Triplet acyl-alkyl radical pairs generated by pulsed laser excitation within the constraints of their nanocrystalline ketone precursors were recently introduced as a potential platform for the robust and repeated instantiation of spin qubit pairs for applications in quantum information science. Here we report the transient absorption spectroscopy of a series of nanocrystalline ketone capable of generating triplet radical pairs with persistent triphenylmethyl radicals forced to remain within bonding distances of highly reactive benzoyl radicals. We propose that triplet radical pair lifetimes in excess of 4 ms are the result of the short inter-radical distances and the colinear orientation of the two singly occupied orbitals, which are expected to result in large singlet-triplet energy gaps, large zero-field splitting parameters, and a poor geometry for spin-obit coupling.

Exceptionally long lifetimes of radical pairs containing the trityl radical in the crystalline solid state

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ACS Fall 2022

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