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Physical Review A

Collisional relaxation of excited-state Zeeman coherences in atomic ytterbium vapor

Arjun G. Yodh, J. E. Golub, THOMAS W. MOSSBERG

Published Aug 1, 1985• 19 citations
Publisher

Abstract

We present the results of an experiment designed to probe the collision-induced relaxation of excited-state Yb Zeeman coherences. Our experiment is sensitive not only to the depolarization-type relaxation mechanisms often observed in optical-pumping experiments, but also to the effects of collisionally induced velocity changes. Our measurements were performed in the 6s6p ${\mathrm{}}^{3}$${P}_{1}$ excited state of the even (I=0) isotopes of gas-phase atomic Yb by means of a trilevel photon-echo technique. Depolarization rates, velocity-change spectra, and total scattering cross sections of Yb-He (Yb-Ar) collisions were measured (deduced). Both rank-1 and rank-2 spherical tensor components of the $^{3}\mathrm{P}_{1}$ state play a role in our experiment, and our results represent averages of potentially different relaxation rates attributable to these quantities. Comparison of our results with rank-0 results obtained elsewhere reveals interesting similarities as well as differences.

DOI
10.1103/physreva.32.844

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Journal of Experimental and Theoretical Physics Letters•Mar 1, 2008•14 citations
We present the results of an experiment designed to probe the collision-induced relaxation of excited-state Yb Zeeman coherences. Our experiment is sensitive not only to the depolarization-type relaxation mechanisms often observed in optical-pumping experiments, but also to the effects of collisionally induced velocity changes. Our measurements were performed in the 6s6p {\mathrm{}}^{3}$${P}_{1} excited state of the even (I=0) isotopes of gas-phase atomic Yb by means of a trilevel photon-echo technique. Depolarization rates, velocity-change spectra, and total scattering cross sections of Yb-He (Yb-Ar) collisions were measured (deduced). Both rank-1 and rank-2 spherical tensor components of the 3P1^{3}\mathrm{P}_{1}3P1​ state play a role in our experiment, and our results represent averages of potentially different relaxation rates attributable to these quantities. Comparison of our results with rank-0 results obtained elsewhere reveals interesting similarities as well as differences.
With a three-level configuration in ytterbium vapor, we have performed the first quantitative investigation of single excited-level scattering using a stimulated photon echo (three-pulse echo). We have studied the collisional relaxation of the echo signal by rare-gas perturbers and have derived a theoretical expression for the relaxation rate. Total elastic cross sections for collisions between Yb(6s6p3P1\mathrm{Yb}(6s6p^{3}P_{1}Yb(6s6p3P1​) and Ne or Xe have been obtained.
Isotropic depolarizing collisions are studied using a stimulated photon echo with a specific polarization of the excitation radiation pulses in a mixture of ytterbium with krypton for the J = 1 ⇄ J = 0 transition of 174Yb. The difference between the relaxation rates of orientation and alignment γ (2) − γ (1) of the 3 P 1(6s6p) 174Yb level is measured as a function of the krypton pressure. The collision photon echo at the J = 1 ⇄ J = 0 transition induced by the anisotropic relaxation is studied for the Yb + Xe mixture. The power of the collision echo increases from zero with the addition of a buffer gas to ytterbium, reaches an optimal level, and decreases with an increase in the buffer gas pressure. The polarization of this collision-induced echo differs from the polarization of the conventional echo. The experimental results are in qualitative agreement with theoretical predictions.
Elastic and depolarizing collisions between excited ytterbium atoms (6s6p 3{}^{3}3P1{P}_{1}P1​ level) and noble gases (He, Ne, and Xe) are investigated using a stimulated-photon-echo technique. The method is sensitive to collisional velocity changes concerning both the total population ${\ensuremath{\rho}}^{0}$ and the alignment ${\ensuremath{\rho}}^{2}$ of the level. More specifically, it enables us to compare precisely the velocity changes associated with elastic scattering and with alignment-preserving scattering. This represents an improvement with regard to previous works. A detailed theoretical discussion of depolarizing collisions in laser spectroscopy is presented. A simplified density-matrix equation is derived under appropriate approximations. Stimulated photon-echo data for elastic scattering are interpreted within the limits of small-angle scattering in a long-range van der Waals potential; total elastic scattering cross sections are derived from comparison between experiment and calculation: ${\mathit{\ensuremath{\sigma}}}_{\mathrm{He}}^{\mathrm{el}}$=220(20) A˚2{\r{}}^{2}˚2, ${\mathit{\ensuremath{\sigma}}}_{\mathrm{Ne}}^{\mathrm{el}}$=320(20) A˚2{\r{}}^{2}˚2, ${\mathit{\ensuremath{\sigma}}}_{\mathrm{Xe}}^{\mathrm{el}}$=1240(60) A˚2{\r{}}^{2}˚2. Total rates for destruction of alignment are measured in an auxiliary standard photon-echo experiment; the corresponding cross sections are ${\mathit{\ensuremath{\sigma}}}_{\mathrm{He}}^{(2)}$=94(3) A˚2{\r{}}^{2}˚2, ${\mathit{\ensuremath{\sigma}}}_{\mathrm{Ne}}^{(2)}$=123(7) A˚2{\r{}}^{2}˚2, ${\mathit{\ensuremath{\sigma}}}_{\mathrm{Xe}}^{(2)}$=300(20) A˚2{\r{}}^{2}˚2. Stimulated photon-echo data for depolarizing collisions are successfully compared with a calculation that we develop starting from a long-range anisotropic model potential.
Coherent transient (echo) techniques have been employed in a high-precision study of collisional velocity thermalization in a sample of (6s6p)3P1(6s6p)^{3}P_{1}(6s6p)3P1​, excited-state, 174Yb^{174}\mathrm{Yb}174Yb atoms perturbed by He or Ar. This work probes the comparative response of aligned and oriented atoms to both depolarizing and to weak, nondepolarizing and/or velocity-changing collisions. By direct inversion of our time-domain echo relaxation data, we also provide a model-independent determination of velocity-change spectra (collision kernels) for nondepolarizing collisions.
Polarization stimulated photon echo technique is applied to measure the difference between relaxation rates of alignment and orientation of the level 3P1 (6s6p) of 174Yb. At the transition 1S0 (6s2) - 3P1 (6s6p) 174Yb (of type 0 ↔ 1) a collision induced echo is revealed, which is generated by two pulses of linear and mutually orthogonal polarizations. Photon echo arises exclusively due to collisions between atoms of ytterbium and buffer gases; its power depends non-monotonously on the buffer pressure, and the echo polarizations coincides with the polarization of the first exciting pulse of radiation.
A photon echo induced exclusively by collisions of ytterbium atoms with buffer gas atoms has been observed at a 0 ⟷ 1-type1 S 0(6s 2)-3 P 1(6s6p) 174Yb transition. The polarization properties of a collision echo and the buffer gas density dependence of its intensity agree with theoretical predictions of a model of depolarizing collisions that takes into account the dependence of a relaxation matrix on the velocity of active particles. Thus, direct experimental evidence of the relaxation anisotropy due to depolarizing collisions has been obtained.