Events in inorganic chemistry.

Sila-Diamondoids: Atomically Precise Clusters of Crystalline Silicon

This talk will describe the synthesis, derivatization, and quantum transport properties of silicon diamondoids—atomically precise clusters of crystalline silicon. First, we describe strategies for the functionalization of the fundamental silicon diamondoid cluster, sila-adamantane. Mechanistic insights support that an aluminate-stabilized silylium at the 2-position of sila-adamantane is the terminal intermediate in its isomerization synthesis; we can intercept this intermediate to install halides at the 2-position.

More Than Simple Lewis Acids - Molecular Perspectives of Rare-Earths at the Interfaces of Catalysis, Sustainability, and Materials

The rare-earths (lanthanides + group III) are critical materials that underlie numerous technological advances ranging from information storage, human health, high-performance electronics, energy and the environment, and catalysis. Robust connections between molecular structure, properties, and function are central to advancing the performance and sustainability of these materials; however, achieving this can be limited by the complexity and heterogeneity in homogeneous and heterogeneous systems alike.

Discovery of Manganese-Dependent Monooxygenases

The aerobic oxidation of carbon–hydrogen (C–H) bonds in biology is currently known to be accomplished by a limited set of cofactors that largely include heme, nonheme iron, and copper. While manganese cofactors perform difficult oxidation reactions, including water oxidation within Photosystem II, they are generally not known to be used for C–H bond oxidation, and those that do catalyze this important reaction display highly limited intrinsic reactivity.

C-H functionalization inspired by copper enzymes

Abstract: High-valent Cu(III) complexes have long been proposed as important intermediates in biological redox processes and organic transformations involving the activation of C-H bonds. However, the proposed high-valent Cu(III) intermediates often elude detection due to their fleeting lifetimes. In the first part of my talk, I will present a series of dicopper (II,III) coordination complexes as models to understand the reactivity of NO and NO2- at dicopper enzymes.

Control of Reaction Outcome by Iron Oxygenases

Enzymes that use iron cofactors to activate molecular oxygen for hydroxylation, halogenation, desaturation, epoxidation, fragmentation, and peroxidation of unactivated carbon centers must guide their very reactive intermediates down preferred reaction paths to their specific outcomes. Our growing understanding of the general and enzyme-specific control strategies used by these enzymes has enabled the development of new catalytic capabilities and provided a roadmap for deployment of these enzymes in biocatalysis.

Molecular Quantum Information Science with Electron Spins

Abstract: Quantum technologies based on molecular electron spin coherence afford unique potential in miniaturization, spatial localization, and tunability through synthetic chemistry and our ability to leverage and manipulate more complex biological systems. However, many applications within molecular quantum information science hinge on prolonged spin relaxation, a process that effectively leaks quantum information into the environment. Additionally, applications such as quantum sensing with molecular quantum bits (qubits) have only recently undergone exploration.

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