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Resonant atomic interactions: nonreciprocal and nonconservative forces, and radiative properties of excited atoms

Julio Sánchez Cánovas

Published Jan 1, 2025• 0 citations
Publisher

Abstract

The quantum description of the electromagnetic (EM) field, even in the absence of sources, reveals that the vacuum exhibits fluctuations in the energy and of the components of the field, known as quantum vacuum fluctuations. The coupling of these quantum fluctuations of the vacuum to electric charges leads to experimentally observable phenomena, such as the spontaneous emission of an excited atom, the Lamb effect, the Casimir effect, and the van der Waals interactions, which have been historically fundamental for the confirmation of the existence of these fluctuations. The optical response of simple atoms and the EM interaction between two atoms constitute the simplest realistic phenomena for studying these effects. This thesis focuses on the fundamental study of the properties of interatomic interactions, addressing aspects such as their dependence on the interatomic distance, their time dependence, and the emergence of nonreciprocal interatomic forces due to parity breaking. In particular, the detailed analysis of the electric dipole forces in a system of two atoms, one of which is initially excited, is carried out, along with the study of the implication of the resonant interactions in the appearance of collective effects in absorption and emission processes of many-atom systems. Due to the inherently time-dependent nature of the resonant forces between excited atoms, a time-dependent Hamiltonian approach is employed. The atomic interaction processes are represented with time-ordered diagrams. It is obtained that the atoms are subjected to resonant conservative forces, directed along the interatomic axis, which exert a net force on the system. This result implies an apparent violation of the action-reaction principle due to the lack of conservation of the kinetic momentum of the atoms. However, this net force on the atomic system is compensated by the time derivative of the transversal momentum of the EM field, associated with the resonant photons that mediate the interaction, ensuring the conservation of the total momentum of the system. In addition to these conservative forces, there are nonconservative forces which are a consequence of the time derivative of the so-called longitudinal momentum of the electromagnetic field and contain components perpendicular to the interatomic axis. We analyze the particular case of the interaction between identical atoms. In this scenario, the net force on the system becomes time-dependent. Furthermore, states with degenerate energy arise and evolve coherently through the periodic transfer of resonant photons between the atoms. This implies that in these degenerate states, there are contributions from interatomic interactions that cannot be expressed as an energy shift in the atomic wave functions. Consequently, these interactions give rise to collective phenomena observable in photon absorption and emission processes. At the same time, the strength of these forces is markedly superior to that calculated for different atoms, which makes this scenario a more favorable set-up for the experimental observation of the nonreciprocal forces and the associated coherent phenomena. Concerning collective effects and their application in the design of multi-atomic qubits, these phenomena have significant implications for the scalability and connectivity of such systems. To describe these collective properties, we have formulated a Hamiltonian that incorporates both the interaction processes, i.e., those that give rise to dynamic coherence and incoherence effects, and the stationary interaction processes that renormalize the energy of the atomic states. It is found that the photon absorption probability is determined by the ratio between the interatomic interaction and the intensity of the laser that excites the system. On the other hand, the spontaneous emission of photons is proportional to the number of decay channels, which decrease when the interatomic interaction between excited states breaks the degeneracy in the subspaces associated with the same number of excitations.

