Redefining near-unity luminescence in quantum dots with photothermal threshold quantum yield

Superefficient light emission A challenge to improving synthesis methods for superefficient light-emitting semiconductor nanoparticles is that current analytical methods cannot measure efficiencies above 99%. Hanifi et al. used photothermal deflection spectroscopy to measure very small nonradiative decay components in quantum dot photoluminescence. The method allowed them to tune the synthesis of CdSe/CdS quantum dots so that the external luminescent efficiencies exceeded 99.5%. This is important for applications that require an absolute minimum amount of photon energy to be lost as heat, such as photovoltaic luminescent concentrators. Science, this issue p. 1199 CdSe/CdS nanoparticles have been synthesized with external luminescence efficiencies that exceed 99.5%. A variety of optical applications rely on the absorption and reemission of light. The quantum yield of this process often plays an essential role. When the quantum yield deviates from unity by significantly less than 1%, applications such as luminescent concentrators and optical refrigerators become possible. To evaluate such high performance, we develop a measurement technique for luminescence efficiency with sufficient accuracy below one part per thousand. Photothermal threshold quantum yield is based on the quantization of light to minimize overall measurement uncertainty. This technique is used to guide a procedure capable of making ensembles of near-unity emitting cadmium selenide/cadmium sulfide (CdSe/CdS) core-shell quantum dots. We obtain a photothermal threshold quantum yield luminescence efficiency of 99.6 ± 0.2%, indicating nearly complete suppression of nonradiative decay channels.