Room-temperature optically detected coherent control of molecular spins

Abstract

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.

9 pages, 4 figures

References in corpus (4)

• High-sensitivity diamond magnetometer with nanoscale resolution
• Reversible spin-optical interface in luminescent organic radicals
• Molecular imaging by optically-detected electron spin resonance of nitrogen-vacancies in nanodiamond
• Quantum sensing of magnetic fields with molecular color centers

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• Growth of few-layer molecular crystals of PTCDI on hexagonal boron nitride by microspacing air-gap sublimation
• Organic molecules as single-photon sources
• Floquet Engineering Clock Transitions in Magnetic Molecules