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Engineering perovskite precursor ink to widen the processing window is crucial to obtaining uniform, compact, and pinhole-free perovskite films at scale using industrially relevant solution coating techniques. Here, we introduce a ternary solvent system and systematically investigate the impacts of coordinating solvents, N -methyl-2-pyrrolidone (NMP) and N , N '-dimethylpropyleneurea (DMPU), on the physical properties of the slot-die-coated perovskite films and on the corresponding device performance. Tailoring NMP and DMPU concentrations in the precursor ink allows us to control the perovskite intermediate phase formation and widen the processing window, enabling the reproducible production of perovskite films with high photoelectrical quality at scale. Using the optimized precursor ink, we demonstrate slot-die-coated perovskite minimodules with power conversion efficiencies of 19 and 16% on 56 and 100 cm 2 substrates, respectively.

Light-induced performance changes in metal halide perovskite solar cells (PSCs) have been studied intensively over the last decade, but little is known about the variation in microscopic optoelectronic properties of the perovskite heterojunctions in a completed device during operation. Here, we combine Kelvin probe force microscopy and transient reflection spectroscopy techniques to spatially resolve the evolution of junction properties during the operation of metal-halide PSCs and study the light-soaking effect. Our analysis showed a rise of an electric field at the hole-transport layer side, convoluted with a more reduced interfacial recombination rate at the electron-transport layer side in the PSCs with an n-i-p structure. The junction evolution is attributed to the effects of ion migration and self-poling by built-in voltage. Device performances are correlated with the changes of electrostatic potential distribution and interfacial carrier dynamics. Our results demonstrate a new route for studying the complex operation mechanism in PSCs.

The structural and optical properties of hybrid organic-inorganic metal halide perovskite solar cells are measured by spectroscopic ellipsometry to reveal an optically distinct interfacial layer among the back contact metal, charge transport, and absorber layers. Understanding how this interfacial layer impacts performance is essential for developing higher performing solar cells. This interfacial layer is modeled by Bruggeman effective medium approximations (EMAs) to contain perovskite, C 60 , BCP, and metal. External quantum efficiency (EQE) simulations that consider scattering, electronic losses, and the formation of nonparallel interfaces are created with input derived from ellipsometry structural-optical models and compared with experimental EQE to estimate optical losses. This nonplanar interface causes optical losses in short circuit current density ( J SC ) of up to 1.2 mA cm -2 . A study of glass/C 60 /SnO 2 /Ag or Cu and glass/C 60 /BCP/Ag film stacks shows that C 60 and BCP mix, but replacing BCP with SnO 2 can prevent mixing between the ETLs to prevent contact between C 60 and back contact metal and enable the formation of a planar interface between ETLs and back contact metals.

The Urbach energy indicating the width of the exponentially decaying sub-bandgap absorption tail is commonly used as the indicator of electronic quality of thin-film materials used as absorbers in solar cells. Urbach energies of hybrid inorganic-organic metal halide perovskites with various anion-cation compositions are measured by photothermal deflection spectroscopy. The variation in anion-cation composition has a substantial effect on the measured Urbach energy and hence the electronic quality of the perovskite. Depending upon the compositions, the Urbach energy varies from 18 to 65 meV for perovskite films with similar bandgap energies. For most of the perovskite compositions studied here including methylammonium (MA) + formamidinium (FA)-based Pb iodides, mixed Sn + Pb narrow-bandgap perovskites with low or intermediate Sn contents, and wide-bandgap FA + Cs- and I + Br-based perovskites, the correlation between the Urbach energy of the perovskite thin film and open-circuit voltage ( V OC ) deficit for corresponding solar cells shows a direct relationship with reduction of the Urbach energy occurring with a beneficial decrease in the V OC deficit. However, due to issues related to material quality, impurity phases and stability in laboratory ambient air, and unoptimized film processing techniques, the solar cells incorporating Cs-based inorganic and mixed Sn + Pb perovskites with a higher than optimum Sn content show a higher V OC deficit even though the corresponding films show a lower Urbach energy.

Copper (Cu) incorporation is a key process for fabricating efficient CdTe-based thin-film solar cells and has been used in CdTe-based solar cell module manufacturing. Here, we investigate the effects of different Cu precursors on the performance of CdTe-based thin-film solar cells by incorporating Cu using a metallic Cu source (evaporated Cu) and ionic Cu sources (solution-processed cuprous chloride (CuCl) and copper chloride (CuCl 2 )). We find that ionic Cu precursors offer much better control in Cu diffusion than the metallic Cu precursor, producing better front junction quality, lower back-barrier heights, and better bulk defect property. Finally, outperforming power conversion efficiencies of 17.2 and 17.5% are obtained for devices with cadmium sulfide and zinc magnesium oxide as the front window layers, respectively, which are among the highest reported CdTe solar cells efficiencies. Our results suggest that an ionic Cu precursor is preferred as the dopant to fabricate efficient CdTe thin-film solar cells and modules.

