In this work, the primary product branching ratio (BR) for the reaction of state-prepared nitrogen cation (N(2)(+)) with acetonitrile (CH(3)CN), a possible minor constituent of Titan's upper atmosphere, is reported. The ion-molecule reaction occurs in the collision region of the supersonic nozzle expansion that is characterized by a rotational temperature of 45 ± 5 K. A BR of 0.86 ± 0.01/0.14 ± 0.01 is obtained for the formation CH(2)CN(+) and the CH(3)CN(+) product ions, respectively. The reported BR overwhelmingly favors the formation of CH(2)CN(+) product channel and is consistent with a simple capture process that is accompanied by a nonresonant dissociative charge transfer reaction. The BRs are independent of the N(2) rotational levels excited. Apart from providing insights onto the dynamics of the title ion-molecule reaction, the reported BR represents the most accurate available low-temperature experimental measurement for the reaction useful to aid in the accurate modeling of Titan's nitrile chemistry.
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http://dx.doi.org/10.1021/jp207096c | DOI Listing |
Nat Chem
June 2022
Department of Chemistry, Stanford University, Stanford, CA, USA.
The collision dynamics between a pair of aligned molecules in the presence of a partial-wave resonance provide the most sensitive probe of the long-range anisotropic forces important to chemical reactions. Here we control the collision temperature and geometry to probe the dynamics of cold (1-3 K) rotationally inelastic scattering of a pair of optically state-prepared D molecules. The collision temperature is manipulated by combining the gating action of laser state preparation and detection with the velocity dispersion of the molecular beam.
View Article and Find Full Text PDFJ Phys Chem A
February 2020
State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , Dalian , Liaoning 116023 , China.
Vibrationally excited reaction of Cl + D ( = 1, = 0) → DCl + D was investigated by a high-resolution crossed beam experiment, with D molecules in the vibrationally excited state prepared by the scheme of stimulated Raman pumping. Differential cross sections (DCSs) were obtained at three collision energies of 4.03, 4.
View Article and Find Full Text PDFJ Chem Phys
October 2016
Institute of Atomic and Molecular Sciences, Academia Sinica, P.O. Box 23-166, Taipei 10617, Taiwan.
A complete set of four polarization-dependent differential cross sections in the reactions of Cl + aligned-CHD(v=1,jK)→DCl(v=0)+CHD(v=1) is reported here for two different, rotationally polarized states with j = 1: specifically the jK=10 state prepared via the R(0) excitation and the 1±1 state via Q(1). In stark contrast to the complicated situation of the HCl(v) + CD(v = 0) channel reported in Paper-I, the stereo-requirement of this isotopic channel for both polarized reactants appears quite straightforward and consistent with a direct rebound mechanism. The extent of steric effects is moderate and relatively smaller than the alternative H-atom abstraction channel.
View Article and Find Full Text PDFRev Sci Instrum
March 2015
Max Planck Institute for Nuclear Physics, Saupfercheckweg 1, 69117 Heidelberg, Germany.
A reaction microscope (ReMi) has been combined with a magneto-optical trap (MOT) for the kinematically complete investigation of atomic break-up processes. With the novel MOTReMi apparatus, the momentum vectors of the fragments of laser-cooled and state-prepared lithium atoms are measured in coincidence and over the full solid angle. The first successful implementation of a MOTReMi could be realized due to an optimized design of the present setup, a nonstandard operation of the MOT, and by employing a switching cycle with alternating measuring and trapping periods.
View Article and Find Full Text PDFJ Phys Chem A
January 2012
Department of Chemistry, Wayne State University, Detroit, Michigan 48202, United States.
In this work, the primary product branching ratio (BR) for the reaction of state-prepared nitrogen cation (N(2)(+)) with acetonitrile (CH(3)CN), a possible minor constituent of Titan's upper atmosphere, is reported. The ion-molecule reaction occurs in the collision region of the supersonic nozzle expansion that is characterized by a rotational temperature of 45 ± 5 K. A BR of 0.
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