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arXiv:2605.28511

Chirped-pulse engineering for robust control of single-molecule orientation in a cavity

Li-Bao Fan, Yu Guo, Shan Ma, Chuan-Cun Shu

quant-phSubmitted May 27, 2026• Announced May 28, 2026• 0 citations
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Abstract

We present a theoretical investigation of coherent control over the orientation of an individual molecule strongly coupled with a cavity using chirped-pulse driving. Specifically, we explore the dynamics of carbonyl sulfide (OCS) molecules under the influence of two chirped pulses with different spectral phases. We compare two pulse configurations: one with equal chirp rates ($β_{+} = β_{-}$) and another with unequal chirp rates ($β_{+} \neq β_{-}$). Numerical simulations reveal that chirped pulses enable precise control of the molecular orientation, achieving a maximum orientation degree of 0.5773. By analyzing the distribution of molecular polariton states, we show that chirped pulses can activate multiphoton processes, leading to deviations from the predictions of first-order Magnus expansion methods. Additionally, we demonstrate the robustness of the maximum orientation with respect to chirp amplitude and detuning, providing insights into the role of pulse parameters in optimizing control. This work introduces a new strategy for controlling molecular orientation in cavity-based systems and offers valuable perspectives for future experimental applications.

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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.

Acta Physica Sinica•Jan 1, 2025•0 citations
We present a theoretical investigation of coherent control over the orientation of an individual molecule strongly coupled with a cavity using chirped-pulse driving. Specifically, we explore the dynamics of carbonyl sulfide (OCS) molecules under the influence of two chirped pulses with different spectral phases. We compare two pulse configurations: one with equal chirp rates (β+=β−β_{+} = β_{-}β+​=β−​) and another with unequal chirp rates (β+≠β−β_{+} \neq β_{-}β+​=β−​). Numerical simulations reveal that chirped pulses enable precise control of the molecular orientation, achieving a maximum orientation degree of 0.5773. By analyzing the distribution of molecular polariton states, we show that chirped pulses can activate multiphoton processes, leading to deviations from the predictions of first-order Magnus expansion methods. Additionally, we demonstrate the robustness of the maximum orientation with respect to chirp amplitude and detuning, providing insights into the role of pulse parameters in optimizing control. This work introduces a new strategy for controlling molecular orientation in cavity-based systems and offers valuable perspectives for future experimental applications.
We theoretically explore the precise control of a molecular polariton by strongly coupling the lowest three rotational states of a single molecule with a single-mode cavity. We examine two distinct cavity resonance configurations: a fundamental frequency cavity $({\ensuremath{\omega}}_{c}=2B$ with the rotational constant B)B)B) resonating with the lowest two rotational states, and a second harmonic cavity $({\ensuremath{\omega}}_{c}=4B)$ coupling with the first and second excited rotational states. We propose two control schemes based on the two polariton configurations and derive the corresponding pulse-area theorems to achieve a theoretical maximum orientation of 0.7746, identical to the molecule without the cavity. The control schemes are analyzed in carbonyl sulfide (OCS) molecules in their ground rotational state. Our numerical simulation results demonstrate the theoretical control schemes and analyze the sensitivity of the molecular polariton orientation degree to the control field bandwidth and phases. This work provides a valuable reference for achieving maximum field-free orientation of ultracold three-state molecules in a cavity using analytically designed pulses.
Abstract We perform a combined analytical and numerical investigation to explore how an analytically designed pulse can precisely control the rotational motions of a single-molecular polariton formed by the strong coupling of two low-lying rotational states with a single-mode cavity. To this end, we derive a pulse-area theorem that gives amplitude and phase conditions of the pulses in the frequency domain for driving the polariton from a given initial state to an arbitrary coherent state. The pulse-area theorem is examined for generating the maximum degree of orientation using a pair of pulses. We show that the phase condition can be satisfied by setting the initial phases of the two identically overlapped pulses or by controlling the time delay between pulses for practical applications.
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.
We discuss a novel method to create maximum coherence in a two-level system that is selectively excited among many having similar frequencies by making use of two specifically chirped pulses in the Raman configuration. The feasibility of the method is analyzed in the presence of decoherence caused by vibrational energy relaxation and collisional dephasing. It has been demonstrated that a high value of coherence may be sustained by the implementation of two chirped pulse trains prepared in accordance with the proposed method and having the same period as the vibrational energy relaxation time. Maximum coherence between predetermined states in atoms and molecules is an important aspect of many problems in quantum optics. One possible example is the generation of optimal CARS signal in the CARS microscopy aiming to reveal structures constituted of particular molecular groups. Presently, in experiments on biological imaging, the CARS signal is generated with implementation of picosecond laser pulses (1), a narrow spectral bandwidth of which allows one to address a particular molecular group with a good accuracy. Aiming to improve chemical sensitivity and to get optimal CARS signal for given pulse intensity we propose to use the quantum control methods for selective excitation of required vibrations in complex molecular systems. We developed a novel method that allows one to achieve maximum coherence in a predetermined vibrational mode in a multimode mole- cular system via the Raman transitions induced by the pump and Stokes chirped pulses. According to the Maxwell-Bloch equations, maximum coherence is the condition for the CARS signal to acquire the highest intensity upon propagation through a molecular medium (2). The mechanism of creation of maximum coherence underlying the proposed method is based on the adiabatic passage. An important aspect in the investigations asso- ciated with a condense phase is decoherence. Two main sources of decoherence, the vibrational energy relaxa- tion and collisional dephasing, may significantly affect the CARS signal intensity. The phase control of molecular processes in the presence of collisions was
A novel chirped pulse control scheme is presented based on Coherent Anti-Stokes Raman Spectroscopy (C-CARS) aiming at maximizing the vibrational coherence in atoms and molecules. The scheme utilizes chirping of the three incoming pulses, the pump, the Stokes and the probe, in the four-wave mixing process of C-CARS to fulfill the adiabatic passage conditions. The derivation of the scheme is based on simplifying the four-level system into a 'super-effective' two level system via rotating wave approximation and adiabatic elimination of the excited state manifold. The robustness, spectral selectivity and adiabatic nature of C-CARS method may prove useful for sensing, imaging, and detection. It is demonstrated that the selectivity in excitation of vibrational degrees of freedom can be controlled by carefully choosing the spectral chirp rate of the pulses. The C-CARS control scheme is applied to a surrogate methanol molecule to generate an optimal anti-Stokes signal backscattered from a cloud of molecules a kilometer away. The theory is based on the solution of the coupled Maxwell-Liouville von Neumann equations and focuses on the quantum effects induced in the target molecules by the control pulse trains. The propagation effects of pulses through the medium are evaluated and the buildup of the molecular-specific anti-Stokes signal is demonstrated numerically. A deep learning technique, using Convolutional Neural Networks (CNN), is implemented to characterize the control pulses and evaluate time-dependent phase characteristics from them. The effects of decoherence induced by spontaneous decay and collisional dephasing are also examined. Additionally, we present the technique of Fractional Stimulated Raman Adiabatic Passage (F-STIRAP) and demonstrate that it can be utilized for remote detection in a multi-level system by creation of a maximally coherent superposition state.
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.