Computational design of Solvated-electron-based Materials for Applications in Redox Chemistry and Quantum Information

Auburn University, Auburn AL

Investigators

Abstract

With support from the Chemical Structure and Dynamics (CSD) program in the Division of Chemistry, Professors Evangelos Miliordos, Marcelo Kuroda, and Konstantin Klyukin of Auburn University are employing computational methods to a novel class of electronic materials known as solvated electron precursor electrides (SEPEs). Electrides are materials comprised of atomic or molecular layers with diffuse electrons occupying the interstitial space between the layers. These diffuse electrons could give rise to new electronic and magnetic properties that could be harnessed for a range of technologies, including advanced quantum computing, but their behavior is difficult to describe, making it difficult to connect it with the underlying molecular framework. Professor Miliordos, Kuroda, and Klyukin and their students will develop state-of-the-art computational simulations based on molecular and periodic approaches to model these diffuse electrons. Their work could clarify the structure-property-function relationships in these systems and advance the rational design and experimental realization of SEPE-based materials. The project will also provide research opportunities for graduate and undergraduate students and thus contribute to the development of STEM workforce. Solvated electron precursors are made of a positively charged metal centers fully coordinated by ligands which can sustain at least one peripheral diffuse electron, not bound to a specific atom or molecule. The aggregation of multiple SEPs leads to the formation of nanoparticles and materials known as SEPEs. The work of Professors Miliordos, Kuroda, and Klyukin will analyze the properties of structures where SEPs are connected via molecular bridges (linked-SEPEs) or are deposited on surfaces (surface immobilized SEPEs). The tunable composition of the electride-based material platforms offers enhanced control of the topological and electronic features owing to the variety of metals, ligands, materials, and linkers that can be used. Employing high-level multi-reference and density functional studies, this study will elucidate the underlying mechanisms defining their properties. This work will also provide design guidelines for a range of applications, including the development of chemical catalysts with low activation energy barriers, the reduction of overpotentials in electrochemical processes, the facilitation of multi-electron redox reactions, and the creation of qubits with extended coherence times and controlled entanglement. This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.