Improving DFT descriptions of surface chemistry

Approximate, semi-local density functional theory (DFT) suffers from delocalization error that can lead to a paradoxical model of catalytic surfaces that both overbind adsorbates yet are also too stable. We investigate the effect of two widely applied approaches for delocalization error correction, i) affordable DFT+U (i.e., semi-local DFT augmented with a Hubbard U) and ii) hybrid functionals with an admixture of Hartree-Fock (HF) exchange, on surface and adsorbate energies across a range of rutile transition metal oxides widely studied for their promise as water splitting catalysts.

Machine learning spin-state-dependent catalysis

Metal–oxo moieties are important catalytic intermediates in the selective partial oxidation of hydrocarbons and in water splitting. Stable metal–oxo species have reactive properties that vary depending on the spin state of the metal, complicating the development of structure–property relationships. To overcome these challenges, we train machine-learning (ML) models capable of predicting metal–oxo formation energies across a range of first-row metals, oxidation states, and spin states.

Improved uncertainty quantification for discovery

Machine learning (ML) models, such as artificial neural networks, have emerged as a complement to high-throughput screening, enabling characterization of new compounds in seconds instead of hours. The promise of ML models to enable large-scale, chemical space exploration can only be realized if it is straightforward to identify when molecules and materials are outside the model’s domain of applicability.

Enumeration for de novo inorganic chemistry

Despite being attractive targets for functional materials, the discovery of transition metal complexes with high-throughput computational screening is challenged by the amount of feasible coordination numbers, spin states, or oxidation states and the potentially large sizes of ligands. To overcome these limitations, we take inspiration from organic chemistry where full enumeration of neutral, closed shell molecules under the constraint of size has enriched discovery efforts.


About Us

The Kulik group focuses on the development and application of new electronic structure methods and atomistic simulations tools in the broad area of catalysis.

Our Interests

We are interested in transition metal chemistry, with applications from biological systems (i.e. enzymes) to nonbiological applications in surface science and molecular catalysis.

Our Focus

A key focus of our group is to understand mechanistic features of complex catalysts and to facilitate and develop tools for computationally driven design.

Contact Us

Questions or comments? Let us know! Contact Dr. Kulik: