TY - JOUR
T1 - Evolutionary Optimization of a Charge Transfer Ionic Potential Model for Ta/Ta-Oxide Heterointerfaces
AU - Sasikumar, Kiran
AU - Narayanan, Badri
AU - Cherukara, Mathew
AU - Kinaci, Alper
AU - Sen, Fatih G.
AU - Gray, Stephen K.
AU - Chan, Maria K.Y.
AU - Sankaranarayanan, Subramanian K.R.S.
N1 - Funding Information:
This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility, supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02- 05CH11231. Use of the Center for Nanoscale Materials was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02- 06CH11357.
Publisher Copyright:
© 2017 American Chemical Society.
PY - 2017/4/25
Y1 - 2017/4/25
N2 - Heterostructures of tantalum and its oxide are of tremendous technological interest for myriad technological applications, including electronics, thermal management, catalysis, and biochemistry. In particular, local oxygen stoichiometry variation in TaOx memristors comprising thermodynamically stable metallic (Ta) and insulating oxide (Ta2O5) have been shown to result in fast switching on the subnanosecond time scale over a billion cycles. This rapid switching opens up the potential for advanced functional platforms such as stateful logic operations and neuromorphic computation. Despite its broad importance, an atomistic scale understanding of oxygen stoichiometry variation across Ta/TaOx heterointerfaces, such as during early stages of oxidation and oxide growth, is not well understood. This is mainly due to the lack of a unified interatomic potential model for tantalum oxides that can accurately describe metallic (Ta) and ionic (TaOx) as well as mixed (Ta/TaOx interfaces) bonding environments simultaneously. To address this challenge, we introduce a Charge Transfer Ionic Potential (CTIP) model for Ta/Ta-oxide system by training the model against lattice parameters, cohesive energies, equations of state (EOS), elastic properties, and surface energies of the various experimentally observed Ta2O5 polymorphs (hexagonal, orthorhombic, and monoclinic) obtained from density functional theory (DFT) calculations. The best CTIP parameters are determined by employing a global optimization scheme driven by genetic algorithms followed by local simplex optimization. Our newly developed CTIP potential accurately predicts structure, thermodynamics, and energetic ordering of polymorphs, as well as elastic and surface properties of both Ta and Ta2O5, in excellent agreement with DFT calculations and experiments. We employ our newly parametrized CTIP potential to investigate the early stages of oxidation and atomic scale mechanisms associated with oxide growth on the Ta surface at various temperatures. The CTIP potential developed in this work is an invaluable tool to investigate atomic-scale mechanisms and transport phenomena underlying the response of Ta/TaOx interfaces to external stimuli (e.g, temperature, pressure, strain, electric field, etc.), as well as other interesting dynamical phenomena including the physics of switching dynamics in TaOx based memristors and neuromorphic devices.
AB - Heterostructures of tantalum and its oxide are of tremendous technological interest for myriad technological applications, including electronics, thermal management, catalysis, and biochemistry. In particular, local oxygen stoichiometry variation in TaOx memristors comprising thermodynamically stable metallic (Ta) and insulating oxide (Ta2O5) have been shown to result in fast switching on the subnanosecond time scale over a billion cycles. This rapid switching opens up the potential for advanced functional platforms such as stateful logic operations and neuromorphic computation. Despite its broad importance, an atomistic scale understanding of oxygen stoichiometry variation across Ta/TaOx heterointerfaces, such as during early stages of oxidation and oxide growth, is not well understood. This is mainly due to the lack of a unified interatomic potential model for tantalum oxides that can accurately describe metallic (Ta) and ionic (TaOx) as well as mixed (Ta/TaOx interfaces) bonding environments simultaneously. To address this challenge, we introduce a Charge Transfer Ionic Potential (CTIP) model for Ta/Ta-oxide system by training the model against lattice parameters, cohesive energies, equations of state (EOS), elastic properties, and surface energies of the various experimentally observed Ta2O5 polymorphs (hexagonal, orthorhombic, and monoclinic) obtained from density functional theory (DFT) calculations. The best CTIP parameters are determined by employing a global optimization scheme driven by genetic algorithms followed by local simplex optimization. Our newly developed CTIP potential accurately predicts structure, thermodynamics, and energetic ordering of polymorphs, as well as elastic and surface properties of both Ta and Ta2O5, in excellent agreement with DFT calculations and experiments. We employ our newly parametrized CTIP potential to investigate the early stages of oxidation and atomic scale mechanisms associated with oxide growth on the Ta surface at various temperatures. The CTIP potential developed in this work is an invaluable tool to investigate atomic-scale mechanisms and transport phenomena underlying the response of Ta/TaOx interfaces to external stimuli (e.g, temperature, pressure, strain, electric field, etc.), as well as other interesting dynamical phenomena including the physics of switching dynamics in TaOx based memristors and neuromorphic devices.
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U2 - 10.1021/acs.chemmater.7b00312
DO - 10.1021/acs.chemmater.7b00312
M3 - Article
AN - SCOPUS:85018652296
SN - 0897-4756
VL - 29
SP - 3603
EP - 3614
JO - Chemistry of Materials
JF - Chemistry of Materials
IS - 8
ER -