Direct Time-Domain Observation of l-Doubling via Centrifugal-Distortion Pre-compensation
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arXiv
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| Auteurs principaux: | , , , , |
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| Format: | Preprint |
| Publié: |
2026
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| _version_ | 1866913086198251520 |
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| author | Sternbach, Inbar Moshe, Kfir Rutman Beer, Amit Hazra, Soumitra Fleischer, Sharly |
| author_facet | Sternbach, Inbar Moshe, Kfir Rutman Beer, Amit Hazra, Soumitra Fleischer, Sharly |
| contents | 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. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2605_02512 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Direct Time-Domain Observation of l-Doubling via Centrifugal-Distortion Pre-compensation Sternbach, Inbar Moshe, Kfir Rutman Beer, Amit Hazra, Soumitra Fleischer, Sharly Quantum Physics Chemical Physics Optics 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. |
| title | Direct Time-Domain Observation of l-Doubling via Centrifugal-Distortion Pre-compensation |
| topic | Quantum Physics Chemical Physics Optics |
| url | https://arxiv.org/abs/2605.02512 |