Efficient perovskite solar cells via improved carrier management.

Metal halide perovskite solar cells (PSCs) are an emerging photovoltaic technology with the potential to disrupt the mature silicon solar cell market. Great improvements in device performance over the past few years, thanks to the development of fabrication protocols1-3, chemical compositions4,5 and phase stabilization methods6-10, have made PSCs one of the most efficient and low-cost solution-processable photovoltaic technologies. However, the light-harvesting performance of these devices is still limited by excessive charge carrier recombination. Despite much effort, the performance of the best-performing PSCs is capped by relatively low fill factors and high open-circuit voltage deficits (the radiative open-circuit voltage limit minus the high open-circuit voltage)11. Improvements in charge carrier management, which is closely tied to the fill factor and the open-circuit voltage, thus provide a path towards increasing the device performance of PSCs, and reaching their theoretical efficiency limit12. Here we report a holistic approach to improving the performance of PSCs through enhanced charge carrier management. First, we develop an electron transport layer with an ideal film coverage, thickness and composition by tuning the chemical bath deposition of tin dioxide (SnO2). Second, we decouple the passivation strategy between the bulk and the interface, leading to improved properties, while minimizing the bandgap penalty. In forward bias, our devices exhibit an electroluminescence external quantum efficiency of up to 17.2 per cent and an electroluminescence energy conversion efficiency of up to 21.6 per cent. As solar cells, they achieve a certified power conversion efficiency of 25.2 per cent, corresponding to 80.5 per cent of the thermodynamic limit of its bandgap.

Homogenized halides and alkali cation segregation in alloyed organic-inorganic perovskites.

The role of the alkali metal cations in halide perovskite solar cells is not well understood. Using synchrotron-based nano-x-ray fluorescence and complementary measurements, we found that the halide distribution becomes homogenized upon addition of cesium iodide, either alone or with rubidium iodide, for substoichiometric, stoichiometric, and overstoichiometric preparations, where the lead halide is varied with respect to organic halide precursors. Halide homogenization coincides with long-lived charge carrier decays, spatially homogeneous carrier dynamics (as visualized by ultrafast microscopy), and improved photovoltaic device performance. We found that rubidium and potassium phase-segregate in highly concentrated clusters. Alkali metals are beneficial at low concentrations, where they homogenize the halide distribution, but at higher concentrations, they form recombination-active second-phase clusters.

Evolution of the Single-Nanocrystal Photoluminescence Linewidth with Size and Shell: Implications for Exciton-Phonon Coupling and the Optimization of Spectral Linewidths.

The optimization of photoluminescence spectral linewidths in semiconductor nanocrystal preparations involves minimizing both the homogeneous and inhomogeneous contributions to the ensemble spectrum. Although the inhomogeneous contribution can be controlled by eliminating interparticle inhomogeneities, far less is known about how to synthetically control the homogeneous, or single-nanocrystal, spectral linewidth. Here, we use solution photon-correlation Fourier spectroscopy (S-PCFS) to measure how the sample-averaged single-nanocrystal emission linewidth of CdSe core and core/shell nanocrystals change with systematic changes in the size of the cores and the thickness and composition of the shells. We find that the single-nanocrystal linewidth at room temperature is heavily influenced by the nature of the CdSe surface and the epitaxial shell, which have a profound impact on the internal electric fields that affect exciton-phonon coupling. Our results explain the wide variations, both experimental and theoretical, in the magnitude and size dependence in previous reports on exciton-phonon coupling in CdSe nanocrystals. Moreover, our findings offer a general pathway for achieving the narrow spectral linewidths required for many applications of nanocrystals.

Quantum dot light-emitting devices with electroluminescence tunable over the entire visible spectrum.

Improvements in quantum dot light-emitting device (QD-LED) performance are achieved by the choice of organic charge transporting layers, by use of different colloidal QDs for the different parts of the visible spectrum, and by utilizing a recently demonstrated robust QD deposition method. Spectrally narrow electroluminescence of our QD-LEDs is tuned over the entire visible wavelength range from lambda = 460 nm (blue) to lambda = 650 nm (deep red). By printing close-packed monolayers of different QD types inside an identical QD-LED structure, we demonstrate that different color QD-LEDs with QDs of different chemistry can be fabricated on the same substrate. We discuss mechanisms responsible for efficiency increase for green (4-fold) and orange (30%) QD-LEDs as compared to previous reports and outline challenges associated with achieving high-efficiency blue QD-LEDs.

Ternary I-III-VI quantum dots luminescent in the red to near-infrared.

We report the synthesis of a size series of copper indium selenide quantum dots (QDs) of various stoichiometries exhibiting photoluminescence (PL) from the red to near-infrared (NIR). The synthetic method is modular, and we have extended it to the synthesis of luminescent silver indium diselenide QDs. Previous reports on QDs luminescent in the NIR region have been primarily restricted to binary semiconductor systems, such as InAs, PbS, and CdTe. This work seeks to expand the availability of luminescent QD materials to ternary I-III-VI semiconductor systems.