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Title: Understanding Lithium Solvation and Diffusion through Topological Analysis of First-Principles Molecular Dynamics

Abstract

The performance of lithium-ion batteries is strongly influenced by the ionic conductivity of the electrolyte, which depends on the speed at which Li ions migrate across the cell and relates to their solvation structure. The choice of solvent can greatly impact, both, the solvation and diffusivity of Li ions. In this work, we present our application of the topological techniques to extract and predict such behavior in the data generated by the first-principles molecular dynamics simulation of Li ions in an important organic solvent -ethylene carbonate. More specifically, we use the scalar topology of the electron charge density field to analyze the evolution of the solvation structures. This allows us to derive a parameter-free bond definition for lithium-oxygen bonds, to provide a quantitative measure for bond strength, and to understand the regions of influence of each atom in the simulation. This has provided new insights into how and under what conditions certain bonds may form and break. As a result, we can identify and, more importantly, predict, unstable configurations in solvation structures. This can be very useful in understanding when small changes to the atoms' movements can cause significantly different bond structures to evolve. Ultimately, this promises to allow scientistsmore » to explore lithium ion solvation and diffusion more systematically, with the aim of new insights and potentially accelerating the calculations themselves.« less

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1331475
Report Number(s):
LLNL-TR-704318
DOE Contract Number:  
AC52-07NA27344
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 97 MATHEMATICS, COMPUTING, AND INFORMATION SCIENCE

Citation Formats

Bhatia, Harsh, Gyulassy, Attila, Ong, Mitchell, Lordi, Vincenzo, Draeger, Erik, Pask, John, Pascucci, Valerio, and Bremer, Peer -Timo. Understanding Lithium Solvation and Diffusion through Topological Analysis of First-Principles Molecular Dynamics. United States: N. p., 2016. Web. doi:10.2172/1331475.
Bhatia, Harsh, Gyulassy, Attila, Ong, Mitchell, Lordi, Vincenzo, Draeger, Erik, Pask, John, Pascucci, Valerio, & Bremer, Peer -Timo. Understanding Lithium Solvation and Diffusion through Topological Analysis of First-Principles Molecular Dynamics. United States. doi:10.2172/1331475.
Bhatia, Harsh, Gyulassy, Attila, Ong, Mitchell, Lordi, Vincenzo, Draeger, Erik, Pask, John, Pascucci, Valerio, and Bremer, Peer -Timo. Tue . "Understanding Lithium Solvation and Diffusion through Topological Analysis of First-Principles Molecular Dynamics". United States. doi:10.2172/1331475. https://www.osti.gov/servlets/purl/1331475.
@article{osti_1331475,
title = {Understanding Lithium Solvation and Diffusion through Topological Analysis of First-Principles Molecular Dynamics},
author = {Bhatia, Harsh and Gyulassy, Attila and Ong, Mitchell and Lordi, Vincenzo and Draeger, Erik and Pask, John and Pascucci, Valerio and Bremer, Peer -Timo},
abstractNote = {The performance of lithium-ion batteries is strongly influenced by the ionic conductivity of the electrolyte, which depends on the speed at which Li ions migrate across the cell and relates to their solvation structure. The choice of solvent can greatly impact, both, the solvation and diffusivity of Li ions. In this work, we present our application of the topological techniques to extract and predict such behavior in the data generated by the first-principles molecular dynamics simulation of Li ions in an important organic solvent -ethylene carbonate. More specifically, we use the scalar topology of the electron charge density field to analyze the evolution of the solvation structures. This allows us to derive a parameter-free bond definition for lithium-oxygen bonds, to provide a quantitative measure for bond strength, and to understand the regions of influence of each atom in the simulation. This has provided new insights into how and under what conditions certain bonds may form and break. As a result, we can identify and, more importantly, predict, unstable configurations in solvation structures. This can be very useful in understanding when small changes to the atoms' movements can cause significantly different bond structures to evolve. Ultimately, this promises to allow scientists to explore lithium ion solvation and diffusion more systematically, with the aim of new insights and potentially accelerating the calculations themselves.},
doi = {10.2172/1331475},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Tue Sep 27 00:00:00 EDT 2016},
month = {Tue Sep 27 00:00:00 EDT 2016}
}

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