Metal halide perovskites of the general formula ABX 3 -where A is a monovalent cation such as caesium, methylammonium or formamidinium; B is divalent lead, tin or germanium; and X is a halide anion-have shown great potential as light harvesters for thin-film photovoltaics [1][2][3][4][5] . Among a large number of compositions investigated, the cubic α-phase of formamidinium lead triiodide (FAPbI 3 ) has emerged as the most promising semiconductor for highly efficient and stable perovskite solar cells [6][7][8][9] , and maximizing the performance of this material in such devices is of vital importance for the perovskite research community. Here we introduce an anion engineering concept that uses the pseudo-halide anion formate (HCOO − ) to suppress anion-vacancy defects that are present at grain boundaries and at the surface of the perovskite films and to augment the crystallinity of the films. The resulting solar cell devices attain a power conversion efficiency of 25.6 per cent (certified 25.2 per cent), have long-term operational stability (450 hours) and show intense electroluminescence with external quantum efficiencies of more than 10 per cent. Our findings provide a direct route to eliminate the most abundant and deleterious lattice defects present in metal halide perovskites, providing a facile access to solution-processable films with improved optoelectronic performance.Perovskite solar cells (PSCs) have attracted much attention since their first demonstration in 2009 [1][2][3][4][5] . The rapid expansion of research into PSCs has been driven by their low-cost solution processing and attractive optoelectronic properties, including a tunable bandgap 6 , high absorption coefficient 10 , low recombination rate 11 and high mobility of charge carriers 12 . Within a decade, the power conversion efficiency (PCE) of single-junction PSCs progressed from 3% to a certified value of 25.5% 13 , the highest value obtained for thin-film photovoltaics. Moreover, through the use of additive and interface engineering strategies, the long-term operational stability of PSCs now exceeds 1,000 hours in full sunlight 14,15 . PSCs therefore show great promise for deployment as the next generation of photovoltaics.Compositional engineering plays a key part in achieving highly efficient and stable PSCs. In particular, mixtures of methylammonium lead triiodide (MAPbI 3 ) with formamidinium lead triiodide (FAPbI 3 ) have been extensively studied 5,7 . Compared to MAPbI 3 , FAPbI 3 is thermally more stable and has a bandgap closer to the Shockley-Queisser limit 6 , rendering FAPbI 3 the most attractive perovskite layer for single-junction PSCs.Unfortunately, thin FAPbI 3 films undergo a phase transition from the black α-phase to a photoinactive yellow δ-phase below a temperature of 150 °C. Previous approaches to overcome this problem have included mixing FAPbI 3 with a combination of methylammonium (MA + ), caesium (Cs + ) and bromide (Br − ) ions; however, this comes at the cost of blue-shifted absorbance and phase segregation under...
Kim and co-workers report systematical studies with methylammonium chloride (MACl) in formamidinium lead iodide (FAPbI 3 )-based perovskite thin films. The MACl addition could induce the intermediate phase with pure a-phase without annealing, effectively stabilizing the structure, only through cationic site substitution. The film quality can be significantly improved, exhibiting a 63 increase in grain size, a 33 increase in phase crystallinity, and a 4.33 increase in photoluminescence lifetime. The resulting optimized solar cells achieved a peakscan efficiency of above 24%.
The optoelectronic tunability offered by colloidal quantum dots (CQDs) is attractive for photovoltaic applications but demands proper band alignment at electrodes for efficient charge extraction at minimal cost to voltage. With this goal in mind, self-assembled monolayers (SAMs) can be used to modify interface energy levels locally. However, to be effective SAMs must be made robust to treatment using the various solvents and ligands required for to fabricate high quality CQD solids. We report robust self-assembled monolayers (R-SAMs) that enable us to increase the efficiency of CQD photovoltaics. Only by developing a process for secure anchoring of aromatic SAMs, aided by deposition of the SAMs in a water-free deposition environment, were we able to provide an interface modification that was robust against the ensuing chemical treatments needed in the fabrication of CQD solids. The energy alignment at the rectifying interface was tailored by tuning the R-SAM for optimal alignment relative to the CQD quantum-confined electron energy levels. This resulted in a CQD PV record power conversion efficiency (PCE) of 10.7% with enhanced reproducibility relative to controls.
Ultralight and flexible perovskite solar cells with the orthogonal AgNW electrodes exhibit an excellent power-per-weight of 29.4 W g−1.
Edged-selectively fluorine (F) functionalized graphene nanoplatelets (EFGnPs-F) with a p-i-n structure of perovskite solar cells achieved 82% stability relative to initial performance over 30 days of air exposure without encapsulation. The enhanced stability stems from F-substitution on EFGnPs; fluorocarbons such as polytetrafluoroethylene are well-known for their superhydrophobic properties and being impervious to chemical degradation. These hydrophobic moieties tightly protect perovskite layers from air degradation. To directly compare the effect of similar hydrophilic graphene layers, edge-selectively hydrogen functionalized graphene nanoplatelet (EFGnPs-H) treated devices were tested under the same conditions. Like the pristine MAPbI perovskite devices, EFGnPs-H treated devices were completely degraded after 10 days. The hydrophobic properties of EFGnPs-F were characterized by contact angle measurement. The test results showed great water repellency compared to pristine perovskite films or EFGnPs-H coated films. This resulted in highly air-stable p-i-n perovskite solar cells.
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