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research article

Implications of the DFT plus U method on polaron properties in energy materials

Wang, Zi
•
Brock, Casey
•
Matt, Amina
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2017
Physical Review B

To model polaronic behavior in strongly correlated transition-metal oxideswith ab initio methods, one typically requires a level of theory beyond that of local density or general gradient density functional theory (DFT) approximations to account for the strongly correlated d-shell interactions of transition-metal oxides. In the present work, we utilize density functional theory with additional on-site Hubbard corrections (DFT+ U) to calculate polaronic properties in two lithium ion battery cathode materials, Li x FePO4 and Li x Mn2O4, and two photocatalytic materials, TiO2 and Fe2O3. We investigate the effects of the + U on-site projection on polaronic properties. Through systematic comparison with hybrid functional calculations, it is shown that + U projection in these model materials can impact upon the band gap, polaronic hopping barrier, and polaronic eigenstate offset from the band edges in a nontrivial manner. These properties are shown to have varying degrees of coupling and dependence on the + U projection in each example material studied, which has important implications for arriving at systematic material predictions of polaronic properties in transition-metal oxides.

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Type
research article
DOI
10.1103/PhysRevB.96.125150
Web of Science ID

WOS:000411768800001

Author(s)
Wang, Zi
Brock, Casey
Matt, Amina
Bevan, Kirk H.
Date Issued

2017

Publisher

Amer Physical Soc

Published in
Physical Review B
Volume

96

Issue

12

Article Number

125150

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
IMX  
Available on Infoscience
November 8, 2017
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/142059
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