Rotational excitation of molecules in the regime of strong ro-vibrational coupling: Comparison between an optical centrifuge and a transform-limited pulse

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Main Authors: García-Garrido, J. M., Milner, V., Koch, C. P., González-Férez, R.
Format: Preprint
Published: 2025
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author García-Garrido, J. M.
Milner, V.
Koch, C. P.
González-Férez, R.
author_facet García-Garrido, J. M.
Milner, V.
Koch, C. P.
González-Férez, R.
contents We investigate theoretically the ability of an optical centrifuge - a laser pulse whose linear polarization is rotating at an accelerated rate, to control molecular rotation in the regime when the rigid-rotor approximation breaks down due to coupling between the vibrational and rotational degrees of freedom. Our analysis demonstrates that the centrifuge field enables controlled excitation of high rotational states while maintaining relatively low spread along the vibrational coordinate. We contrast this to the rotational excitation by a linearly polarized Gaussian pulse of equal spectral width and pulse energy which, although comparable to the centrifuge-induced rotation, is unavoidably accompanied by a substantial broadening of the vibrational wavepacket.
format Preprint
id arxiv_https___arxiv_org_abs_2512_09746
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Rotational excitation of molecules in the regime of strong ro-vibrational coupling: Comparison between an optical centrifuge and a transform-limited pulse
García-Garrido, J. M.
Milner, V.
Koch, C. P.
González-Férez, R.
Quantum Physics
Atomic Physics
Chemical Physics
Computational Physics
We investigate theoretically the ability of an optical centrifuge - a laser pulse whose linear polarization is rotating at an accelerated rate, to control molecular rotation in the regime when the rigid-rotor approximation breaks down due to coupling between the vibrational and rotational degrees of freedom. Our analysis demonstrates that the centrifuge field enables controlled excitation of high rotational states while maintaining relatively low spread along the vibrational coordinate. We contrast this to the rotational excitation by a linearly polarized Gaussian pulse of equal spectral width and pulse energy which, although comparable to the centrifuge-induced rotation, is unavoidably accompanied by a substantial broadening of the vibrational wavepacket.
title Rotational excitation of molecules in the regime of strong ro-vibrational coupling: Comparison between an optical centrifuge and a transform-limited pulse
topic Quantum Physics
Atomic Physics
Chemical Physics
Computational Physics
url https://arxiv.org/abs/2512.09746