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Optics Letters

Frequency shifts and lifetime changes of sodium atoms near rough metal surfaces

Frank Balzer, Vladimir G Bordo, Horst‐Günter Rubahn

Published Aug 15, 1997• 8 citations
Publisher

Abstract

Two-photon laser-induced fluorescence measurements of transition frequencies and lifetimes of laser-excited Na atoms are presented as a function of distance (2-3nm) to metal surfaces of different roughness. We characterized the surface roughness by fitting a Gaussian height-height correlation function to force microscopic data. An unusually small red shift of the Na transition frequency of a few hundred megahertz was observed. In the framework of a quantum-mechanical linear optical response formalism we fitted the lifetime and the frequency shift data simultaneously to obtain effective parameters of a selvedge dielectric function. In that way we are able to take into account both surface roughness and nonlocality, which in turn result in the observed small frequency shifts.

DOI
10.1364/ol.22.001262

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Two-photon laser-induced fluorescence measurements of transition frequencies and lifetimes of laser-excited Na atoms are presented as a function of distance (2-3nm) to metal surfaces of different roughness. We characterized the surface roughness by fitting a Gaussian height-height correlation function to force microscopic data. An unusually small red shift of the Na transition frequency of a few hundred megahertz was observed. In the framework of a quantum-mechanical linear optical response formalism we fitted the lifetime and the frequency shift data simultaneously to obtain effective parameters of a selvedge dielectric function. In that way we are able to take into account both surface roughness and nonlocality, which in turn result in the observed small frequency shifts.
Abstract : The photon correlations of resonance fluorescence emitted by a degenerate two-level atom near a metal surface are studied. An intense non monochromatic optical laser drives a low lying atomic transition, and the emitted fluorescence is detected by a photon counter. An expression for the spontaneous decay operator is derived, and it appears that the various substates of the upper level have a different lifetime due to the presence of the surface, or equivalently, due to the loss of spherical symmetry. The temporal photon correlation function is then evaluated in terms of a photon-emission operator and the time evolution operator for the atomic density matrix. The general theory is exemplified with a detailed elaboration of the j sub g = 0 yields j sub e = 1 transition, for which the two-photon correlation is obtained explicitly as a function of the lifetime A(h), depending on the atom surface distance h, the laser linewidth, the detuning from resonance, and the dipole-coupling strength with the external field. Keywords: Photon correlations; Resonance fluorescence; Atom near metal surface; Loss of spherical symmetry; Substates; Different lifetimes.
The photon correlations of resonance fluorescence emitted by a degenerate two-level atom near a metal surface are studied. An intense non-monochromatic optical laser drives a low-lying atomic transition, and the emitted fluorescence is detected by a photon counter. An expression for the spontaneous decay operator is derived, and it appears that the various substates of the upper level have a different lifetime due to the presence of the surface, or equivalently, due to the loss of spherical symmetry. The temporal photon correlation function is then evaluated in terms of a photon-emission operator and the time evolution operator for the atomic density matrix. The general theory is exemplified with a detailed elaboration of the j/sub g/ = 0 yields j/sub e/ = 1 transition, for which the two-photon correlation is obtained explicitly as a function of the lifetime A(h), depending on the atom surface distance h, the laser linewidth, the detuning from resonance, and the dipole-coupling strength with the external field.
The photon correlations of resonance fluorescence emitted by a degenerate two-level atom near a metal surface are studied. An intense nonmonochromatic optical laser drives a low-lying atomic transition, and the emitted fluorescence is detected by a photon counter. An expression for the spontaneous-decay operator is derived, and it appears that the various substates of the upper level have a different lifetime due to the presence of the surface, or equivalently, due to the loss of spherical symmetry. The temporal photon correlation function is then evaluated in terms of a photon-emission operator and the time-evolution operator for the atomic density matrix. The general theory is exemplified with a detailed elaboration of the jg{j}_{g}jg​=0\ensuremath{\rightarrow}je{j}_{e}je​=1 transition, for which the two-photon correlation is obtained explicitly as a function of the inverse lifetime A(h), depending on the atom-surface distance h, the laser linewidth, the detuning from resonance, and the dipole-coupling strength with the external field.
The resonance fluorescence spectrum of two atoms near a perfectly conducting metal is investigated. A quantum-mechanical version of the image method, taking into account the dipole-dipole interaction, is adopted to study the excitation spectrum. Within the framework of this approach, each single atom and its corresponding image are kinematically correlated, while dynamically they are actually independent. The effects of the surface are directly exhibited in the decay rates, the frequency shift, and the spectrum. The influence of the surface is found to be large for weak fields but becomes very small for high intensities of the pump field.
By means of the linear response method, the surface-dressed optical Bloch equations (SBE) for atoms absorbed on a solid surface are obtained. These SBE are different from the earlier oxies. The difference-lies in the fact that here the influences of the solid surface on the spontaneous decay rate and the Lamb shift of the adsorbed atoms have been taken into account. Using the SBE and the regression theorem, the resonance fluorescence spectrum for the adatoms are obtained. Through analyzing these spectrum numerically, it is found that the solid surface will exert a significant influences both on the sidebands and peak hights. Namely, when the adatoms approach the surface, the distance between the two sidebands will become larger and the height for each peak will go down until the peaks disappear one by one.