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The complete interpretation of small perturbation frequency‐domain measurements on perovskite solar cells has proven to be challenging. This is particularly true in the case of intensity‐modulated photocurrent/photovoltage spectroscopy (IMPS/IMVS) measurements in which the high frequency response is obscured by instrument limitations. Herein, a new experimental methodology capable of accurately resolving the high frequency response—often observable in the second and third quadrants of the complex plane—of a range of perovskite devices is demonstrated. By combining single‐frequency IMPS/IMVS measurements, it is able to construct the time dependence of the IMPS/IMVS response of these devices during their initial response to illumination. This reveals significant negative photocurrent/photovoltage signals at high frequency while devices reach steady state, which is in keeping with observations made from comparable time‐domain transient measurements. These techniques allow the underlying interfacial recombination and ion migration processes to be assessed, which are not always evident using steady‐state measurements. The ability to study and mitigate these processes is vital in optimizing the real‐world operation of devices. [ABSTRACT FROM AUTHOR]

Perovskite solar cells have emerged as a promising and highly efficient solar technology. Despite efficiencies continuing to climb, the prospect of industrial manufacture is in part hampered by concerns regarding the safety and sustainability of the solvents used in lab scale manufacture. In this paper, we aim to present a methodology for green solvent selection informed by EHS considerations from the CHEM-21 solvent guide for successful methylammonium lead triiodide (MAPbI3) precursor dissolution. Through the use of this methodology we present a N,N-dimethylformamide (DMF)-free alternative solvent system for deposition of MAPbI3 precursors (MAI and PbI2) consisting of dimethyl sulfoxide (DMSO), dimethylpropyleneurea (DMPU), 2-methyltetrahydrofuran (2-MeTHF) and ethanol (EtOH). We have investigated 3 candidate solutions with slightly different compositions of these four solvents, all of which produce dense, uniform and pinhole-free perovskite films via spin coating. All three candidate solutions (A–C) match the average device efficiencies of the DMF/DMSO control devices (12.4%) with candidate A, which consists of 40% DMSO, 30% DMPU, 20% 2-MeTHF and 10% EtOH (vol%), producing a champion PCE of 16.1% compared to 16.2% for DMF/DMSO (80/20 vol%). Perovskite films cast from the three candidate solutions show improved crystallinity, higher fluorescence emission, and improved crystal size uniformity than those cast from DMF/DMSO. This work aims to: highlight the key solvent parameters which determine effective MAPbI3 precursor dissolution; provide a set of criteria for appropriate alternative solvent selection; and demonstrate the application of green chemistry principles to solvent selection for perovskite photovoltaic manufacturing. [ABSTRACT FROM AUTHOR]

Perovskite solar cells (PSCs) have already achieved comparable performance to industrially established silicon technologies. However, high performance and stability must be also be achieved at large area and low cost to be truly commercially viable. The fully printable triple-mesoscopic carbon perovskite solar cell (mCPSC) has demonstrated unprecedented stability and can be produced at low capital cost with inexpensive materials. These devices are inherently scalable, and large-area modules have already been fabricated using low-cost screen printing. As a uniquely stable, scalable and low-cost architecture, mCPSC research has advanced significantly in recent years. This review provides a detailed overview of advancements in the materials and processing of each individual stack layer as well as in-depth coverage of work on perovskite formulations, with the view of highlighting potential areas for future research. Long term stability studies will also be discussed, to emphasise the impressive achievements of mCPSCs for both indoor and outdoor applications. [ABSTRACT FROM AUTHOR]

Mesoporous carbon stack architecture is attracting considerable interest as a candidate for scalable, low‐cost perovskite solar cells amenable to high‐throughput manufacturing. These cells are characterized by microns‐thick mesoporous titania and zirconia layers capped by a nonselective carbon electrode with the whole stack being infused with a perovskite semiconductor. Although the architecture does not deliver the >20% power conversion efficiencies characteristic of perovskite planar and mesoporous geometries, it does produce cells with respectable efficiencies >16%, which is unexpected due to the carbon electrode being a nonideal anode and the active layers being so thick. Optimization of these cells requires an understanding of the coupled efficiencies of light absorption, charge generation, and extraction which is currently unavailable. Herein, a combined experimental‐simulation study that elucidates photogeneration and extraction is reported. By determining the optical constants of the individual components and using effective‐medium approximations, the internal quantum efficiencies (IQE) in both the titania and zirconia layers are determined to be ≈85%. Numerical drift‐diffusion simulations indicate that this high IQE is a consequence of the thick junctions reducing minority carrier concentrations at the electrodes, thereby decreasing surface recombination. This insight can now be used to tune the carbon stack for efficiency and simplicity. [ABSTRACT FROM AUTHOR]

A combination of high‐resolution mapping techniques is developed to probe the homogeneity and defects of mesoscopic perovskite solar cells. Three types of cells using a one‐step infiltration process with methylammonium lead iodide (MAPbI3) or 5‐ammoniumvaleric acid‐MAPbI3 solutions, or two‐step process with MAPbI3 solution are investigated. The correlation between photoluminescence, photocurrent, electroluminescence, and Raman maps gives a detailed understanding of the different infiltration mechanisms, electronic contact at interfaces, and effect on local photocurrent for the cells. The one‐step MAPbI3 cell has very limited infiltration of the perovskite solution which results in poor device performance. High loading of the mesopores of the TiO2 and ZrO2 scaffold is observed when using 5‐ammoniumvaleric acid, but some micrometer‐sized non‐infiltrated areas remain due to dense carbon flakes hindering perovskite infiltration. The two‐step cell has a complex morphology with features having either beneficial or detrimental effects on the local photocurrent. The results not only provide key insights to achieving better infiltration and homogeneity of the perovskite film in mesoporous devices but can also aid further work on planar devices to develop efficient extraction layers. Moreover, this multi‐mapping approach allows the correlation of the local photophysical properties of full perovskite devices, which would be challenging to obtain by other techniques. [ABSTRACT FROM AUTHOR]