Two advances that address the main challenges of all-perovskite two-terminal tandem solar cell fabrication are reported. First, a nucleation layer is used to enable high-quality atomic layer deposition-based recombination layers that reduce electronic losses. Second, cation tuning is used for wide-band-gap perovskite solar cells that produce high, stable voltages. Combining these advances allows us to fabricate tandem perovskite solar cells on both rigid and flexible plastic substrates that have high efficiency and promising stability.

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We present a cation-exchange approach for tunable A-site alloys of cesium (Cs+) and formamidinium (FA+) lead triiodide perovskite nanocrystals that enables the formation of compositions spanning the complete range of Cs1–x FA x PbI3, unlike thin-film alloys or the direct synthesis of alloyed perovskite nanocrystals. These materials show bright and finely tunable emission in the red and near-infrared range between 650 and 800 nm. The activation energy for the miscibility between Cs+ and FA+ is measured (∼0.65 eV) and is shown to be higher than reported for X-site exchange in lead halide perovskites. We use these alloyed colloidal perovskite quantum dots to fabricate photovoltaic devices. In addition to the expanded compositional range for Cs1–x FA x PbI3 materials, the quantum dot solar cells exhibit high open-circuit voltage (V OC) with a lower loss than the thin-film perovskite devices of similar compositions.

Go big or go home'' could never be a truer statement, especially when it comes to energy. The world population is increasing, the energy use per person is growing more rapidly, and the total electricity use per person is growing even more quickly than that. To handle this demand, energy production must be increased, and it is critical for renewable sources to be used. Currently three quarters of a terawatt of power generated from photovoltaics (PVs) has been installed. At a somewhat optimistic average power-conversion efficiency of 18%, the distributed surface area of high purity optoelectronic grade semiconductor photovoltaic panels pointed at the sun is substantially larger than the area of the whole state of Rhode Island or nearly double the land mass of Luxembourg. While photovoltaic production continues to ramp to immense proportions, perovskite semiconductors are poised to greatly complement existing technology. On the other end of the size spectrum, the study of semiconductor nanocrystals or quantum dots (QDs) has led to advanced structures and deeper understanding within halide perovskite semiconductors. In this article, we show how the development of nanoscale metal halide perovskite semiconductors have gained prominence surpassing all other QD materials in terms of efficiency, and are becoming a platform for further improving technology to solve big energy challenges.

Colloidal metal halide perovskite nanocrystals (NCs) with chiral ligands are outstanding candidates as a circularly polarized luminescence (CPL) light source due to many advantages such as high photoluminescence quantum efficiency, large spin–orbit coupling, and extensive tunability via composition and choice of organic ligands. However, achieving pronounced and controllable polarized light emission remains challenging. Here, we develop strategies to achieve high CPL responses from colloidal formamidinium lead bromide (FAPbBr3) NCs at room temperature using chiral surface ligands. First, we show that replacing a portion of typical ligands (oleylamine) with short chiral ligands ((R)-2-octylamine) during FAPbBr3 NC synthesis results in small and monodisperse NCs that yield high CPL with average luminescence dissymmetry g-factor, g lum = 6.8 × 10–2. To the best of our knowledge, this is the highest among reported perovskite materials at room temperature to date and represents around 10-fold improvement over the previously reported colloidal CsPbCl x Br y I3‑x‑y NCs. In order to incorporate NCs into any optoelectronic or spintronic application, the NCs necessitate purification, which removes a substantial amount of the chiral ligands and extinguishes the CPL signals. To circumvent this issue, we also developed a postsynthetic ligand treatment using a different chiral ligand, (R-/S-)­methylbenzylammonium bromide, which also induces a CPL with an average g lum = ±1.18 × 10–2. This postsynthetic method is also amenable for long-range charge transport since methylbenzylammonium is quite compact in relation to other surface ligands. Our demonstrations of high CPL and g lum from both as-synthesized and purified perovskite NCs at room temperature suggest a route to demonstrate colloidal NC-based spintronics.