Optical Addressability of the Arylnitrene Spin Triplet

Abstract

Optically addressable spin systems are key to quantum technologies, but solid-state defects such as nitrogen-vacancy centers face challenges in scalability and tunability. Here, we computationally explore arylnitrenes as molecular alternatives. High-accuracy calculations confirm a robust triplet ground state with spin-selective intersystem crossing and spin-vibronic-mediated reverse intersystem crossing, enabling efficient spin-state initialization. While pristine arylnitrene has weak optical transitions, targeted chemical modifications significantly enhance its emission capabilities without disrupting the symmetry rules governing the spin-state preparation mechanism. Combined with recent advances in nitrene stabilization and positioning, these results establish arylnitrenes as promising candidates for molecular spin qubits.