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• W4320912802 abstract "Mixed quantum classical (MQC)-initial value representation (IVR) is a recently introduced semiclassical framework that allows for selective quantization of the modes of a complex system. In the quantum limit, MQC reproduces the semiclassical Double Herman-Kluk IVR results, accurately capturing nuclear quantum coherences and conserving zero-point energy. However, in the classical limit, although MQC mimics the Husimi-IVR for real-time correlation functions with linear operators, it is significantly less accurate for non-linear correlation functions with errors even at time zero. Here, we identify the origin of this discrepancy in the MQC formulation and propose a modification. We analytically show that the modified MQC approach is exact for all correlation functions at time zero, and in a study of zero-point energy (ZPE) flow, we numerically demonstrate that it correctly obtains the quantum and classical limits as a function of time. Interestingly, although classical-limit MQC simulations show the expected, unphysical ZPE leakage, we find that it is possible to predict and even modify the direction of ZPE flow through selective quantization of the system, with the quantum-limit modes accepting energy but preserving the minimum quantum mechanically required energy." @default.
• W4320912802 created "2023-02-16" @default.
• W4320912802 creator A5052144654 @default.
• W4320912802 creator A5072409019 @default.
• W4320912802 date "2023-03-08" @default.
• W4320912802 modified "2023-09-27" @default.
• W4320912802 title "Non-linear correlation functions and zero-point energy flow in mixed quantum–classical semiclassical dynamics" @default.
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• W4320912802 doi "https://doi.org/10.1063/5.0133222" @default.
• W4320912802 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/36922136" @default.
• W4320912802 hasPublicationYear "2023" @default.
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