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Molecular Structure, Spectra and Reactions: The Development of New Theory, Its Implementations and Applications

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Technical Report,01 Sep 2014,30 Jun 2018

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University of Florida Gainesville United States

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In the last four years of our work for AFOSR, we have done a number of things that build on our proof of an exact, correlated orbital theory as an effective one-particle theory. The idea is to provide coupled-cluster CC accuracy for molecular structure and spectra, but within a computational framework that exploits its one-particle character. This makes it possible to do much larger systems than can be done in traditional CC theory, even with our development of massively parallel computer programs like ACES 3 and 4. This effort also ties to CC theory, that has to converge to the correct answer in appropriate limits. COT has Kohn-Sham density functional theory DFT as a special case. Exploiting this connection has led to four new consistent DFT functionals of the QTP family. Unlike conventional DFT1, they provide an accurate one-particle spectrum, solve the problem of charge-transfer excited states in KS-DFT, provide accurate densities and activation barriers, give excellent fully relaxed core ionizations and excitation spectra, and ameliorate the pervasive self-interaction problem of KS-DFT. Several further developments are anticipated, including their extension to infinite polymers and solids.

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  • Atomic and Molecular Physics and Spectroscopy

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