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Register a new userQuantum-state resolved bimolecular collisions of velocity-controlled OH with NO radicals
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Added by
Sebastiaan Y.T. van de Meerakker
Publication date
2012
fields
Physics
and research's language is
English
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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 cross 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.
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The Stark deceleration of OH radicals in both low-field-seeking and high-field-seeking levels of the rovibronic ${}^2Pi_{3/2},v=0,J=3/2$ ground state is demonstrated using a single experimental setup. Applying alternating-gradient focusing, OH radicals in their low-field-seeking ${}^2Pi_{3/2},v=0,J=3/2,f$ state have been decelerated from 345 m/s to 239 m/s, removing 50 % of the kinetic energy using only 27 deceleration stages. The alternating-gradient decelerator allows to independently control longitudinal and transverse manipulation of the molecules. Optimized high-voltage switching sequences for the alternating-gradient deceleration are applied, in order to adjust the dynamic focusing strength in every deceleration stage to the changing velocity over the deceleration process. In addition we have also decelerated OH radicals in their high-field-seeking ${}^2Pi_{3/2},v=0,J=3/2,e$ state from 355 m/s to 316 m/s. For the states involved, a real crossing of hyperfine levels occurs at 640 V/cm, which is examined by varying a bias voltage applied to the electrodes.
We report on the Stark deceleration of a pulsed molecular beam of NO radicals. Stark deceleration of this chemically important species has long been considered unfeasible due to its small electric dipole moment of 0.16 D. We prepared the NO radicals in the X 2{Pi}3/2, v=0, J=3/2 spin-orbit excited state from the X 2{Pi}1/2, v=0, J=1/2 ground state by Franck-Condon pumping via the A 2{Sigma}+ state. The larger effective dipole moment in the J=3/2 level of the X 2{Pi}3/2, v=0 state, in combination with a 316-stages-long Stark decelerator, allowed us to decelerate NO radicals from 315.0 m/s to 229.2 m/s, thus removing 47 % of their kinetic energy. The measured time-of-flight profiles of the NO radicals exiting the decelerator show good agreement with the outcome of numerical trajectory simulations.
Neutral molecules, isolated in the gas-phase, can be prepared in a long-lived excited state and stored in a trap. The long observation time afforded by the trap can then be exploited to measure the radiative lifetime of this state by monitoring the temporal decay of the population in the trap. This method is demonstrated here and used to benchmark the Einstein $A$-coefficients in the Meinel system of OH. A pulsed beam of vibrationally excited OH radicals is Stark decelerated and loaded into an electrostatic quadrupole trap. The radiative lifetime of the upper $Lambda$-doublet component of the $X ^2Pi_{3/2}, v=1, J=3/2$ level is determined as $59.0 pm 2.0$ ms, in good agreement with the calculated value of $57.7 pm 1.0$ ms.
We investigate the ultracold reaction dynamics of magnetically trapped NH($X ^3Sigma^-$) radicals using rigorous quantum scattering calculations involving three coupled potential energy surfaces. We find that the reactive NH + NH cross section is driven by a short-ranged collisional mechanism, and its magnitude is only weakly dependent on magnetic field strength. Unlike most ultracold reactions observed so far, the NH + NH scattering dynamics is non-universal. Our results indicate that chemical reactions can cause more trap loss than spin-inelastic NH + NH collisions, making molecular evaporative cooling more difficult than previously anticipated.
Whereas collisions between atoms and molecules are largely understood, collisions between two molecules have proven much harder to study. In both experiment and theory, our ability to determine quantum state-resolved bimolecular cross sections lags behind their atom-molecule counterparts by decades. For many bimolecular systems, even rules of thumb -- much less intuitive understanding -- of scattering cross sections are lacking. Here, we report the measurement of state-to-state differential cross sections on the collision of state-selected and velocity-controlled nitric oxide (NO) radicals and oxygen (O2) molecules. Using velocity map imaging of the scattered NO radicals, the full product-pair correlations of rotational excitation that occurs in both collision partners from individual encounters are revealed. The correlated cross sections show surprisingly good agreement with quantum scattering calculations using ab initio NO-O2 potential energy surfaces. The observations show that the well-known energy-gap law that governs atom-molecule collisions does not generally apply to bimolecular excitation processes, and reveal a propensity rule for the vector correlation of product angular momenta.
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