Integrated computational framework for designing dynamically controlled alloy-oxide heterostructures
The team at the U. of California, Santa Barbara (Anton Van der Ven (PI), Harsha Gunda, Carlos Levi, Mayela Aldaz Cervantes) and U. of Michigan (Krishna Garikipati, Greg Teichert, Emmanuelle Marquis, Kathleen Chou, Peng-Wei Chu)
The aim of this program is to develop an infrastructure that integrates synthesis, multi-scale computation and precise experimental characterization to predict and elucidate the evolution of complex heterostructures and multi-phase coexistence. We are developing this infrastructure in the context of a fundamental study of oxidation processes of Ti and its alloys. Our study of oxidation reactions starts from the crystallographic and electronic structure and seeks to merge experimentally obtained mechanistic understanding of the evolution of metal-oxide heterostructures with predictive modeling. While the focus of this project is on oxidation in model systems, the integrated multiscale modeling methodology being developed here will be applicable to any dynamically evolving heterostructure involving phase evolution coupled with atomic and electronic transport. This includes batteries (Li-ion, Na-ion, Mg-ion as well as metal air batteries), fuel cells, and corrosion processes.
Our model systems, Ti and its alloys, are of tremendous importance in a wide variety of technological applications. Ti alloys are used in aerospace applications due to their high specific strength and corrosion resistance and as biomedical implants due to their excellent biocompatibility. The oxides of Ti also exhibit exceptional photocatalytic activity and have potential to serve as electrode materials in Li-ion and Na-ion batteries. In all these applications, the oxides of Ti play an important role and precise control of oxide formation during synthesis is crucial. The development of an integrated computational and experimental methodology will enable the rational design of new oxide heterostructures for a wide variety of applications.
The activities focus on model systems presenting a clear case for benchmarking and validating multiscale models that bridge descriptions of atomistic processes with continuum length scales. A major objective is to define design criteria for the stability and evolution of oxide/metal structures.
Experimental measurements are tightly integrated with modeling tasks, providing both input and validation. While the emphasis is on oxidation in model systems that exhibit a range of dynamic phenomena involving interfaces between different phases, the tools and integrated research methodology are applicable to any dynamically evolving heterostructure system coupling phase evolution with atomic and electronic transport. This includes batteries, fuel cells, and corrosion processes.
- CASM is a software package designed to perform first-principles statistical mechanical studies of multi-component crystalline solids. CASM interfaces with first-principles electronic structure codes, automates the construction and parameterization of effective Hamiltonians and subsequently builds highly optimized (kinetic) Monte Carlo codes to predict finite temperature thermodynamic and kinetic properties. https://github.com/prisms-center/CASMcode
- The mechanoChem code is an isogeometric analysis based code used to solve the partial differential equations describing solid mechanics (including gradient elasticity) and chemistry (including the Cahn-Hilliard phase field model). https://github.com/mechanoChem/mechanoChem
Data (Materials Commons)
- Initial data illustrating the oxidation behavior of pure Ti. link.
- Links will be updated soon!
- A three dimensional field formulation, and isogeometric solutions to point and line defects using Toupin’s theory of gradient elasticity at finite strains. Z. Wang, S. Rudraraju, K. Garikipati, Journal of the Mechanics and Physics of Solids, 94, 336-361 (2016). link
A comparison of Redlich-Kister polynomial and cubic spline representations of the chemical potential in phase field computations. Gregory H. Teichert, N. S. Harsha Gunda, Shiva Rudraraju, Anirudh Raju Natarajan, Brian Puchala, Krishna Garikipati, Anton Van der Ven (2016) Computational Materials Science, 128, 127–139 (2017) link
Li intercalation mechanisms in CaTi5O11, a bronze-B derived compound. D. Chang, A. Van der Ven, Physical Chemistry Chemical Physics, 18, 32042-32049 (2016). link
A variational treatment of material configurations with application to interface motion and microstructural evolution. G. H. Teichert, S. Rudraraju, K. Garikipati, Journal of the Mechanics and Physics of Solids, 99, 338-356 (2017). link
- Influence of a silicon-bearing film on the early stage oxidation of pure titanium. Kathleen Chou, Peng-Wei Chu , Carlos G. Levi , Emmanuelle A. Marquis. Journal of Materials Research (2017) 1-11. link
- Kathleen Chou. Poster to be presented at the Gordon conference on high temperature corrosion – July 2017
(NSF award #1436154)