Two-photon upconversion affected by intermolecule correlations near metallic nanostructures

We investigate an efficient two-photon upconversion process in more than one molecule coupled to an optical antenna. In the previous paper [Y. Osaka et al., Phys. Rev. Lett. 112, 133601 (2014)], we considered the two-photon upconversion process in a single molecule within one-dimensional input-output theory and revealed that controlling the antenna-molecule coupling enables the efficient upconversion with radiative loss in the antenna suppressed. In this paper, aiming to propose a way to enhance the total probability of antenna-photon scattering, we extend the model to the case of multiple molecules. In general, the presence of more than one molecule decreases the upconversion probability because they equally share the energy of the two photons. However, it is shown that we can overcome the difficulty by controlling the intermolecule coupling. Our result implies that, without increasing the incident photon number (light power), we can enlarge the net probability of the two-photon upconversion.