State-Selective Control for Dissipative Vibrational Dynamics of HOD by Shaped Ultrashort Infrared Laser Pulses

Korolkov, M. V.; Manz, J.; Paramonov, G. K.

doi:10.1021/jp960930y

Cited by 33 publications

(24 citation statements)

References 71 publications

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“…It is interesting to note that this situation exactly corresponds to the one described by Korolkov et al 13 for the excitation of a diatomic molecule by half-cycle pulses. They describe dissociation of the molecule by a positive half-cycle pulse, but a continuous pump-dump process to high-lying vibrational states via continuum states without dissociation upon a sign change of the field.…”

Section: B Wave Packet Motionsupporting

confidence: 72%

“…Note however that this time scale argument will hold more generally; it should also apply in single well systems, e.g., in the dissociation of a diatomic molecule. 13 This internal quenching mechanism also explains why continuous effective one-cycle pulses with a ϩsine shape cannot drive HCN→HNC isomerization, and why population transfer with effective one-cycle and sub-one-cycle pulses is so extremely sensitive to the CEP. 1 In the 3D system, in addition to the basic quasi-1D wave packet motion and its associated peak-and recurrence pattern, there is room for additional ''higher-dimensional'' mechanisms.…”

Section: Discussionmentioning

confidence: 99%

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Molecular isomerization induced by ultrashort infrared pulses. II. Pump–dump isomerization using pairs of time-delayed half-cycle pulses

Uiberacker

Jakubetz

2004

The Journal of Chemical Physics

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We investigate population transfer across the barrier in a double-well potential, induced by a pair of time-delayed single-lobe half-cycle pulses. We apply this setup both to a one-dimensional (1D) quartic model potential and to a three-dimensional potential representing HCN-->HNC isomerization. Overall the results for the two systems are similar, although in the 3D system some additional features appear not seen in the 1D case. The generic mechanism of population transfer is the preparation by the pump pulse of a wave packet involving delocalized states above the barrier, followed by the essentially 1D motion of the delocalized part of wave packet across the barrier, and the eventual de-excitation by the dump pulse to localized states in the other well. The correct timing is given by the well-to-well passage time of the wave packet and its recurrence properties, and by the signs of the field lobes which determine the direction and acceleration or deceleration of the wave packet motion. In the 3D system an additional pump-pump-dump mechanism linked to wave packet motion in the reagent well can mediate isomerization. Since the transfer time and the pulse durations are of the same order of magnitude, there is also a marked dependence of the dynamics and the transfer yield on the pulse duration. Our analysis also sheds light on the pronounced carrier envelope phase dependence previously observed for isomerization and molecular dissociation with one-cycle and sub-one-cycle pulses.

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Section: B Wave Packet Motionsupporting

confidence: 72%

Section: Discussionmentioning

confidence: 99%

Molecular isomerization induced by ultrashort infrared pulses. II. Pump–dump isomerization using pairs of time-delayed half-cycle pulses

Uiberacker

Jakubetz

2004

The Journal of Chemical Physics

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“…It has been solved by using several modifications of standard numerical methods, 36 in particular, the Adams-Bashforth-Moulton schemes for a predictor-corrector method similar to our previous works. 16,24,[37][38][39] The initial conditions to Eq. ͑25͒,…”

Section: ͑10͒mentioning

confidence: 99%

Mode-selective excitation of hydrogen atoms on a Si surface: Non-Markovian and Markovian treatment of infrared laser driven dissipative quantum dynamics

et al. 2007

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Mode-selective excitation of adsorbates by shaped infrared laser pulses is investigated here theoretically, for the example of a H atom on a hydrogen-covered Si͑100͒-2 ϫ 1 surface. The mode-selective excitation is perturbed by the intermode coupling within the system ͑bending and stretching modes͒ and by system-bath coupling to substrate phonons. Using a force-field based model, vibration-phonon coupling was found and predicted to lead to vibrational relaxation of the H-Si stretching mode on a ns timescale, and of the Si-Si-H bending mode on a ps timescale ͓I. Andrianov and P. Saalfrank, J. Chem. Phys. 124, 034710 ͑2006͔͒. To address the question as to whether in such a dissipative situation mode-selective control of adsorbate vibrational dynamics is still possible, a system-bath ansatz is used to derive an open-system density matrix theory in which the H vibrations are driven either by sin 2 , or by freely optimized infrared ps laser pulses. Both for the Si-H stretching and Si-Si-H bending vibrations mode-selective excitation is predicted to be possible. It is also found that the Markov approximation works well in most of the applications, and that simple sin 2 are nearly as effective as pulses which were freely optimized by optimal control theory.

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“…the IR and UV laser pulses are Y -and Z-polarized, respectively, and they do not overlap. The field amplitudes of the pulses used for quantum ignition correspond to maximum intensities I max;k ¼ e 0 Á c Á jE 0 k j 2 ; the field amplitudes E 0 IR and E 0 UV are chosen such that both I max;IR and I max;UV are below the Keldish limit for ionisation [23].…”

Section: Model and Techniquesmentioning

confidence: 99%

Quantum ignition of intramolecular rotation by means of IR + UV laser pulses

Fujimura

González

Kröner

et al. 2004

Chemical Physics Letters

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State-Selective Control for Dissipative Vibrational Dynamics of HOD by Shaped Ultrashort Infrared Laser Pulses

Cited by 33 publications

References 71 publications

Molecular isomerization induced by ultrashort infrared pulses. II. Pump–dump isomerization using pairs of time-delayed half-cycle pulses

Molecular isomerization induced by ultrashort infrared pulses. II. Pump–dump isomerization using pairs of time-delayed half-cycle pulses

Mode-selective excitation of hydrogen atoms on a Si surface: Non-Markovian and Markovian treatment of infrared laser driven dissipative quantum dynamics

Quantum ignition of intramolecular rotation by means of IR + UV laser pulses

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