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Topical Meeting on Microphysics of Surfaces, Beams, and Adsorbates

Excitation of Interacting Adatoms and Surface-Dressed Bloch Equation

Jui‐Teng Lin

Published Jan 1, 1985• 0 citations
Publisher

Abstract

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.

DOI
10.1364/msba.1985.tub3

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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.
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.
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.
Spontaneous-emission properties and resonance fluorescence for a two-level adatom near the surface of a semi-infinite superlattice with quasiperiodic structure are studied by use of surface-dressed optical Bloch equations and Maxwell's equations. Effects of dielectric properties and the geometric structure of this superlattice on spontaneous-decay rate and frequency shift, resonance-fluorescence spectrum, time evolution of adatomic inversion, and fluctuations of the dipole moment for this adatom are discussed and some novel phenomena are discovered.
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.
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Adsorbed atoms on the surface of a harmonic lattice are immersed in a strong laser field. The optical Bloch equations are derived, which include the thermal relaxation and the coherent excitation of the adbond. This is accomplished by a transformation to dressed states, which diagonalizes the interaction with the laser. The single-phonon couplings are then understood as transitions between dressed states. The radiative contributions for arbitrarily strong fields are obtained in the master equation, and it is shown that the coherences with respect to the dressed states decay exponentially, due to the phonon relaxation. General properties of the competing phonon-induced redistribution and optical excitation of the level populations are presented, and exemplified by an explicit elaboration of a three-level system. The results are amenable to analytical evaluation once the interaction potential is prescribed, and extensions of the approach to include multiphonon processes are straightforward.