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Organic–inorganic hybrid halide perovskite solar cells are promising for next-generation thin-film solar cells, demonstrating power conversion efficiency exceeding 25%. In particular, single-crystal perovskite materials are estimated to possess superior optoelectronic properties that can further enhance the efficiency. However, fabricating thin single-crystal perovskite for a light-absorber layer remains challenging. In this study, a 40-µm-thick single-crystalline MAPbBr3 perovskite is fabricated by inverse temperature crystallization (ITC) with a selective seed-transfer technique. By using a separate seed growth process and a seed-transfer process, a 16.23-mm2-large single domain high-quality single-crystalline MAPbBr3 perovskite can be grown without additional nucleation. The grown single-crystal MAPbBr3 exhibits a low surface roughness of 0.51 nm and low trap density of 7.61 × 108 cm−3. We also fabricate solar cells with single-crystalline MAPbBr3 using a glass substrate coated with SnO2 and indium-tin-oxide thin films. The single-crystal MAPbBr3-based solar cells demonstrate a power conversion efficiency of 4.31%.

The halide perovskite Ruddlesden-Popper (RP) phases are a homologous layered subclass of solution-processable semiconductors that have aroused great attention, especially for developing long-term solar photovoltaics. They are defined as (A′)2(A)n-1PbnX3n+1 (A′ = spacer cation, A = cage cation, and X = halide anion). The orientation control of low-temperature self-assembled thin films is a fundamental issue associated with the ability to control the charge carrier transport perpendicular to the substrate. Here we report new chemical derivatives designed from a molecular perspective using a novel spacer cation 3-phenyl-2-propenammonium (PPA) with conjugated backbone as a low-temperature strategy to assemble more efficient solar cells. First, we solved and refined the crystal structures of single crystals with the general formula (PPA)2(FA0.5MA0.5)n-1PbnI3n+1 (n = 2 and 3, space group C2) using X-ray diffraction and then used the mixed halide (PPA)2(Cs0.05(FA0.88MA0.12)0.95)n-1Pbn(I0.88Br0.12)3n+1 analogues to achieve more efficient devices. While forming the RP phases, multiple hydrogen bonds between PPA and inorganic octahedra reinforce the layered structure. For films we observe that as the targeted layer thickness index increases from n = 2 to n = 4, a less horizontal preferred orientation of the inorganic layers is progressively realized along with an increased presence of high-n or 3D phases, with an improved flow of free charge carriers and vertical to substrate conductivity. Accordingly, we achieve an efficiency of 14.76% for planar p-i-n solar cells using PPA-RP perovskites, which retain 93.8 ± 0.25% efficiency with encapsulation after 600 h at 85 °C and 85% humidity (ISOS-D-3).

Perovskite solar cells (PSCs) have achieved power-conversion efficiency of 25.2%; however, their working principle remains under debate, and the stability issue has not been solved. Herein, we reve...

Layered Ruddlesden-Popper perovskite (RPP) photovoltaics have gained substantial attention owing to their excellent air stability. However, their photovoltaic performance is still limited by the unclear real-time charge-carrier mechanism of operating devices. Herein, we report the correlation between the charge-carrier mechanism and the spatially heterogeneous RPP bulks induced by distinct sublattice cations in the state-of-the-art antisolvent-driven RPP devices. In particular, abnormal heterogeneities ranging from the lateral long-range to local sub-grain scale and corresponding charge-carrier behaviours are visualized for triple-cation RPPs. We discovered that such heterogeneities with a unitary 2D/3D hybrid suppress lattice vibrations and reduce Fröhlich interactions by about 2 times, significantly promoting charge-carrier dynamics. Consequently, optimized triple-cation RPP solar cells greatly outperform their mono-cation counterparts. Furthermore, this principle can be applicable irrespective of 2D layer thickness (n > 2) and substrate type. This work provides a rationale for leveraging a disordered structure to stimulate charge-carrier motion and suggests the design principle of low-dimensional perovskites.

Capability to fabricate high-performance membrane electrode assemblies (MEAs) is a key to the commercialization of direct methanol fuel cells (DMFCs). This work reports an interface engineering method to introduce a multiscale patterned membrane and a guided metal cracked layer between the catalyst layer and the membrane by the creep-assisted sequential imprinting and simple stretching technique. The MEA with a multiscale patterned membrane, where the nanopatterns covered the whole surface even on the side surface of microstructures, showed improved performance owing to enhanced mass transport by the thinned electrode, effective utilization of the active sites, and increased Pt utilization. To obtain further performance enhancement, we incorporated a guided gold cracked layer into the MEA with the multiscale patterned membrane. The electrochemically inactive thin gold layer acted as a physical barrier for methanol crossover and the guided cracks provided multiple proton pathways. Our interface engineering utility resulted in an enhancement of the device performance by 42.3% compared with that of the reference.

It is unmistakably paradoxical that the most vulnerable aspect of the photoactive organic–inorganic hybrid perovskite is its instability against light. Why and how perovskites break down under light irradiation and what happens at the atomistic level of these materials during the degradation process still remain unanswered. In this paper, we found the culprit and verified the mechanism for the irreversible degradation of hybrid perovskite materials from our experimental investigation and ab initio molecular dynamics (AIMD) simulation. We initially found that the electrostatic charges generated by light irradiation and trapped along the grain boundaries of the perovskite crystal result in oxygen-induced irreversible degradation in dry air. This result, together with our previous experimental finding on the same critical role of trapped charges in the perovskite degradation under moisture, suggests that the trapped charges are the main culprit in both the oxygen- and moisture-induced degradation of perovskite materials. Detailed roles of oxygen and water molecules were investigated using AIMD simulation by tracking the atomic motions in the outermost layers of the oxygen- or water-covered methylammonium lead triiodide (denoted MAPbI3 for CH3NH3PbI3) perovskite crystal with trapped charges. In the first few picoseconds of our simulation, trapped charges start disrupting the crystal structure, leading to a short-range interaction between oxygen or water molecules and the compositional ions of MAPbI3. We found that there exist different degradation pathways depending on both the polarity of the trapped charge and the kind of gas molecule. We also verified that a more structurally stable, multi-component perovskite material (with the composition of MA0.6FA0.4PbI2.9Br0.1) showed much stronger resistance against light-induced degradation than MAPbI3 even in 100%-oxygen ambience or humid air.