Reduction in p-doping of the organic hole transport layer (HTL) leads to substantial improvements in PV performance in planar p–i–n perovskite solar cells.

Increasing the open circuit voltage (Voc) is one of the key strategies for further improvement of the efficiency of perovskite solar cells. It requires fundamental understanding of the complex optoelectronic processes related to charge carrier generation, transport, extraction and their loss mechanisms inside a device upon illumination. Herein we report the important origin of Voc losses in methylammonium lead iodide perovskite (MAPI) based solar cells, which results from undesirable positive charge (hole) accumulation at the interface between the perovskite photoactive layer and the PEDOT:PSS hole transport layer. We show strong correlation between the thickness-dependent surface photovoltage and device performance, unraveling that the interfacial charge accumulation leads to charge carrier recombination and results in a large decrease in Voc for the PEDOT:PSS/MAPI inverted devices (180 mV reduction in 50-nm-thick device compared to 230-nm-thick one). In contrast, accumulated positive charges at the TiO2/MAPI interface modify interfacial energy band bending, which leads to an increase in Voc for the TiO2/MAPI conventional devices (70 mV increase in 50-nm-thick device compared to 230-nm-thick one). Our results provide an important guideline for better control of interfaces in perovskite solar cells to improve device performance further.

Metal halide perovskites (MHPs) have emerged as promising materials for light‐emitting diodes owing to their narrow emission spectrum and wide range of color tunability. However, the low exciton binding energy in MHPs leads to a competition between the trap‐mediated nonradiative recombination and the bimolecular radiative recombination. Here, efficient and stable green emissive perovskite light‐emitting diodes (PeLEDs) with an external quantum efficiency of 14.6% are demonstrated through compositional, dimensional, and interfacial modulations of MHPs. The interfacial energetics and optoelectronic properties of the perovskite layer grown on a nickel oxide (NiOx) and poly(3,4‐ethylenedioxythiophene):polystyrene sulfonate hole injection interfaces are investigated. The better interface formed between the NiOx/perovskite layers in terms of lower density of traps/defects, as well as more balanced charge carriers in the perovskite layer leading to high recombination yield of carriers are the main reasons for significantly improved device efficiency, photostability of perovskite, and operational stability of PeLEDs.

Carbon dots on photoactive semiconductor nanomaterials have represented an effective strategy for enhancing their photoelectrochemical (PEC) activity. By carefully designing and manipulating carbon dots/support composite, a high photocurrent could be obtained. Currently, there is not much fundamental understanding of how the interaction between such materials can facilitate the reaction process. This hinders the wide applicability in PEC devices. To address this need of improving the fundamental understanding of carbon dots/semiconductor nanocomposite, we have taken the TiO 2 case as a model semiconductor system with nitrogen-doped carbon dots (NCDs).We present here with in-depth investigation of the structural hybridization and energy transitions in the NCDs/TiO 2 photoelectrode via high-resolution scanning transmission microscopy (HR-STEM), electron energy loss spectroscopy (EELS), UV-Vis absorption, electrochemical impedance spectroscopy (EIS), Mott-Schottky (M-S), time-correlated single photon counting (TCSPC) and ultra-violet photoelectron spectroscopy (UPS), which shed some light on the charge transfer process at the carbon dots and TiO 2 interface. We show that N doping in carbon dots can effectively prolong the carrier lifetime, and the hybridisation of NCDs and TiO 2 is able not only to extend TiO 2 light response into the visible range but also to form heterojunction at the NCDs/TiO 2 interface with properly aligned band structure that allows a spatial separation of the charges. This work is arguably the first to report the direct probing of the band positions of carbon dots-TiO nanoparticle composite in a PEC system for understanding the energy transfer mechanism, demonstrating the favourable role of NCDs in the photocurrent response of TiO 2 for water oxidation process. This study reveals the importance of combining structural, photophysical and electrochemical experiments to develop a comprehensive understanding of the nanoscale charge transfer processes between the carbon dots and their catalyst supports.

Low‐light applications provide an exciting market opportunity for organic solar cells (OSCs). However, so far, studies have only considered OSCs of limited commercial viability. Herein, the applicability of a fully‐scalable, flexible, inverted non‐fullerene acceptor (NFA) containing OSC is demonstrated by showing its superior performance to silicon under low‐light, achieving 40 µW cm−2 maximum power output at 1300 lx illumination. The effect of parasitic resistance and dark current on low‐light performance are identified. Furthermore, an atmosphere sensitive light‐soaking (LS) effect, critical for low‐light performance and resulting in undesirable S‐shaped current‐voltage characteristics, is analyzed. By employing different interlayers and photoactive layers (PALs) the origin of this LS effect is identified as poor electron extraction at the electron transport layer (ETL)/PAL interface when the common ETL ZnO is used. Two strategies are implemented to overcome the LS effect: replacement of ZnO with SnO2 nanoparticles to reduce ETL sub‐gap electron trap states or tuning the NFA energy levels to optimize interfacial energetics. Finally, the commercial viability of these LS‐free devices is demonstrated by fabricating fully printed large‐area modules (21.6 cm2) achieving a maximum power output of 17.2 µW cm−2, providing the most relevant example of the currently obtainable performance in commercial low‐light OSCs.