TY - JOUR
T1 - Observing collisions beyond the secular approximation limit
AU - Ma, Junyang
AU - Zhang, Haisu
AU - Lavorel, Bruno
AU - Billard, Franck
AU - Hertz, Edouard
AU - Wu, Jian
AU - Boulet, Christian
AU - Hartmann, Jean Michel
AU - Faucher, Olivier
N1 - Publisher Copyright:
© 2019, The Author(s).
PY - 2019/12/1
Y1 - 2019/12/1
N2 - 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.
AB - 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.
UR - https://www.scopus.com/pages/publications/85076822676
U2 - 10.1038/s41467-019-13706-0
DO - 10.1038/s41467-019-13706-0
M3 - 文章
C2 - 31852905
AN - SCOPUS:85076822676
SN - 2041-1723
VL - 10
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 5780
ER -