Dynamic Stark Control of Photochemical Processes

Sussman, Benjamin J.; Townsend, David; Ivanov, Misha; Stolow, Albert

doi:10.1126/science.1132289

Cited by 346 publications

(309 citation statements)

References 25 publications

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“…Also there is a great deal of interest in controlling photochemical reactions and intersystem crossings by means of optical fields. For example, control of the chemical reaction potential energy surface using the non-resonant dynamic Stark effect has been demonstrated [15]. In principle, this control scheme could also be used in experiments that investigate the role of electron spin in entrance-channel controlled and excited state reactive collisions.…”

mentioning

confidence: 99%

Quantum Control of the Spin-Orbit Interaction Using the Autler-Townes Effect

et al. 2011

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mentioning

confidence: 99%

Quantum Control of the Spin-Orbit Interaction Using the Autler-Townes Effect

et al. 2011

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“…80,81 It should be stressed here that these two effects are identical in terms of the physical control mechanism; they simply act upon different degrees of freedom within the molecular system in question (rotations and vibrations, respectively). More recently, we have also used the Stark effect for transferring population in atomic gas ensembles.…”

Section: Control Interactionmentioning

confidence: 99%

A Stark Future for Quantum Control

2010

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We present an overview of developments using the nonresonant dynamic Stark effect within the fields of time-resolved molecular dynamics and quantum control, drawing on examples from our own recent work. Particular emphasis is placed on the notion that "dynamics" and "control" are not distinct disciplines and that a clear synergy exits between these areas which has, up to now, been somewhat underexploited. The dynamic Stark effect is a universal interaction which we expect to have broad applicability.

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“…[2][3][4] Another strategy is to apply a static electric field to shift the energy of a state of ionic character as in the Stark effect 5,6 (see ref. 7 for the non-resonant dynamical Stark effect). More dynamical methods, which aim to suppress the transition either by preparing wavepackets that do not reach the CI 8 or that destructively interfere there, 9 have also been proposed.…”

Section: Introductionmentioning

confidence: 99%

Monitoring the effect of a control pulse on a conical intersection by time-resolved photoelectron spectroscopy

Arasaki

Wang

McKoy

et al. 2011

Phys. Chem. Chem. Phys.

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We have previously shown how femtosecond angle-and energy-resolved photoelectron spectroscopy can be used to monitor quantum wavepacket bifurcation at an avoided crossing or conical intersection and also how a symmetry-allowed conical intersection can be effectively morphed into an avoided crossing by photo-induced symmetry breaking. The latter result suggests that varying the parameters of a laser to modify a conical intersection might control the rate of passage of wavepackets through such regions, providing a gating process for different chemical products. In this paper, we show with full quantum mechanical calculations that such optical control of conical intersections can actually be monitored in real time with femtosecond angle-and energy-resolved photoelectron spectroscopy. In turn, this suggests that one can optimally control the gating process at a conical intersection by monitoring the photoelectron velocity map images, which should provide far more efficient and rapid optimal control than measuring the ratio of products. To demonstrate the sensitivity of time-resolved photoelectron spectra for detecting the consequences of such optical control, as well as for monitoring how the wavepacket bifurcation is affected by the control, we report results for quantum wavepackets going through the region of the symmetry-allowed conical intersection between the first two 2 A 0 states of NO 2 that is transformed to an avoided crossing. Geometry-and energy-dependent photoionization matrix elements are explicitly incorporated in these studies. Time-resolved photoelectron angular distributions and photoelectron images are seen to systematically reflect the effects of the control pulse.

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Dynamic Stark Control of Photochemical Processes

Cited by 346 publications

References 25 publications

Quantum Control of the Spin-Orbit Interaction Using the Autler-Townes Effect

Quantum Control of the Spin-Orbit Interaction Using the Autler-Townes Effect

A Stark Future for Quantum Control

Monitoring the effect of a control pulse on a conical intersection by time-resolved photoelectron spectroscopy

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