Few-cycle laser pulses to obtain spatial separation of OHF- dissociation products.
In a two-part theoretical study, field-free orientation of OHF(-) is achieved by means of moderately intense half-cycle, infrared laser pulses. In the first step, a short linearly polarized pulse excites a superposition of rigid rotor rotational eigenstates via interaction with the permanent dipole moment of OHF(-). After the field has been switched off, pronounced molecular orientation is observed for several picoseconds. In the second step, femtosecond few-cycle laser pulses are applied to the oriented system to steer vibrational dynamics, modeled by anharmonic vibrational wave functions calculated on a potential energy surface obtained with unrestricted fourth order Moller-Plesset ab initio calculations. The result is selective bond breaking of OHF, followed by the spatial separation of dissociation products in the space-fixed frame. Due to revivals in the rotational wavepacket, product yields can be enhanced over long times.
Elghobashi-Meinhardt
Nadia
N
Computational Molecular Biophysics, Interdisciplinary Center for Scientific Computing (IWR), University of Heidelberg, Im Neuenheimer Feld 368, 69120 Heidelberg, Germany. nadia.elghobashi@iwr.uni-heidelberg.de
González
Leticia
L
Barth
Ingo
I
Seideman
Tamar
T
D006858:Hydrofluoric Acid / Q000737:chemistry*; D007834:Lasers; D008962:Models, Theoretical; D010100:Oxygen / Q000737:chemistry*
D006858:Hydrofluoric Acid; D010100:Oxygen