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arXiv · 2309.04580

Zombie Cats on the Quantum-Classical Frontier: Wigner-Moyal and Semiclassical Limit Dynamics of Quantum Coherence in Molecules

Austin T. Green·Craig C. Martens
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Abstract

In this paper, we investigate the time evolution of quantum coherence -- the off-diagonal elements of the density matrix of a multistate quantum system -- from the perspective of the Wigner-Moyal formalism. This approach provides an exact phase space representation of quantum mechanics. We consider the coherent evolution of nuclear wavepackets in a molecule with two electronic states. For harmonic potentials, the problem is exactly soluble for both fully quantum and semiclassical descriptions. We highlight serious deficiencies of the semiclassical treatment of coherence for general systems and illustrate how even qualitative accuracy requires higher terms in the Moyal expansion to be included. The model provides an experimentally relevant example of a molecular Schrodinger's cat state. The alive and dead cats of the exact two state quantum evolution collapses into a "zombie" cat in the semiclassical limit -- an averaged behavior, neither alive nor dead, leading to significant errors. The inclusion of the Moyal correction restores a faithful simultaneously alive and dead representation of the cat that is experimentally observable.

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Austin T. Green, Craig C. Martens. 2023-09-08. Zombie Cats on the Quantum-Classical Frontier: Wigner-Moyal and Semiclassical Limit Dynamics of Quantum Coherence in Molecules. https://arxiv.org/abs/2309.04580

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