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The Journal of Chemical Physics

Resonance fluorescence of a two-level atom near a metal surface

Xi-Yi Huang, Jui‐Teng Lin, Thomas F. George

Published Jan 15, 1984• 31 citations
Publisher

Abstract

A derivation of surface-dressed optical Bloch equations, involving a treatment of surface-reflected photons and a surface plasmon resonance, is presented for a collision-damped two-level atom near or adsorbed on a metal surface. Effects of the laser bandwidth are included by means of a phase-diffusion model for the driving field. In the weak-field or large detuning limit, the population inversion and resonance fluorescence spectrum are analytically obtained. These quantities along with the surface-induced phase-decay constant of the adatom show strong oscillatory behavior as a function of the adatom–surface distance.

DOI
10.1063/1.446747

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Resonance fluorescence of an adatom near solid surfaces

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By using the reservoir theory and Dekker's quantization procedure for a dissipation system, a set of new surface-dressed optical Bloch equations including the surface-induced frequency shift as well as the decay rate is derived to calculate the resonance fluorescence spectrum of an adatom near a bulk solid surface. A mediate layer composed of nonabsorbing dielectric is placed to separate the adatom and the bulk solid. The size and the dielectric effects of this layer are found to be as important as those effects from the bulk solid. These effects will be directly exhibited in the decay rates and the frequency shifts. The resonance fluorescence spectrum is discussed in different cases and is found to be strongly affected by the surfaces.

Physical Review A•Feb 1, 1987•14 citations
A derivation of surface-dressed optical Bloch equations, involving a treatment of surface-reflected photons and a surface plasmon resonance, is presented for a collision-damped two-level atom near or adsorbed on a metal surface. Effects of the laser bandwidth are included by means of a phase-diffusion model for the driving field. In the weak-field or large detuning limit, the population inversion and resonance fluorescence spectrum are analytically obtained. These quantities along with the surface-induced phase-decay constant of the adatom show strong oscillatory behavior as a function of the adatom–surface distance.
A derivation of surface-dressed optical Bloch equations, involving a treatment of surface-reflected photons and a surface plasmon resonance, is presented for a collision-damped two-level atom near or adsorbed on a metal surface. Effects of the laser bandwidth are included by means of a phase-diffusion model for the driving field. In the weak-field or large detuning limit, the population inversion and resonance fluorescence spectrum are obtained analytically. These quantities along with the surface-induced phase-decay constant of the adatom show strong oscillatory behavior as a function of the adatom-surface distance.
Surface-dressed optical Bloch equations are solved for a two-level atom near or adsorbed on a rough surface, which is modeled as a hemispheroid protrusion on a perfectly conducting surface. Effects of the laser bandwidth are included by means of a phase-diffusion model. The presence of the surface roughness generates a dephasing broadening mechanism on the adatomic resonance fluorescence spectrum, which can be strongly enhanced by plasmon resonances depending on the shape of the hemispheroid. The dependence of the electrodynamics of the adatom on the adatom-hemispheroid distance is also evaluated.
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.
The influence of a solid surface on the electronic excitation of a group of two-level adatoms and the associated power spectrum is investigated by means of a nonlinear surface-dressed Bloch equation. In the presence of a surface at a distance from the adatom which is comparable to the optical wavelength, the energy transfer dynamics is inflenced by the following factors: (i) nonradiative energy relaxation of the excited adatom via electron-phonon coupling, (ii) radiative spontaneous decay and stimulated emission caused by both the applied field and the reflected field, (iii) the oscillatory behavior of the adatom lifetime due to the interference between the applied and reflected field, (iv) the reflectivity and refrection index of the surface, (v) dipole dephasing caused by the surface phonons and plasmons, and (vi) interaction among the adatoms.
By using the reservoir theory and Dekker's quantization procedure for a dissipation system, a set of new surface-dressed optical Bloch equations including the surface-induced frequency shift as well as the decay rate is derived to calculate the resonance fluorescence spectrum of an adatom near a bulk solid surface. A mediate layer composed of nonabsorbing dielectric is placed to separate the adatom and the bulk solid. The size and the dielectric effects of this layer are found to be as important as those effects from the bulk solid. These effects will be directly exhibited in the decay rates and the frequency shifts. The resonance fluorescence spectrum is discussed in different cases and is found to be strongly affected by the surfaces.