Second Response Theory: A Theoretical Formalism for the Propagation of Quantum Superpositions

• URL: http://arxiv.org/abs/2306.07924v4
• Date: Wed, 6 Sep 2023 20:06:34 GMT
• Title: Second Response Theory: A Theoretical Formalism for the Propagation of Quantum Superpositions
• Authors: Mart\'in A. Mosquera
• Abstract summary: We expand a previously developed size-extensive formalism within coupled cluster theory, called second response theory, so it propagates quantum systems. Our theory shows strong consistency with numerically exact results for the determination of quantum mechanical observables, probabilities, and coherences.
• Score: 0.0
• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: The propagation of general electronic quantum states provides information of the interaction of molecular systems with external driving fields. These can also offer understandings regarding non-adiabatic quantum phenomena. Well established methods focus mainly on propagating a quantum system that is initially described exclusively by the ground state wavefunction. In this work, we expand a previously developed size-extensive formalism within coupled cluster theory, called second response theory, so it propagates quantum systems that are initially described by a general linear combination of different states, which can include the ground state, and show how with a special set of time-dependent cluster operators such propagations are performed. Our theory shows strong consistency with numerically exact results for the determination of quantum mechanical observables, probabilities, and coherences. We discuss unperturbed non-stationary states within second response theory and their ability to predict matrix elements that agree with those found in linear and quadratic response theories. This work also discusses an approximate regularized methodology to treat systems with potential instabilities in their ground-state cluster amplitudes, and compares such approximations with respect to reference results from standard unitary theory.

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