Contact
Faculty Assistant

Nari L. Baughman
baughman@princeton.edu
Engineering Quad, D404
609-258-9196

Research Focus

Development and application of first principles quantum mechanics based simulation methods for molecules and materials, with particular emphasis on energy applications.

Teaching at Princeton has been the highlight of my career in Chemistry.

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 do 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.
Research Areas
Inorganic Chemistry
Materials
Spectroscopy / Physical Chemistry
Honors

Fred Kavli Innovations in Chemistry Lecturer, American Chemical Society (2016)
 
Member, National Academy of Engineering (2015)
 
2015-16 Joseph O. Hirschfelder Prize in Theoretical Chemistry, Theoretical Chemistry Institute at the University of Wisconsin, Madison (2015)
 
2014 Ira Remsen Award, Maryland Section of the American Chemical Society, Johns Hopkins University (2014)
 
Sigillo D’Oro (Golden Sigillum) Medal, Italian Chemical Society, Scuola Normale Superiore, Pisa, Italy (2013)
 
Docteur Honoris Causa from L’Ecole Polytechnique Federale de Lausanne, Switzerland (EPFL) (2012)
 
August Wilhelm von Hofmann Lecture Award, German Chemical Society (2011)
 
Member, International Academy of Quantum Molecular Science (2009)
 
Member, National Academy of Sciences (2008)
 
Fellow, American Academy of Arts and Sciences (2008)

Selected Recent Publications

K. Yu and E. A. Carter, “Determining and Controlling the Stoichiometry of Cu2ZnSnS4 Photovoltaics: the Physics and Its Implications,” Chem. Mater., 28, 4415 (2016). doi: 10.1021/acs.chemmater.6b01612

M. Chen, X. Jiang, H. Zhuang, L. Wang, and E. A. Carter, “Petascale Orbital-Free Density Functional Theory Enabled by Small-Box Algorithms,” J. Chem. Theor. Comp., 12, 2950 (2016). doi: 10.1021/acs.jctc.6b00326

A. M. Ritzmann, J. M. Dieterich, and E. A. Carter, “Density Functional Theory +U Analysis of the Electronic Structure and Defect Chemistry of LSCF (La0.5Sr0.5Co0.25Fe0.75O3-δ),” Phys. Chem. Chem. Phys., 18, 12260 (2016). doi: 10.1039/C6CP01720G

H. Zhuang, A. J. Tkalych, and E. A. Carter, “Understanding and Tuning the Hydrogen Evolution Reaction on Pt-Covered Tungsten Carbide Cathodes,” J. Electrochem. Soc., 163, F629 (2016). doi: 10.1149/2.0481607jes

J. Xia and E. A. Carter, “Orbital-Free Density Functional Theory Study of Amorphous Li-Si Alloys and Introduction of a Simple Density Decomposition Formalism,” Modell. Simul. Mater. Sci. Eng., 24, 035014 (2016). doi: 10.1088/0965-0393/24/3/035014

T. Tan, X. Yang, Y. Ju, and E. A. Carter, “Ab Initio Reaction Kinetics of CH3OC(=O) and CH2OC(=O)H Radicals,” J. Phys. Chem. B, 120, 1590 (2016). doi: 10.1021/acs.jpcb.5b07959

J. M. P. Martirez and E. A. Carter, “Thermodynamic Constraints in Using AuM (M= Fe, Co, Ni and Mo) alloys as N2 Dissociation Catalysts: Functionalizing a Plasmon-Active Metal,” ACS Nano, 10, 2940 (2016). doi: 10.1021/acsnano.6b00085

N. Alidoust, M. Lessio, and E. A. Carter, “Cobalt (II) oxide and nickel (II) oxide alloys as potential intermediate-band semiconductors: A theoretical study,” J. Appl. Phys., 119, 025102 (2016). doi: 10.1063/1.4939286