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Physical Review Letters

Measurement of the Potassium 4 P Excited State Diffusion Coefficient in Xenon Gas Using Degenerate Four-Wave Mixing

David S. Glassner, R. J. Knize

Published Mar 20, 1995• 6 citations
Publisher

Abstract

We present a method for measuring the diffusion coefficients for excited atoms in buffer gases that uses degenerate four-wave mixing. We show that, for low beam intensities and atomic densities, the relative angular response of the degenerate four-wave mixing signal is dependent on the excited state diffusion and decay rate only, and that it is independent of the ground state diffusion. We have experimentally measured the diffusion of potassium atoms in the $4P$ state in xenon and found that the diffusion coefficient $D$ at 155 \ifmmode^\circ\else\textdegree\fi{}C and 760 torr is 0.084(4) c${\mathrm{m}}^{2}$ ${\mathrm{s}}^{--1}$.

DOI
10.1103/physrevlett.74.2212

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Analysis of the relative angular response of the degenerate four-wave mixing signal in alkali-metal atoms mixed with a buffer gas allows direct determination of the excited-state diffusion coefficients. The measured diffusion coefficients D at 96 \ifmmode^\circ\else\textdegree\fi{}C and 760 torr for the cesium 6${\mathit{P}}_{1/2}$ and 6${\mathit{P}}_{3/2}$ state atoms in neon gas are 0.348(4) ${\mathrm{cm}}^{2}$ ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$ and 0.281(8) ${\mathrm{cm}}^{2}$ ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$, respectively. \textcopyright{} 1996 The American Physical Society.

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We present a method for measuring the diffusion coefficients for excited atoms in buffer gases that uses degenerate four-wave mixing. We show that, for low beam intensities and atomic densities, the relative angular response of the degenerate four-wave mixing signal is dependent on the excited state diffusion and decay rate only, and that it is independent of the ground state diffusion. We have experimentally measured the diffusion of potassium atoms in the 4P4P4P state in xenon and found that the diffusion coefficient DDD at 155 \ifmmode^\circ\else\textdegree\fi{}C and 760 torr is 0.084(4) cm2{\mathrm{m}}^{2}m2 s−−1{\mathrm{s}}^{--1}s−−1.
Analysis of the relative angular response of the degenerate four-wave mixing signal in alkali-metal atoms mixed with a buffer gas allows direct determination of the excited-state diffusion coefficients. The measured diffusion coefficients D at 96 \ifmmode^\circ\else\textdegree\fi{}C and 760 torr for the cesium 6P1/2{\mathit{P}}_{1/2}P1/2​ and 6P3/2{\mathit{P}}_{3/2}P3/2​ state atoms in neon gas are 0.348(4) cm2{\mathrm{cm}}^{2}cm2 ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$ and 0.281(8) cm2{\mathrm{cm}}^{2}cm2 ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$, respectively. \textcopyright{} 1996 The American Physical Society.
The population of the 3P state in atomic sodium produced by absorption in the extreme blue wing of the D lines is measured by excited-state degenerate four-wave mixing (ESDFWM). The strength of this ESDFWM signal is shown to give a measure of the pressure-broadened extreme-wing absorption coefficient alpha ( omega ). Relative values of alpha ( omega ) for the rare gases He, Ne and Ar are measured and compared with values calculated from theoretical interatomic potentials and from extreme-wing emission data. Very good agreement is found demonstrating the ability of this nonlinear technique to make accurate measurements of small excited-state densities with excellent spatial and temporal resolution. Advantages of the method for other applications are briefly discussed.
We present a robust method for measuring diffusion coefficients of warm atoms in buffer gases. Using optical pumping, we manipulate the atomic spin in a thin cylinder inside the cell. Then, we observe the spatial spread of optically pumped atoms in time using a camera, which allows us to determine the diffusion coefficient. As an example, we demonstrate measurements of diffusion coefficients of rubidium in neon, krypton and xenon acting as buffer gases. We have determined the normalized (273 K, 760 Torr) diffusion coefficients to be 0.18 ± 0.03 cm 2 /s for neon, 0.07 ± 0.01 cm 2 /s for krypton and 0.052 ± 0.006 cm 2 /s for xenon.
We present a robust method for measuring diffusion coefficients of warm atoms in buffer gases. Using optical pumping, we manipulate the atomic spin in a thin cylinder inside the cell. Then, we observe the spatial spread of optically pumped atoms in time using a camera, which allows us to determine the diffusion coefficient. As an example, we demonstrate measurements of diffusion coefficients of rubidium in neon, krypton and xenon acting as buffer gases. We have determined the normalized (273 K, 760 Torr) diffusion coefficients to be 0.18 ± 0.03 cm 2 /s for neon, 0.07 ± 0.01 cm 2 /s for krypton and 0.052 ± 0.006 cm 2 /s for xenon.
We present comprehensive determinations of the diffusion coefficients DDD at $T=24\phantom{\rule{0.16em}{0ex}}{}^{\ensuremath{\circ}}\mathrm{C}$ for trace amounts of naturally abundant Rb atoms in inert, naturally abundant He, Ne, N2{\mathrm{N}}_{2}N2​, Ar, Kr, and Xe buffer gases using a single measurement technique. They have been measured by establishing a spatially periodic population grating in the Rb sample using two laser beams that intersect at a small angle $\ensuremath{\theta}$ of a few milliradians. The atomic population grating decays exponentially in time due to diffusive motion induced by momentum-changing elastic collisions between Rb and buffer gas atoms or molecules. This decay is monitored by observing the scattered field from a readout beam aligned along the direction of one of the excitation beams. We distinguish the contribution of diffusion from other collisional processes by measuring the characteristic ${\ensuremath{\theta}}^{2}$ dependence of the decay rate. We also measure the systematic dependence of the decay rate on the buffer gas pressure over a range of 7000 to 9000090\phantom{\rule{0.16em}{0ex}}00090000 Pa. In this manner, we obtain diffusion coefficients at standard atmospheric pressure of 101325101\phantom{\rule{0.16em}{0ex}}325101325 Pa and at a temperature of $24.0(5)\phantom{\rule{0.16em}{0ex}}{}^{\ensuremath{\circ}}\mathrm{C}$. We use two models to correct for systematic effects due to the transit time, one assuming a rectangular profile of the population distribution and a rectangular readout beam profile, and a second using Gaussian profiles. We obtain weighted averages of 0.33(5), 0.214(14), 0.132(7), 0.123(9), 0.093(9), and 0.073(4)cm20.073(4)\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{2}0.073(4)cm2/s for Rb in He, Ne, N2{\mathrm{N}}_{2}N2​, Ar, Kr, and Xe, respectively. The number in parentheses represents one standard deviation of the combined statistical and systematic uncertainty. We also compare these data with diffusion coefficients obtained using quantum, classical, and semiclassical theoretical methods based on the most accurate interatomic interaction potentials from the literature. Near room temperature, simulations of DDD using classical and quantum methods agree within their intrinsic, sub-1% standard uncertainties. We find that the semiclassical model only gives the correct orders of magnitude for DDD. Our computed diffusion coefficients based on the quantum theory agree with the experimental determinations when systematic effects are taken into account. Our measurements and modeling are relevant to the optimization of magnetometers, biomedical imaging using spin-polarized noble gases, tests of collision models based on interatomic potentials, and the development of pressure sensors.