Ultrafast hydrogen migration in acetylene cation driven by non-adiabatic effects

Madjet, Mohamed El-Amine; Li, Zheng; Vendrell, Oriol

doi:10.1063/1.4793215

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Ultrafast hydrogen migration in acetylene cation driven by non-adiabatic effects

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Li, Zheng
International Max Planck Research School for Ultrafast Imaging & Structural Dynamics (IMPRS-UFAST), Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science, DESY, Notkestrasse 85, D-22607 Hamburg, Germany;
Department of Physics, University of Hamburg, D-20355 Hamburg, Germany;

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Citation

Madjet, M.-E.-A., Li, Z., & Vendrell, O. (2013). Ultrafast hydrogen migration in acetylene cation driven by non-adiabatic effects. The Journal of Chemical Physics, 138(9): 094311. doi:10.1063/1.4793215.

Cite as: https://hdl.handle.net/11858/00-001M-0000-002B-24E3-C

Abstract

Non-adiabatic dynamics of the acetylene cation is investigated using mixed quantum-classical dynamics based on trajectory surface hopping. To describe the non-adiabatic effects, two surface hopping methods are used, namely, Tully’s fewest switches and Landau-Zener surface hopping. Similarities and differences between the results based on those two methods are discussed. We find that the photoionization of acetylene into the first excited state A²Σ_g⁺ drives the molecule from the linear structure to a trans-bent structure. Through a conical intersection the acetylene cation can relax back to either the ground state of acetylene or vinylidene. We conclude that hydrogen migration always takes place after non-radiative electronic relaxation to the ground state of the monocation. Based on the analysis of correlation functions we identify coherent oscillations between acetylene and vinylidene with a period of about 70 fs after the electronic relaxation.