Observation of correlated excitations in bimolecular collisions.

作者: Sebastiaan Y. T. van de Meerakker , Sjoerd N. Vogels , Gerrit C. Groenenboom , Tijs Karman , Ad van der Avoird

DOI: 10.1038/S41557-018-0004-0

关键词: Inelastic collisionChemistryAtoms in moleculesPotential energyMoleculeMolecular physicsScattering theoryExcitationAb initioScattering

摘要: Although collisions between atoms and molecules are largely understood, two have proven much harder to study. In both experiment theory, our ability determine quantum-state-resolved bimolecular cross-sections lags behind their atom–molecule counterparts by decades. For many systems, even rules of thumb—much less intuitive understanding—of scattering cross sections lacking. Here, we report the measurement state-to-state differential on collision state-selected velocity-controlled nitric oxide (NO) radicals oxygen (O2) molecules. Using velocity map imaging scattered NO radicals, full product-pair correlations rotational excitation that occurs in partners from individual encounters revealed. The correlated show surprisingly good agreement with quantum calculations using ab initio NO−O2 potential energy surfaces. observations well-known energy-gap law governs does not generally apply processes, reveal a propensity rule for vector correlation product angular momenta. Collisions understood; however, understanding is lacking because they significantly study, Now, excitations been observed inelastic O2 It shown processes.

参考文章(38)
Zhiguo Zhang, Zhichao Chen, Cunshun Huang, Yang Chen, Dongxu Dai, David H. Parker, Xueming Yang, Imaging the Pair-Correlated HNCO Photodissociation: The NH(a1Δ) + CO(X1Σ+) Channel Journal of Physical Chemistry A. ,vol. 118, pp. 2413- 2418 ,(2014) , 10.1021/JP500625M
F. J. Aoiz, M. Brouard, S. D. S. Gordon, B. Nichols, S. Stolte, V. Walpole, A new perspective: imaging the stereochemistry of molecular collisions. Physical Chemistry Chemical Physics. ,vol. 17, pp. 30210- 30228 ,(2015) , 10.1039/C5CP03273C
Steven Stolte, Aiming the molecular arrow Nature. ,vol. 353, pp. 391- 392 ,(1991) , 10.1038/353391A0
Alexander von Zastrow, Jolijn Onvlee, Sjoerd N. Vogels, Gerrit C. Groenenboom, Ad van der Avoird, Sebastiaan Y. T. van de Meerakker, State-resolved diffraction oscillations imaged for inelastic collisions of NO radicals with He, Ne and Ar Nature Chemistry. ,vol. 6, pp. 216- 221 ,(2014) , 10.1038/NCHEM.1860
S. Yan, Y.-T. Wu, B. Zhang, X.-F. Yue, K. Liu, Do Vibrational Excitations of CHD3 Preferentially Promote Reactivity Toward the Chlorine Atom Science. ,vol. 316, pp. 1723- 1726 ,(2007) , 10.1126/SCIENCE.1142313
Kopin Liu, Product pair correlation in bimolecular reactions Physical Chemistry Chemical Physics. ,vol. 9, pp. 17- 30 ,(2007) , 10.1039/B614801H
T. Wang, J. Chen, T. Yang, C. Xiao, Z. Sun, L. Huang, D. Dai, X. Yang, D. H. Zhang, Dynamical resonances accessible only by reagent vibrational excitation in the F + HD->HF + D reaction. Science. ,vol. 342, pp. 1499- 1502 ,(2013) , 10.1126/SCIENCE.1246546
M Brouard, H Chadwick, CJ Eyles, FJ Aoiz, J Kłos, None, The k-j-j' vector correlation in inelastic and reactive scattering. Journal of Chemical Physics. ,vol. 135, pp. 084305- 084305 ,(2011) , 10.1063/1.3625637
U. Buck, F. Huisken, G. Maneke, J. Schaefer, State resolved rotational excitation in HD+D2 collisions. II. Angular dependence of 0→2 transitions Journal of Chemical Physics. ,vol. 74, pp. 4430- 4438 ,(1981) , 10.1063/1.445335