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The ability to passivate defects and modulate the interface energy‐level alignment (IEA) is key to boost the performance of perovskite solar cells (PSCs). Herein, we report a robust route that simultaneously allows defect passivation and reduced energy difference between perovskite and hole transport layer (HTL) via the judicious placement of polar chlorine‐terminated silane molecules at the interface. Density functional theory (DFT) points to effective passivation of the halide vacancies on perovskite surface by the silane chlorine atoms. An integrated experimental and DFT study demonstrates that the dipole layer formed by the silane molecules decreases the perovskite work function, imparting an Ohmic character to the perovskite/HTL contact. The corresponding PSCs manifest a nearly 20 % increase in power conversion efficiency over pristine devices and a markedly enhanced device stability. As such, the use of polar molecules to passivate defects and tailor the IEA in PSCs presents a promising platform to advance the performance of PSCs.

 

Metal halide perovskite nanocrystals (PNCs) have recently garnered tremendous research interest due to their unique optoelectronic properties and promising applications in photovoltaics and optoelectronics. Metal halide PNCs can be combined with polymers to create nanocomposites that carry an array of advantageous characteristics. The polymer matrix can bestow stability, stretchability, and solution‐processability while the PNCs maintain their size‐, shape‐ and composition‐dependent optoelectronic properties. As such, these nanocomposites possess great promise for next‐generation displays, lighting, sensing, biomedical technologies, and energy conversion. The recent advances in metal halide PNC/polymer nanocomposites are summarized here. First, a variety of synthetic strategies for crafting PNC/polymer nanocomposites are discussed. Second, their array of intriguing properties is examined. Third, the broad range of applications of PNC/polymer nanocomposites is highlighted, including light‐emitting diodes (LEDs), lasers, and scintillators. Finally, an outlook on future research directions and challenges in this rapidly evolving field are presented.

 

Approaches to achieve stable perovskite nanocrystals (PNCs) of interest, in particular those with large structural anisotropy, through protective coating of the inorganic shell at a single‐nanocrystal (NC) level are comparatively few and limited in scope. Reported here is a robust amphiphilic‐diblock‐copolymer‐enabled strategy for crafting highly‐stableanisotropicCsPbBr₃nanosheets (NSs) by in situ formation of a uniform inorganic shell (1st shielding) that is intimately ligated with hydrophobic polymers (2nd shielding). The dual‐protected NSs display an array of remarkable stabilities (i.e., thermal, photostability, moisture, polar solvent, aliphatic amine, etc.) and find application in white‐light‐emitting diodes. In principle, by anchoring other multidentate amphiphilic polymer ligands on the surface of PNCs, followed by templated‐growth of shell materials of interest, a rich variety of dual‐shelled, multifunctional PNCs with markedly improved stabilities can be created for use in optics, optoelectronics, and sensory devices.

 

2D black phosphorene (BP) carries a stellar set of physical properties such as conveniently tunable bandgap and extremely high ambipolar carrier mobility for optoelectronic devices. Herein, the judicious design and positioning of BP with tailored thickness as dual‐functional nanomaterials to concurrently enhance carrier extraction at both electron transport layer/perovskite and perovskite/hole transport layer interfaces for high‐efficiency and stable perovskite solar cells is reported. The synergy of favorable band energy alignment and concerted cascade interfacial carrier extraction, rendered by concurrent positioning of BP, delivered a progressively enhanced power conversion efficiency of 19.83% from 16.95% (BP‐free). Investigation into interfacial engineering further reveals enhanced light absorption and reduced trap density for improved photovoltaic performance with BP incorporation. This work demonstrates the appealing characteristic of rational implementation of BP as dual‐functional transport material for a diversity of optoelectronic devices, including photodetectors, sensors, light‐emitting diodes, etc.

