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Physical Review Letters

Stimulated Photon Echo for Collisional Study in Yb Vapor

J. Keller, J.-L. Le Gouët

Published Jun 4, 1984• 32 citations
Publisher

Abstract

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 $\mathrm{Yb}(6s6p^{3}P_{1}$) and Ne or Xe have been obtained.

DOI
10.1103/physrevlett.52.2034

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Stimulated photon echo for angular analysis of elastic and depolarizing Yb/emph>– noble-gas collisions

J. Keller, J.-L. Le Gouët

Elastic and depolarizing collisions between excited ytterbium atoms (6s6p ${}^{3}$${P}_{1}$ 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${\r{}}^{2}$, ${\mathit{\ensuremath{\sigma}}}_{\mathrm{Ne}}^{\mathrm{el}}$=320(20) A${\r{}}^{2}$, ${\mathit{\ensuremath{\sigma}}}_{\mathrm{Xe}}^{\mathrm{el}}$=1240(60) A${\r{}}^{2}$. 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${\r{}}^{2}$, ${\mathit{\ensuremath{\sigma}}}_{\mathrm{Ne}}^{(2)}$=123(7) A${\r{}}^{2}$, ${\mathit{\ensuremath{\sigma}}}_{\mathrm{Xe}}^{(2)}$=300(20) A${\r{}}^{2}$. Stimulated photon-echo data for depolarizing collisions are successfully compared with a calculation that we develop starting from a long-range anisotropic model potential.

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Depolarizing collisions in ytterbium vapor: Isotropic and anisotropic relaxation

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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.

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Full set of relaxation constants for 174 Yb level (6s6p) 3 P 1 in collisions with rare gases

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Abstract For the first time, a complete set of decay parameters, due to collisions of 174 Yb atoms with noble gas atoms and with ytterbium atoms, was experimentally found for the 174 Yb (6s6p) 3 P 1 level. The method of stimulated photon echo with special angles between the polarization vectors of light pulses forming an echo at the 174 Yb (6s 2 ) 1 S 0 —(6s6p) 3 P 1 transition (type 0 ↔ 1 ) is used. For each buffer gas of He, Ne, Ar, Kr, Xe, and Yb, the decay rate constants of population, orientation and alignment for the collision destruction of the 3 P 1 level of 174 Yb atoms are determined. All the decay rates demonstrated their linear increase with a buffer gas pressure, and the corresponding relaxation constants are determined. Each of the indicated relaxation constants, as well as the difference between the alignment and orientation relaxation constants, increases with the increasing buffer gas mass.

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Stimulated photon echo for elastic and depolarizing collision studies

J. Keller, J.-L. Le Gouët

Among various photon echo phenomena which have been predicted and observed in vapours [1], stimulated photon echo (three pulse echo) is a very attractive tool to investigate angular dependence of collisional processes. Already applied to the study of small angle elastic scattering [2] this method may also prove adequate for studying quasi-resonant inelastic processes involving excited species such as depolarizing collisions, collisional transitions between hyperfine, fine or rotational sublevels, energy pooling collisions. For all these processes total cross sections have already been obtained in the past by different experimental ways. However they deserve to be reexamined in the perspective of their angular dependence.

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

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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.

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Photon echo and stimulated photon echo study of various collisional-relaxation channels

Н. Н. Рубцова, L. S. Vasilenko, Хворостов Евгений Борисович

Collisional relaxation in SF6 gas and its mixtures with He and Xe is studied by photon echo and stimulated photon echo methods from the standpoint of the possibility of identifying the contributions of different types of collisions. The nonexponential nature of the kinetic curve of the photon echo is clearly observed for pure SF6, it is weaker in the mixture SF6+Xe, and it is virtually completely absent for high degrees of dilution of SF6 with helium. These features can be explained on the basis of estimates, made from experimental data, of the critical delay between the exciting pulses (for which the nonexponential behavior should be most strongly manifested). In pure SF6 it is possible to distinguish the contribution of the inelastic channel (rotational relaxation) and the contribution of weak collisions. To distinguish successfully the relaxation channels in mixtures with buffer gases a heavier buffer gas and a much better time resolution must be used. It is shown that data obtained on the orientation and alignment relaxation rates by the stimulated photon echo method can serve as an upper limit for the rates of inelastic processes which cannot be measured by the photon echo method. The combined use of photon echo and stimulated photon echo methods made it possible to obtain data on the cross sections for elastic and inelastic scattering of the collisional pairs SF6–SF6, SF6–Xe, and SF6–He.

Journal of Experimental and Theoretical Physics•Jul 1, 1999•1 citation
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.
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.
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.
Abstract For the first time, a complete set of decay parameters, due to collisions of 174 Yb atoms with noble gas atoms and with ytterbium atoms, was experimentally found for the 174 Yb (6s6p) 3 P 1 level. The method of stimulated photon echo with special angles between the polarization vectors of light pulses forming an echo at the 174 Yb (6s 2 ) 1 S 0 —(6s6p) 3 P 1 transition (type 0 ↔ 1 ) is used. For each buffer gas of He, Ne, Ar, Kr, Xe, and Yb, the decay rate constants of population, orientation and alignment for the collision destruction of the 3 P 1 level of 174 Yb atoms are determined. All the decay rates demonstrated their linear increase with a buffer gas pressure, and the corresponding relaxation constants are determined. Each of the indicated relaxation constants, as well as the difference between the alignment and orientation relaxation constants, increases with the increasing buffer gas mass.
Among various photon echo phenomena which have been predicted and observed in vapours [1], stimulated photon echo (three pulse echo) is a very attractive tool to investigate angular dependence of collisional processes. Already applied to the study of small angle elastic scattering [2] this method may also prove adequate for studying quasi-resonant inelastic processes involving excited species such as depolarizing collisions, collisional transitions between hyperfine, fine or rotational sublevels, energy pooling collisions. For all these processes total cross sections have already been obtained in the past by different experimental ways. However they deserve to be reexamined in the perspective of their angular dependence.
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.
Collisional relaxation in SF6 gas and its mixtures with He and Xe is studied by photon echo and stimulated photon echo methods from the standpoint of the possibility of identifying the contributions of different types of collisions. The nonexponential nature of the kinetic curve of the photon echo is clearly observed for pure SF6, it is weaker in the mixture SF6+Xe, and it is virtually completely absent for high degrees of dilution of SF6 with helium. These features can be explained on the basis of estimates, made from experimental data, of the critical delay between the exciting pulses (for which the nonexponential behavior should be most strongly manifested). In pure SF6 it is possible to distinguish the contribution of the inelastic channel (rotational relaxation) and the contribution of weak collisions. To distinguish successfully the relaxation channels in mixtures with buffer gases a heavier buffer gas and a much better time resolution must be used. It is shown that data obtained on the orientation and alignment relaxation rates by the stimulated photon echo method can serve as an upper limit for the rates of inelastic processes which cannot be measured by the photon echo method. The combined use of photon echo and stimulated photon echo methods made it possible to obtain data on the cross sections for elastic and inelastic scattering of the collisional pairs SF6–SF6, SF6–Xe, and SF6–He.