability. By accounting for radiation reaction and scattering losses, we obtain a compact expression for the dynamic polarizability. Dipole radiation and atomic decay rates can be enhanced via LDOS engineering, and the enhancement factor is referred to as the Purcell factor. We show that if the LDOS gets enhanced in a certain frequency range, it must be reduced in other frequency ranges, a feature described by the LDOS sum rule. After discussing the properties of a single dipole, we continue with analyzing the interaction between multiple dipoles. We derive the interaction potential and calculate the energy transfer rate between dipoles. For short distances we recover the famous Förster energy transfer formula. If the interaction energy becomes sufficiently large, we enter the regime of strong coupling, which gives rise to hybridized and delocalized modes, level splittings, and entanglement.