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We present ultrahigh-resolution measurements of state-to-state inelastic differential cross sections for NO-Ne and NO-Ar collisions, obtained by combining the Stark deceleration and velocity map imaging techniques. We show that for counterpropagating crossed beam geometries, the effect of the velocity spreads of the reagent beams on the angular resolution of the images is minimized. Futhermore, the counterpropagating geometry results in images that are symmetric with respect to the relative velocity vector. This allows for the use of inverse Abel transformation methods that enhance the resolution further. State-resolved diffraction oscillations in the differential cross sections are measured with an angular resolution approaching 0.3$^circ$. Distinct structures observed in the cross sections gauge the quality of recent emph{ab initio} potential energy surfaces for NO-rare gas atom collisions with unprecedented precision.
Whereas atom-molecule collisions have been studied with complete quantum state resolution, interactions between two state-selected molecules have proven much harder to probe. Here, we report the measurement of state-resolved inelastic scattering cros s sections for collisions between two open-shell molecules that are both prepared in a single quantum state. Stark-decelerated OH radicals were scattered with hexapole-focused NO radicals in a crossed beam configuration. Rotationally and spin-orbit inelastic scattering cross sections were measured on an absolute scale for collision energies between 70 and 300 cm$^{-1}$. These cross sections show fair agreement with quantum coupled-channels calculations using a set of coupled model potential energy surfaces based on ab initio calculations for the long-range non-adiabatic interactions and a simplistic short-range interaction. This comparison reveals the crucial role of electrostatic forces in complex molecular collision processes.
We present detailed calculations on resonances in rotationally and spin-orbit inelastic scattering of OH ($X,^2Pi, j=3/2, F_1, f$) radicals with He and Ne atoms. We calculate new emph{ab initio} potential energy surfaces for OH-He, and the cross sect ions derived from these surfaces compare favorably with the recent crossed beam scattering experiment of Kirste emph{et al.} [Phys. Rev. A textbf{82}, 042717 (2010)]. We identify both shape and Feshbach resonances in the integral and differential state-to-state scattering cross sections, and we discuss the prospects for experimentally observing scattering resonances using Stark decelerated beams of OH radicals.
We present a combined experimental and theoretical study on the rotationally inelastic scattering of OH ($X,^2Pi_{3/2}, J=3/2, f$) radicals with the collision partners He, Ne, Ar, Kr, Xe, and D$_2$ as a function of the collision energy between $sim 7 0$ cm$^{-1}$ and 400~cm$^{-1}$. The OH radicals are state selected and velocity tuned prior to the collision using a Stark decelerator, and field-free parity-resolved state-to-state inelastic relative scattering cross sections are measured in a crossed molecular beam configuration. For all OH-rare gas atom systems excellent agreement is obtained with the cross sections predicted by close-coupling scattering calculations based on accurate emph{ab initio} potential energy surfaces. This series of experiments complements recent studies on the scattering of OH radicals with Xe [Gilijamse emph{et al.}, Science {bf 313}, 1617 (2006)], Ar [Scharfenberg emph{et al.}, Phys. Chem. Chem. Phys. {bf 12}, 10660 (2010)], He, and D$_2$ [Kirste emph{et al.}, Phys. Rev. A {bf 82}, 042717 (2010)]. A comparison of the relative scattering cross sections for this set of collision partners reveals interesting trends in the scattering behavior.
We present an experimental study on the rotational inelastic scattering of OH ($X^2Pi_{3/2}, J=3/2, f$) radicals with He and D$_2$ at collision energies between 100 and 500 cm$^{-1}$ in a crossed beam experiment. The OH radicals are state selected an d velocity tuned using a Stark decelerator. Relative parity-resolved state-to-state inelastic scattering cross sections are accurately determined. These experiments complement recent low-energy collision studies between trapped OH radicals and beams of He and D$_2$ that are sensitive to the total (elastic and inelastic) cross sections (Sawyer emph{et al.}, emph{Phys. Rev. Lett.} textbf{2008}, emph{101}, 203203), but for which the measured cross sections could not be reproduced by theoretical calculations (Pavlovic emph{et al.}, emph{J. Phys. Chem. A} textbf{2009}, emph{113}, 14670). For the OH-He system, our experiments validate the inelastic cross sections determined from rigorous quantum calculations.
Beams of neutral polar molecules in a low-field seeking quantum state can be slowed down using a Stark decelerator, and can subsequently be loaded and confined in electrostatic quadrupole traps. The efficiency of the trap loading process is determine d by the ability to couple the decelerated packet of molecules into the trap without loss of molecules and without heating. We discuss the inherent difficulties to obtain ideal trap loading, and describe and compare different trap loading strategies. A new split-endcap quadrupole trap design is presented that enables improved trap loading efficiencies. This is experimentally verified by comparing the trapping of OH radicals using the conventional and the new quadrupole trap designs.
With a Stark decelerator, beams of neutral polar molecules can be accelerated, guided at a constant velocity, or decelerated. The effectiveness of this process is determined by the 6D volume in phase space from which molecules are accepted by the Sta rk decelerator. Couplings between the longitudinal and transverse motion of the molecules in the decelerator can reduce this acceptance. These couplings are nearly absent when the decelerator operates such that only every third electric field stage is used for deceleration, while extra transverse focusing is provided by the intermediate stages. For many applications, the acceptance of a Stark decelerator in this so-called $s=3$ mode significantly exceeds that of a decelerator in the conventionally used ($s=1$) mode. This has been experimentally verified by passing a beam of OH radicals through a 2.6 meter long Stark decelerator. The experiments are in quantitative agreement with the results of trajectory calculations, and can qualitatively be explained with a simple model for the 6D acceptance. These results imply that the 6D acceptance of a Stark decelerator in the $s=3$ mode of operation approaches the optimum value, i.e. the value that is obtained when any couplings are neglected.
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