Journal
PHYSICAL REVIEW LETTERS
Volume 120, Issue 12, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevLett.120.123001
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- excellence cluster The Hamburg Centre for Ultrafast Imaging-Structure, Dynamics and Control of Matter at the Atomic Scale of the Deutsche Forschungsgemeinschaft
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The effect of nuclear dynamics and conical intersections on electronic coherences is investigated employing a two-state, two-mode linear vibronic coupling model. Exact quantum dynamical calculations are performed using the multiconfiguration time-dependent Hartree method. It is found that the presence of a nonadiabatic coupling close to the Franck-Condon point can preserve electronic coherence to some extent. Additionally, the possibility of steering the nuclear wave packets by imprinting a relative phase between the electronic states during the photoionization process is discussed. It is found that the steering of nuclear wave packets is possible given that a coherent electronic wave packet embodying the phase difference passes through a conical intersection. A conical intersection close to the Franck-Condon point is thus a necessary prerequisite for control, providing a clear path towards attochemistry.
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