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Physical Review A

Collision effects and the quantum-to-classical transition in a periodically kicked molecular rotor

A. Espaignol, Franck Billard, E. Hertz, Pierre Béjot, E. Cormier, Dominique Sugny, O. Faucher, Jean‐Michel Hartmann

Published Aug 5, 2026• 0 citations
Publisher

Abstract

Purely quantum phenomena such as dynamical localization (DL) can be observed in a molecular rotor subjected to a periodic train of short and intense laser pulses in the gas phase. Using requantized Classical Molecular Dynamics Simulations, we investigate the impact of collisional effects for O2 molecules. We consider different trains of kicks for which the system exhibits quantum resonance, DL, or Bloch oscillations under collision-free conditions. Within achievable experimental conditions, we demonstrate that, as the gas pressure increases, all the dynamics become progressively similar, leading to a quantum-to-classical transition. We study how decoherence induced by intermolecular collisions reduces the quantum interferences through loss of memory. These findings pave the way for future experimental investigations and further theoretical studies on the influence of dissipation on quantum effects in rotational dynamics.

DOI
10.1103/8mxh-qt96

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Purely quantum phenomena such as dynamical localization (DL) can be observed in a molecular rotor subjected to a periodic train of short and intense laser pulses in the gas phase. Using requantized Classical Molecular Dynamics Simulations, we investigate the impact of collisional effects for O2 molecules. We consider different trains of kicks for which the system exhibits quantum resonance, DL, or Bloch oscillations under collision-free conditions. Within achievable experimental conditions, we demonstrate that, as the gas pressure increases, all the dynamics become progressively similar, leading to a quantum-to-classical transition. We study how decoherence induced by intermolecular collisions reduces the quantum interferences through loss of memory. These findings pave the way for future experimental investigations and further theoretical studies on the influence of dissipation on quantum effects in rotational dynamics.
We report the observation of rotational Bloch oscillations in a gas of nitrogen molecules kicked by a periodic train of femtosecond laser pulses. A controllable detuning from the quantum resonance creates an effective accelerating potential in angular momentum space, inducing Bloch-like oscillations of the rotational excitation. These oscillations are measured via the temporal modulation of the refractive index of the gas. Our results introduce room-temperature laser-kicked molecules as a new laboratory for studies of localization phenomena in quantum transport.
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.
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.
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We point out the breakdown of two approximations widely used to describe decoherence in open quantum systems, the secular and Markov approximations. We probe their limits by studying the influence of pressure on the alignment revivals (echoes) created in properly chosen gas mixtures (HCl and CO2, pure and diluted in He) by one (two) intense and short laser pulse(s). Experiments, as well as predictions using molecular dynamics simulations, consistently demonstrate in some of the aforementioned systems the break-down of these approximations at very short times (<15 ps) after the laser kick(s).