  Systems exhibiting both spin and orbital degrees of freedom, of which Er3+ is
one, can offer mechanisms for manipulating and measuring spin states via
optical excitations. Motivated by the possibility of observing
photoluminescence and electron paramagnetic resonance from the same species
located within a fullerene molecule, we initiated an EPR study of Er3+ in
ErSc2N@C80. Two orientations of the ErSc2N rotor within the C80 fullerene are
observed in EPR, consistent with earlier studies using photoluminescence
excitation (PLE) spectroscopy. For some crystal field orientations, electron
spin relaxation is driven by an Orbach process via the first excited electronic
state of the 4I_15/2 multiplet. We observe a change in the relative populations
of the two ErSc2N configurations upon the application of 532 nm illuminations,
and are thus able to switch the majority cage symmetry. This
photoisomerisation, observable by both EPR and PLE, is metastable, lasting many
hours at 20 K.
