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Rapid and deliberate patterning of nanomaterials over a large area is desirable for device manufacturing. We report a method for meniscus‐assisted self‐assembly (MASA)‐enabled rapid positioning of hierarchically assembled dots and stripes composed of luminescent conjugated polymer over two length scales. Periodically arranged conjugated poly(9,9‐dioctylfluorene) (PFO) polymers, yield dots, punch‐holes and stripes at microscopic scale via MASA. Concurrent self‐assembly of PFOs into two‐dimensional lenticular crystals within each dot, punch‐hole and stripe is realized at nanoscopic scale. Hierarchical assembly is achieved by constraining the evaporation of the PFOs solution in two approximately parallel plates via a MASA process. The three‐phase contact line (TCL) of the liquid meniscus of the PFOs was printed using the upper plate, yielding an array of curved stripes. Rapid creation of hierarchical assemblies via MASA opens up possibilities for large‐scale organization of a wide range of soft matters and nanomaterials.

Rapid and deliberate patterning of nanomaterials over a large area is desirable for device manufacturing. We report a method for meniscus‐assisted self‐assembly (MASA)‐enabled rapid positioning of hierarchically assembled dots and stripes composed of luminescent conjugated polymer over two length scales. Periodically arranged conjugated poly(9,9‐dioctylfluorene) (PFO) polymers, yield dots, punch‐holes and stripes at microscopic scale via MASA. Concurrent self‐assembly of PFOs into two‐dimensional lenticular crystals within each dot, punch‐hole and stripe is realized at nanoscopic scale. Hierarchical assembly is achieved by constraining the evaporation of the PFOs solution in two approximately parallel plates via a MASA process. The three‐phase contact line (TCL) of the liquid meniscus of the PFOs was printed using the upper plate, yielding an array of curved stripes. Rapid creation of hierarchical assemblies via MASA opens up possibilities for large‐scale organization of a wide range of soft matters and nanomaterials.

Despite recent rapid advances in metal halide perovskites for use in optoelectronics, the fundamental understanding of the electrical‐poling‐induced ion migration, accounting for many unusual attributes and thus performance in perovskite‐based devices, remain comparatively elusive. Herein, the electrical‐poling‐promoted polarization potential is reported for rendering hybrid organic–inorganic perovskite photodetectors with high photocurrent and fast response time, displaying a tenfold enhancement in the photocurrent and a twofold decrease in the response time after an external electric field poling. First, a robust meniscus‐assisted solution‐printing strategy is employed to facilitate the oriented perovskite crystals over a large area. Subsequently, the electrical poling invokes the ion migration within perovskite crystals, thus inducing a polarization potential, as substantiated by the surface potential change assessed by Kelvin probe force microscopy. Such electrical‐poling‐induced polarization potential is responsible for the markedly enhanced photocurrent and largely shortened response time. This work presents new insights into the electrical‐poling‐triggered ion migration and, in turn, polarization potential as well as into the implication of the latter for optoelectronic devices with greater performance. As such, the utilization of ion‐migration‐produced polarization potential may represent an important endeavor toward a wide range of high‐performance perovskite‐based photodetectors, solar cells, transistors, scintillators, 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.

In den letzten Jahren gab es rasante Fortschritte bei der Synthese von Bleihalogenid‐Perowskit‐Nanokristallen (NCs) für den Einsatz in Solarzellen, Leuchtdioden, Lasern und Photodetektoren. Sie besitzen eine Reihe faszinierender optischer, excitonischer und Ladungstransporteigenschaften, einschließlich hervorragender Photolumineszenz‐Quantenausbeuten (PLQY) und abstimmbaren optischen Bandlücken. Die notwendige Verwendung von Blei, einem toxischen Element, gibt jedoch Anlass zu ernsthafter Besorgnis über die zukünftige kommerzielle Entwicklung. Um das Problem der Toxizität zu lösen, wurden in jüngster Zeit intensive Forschungsarbeiten zur Entwicklung bleifreier Halogenid‐Perowskit(LFHP)‐NCs durchgeführt. In diesem Aufsatz geben wir einen Überblick über die derzeit erforschten LFHP‐NCs mit den Schwerpunkten Kristallstruktur, Synthese, optische Eigenschaften und Umgebungsstabilität (z. B. UV‐, Wärme‐ und Feuchtigkeitsbeständigkeit). Darüber hinaus werden Strategien zur Verbesserung der optischen Eigenschaften und Stabilitäten von LFHP‐NCs sowie deren neueste Anwendungen diskutiert.

