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An illustration of the proposed spin-selective ISC mechanism for the observed PLDMR behaviour. At B z > 0.7 T and T < 0.8 K the m s = −1 sublevel in the ground state triplet is occupied, which has a small ISC probability. B z is the static magnetic field applied along the z -axis. When microwaves are switched on (right), a microwave-induced Δ m s = 1 transition drives population from m s = −1 to m s = 0 within the ground state. This m s = 0 sublevel has a higher probability for ISC in the excited state, which leads to more singlet PL and reduced triplet PL, manifest as a large PLDMR contrast. The samples for a were thin films made with 0.1 wt% M 2 TTM-3Flr-M 2 TTM doped into polystyrene, and in b , we doped 10 nM of M 2 TTM-3Flr-M 2 TTM into PhCl 3 crystal. The crystals were prepared using slow evaporation of a solution, which were subsequently washed and polished, as described in Supplementary Information Section 13 .

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