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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Spectrum of resonance fluorescence excited by an evanescent wave at a gas-solid interface

Vladimir G Bordo

Published Jul 21, 1994• 0 citations
Publisher

Abstract

We present the results of a theoretical investigation of the fluorescence spectrum from the gas of two-level atoms strongly driven by an evanescent wave (EW). The mean time-of-flight of atoms across the EW is supposed to be less than the relaxation times in the gas volume. Assuming the atomic absorption line to be Doppler-broadened we analyze two specific cases: (1) the atoms over the whole Doppler contour are excited by the EW in the adiabatic-following regime and (2) the EW 'burns out the hole' inside the absorption line. In case (1) in addition to the well- known Mollow triplet the line at the atomic transition frequency appears due to the transient behavior of the atoms departing the surface. In case (2) the spectrum has a sub-Doppler structure sensitive to the type of the atom-surface scattering (diffuse, specular or inelastic). In both cases the spectrum depends on the sticking probability and phases of the scattering in the ground and excited states.

DOI
10.1117/12.180839

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We present the results of a theoretical investigation of the fluorescence spectrum from the gas of two-level atoms strongly driven by an evanescent wave (EW). The mean time-of-flight of atoms across the EW is supposed to be less than the relaxation times in the gas volume. Assuming the atomic absorption line to be Doppler-broadened we analyze two specific cases: (1) the atoms over the whole Doppler contour are excited by the EW in the adiabatic-following regime and (2) the EW 'burns out the hole' inside the absorption line. In case (1) in addition to the well- known Mollow triplet the line at the atomic transition frequency appears due to the transient behavior of the atoms departing the surface. In case (2) the spectrum has a sub-Doppler structure sensitive to the type of the atom-surface scattering (diffuse, specular or inelastic). In both cases the spectrum depends on the sticking probability and phases of the scattering in the ground and excited states.
The effect of collisions on the resonance fluorescence spectrum of two-level atoms excited by monochromatic resonance radiation is studied. Analysis is performed for systems where the Doppler broadening is small compared to the collision frequency (high buffer gas pressures) and for the general case where collisions arbitrarily change the phase of the radiation-induced dipole moment (from completely interrupted to completely unaffected phase of the dipole moment). Both at a relatively low and at a high excitation radiation intensity, the resonance fluorescence spectrum is shown to depend on whether the two-level system is closed or open. This is especially true for the narrow unshifted Rayleigh scattering line. It is shown that, although the absorption line is homogeneously broadened, the resonance fluorescence spectrum exhibits a clearly pronounced anisotropy. In a direction close to the direction of propagation of the excitation radiation, the Rayleigh scattering line is maximally narrowed. Under certain conditions (that can easily be created in experiments), the width of this line is proportional to the diffusion coefficient of atoms interacting with the radiation.
The effect of collisions on the resonance fluorescence spectrum of three-level atoms with a V-configuration of levels when excited by two monochromatic resonance fields has been theoretically investigated. The analysis has been carried out for the systems with a small Doppler broadening compared to the collision frequency (high buffer gas pressures) and for the general case of an arbitrary change (from complete failure to complete preservation) of the phase memory at any of the three transitions in the V-system. It has been shown that in the three-level V-type atoms excited by two monochromatic fields, the resonant fluorescence spectrum (the number of spectral lines and their widths) at one of the transitions strongly depends on the presence of resonant radiation at the adjacent transition. Under certain conditions, the line widths will be completely determined by the relaxation characteristics of the adjacent transition and, in particular, can be repeatedly narrowed with an increase in the radiation intensity at the adjacent transition. It has been shown that despite the homogeneous nature of the broadening of the absorption lines, the resonance fluorescence spectrum has a pronounced anisotropy with respect to the mutual orientation of the wave vectors of spontaneous and exciting radiation. It has been established that the line widths in the resonance fluorescence spectrum are proportional to the diffusion coefficient of the atoms interacting with radiation under certain conditions. This fact can serve as the basis for a spectroscopic method for measuring the transport frequencies of the collisions of the radiation-absorbing particles with the buffer ones. It has been shown that the effects of phase memory in the collisions lead to a strong qualitative and quantitative modification of the resonance fluorescence spectrum.
The relaxation process and resonance fluorescence of a two-level atom strongly driven by stochastically fluctuating laser light is studied. A laser with small intensity fluctuations about a constant mean value and a diffusing phase is assumed. Depending on the relative time scales of the intensity fluctuations and the atomic response to these fluctuations, the time decay of the atomic population is found to be non-exponential. The broadening of the sidebands in the triplet spectrum of resonance fluorescence is shown to be non-Lorentzian.
The effect of the laser linewidth on the resonance fluorescence spectrum of a two-level atom is revisited. The novel spectral features, such as hole-burning and dispersive profiles at line centre of the fluorescence spectrum are predicted when the laser linewidth is much greater than its intensity. The unique features result from quantum interference between different dressed-state transition channels. c # 1999 Elsevier Science B.V. PACS : 42.50.Hz; 32.80.-t Keywords: Resonance fluorescence; Laser linewidth; Quantum interference The study of resonance fluorescence spectra has provided much fundamental insight into the subject of atom1light interactions. It is well known that for weak laser field excitation, the spectrum exhibits a Lorentzian lineshape, whereas it develops into the Mollow triplet for strong field excitation [1]. The latter is a direct signature of stimulated emissions and absorptions of the atom during the time interval for one spontaneous decay. Recently, considera...
The two-photon spectrum of sodium atoms, excited by two counterpropagating evanescent waves, is investigated both experimentally and theoretically. Sub-Doppler linewidths are observed, which are quantitatively reproduced by a rigorous theoretical approach that takes into account optical pumping and transit time broadening due to the translational motion of the arriving and departing atoms through the evanescent-wave fields. The velocity distribution of the atoms desorbing from the surface is found to obey a cosine law, which has a significant influence on the observed line shapes.
Using a cw dye laser beam normally incident on a glass-Na-vapor interface, fluorescence excitation spectra of the D1{D}_{1}D1​ line are measured. By observing the fluorescence transmitted into the glass above the angle of total reflection, only evanescent light emitted within about a wavelength distance from the interface is observed. The measured spectra show a cutoff on the high-frequency side which is direct evidence for the transient behavior of the induced polarization of resonantly excited vapor atoms which have collided at the solid interface.