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Physical Review A

Collision-induced Ramsey resonances in Sm vapor

Egbert Buhr, J. Mlynek

Published Sep 1, 1987• 9 citations
Publisher

Abstract

We report detailed studies of Ramsey-type resonances due to collisional velocity diffusion of Sm atoms within the Doppler-broadened $^{7}\mathrm{F}_{1}$\ensuremath{\rightarrow}${\mathrm{}}^{7}$${\mathrm{F}}_{0}$ $^{154}\mathrm{Sm}$ transition at \ensuremath{\lambda}=570.68 nm in the presence of rare-gas perturbers (He,Ne,Ar,Kr,Xe). The experimental technique uses counterpropagating laser fields and relies on coherent resonance Raman processes to excite and detect sublevel coherence optically. A modulated pump laser field is used for velocity-selective resonance Raman excitation of oscillating Zeeman coherence in the J=1 ground state of Sm; the sublevel coherence is monitored by Raman heterodyne detection using a counterpropagating, unmodulated probe laser field. If the pump and probe fields interact with different atomic velocity subgroups, a signal only occurs in the presence of velocity-changing collisions which provide a transport of the Sm atoms with sublevel coherence in velocity space. The sublevel resonance curves turn out to be sensitive to both depolarizing and velocity-changing collisions; the measured line shapes show the characteristic features of Ramsey-type resonances. Our theoretical treatment is based on a novel four-level density matrix calculation; the analysis reveals that the temporal evolution of the collisional velocity-diffusion processes can simply be obtained by means of a Fourier transformation of the measured sublevel resonance curves. In the case of He perturbers the diffusion in velocity space can be described by a Fokker-Planck equation; here, the theoretical fits of the measured sublevel resonance curves directly yield the time constant for collisional thermalization and the cross section for depolarizing collisions. In the case of the heavier rare gases, however, the Fokker-Planck model fails to describe the velocity thermalization; here, the Keilson-Storer kernel yields a better agreement with the experimental data. We derive cross sections for depolarizing and velocity-changing collisions and values for the collisional velocity changes associated with orientation-preserving collisions.

