Efficient two-photon excitation by photonic dimers

In this Letter, we show that photonic dimers, the quantum mechanical bound states of two photons, enable efficient nonlinear two-photon excitation, primarily due to the Lorentzian energy anti-correlation and to the temporal proximity between the constituent photons. We analytically and numerically demonstrate the order-of-magnitude improvement of the excitation efficiency per photon by the photonic dimers over the ultrashort pulses from a laser. We further show that, owing to the high excitation efficiency, the two-photon transition rate by photonic dimers deviates from the well-known linear intensity dependence at low intensities. Possible approaches for generating the photonic dimers in semiconductor platforms are also investigated.