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arXiv:1806.09921 · Physical Review Letters

Rotational Alignment Decay and Decoherence of Molecular Superrotors

Benjamin A. Stickler, Farhad Taher Ghahramani, Klaus Hornberger

Published Dec 14, 2018• 14 citations
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Abstract

We present the quantum master equation describing the coherent and incoherent dynamics of a rapidly rotating molecule in the presence of a thermal background gas. The master equation relates the rate of rotational alignment decay and decoherence to the microscopic scattering amplitudes, which we calculate for anisotropic van der Waals scattering. For large rotational energies, we find quantitative agreement of the resulting alignment decay rate with recent superrotor experiments.

DOI
10.1103/physrevlett.121.243402

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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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