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Charge Density and Redox Potential of LiNiO 2 Using Ab Initio Diffusion Quantum Monte Carlo
Name
1911.01610.pdf
Description
Submitted version
Size
2.91 MB
Format
Adobe PDF
Checksum (MD5)
7947b53c545140842b60aeba9fb85a66
Author(s)
Saritas, Kayahan
Fadel, Eric R
Kozinsky, Boris
Grossman, Jeffrey C
Journal
Journal of Physical Chemistry C
Publisher
American Chemical Society (ACS)
Version
Original manuscript
Abstract
Copyright © 2020 American Chemical Society. We investigate the charge densities, lithium intercalation potentials, and Li-diffusion barrier energies of LixNiO2 (0.0 < x < 1.0) system using the diffusion quantum Monte Carlo (DMC) method. We find an average redox potential of 4.1(2) eV and a Li-diffusion barrier energy of 0.39(3) eV with DMC. Comparisoin of the charge densities from DMC and density functional theory (DFT) and show that local and semilocal DFT functionals yield spin polarization densities with an incorrect sign on the oxygen atoms. The SCAN functional and Hubbard-U correction improves the polarization density around Ni and O atoms, resulting in smaller deviations from the DMC densities. DMC accurately captures the many-body nature of Ni-O bonding, hence yielding accurate lithium intercalation voltages, polarization densities, and reaction barriers. ©
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DOI of Published Version
10.1021/ACS.JPCC.9B10372
