Observing collisions beyond the secular approximation limit
Abstract
Energy transfer through quantum coherences plays an essential role in diverse natural phenomena and technological applications, such as human vision, light-harvesting complexes, quantum heat engines, and quantum information and computing. The understanding of the long-lived coherence involved in these phenomena requires a detailed modeling of the system-bath interactions beyond the so-called secular and/or Markovian approximations. Despite continuous theoretical progress on understanding nonsecular dynamics in the last decades, convincing experimental observations are still lacking. By using the laser-kicked molecular rotor as a model system, we here experimentally unveil the nonsecular dynamics in the rotational relaxation of molecules due to thermal collisions. Specifically, the rotational coherence in gas-phase molecules is systematically probed and characterized by the recently discovered rotational alignment echoes featuring a decoherence and dissipation process which can only be explained by the nonsecular quantum master equations for modeling molecular collisions.
Cite
@article{arxiv.1908.09531,
title = {Observing collisions beyond the secular approximation limit},
author = {J. Ma and H. Zhang and B. Lavorel and F. Billard and E. Hertz and J. Wu and C. Boulet and J. -M. Hartmann and O. Faucher},
journal= {arXiv preprint arXiv:1908.09531},
year = {2019}
}