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arXiv:1603.08195 · Physical Review A

Two-atom interaction energies with one atom in an excited state: van der Waals potentials versus level shifts

M. Donaire

Published May 16, 2016• 19 citations

Abstract

I revisit the problem of the interaction between two dissimilar atoms with one atom in an excited state, recently addressed by Berman [Phys. Rev. A 91, 042127 (2015)], Donaire et al. [Phys. Rev. Lett. 115, 033201 (2015)], and Milonni and Rafsanjani [Phys. Rev. A 92, 062711 (2015)], for which precedent approaches have given conflicting results. In the first place, I discuss to what extent these works provide equivalent results. I show that the phase-shift rate of the two-atom wave function computed by Berman, the van der Waals potential of the excited atom by Donaire et al., and the level shift of the excited atom by Milonni and Rafsanjani possess equivalent expressions in the quasistationary approximation. In addition, I show that the level shift of the ground-state atom computed by Milonni and Rafsanjani is equivalent to its van der Waals potential. A diagrammatic representation of all those quantities is provided. The equivalences among them are, however, not generic. In particular, it is found that for the case of the interaction between two identical atoms excited, the phase-shift rate and the van der Waals potentials differ. Concerning the conflicting results of previous approaches in regards to the spatial oscillation of the interactions, I conclude, in agreement with Berman and with Milonni and Rafsanjani, that they refer to different physical quantities. The impacts of free-space dissipation and finite excitation rates on the dynamics of the potentials are analyzed. In contrast with Milonni and Rafsanjani, the oscillatory versus monotonic spatial forms of the potentials of each atom are found not to be related to the reversible versus irreversible nature of the excitation transfer involved.

DOI: 10.1103/physreva.93.052706

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I revisit the problem of the interaction between two dissimilar atoms with one atom in an excited state, recently addressed by Berman [Phys. Rev. A 91, 042127 (2015)], Donaire et al. [Phys. Rev. Lett. 115, 033201 (2015)], and Milonni and Rafsanjani [Phys. Rev. A 92, 062711 (2015)], for which precedent approaches have given conflicting results. In the first place, I discuss to what extent these works provide equivalent results. I show that the phase-shift rate of the two-atom wave function computed by Berman, the van der Waals potential of the excited atom by Donaire et al., and the level shift of the excited atom by Milonni and Rafsanjani possess equivalent expressions in the quasistationary approximation. In addition, I show that the level shift of the ground-state atom computed by Milonni and Rafsanjani is equivalent to its van der Waals potential. A diagrammatic representation of all those quantities is provided. The equivalences among them are, however, not generic. In particular, it is found that for the case of the interaction between two identical atoms excited, the phase-shift rate and the van der Waals potentials differ. Concerning the conflicting results of previous approaches in regards to the spatial oscillation of the interactions, I conclude, in agreement with Berman and with Milonni and Rafsanjani, that they refer to different physical quantities. The impacts of free-space dissipation and finite excitation rates on the dynamics of the potentials are analyzed. In contrast with Milonni and Rafsanjani, the oscillatory versus monotonic spatial forms of the potentials of each atom are found not to be related to the reversible versus irreversible nature of the excitation transfer involved.

We present a time-dependent quantum calculation of the van der Waals interaction between a pair of dissimilar atoms, one of which is initially excited while the other one is in its ground state. For small detuning, the interaction is predominantly mediated at all distances by the exchange of doubly resonant photons between the two atoms. We find that it presents both temporal and spatial oscillations. Spatially oscillating terms depend on the resonant frequencies of both atoms, while the frequency of the time oscillations is given by their detuning. We analyze the physical content of our findings and discuss to what extent previous conflicting stationary approaches provide compatible results. A proper account of causality is found essential in order to obtain the correct result.

We compute the conservative van der Waals forces between two atoms, one of which is initially excited, in the limit of identical atoms. Starting with the perturbative calculation of the interaction between two dissimilar atoms, we show that a time-dependent approach in the weak-interaction approximation is essential in considering the identical-atom limit in the perturbative regime. In this limit we find that, at leading order, the van der Waals forces are fully resonant and grow linearly in time, being different upon each atom. The resultant net force upon the two-atom system is related to the directionality of spontaneous emission, which results from the violation of parity symmetry. The strength of this force is much greater than that found in dissimilar atoms, raising the possibility of its experimental detection. In contrast to the usual stationary van der Waals forces, the time-dependent conservative forces cannot be written as the gradients of the expectation values of the interaction potentials, but as the expectation values of the gradients of the interaction potentials only.