Despite recent progress in producing perovskite nanowires (NWs) for optoelectronics, it remains challenging to solution‐print an array of NWs with precisely controlled position and orientation. Herein, we report a robust capillary‐assisted solution printing (CASP) strategy to rapidly access aligned and highly crystalline perovskite NW arrays. The key to the CASP approach lies in the integration of capillary‐directed assembly through periodic nanochannels and solution printing through the programmably moving substrate to rapidly guide the deposition of perovskite NWs. The growth kinetics of perovskite NWs was closely examined by in situ optical microscopy. Intriguingly, the as‐printed perovskite NWs array exhibit excellent optical and optoelectronic properties and can be conveniently implemented for the scalable fabrication of photodetectors.

Despite recent progress in producing perovskite nanowires (NWs) for optoelectronics, it remains challenging to solution‐print an array of NWs with precisely controlled position and orientation. Herein, we report a robust capillary‐assisted solution printing (CASP) strategy to rapidly access aligned and highly crystalline perovskite NW arrays. The key to the CASP approach lies in the integration of capillary‐directed assembly through periodic nanochannels and solution printing through the programmably moving substrate to rapidly guide the deposition of perovskite NWs. The growth kinetics of perovskite NWs was closely examined by in situ optical microscopy. Intriguingly, the as‐printed perovskite NWs array exhibit excellent optical and optoelectronic properties and can be conveniently implemented for the scalable fabrication of photodetectors.

Thermoresponsive nanoparticles (NPs) represent an important hybrid material comprising functional NPs with temperature‐sensitive polymer ligands. Strikingly, significant discrepancies in optical and catalytic properties of thermoresponsive noble‐metal NPs have been reported, and have yet to be unraveled. Reported herein is the crafting of Au NPs, intimately and permanently ligated by thermoresponsive poly(N‐isopropylacrylamide) (PNIPAM), in situ using a starlike block copolymer nanoreactor as model system to resolve the paradox noted above. As temperature rises, plasmonic absorption of PNIPAM‐capped Au NPs red‐shifts with increased intensity in the absence of free linear PNIPAM, whereas a greater red‐shift with decreased intensity occurs in the presence of deliberately introduced linear PNIPAM. Remarkably, the absence or addition of free linear PNIPAM also accounts for non‐monotonic or switchable on/off catalytic performance, respectively, of PNIPAM‐capped Au NPs.

Thermoresponsive nanoparticles (NPs) represent an important hybrid material comprising functional NPs with temperature‐sensitive polymer ligands. Strikingly, significant discrepancies in optical and catalytic properties of thermoresponsive noble‐metal NPs have been reported, and have yet to be unraveled. Reported herein is the crafting of Au NPs, intimately and permanently ligated by thermoresponsive poly(N‐isopropylacrylamide) (PNIPAM), in situ using a starlike block copolymer nanoreactor as model system to resolve the paradox noted above. As temperature rises, plasmonic absorption of PNIPAM‐capped Au NPs red‐shifts with increased intensity in the absence of free linear PNIPAM, whereas a greater red‐shift with decreased intensity occurs in the presence of deliberately introduced linear PNIPAM. Remarkably, the absence or addition of free linear PNIPAM also accounts for non‐monotonic or switchable on/off catalytic performance, respectively, of PNIPAM‐capped Au NPs.