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Title: Electrostatic Estimation of Intercalant Jump-Diffusion Barriers Using Finite-Size Ion Models

Abstract

© 2018 American Chemical Society. We report on a scheme for estimating intercalant jump-diffusion barriers that are typically obtained from demanding density functional theory-nudged elastic band calculations. The key idea is to relax a chain of states in the field of the electrostatic potential that is averaged over a spherical volume using different finite-size ion models. For magnesium migrating in typical intercalation materials such as transition-metal oxides, we find that the optimal model is a relatively large shell. This data-driven result parallels typical assumptions made in models based on Onsager's reaction field theory to quantitatively estimate electrostatic solvent effects. Because of its efficiency, our potential of electrostatics-finite ion size (PfEFIS) barrier estimation scheme will enable rapid identification of materials with good ionic mobility.

Authors:
ORCiD logo [1];  [1];  [2]; ORCiD logo [1];  [3]; ORCiD logo [1];  [3]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Publication Date:
Research Org.:
National Energy Research Scientific Computing Center, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1422650
Alternate Identifier(s):
OSTI ID: 1508582; OSTI ID: 1530332
Grant/Contract Number:  
AC02-05CH11231; AC02-06CH11357; EDCBEE; 3F-31144
Resource Type:
Journal Article: Published Article
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 9; Journal Issue: 3; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Zimmermann, Nils E. R., Hannah, Daniel C., Rong, Ziqin, Liu, Miao, Ceder, Gerbrand, Haranczyk, Maciej, and Persson, Kristin A. Electrostatic Estimation of Intercalant Jump-Diffusion Barriers Using Finite-Size Ion Models. United States: N. p., 2018. Web. doi:10.1021/acs.jpclett.7b03199.
Zimmermann, Nils E. R., Hannah, Daniel C., Rong, Ziqin, Liu, Miao, Ceder, Gerbrand, Haranczyk, Maciej, & Persson, Kristin A. Electrostatic Estimation of Intercalant Jump-Diffusion Barriers Using Finite-Size Ion Models. United States. doi:10.1021/acs.jpclett.7b03199.
Zimmermann, Nils E. R., Hannah, Daniel C., Rong, Ziqin, Liu, Miao, Ceder, Gerbrand, Haranczyk, Maciej, and Persson, Kristin A. Wed . "Electrostatic Estimation of Intercalant Jump-Diffusion Barriers Using Finite-Size Ion Models". United States. doi:10.1021/acs.jpclett.7b03199.
@article{osti_1422650,
title = {Electrostatic Estimation of Intercalant Jump-Diffusion Barriers Using Finite-Size Ion Models},
author = {Zimmermann, Nils E. R. and Hannah, Daniel C. and Rong, Ziqin and Liu, Miao and Ceder, Gerbrand and Haranczyk, Maciej and Persson, Kristin A.},
abstractNote = {© 2018 American Chemical Society. We report on a scheme for estimating intercalant jump-diffusion barriers that are typically obtained from demanding density functional theory-nudged elastic band calculations. The key idea is to relax a chain of states in the field of the electrostatic potential that is averaged over a spherical volume using different finite-size ion models. For magnesium migrating in typical intercalation materials such as transition-metal oxides, we find that the optimal model is a relatively large shell. This data-driven result parallels typical assumptions made in models based on Onsager's reaction field theory to quantitatively estimate electrostatic solvent effects. Because of its efficiency, our potential of electrostatics-finite ion size (PfEFIS) barrier estimation scheme will enable rapid identification of materials with good ionic mobility.},
doi = {10.1021/acs.jpclett.7b03199},
journal = {Journal of Physical Chemistry Letters},
issn = {1948-7185},
number = 3,
volume = 9,
place = {United States},
year = {2018},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1021/acs.jpclett.7b03199

Citation Metrics:
Cited by: 1 work
Citation information provided by
Web of Science

Figures / Tables:

Figure 1. Figure 1.: A magnesium ion (large white spheres) intercalated in δ-V2O5 (V: gray; O: red) hops from site 1 to site 2 and, thereby, experiences an energy barrier ΔE. The change of electrostatic potential (isosurfaces) along the path may be used to estimate ΔE.

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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.