Following upon our recent work on vector correlations in the Ar-NO collisions [Lemeshko and Friedrich, Phys. Chem. Chem. Phys. 12, 1038 (2010)], we compare model results with close-coupling calculations for a range of channels and collision energies for the He-NO system. The striking agreement between the model and exact polarization moments indicates that the stereodynamics of rotationally inelastic atom-molecule collisions at thermal energies is governed by diffraction of matter waves from a two-dimensional repulsive core of the atom-molecule potential. Furthermore, the model polarization moments characterizing the He-NO, He-O(2), He-OH, and He-CaH stereodynamics are found to coalesce into a single, distinctive pattern, which can serve as a "fingerprint" to identify diffraction-driven stereodynamics in future work.
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http://dx.doi.org/10.1063/1.3386530 | DOI Listing |
Faraday Discuss
August 2024
Departamento de Química Física, Universidad Complutense, Madrid 28040, Spain.
In molecular dynamics, a fundamental question is how the outcome of a collision depends on the relative orientation of the collision partners before their interaction begins (the stereodynamics of the process). The preference for a particular orientation of the reactant complex is intimately related to the idea of a collision mechanism and the possibility of control, as revealed in recent experiments. Indeed, this preference holds not only for chemical reactions involving complex polyatomic molecules, but also for the simplest inelastic atom-diatom collisions at cold collision energies.
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August 2024
Department of Chemistry, Faculty of Science and Engineering, Swansea University, Swansea, SA2 8PP, UK.
A magnetically manipulated molecular beam technique is used to change the rotational orientation of H molecules which collide with a stepped Cu(511) surface and explore how the polarisation dependence of molecules scattering into the specular channel changes as a function of surface temperature. At all temperatures, H molecules that are rotating like cartwheels are more likely to be scattered into the specular channel than those that are rotating like helicopters. Furthermore, the scattered molecules are more likely to be rotating like cartwheels, regardless of their state before the collision.
View Article and Find Full Text PDFJ Phys Chem Lett
November 2023
State Key Laboratory of Precision Spectroscopy, East China Normal University, Shanghai 200241, China.
We report the stereodynamic control of D formation from the laser-induced bimolecular reaction in a weakly bound D-D dimer via impulsive molecular alignment. Using a linearly polarized moderately intense femtosecond pump pulse, the D molecules in the dimer were prealigned prior to the bimolecular reaction triggered by a delayed probe pulse. The rotationally excited D in the dimer was observed to rotate freely as if it were a monomer.
View Article and Find Full Text PDFPhys Chem Chem Phys
July 2023
Anhui Province Key Laboratory of Optoelectric Materials Science and Technology, Department of Physics, Anhui Normal University, Wuhu, Anhui 241000, China.
State-to-state rotational energy transfer in collisions of ground ro-vibrational state CO molecules with N molecules has been studied using the crossed molecular beam method under kinematically equivalent conditions used for CO + CO rotationally inelastic scattering described in a previously published report (Sun , , 2020, , 307-309). The collisionally excited CO molecule products are detected by the same (1 + 1' + 1'') VUV (Vacuum Ultra-Violet) resonance enhanced multiphoton ionization scheme coupled with velocity map ion imaging. We present differential cross sections and scattering angle resolved rotational angular momentum alignment moments extracted from experimentally measured CO + N scattering images and compare them with theoretical predictions from quasi-classical trajectories (QCT) on a newly calculated CO-N potential energy surface (PES).
View Article and Find Full Text PDFJ Phys Chem A
January 2023
Department of Chemistry, Stanford University, Stanford, California94305, United States.
The amount of information that can be obtained from a scattering experiment depends upon the precision with which the quantum states are defined in the incoming channel. By precisely defining the incoming states and measuring the outgoing states in a scattering experiment, we set up the boundary condition for experimentally solving the Schrödinger equation. In this Perspective we discuss cold inelastic scattering experiments using the most theoretically tractable H and its isotopologues as the target.
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