Room-temperature optically detected coherent control of molecular spins

• Main Authors: Mena, Adrian, Mann, Sarah K, Cowley-Semple, Angus, Bryan, Emma, Heutz, Sandrine, McCamey, Dane R, Attwood, Max, Bayliss, Sam L
• Format: Journal Article
• Language: English
• Published: 12-02-2024
• Subjects: Physics - Chemical Physics; Physics - Quantum Physics
• DOI: 10.48550/arxiv.2402.07572

Phys. Rev. Lett. 133, 120801 (2024) Benefiting from both molecular tunability and versatile methods for
deployment, optically interfaced molecular spins are a promising platform for
quantum technologies such as sensing and imaging. Room-temperature optically
detected coherent spin control is a key enabler for many applications,
combining sensitive readout, versatile spin manipulation, and ambient
operation. Here we demonstrate such functionality in a molecular spin system.
Using the photoexcited triplet state of organic chromophores (pentacene doped
in a para-terphenyl host), we optically detect coherent spin manipulation with
photoluminescence contrasts exceeding 10% and microsecond coherence times at
room temperature. We further demonstrate how coherent control of multiple
triplet sublevels can significantly enhance optical spin contrast, and extend
optically detected coherent control to a thermally evaporated thin film,
retaining high photoluminescence contrast and coherence times of order one
microsecond. These results open opportunities for room-temperature quantum
technologies that can be systematically tailored through synthetic chemistry.