A significant fraction of global electricity demand is for lighting. Enabled by the realization and development of efficient GaN blue light-emitting diodes (LEDs), phosphor-based solid-state white LEDs provide a much higher efficiency alternative to incandescent and fluorescent lighting, which are being broadly implemented. However, a key challenge for this industry is to achieve the right photometric ranges and application-specific emission spectra via cost-effective means. Here, we synthesize organic–inorganic lead halide-based perovskite crystals with broad spectral tuneability. By tailoring the composition of methyl and octlyammonium cations in the colloidal synthesis, meso- to nanoscale 3D crystals (5–50 nm) can be formed with enhanced photoluminescence efficiency. By increasing the octlyammonium cations content, we observe platelet formation of 2D layered perovskite sheets; however, these platelets appear to be less emissive than the 3D crystals. We further manipulate the halide composition of the perovskite crystals to achieve emission covering the entire visible spectrum. By blending perovskite crystals with different emission wavelengths in a polymer host, we demonstrate the potential to replace conventional phosphors and provide the means to replicate natural white light when excited by a blue GaN LED.

We demonstrate a method for controlled p-doping of the halide perovskite surface using molecular dopants, resulting in reduced non-radiative recombination losses and improved device performance.

Metal halide perovskite solar cells have now reached efficiencies of over 22%. To date, the most efficient perovskite solar cells have the n-i-p device architecture and use 2,2′,7,7′-tetrakis­(N,N′-di-p-methoxyphenylamine)-9,9′-spirobifluorene or poly­(triarylamine) as the hole transport material (HTM), which are typically doped with lithium bis­((trifluomethyl)­sulfonyl)­amide (Li-TFSI). Li-TFSI is hygroscopic and detrimental to the long-term performance of the solar cells, limiting its practical use. In this work, we successfully replace Li-TFSI by molybdenum tris­(1-(methoxycarbonyl)-2-(trifluoromethyl)­ethane-1,2-dithiolene), Mo­(tfd-CO2Me)3, or molybdenum tris­(1-(trifluoroacetyl)-2-(trifluoromethyl)­ethane-1,2-dithiolene), Mo­(tfd-COCF3)3. With these two dopants, we achieve stabilized power conversion efficiencies up to 16.7% and 15.7% with average efficiencies of 14.8% ± 1.1% and 14.4% ± 1.2%, respectively. Moreover, we observe a significant enhancement of the long-term stability of perovskite solar cells under 85 °C thermal stressing in air.

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