Path-integral imaginary-time TDDFT simulation of the hydrogen-bonded systems

ORAL

Abstract

We have recently developed a new imaginary-time time-dependent density-functional theory (itTDDFT)-based approach for computing the ground-state electron-ionic structure of atomistic systems[1]. In this method the ionic degrees of freedom are treated in the path-integral formalism, whereas electronic degrees of freedom are treated with itTDDFT. Our method, given an exact functional of the electronic density, is in principle exact in the zero-temperature limit. With approximate functionals it offers a practical path to direct ab initio simulation of molecular and condensed matter systems going beyond the Born-Oppenheimer approximation. In this work we apply our method to study properties of hydrogen-bonded and tautomeric molecules: hydrogen sulfide, formic acid and terephthalic acid dimers. We compare the results of our simulations to known experimental and theoretical results.

[1] Kolesov G, Kaxiras E, Manousakis E. Density functional theory beyond the Born-Oppenheimer approximation: accurate treatment of the ionic zero-point motion. arXiv:1804.10852. Accepted at Phys. Rev. B (2018)

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Presenters

  • Grigory Kolesov

    Harvard University

Authors

  • Grigory Kolesov

    Harvard University

  • Efstratios Manousakis

    University of Athens, Panepistimioupolis, Zografos, Athens, Greece; Florida State University, Tallahassee, FL, USA; National High Magnetic Field Laboratory, Department of Physics and National High Magnetic Field Laboratory, Florida State University, Florida State University, National High Magnetic Field Laboratory, Florida State University, Physics, Florida State University and National High Magnetic Field Laboratory, Florida State Univ

  • Efthimios Kaxiras

    Harvard University, Department of Physics, Harvard University, Physics, Harvard University