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Physical Review Letters

Angular Scattering Distribution By Doppler Spectroscopy: Na(3P12)+Ar→Na(3P32)+Ar

William D. Phillips, John A. Serri, Douglas J. Ely, David E. Pritchard, Kermit R. Way, James L. Kinsey

Published Oct 2, 1978• 46 citations
Publisher

Abstract

We have developed a new method for determining state-resolved differential cross sections in inelastic collisions. A single-frequency laser provides level-specific detection of scattered atoms, while the Doppler shift of the same laser provides a completely non-mechanical angular selectivity in the detection. We have used this technique to make the first measurement of an alkali fine-structure transfer cross section in which both the scattering angle and final state are determined.

DOI
10.1103/physrevlett.41.937

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Journal of Physics B Atomic Molecular and Optical Physics•Dec 28, 1997•22 citations
We have developed a new method for determining state-resolved differential cross sections in inelastic collisions. A single-frequency laser provides level-specific detection of scattered atoms, while the Doppler shift of the same laser provides a completely non-mechanical angular selectivity in the detection. We have used this technique to make the first measurement of an alkali fine-structure transfer cross section in which both the scattering angle and final state are determined.
We present measurements of differential elastic cross sections for various alkali-alkali pairs, as well as the angular dependence of the probability of electron spin exchange in these collisions. The resolution is sufficient to reveal interference structure in the angular dependence of both quantities. We describe our apparatus, which polarizes one incident beam and analyzes the polarization of the scattered atoms, and discuss the measurement and data-reduction procedures. Results are presented in the range 0.1-0.2 eV for the systems Na-Cs, Na-Rb, Na-K, K-Cs, and K-Rb.
We report on the measurement of the linear polarization degree of the 3s2S1/23s{\phantom{\rule{0.16em}{0ex}}}^{2}\phantom{\rule{-0.16em}{0ex}}{S}_{1/2}3s2S1/2​ $\ensuremath{\rightarrow}$ 3p2P3/23p{\phantom{\rule{0.16em}{0ex}}}^{2}\phantom{\rule{-0.16em}{0ex}}{P}_{3/2}3p2P3/2​ $\ensuremath{\rightarrow}$ 5s2S1/25s{\phantom{\rule{0.16em}{0ex}}}^{2}\phantom{\rule{-0.16em}{0ex}}{S}_{1/2}5s2S1/2​ transition in atomic sodium. A linearly polarized pump laser creates an alignment in the excited 23{}^{23}23Na 3p2P3/23p{\phantom{\rule{0.16em}{0ex}}}^{2}\phantom{\rule{-0.16em}{0ex}}{P}_{3/2}3p2P3/2​ level. From the spectra, we extracted the inelastic collision cross section for the disalignment of the excited atoms by collisions with ground-level argon or xenon atoms. Measurements were done by monitoring the intensity of the cascade fluorescence from the 4p2P1/24p{\phantom{\rule{0.16em}{0ex}}}^{2}\phantom{\rule{-0.16em}{0ex}}{P}_{1/2}4p2P1/2​ $\ensuremath{\rightarrow}$ 3s2S1/23s{\phantom{\rule{0.16em}{0ex}}}^{2}\phantom{\rule{-0.16em}{0ex}}{S}_{1/2}3s2S1/2​ transition at 330.29 nm, in the presence of Ar and Xe for pressures ranging from 5.3 to 146.6 mbar. We demonstrated that the polarization measurement can provide important information about the alignment-dependent inelastic process in alkali-metal--rare-gas collisions. A depolarization cross-section value of 196 (22) \AA{}2{}^{2}2 for Na-Ar and 357 (21) \AA{}2{}^{2}2 for Na-Xe are obtained.
Differential cross sections for the transition K(4P3/2{P}_{3/2}P3/2​\ensuremath{\rightarrow}4P1/2{P}_{1/2}P1/2​) induced by He and Ar have been studied both experimentally and theoretically. Calculations were performed using a full quantal close-coupling formalism. The angular distribution of the scattered atoms is measured by Doppler shift (ADDS method). The comparison with the theoretical calculations is performed on the basis of thorough kinematic analysis. In addition, the polarization effects corresponding to the experimental conditions are taken into account carefully. This allows one to test the accuracy of various interaction potentials available for the K-He and -Ar systems. The most interesting result concerns the K-He l-dependent pseudopotentials, which are found accurate to a sufficiently high level to allow good predictions of the observed differential cross-section patterns. In particular the positions and amplitudes of the cross-section oscillations at large center-of-mass scattering angles are well reproduced. The results for Ar show that the K-Ar potentials must be improved. Finally, taking the K(4P)-He fine-structure transition as an example, it has been shown how polarization effects may be used in ADDS measurements to obtain information on the dynamics of the collision process.
We present measurements of the state-to-state differential scattering cross section (DCS) for X 16Cg Na2 with Xe using a new sub-Doppler spectroscopic method and compare results with those obtained using molecular beam techniques on the same system; the agreement is good. Criteria for comparison are based on the recent finding (McCaffery A J and Wilson R J 1996 Phys. Rev. Lett. 77 48) that simple quasiclassical vector relations determine the direction of the initial relative velocity vector and the scattering angle. The incident velocity direction is such that the perpendicular component just opens the inelastic channel and the parallel component is scattered. The relationship is Newtonian but is modified by the molecule’s characteristic quantum structure. Angular distributions from a range of experiments are found to obey the vector relation, suggesting that atom–molecule collisions are controlled by a quantum-modified Newtonian mechanics, the modification arising as a consequence of the internal energy level structure of the molecule. We introduce the term quantum-constrained kinematics to describe the hybrid mechanics and suggest that this may also influence other collisional events.