DOI
10.1103/physreva.36.2684

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We report detailed studies of Ramsey-type resonances due to collisional velocity diffusion of Sm atoms within the Doppler-broadened 7F1^{7}\mathrm{F}_{1}7F1​\ensuremath{\rightarrow}{\mathrm{}}^{7}$${\mathrm{F}}_{0} 154Sm^{154}\mathrm{Sm}154Sm transition at \ensuremath{\lambda}=570.68 nm in the presence of rare-gas perturbers (He,Ne,Ar,Kr,Xe). The experimental technique uses counterpropagating laser fields and relies on coherent resonance Raman processes to excite and detect sublevel coherence optically. A modulated pump laser field is used for velocity-selective resonance Raman excitation of oscillating Zeeman coherence in the J=1 ground state of Sm; the sublevel coherence is monitored by Raman heterodyne detection using a counterpropagating, unmodulated probe laser field. If the pump and probe fields interact with different atomic velocity subgroups, a signal only occurs in the presence of velocity-changing collisions which provide a transport of the Sm atoms with sublevel coherence in velocity space. The sublevel resonance curves turn out to be sensitive to both depolarizing and velocity-changing collisions; the measured line shapes show the characteristic features of Ramsey-type resonances. Our theoretical treatment is based on a novel four-level density matrix calculation; the analysis reveals that the temporal evolution of the collisional velocity-diffusion processes can simply be obtained by means of a Fourier transformation of the measured sublevel resonance curves. In the case of He perturbers the diffusion in velocity space can be described by a Fokker-Planck equation; here, the theoretical fits of the measured sublevel resonance curves directly yield the time constant for collisional thermalization and the cross section for depolarizing collisions. In the case of the heavier rare gases, however, the Fokker-Planck model fails to describe the velocity thermalization; here, the Keilson-Storer kernel yields a better agreement with the experimental data. We derive cross sections for depolarizing and velocity-changing collisions and values for the collisional velocity changes associated with orientation-preserving collisions.
We report on the observation of novel Ramsey-type resonances due to collisional velocity diffusion in atomic samarium vapor in the presence of rare-gas perturbers. The experimental technique uses counterpropagating laser fields and relies on coherent resonance Raman processes to optically excite and detect sublevel coherence within the Doppler-broadened 154Sm^{154}\mathrm{Sm}154Sm $\ensuremath{\lambda}=570.68$-nm $^{7}F_{1}\ensuremath{-}^{7}F_{0}$ transition. The experimental findings are in good agreement with theoretical predictions based on a Fokker-Planck equation; time constants for the collisional thermalization of Sm in He and Ne atmospheres are derived from our data.
We report new results on the effect of collisions on radio-frequency (rf) -laser double resonances in an atomic vapor under conditions of velocity-selective optical pumping. Our experiments are performed on Zeeman resonances in the 4${f}^{6}666{s}^{2}$ 7{\mathrm{}}^{7}7F1{F}_{1}F1​--4${f}^{6}$6s6p 7{\mathrm{}}^{7}7F0{F}_{0}F0​ transition in samarium vapor in the presence of rare-gas perturbers (He, Ne, Ar, Xe). The collisional relaxation of the rf-generated sublevel coherence is studied using Raman heterodyne detection; this recently introduced spectroscopic technique is capable of separately yielding signal contributions originating from optically resonant and off-resonant atoms. The corresponding measurements clearly reveal that velocity-changing collisions (VCC) can completely determine the characteristics of the rf-laser double-resonance signals. Our experimental findings on the linewidths and line shapes of the rf resonances are in satisfactory quantitative agreement with theoretical predictions that are based on a novel four-level density-matrix calculation; here a Keilson-Storer collision kernel is used to describe the velocity diffusion processes. The comparison of calculated and measured results also permits us to derive cross sections for VCC and depolarizing collisions; moreover, information on the spectrum of the velocity changes connected with alignment-preserving collisions can be obtained.
Optical pumping performed with a quasi monochromatic laser beam in an atomic gas introduces a redistribution of Zeeman populations selectively in a single velocity class. In the limit of low pumping intensity the rate theory is valid for a description of velocity-selective optical pumping (V.S.O.P.). Well-defined atomic observables (population, orientation, alignment) and their velocity-correlated collisional relaxation can be studied. Also, a modified scheme for the detection of second order effects of optical pumping allows one to observe light shift induced signals. In particular, V.S.O.P. and its combination with modulated pumping, magnetic depolarization (level crossing), and magnetic resonance techniques provide information about the atomic collision characteristics such as collision rates and kernels for velocity-changing collisions.
We investigate the evolution of the atomic coherence between Zeeman sublevels with $\ensuremath{\Delta}{m}_{F}=2$ in the region between pump and probe laser beams, in a Rb vapor cell using the Hanle configuration. The transmission of the probe beam, placed inside the hollow pump beam, shows the narrowing of the Hanle resonance (at external magnetic field B=0B=0B=0) by Ramsey fringes whose separation from the central peak depends on the distance between the beams. The temporal evolution of the pump induced alignment is evident from the changes of the probe transmission spectra with increasing the angle between linear polarizations of each beam. Experimental results are in agreement with the results of the model which calculates probe fluorescence by solving time-dependent optical Bloch equations, from the time when atom enters the pump beam to the time when it leaves the probe beam. The results for total excited state populations were averaged over atomic velocities distribution.
Optical four-wave mixing resonances in sodium vapor induced by collisions with inert buffer gases (He, Ar, Xe, N2{\mathrm{N}}_{2}N2​) are characterized at high resolution ( 5 MHz) using lasers tuned near the DDD lines of Na. These resonances are interpreted in terms of coherent scattering from a population grating established by collisional absorption of the incident radiation. The roles of homogeneous and inhomogeneous contributions to the resonance line shapes are clarified. The line shapes exhibit structure sharper than the predicted linewidth, that characteristic of the 3P3P3P-to-3S3S3S transition rate. We show that this is caused by collision-induced optical pumping which introduces the ground-state lifetime into the grating relaxation physics. These long-lived gratings are exemplified dramatically by experiments in the presence of N2{\mathrm{N}}_{2}N2​ which collisionally quenches the Na 3P3P3P states. Similar results are obtained in Xe where it is argued that excimer formation with the 3P3P3P states plays a role in the population dynamics. Model calculations of the effects of sodium level degeneracy on the grating dynamics are presented to support these conclusions. Finally we present data illustrating interference between the collision-induced population grating resonances detailed here and collision-induced coherent Raman resonances between Zeeman sublevels of the ground state.