2020/03/04 by Jacob R. Lindale, Shannon L. Eriksson, Lindale, Jacob R. +5 · 1 citation
Biochemistry, Genetics and Molecular Biology · Physics and Astronomy · #Chemical Physics (physics.chem-ph) #Electron Spin Resonance Studies #FOS: Physical sciences #Photosynthetic Processes and Mechanisms #Spectroscopy and Quantum Chemical Studies
paper · pdf · doi:10.48550/arxiv.2003.02342
openalex publication_date 2020/03/04 · openalex created_date 2022/07/26 · openalex updated_date 2026/07/28
Many important applications in biochemistry, materials science, and catalysis\nsit squarely at the interface between quantum and statistical mechanics:\ncoherent evolution is interrupted by discrete events, such as binding of a\nsubstrate or isomerization. Theoretical models for such dynamics usually\ntruncate the incorporation of these events to the linear-response limit, thus\nrequiring small step sizes. Here, we completely re-assess the foundations of\nchemical exchange models and redesign a master equation treatment accurate to\nall orders in perturbation theory. The net result is an astonishingly simple\ncorrection to the traditional picture which vastly improves convergence with no\nincreased computational cost. We demonstrate that this approach accurately and\nefficiently extracts physical parameters from highly complex experimental data,\nsuch as coherent hyperpolarization dynamics in magnetic resonance, and is\napplicable to a wide range of other systems.\n