Resonance fluorescence of a two-level atom near a metal surface. 2. Case of a strong driving field

Abstract

helpful discussions; Melinda W. Certain for assistance in some of our derivations; Kay Kilcoyne and Cathy Ryan for their excellent typing; and Betty Hirschfelder for her critical proofreading. AppendixExpressions for Exact Density Matrix Elements of Semiclassical Two-Level Systems. The general expression for the density matrix, eq 1.33, can be specialized to the case of a two-level system. Taking the initial condition to be poo(to=O) = 1, and performing some algebraic simplifications, we obtainIn these expressions the summation variables range over all positive and negative integer values, including zero. Note that para = 1 ppp and Im (pag) is not required. It is sometimes convenient to restrict one's attention to the long-time averages of the density matrix elements, defined as Performing this average on eq A1 gives ( P p p ) = I T (a,2klx+)IZ~I(P,21+1 lx+)12 + IC k (~, 2 k 1~-) 1~~1 ( P , 2 1 + 1 Ix-)Iz (A4) while (~~0 ) = 0. We refer to ( p a p ) as the "saturation".The surface-dressed optical Bloch equations for a two-level atom near a metal surface are solved for the case of a strong driving field. An analytic form is obtained for the adatomic resonance fluorescence spectrum. Due to the multiphoton effects of the surface-reflected field and the surface plasmon resonance, the three-peak spectrum is strongly influenced by the surface. A unique surface-induced asymmetry in the side peaks is revealed.

Photodissociation of molecules at structured metallic surfaces

“…3 that at -the plasmon resonance one can still have a large enhancement in the cross section even at distances far from the surface. This might be the crucial justification for the observation of Ehrlich and Osgood, 13who found that an appreciable amount of molecular dissociation occurs already in the gas phase * far above the substrate for Cd(CH ) 2 but not for Al (CH).…”

Theory of laser-induced phenomena on conventional and phase-conjugated surfaces

“…1 for the case of a silver surface. 8 The key feature, which is a unique behavior due to the surface, is that for certain atom-surface distances H is larger than H+, whereas in the pure gas-phase ,.…”