Machine Learning Applied to a Variable Charge Atomistic Model for Cu/Hf Binary Alloy Oxide Heterostructures [Machine Learning a Variable Charge Atomistic Model for Cu/Hf Binary Alloy Oxide Heterostructures]

Sasikumar, Kiran; Chan, Henry; Narayanan, Badri; Sankaranarayanan, Subramanian K. R. S.

doi:10.1021/acs.chemmater.8b03969

Title: Machine Learning Applied to a Variable Charge Atomistic Model for Cu/Hf Binary Alloy Oxide Heterostructures [Machine Learning a Variable Charge Atomistic Model for Cu/Hf Binary Alloy Oxide Heterostructures]

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Abstract

Alloy oxide heterostructures are essential for a wide variety of energy applications, including anticorrosion coatings, bifunctional catalysis, energy storage, as well as emerging platforms for multilevel nonvolatile memory and neuromorphic devices. The key role played by oxide composition, density, and stoichiometry in governing electrochemical reactions, interface structure, and ionic transport in alloy oxides remains largely unknown. This is primarily due to the lack of variable charge interatomic potential models that can adequately describe the various atomic/ionic interactions in alloy oxides within a unified framework. Here, we introduce a charge transfer ionic potential (CTIP) model for Cu/Hf/O alloy system and demonstrate its ability to accurately capture the complex potential energy surface owing to dynamically varying interactions, including metallic (Cu/Hf), ionic (Cu/Hf/Ox), mixed environment (interfaces). We leverage supervised machine learning methods powered by genetic algorithms coupled with local simplex optimization to efficiently navigate through a high-dimensional parameter space and identify an optimum set of an independent set of CTIP parameters. We train our model against an extensive first-principles based data set that includes lattice constants, cohesive energies, equations of state, and elastic constants of various experimentally observed polymorphs of hafnia, copper oxide, hafnium, as well as copper. Our machine-learned CTIP model capturesmore »« less

Authors:

Sasikumar, Kiran ^[1];

^[1]; Narayanan, Badri ^[2];

^[3]

Argonne National Lab. (ANL), Argonne, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Louisville, Louisville, KY (United States)
Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Chicago, Chicago, IL (United States)

Publication Date:: Wed Apr 10 00:00:00 EDT 2019

Research Org.:: Argonne National Lab. (ANL), Argonne, IL (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1559462

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: Chemistry of Materials

Additional Journal Information:: Journal Volume: 31; Journal Issue: 9; Journal ID: ISSN 0897-4756

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE

Citation Formats


                    Sasikumar, Kiran, Chan, Henry, Narayanan, Badri, and Sankaranarayanan, Subramanian K. R. S. Machine Learning Applied to a Variable Charge Atomistic Model for Cu/Hf Binary Alloy Oxide Heterostructures [Machine Learning a Variable Charge Atomistic Model for Cu/Hf Binary Alloy Oxide Heterostructures].  United States: N. p., 2019. 
Web.  doi:10.1021/acs.chemmater.8b03969.

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                    Sasikumar, Kiran, Chan, Henry, Narayanan, Badri, & Sankaranarayanan, Subramanian K. R. S. Machine Learning Applied to a Variable Charge Atomistic Model for Cu/Hf Binary Alloy Oxide Heterostructures [Machine Learning a Variable Charge Atomistic Model for Cu/Hf Binary Alloy Oxide Heterostructures].  United States.  https://doi.org/10.1021/acs.chemmater.8b03969

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                    Sasikumar, Kiran, Chan, Henry, Narayanan, Badri, and Sankaranarayanan, Subramanian K. R. S. Wed .  
"Machine Learning Applied to a Variable Charge Atomistic Model for Cu/Hf Binary Alloy Oxide Heterostructures [Machine Learning a Variable Charge Atomistic Model for Cu/Hf Binary Alloy Oxide Heterostructures]".  United States.  https://doi.org/10.1021/acs.chemmater.8b03969.  https://www.osti.gov/servlets/purl/1559462.

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@article{osti_1559462,

  title        = {Machine Learning Applied to a Variable Charge Atomistic Model for Cu/Hf Binary Alloy Oxide Heterostructures [Machine Learning a Variable Charge Atomistic Model for Cu/Hf Binary Alloy Oxide Heterostructures]},

  author       = {Sasikumar, Kiran and Chan, Henry and Narayanan, Badri and Sankaranarayanan, Subramanian K. R. S.},

  abstractNote = {Alloy oxide heterostructures are essential for a wide variety of energy applications, including anticorrosion coatings, bifunctional catalysis, energy storage, as well as emerging platforms for multilevel nonvolatile memory and neuromorphic devices. The key role played by oxide composition, density, and stoichiometry in governing electrochemical reactions, interface structure, and ionic transport in alloy oxides remains largely unknown. This is primarily due to the lack of variable charge interatomic potential models that can adequately describe the various atomic/ionic interactions in alloy oxides within a unified framework. Here, we introduce a charge transfer ionic potential (CTIP) model for Cu/Hf/O alloy system and demonstrate its ability to accurately capture the complex potential energy surface owing to dynamically varying interactions, including metallic (Cu/Hf), ionic (Cu/Hf/Ox), mixed environment (interfaces). We leverage supervised machine learning methods powered by genetic algorithms coupled with local simplex optimization to efficiently navigate through a high-dimensional parameter space and identify an optimum set of an independent set of CTIP parameters. We train our model against an extensive first-principles based data set that includes lattice constants, cohesive energies, equations of state, and elastic constants of various experimentally observed polymorphs of hafnia, copper oxide, hafnium, as well as copper. Our machine-learned CTIP model captures the structure, elastic properties, thermodynamics, and energetic ordering of various polymorphs. It also accurately predicts the surface properties of both oxides and their metals. To demonstrate the suitability of our CTIP model for investigating dynamic processes, we employed it to identify the atomistic scale mechanisms associated with the initial nanoscale oxidation and surface oxide growth on Cu-doped hafnia surfaces. Here, our machine-learned CTIP model can be used to probe the dynamic response of Cu/Hf/O alloy interfaces subjected to external stimuli (e.g., electric field, pressure, temperature, strain, etc.) and a variety of atomistic phenomena including the dynamics of switching in emerging neuromorphic platforms.},

  doi          = {10.1021/acs.chemmater.8b03969},

  journal      = {Chemistry of Materials},

  number       = 9,

  volume       = 31,

  place        = {United States},

  year         = {Wed Apr 10 00:00:00 EDT 2019},

  month        = {Wed Apr 10 00:00:00 EDT 2019}

}

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