DOI
10.35376/10324/75876

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The quantum description of the electromagnetic (EM) field, even in the absence of sources, reveals that the vacuum exhibits fluctuations in the energy and of the components of the field, known as quantum vacuum fluctuations. The coupling of these quantum fluctuations of the vacuum to electric charges leads to experimentally observable phenomena, such as the spontaneous emission of an excited atom, the Lamb effect, the Casimir effect, and the van der Waals interactions, which have been historically fundamental for the confirmation of the existence of these fluctuations. The optical response of simple atoms and the EM interaction between two atoms constitute the simplest realistic phenomena for studying these effects. This thesis focuses on the fundamental study of the properties of interatomic interactions, addressing aspects such as their dependence on the interatomic distance, their time dependence, and the emergence of nonreciprocal interatomic forces due to parity breaking. In particular, the detailed analysis of the electric dipole forces in a system of two atoms, one of which is initially excited, is carried out, along with the study of the implication of the resonant interactions in the appearance of collective effects in absorption and emission processes of many-atom systems. Due to the inherently time-dependent nature of the resonant forces between excited atoms, a time-dependent Hamiltonian approach is employed. The atomic interaction processes are represented with time-ordered diagrams. It is obtained that the atoms are subjected to resonant conservative forces, directed along the interatomic axis, which exert a net force on the system. This result implies an apparent violation of the action-reaction principle due to the lack of conservation of the kinetic momentum of the atoms. However, this net force on the atomic system is compensated by the time derivative of the transversal momentum of the EM field, associated with the resonant photons that mediate the interaction, ensuring the conservation of the total momentum of the system. In addition to these conservative forces, there are nonconservative forces which are a consequence of the time derivative of the so-called longitudinal momentum of the electromagnetic field and contain components perpendicular to the interatomic axis. We analyze the particular case of the interaction between identical atoms. In this scenario, the net force on the system becomes time-dependent. Furthermore, states with degenerate energy arise and evolve coherently through the periodic transfer of resonant photons between the atoms. This implies that in these degenerate states, there are contributions from interatomic interactions that cannot be expressed as an energy shift in the atomic wave functions. Consequently, these interactions give rise to collective phenomena observable in photon absorption and emission processes. At the same time, the strength of these forces is markedly superior to that calculated for different atoms, which makes this scenario a more favorable set-up for the experimental observation of the nonreciprocal forces and the associated coherent phenomena. Concerning collective effects and their application in the design of multi-atomic qubits, these phenomena have significant implications for the scalability and connectivity of such systems. To describe these collective properties, we have formulated a Hamiltonian that incorporates both the interaction processes, i.e., those that give rise to dynamic coherence and incoherence effects, and the stationary interaction processes that renormalize the energy of the atomic states. It is found that the photon absorption probability is determined by the ratio between the interatomic interaction and the intensity of the laser that excites the system. On the other hand, the spontaneous emission of photons is proportional to the number of decay channels, which decrease when the interatomic interaction between excited states breaks the degeneracy in the subspaces associated with the same number of excitations.
We perform a time-dependent quantum computation of the van der Waals interaction between two free identical atoms, one of which is initially excited. Making use of the perturbative approach developed in Refs. It is shown that, in addition to an off-resonant interaction force between the two atoms, the two-atom system is subjected to a net force which oscillates periodically in time. We prove that the apparently missing momentum is carried by the resonant photons which mediate the periodic transfer of the excitation between the atoms, guaranteeing this way the satisfaction of the action-reaction principle in the quantum realm. Remarkably, since mediating photons remain virtual throughout the process, their momentum is virtual and thus unaccessible experimentally. Ultimately, as the de-excitation of the system takes place, that momentum turns into actual when carried off by the real photon which is emitted spontaneously. Hence, the directionality of such an emission constitutes a vestige of the net force acting upon the two-atom system while excited.
An atomic electron, in the vacuum of photons, can emit and reabsorb photons of any frequency. Such processes give rise to well known radiative corrections (Lamb—shift, g — 2, natural width of excited states...). We review in this paper similar effects which can be induced by the interaction of an atomic electron with an incident electromagnetic wave, and we try to get some physical insight in radiative processes by comparing these two types of « spontaneous » and « induced » effects. Optical pumping methods have been very useful for studying how atoms are perturbed by optical or RF photons. The Zeeman sublevels of an atomic ground state are broadened and shifted by a resonant or quasiresonant optical irradiation. The corresponding light-shifts (or « Lamp-shifts » as A. Kastler called them) are due to virtual absorptions and reemissions of incident photons. Another example of an induced effect is the modification of the magnetic properties of an atomic level due to a high frequency non resonant RF irradiation. The Larmor precession is slowed down and becomes anisotropic. The two previous examples correspond to two situations leading to simple calculations. For a resonant or quasiresonant excitation, a single atomic transition needs to be considered. Non perturbative treatments can be given which include the effect of the atom field coupling to all orders. For example, the « dressed atom » approach allows a unified treatment of various effects such as light shifts, Autler-Townes doublets resonance fluorescence triplets... On the other hand, for a high frequency irradiation, all atomic transitions must be included. It is possible in this case to derive an effective hamiltonian describing, to lowest order in the fine structure constant α, how electronic energy levels are perturbed in the presence of N photons ω. The remaining part of the paper is devoted to the analysis of such a situation. The terms of the effective hamiltonian proportional to the number N of incident photons correspond to the induced effects. They can be fully interpreted in semiclassical terms and they describe how the slow motion of the electron in the external static fields is