Direct Time-Domain Observation of l-Doubling via Centrifugal-Distortion Pre-compensation

• URL: http://arxiv.org/abs/2605.02512v1
• Date: Mon, 04 May 2026 12:07:23 GMT
• Title: Direct Time-Domain Observation of l-Doubling via Centrifugal-Distortion Pre-compensation
• Abstract summary: We demonstrate direct time-domain observation of l-doubling contributions in molecular rotational dynamics using shaped femtosecond laser pulses.<n>A cubic spectral phase compresses selected revivals into near single-cycle events.<n>The resulting distortion-free revivals reveal temporally separated l-doubling contributions that remain unresolved in conventional impulsive alignment experiments.
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• License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
• Abstract: We demonstrate direct time-domain observation of l-doubling contributions in molecular rotational dynamics using shaped femtosecond laser pulses. By imposing a tailored spectral phase on the excitation pulse, we pre-compensate centrifugal distortion, which otherwise leads to temporally broadened, multi-cycle revival structures that obscure fine rotational features. A cubic spectral phase [Phys. Rev. A 107, 053108 (2023)] compresses selected revivals into near single-cycle events, in agreement with an analytic expression derived from molecular rotational constants, enabling predictive pulse design beyond numerical optimization. The resulting distortion-free revivals reveal temporally separated l-doubling contributions that remain unresolved in conventional impulsive alignment experiments. The method proves robust against experimental imperfections, including spatial light modulator discretization. While selective control of individual l-doubling components becomes feasible, here we focus on their direct observation in the time domain.

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