Three-photon excitation of quantum two-level systems

We demonstrate experimentally the long-standing fundamental theoretical prediction that quantum two-level systems can only be efficiently resonantly excited via multi-photon pulses involving an odd number of photons. This prediction can be seen directly from time-dependent Floquet theory that also allows us to quantify the strength of the multi-photon processes. For the experimental demonstration, we perform spectroscopy measurements on a single InGaN quantum dot with a variety of laser detunings, and observe that the system can be excited in a resonant three-photon process, whilst resonant two-photon excitation is entirely suppressed. Finally, we exploit this technique to probe intrinsic properties of InGaN quantum dots. In contrast to non-resonant excitation, slow relaxation of charge carriers is avoided which allows us to measure directly the radiative lifetime of the lowest energy exciton states. Since the emission energy is detuned far from the resonant driving laser field, polarization filtering is not required and emission with a greater degree of linear polarization is observed compared to non-resonant excitation.