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

    Li-Bao Fan1,2, Yu Guo2,*, Shan Ma3, and Chuan-Cun Shu1,†

    • *Contact author: guoyu@csust.edu.cn
    • †Contact author: cc.shu@csu.edu.cn

    Phys. Rev. A 113, 063106 – Published 8 June, 2026

    DOI: https://doi.org/10.1103/xt3w-w8ly

    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+≠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 strategy for controlling molecular orientation in cavity-based systems and offers valuable perspectives for future experimental applications.

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