Quantum control via the dynamic Stark effect: Application to switched rotational wave packets and molecular axis alignment

Sussman, Benjamin J.; Underwood, Jonathan G.; Lausten, Rune; Ivanov, Misha; Stolow, Albert

doi:10.1103/physreva.73.053403

Cited by 80 publications

(50 citation statements)

References 53 publications

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“…In previous publications, we have successfully demonstrated the use of the NRDSE as a tool for the control of molecular axis alignment 78,79 and in the control of chemical branching ratios. 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).…”

Section: Control Interactionmentioning

confidence: 99%

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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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Section: Control Interactionmentioning

confidence: 99%

“…The derivation of the nonresonant dynamic Stark effect Hamiltonian can be developed from a number of approaches. 79,86 The most expedient approach (which includes the strongest approximations) is to replace the dipole operator µ with its expectation value, as calculated from its Taylor series expansion…”

Section: Nonresonant Dynamic Stark Effectmentioning

confidence: 99%

A Stark Future for Quantum Control

2010

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“…Most field-free orientation schemes are based on the excitation of the rotational energy states of both odd and even rotational quantum numbers [20], in contrast to the * sichu@ku.edu prevalent schemes of aligning laser pulses that typically induce the excitation of the rotational energy states using primarily the second-order Stark dynamical couplings [21]. Theoretical studies have been performed on field-free orientation [22][23][24], and several monotonically convergent quantum control algorithms have been developed for finding optimal fields at both zero and finite temperatures [25][26][27][28][29][30].…”

Section: Introductionmentioning

confidence: 99%

Maximum attainable field-free molecular orientation of a thermal ensemble with near–single-cycle THz pulses

Liao

Rabitz

et al. 2013

Phys. Rev. A

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Recently, single-cycle THz pulses have been demonstrated in the laboratory to successfully induce field-free orientation in gas-phase polar molecules at room temperature [Phys. Rev. Lett. 107, 163603 (2011)]. In this paper, we examine the maximum attainable field-free molecular orientation with optimally shaped linearly polarized near-single-cycle THz laser pulses of a thermal ensemble. Large-scale benchmark optimal control simulations are performed, including rotational energy levels with the rotational quantum numbers up to J = 100 for OCS linear molecules. The simulations are made possible by an extension of the recently formulated fast search algorithm, the two-point boundary-value quantum control paradigm, to the mixed-states optimal control problems in the present work. It is shown that a very high degree of field-free orientation can be achieved by strong, optimally shaped near-single-cycle THz pulses. The extensive numerical simulations showed that the maximum attainable J -dependent field-free orientation (equal to 0.714 for J = 60 and 0.837 for J = 100 at 100 K) in the near-single-cycle THz pulse region is close to 92% of the corresponding optimal bound that can be attained by arbitrarily long pulses. It is also found that a smaller amplitude for the optimal control field corresponds to a smaller J (e.g., ≈ 0.005 a.u. for J = 60 and ≈ 0.01 a.u. for J = 100) in the model simulations. The latter finding may underline the actual experimental performance of the field-free molecular orientation, since presently the available amplitude of single-cycle THz pulses can only reach slightly beyond 20 MV/cm (≈0.0038 a.u.).

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“…This technique has potential application as a route to nonperturbative control of molecular dynamics. The approach adds to the existing toolbox of coherent control processes [1] including, for example, molecular alignment [2], two-photon absorption [3], and multiphoton ionization [4]. Here we introduce the principles of the technique, present a successful demonstration of phase-stable rotational coherence preparation in hydrogen gas where we use the coherence to generate sidebands on ultrashort probe radiation by molecular phase modulation (MPM), and give a theoretical interpretation.…”

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confidence: 99%

“…Full interpulse phase locking has been achieved by using a ns-duration pulse and its second harmonic as pump pulses [11]. In an alternative approach, switched wave-packet techniques have been used to drive molecular motion by adiabatic turn-on and impulsive turn-off of the pump field [2]. Similar schemes have been studied theoretically [12,13].…”

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confidence: 99%