Nanocrystal (NC) luminescent solar concentrators (LSCs) represent a promising clean-energy technology capable of concentrating direct and diffuse light to reduce the area of photovoltaic (PV) cells – which are energetically costly to manufacture – required to meet energy demands. We have been developing Yb3+-doped CsPbX3 (X = Cl, Br) perovskite NCs that efficiently convert single high-energy photons into pairs of low-energy photons, generating photoluminescence quantum yields approaching 200%. This process – known as quantum cutting – can improve LSC efficiencies by converting poorly used blue photons into near-infrared photons that are absorbed perfectly by silicon solar cells. These findings led to invention of a fundamentally new and simple monolithic bilayer LSC device structure that capitalizes on the unique properties of quantum-cutting Yb3+-doped CsPbX3 NCs.