Probing the Design Rules for Optimizing Electron Spin Relaxation in Densely Packed Triplet Media for Quantum Applications

Quantum technologies using electron spins have the advantage of employing chemical qubit media with tunable properties. The principal objective of material engineers is to enhance photoexcited spin yields and quantum spin relaxation. In this study, we demonstrate a facile synthetic approach to control spin properties in charge-transfer cocrystals consisting of 1,2,4,5-tetracyanobenzene (TCNB) and acetylated anthracene. We find that the extent and position of acetylation control the degree of charge-transfer and the optical band gap by modifying crystal packing and electronic structure. We further reveal that while the spin polarization of the triplet state is slightly reduced compared to prototypical Anthracene:TCNB, the phase memory (<i>T</i> _m) and, for 9-acetylanthracene:TCNB spin-lattice relaxation (<i>T</i> ₁) time, could be enhanced up to 2.4 times. Our findings are discussed in the context of quantum microwave amplifiers, known as masers, and show that acetylation could be a powerful tool for improving organic materials for quantum sensing applications.