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Freedman, Danna E. Yi, Seungyeon Massachusetts Institute of Technology. Department of Chemistry 2025-08-11T14:19:04Z 2025-08-11T14:19:04Z 2025-05 2025-06-11T15:13:09.803Z https://hdl.handle.net/1721.1/162332 https://orcid.org/0000-0001-9383-7712 Optical detection of magnetic phenomena offers a compelling pathway toward the development of highly sensitive and versatile molecular sensors. This thesis investigates the design of metal complexes tailored for magnetic field read-out through light–matter interactions, focusing on two strategies. The first section explores magnetochiral dichroism (MChD), an optical effect that emerges from the interplay between molecular chirality and magnetism. By systematically varying the metal centers within a series of chiral lanthanide complexes—specifically, Tb³⁺ and Dy³⁺—we examine how differences in magnetic moment modulate the MChD response. This comparative study reveals fundamental chemical design principles for enhancing MChD intensity and deepens our understanding of how structural and electronic factors jointly shape this directional optical effect. The second section addresses the challenge of engineering optically addressable molecular qubits based on Ni²⁺ complexes. Realizing effective spin-state read-out in these systems requires precise control over both magnetic and photophysical properties. To this end, we investigate ligand modification strategies aimed at enhancing luminescence while preserving an S = 1 ground state suitable for quantum applications. Collectively, we hope these studies contribute to a better understanding of the design space for spin–photon coupled molecular systems, offering new tools for magnetooptical sensing. Ph.D. Massachusetts Institute of Technology Attribution-ShareAlike 4.0 International (CC BY-SA 4.0) Copyright retained by author(s) https://creativecommons.org/licenses/by-sa/4.0/ Leveraging Metal Complexes for Optical Read-out of Magnetic Fields Thesis application/pdf Doctoral Doctor of Philosophy Publication unknown unknown <Publication xmlns="https://www.openaire.eu/cerif-profile/1.1/" id="7a40e705-61f1-4293-b446-fcd0705a04ac"> <Type xmlns="https://www.openaire.eu/cerif-profile/vocab/COAR_Publication_Types">http://purl.org/coar/resource_type/c_1843</Type> <Title>Leveraging Metal Complexes for Optical Read-out of Magnetic Fields</Title> <PublishedIn> <Publication> </Publication> </PublishedIn> <PublicationDate>2025-05</PublicationDate> <Authors> <Author> <DisplayName>Yi, Seungyeon</DisplayName> <Affiliation> <OrgUnit> </OrgUnit> </Affiliation> </Author> </Authors> <Editors> </Editors> <Publishers> <Publisher> <DisplayName>Massachusetts Institute of Technology</DisplayName> <OrgUnit /> </Publisher> </Publishers> <License>https://creativecommons.org/licenses/by-sa/4.0/</License> <Abstract>Optical detection of magnetic phenomena offers a compelling pathway toward the development of highly sensitive and versatile molecular sensors. This thesis investigates the design of metal complexes tailored for magnetic field read-out through light–matter interactions, focusing on two strategies. The first section explores magnetochiral dichroism (MChD), an optical effect that emerges from the interplay between molecular chirality and magnetism. By systematically varying the metal centers within a series of chiral lanthanide complexes—specifically, Tb³⁺ and Dy³⁺—we examine how differences in magnetic moment modulate the MChD response. This comparative study reveals fundamental chemical design principles for enhancing MChD intensity and deepens our understanding of how structural and electronic factors jointly shape this directional optical effect. The second section addresses the challenge of engineering optically addressable molecular qubits based on Ni²⁺ complexes. Realizing effective spin-state read-out in these systems requires precise control over both magnetic and photophysical properties. To this end, we investigate ligand modification strategies aimed at enhancing luminescence while preserving an S = 1 ground state suitable for quantum applications. Collectively, we hope these studies contribute to a better understanding of the design space for spin–photon coupled molecular systems, offering new tools for magnetooptical sensing.</Abstract> <Access xmlns="http://purl.org/coar/access_right" > </Access> </Publication>