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All-Carbon Polyradical Architectures

Abstract

Scanning probe techniques at the vacuum-solid interface have unlocked new avenues in the synthesis and study of reactive materials. The study of stable radicals has grown as a field since the onset of the twentieth century. Polyaromatic hydrocarbons (PAHs) have represented a significant portion of these studies. Though as the degree of radical or radicaloid nature of target structures increases, their solution synthesis and study become more challenging. Diradical(oid)s have been studied more regularly since the end of the twentieth century, with the achievement of tetraradical(oid)s and hexaradical(oid)s occurring only in the last few years. The solid-vacuum interfaces and scanning probe microscopy (SPM) have permitted an enormous leap in the accessibility of target structures and the robustness of characterization. For example, zigzag-edged graphene nanoribbons, unsubstituted triangulene molecules, and magnetic porphyrins have been studied using these methods. These methods have allowed a more detailed inspection of the magnetic properties of open-shell carbon materials. The work described in this dissertation targets all-carbon polyradical nanomaterials for the study of fundamental phenomena in carbon magnetism. This work has implications for next-generation spintronics and quantum computing. Chapter 2 focuses on the synthesis of a modular spin supergraphene of S = ½ phenalenyl and its 1-dimensional superpolyacetylene analogues. Chapter 3 focuses on the analogous study of S = 1 triangulene modular periodic materials. Chapter 4 focuses on 1-dimensional polyradical graphene nanoribbons (GNRs) in solution and at the vacuum-gold interface. These materials hold promise for achieving fully integrated molecular circuits. And finally, Chapter 5 focuses on 0-dimensional magnetic structures, biphenalenyl and bottom-up synthesis of a nitrogen-vacancy (NV) center.

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