Optimal control of molecular alignment in dissipative media

Pelzer, Adam; Ramakrishna, S.; Seideman, Tamar

doi:10.1063/1.2408423

Cited by 25 publications

(31 citation statements)

References 49 publications

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“…This control is taken as a prototype to test the efficiency of the algorithm. The application of OCT to molecular alignment and orientation is relatively recent [22,12,43]. One of the main results of Ref.…”

Section: Algorithm IImentioning

confidence: 99%

Monotonically convergent optimal control theory of quantum systems under a nonlinear interaction with the control field

et al. 2008

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Abstract. We consider the optimal control of quantum systems interacting non-linearly with an electromagnetic field. We propose new monotonically convergent algorithms to solve the optimal equations. The monotonic behavior of the algorithm is ensured by a non-standard choice of the cost which is not quadratic in the field. These algorithms can be constructed for pure and mixedstate quantum systems. The efficiency of the method is shown numerically on molecular orientation with a nonlinearity of order 3 in the field. Discretizing the amplitude and the phase of the Fourier transform of the optimal field, we show that the optimal solution can be well-approximated by pulses that could be implemented experimentally.

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Section: Algorithm IImentioning

confidence: 99%

Monotonically convergent optimal control theory of quantum systems under a nonlinear interaction with the control field

et al. 2008

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“…In case of pure state systems at a temperature T = 0 K, the target state |φ f is simply the eigenvector of maximum eigenvalue of the projection of the operator cos 2 θ onto H jopt . The optimal control of molecular orientation and alignment has been considered in a series of articles [46,47,52,27]. The novelty of our approach lies in the fact that we will consider in addition spectral constraints which leads to new optimal control fields.…”

Section: Monotonically Convergent Algorithmmentioning

confidence: 99%

“…Molecular alignment has been optimized both experimentally [39,40,41,42] and theoretically in different studies using genetic algorithms [43,44,45] or optimal control theory [46,47]. Note that previous optimal control studies have not considered spectral constraints.…”

Section: Introductionmentioning

confidence: 99%

Monotonically convergent optimal control theory of quantum systems with spectral constraints on the control field

et al. 2009

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We propose a new monotonically convergent algorithm which can enforce spectral constraints on the control field (and extends to arbitrary filters). The procedure differs from standard algorithms in that at each iteration the control field is taken as a linear combination of the control field (computed by the standard algorithm) and the filtered field. The parameter of the linear combination is chosen to respect the monotonic behavior of the algorithm and to be as close to the filtered field as possible. We test the efficiency of this method on molecular alignment. Using band-pass filters, we show how to select particular rotational transitions to reach high alignment efficiency. We also consider spectral constraints corresponding to experimental conditions using pulse shaping techniques. We determine an optimal solution that could be implemented experimentally with this technique.

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“…Whereas the interest in alignment as a potential means of controlling solution dynamics is long understood, its potential as a means of understanding systembath interactions is suggested in recent studies. 43,44 The application of coherent control strategies to the case of rotational excitation and nonadiabatic alignment is thus inviting.…”

Section: Introductionmentioning

confidence: 99%

Optimal control of rotational motions in dissipative media

Pelzer

Ramakrishna

Seideman

2008

The Journal of Chemical Physics

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We apply optimal control theory to explore and manipulate rotational wavepacket dynamics subject to a dissipative environment. In addition to investigating the extent to which nonadiabatic alignment can make a useful tool in the presence of decoherence and population relaxation, we use coherent rotational superpositions as a simple model to explore several general questions in the control of systems interacting with a bath. These include the extent to which a pure state can be created out of a statistical ensemble, the degree to which control theory can develop superposition states that resist dissipation, and the nature of environments that prohibits control. Our results illustrate the information content of control studies regarding the dissipative properties of the bath and point to the strategies that optimize different targets in wavepacket alignment in nonideal environments. As an interesting aside, the method is used to illustrate the limit where the coherence-based approach to molecular alignment converges to traditional incoherent approaches.

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Optimal control of molecular alignment in dissipative media

Cited by 25 publications

References 49 publications

Monotonically convergent optimal control theory of quantum systems under a nonlinear interaction with the control field

Monotonically convergent optimal control theory of quantum systems under a nonlinear interaction with the control field

Monotonically convergent optimal control theory of quantum systems with spectral constraints on the control field

Optimal control of rotational motions in dissipative media

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