Hierarchical TS-1 has attracted enormous attention from both academia and industry due to its remarkable catalytic performance in epoxidation reactions. However, sustainable synthesis of hierarchical-nanosized TS-1 without mesoporogens is still challenging. In this work, we report a facile and mesoporogen-free strategy to simultaneously manipulate pore structure and particle size of TS-1 employing the concentrated system. Taking advantage of the suspended nuclei in the concentrated system as confirmed by the DLS-PSD and atomic force microscopy, the novel TS-1 is demonstrated to have higher Ti concentration on surface, higher surface area (539 m 2 /g), abundant mesopores, and reduced crystal size (ca. 150 nm). Moreover, this Au-Ti bifunctional catalyst shows a good PO formation rate with enhanced catalytic stability due to the hierarchical structure. This strategy opens a novel way for the green synthesis of hierarchical-nanosized TS-1 and facilitates industrial development of the Au/TS-1 catalyst for propene epoxidation.

Perovskite solar cell device performance is affected by optical and electronic losses. To minimize these losses in solar cells, it is important to identify their sources. Here, we report the optical and electronic losses arising from physically mixed interfacial layers between the adjacent component materials in highly efficient two terminal (2T) all-perovskite tandem, single-junction wide-bandgap, and single-junction narrow-bandgap perovskite-based solar cells. Physically mixed interfacial layers as the sources of optical and electronic losses are identified from spectroscopic ellipsometry measurements and data analysis followed by comparisons of simulated and measured external quantum efficiency spectra. Parasitic absorbance in the physically mixed regions between silver metal electrical contacts and electron transport layers (ETLs) near the back contact and a physical mixture of commercial indium tin oxide and hole transport layers (HTL) near the front electrical contact lead to substantial optical loss. A lower-density void + perovskite nucleation layer formed during perovskite deposition at the interface between the perovskite absorber layer and the HTL causes electronic losses because of incomplete collection of photogenerated carriers likely originating from poor coverage and passivation of the initially nucleating grains.

The two-step solution-based process has demonstrated substantial success in fabricating high-efficiency perovskite solar cells in recent years. Despite the high performance, the underlying mechanisms that govern the formation of perovskite films and corresponding device performance are yet to be fully understood. Particularly, organic cation composition used in the two-step solution processing of mixed-cation lead halide perovskite solar cells plays a critical role in the perovskite film formation and the resultant device performance. However, little is understood about the impacts of organic cation composition on the current density-voltage ( J - V ) hysteretic behavior and stability of perovskite solar cells. To address this need, here, we study the effect of mixed organic cations, that is, the fraction of formamidinium (FA) and methylammonium (MA) contents, used for the two-step solution-processed perovskite thin films on solar cell performance, including efficiency, J - V hysteresis, and stability. In addition to the efficiency variations, we find that perovskite solar cells based on FA-rich and MA-rich stoichiometries show distinct characteristics in J - V hysteresis and stability. The origins of such a discrepancy are attributed to the thermodynamically driven conversion from lead iodide to perovskites, which is determined by the combination of organic cations. The perovskite solar cells based on the mixed cation FA 0.6 MA 0.4 PbI 3 composition show a champion power conversion efficiency of over 21% and robust stability (retaining more than 90% of initial efficiency) under maximum power-point tracking in dry nitrogen for more than 500 h. Our work provides insights on understanding the formation of perovskite films in the two-step process, which may benefit further investigation on perovskite solar cells.

Recently, halide perovskites have upstaged decades of solar cell development by reaching power conversion efficiencies that surpass the performance of polycrystalline silicon. The efficiency improvement in the perovskite cells is related to repeated recycling between photons and electron-hole pairs, reduced recombination losses, and increased carrier lifetimes. Here, we demonstrate a novel approach toward augmenting the perovskite solar cell efficiency by invoking the Förster Resonance Energy Transfer (FRET) mechanism. FRET occurs in the near-field region as the bacteriorhodopsin (bR) protein, and perovskite has similar optical gaps. Titanium dioxide functionalized with the bR protein is shown to accelerate the electron injection from excitons produced in the perovskite layer. FRET predicts the strength of long-range excitonic transport between the perovskite and bR layers. Solar cells incorporating TiO 2 /bR layers are found to exhibit much higher photovoltaic performance as compared to baseline cells without bR. These results open the opportunity to develop a new class of bioperovskite solar cells with improved performance and stability.

Control over grain size and crystallinity is important for preparation of methylammonium lead iodide (MAPbI 3 ) solar cells. We explore the effects of using small concentrations of Cd 2+ and unusually high concentrations of methylammonium iodide during the growth of MAPbI 3 in the two-step solution process. In addition to improved crystallinity and an enhancement in the size of the grains, time-resolved photoluminescence measurements indicated a dramatic increase in the carrier lifetime. As a result, devices constructed with the Cd-modified perovskites showed nearly a factor of 2 improvement in the power conversion efficiency (PCE) relative to similar devices prepared without Cd addition. The grains also showed a higher degree of orientation in the ⟨110⟩ direction, indicating a change in the growth mechanism, and the films were compact and smooth. We propose a Cd-modified film growth mechanism that invokes a critical role for low-dimensional Cd perovskites to explain the experimental observations.