How Well Can Quantum Embedding Method Predict the Reaction Profiles for Hydrogenation of Small Li Clusters?

Quantum computing leverages the principles of quantum mechanics in novel ways to tackle complex chemistry problems that cannot be accurately addressed using traditional quantum chemistry methods. However, the high computational cost and available number of physical qubits with high fidelity limit its application to small chemical systems. This work employed a quantum-classical framework which features a quantum active space-embedding approach to perform simulations of chemical reactions that require up to 14 qubits.

Au(SR) Nanocluster and a Periodic Pattern from Six to Fourteen Free Electrons in Core Size Evolution.

An Au(S-Bu) nanocluster (NC) is synthesized using the bulky -butyl thiol as the ligand. Single-crystal X-ray crystallography reveals that it has an Au core which evolves from the Au core in the previously reported Au(S-Bu), and the Au core is protected by longer staple-like surface motifs. The new Au NC extends the members of the face-centered cubic structural evolution by adding an Au triangle and an Au tetrahedron unit.

Boosting CO Electrochemical Reduction with Atomically Precise Surface Modification on Gold Nanoclusters.

Thiolate-protected gold nanoclusters (NCs) are promising catalytic materials for the electrochemical CO reduction reaction (CO RR). In this work an atomic level modification of a Au NC is made by substituting two surface Au atoms with two Cd atoms, and it enhances the CO RR selectivity to 90-95 % at the applied potential between -0.5 to -0.

Kinetic Monte Carlo simulation of CO adsorption on sulfur-covered Pd(100).

The use of atomistic Kinetic Monte Carlo method was explored to examine the influence of sulfur poisoning on CO adsorption on Pd(100) surface. The model explicitly incorporates key elementary processes such as CO adsorption and CO desorption including diffusion of surface CO and S species. Relevant energetic and kinetic parameters were derived using information calculated from density functional theory as a starting point.

Photomediated Oxidation of Atomically Precise Au25(SC2H4Ph)18(-) Nanoclusters.

The anionic charge of atomically precise Au25(SC2H4Ph)18(-) nanoclusters (abbreviated as Au25(-)) is thought to facilitate the adsorption and activation of molecular species. We used optical spectroscopy, nonaqueous electrochemistry, and density functional theory to study the interaction between Au25(-) and O2. Surprisingly, the oxidation of Au25(-) by O2 was not a spontaneous process.

Experimental and computational investigation of Au25 clusters and CO2: a unique interaction and enhanced electrocatalytic activity.

Atomically precise, inherently charged Au(25) clusters are an exciting prospect for promoting catalytically challenging reactions, and we have studied the interaction between CO(2) and Au(25). Experimental results indicate a reversible Au(25)-CO(2) interaction that produced spectroscopic and electrochemical changes similar to those seen with cluster oxidation. Density functional theory (DFT) modeling indicates these changes stem from a CO(2)-induced redistribution of charge within the cluster.

A flexible nudged elastic band program for optimization of minimum energy pathways using ab initio electronic structure methods.

A driver program for carrying out nudged elastic band optimizations of minimum energy reaction pathways is described. This approach allows for the determination of minimum energy pathways using only energies and gradient information. The driver code has been interfaced with the GAUSSIAN 98 program.