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arXiv:physics/0505060 · Physical Review A

Optimally controlled field-free orientation of the kicked molecule

Claude M. Dion, Arne Keller, Osman Atabek

Published Aug 2, 2005• 32 citations
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Abstract

Efficient and long-lived field-free molecular orientation is achieved using only two kicks appropriately delayed in time. The understanding of the mechanism rests upon a molecular target state providing the best efficiency versus persistence compromise. An optimal control scheme is referred to for fixing the free parameters (amplitudes and the time delay between them). The limited number of kicks, the robustness and the transposability to different molecular systems advocate in favor of the process, when considering its experimental feasibility.

DOI
10.1103/physreva.72.023402

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Efficient and long-lived field-free molecular orientation is achieved using only two kicks appropriately delayed in time. The understanding of the mechanism rests upon a molecular target state providing the best efficiency versus persistence compromise. An optimal control scheme is referred to for fixing the free parameters (amplitudes and the time delay between them). The limited number of kicks, the robustness and the transposability to different molecular systems advocate in favor of the process, when considering its experimental feasibility.
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Optimal field-free molecular orientation for a given number of populated states, achieved by using resonant laser pulses, is theoretically investigated for linear molecules. An optimal phase difference between the rotational states can be obtained, at full revival times, after the laser pulses have decayed and these phase conditions are analytically derived for multilevel systems (J>2J>2J>2). The dependence of the phase difference on the duration and absolute area of the laser pulses is analyzed. Finally, the optimal degree of molecular orientation can be obtained by adjusting the ratios of the peak amplitudes of the laser pulses, with the carrier-envelope phases or the delay time between the pulses fulfilling the phase conditions.
The capability to control molecular rotation for field-free orientation, which arranges molecules in specific spatial directions without external fields, is crucial in physics, chemistry, and quantum information science. However, conventional methods typically lead to transient orientations characterized by periodic directional reversals and necessitate the generation of coherent superpositions across a broad spectrum of rotational states of ultracold molecules. In this work, we develop a theoretical framework for achieving unidirectional field-free orientation by selectively manipulating two specific rotational states of symmetric top molecules. By leveraging the interplay between coherent superpositions and the precise selection of initial states, we demonstrate that both the maximum achievable orientation and its direction can be effectively controlled. To attain the desired two-state orientation, we present a quantum control strategy that utilizes a single control pulse, significantly simplifying the complexities of conventional multistate or multipulse schemes. Numerical simulations validate the effectiveness and feasibility of this approach for methyl iodide (CH3_33​I) molecules, even when accounting for molecular centrifugal distortion.The results highlight the critical roles of initial-state selection and quantum coherence in achieving long-lasting, high unidirectional molecular orientation, opening new directions in stereochemistry, precision spectroscopy, and quantum computing.
In a typical experiment aiming to control quantum dynamics phenomena, each molecule experiences the same temporal laser field, but with an amplitude that depends on the spatial location and orientation of the molecule in the laser beam. It is proved under commonly arising conditions that at least one optimal laser field exists which will control all molecules in the sample, regardless of their orientation or spatial location. The optimal laser field may consist of a multipolarization control containing up to three orthogonal, independently shaped components. The analysis also includes the prospect of multipartite control where the field couples distinct groupings of states (e.g., multiple vibronic states), but without direct coupling within a group of states. This conclusion shows that achieving quantum control is not a matter of striking a compromise over the sample diversity, but rather a task subject to optimization to reach the highest possible level of control for all molecules in the sample.