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arXiv:1503.04950 · Annalen der Physik

Nonlinear selective reflection spectroscopy of V‐type atomic system at the gas‐solid interface

Tengfei Meng, Zhonghua Ji, Dianqiang Su, Yanting Zhao, Liantuan Xiao, Suotang Jia

Published Feb 11, 2016• 3 citations
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Abstract

We theoretically present the nonlinear selective reflection spectroscopy of V‐type atomic system at gas‐solid interface in a pump‐probe scheme. The saturation and coherence effects are distinguished by solving Liouville equation in the absence and presence of reduced density matrix element between the two excited levels. When the coherence effect exists, two peaks appear in reflection spectroscopy with asymmetry lineshape. We investigate the dependence of reflection spectroscopy on pump field intensity, frequency detuning and coherent decay rate induced by collision between atoms. The lineshape can be explained based on reflection spectroscopy contributed from atoms with negative (before collision) and positive (after collision) velocities, single‐photon and two‐photon processes. This study is helpful for investigating quantum coherence and dynamic processes of atoms at gas‐solid interface.

DOI
10.1002/andp.201500357

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We theoretically present the nonlinear selective reflection spectroscopy of V‐type atomic system at gas‐solid interface in a pump‐probe scheme. The saturation and coherence effects are distinguished by solving Liouville equation in the absence and presence of reduced density matrix element between the two excited levels. When the coherence effect exists, two peaks appear in reflection spectroscopy with asymmetry lineshape. We investigate the dependence of reflection spectroscopy on pump field intensity, frequency detuning and coherent decay rate induced by collision between atoms. The lineshape can be explained based on reflection spectroscopy contributed from atoms with negative (before collision) and positive (after collision) velocities, single‐photon and two‐photon processes. This study is helpful for investigating quantum coherence and dynamic processes of atoms at gas‐solid interface.
We theoretically and experimentally investigate hyperfine dipole-dipole broadening in the selective reflection (SR) spectroscopy at the gas-solid interface with the atomic density of 10 14 –10 15 cm −3 . The two-level SR theory considering pump beam and dipole-dipole interaction between excited-state atom and ground-state atom is presented. The numerical simulation of the SR spectrum is in agreement with experimental results. The reduction of spectral width is observed by introducing a pump beam which is an effective technique to improve the resolution of spectroscopy. We analyze the dependence of dipole-dipole broadening on atomic density and pump beam power. This study is helpful for the description of the SR spectroscopy at the gas-solid interface where the Doppler broadening is comparable with dipole-dipole broadening.
We report on recent developments in selective reflection spectroscopy at a vapor interface. In FM linear spectroscopy, the long range van der Waals surface interaction, responsible for lineshapes distortions and shifts, is quantitatively well understood with respect to the nature of the dielectric surface. Pump‐probe saturation effects in reflection spectroscopy on a two‐level system offer alternate ways of probing surface interaction, while nonlinear reflection spectrsocopy on a three‐level cascade system provides a unique tool for probing in a vapor cell the velocity distribution of desorbing atoms.
We study the cascade three-level selective-reflection spectroscopy for normal incidence at a dielectric--atomic-vapor interface in a pump-probe scheme. Taking into account the effects of spatial dispersion arising from deexcitation by collisions with the interface and the transient response of atoms leaving the surface, we evaluate the modification of the probe-field reflection induced by the presence of the pump field in terms of a nonlocal nonlinear susceptibility. The dependence of this susceptibility on the probe frequency for various given pump frequencies is calculated. Sub-Doppler structures in the selective reflection spectrum are obtained and analyzed. Potential applications to the study of the interaction of highly excited atomic states with the surface are indicated.
Selective reflection (SR) from the interface between transparent medium and dilute vapour is caused by the atomic vapor near the interface. The sub-Doppler structure in SR is due to the deexcitation caused by the collision between atomic vapor and the wall. Beacuse the interaction region between atomic vapor and incident light is on the order of a few hundred nanometers, SR has low optical loss and high spatial resolution. The experimental device of SR is simple. Because of the above characteristics, the SR has been widely studied and applied. The nonlinear SR spectrum of quasi lambda-type four-level system at gas-solid interface is studied theoretically in this paper. By sloving the density matrix equations, the approximate analytic solution of the matrix element associated with the probe field is obtained at normal incidence when the intensity of the probe field is very weak. The effect of the Rabi frequency, the detuning of the signal field and the detuning of the coupling field on the lineshape are analyzed by numerical simulation, respectively. Three peaks and two transparent windows appear in SR spectrum when the detuning of coupling field and signal field are both zero. The middle peak is generated due to the participation of signal field, and the other two peaks are caused by the other two fields. The linewidth and the amplitude of the middle peak can be changed by varying the Rabi frequency of signal field, and the other two peaks have little effect on the Rabi frequency of signal field. The signal generated due to the participation of signal field can be transformed from peak to transparent window when the detuning value of the signal field is equal to the Rabi frequency of coupling field. When the detuning value of the signal field is not equal to the Rabi frequency of coupling field, a dispersion-like signal between reflection peak and transparent window is generated due to the participation of signal field. The position of peak and transparent window can be manipulated by controlling the detuning value of the coupling field. When the detuning value of coupling field decreases from zero, three peaks all shift to red detuning direction. When the detuning value of coupling field is blue-detuned and increases, three peaks all shift to blue detuning direction. The numerical results can be explained by using the various electric transition pathways and dressed state theory. This study is helpful in investigating quantum coherence and dynamic process of atoms at gas-solid interface.
Special hole-burning effects on the spectrum of gas atoms near a glass–vapour interface were obtained by observing the reflection of a weak probe beam. Sub-Doppler reflection spectroscopy has been achieved and the unabsorption dip was measured for different pump laser power and detuning. The nonlinear optical properties of the atomic system were investigated by taking into account the collisions between the atoms and the walls of the cell. We also demonstrated the absorption reduction in a V-type energy level configuration with a linewidth of about 6.5 MHz. The experimental results agree with reasonable accuracy with the predictions derived from a theoretical explanation of the nonlinear optical susceptibility.
We present an experimental study of nonlinear selective reflection at a dielectric--Cs-vapor interface, in a three-level cascade-up scheme. The nonlinear reflection at the Cs D2{\mathit{D}}_{2}D2​ resonance line is monitored in the presence of resonant irradiation at 621 nm or 658 nm (6P3/2{\mathit{P}}_{3/2}P3/2​\ensuremath{\rightarrow}8D5/2{\mathit{D}}_{5/2}D5/2​,9S1/2{\mathit{S}}_{1/2}S1/2​). Experimental reflection spectra with either counterpropagating or copropagating light beams are analyzed and compared with the theoretical predictions of F. Schuller et al. [Phys. Rev. A 47, 519 (1993)]. For a blue-detuned pump and copropagating geometry an alternative type of three-level coherent reflection resonances, specifically associated with desorbing atoms, is observed. Also observed is the nonlinear reflection associated with the off-resonant, two-photon dispersion of atoms moving parallel to the window surface. Probe beam saturation is responsible for the appearance of additional resonant features in reflection spectra. Finally we analyze crossover spectral resonances which arise from nondegenerate, four-wave-mixing processes induced by the combined influence of counterpropagating pump and probe beams, and the pump beam being partially reflected by the window.