Optically inactive or dark excitons play an important role in exciton and polariton devices. On one hand, they supply excitons to the light cone and feed the photoluminescence signal. On the other hand, they repel radiatively active excitons due to the exchange interaction and contribute to the formation of lateral potentials for exciton and polariton condensates. On top of this, they play an important role in scattering and energy relaxation dynamics of quasiparticles in semiconductors. So far, because of optical inaccessibility, studies were focused typically on one experimental technique, giving information about one quantity of dark excitons. Here we present a comprehensive study of the dark exciton reservoir in a high-quality 14-nm GaAs/AlGaAs quantum well using several experimental techniques. We develop a new method of nonradiative broadening spectroscopy of exciton resonances and combine it with nondegenerate pump-probe spectroscopy. The exciton and carrier dynamics in the reservoir is monitored via dynamic broadening of exciton resonances induced by exciton-exciton and exciton-carrier scattering. The dynamics is found to be strongly dependent on the optical excitation conditions. Based on the experimental results, we develop a model of dynamics in a reservoir of excitons and free carriers. The model allows us to describe the experimentally measured photoluminescence kinetics with no fitting parameters. We also demonstrate the optical control of the dark exciton density by means of an additional excitation that creates imbalance of free carriers depleting the reservoir. These results shed light onto the dynamics of the excitonic “dark matter” and pave the way to the high-precision engineering of optically induced potentials in exciton-polariton and integrated photonic devices. We expect that the observed results can be transferred also to other semiconductors so that the current quantum well serves as a high-quality model system.

• Received 21 April 2021
• Revised 15 June 2021
• Accepted 17 June 2021

DOI:https://doi.org/10.1103/PhysRevB.104.035414