Many phenomena cannot be probed by experiments because the conditions are too extreme (high T, p), the species too short-lived, or the features are buried with no obvious way to probe them. In these situations, computer simulations can fill a niche of knowledge. My research is concerned with developing and applying accurate quantum mechanics based simulation tools for predicting the behavior of molecules and materials. By starting from the fundamental laws of quantum mechanics, we are able to develop independent means of characterization, i.e., non-empirical, predictive tools that do not rely on any information from experiment. Such independent tools are validated against known measurements to assess accuracy and then are used to predict properties for which measurements to not exist. Interested students will need strong backgrounds in undergraduate level mathematics, physical chemistry, quantum mechanics, and potentially solid state physics. Experience with computer programming is not essential but is a plus.
Ongoing methods development projects include:
- Our linear scaling orbital-free density functional theory (OF-DFT) method now handles up to a million atoms. Here the challenge is to develop accurate yet efficient kinetic energy density functionals. A recent breakthrough allowed us to extend the reliable reach of OF-DFT beyond nearly-free-electron-like metals to covalently bonded materials.
- Our fast algorithms for multireference correlated wavefunction (CW) theories provide accurate descriptions of ground and excited states of molecules containing up to 50 heavy atoms (e.g., we reduced the conventional O(N6) scaling of multi-reference configuration interaction all the way down to linear while retaining chemical accuracy).
- Our embedded CW theory combines quantum chemistry with periodic DFT (or our ab initio DFT+U theory) to treat local ground and excited electronic states in condensed matter, including strongly correlated electron materials.
Applications are focused on materials characterization and design for energy applications, including the following:
- Evaluation of pyrolysis and combustion thermochemistry and kinetics of biodiesel fuel
- Characterization of redox chemistry, ion diffusion, and conductivity in solid oxide fuel cell cathode materials
- Mechanical properties of aluminum and magnesium alloys, toward design of lightweight, fuel-efficient vehicles
- Local and band-to-band excitation energies, and carrier lifetime and mobility, in alternative photovoltaic materials
- Evaluation of redox chemistry on surfaces of novel photocatalysts for water splitting to produce hydrogen fuel
Selected Recent Publications
- T. S. Chwee and E. A. Carter, “Cholesky Decomposition within Local Multireference Singles and Doubles Configuration Interaction,” J. Chem. Phys., 132, 074104 (2010).
- C. Huang and E. A. Carter, “Nonlocal orbital-free kinetic energy density functional for semiconductors,” Phys. Rev. B, 81, 045206 (2010).
- D. F. Johnson and E. A. Carter, “First Principles Assessment of Hydrogen Absorption into FeAl and Fe3Si: Towards Prevention of Steel Embrittlement,” Acta Materialia, 58, 638 (2010).
- S. Sharifzadeh, P. Huang, and E. A. Carter, “Origin of Tunneling Lineshape Trends for Kondo States of Co Adatoms on Coinage Metal Surfaces,” J. Phys.: Condens. Matter, 21, 355501 (2009).
- L. Hung and E. A. Carter, “Accurate Simulations of Metals at the Mesoscale: Explicit Treatment of 1 Million Atoms with Quantum Mechanics,” Chem. Phys. Lett., 475, 163 (2009). (Cover Article)
- I. Milas and E. A. Carter, “Effect of Dopants on Alumina Grain Boundary Sliding: Implications for Creep Inhibition,” J. Mater. Sci., 44, 1741 (2009).
- E. A. Carter, “Challenges in Modeling Materials Properties without Experimental Input,” Science, 321, 800 (2008).
- K. A. Marino and E. A. Carter, “The effect of platinum on defect formation energies in β-NiAl,” Acta Materialia, 56, 3502 (2008).
- N. J. Mosey, P. Liao, and E. A. Carter, “Rotationally-Invariant ab initio Evaluation of Coulomb and Exchange Parameters for DFT + U Calculations,” J. Chem. Phys., 129, 014103 (2008).
- A. Ramasubramaniam and E. A. Carter, “Coupled quantum-atomistic and quantum-continuum mechanics methods in materials research,” Materials Research Society Bulletin, 32, 913 (2007).
- G. Ho, M.T. Ong, K.J. Caspersen, and E. A. Carter, “Energetics and Kinetics of Vacancy Diffusion and Aggregation in Shocked Aluminum via Orbital-Free Density Functional Theory,” PhysChemChemPhys, 9, 4951 (2007). (Cover Article)
- K. M. Carling and E. A. Carter, “Effects of segregating elements on the adhesive strength and structure of the α-Al2O3/β-NiAl interface,” Acta Materialia, 55, 2791 (2007).
- P. Huang and E. A. Carter, “Self-consistent embedding theory for locally correlated configuration interaction wave functions in condensed matter,” J. Chem. Phys., 125, 084102 (2006).
- P. Huang and E. A. Carter, “Local electronic structure around a single Kondo impurity,” Nano Letters, 6, 1146 (2006). (Cover Article)
- A. Andersen and E. A. Carter, “Insight into Selected Reactions in Low-Temperature Dimethyl Ether Combustion from Born-Oppenheimer Molecular Dynamics,” J. Phys. Chem., 110, 1393 (2006).