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arXiv:0901.3084 · Physical Review A

Atomic multipole relaxation rates near surfaces

J. A. Crosse, Stefan Scheel

Published Jun 18, 2009• 20 citations
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Abstract

The spontaneous relaxation rates for an atom in free space and close to an absorbing surface are calculated to various orders of the electromagnetic multipole expansion. The spontaneous decay rates for dipole, quadrupole, and octupole transitions are calculated in terms of their respective primitive electric multipole moments and the magnetic relaxation rate is calculated for the dipole and quadrupole transitions in terms of their respective primitive magnetic multipole moments. The theory of electromagnetic-field quantization in magnetoelectric materials is used to derive general expressions for the decay rates in terms of the dyadic Green's function. We focus on the decay rates in free space and near an infinite half space. For the decay of atoms near to an absorbing dielectric surface, we find a hierarchy of scaling laws depending on the atom-surface distance $z$.

DOI
10.1103/physreva.79.062902

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The spontaneous relaxation rates for an atom in free space and close to an absorbing surface are calculated to various orders of the electromagnetic multipole expansion. The spontaneous decay rates for dipole, quadrupole, and octupole transitions are calculated in terms of their respective primitive electric multipole moments and the magnetic relaxation rate is calculated for the dipole and quadrupole transitions in terms of their respective primitive magnetic multipole moments. The theory of electromagnetic-field quantization in magnetoelectric materials is used to derive general expressions for the decay rates in terms of the dyadic Green's function. We focus on the decay rates in free space and near an infinite half space. For the decay of atoms near to an absorbing dielectric surface, we find a hierarchy of scaling laws depending on the atom-surface distance zzz.
Quadrupole radiation of an atom in an arbitrary environment is investigated within classical as well as quantum electrodynamical approaches. Analytical expressions for decay rates are obtained in terms of the Green's function of Maxwell equations. The equivalence of both approaches is shown. General expressions are applied to analyze the quadrupole decay rate of an atom placed between two half spaces with arbitrary dielectric constant. It is shown that in the case where the atom is close to the surface, the total decay rate is inversely proportional to the fifth power of distance between an atom and a plane interface.
The structure of spontaneous decay of atoms in the vicinity of a surface is shown to be determined by spatial symmetries. The spontaneous-decay operator for a degenerate two level atom is derived, and with symmetry considerations the number of free parameters is reduced to two. Only the dimensionless and normalized inverse lifetimes b-parallel and b-perpendicular for a parallel and perpendicular dipole moment with respect to the surface, respectively, enter the expression for the relaxation operator for any atom near any surface. These two parameters incorporate the atom-surface-distance dependence of all Einstein coefficients for spontaneous decay, and all optical properties of the substrate material. It is shown that the specific features of spontaneous decay are mainly geometrical, and a consequence of symmetries of the vacuum radiation field, irrespective of the presence of the atom. With an example, it is shown how the parameters b-parallel and b-perpendicular can be calculated in a particular case. It is also pointed out that an explicit quantization of the radiation field can be avoided, even though the process of spontaneous emission is purely quantum mechanical.
Abstract : Optical properties of an atom in the vicinity of a metal or dielectric are different from those in free space. The spontaneous decay of an atom with two degenerate levels is studied, where the relaxation operator is obtained as a function of the atom-surface separation and the complex bulk dielectric constant epsilon(omega). The Einstein coefficient A(m)(e) of an excited state jeme appears to depend on the magnetic quantum number me. A sum rule for A(m)(e) is derived, and from the rotational symmetry with respect to the surface normal it is found that A(m)(e) = A(-m)(e). A general expression for the fluorescent radiation field in the far zone is then derived, which incorporates the polarization properties of the fluorescence, as they are modified by the presence of the dielectric. It is shown that the angular distribution of the emitted intensity depends strongly on epsilon(omega), and it is pointed out how information about the substrate, e.g., epsilon(omega), can be extracted from the temporal statistical behavior of the emitted photons. It is emphasized that the major surface effects are purely geometrical, despite the essential quantum nature of the problem. Keywords: Spontaneous decay, Atomic fluorescence, Atom near metal surface, Absorbing dielectric, Einstein coefficient, Magnetic quantum number.
Optical properties of an atom in the vicinity of a metal or dielectric are different from those in free space. The spontaneous decay of an atom with two degenerate levels is studied, where the relaxation operator is obtained as a function of the atom-surface separation and the complex bulk dielectric of an excited state \ensuremath{\Vert}je{j}_{e}je​me{m}_{e}me​〉 appears to depend on the magnetic is derived, and from the rotational symmetry with respect to the surface normal it is found . A general expression for the fluorescent radiation field in the far zone is then derived, which incorporates the polarization properties of the fluorescence, as they are modified by the presence of the dielectric. It is shown that the angular distribution of the emitted intensity depends strongly on \ensuremath{\epsilon}(\ensuremath{\omega}), and it is pointed out how information about the substrate, e.g., \ensuremath{\epsilon}(\ensuremath{\omega}), can be extracted from the temporal statistical behavior of the emitted photons. It is emphasized that the major surface effects are purely geometrical, despite the essential quantum nature of the problem.
The lifetime of an excited atom near an absorbing dielectric surface is calculated from an exact solution of a microscopic Hamiltonian model, which includes the effects of dispersion, local-field correction, and near-field Coulomb interaction. Results for the total decay rate are shown to be in excellent agreement with those based on classical electromagnetic theory and to yield the well-known result for the rate of nonradiative energy transfer in the limit of very small distance from the surface. \textcopyright{} 1996 The American Physical Society.
We present calculations of the rates of decay of an excited atom embedded in an absorbing dielectric. Decay can occur by spontaneous emission into transverse radiative modes of the electromagnetic field and by Joule heating via longitudinal coupling of the atom to the dielectric. The spontaneous emission (transverse) decay rate is modified in a dielectric, being the free-space rate multiplied by the real part of the refractive index at the transition frequency of the atom. There is a further modification due to the difference between the macroscopic dielectric field and the local field at the position of the atom. In addition there is a longitudinal decay rate which is proportional to the imaginary part of the dielectric constant and therefore vanishes in non-absorbing media. We derive expressions for each of these rates of decay and discuss the physical mechanisms leading to them.