The dynamics of the Eley-Rideal abstraction reaction of hydrogen atoms on a movable graphitic surface is investigated for the first time in a numerically exact fully quantum setting. A system-bath strategy was applied where the two recombining H atoms and a substrate C atom form a relevant subsystem, while the rest of the lattice takes the form of an independent oscillator bath. High-dimensional wavepacket simulations were performed in the collision energy range 0.2-1.0 eV with the help of the multi-layer multi-configuration time-dependent Hartree method, focusing on the collinear reaction on a zero-temperature surface. Results show that the dynamics is close to a sudden limit in which the reaction is much faster than the substrate motion. Unpuckering of the surface is fast (some tens of fs) but starts only after the formation of H2is completed, thereby determining a considerable substrate heating (∼0.8 eV per reactive event). Energy partitioning in the product molecule favors translational over vibrational energy, and H2molecules are vibrationally hot (∼1.5 eV) though to a lesser extent than previously predicted.

Full quantum dynamical investigation of the Eley-Rideal reaction forming H2on a movable graphitic substrate at: T = 0 K / M. Pasquini, M. Bonfanti, R. Martinazzo. - In: PHYSICAL CHEMISTRY CHEMICAL PHYSICS. - ISSN 1463-9076. - 20:2(2018 Jan 14), pp. 977-988.

Full quantum dynamical investigation of the Eley-Rideal reaction forming H2on a movable graphitic substrate at: T = 0 K

M. Pasquini
Primo
;
M. Bonfanti
Secondo
;
R. Martinazzo
Ultimo
2018-01-14

Abstract

The dynamics of the Eley-Rideal abstraction reaction of hydrogen atoms on a movable graphitic surface is investigated for the first time in a numerically exact fully quantum setting. A system-bath strategy was applied where the two recombining H atoms and a substrate C atom form a relevant subsystem, while the rest of the lattice takes the form of an independent oscillator bath. High-dimensional wavepacket simulations were performed in the collision energy range 0.2-1.0 eV with the help of the multi-layer multi-configuration time-dependent Hartree method, focusing on the collinear reaction on a zero-temperature surface. Results show that the dynamics is close to a sudden limit in which the reaction is much faster than the substrate motion. Unpuckering of the surface is fast (some tens of fs) but starts only after the formation of H2is completed, thereby determining a considerable substrate heating (∼0.8 eV per reactive event). Energy partitioning in the product molecule favors translational over vibrational energy, and H2molecules are vibrationally hot (∼1.5 eV) though to a lesser extent than previously predicted.
Physics and Astronomy (all); Physical and Theoretical Chemistry
Settore CHIM/02 - Chimica Fisica
6-dic-2017
Article (author)
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Utilizza questo identificativo per citare o creare un link a questo documento: http://hdl.handle.net/2434/599744
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