modified by the high frequency vibration in the incident monochromatic wave. For example, the vibrating electron averages the static potential over a finite length, the angular oscillation of the spin reduces the effective magnetic moment. The remaining terms, which are independent of N, exist even in the vacuum of photons (N = 0) and describe the contribution of the mode ω to spontaneous radiative corrections. It is possible to split them into two parts. The first one has the same structure as the N-dependent terms, with N replaced by 1/2. It describes the corrections due to the vibration of the electron in vacuum fluctuations which have a spectral power density ħω/2 per mode. The second part represents the effect of radiation reaction, i.e. the interaction of the electron with its self field. Such an interpretation is confirmed by a Heisenberg equations approach where the total force acting upon the electron is split into two physical (i.e. hermitian) parts representing respectively the effect of the vacuum « free » field and the effect of the « source » field produced by the electron itself. These considerations are finally applied to the problem of the positive sign of g - 2. The g-factor can be written as 2 ωL/ωc, where ω L is the Larmor frequency of the spin and ωc the cyclotron frequency of the charge for an electron in a weak static field B 0. In the absence of radiative corrections, g = 2, and ω L = ωc. To lowest order in 1/c (order zero), radiation reaction slows down ωc but not ωL (a charge is more coupled to its self field than a magnetic moment). The effect of vacuum fluctuations appears only at order 2 in 1/c and corresponds to relativistic and magnetic effects which slow down both ωL and ωc. Therefore, it appears that, in the non relativistic domain, the main effect is a reduction of ωc by radiation reaction and this explains why 2 ωL/ωc becomes larger than 2. A complete relativistic calculation (to all orders in 1/ c, but to lowest order in α) does not change this conclusion since the contribution of non relativistic modes (ħω < mc2) is predominant in the integral giving g — 2.
The dynamical and radiative features of an excited system of two identical atoms are analyzed. The metastability of the system, the directionality of its emission, and its internal forces are studied. Closed-form expressions are derived for the time propagator of the system, for the angular distribution of its spontaneous emission, and for its internal dipole forces, both conservative and nonconservative. The latter reveals the presence of nonreciprocal forces, which leads to a net time-dependent force upon the system. We estimate that, for a free binary system of Li Rydberg atoms, the net internal force may cause a displacement of its center of mass as large as 120 nm over a lifetime.
A net force on a system of two dissimilar atoms, one of which is excited, is shown to result from their van der Waals interaction. It is accompanied by a net transfer of linear momentum to the quantum fluctuations of the electromagnetic field. This momentum results from the asymmetric interference of the virtual photons scattered off each atom along the interatomic direction, which is in itself a manifestation of the optical theorem. Ultimately, the virtual photons' momentum, of equal strength and opposite direction to the momentum gained by the two-atom system while excited, is released through directional spontaneous emission, which allows for an indirect measure, a posteriori, of the total force on the excited system. A quantitative prediction is made in a two-alkali atom system. It is conjectured that a net force and hence a nonzero momentum of quantum fluctuations take place in any asymmetrically excited system.
The Rabi Hamiltonian, describing the interaction between a two-level atomic system and a single-cavity mode of the electromagnetic field, is one of the fundamental models in quantum optics. The model becomes exactly solvable by considering an atom without permanent dipole moments, whose excitation energy is quasiresonant with the cavity photon energy, and by neglecting the nonresonant (counter-rotating) terms. In this case, after including the decay of either the atom or the cavity mode to a continuum, one can derive the well-known phenomenology of quasiresonant transitions, including the fluorescence triplets. In this work we consider the most general Rabi model, incorporating the effects of permanent atomic electric dipole moments. Based on a perturbative analysis, we compare the intensities of emission lines induced by rotating terms, counter-rotating terms, and parity-symmetry-breaking terms in order to identify the parameter regimes in which these different contributions play a significant role. The analysis reveals that the emission strength related to the existence of permanent dipoles may surpass the one due to the counter-rotating interaction terms but is usually much weaker than the emission due to the main, resonant coupling. This ratio can be modified in systems with a reduced dimensionality or by engineering the energy spectral density of the continuum.
The usual form of electromagnetic forces is given by but for neutral atoms q = 0. The next order of force is the dipole term, but this also vanishes because neutral atoms have no inherent dipole moment. However, a dipole moment can be induced by a field, and this is most efficient if the field is alternating near the atomic resonance frequency. Since these frequencies are typically in the optical range, dipole moments are efficiently induced by shining nearly resonant light on the atoms. Laser cooling and trapping rely on the interaction between laser light and atoms to exert a controllable force on the atoms, and many sophisticated schemes have been developed using the special properties of the interaction. This chapter begins with the simplest schemes for exerting optical forces on atoms, namely a single-frequency light field interacting with a two-level atom. Although this is the simplest possible scheme, it is pedagogically valuable because it shows many of the features that will be encountered further on. The ultimate temperature using such a scheme is limited, but lower temperatures can be achieved with multilevel atoms. This topic is addressed later in the chapter. Two kinds of optical forces When an atom absorbs nearly resonant light, it makes a transition to the excited state, and its subsequent return to the ground state can be either by spontaneous or by stimulated emission. The nature of the optical force that arises from these two different processes is quite different, and will be described separately [1]. The spontaneous emission case is different from the familiar quantum mechanical calculations using state vectors to describe the state of the system, because spontaneous emission causes the state of the system to evolve from a pure state into a mixed state (see Exercise 6.9). Spontaneous emission is an essential ingredient for the dissipative nature of the optical forces in monochromatic light, and the density matrix is needed to describe it (see Chap. 6). When an atom absorbs light, its energy excites the atom and its angular momentum changes the electron's orbit. Both of these are internal atomic properties. However, the linear momentum of the light, can change only the external, translational motion of the atom.