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Physical Review A

Multilevel pulse-area theorem for precise quantum control of molecular vibration and rotation

Jie Yang, Qian-Qian Hong, Shan Ma, Songshan Ma, Chuan‐Cun Shu

Published Feb 20, 2026• 1 citation
Publisher
DOI
10.1103/mnxs-hjjn

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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.
We present a theoretical framework for universal single-qutrit control in asymmetric-top molecules, advancing molecular quantum information processing. In this approach, the qutrit is encoded in three rotational eigenstates, with an auxiliary state providing independent phase control within the computational manifold. We explore an analytic protocol for arbitrary single-qutrit gates, combining directly addressable SU(2) rotations with auxiliary-state-mediated phase operations. To support this, we derive a multilevel pulse-area theorem that provides an explicit analytic mapping between gate parameters and control fields, enabling systematic design of high-fidelity microwave pulse sequences. Numerical simulations with 1,2-propanediol confirm the robustness of our approach, achieving Walsh-Hadamard gates with minimal leakage from the computational subspace. We further examine four SU(2) decomposition strategies and find that phase-error sensitivity depends on the decomposition sequence, while amplitude errors propagate along specific coherence pathways. Our results establish asymmetric-top molecules as a viable platform for qutrit-based quantum operations and offer an analytical method for precise quantum control of complex multilevel systems.