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

Abstract

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]; ORCiD logo;  [2]; ORCiD logo;  [2]
  1. Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States
  2. Department of Materials Science and Engineering, University of California, Berkeley, California 94720, 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)
OSTI Identifier:
1422650
Alternate Identifier(s):
OSTI ID: 1508582; OSTI ID: 1530332
Grant/Contract Number:  
EDCBEE; 3F-31144; AC02-05CH11231; AC02-06CH11357
Resource Type:
Published Article
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Name: Journal of Physical Chemistry Letters 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. https://doi.org/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. https://doi.org/10.1021/acs.jpclett.7b03199
Zimmermann, Nils E. R., Hannah, Daniel C., Rong, Ziqin, Liu, Miao, Ceder, Gerbrand, Haranczyk, Maciej, and Persson, Kristin A. Mon . "Electrostatic Estimation of Intercalant Jump-Diffusion Barriers Using Finite-Size Ion Models". United States. https://doi.org/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 = {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},
number = 3,
volume = 9,
place = {United States},
year = {2018},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/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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    Works referencing / citing this record:

    Highly efficient evaluation of diffusion networks in Li ionic conductors using a 3D-corrugation descriptor
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    Predicting charge density distribution of materials using a local-environment-based graph convolutional network
    journal, November 2019


    Boosting ionic conductivity in antiperovskite Li 3 OCl via defect engineering: Interstitial versus vacancy
    journal, November 2019


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