Photoinduced Spin Polarization of a Gadolinium Complex

This paper explores the interaction between a photoexcited organic chromophore and a gadolinium(III) ion in a complex, which exhibits an intriguing time evolution of the spin polarization in its electron paramagnetic resonance (EPR) signature. Time-resolved EPR, transient absorption, and photoluminescence spectroscopies combine with results from density functional theory and spectral simulations to allow elucidation of the photochemical mechanism and its impact on the complex's magnetic properties. We show that perturbation of the polarization of a gadolinium(III) ion is possible via photoexcitation of a neighboring, organic chromophore, reflected in the inversion of the lanthanide ion's EPR signal. We, therefore, suggest a new avenue to initialize and manipulate lanthanide-based qudits with potential applications in quantum information science.