Observing collisions beyond the secular approximation limit

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 approximati...

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Bibliographic Details
Published in:Nature communications 2019-12, Vol.10 (1), p.5780-7, Article 5780
Main Authors: Ma, Junyang, Zhang, Haisu, Lavorel, Bruno, Billard, Franck, Hertz, Edouard, Wu, Jian, Boulet, Christian, Hartmann, Jean-Michel, Faucher, Olivier
Format: Article
Language:English
Subjects:
140/125
140/133
639/766/36/1120
639/766/36/1121
Approximation
Echoes
Gases
Humanities and Social Sciences
Lasers
Mathematical analysis
Molecular relaxation
multidisciplinary
Nitrous oxide
Physics
Science
Science (multidisciplinary)
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Summary: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 N 2 O 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. Ultrafast molecular relaxation can be probed with short laser pulses. Here the authors study collisional behavior of a N 2 O and He mixture beyond secular approximation by aligning them using laser pulses and probing their rotational echoes.
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-019-13706-0