TY - JOUR
T1 - Few-cycle laser pulses to obtain spatial separation of OHF- dissociation products
AU - Elghobashi-Meinhardt, Nadia
AU - González, Leticia
AU - Barth, Ingo
AU - Seideman, Tamar
N1 - Funding Information:
T.S. is grateful to the Alexander von Humboldt Foundation for a generous award that supported her visit to Berlin in the course of which this research was initiated. T.S. is grateful also to Professor Jörn Manz and Professor Martin Wolf for their kind hospitality during her visits to Berlin. N.E. gratefully acknowledges financial support from the “Berliner Programm zur Förderung der Chancengleichheit für Frauen in Forschung und Lehre.” Helpful discussions with B. Friedrich and E. L. Hamilton are acknowledged. This work has been done in the framework of the Graduiertenkolleg 788 “Hydrogen Bonds and Hydrogen Transfer” and was supported in part by the U.S. Department of Energy (Grant No. DAAD19-03-R0017).
PY - 2009
Y1 - 2009
N2 - 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 Møller-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.
AB - 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 Møller-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.
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U2 - 10.1063/1.3054276
DO - 10.1063/1.3054276
M3 - Article
C2 - 19154031
AN - SCOPUS:58449131899
SN - 0021-9606
VL - 130
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
IS - 2
M1 - 024310
ER -