Magnetic Molecules for Quantum Information
A high-resolution spin-photon interface with molecular rare-earth ion qubits
9:12 am – 9:48 amCoherent coupling of electron spins and photons requires spin-selective optical transitions that are robust to environmental noise. This bridge between microwave and optical frequencies can enable photon-mediated scaling and control in quantum technologies, as demonstrated in trapped atom, ion, and solid-state spin qubits. Molecular analogs of such systems hold promise as a nascent qubit platform that can leverage the tools of synthetic chemistry to tailor quantum properties, but have thus far been limited by broad, incoherent optical transitions. We describe the development of optically addressable molecular qubits utilizing a central spin-bearing rare-earth ion. We demonstrate coherent control of the spin ground-state and high-resolution spin-selective optical transitions. The resulting spin-optical interface enables high-contrast detection and direct optical control of ground-state spin polarization. Given the remarkable capacity for optical coherence with rare-earth ions, this demonstration provides a key step toward engineering coherent spin-photon coupling by chemical design.