Ultrafast non-Franck–Condon transitions via a two-pulse scheme

Møller, Klaus Braagaard; Henriksen, Niels Engholm

doi:10.1016/j.cplett.2003.12.056

Cited by 3 publications

(1 citation statement)

References 18 publications

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“…1). An experimental procedure based on a sequence of IR followed by UV pulses has been theoretically proposed 31 in order to induce such a non-Franck-Condon transition, 32 based on the idea that a wavepacket can be first localised on the ground state, then projected onto the excited state. (An IR + UV scheme has also been proposed in order to selectively create and transfer momentum to an initial wavepacket, 33,34 which is the alternative control scheme for switching off re-crossing that we discuss in the next section IV.3).…”

Section: Iv2 Preventing the Initial Relaxation Along The Q S Coordina...mentioning

confidence: 99%

Controlling the mechanism of fulvene S1/S0 decay: switching off the stepwise population transfer

Mendive-Tapia

Lasorne

Worth

et al. 2010

Phys. Chem. Chem. Phys.

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Direct quantum dynamics simulations were performed to model the radiationless decay of the first excited state S(1) of fulvene. The full space of thirty normal mode nuclear coordinates was explicitly considered. By default, ultrafast internal conversion takes place centred on the higher-energy planar region of the S(1)/S(0) conical intersection seam, giving the stepwise population transfer characteristic of a sloped surface crossing, and leading back to the ground state reactant. Two possible schemes for controlling whether stepwise population transfer occurs or not-either altering the initial geometry distribution or the initial momentum composition of the photo-excited wavepacket-were explored. In both cases, decay was successfully induced to occur in the lower-energy twisted/peaked region of the crossing seam, switching off the stepwise population transfer. This absence of re-crossing is a direct consequence of the change in the position on the intersection at which decay occurs (our target for control), and its consequences should provide an experimentally observable fingerprint of this system.

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Section: Iv2 Preventing the Initial Relaxation Along The Q S Coordina...mentioning

confidence: 99%

Controlling the mechanism of fulvene S1/S0 decay: switching off the stepwise population transfer

Mendive-Tapia

Lasorne

Worth

et al. 2010

Phys. Chem. Chem. Phys.

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Suppressing the Spreading of Continuum Wave Packets via Chirped Laser Pulses

et al. 2004

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We investigate the focusing, that is, the reversing of spreading of continuum wave packets created with chirped laser pulses in the weak-field limit. Focusing can be accomplished when a negative position−momentum correlation is created in the wave packet. Specializing to constant and linear (repulsive) potentials, we show analytically that in a constant potential wave packet spreading can be compensated with positively chirped laser pulses, whereas in the linear potential negatively chirped laser pulses are required, in the short-pulse limit. The analytical results for the linear potential are supported by numerical simulations. The results are discussed in the context of a classical model for wave packet focusing.

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Computational Modelling of Excited State Decay in Polyatomic Molecules

Tapia¹

2013

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Ultrafast non-Franck–Condon transitions via a two-pulse scheme

Cited by 3 publications

References 18 publications

Controlling the mechanism of fulvene S1/S0 decay: switching off the stepwise population transfer

Controlling the mechanism of fulvene S1/S0 decay: switching off the stepwise population transfer

Suppressing the Spreading of Continuum Wave Packets via Chirped Laser Pulses

Computational Modelling of Excited State Decay in Polyatomic Molecules

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