Unlocking the potential of photoexcited molecular electron spins for room temperature quantum information processing

Abstract Future information processing technologies like quantum memory devices have the potential to store and transfer quantum states to enable quantum computing and networking. A central consideration in practical applications for such devices is the nature of the light-matter interface which determines the storage state density and efficiency. Here, we employ an organic radical, α , γ -bisdiphenylene- β -phenylallyl doped into an o-terphenyl host to explore the potential for using tuneable and high-performance molecular media in microwave-based quantum applications. We demonstrate that this radical system exhibits millisecond-long spin-lattice relaxation and microsecond-long phase memory times at room temperature, while also having the capability to generate an oscillating spin-polarized state using a co-dissolved photo-activated tetraphenylporphyrin moiety, all enabled by using a viscous liquid host. This latest system builds upon collective wisdom from previous molecules-for-quantum literature by combining careful host matrix selection, with dynamical decoupling, and photoexcited triplet-radical spin polarisation to realise a versatile and robust quantum spin medium.