High pressure electron spin resonance of the endohedral fullerene $^{15}\mathrm{N@C}_{60}$

Abstract

We measure the electron spin resonance spectrum of the endohedral fullerene molecule 15 N@C 60 at pressures ranging from atmospheric pressure to 0.25 GPa, and find that the hyperfine coupling increases linearly with pressure. We present a model based on van der Waals interactions, which accounts for this increase via compression of the fullerene cage and consequent admixture of orbitals with a larger hyperfine coupling. Combining this model with theoretical estimates of the bulk modulus, we predict the pressure shift and compare it to our experimental results, finding fair agreement given the spread in estimates of the bulk modulus. The spin resonance linewidth is also found to depend on pressure. This is explained by considering the pressure-dependent viscosity of the solvent, which modifies the effect of dipolar coupling between spins within fullerene clusters.