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Bond breaking in light-induced potentials.

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TLDR
It is shown that (1) the photodissociation bands can be blueshifted and (2) the asymptotic state of the fragments depends on the chosen pulse sequence.
Abstract
We study the photodissociation of ICl− under moderately strong (TW/cm2) and short (below picosecond) laser pulses. Using a single resonant pump pulse, the photodissociation spectra shows two barely overlapping bands corresponding to Frank–Condon excitation and dissociation in two electronic states. By adding a nonresonant stronger control pulse we show that (1) the photodissociation bands can be blueshifted and (2) the asymptotic state of the fragments depends on the chosen pulse sequence. If the pump pulse precedes the control pulse or the control pulse straddles the pump pulse, the outgoing wave packet has components in the two dissociation channels, whereas if the control pulse precedes the pump pulse, the photodissociation proceeds selectively in a single channel.

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Stimulated Raman adiabatic passage in physics, chemistry, and beyond

TL;DR: The stimulated Raman adiabatic passage (STIRAP) was introduced by Gaubatz et al. as discussed by the authors, which allows efficient and selective population transfer between quantum states without suffering loss due to spontaneous emission.
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Control of ultrafast molecular photodissociation by laser-field-induced potentials

TL;DR: This work explores the transition from the weak- to the strong-field regimes of laser control for the dissociation of a polyatomic molecule, methyl iodide, and finds that the control over the yield of the photodissociation reaction proceeds through the creation of a light-induced conical intersection.
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Nonadiabatic ab initio molecular dynamics including spin–orbit coupling and laser fields

TL;DR: Nonadiabatic ab initio molecular dynamics including spin-orbit coupling (SOC) and laser fields is investigated as a general tool for studies of excited-state processes and triplet states can now be treated within the given framework.
Journal ArticleDOI

Identifying Strong-Field Effects in Indirect Photofragmentation Reactions

TL;DR: In this paper, a theoretical analysis combined with a time-dependent wavepacket calculation is performed to show how a strong ultrafast laser field affects the photofragment products.
Journal ArticleDOI

A Stark future for quantum control.

TL;DR: An overview of developments using the nonresonant dynamic Stark effect within the fields of time-resolved molecular dynamics and quantum control, with particular emphasis on the notion that "dynamics" and "control" are not distinct disciplines.
References
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Journal ArticleDOI

Time-dependent quantum-mechanical methods for molecular dynamics

TL;DR: In this article, a general framework of time-dependent quantum-mechanical methods for molecular dynamics calculations is described, including the Fourier method, which is able to represent a system in phase space with the efficiency of one sampling point per unit volume in phasespace h, so that, with the proper choice of the initial wave function, exponential convergence is obtained in relation to the number of sampling points.
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Control of Chemical Reactions by Feedback-Optimized Phase-Shaped Femtosecond Laser Pulses

TL;DR: Tailored femtosecond laser pulses from a computer-controlled pulse shaper were used to optimize the branching ratios of different organometallic photodissociation reaction channels, showing that two different bond-cleaving reactions can be selected, resulting in chemically different products.
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Teaching lasers to control molecules.

TL;DR: This work simulates an apparatus that learns to excite specified rotational states in a diatomic molecule and uses a learning procedure to direct the production of pulses based on fitness'' information provided by a laboratory measurement device.
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Control of selectivity of chemical reaction via control of wave packet evolution

TL;DR: In this article, a time-dependent formulation of two-photon spectroscopy is employed to show that selectivity of reactivity can be achieved via coherent twophoton processes, and the problem of finding the optimum waveform (i.e., coherent pulse sequence) that will maximize the formation of a desired chemical species is formulated as a problem in the calculus of variations.
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Selective Bond Dissociation and Rearrangement with Optimally Tailored, Strong-Field Laser Pulses

TL;DR: Strong-field control appears to have generic applicability for manipulating molecular reactivity because the tailored intense laser fields can dynamically Stark shift many excited states into resonance, and consequently, the method is not confined by resonant spectral restrictions found in the perturbative (weak-field) regime.
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