Enhancing two-photon spontaneous emission in rare earths using graphene and graphene nanoribbons

The enhancement of two-photon spontaneous emission (2PSE) from trivalent and divalent rare earth ions in proximity to graphene and graphene nanoribbons is calculated for achievable experimental conditions using a combination of finite difference time domain simulations and direct computation of transition rates between energy levels in rare earths. For Er$^{3+}$, we find that the 2PSE rate is initially 8 orders lower than the single-photon spontaneous emission rate but that, with enhancement, 2PSE can reach 2.5% of the overall decay. When graphene nanoribbons are used, we also show that the emission of free-space photon pairs from Er$^{3+}$ at 3 - 3.2 $\mu$m via 2PSE can be increased by $\sim 400$. Our calculations show significantly less relative graphene-enhanced 2PSE than previous works, and we attribute this variation to differences in emitter size and assumed graphene mobility. We also show that the internal energy structure of the ion can have an impact on degree of 2PSE enhancement achievable and find that divalent rare earths are more favorable.
Comment: 10 pages, 5 figures. Supplement contains 14 pages and 13 included figures. To be submitted to Physical Review B