Quantum-State Resolved Bimolecular Collisions of Velocity-Controlled OH with NO Radicals
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 m...
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| Published in: | Science (American Association for the Advancement of Science) Vol. 338; no. 6110; pp. 1060 - 1063 |
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| Main Authors: | , , , , , , , , , |
| Format: | Journal Article |
| Language: | English |
| Published: |
Washington, DC
American Association for the Advancement of Science
23-11-2012
The American Association for the Advancement of Science |
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| Abstract | 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 hydroxyl (OH) radicals were scattered with hexapole-focused nitric oxide (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 nonadiabatic 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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| AbstractList | As advances in computing power and algorithm design parallel the increasing sophistication of experimental apparatus, theory and measurement are perpetually trading places as to which can detail the dynamics of molecular interactions more precisely. At present, collisions of an atom with a diatomic molecule can be studied comparably in both domains. In contrast, collisions of two diatomics each bearing an unpaired electron manifest too many degrees of freedom for computational quantum mechanics. Kirste et al. (p. 1060) have now experimentally resolved the rotational dynamics of one such case--the inelastic scattering of NO + OH--and find that a simplified theoretical model focusing on long range interactions predicts the outcome surprisingly well. Such approximations could render many analogous systems moderately predictable. [PUBLICATION ABSTRACT] 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 hydroxyl (OH) radicals were scattered with hexapole-focused nitric oxide (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 nonadiabatic interactions and a simplistic short-range interaction. This comparison reveals the crucial role of electrostatic forces in complex molecular collision processes. [PUBLICATION ABSTRACT] 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 hydroxyl (OH) radicals were scattered with hexapole-focused nitric oxide (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 nonadiabatic interactions and a simplistic short-range interaction. This comparison reveals the crucial role of electrostatic forces in complex molecular collision processes. 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 hydroxyl (OH) radicals were scattered with hexapole-focused nitric oxide (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 nonadiabatic interactions and a simplistic short-range interaction. This comparison reveals the crucial role of electrostatic forces in complex molecular collision processes. When Molecules CollideAs advances in computing power and algorithm design parallel the increasing sophistication of experimental apparatus, theory and measurement are perpetually trading places as to which can detail the dynamics of molecular interactions more precisely. At present, collisions of an atom with a diatomic molecule can be studied comparably in both domains. In contrast, collisions of two diatomics each bearing an unpaired electron manifest too many degrees of freedom for computational quantum mechanics. Kirste et al. (p. 1060) have now experimentally resolved the rotational dynamics of one such case-the inelastic scattering of NO + OH-and find that a simplified theoretical model focusing on long range interactions predicts the outcome surprisingly well. Such approximations could render many analogous systems moderately predictable. As advances in computing power and algorithm design parallel the increasing sophistication of experimental apparatus, theory and measurement are perpetually trading places as to which can detail the dynamics of molecular interactions more precisely. At present, collisions of an atom with a diatomic molecule can be studied comparably in both domains. In contrast, collisions of two diatomics each bearing an unpaired electron manifest too many degrees of freedom for computational quantum mechanics. Kirste et al. (p. 1060 ) have now experimentally resolved the rotational dynamics of one such case—the inelastic scattering of NO + OH—and find that a simplified theoretical model focusing on long range interactions predicts the outcome surprisingly well. Such approximations could render many analogous systems moderately predictable. Precise experiments on bimolecular collisions show that simplifications rendering theory tractable confer reasonable accuracy. 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 hydroxyl (OH) radicals were scattered with hexapole-focused nitric oxide (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 nonadiabatic interactions and a simplistic short-range interaction. This comparison reveals the crucial role of electrostatic forces in complex molecular collision processes. |
| Author | Wang, Xingan Gubbels, Koos B. Janssen, Liesbeth M. C. van de Meerakker, Sebastiaan Y. T. van der Avoird, Ad Meijer, Gerard Kirste, Moritz Groenenboom, Gerrit C. Schewe, H. Christian Liu, Kopin |
| Author_xml | – sequence: 1 givenname: Moritz surname: Kirste fullname: Kirste, Moritz – sequence: 2 givenname: Xingan surname: Wang fullname: Wang, Xingan – sequence: 3 givenname: H. Christian surname: Schewe fullname: Schewe, H. Christian – sequence: 4 givenname: Gerard surname: Meijer fullname: Meijer, Gerard – sequence: 5 givenname: Kopin surname: Liu fullname: Liu, Kopin – sequence: 6 givenname: Ad surname: van der Avoird fullname: van der Avoird, Ad – sequence: 7 givenname: Liesbeth M. C. surname: Janssen fullname: Janssen, Liesbeth M. C. – sequence: 8 givenname: Koos B. surname: Gubbels fullname: Gubbels, Koos B. – sequence: 9 givenname: Gerrit C. surname: Groenenboom fullname: Groenenboom, Gerrit C. – sequence: 10 givenname: Sebastiaan Y. T. surname: van de Meerakker fullname: van de Meerakker, Sebastiaan Y. T. |
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| Copyright | Copyright © 2012 American Association for the Advancement of Science 2014 INIST-CNRS Copyright © 2012, American Association for the Advancement of Science |
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| Keywords | Inorganic compounds Molecule-molecule collisions Inorganic free radical Open shell molecule Elastic scattering Potential surface Hydroxyl radicals Diatomic molecules State to state study Nitroxyl radicals |
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| Snippet | Whereas atom-molecule collisions have been studied with complete quantum-state resolution, interactions between two state-selected molecules have proven much... As advances in computing power and algorithm design parallel the increasing sophistication of experimental apparatus, theory and measurement are perpetually... When Molecules CollideAs advances in computing power and algorithm design parallel the increasing sophistication of experimental apparatus, theory and... |
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| SubjectTerms | Algorithms Approximation Atomic and molecular collision processes and interactions Atomic and molecular physics Atoms Collisions Computation Diatomic molecules Dynamical systems Dynamics Electrostatics Energy Exact sciences and technology Free radicals Hydroxyl Radical - chemistry Inelastic scattering Laser beams Materials Mathematical analysis Mathematical models Molecular beams Molecular biology Molecules Nitric Oxide - chemistry Physics Quantum Mechanics Quantum physics Quantum Theory Reagents Rotational states Scattering of atoms, molecules and ions State-to-state scattering analyses Static Electricity Velocity |
| Title | Quantum-State Resolved Bimolecular Collisions of Velocity-Controlled OH with NO Radicals |
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