Two-photon upconversion affected by intermolecule correlations near metallic nanostructures

Abstract

We investigate an efficient two-photon up-conversion process in more than one molecule coupled to an optical antenna. In the previous work [Y. Osaka et al., PRL 112, 133601 (2014)], we considered the two-photon up-conversion process in a single molecule within one-dimensional inputoutput theory, and revealed that controlling the antenna-molecule coupling enables the efficient up-conversion with radiative loss in the antenna suppressed. In this work, 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 up-conversion probability because they equally share the energy of the two photons. However, it is shown that we can overcome the difficulty by controlling the inter-molecule coupling. Our result implies that, without increasing the incident photon number (light power), we can enlarge the net probability of the two-photon up-conversion.

Weak-Light Nonlinearity Using a Dark State in Coupled Quantum Dots

“…37,38) Although the strong dissipation in the metal can be a serious bottleneck for weaklight nonlinearity, 39,40) it is known that the quantum interference between the plasmon and target provides a positive insight into the solutions. [41][42][43][44][45] When the typical size of the metallic structures is much smaller than the light wavelength, they exhibit the saturations in the optical absorption and emission, which can be qualitatively explained within the twolevel plasmon model. [46][47][48][49][50] Thus, we employ the Hamiltonian for the plasmons as…”