The
spin relaxation dynamics of Cr3+ substitutional
dopants in ∼10 nm colloidal SrTiO3 nanocrystals
(NCs) has been studied by variable-temperature electron paramagnetic
resonance (EPR) spectroscopy and continuous wave EPR power saturation
measurements between 4.2 and 50 K. The presence of self-trapped electrons
introduced by anaerobic ultraviolet irradiation (photodoping) is able
to effectively accelerate the spin relaxation dynamics of localized
spins of Cr3+ through a cross-relaxation process. The extra
electrons introduced during photodoping trap on Ti-sites, creating
Ti3+ defects with EPR transitions that are observed only
at cryogenic temperatures because of fast spin–lattice relaxation.
The change in the spin relaxation upon photodoping the Cr-doped SrTiO3 NCs is totally reversible upon opening the sample to air.
This result provides a novel strategy to modulate spin dynamics in
individual NCs using photons where long-lived spins on dopant ions
couple to the fast-relaxing spins from metastable, transient defects.