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U.S. Department of Energy
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Chemical Reactivity Through Adaptive Quantum Mechanics/Many-Body Representations: Theoretical Development, Software Implementation, and Applications (Final Report)

Technical Report ·
DOI:https://doi.org/10.2172/2203697· OSTI ID:2203697
 [1]
  1. University of California, San Diego, CA (United States); University of California, San Diego

The main objective of this research project was the development and application of a new theoretical/computational framework to model chemical transformations and electronic excitations in fluid mixtures across different phases. Our theoretical/computational framework combines our data-driven many-body (DD-MB) potentials representing molecular interactions with adaptive schemes for modeling chemical reactions in solution. The combination of these two components resulted in an adaptive quantum mechanics/many-body (adQM/MB) method that largely suppresses discontinuities between QM and MM regions, which affect existing QM/MM methods, and thus provides an accurate representation of both quantum mechanical and environmental effects through a rigorous description of mutual polarization between QM and MM regions. The implementation of our DD-MB potentials and adQM/MB method in popular software enabled computer simulations of solvation phenomena, reactive processes, and electronic excitations in fluid mixtures with chemical and spectroscopic accuracy, representing a major step toward realistic computer simulations of a wide range of molecular systems relevant to the DOE mission.

Research Organization:
University of California, San Diego, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
DOE Contract Number:
SC0019490
OSTI ID:
2203697
Report Number(s):
DOE-UCSD--0019490
Country of Publication:
United States
Language:
English

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