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 (CH $_3$ 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 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 (CH$_3$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.

quant-pharXiv:2512.21012Dec 25, 20250 citations

STRONG FIELD COHERENT CONTROL IN MOLECULES

Brett J. Pearson, D. S. MORRIS, P. H. Bucksbaum +1 more

May 1, 20021 citation

Precise quantum control of molecular rotation toward a desired orientation

Qian-Qian Hong, Daoyi Dong, Niels E. Henriksen +3 more

The lack of a direct map between control fields and desired control objectives poses a significant challenge in applying quantum control theory to quantum technologies. Here, we propose an analytical framework to precisely control a limited set of quantum states and construct desired coherent superpositions using a well-designed laser pulse sequence with optimal amplitudes, phases, and delays. This theoretical framework that corresponds to a multilevel pulse-area theorem establishes a straightforward mapping between the control parameters of the pulse sequence and the amplitudes and phases of rotational states within a specific subspace. As an example, we utilize this approach to generate 15 distinct and desired rotational superpositions of ultracold polar molecules, leading to 15 desired field-free molecular orientations. By optimizing the superposition of the lowest 16 rotational states, we demonstrate that this approach can achieve a maximum orientation value of | 〈 cos θ 〉 | max above 0.99, which is very close to the global optimal value of 1 that could be achieved in an infinite-dimensional state space. This work marks a significant advancement in achieving precise control over multilevel subsystems within molecules. It holds potential applications in molecular alignment and orientation, as well as in various interdisciplinary fields related to the precise quantum control of ultracold polar molecules, opening up considerable opportunities in molecular-based quantum techniques.The lack of a direct map between control fields and desired control objectives poses a significant challenge in applying quantum control theory to quantum technologies. Here, we propose an analytical framework to precisely control a limited set of quantum states and construct desired coherent superpositions using a well-designed laser pulse sequence with optimal amplitudes, phases, and delays. This theoretical framework that corresponds to a multilevel pulse-area theorem establishes a straightforward mapping between the control parameters of the pulse sequence and the amplitudes and phases of rotational states within a specific subspace. As an example, we utilize this approach to generate 15 distinct and desired rotational superpositions of ultracold polar molecules, leading to 15 desired field-free molecular orientations. By optimizing the superposition of the lowest 16 rotational states, we demonstrate that this approach can achieve a maximum orientation value of | 〈 cos θ 〉 | max above 0.99, which is very close to the global optimal value of 1 that could be achieved in an infinite-dimensional state space. This work marks a significant advancement in achieving precise control over multilevel subsystems within molecules. It holds potential applications in molecular alignment and orientation, as well as in various interdisciplinary fields related to the precise quantum control of ultracold polar molecules, opening up considerable opportunities in molecular-based quantum techniques.

arXiv:2502.10196Physical Review ResearchFeb 28, 202517 citations

Control of Molecular and Quantum Systems

Springer eBooksJun 29, 20076 citations

Quantum control of field-free molecular orientation

Qian-Qian Hong, Zhenzhong Lian, Chuan‐Cun Shu +1 more

Generating field-free (non-stationary) orientation of molecules in space has been a longstanding goal in the field of quantum control of molecular rotation, which has significant applications in physical chemistry, chemical physics, strong-field physics, and quantum information science. In this Perspective, we review and examine several representative control schemes developed in recent years and implemented in theoretical and experimental areas for generating field-free orientation of molecules. By conducting numerical simulations of different control schemes on the same molecular system, we demonstrate that quantum coherent control, specifically targeting a limited number of the lowest-lying rotational levels to achieve an optimal superposition, can result in a high degree of orientation. To this end, we provide an overview of our latest developed analytical method, which enables the precise design of terahertz field parameters through resonant excitation. This design approach facilitates the attainment of desired field-free orientations by optimizing the amplitudes and phases of rotational wave functions for the selected rotational levels. Finally, we outlook the significance of such progress in multiple frontier research fields, highlighting its potential applications in ultracold physics, quantum computation, quantum simulation, and quantum metrology.Generating field-free (non-stationary) orientation of molecules in space has been a longstanding goal in the field of quantum control of molecular rotation, which has significant applications in physical chemistry, chemical physics, strong-field physics, and quantum information science. In this Perspective, we review and examine several representative control schemes developed in recent years and implemented in theoretical and experimental areas for generating field-free orientation of molecules. By conducting numerical simulations of different control schemes on the same molecular system, we demonstrate that quantum coherent control, specifically targeting a limited number of the lowest-lying rotational levels to achieve an optimal superposition, can result in a high degree of orientation. To this end, we provide an overview of our latest developed analytical method, which enables the precise design of terahertz field parameters through resonant excitation. This design approach facilitates the attainment of desired field-free orientations by optimizing the amplitudes and phases of rotational wave functions for the selected rotational levels. Finally, we outlook the significance of such progress in multiple frontier research fields, highlighting its potential applications in ultracold physics, quantum computation, quantum simulation, and quantum metrology.

Physical Chemistry Chemical PhysicsJan 1, 202326 citations

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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.