 

In recent years, there have been rapid advances in the synthesis of lead halide perovskite nanocrystals (NCs) for use in solar cells, light emitting diodes, lasers, and photodetectors. These compounds have a set of intriguing optical, excitonic, and charge transport properties, including outstanding photoluminescence quantum yield (PLQY) and tunable optical band gap. However, the necessary inclusion of lead, a toxic element, raises a critical concern for future commercial development. To address the toxicity issue, intense recent research effort has been devoted to developing lead‐free halide perovskite (LFHP) NCs. In this Review, we present a comprehensive overview of currently explored LFHP NCs with an emphasis on their crystal structures, synthesis, optical properties, and environmental stabilities (e.g., UV, heat, and moisture resistance). In addition, strategies for enhancing optical properties and stabilities of LFHP NCs as well as the state‐of‐the‐art applications are discussed. With the perspective of their properties and current challenges, we provide an outlook for future directions in this rapidly evolving field to achieve high‐quality LFHP NCs for a broader range of fundamental research and practical applications.

 

Instability of perovskite quantum dots (QDs) toward humidity remains one of the major obstacles for their long‐term use in optoelectronic devices. Herein, a general amphiphilic star‐like block copolymer nanoreactor strategy for in situ crafting a set of hairy perovskite QDs with precisely tunable size and exceptionally high water and colloidal stabilities is presented. The selective partition of precursors within the compartment occupied by inner hydrophilic blocks of star‐like diblock copolymers imparts in situ formation of robust hairy perovskite QDs permanently ligated by outer hydrophobic blocks via coprecipitation in nonpolar solvent. These size‐ and composition‐tunable perovskite QDs reveal impressive water and colloidal stabilities as the surface of QDs is intimately and permanently ligated by a layer of outer hydrophobic polymer hairs. More intriguingly, the readily alterable length of outer hydrophobic polymers renders the remarkable control over the stability enhancement of hairy perovskite QDs.

 

Lead halide perovskite nanocrystals possess incredible potential as next generation emitters due to their stellar set of optoelectronic properties. Unfortunately, their instability towards many ambient conditions and reliance on batch processing hinder their widespread utilities. Herein, we address both challenges by continuously synthesizing highly stable perovskite nanocrystals via integrating star-like block copolymer nanoreactors into a house-built flow reactor. Perovskite nanocrystals manufactured in this strategy display significantly enhanced colloidal, UV, and thermal stabilities over those synthesized with conventional ligands. Such scaling up of highly stable perovskite nanocrystals represents an important step towards their eventual use in many practical applications in optoelectronic materials and devices. 

As one of the latest additions to the 2D nanomaterials family, black phosphorene (BP, monolayer or few-layer black phosphorus) has gained much attention in various forms of solar cells. This is due largely to its intriguing semiconducting properties such as tunable direct bandgap (from 0.3 eV in the bulk to 2.0 eV in the monolayer), extremely high ambipolar carrier mobility, broad visible to infrared light absorption, etc. These appealing optoelectronic attributes make BP a multifunctional nanomaterial for use in solar cells via tailoring carrier dynamics, band energy alignment, and light harvesting, thereby promoting the rapid development of third-generation solar cells. Notably, in sharp contrast to the copious work on revealing the fundamental properties of BP, investigation into the utility of BP is comparatively less, particularly in the area of photovoltaics. Herein, we first identify and summarize an array of unique characteristics of BP that underpin its application in photovoltaics, aiming at providing inspiration to develop new designs and device architectures of photovoltaics. Subsequently, state-of-the-art synthetic routes ( i.e. , top-down and bottom-up) to scalable BP production that facilitates its applications in optoelectronic materials and devices are outlined. Afterward, recent advances in a diverse set of BP-incorporated solar cells, where BP may impart electron and/or hole extraction and transport, function as a light absorber, provide dielectric screening for enhancing exciton dissociation, and modify the morphology of photoabsorbers, are discussed, including organic solar cells, dye-sensitized solar cells, heterojunction solar cells and perovskite solar cells. Finally, the challenges and opportunities in this rapidly evolving field are presented.