We present a formula for the body-assisted van der Waals interaction potential between two atoms, one or both being prepared in an excited energy eigenstate. The presence of an arbitrary arrangement for a material environment is taken into account via the Green function. The resulting formula supports one of two conflicting findings recorded. The consistency of our formula is investigated by applying it for the case of two atoms in free space and comparing the resulting expression with the one found from the limiting Casimir-Polder potential between an excited atom and a small dielectric sphere.

van der Waals interactions between atoms and dielectric surfaces are reinvestigated. To describe the nonretarded interaction potential between a dispersive dielectric surface and an atom in an arbitrary internal energy state, we derive a general expression in terms of an integral, over real frequency, of the combined atom and surface polarizabilities. It is shown that, for excited atoms, the expression is equivalent to the one obtained by Wylie and Sipe [Phys. Rev. A 32, 2030 (1985)]. We thus demonstrate how to extend this approach to excited atoms interacting with birefringent dielectrics. For isotropic dielectrics, a method of integration in closed form allows us to derive an approximate formula for the van der Waals interaction constant in terms of resonance frequencies and oscillator strengths of both the atom and the dielectric. Frequency-dependent ``dielectric reflection'' coefficients are introduced for virtual atomic dipole couplings either in absorption or in emission. In absorption, the reflection coefficient is always positive and smaller than unity. In emission, it may take arbitrary values, positive or negative (corresponding to van der Waals repulsion). Such a behavior is shown to be related to resonant excitation exchange between the atomic system and the dielectric medium, when an atomic transition frequency gets in resonance with a dielectric absorption band. Numerical calculations performed for the cesium-sapphire system are shown to be in good agreement with data obtained by selective-reflection spectroscopy. Finally, experimental tests of the birefringent character of the sapphire response are discussed.

The interaction of two excited hydrogen atoms in metastable states constitutes a theoretically interesting problem because of the quasidegenerate

2{P}_{1/2}

levels that are removed from the

2S

states only by the Lamb shift. The total Hamiltonian of the system is composed of the van der Waals Hamiltonian, the Lamb shift, and the hyperfine effects. The van der Waals shift becomes commensurate with the $2S\ensuremath{-}2{P}_{3/2}$ fine-structure splitting only for close approach (

R<100{a}_{0}

, where

{a}_{0}

is the Bohr radius) and one may thus restrict the discussion to the levels with

n=2

and

J=1/2

to a good approximation. Because each

S

or

P

state splits into an

F=1

triplet and an

F=0

hyperfine singlet (eight states for each atom), the Hamiltonian matrix a priori is of dimension 64. A careful analysis of the symmetries of the the problem allows one to reduce the dimensionality of the most involved irreducible submatrix to 12. We determine the Hamiltonian matrices and the leading-order van der Waals shifts for states that are degenerate under the action of the unperturbed Hamiltonian (Lamb shift plus hyperfine structure). The leading first- and second-order van der Waals shifts lead to interaction energies proportional to

1/{R}^{3}

and

1/{R}^{6}

and are evaluated within the hyperfine manifolds. When both atoms are metastable

2S

states, we find an interaction energy of order ${E}_{h}\ensuremath{\chi}{({a}_{0}/R)}^{6}$, where

{E}_{h}

and

\mathcal{L}

are the Hartree and Lamb shift energies, respectively, and $\ensuremath{\chi}={E}_{h}/\mathcal{L}\ensuremath{\approx}6.22\ifmmode\times\else\texttimes\fi{}{10}^{6}$ is their ratio.

We have made a quantitative study of quantum electrodynamic corrections to the atomic energy levels between parallel conducting mirrors. Within the framework of simple two-level atoms, we evaluate the level shifts numerically and discuss the van der Waals, Casimir, and cavity-resonant radiative shifts as their asymptotic forms. In particular, we find that the level shifts of an excited state are substantially different not only from those of a classical dipole radiator but also from those of an excited atom near a single mirror. For the ground state, however, the shifts are qualitatively similar to those near a single mirror. We also apply the results to some simple atomic systems that may be used to test the cavity QED theory.