Breakdown of Born-Oppenheimer Approximation as a Physical Mechanism for Ultrafast Hydrogen Migrations in Strong Laser Driven Molecules
Hirobumi Mineo
Institute of Applied Mechanics, National Taiwan University, No. 1, Sec. 4, Roosevelt Road, Taipei, Taiwan R. O. C.
Institute of Atomic and Molecular Science, Academia Sinica, No. 1, Sec. 4, Roosevelt Road, Taipei, Taiwan R. O. C.
Search for more papers by this authorCorresponding Author
Sheng D. Chao
Institute of Applied Mechanics, National Taiwan University, No. 1, Sec. 4, Roosevelt Road, Taipei, Taiwan R. O. C.
Institute of Applied Mechanics, National Taiwan University, No. 1, Sec. 4, Roosevelt Road, Taipei, Taiwan R. O. C., Tel: +886-2-3366-5066; Fax: +886-2-2363-9290Search for more papers by this authorTsuyoshi Kato
Department of Chemistry, School of Science, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-0033, Japan
Search for more papers by this authorKaoru Yamanouchi
Department of Chemistry, School of Science, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-0033, Japan
Search for more papers by this authorHirobumi Mineo
Institute of Applied Mechanics, National Taiwan University, No. 1, Sec. 4, Roosevelt Road, Taipei, Taiwan R. O. C.
Institute of Atomic and Molecular Science, Academia Sinica, No. 1, Sec. 4, Roosevelt Road, Taipei, Taiwan R. O. C.
Search for more papers by this authorCorresponding Author
Sheng D. Chao
Institute of Applied Mechanics, National Taiwan University, No. 1, Sec. 4, Roosevelt Road, Taipei, Taiwan R. O. C.
Institute of Applied Mechanics, National Taiwan University, No. 1, Sec. 4, Roosevelt Road, Taipei, Taiwan R. O. C., Tel: +886-2-3366-5066; Fax: +886-2-2363-9290Search for more papers by this authorTsuyoshi Kato
Department of Chemistry, School of Science, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-0033, Japan
Search for more papers by this authorKaoru Yamanouchi
Department of Chemistry, School of Science, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-0033, Japan
Search for more papers by this authorAbstract
We propose a physical mechanism based on breakdown of the Born-Oppenheimer approximation to rationalize the ultrafast hydrogen migration in strong laser driven isomerization reactions. A three nuclei (proton, donor, and acceptor) model is employed to develop a three step solution scheme. The proton-donor Coulomb repulsion is shown to be responsible for the high proton mobility. We identify a proton tunneling process and use the Keldysh-Faisal-Reiss theory to calculate the tunneling probability. The effect of laser parameters (intensity, frequency, polarization, and pulse duration) has been studied and found to be consistent with recent experiments.
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