Synthetic Control of Lanthanide Physical Properties Using Functionalized Metallacrowns

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With the support of the Chemical Structure, Dynamics, and Mechanisms-B (CSDM-B) Program in the Division of Chemistry, Professor Vincent L. Pecoraro of the University of Michigan, Ann Arbor will study the synthesis of new metal based molecules that may serve a variety of practical applications such as luminescent imaging, temperature measurements across a broad, technologically important range (150-400 K). As an integral part of these studies, the Pecoraro team will work to develop a fundamental understanding of the electronic structure of lanthanide ions in and out of applied magnetic fields. The studies will be utilized in applications ranging from understanding the production of qubits from lanthanide based molecules used in quantum computers, to measuring precise temperatures for electronic materials or cells and tissues. Research collaborations with scientists at the Centre Biophysique Moleculaire (CBM) in Orleans and University of Paris-Saclay will broaden the experience of trainees from both countries. The results of these studies will be disseminated worldwide and could provide basic science foundations directly relevant to applications varying from the development of white light emitting diodes, to microelectronics and to Josephson junctions for cell biology and medicine. The targeted metallacrowns will also be used in the public educational outreach presentations/activities planned both in the United States and Europe. The main objective of this proposal is the development of MCs in two main areas: innovative luminescent agents and metallacrown-cored dendrimers. The primary objective of this research proposal is to further the understanding of lanthanide electronic structure and to exploit the superb luminescence properties of the lanthanides using functionalized metallacrowns. Scientific collaborations are included that will help expand the impact of this work to areas such as biological imaging or material science. As MCs can incorporate different modular components, the same/similar scaffolds will be used to achieve the varied objectives of these lanthanides metallacrown systems. These systems are well suited to make innovative luminescent imaging agents, novel nanothermometers, and stable metallodendrimers. Emphasis will be placed on shifting the excitation energies for Ga- and Ln-based metallacrown emitters to the red, to provide a more biologically compatible chromophore for near infrared emission studies. To achieve this and other goals, molecules will be synthesized and purified in order to clarify the fundamental electronic structure of these lanthanide complexes, using, for example, Stark spectroscopy.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.