Kewu Bai

A Comprehensive Search for Stable Pt-Pd Nanoalloy Configurations and Their Use as Tunable Catalysts

Using density-functional theory, we predict stable alloy configurations (ground states) for a 1 nm Pt-Pd cuboctahedral nanoparticle across the entire composition range and demonstrate their use as tunable alloy catalysts via hydrogen-adsorption studies. Unlike previous works, we use simulated annealing with a cluster expansion Hamiltonian to perform a rapid and comprehensive search that encompasses both high and low-symmetry configurations. The ground states show Pt(core)-Pd(shell) type configurations across all compositions but with specific Pd patterns. For catalysis studies at room temperatures, the ground states are more realistic structural models than the commonly assumed random alloy configurations. Using the ground states, we reveal that the hydrogen adsorption energy increases (decreases) monotonically with at. % Pt for the {111} hollow ({100} bridge) adsorption site. Such trends are useful for designing tunable Pd-Pt nanocatalysts for the hydrogen evolution reaction.

Correlation between optical absorption redshift and carrier density in phase change materials

Here, we report an optical absorption redshift map for GeTe-Sb2Te3 pseudo-binary alloys. We found that, with phase change from amorphous to crystalline, the observed redshift increases with Ge concentration along pseudo-line of compositions, which directly reflects the enhanced electron delocalization/resonant bonding and increased carrier concentrations in the respective crystal compounds. The measured valence band maximum shift towards the Fermi energy from amorphous to crystalline phase supports the observed similar trend in redshift and carrier density. We show that the correlation between optical redshift and carrier density, attributed to the resonant bonding, can be rationalized by calculating the valence electron concentration, the ionicity, and hybridization.