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Abstract:

Perovskite solar cells (PSCs) comprise a solid perovskite absorber sandwiched between several layers of different charge-selective materials, ensuring unidirectional current flow and high voltage output of the devices. A ‘buffer material’ between the electron-selective layer and the metal electrode in p-type/intrinsic/n-type (p-i-n) PSCs (also known as inverted PSCs) enables electrons to flow from the electron-selective layer to the electrode. Furthermore, it acts as a barrier inhibiting the inter-diffusion of harmful species into or degradation products out of the perovskite absorber. Thus far, evaporable organic molecules and atomic-layer-deposited metal oxides have been successful, but each has specific imperfections. Here we report a chemically stable and multifunctional buffer material, ytterbium oxide (YbOx), for p-i-n PSCs by scalable thermal evaporation deposition. We used this YbOx buffer in the p-i-n PSCs with a narrow-bandgap perovskite absorber, yielding a certified power conversion efficiency of more than 25%. We also demonstrate the broad applicability of YbOx in enabling highly efficient PSCs from various types of perovskite absorber layer, delivering state-of-the-art efficiencies of 20.1% for the wide-bandgap perovskite absorber and 22.1% for the mid-bandgap perovskite absorber, respectively. Moreover, when subjected to ISOS-L-3 accelerated ageing, encapsulated devices with YbOx exhibit markedly enhanced device stability.

Abstract:

The use of a small organic molecular passivator is proven to be a successful strategy for producing higher-performing quasi-2D perovskite light-emitting diodes (PeLEDs). The small organic molecule can passivate defects on the grain surround and surface of perovskite crystal structures, preventing nonradiative recombination and charge trapping. In this study, a new small organic additive called 2, 8-dibromodibenzofuran (diBDF) is reported and examines its effectiveness as a passivating agent in high-performance green quasi-2D PeLEDs. The oxygen atom in diBDF, acting as a Lewis base, forms coordination bonds with uncoordinated Pb²⁺, so enhancing the performance of the device. In addition, the inclusion of diBDF in the quasi-2D perovskite results in a decrease in the abundance of low-n phases, hence facilitating efficient carrier mobility. Consequently, PeLED devices with high efficiency are successfully produced, exhibiting an external quantum efficiency of 19.9% at the emission wavelength of 517 nm and a peak current efficiency of 65.0 cd A-¹.

Abstract:

Mixed lead-tin (Pb:Sn) halide perovskites are promising absorbers withnarrow-bandgaps (1.25–1.4 eV) suitable for high-efficiency all-perovskitetandem solar cells. However, solution processing of optimally thick Pb:Snperovskite films is notoriously difficult in comparison with their neat-Pbcounterparts. This is partly due to the rapid crystallization of Sn-basedperovskites, resulting in films that have a high degree of roughness. Rougherfilms are harder to coat conformally with subsequent layers usingsolution-based processing techniques leading to contact between theabsorber and the top metal electrode in completed devices, resulting in a lossof VOC , fill factor, efficiency, and stability. Herein, this study employs anon-continuous layer of alumina nanoparticles distributed on the surface ofrough Pb:Sn perovskite films. Using this approach, the conformality of thesubsequent electron-transport layer, which is only tens of nanometres inthickness is improved. The overall maximum-power-point-tracked efficiencyimproves by 65% and the steady-state VOC improves by 28%. Application ofthe alumina nanoparticles as an interfacial buffer layer also results in highlyreproducible Pb:Sn solar cell devices while simultaneously improving devicestability at 65 °C under full spectrum simulated solar irradiance. Aged devicesshow a six-fold improvement in stability over pristine Pb:Sn devices,increasing their lifetime to 120 h

Abstract:

Here we deposit the data and code necessary to generate the analysis found in our work. We have included: Simulation output from drift diffusion simulations; Photoluminescence imaging data (in a semi-raw and processed format); Outputs from our Bayesian analysis combining the two; and a clone of the code (from our public git repo) used to generate the analysis.

Abstract:

The ability to characterise perovskite phases non-destructively is key on the route to ensuring their long-term stability in operando. Raman spectroscopy holds the promise to play an important role in this task. Among all perovskites, formamidinium lead iodide (FAPbI3) has emerged as one of the most promising candidates for single-junction photovoltaic cells. However, Raman spectroscopy of FAPbI3 remains challenging as is evidenced by conflicting reports in the literature. Here, we demonstrate that due to the vulnerability of FAPbI3 to laser-induced degradation, the detected Raman spectrum depends strongly on the experimental conditions. This can lead to conflicting results and is revealed as the origin of discrepancies in the literature. We overcome this issue by deploying defocused Raman spectroscopy, preventing laser-induced damage to the sample and simultaneously improving the signal-to-noise ratio, allowing us to furthermore resolve much weaker Raman modes than was previously possible. We offer step-by-step instructions on how to apply this technique to a given spectrometer. Non-destructive characterisation of the FAPbI3 phases further enables us to quantify the phase stability of pristine FAPbI3 crystals and FAPbI3 grown with the high-performance additive methylenediammonium chloride (MDACl2). This shows that the neat crystals fully degrade within two weeks, whereas in samples grown with the additive only about 2% of the crystal bulk is in the δ-phase after 400 days. This establishes defocused Raman spectroscopy as a powerful tool for the characterisation of FAPbI3 and other perovskite materials.