Mapping the surface of InP QD materials

Modifying the optoelectronic properties of nanostructured materials through introduction of dopant atoms has attracted intense interest, but the approaches employed are often trial and error, preventing rational design. We demonstrate the power of large-scale electronic structure calculations with density functional theory (DFT) to build an atlas of preferred sites for a range of M(II) and M(III) dopants in the representative III-V InP magic size cluster (MSC). We quantify the thermodynamic favorability of doping, which we identify to be both specific to the sites within the MSC (i.e., interior vs surface) and to the nature of the dopant atom (i.e., smaller Ga(III) vs larger Y(III) or Sc(III)). For isovalent doping (i.e., Y(III)/Sc(III) or Ga(III)), we observe stronger sensitivity of the predicted energetics to the ligand binding mode on the surface than to the dopant type. For M(II) (i.e., Zn or Cd) dopants, we show that the binding mode of ligand removed to balance charge during the doping reaction is critical. We observe limited cooperativity with dopants up to moderate concentrations, indicating rapid single-dopant estimations of favorability from DFT can efficiently guide rational design.

Our article on this topic was recently accepted in Chemistry of Materials. Check out the preprint here!

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.

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