Optical control and read out of individual electronic spins hosted in solid-state materials has catapulted these platforms to the forefront of quantum sensing and communication technologies. Translating this optical-spin interface into molecular systems would create a synthetically flexible platform to design tailor-made qubits for specific tasks, a potentially transformative approach for atomistic design of quantum technologies. The diverse array of electronic structures of lanthanide ions in solid-state hosts provides the key features to recapitulate the desired optical-spin interface in molecular analogues. Specifically, Ce3+ systems offer ideal quantum sensor targets where the symmetry-allowed 4f-5d transitions result in high fluorescence quantum yields and nanosecond optical emission lifetimes that couple to the ground state spin, while the high optical coherence of the 4f-4f transitions in ions such as Yb3+, Nd3+, and Er3+ provide ideal targets for communication technologies. Here, we outline the design features required to translate the mechanisms for optical-spin addressability of lanthanide defect-based qubit candidates into readily tunable, molecular systems. Well-precedented photocatalyst and molecular magnet materials provide the foundational basis for our molecular design space with low coordinate Ce3+ systems. We then evaluate the optical-spin interface of such candidates with photoluminescence and magnetic resonance spectroscopic characterization which, when coupled with electronic structure calculations, provide a rapid design-characterization-evaluation-iteration feedback mechanism to optimize our molecular design. Introducing this optical-spin interface into lanthanide-based molecular spins represents an essential first step to implement qubits designed from the bottom-up in quantum sensing and networking technologies.

Lanthanide optically addressable molecular qubits for quantum information science

Fall 2022 abstracts, posters, and presentations will launch in mid-September.

ACS Fall 2022

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.