Charge Density and Redox Potential of LiNiO 2 Using Ab Initio Diffusion Quantum Monte Carlo
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-...
| Main Authors: | , , , |
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| Format: | Article |
| Language: | English |
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American Chemical Society (ACS)
2021
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| Online Access: | https://hdl.handle.net/1721.1/132551 |
| _version_ | 1811071928514904064 |
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| author | Saritas, Kayahan Fadel, Eric R Kozinsky, Boris Grossman, Jeffrey C |
| author_facet | Saritas, Kayahan Fadel, Eric R Kozinsky, Boris Grossman, Jeffrey C |
| author_sort | Saritas, Kayahan |
| collection | MIT |
| description | 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. © |
| first_indexed | 2024-09-23T08:58:12Z |
| format | Article |
| id | mit-1721.1/132551 |
| institution | Massachusetts Institute of Technology |
| language | English |
| last_indexed | 2024-09-23T08:58:12Z |
| publishDate | 2021 |
| publisher | American Chemical Society (ACS) |
| record_format | dspace |
| spelling | mit-1721.1/1325512021-09-21T04:01:20Z Charge Density and Redox Potential of LiNiO 2 Using Ab Initio Diffusion Quantum Monte Carlo Saritas, Kayahan Fadel, Eric R Kozinsky, Boris Grossman, Jeffrey C 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. © 2021-09-20T18:22:59Z 2021-09-20T18:22:59Z 2020-11-16T15:13:06Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/132551 en 10.1021/ACS.JPCC.9B10372 Journal of Physical Chemistry C Creative Commons Attribution-Noncommercial-Share Alike http://creativecommons.org/licenses/by-nc-sa/4.0/ application/pdf American Chemical Society (ACS) arXiv |
| spellingShingle | Saritas, Kayahan Fadel, Eric R Kozinsky, Boris Grossman, Jeffrey C Charge Density and Redox Potential of LiNiO 2 Using Ab Initio Diffusion Quantum Monte Carlo |
| title | Charge Density and Redox Potential of LiNiO 2 Using Ab Initio Diffusion Quantum Monte Carlo |
| title_full | Charge Density and Redox Potential of LiNiO 2 Using Ab Initio Diffusion Quantum Monte Carlo |
| title_fullStr | Charge Density and Redox Potential of LiNiO 2 Using Ab Initio Diffusion Quantum Monte Carlo |
| title_full_unstemmed | Charge Density and Redox Potential of LiNiO 2 Using Ab Initio Diffusion Quantum Monte Carlo |
| title_short | Charge Density and Redox Potential of LiNiO 2 Using Ab Initio Diffusion Quantum Monte Carlo |
| title_sort | charge density and redox potential of linio 2 using ab initio diffusion quantum monte carlo |
| url | https://hdl.handle.net/1721.1/132551 |
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