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Physical Review A

Multipole-specific, model-independent, velocity-change spectra of collisionally perturbed P13 -state Yb174 atoms

Arjun G. Yodh, THOMAS W. MOSSBERG, John E. Thomas

Published Dec 1, 1986• 10 citations
Publisher

Abstract

Coherent transient (echo) techniques have been employed in a high-precision study of collisional velocity thermalization in a sample of $(6s6p)^{3}P_{1}$, excited-state, $^{174}\mathrm{Yb}$ 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.

DOI
10.1103/physreva.34.5150

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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.
We report studies of 174Yb^{174}\mathrm{Yb}174Yb 3P1^{3}P_{1}3P1​-orientation velocity-changing kernels with resolution sufficient to observe both classical and wave mechanical features. The measurements employ photon-echo techniques in which the echo intensity depends on the square of an isolated J=1J=1J=1 multipole moment for which the velocity-changing kernel is diagonal.
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 3{\mathrm{}}^{3}3P1{P}_{1}P1​ 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.
We present experiments which study velocity-changing collisions for 174Yb^{174}\mathrm{Yb}174Yb 3P1^{3}P_{1}3P1​ atomic multipoles. New laser polarization-rotation-transient techniques are used to select anisotropic moments for which the velocity-changing collision kernel is diagonal. The results are compared to those obtained for the collisional evolution of the state populations, and demonstrate that wave mechanical effects play an important role in anisotropic-moment scattering.
Isolated-multipole-moment photon-echo techniques for atomic collision studies are described and analyzed. The techniques employ three-pulse photon echoes observed in a polarization rotation configuration such that the echo intensity depends on the square of an isolated J=1 multipole moment for which the velocity-changing kernel is diagonal. This scheme is applied to resolve clearly classical and wave-mechanical features of 3P1^{3}\mathrm{P}_{1}3P1​ orientation kernels for 174gas^{174}\mathrm{gas}174gas scattering. The diagonality (in the sense to be described) of the one-dimensional kernels chosen for study is discussed physically and derived in detail.
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.
Method of stimulated photon echo with specially chosen linear polarizations of exciting pulses of coherent resonant radiation is applied for investigation of collisional decay of orientation and alignment in molecular gas SF6 and its mixtures with buffers He and Xe. These relaxation rates are measured as a function of longitudinal velocities. Within experiment accuracy, no remarkable velocity dependence of depolarizing collisions rates was detected. This result confirms conventional approach of depolarizing collisions theoretical treatment.