Observing collisions beyond the secular approximation limit

Junyang Ma, Haisu Zhang, Bruno Lavorel, Franck Billard, Edouard Hertz, Jian Wu (), Christian Boulet, Jean-Michel Hartmann () and Olivier Faucher ()
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Junyang Ma: UMR 6303 CNRS-Université de Bourgogne Franche-Comté
Haisu Zhang: UMR 6303 CNRS-Université de Bourgogne Franche-Comté
Bruno Lavorel: UMR 6303 CNRS-Université de Bourgogne Franche-Comté
Franck Billard: UMR 6303 CNRS-Université de Bourgogne Franche-Comté
Edouard Hertz: UMR 6303 CNRS-Université de Bourgogne Franche-Comté
Jian Wu: East China Normal University
Christian Boulet: Université Paris-Saclay
Jean-Michel Hartmann: PSL Research University
Olivier Faucher: UMR 6303 CNRS-Université de Bourgogne Franche-Comté

Nature Communications, 2019, vol. 10, issue 1, 1-7

Abstract: Abstract Quantum coherence plays an essential role in diverse natural phenomena and technological applications. The unavoidable coupling of the quantum system to an uncontrolled environment incurs dissipation that is often described using the secular approximation. Here we probe the limit of this approximation in the rotational relaxation of molecules due to thermal collisions by using the laser-kicked molecular rotor as a model system. Specifically, rotational coherences in N2O gas (diluted in He) are created by two successive nonresonant short and intense laser pulses and probed by studying the change of amplitude of the rotational alignment echo with the gas density. By interrogating the system at the early stage of its collisional relaxation, we observe a significant variation of the dissipative influence of collisions with the time of appearance of the echo, featuring a decoherence process that is well reproduced by the nonsecular quantum master equation for modeling molecular collisions.

Date: 2019
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DOI: 10.1038/s41467-019-13706-0

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