Author ORCID Identifier

https://orcid.org/0000-0003-3283-3253

Document Type

Thesis

Date of Award

2024

Degree Name

Master of Science (MS)

Department

Chemistry

First Advisor

Bess Vlaisavljevich

Abstract

There has been a great interest in developing new information technologies. Single molecule magnets (SMMs) are emerging as materials for high density data storage, qubits, and molecular spintronics. SMMs containing lanthanide or actinide centers are of interest due to their potentially high magnetic anisotropy. This would enable the use of SMMs at higher temperatures. Accurately modelling the electronic structure of f-element complexes can be quite challenging. Density Functional Theory (DFT) is a popular choice for optimizing geometry and studying the electronic structure due to its relatively low cost. In certain cases, more accuracy is desired or necessary to predict experimental values. Utilizing methods that can recover strong correlation (i.e., CASSCF) and spin-orbit effects (i.e., CASSCF-SO) can improve this accuracy. This thesis explores the synthesis and geometry of a decanuclear dysprosium-based sandwich SMM using DFT. The bridging ligand's steric hindrance and the stereocenter contribute to the bending creating a cyclic structure. The electronic structure of a series of actinide sandwich structures are assessed with a variety of methodology. This thesis assesses and compares the effects of state truncation with CASSCF-SO and Dirac-CASSCF calculations. These investigations demonstrate the ability of computation to assist experiments with the design, synthesis, and assessment of lanthanide and actinide-based single molecule magnets. These predictions will allow us to better understand the chemistry of these elements and develop new information technologies.

Subject Categories

Chemistry | Computational Chemistry | Inorganic Chemistry

Keywords

actinide, cross-coupling, dirac-casscf, polynuclear complex, sandwich complex, single molecule magnet

Number of Pages

57

Publisher

University of South Dakota

Available for download on Friday, August 29, 2025

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