Dynamics of the S(1D2)+HD(j=0) Reaction at Collision Energies Approaching the Cold Regime: A Stringent Test for Theory

被引:36
作者
Lara, Manuel [2 ]
Chefdeville, Simon [1 ,3 ]
Hickson, Kevin M. [1 ,3 ]
Bergeat, Astrid [1 ,3 ]
Naulin, Christian [1 ,3 ]
Launay, Jean-Michel [4 ]
Costes, Michel [1 ,3 ]
机构
[1] Univ Bordeaux, Inst Mol Sci, F-33400 Talence, France
[2] Univ Autonoma Madrid, Fac Ciencias, Dept Quim Fis Aplicada, E-28049 Madrid, Spain
[3] CNRS, UMR 5255, F-33400 Talence, France
[4] Univ Rennes 1, CNRS UMR 6251, Inst Phys Rennes, F-35042 Rennes, France
关键词
CROSS-SECTIONS; SURFACE; STATE;
D O I
10.1103/PhysRevLett.109.133201
中图分类号
O4 [物理学];
学科分类号
0702 ;
摘要
We report integral cross sections for the S(D-1(2)) + HD(j = 0) -> DS + H and HS + D reaction channels obtained through crossed-beam experiments reaching collision energies as low as 0.46 meV and from adiabatic time-independent quantum-mechanical calculations. While good overall agreement with experiment at energies above 10 meV is observed, neither the product channel branching ratio nor the low-energy resonancelike features in the HS + D channel can be theoretically reproduced. A nonadiabatic treatment employing highly accurate singlet and triplet potential energy surfaces is clearly needed to resolve the complex nature of the reaction dynamics.
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页数:5
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共 31 条
[1]   Quantum mechanical and quasi-classical trajectory reaction probabilities and cross sections for the S(1D)+H2,D2,HD insertion reactions [J].
Bañares, L ;
Castillo, JF ;
Honvault, P ;
Launay, JM .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2005, 7 (04) :627-634
[2]   Kinetics and Dynamics of the S(1D2) + H2 → SH plus H Reaction at Very Low Temperatures and Collision Energies [J].
Berteloite, Coralie ;
Lara, Manuel ;
Bergeat, Astrid ;
Le Picard, Sebastien D. ;
Dayou, Fabrice ;
Hickson, Kevin M. ;
Canosa, Andre ;
Naulin, Christian ;
Launay, Jean-Michel ;
Sims, Ian R. ;
Costes, Michel .
PHYSICAL REVIEW LETTERS, 2010, 105 (20)
[3]   High-dimensional ab initio potential energy surfaces for reaction dynamics calculations [J].
Bowman, Joel M. ;
Czako, Gabor ;
Fu, Bina .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2011, 13 (18) :8094-8111
[4]   Appearance of Low Energy Resonances in CO-Para-H2 Inelastic Collisions [J].
Chefdeville, Simon ;
Stoecklin, Thierry ;
Bergeat, Astrid ;
Hickson, Kevin M. ;
Naulin, Christian ;
Costes, Michel .
PHYSICAL REVIEW LETTERS, 2012, 109 (02)
[5]   Significant nonadiabatic effects in the S(1D)+HD reaction [J].
Chu, Tian-Shu ;
Han, Ke-Li ;
Schatz, George C. .
JOURNAL OF PHYSICAL CHEMISTRY A, 2007, 111 (34) :8286-8290
[6]   Dynamics of the Reaction of Methane with Chlorine Atom on an Accurate Potential Energy Surface [J].
Czako, Gabor ;
Bowman, Joel M. .
SCIENCE, 2011, 334 (6054) :343-346
[7]   Exploring the accuracy level of new potential energy surfaces for the F+HD reactions: from exact quantum rate constants to the state-to-state reaction dynamics [J].
De Fazio, Dario ;
Lucas, Josep M. ;
Aquilanti, Vincenzo ;
Cavalli, Simonetta .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2011, 13 (18) :8571-8582
[8]   Transition-State Spectroscopy of Partial Wave Resonances in the F plus HD Reaction [J].
Dong, Wenrui ;
Xiao, Chunlei ;
Wang, Tao ;
Dai, Dongxu ;
Yang, Xueming ;
Zhang, Dong H. .
SCIENCE, 2010, 327 (5972) :1501-1502
[9]   Physics and Chemistry of Cold Molecules [J].
Dulieu, Olivier ;
Krems, Roman ;
Weidemueller, Matthias ;
Willitsch, Stefan .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2011, 13 (42) :18703-18704
[10]   Quantum dynamics of complex-forming bimolecular reactions [J].
Guo, H. .
INTERNATIONAL REVIEWS IN PHYSICAL CHEMISTRY, 2012, 31 (01) :1-68