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Physical Review A

Sustainable orientation of polar molecules induced by half-cycle pulses

Alex Matos-Abiague, Jamal Berakdar

Published Dec 18, 2003• 61 citations
Publisher

Abstract

Subjecting polar linear molecules to appropriately designed half-cycle electromagnetic pulses induces strong orientation of the molecules. This is deduced by inspecting the quantum dynamics within a simplified model which yields analytical conditions for the parameters of the pulses that lead to strong molecular orientation sustainable for hundreds of picoseconds. These analytical predictions are largely confirmed by a full numerical time-dependent study of the orientation process for NaI molecules. Further strategies for increasing and maintaining the molecular orientation are proposed and numerically illustrated. Our finite-temperature calculations demonstrate that the molecular orientation persists at considerable temperatures.

DOI
10.1103/physreva.68.063411

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Subjecting polar linear molecules to appropriately designed half-cycle electromagnetic pulses induces strong orientation of the molecules. This is deduced by inspecting the quantum dynamics within a simplified model which yields analytical conditions for the parameters of the pulses that lead to strong molecular orientation sustainable for hundreds of picoseconds. These analytical predictions are largely confirmed by a full numerical time-dependent study of the orientation process for NaI molecules. Further strategies for increasing and maintaining the molecular orientation are proposed and numerically illustrated. Our finite-temperature calculations demonstrate that the molecular orientation persists at considerable temperatures.
We explore the possibility of forming a oriented polar molecule directly from a pair of colliding atoms. The process comprises the photoassociation and vibrational stabilization along with the molecular orientation. These processes are driven by a single time-dependent, linearly polarized control field and proceeds entirely within the electronic ground state, leveraging the presence of a permanent dipole moment. The control field is found by means of an optimal quantum control algorithm with a single target observable given by the restriction of the orientation operator on a subset of bound levels. We consider a rovibrational model system for the collision of O + H atoms and solve directly the time-dependent Schrodinger equation. We show that the optimized field is capable of enhancing the molecular orientation already induced by the photoassociation and vibrational stabilization thus yielding oriented polar molecules that can be useful for many applications.
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.
The design of shaping pulse fields for controlling molecular orientation is of great importance in fields of stereochemical reactions, strong-field ionization, and quantum information processing. Traditional quantum optimal control algorithms typically solve the problem of molecular orientation in an infinite-dimensional rotational space, but they often overlook the constraints imposed by experimental limitations. In this work, a multi-objective and multi-constraint quantum optimal control algorithm is proposed to design a pulse field that conforms to the constraints of pulse area and energy. Specifically, the algorithm enforces a zero pulse area condition to eliminate the static field components and maintains constant pulse energy, ensuring compatibility with realistic experimental setups. Under these constraints, the algorithm optimizes the population and phase distribution of a selected number of low-lying rotational states in ultracold molecules to achieve maximum molecular orientation. The effectiveness of the proposed algorithm is demonstrated through numerical studies involving two- and three-state target subspaces, where the creation of a coherent superposition state with optimized population and phase distribution leads to the desired molecular orientation. Furthermore, its scalability is validated by applying it to a more complex 17-state subspace, where a maximum orientation value of 0.99055 is obtained, approaching the global optimal value of 1. Our findings demonstrate that by effectively managing these constraints, the influence of rotational states in the non-target state subspace can be substantially suppressed. The time-frequency analysis of the optimized pulses, combined with the Fourier transform spectrum of the time-dependent degree of orientation, indicates that the maximum molecular orientation is mainly achieved through ladder-climbing excitation of multi-color pulse fields, with the contributions from highly excited states being minimal. This work provides a valuable reference for designing experimentally feasible pulse fields using multi-constraint optimization algorithms, which helps to precisely control a limited number of rotational states to achieve maximum molecular orientation.