From molecular control to quantum technology with the dynamic Stark effect

Bustard, Philip J.; Wu, Guorong; Lausten, Rune; Townsend, David; Stolow, Albert; Sussman, Benjamin J.

doi:10.1039/c1fd00067e

Cited by 11 publications

(8 citation statements)

References 45 publications

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“…Light matter interactions in this intense field regime were studied in atomic [4][5][6][7] and molecular systems [2,[8][9][10] as well as in non-neutral cationic [11][12][13] and anionic [14][15][16][17] systems. Intense laser fields bring forth a variety of nonlinear phenomena, such as the ac stark-shift [18], bond softening [19,20], multiphoton ionization [2,21], above-threshold ionization [22], Coulomb explosion [23,24], and more [25][26][27].…”

Section: Introductionmentioning

confidence: 99%

Z-scan method for nonlinear saturation intensity determination, using focused intense laser beams

2014

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We describe a method for determining saturation peak intensities of nonlinear intense field processes. The Z-scan method takes advantage of the balance between nonlinear response and interaction volume change as an intense laser pulse is focused onto a sample. We derive a robust geometric factor, directly relating the peak intensity at optimal target displacement from the focal plane and the corresponding saturation intensity. The Z-scan method allows obtaining saturation intensities with no need of a priori assumptions about the nonlinear process; surprisingly even for unfavorable finite depth samples. The method is demonstrated experimentally for an intense laser pulse interaction with molecular anions.

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Section: Introductionmentioning

confidence: 99%

Z-scan method for nonlinear saturation intensity determination, using focused intense laser beams

2014

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“…In addition, nonperturbative strong laser fields alter the potential energy surface (PES) via dynamic Stark shifts, exploring new routes to different target states inaccessible in the weak-field regime. Experimental demonstrations of nonresonant Stark control acting on the time scale of the intensity envelope of an ultrashort laser pulse [10] comprise the observation of non-Franck-Condon transitions in bound wave packet motion [11], population control in atoms by shaped laser pulses [12], control of bound vibrational levels [13], and control of the branching ratio in a dissociation reaction [14]. The resonant Stark effect, acting on the time scale of the electron dynamics, provides more efficient manipulation of the energy landscape and in particular enables Stark shifting of molecular states to higher as well as lower energies [15][16][17][18].…”

mentioning

confidence: 99%

Charge Oscillation Controlled Molecular Excitation

et al. 2013

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The direct manipulation of charge oscillations has emerged as a new perspective in chemical reaction control. Here, we demonstrate, in a joint experimental and theoretical study, that the electron dynamics of a molecule is efficiently steered by controlling the interplay of a driving femtosecond laser pulse with the photoinduced charge oscillation. These oscillations have a typical Bohr period of around 1 fs for valence electrons; therefore, control has to be exerted on a shorter time scale. Specifically, we show how precision pulse shaping is used to manipulate the coupled electron and nuclear dynamics in order to address different bound electronic target states in a molecule. We present a strong-field coherent control mechanism which is understood in terms of a simple classical picture and at the same time verified by solving the time-dependent Schrödinger equation. This mechanism is universally applicable and opens a wide spectrum of applications in the reaction control of complex systems.

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“…Finally, we simulate the photoinduced nuclear dynamics along the torsion angle φ in the electric field. The radiation-less decay after photoexcitation is shown in Figure 9, where the change of excited state population, P (1) (t)/P (1) (t = 0), is plotted for different field strengths. The field-free case is indicated by the black line.…”

Section: Conical Intersection and Radiation-less Decay In Electric Fi...mentioning

confidence: 99%

Pyridinylidene-Phenoxide in Strong Electric Fields: Controlling Orientation, Conical Intersection, and Radiation-Less Decay

et al. 2012

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Strong electric fields open new routes for the control of radiation-less decay in molecules with conical intersections. Here, we present quantum chemical and quantum dynamical simulations which demonstrate that the radiation-less decay and related photoisomerization of pyridinylidene-phenoxide can be effectively manipulated with strong electric fields by shifting the conical intersection. Moreover, we show the effects of the electric field on the orientation of the molecules and on the photoexcitation and discuss the conditions for which the field induced coupling between rotational and vibronic states can be neglected.

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From molecular control to quantum technology with the dynamic Stark effect

Cited by 11 publications

References 45 publications

Z-scan method for nonlinear saturation intensity determination, using focused intense laser beams

Z-scan method for nonlinear saturation intensity determination, using focused intense laser beams

Charge Oscillation Controlled Molecular Excitation

Pyridinylidene-Phenoxide in Strong Electric Fields: Controlling Orientation, Conical Intersection, and Radiation-Less Decay

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