Hole transporting materials (HTMs) play a crucial role in achieving highly efficient and stable perovskite solar cells (PSCs). Spirotyped materials being the most widely used HTMs are commonly utilized with dopants, such as Li-TFSI, to improve their carrier mobility significantly. However, dopants could affect the morphology of hole transporting layer negatively by forming defects and pinholes which restrict the performance of devices. Here, we adopt the extended πconjugated structures N-ethylcarbazole and dibenzothiophene to substitute the donor group 4-methoxyphenyl of spiro-OMeTAD, devising two novel HTMs, SC and ST, respectively. Notably, SC possesses low crystallinity and good solubility due to the existence of ethyl in side groups, leading to decent miscibility with Li-TFSI to prevent unfavorable phase-separation. The SC-based device delivers the best power conversion efficiency (PCE) of 21.76% which is higher than that of spiro-OMeTAD (20.73%), attributed to the formation of smooth and pinhole-free morphology. Moreover, it exhibits long-term stability and retains over 90% of initial PCE value for more than 30 days without encapsulation in ambient air. In contrast, the STbased device suffers from dense pinholes induced by its relatively high crystallinity and poor solubility, resulting in a low PCE of 18.18% and inferior stability. Thus, it is effective to modify the side groups in spiro-typed HTMs with specific structures to obtain predictable properties, fabricating PSCs with high efficiency and stability facilely.

The development of quasi-two-dimensional (2D) Ruddlesden-Popper phase perovskite solar cells (PSCs) has greatly improved the stability of devices. However, the presence of quantum confinement effects and insulating spacer cations in...

Mixed-halide perovskite has an irreplaceable role as wide-bandgap absorber in multi-junction tandem solar cells. However, large open-circuit voltage (V oc ) loss due to non-uniform halide distribution and compromised device stability due to photo-induced halide segregation has significantly limited the applications. Here, it is introduced 4-(2-aminoethyl)-benzenesulfonyl fluoride hydrochloride (ABF) with multifunctional groups (sulfonyl, ammonium, and fluoride) to the mixed-halide precursor to demonstrate a downward homogenized crystallization strategy for suppressing the initial vertical halide phase separation during perovskite crystallization and reducing V oc loss. Furthermore, fluoride with strong electronegativity effectively fixes anions and cations, while sulfonyl and ammonium are used to passivate positive charged (halide vacancies) and negative charged (FA/MA vacancies) defects, respectively, thereby reducing the generation of ion vacancies that lead to subsequent photo-induced halide segregation. As a result, the 1.63 and 1.68 eV wide-bandgap perovskite solar cells with inverted structures exhibit the champion power conversion efficiency (PCE) of 21.76% and 20.11% with V oc of 1.18 and 1.21 V, respectively. Most importantly, the optimized devices without encapsulation preserve 86% of initial efficiency after 240 h of continuous illumination under AM 1.5G, showing excellent light stability. Thus, the homogenized crystallization strategy provides highly efficient performance and stability for future tandem solar cell applications.

The two-dimensional (2D)/three-dimensional (3D) heterojunction perovskite solar cell (PSC) has recently been recognized as a promising photovoltaic structure for achieving high efficiency and long-term stability. Rational design of the 2D spacer cation is important to achieve a win–win situation for defects’ passivation and photogenerated carrier extraction. Herein, we carry out first-principles calculation to analyze the dipole moment of phenethylamine-type molecules and their resulting 2D/3D perovskites. Based on the results of theoretical calculation, the dipole moment of 2D cations can be well tuned by varying the number of fluorine atoms on the para-position of the benzene ring, which further determines the interfacial dipole across the 2D/3D heterojunction interface. A high dipole 2D perovskite layer at the interface between the 3D perovskite and hole-transporting material is found to promote charge transport and suppress charge trapping efficiently. As a result, our 2D/3D PSCs exhibit a champion power conversion efficiency over 22% and a fill factor over 83%. Moreover, our solar cells also show a remarkable stability, maintaining 80% of its initial efficiency for more than 1400 h without encapsulation under a 30 ± 5% relative humidity.

In the journey to obtain well-crystallized mixed tin (Sn) -lead (Pb) iodide perovskite films for solar cell application, great difficulties have been presented due to very different crystallization rates between...