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Optical Addressability of the Arylnitrene Spin Triplet

MetadataDetails
Publication Date2025-05-31
JournalThe Journal of Physical Chemistry Letters
AuthorsGaetano Ricci, Claire TonnelƩ, David Casanova
InstitutionsIkerbasque, Donostia International Physics Center
Citations1

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.