Maximizing orientation of a three-state molecule in a cavity with analytically designed pulses

作者：Li‐Bao Fan, Hai-Ji Li, Qi Chen, Hang Zhou, Heng Liu, Chuan‐Cun Shu · 发表于：Physical Review A · 年份：2025 · DOI：10.1103/physreva.111.033119 · 被引用次数：10 · 研究领域：Strong Light-Matter Interactions、Spectroscopy and Quantum Chemical Studies、Laser-Matter Interactions and 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 $B)$ 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.