Lead-Chelating Intermediate for Air-Processed Phase-Pure FAPbI3 Perovskite Solar Cells.

Formamidinium-lead triiodide (FAPbI3) perovskite holds promise as a prime candidate in the realm of perovskite photovoltaics. However, the photo-active α-FAPbI3 phase, existing as a metastable state, is observable solely at elevated temperatures and is susceptible to degradation into the δ-phase in ambient air. Therefore, the attainment of phase-stable α-FAPbI3 in ambient conditions has become a crucial objective in perovskite research. Here, we proposed an efficient conversion process of PbI2 into the α-FAPbI3 perovskites in ambient air. This conversion was facilitated by the introduction of chelating molecules, which interacted with PbI2 to form an intermediate phase. Due to the reduced formation barrier resulting from the altered reaction pathway, this stable intermediate phase transitioned directly into α-FAPbI3 upon the deposition of the organic cation solution, effectively bypassing the formation of δ-FAPbI3. Consequently, the ambient-fabricated FAPbI3 perovskite solar cells (PSCs) exhibited an outstanding power conversion efficiency of 25.08%, along with a high open-circuit voltage of 1.19 V. Furthermore, the unencapsulated devices demonstrated remarkable environmental stability. Notably, this innovative approach promises broad applicability across various chelating molecules, opening new avenues for further progress in the ambient air fabrication of FAPbI3 PSCs.

Droplet-based mechanical transducers modulated by the symmetry of wettability patterns.

Asymmetric mechanical transducers have important applications in energy harvesting, signal transmission, and micro-mechanics. To achieve asymmetric transformation of mechanical motion or energy, active robotic metamaterials, as well as materials with asymmetric microstructures or internal orientation, are usually employed. However, these strategies usually require continuous energy supplement and laborious fabrication, and limited transformation modes are achieved. Herein, utilizing wettability patterned surfaces for precise control of the droplet contact line and inner flow, we demonstrate a droplet-based mechanical transducer system, and achieve multimodal responses to specific vibrations. By virtue of the synergistic effect of surface tension and solid-liquid adhesion on the liquid dynamics, the droplet on the patterned substrate can exhibit symmetric/asymmetric vibration transformation when the substrate vibrates horizontally. Based on this, we construct arrayed patterns with distinct arrangements on the substrate, and employ the swarm effect of the arrayed droplets to achieve three-dimensional and multimodal actuation of the target plate under a fixed input vibration. Further, we demonstrate the utilization of the mechanical transducers for vibration management, object transport, and laser modulation. These findings provide a simple yet efficient strategy to realize a multimodal mechanical transducer, which shows significant potential for aseismic design, optical molding, as well as micro-electromechanical systems (MEMS).

In-Situ Cyclized Polyacrylonitrile as an Electron Selective Layer for n-i-p Perovskite Solar Cell with Enhanced Efficiency and Stability.

In-situ cyclized polyacrylonitrile (CPAN) is developed to replace n-type metal oxide semiconductors (TiO2 or SnO2) as an electron selective layer (ESL) for highly efficient and stable n-i-p perovskite solar cells (PSCs). The CPAN layer is fabricated via facile in-situ cyclization reaction of polyacrylonitrile (PAN) coated on a conducting glass substrate. The CPAN layer is robust and insoluble in common solvents, and possesses n-type semiconductor properties with a high electron mobility of 4.13 x 10-3 cm2 V-1 s-1. With the CPAN as an ESL, the PSC affords a power conversion efficiency (PCE) of 23.12%, which is the highest for the n-i-p PSCs with organic ESLs. Moreover, the device with the CPAN layer holds superior operational stability, maintaining over 90% of their initial efficiency after 500 h continuous light soaking. These results confirm that the CPAN layer would be a desirable low-cost and efficient ESL for n-i-p PSCs and other photoelectronic devices with high performance and stability.

Unveiling the Potential of Two-Terminal Perovskite/Organic Tandem Solar Cells: Mechanisms, Status, and Challenges.

Perovskite/organic tandem solar cells (PO-TSCs) demonstrate exceptional suitability for emerging applications such as building-integrated photovoltaics, wearable devices, and greenhouse farming. By leveraging the distinctive attributes of perovskite and organic materials, which encompass expanded solar spectrum utilization, chemically benign solubility, and soft nature, PO-TSCs position themselves as ideal candidates for high-performance semi-transparent photovoltaics (ST-PVs). Despite these advantages, their development significantly lags behind other perovskite-based counterparts, such as perovskite/perovskite, perovskite/silicon, and perovskite/Cu(In, Ga)Se2. To address existing challenges and unlock the full potential of PO-TSCs, an exploration of the fundamental mechanisms governing tandem photovoltaic devices is embarked. Delving into critical aspects such as charge generation/separation, energy level alignment, and material choices becomes pivotal for optimizing PO-TSC performance. The investigation of monolithic two-terminal PO-TSCs offers insights into achievements and barriers, recognizing the competitive landscape with other TSC counterparts. Further scrutiny of perovskite absorbers and organic absorbers in TSCs reveals strategies aimed at enhancing stability and efficiency. The discussion extends to interconnection layers, elucidating their role in optimizing light transmission and balancing carrier recombination. In conclusion, a compelling outlook on the dynamic landscape of PO-TSCs is presented, highlighting the remarkable efficiency progression and signaling their potential to revolutionize solar energy harvesting technologies.

Printed Divisional Optical Biochip for Multiplex Visualizable Exosome Analysis at Point-of-Care.

Rapid detection of various exosomes is of great significance in early diagnosis and postoperative monitoring of cancers. Here, a divisional optical biochip is reported for multiplex exosome analysis via combining the self-assembly of nanochains and precise surface patterning. Arising from resonance-induced near-field enhancement, the nanochains show distinct color changes after capturing target exosomes for direct visual detection. Then, a series of divisional nanochain-based biochips conjugated with several specific antibodies are fabricated through designed hydrophilic and hydrophobic patterns. Because of the significant wettability difference, one sample droplet is precisely self-splitting into several microdroplets enabling simultaneous identification of multiple target exosomes in 30 min with a sensitivity of 6 × 107 particles mL-1 , which is about two orders lower than enzyme-linked immunosorbent assay. Apart from the trace amount detection, excellent semiquantitative capability is demonstrated to distinguish clinical exosomes from glioblastoma patients and healthy people. This method is simple, versatile, and highly efficient that can be extended as a diagnostic tool for many diseases, promoting the development of liquid biopsy.

Perovskite-based photodetector for real-time and quantitative monitoring of sports motion.

Reliable monitoring the movement amplitude and dynamics during sports exercise is significant for improving training results and preventing training wound. Here, we present a printed perovskite-based photodetector for real-time and quantitative monitoring of sports motion. The ordered nucleation and growth of perovskite crystals are regulated by the 4-acetamidothiophenol (AMTP) at the interface, which promotes the size of perovskite crystals into the micrometer. Benefiting from the uniformity of the AMTP-regulated MAPbI3, the as-prepared photodetector gives great photocurrent response under indoor light or outdoor light. During the exercise, real-time monitoring sports motion is achieved through detecting the illumination changing of photodetectors attaching on the wrist and ankles. Moreover, twelve kinds of common sports can be quantitatively analyzed with the detection of illumination changing on the photodetector. Such photodetector provides an efficient measurement method of wearable electronics for sports monitoring.

Bio-inspired optical structures for enhancing luminescence.

Luminescence is an essential signal for many plants, insects, and marine organisms to attract the opposite sex, avoid predators, and so on. Most luminescent living organisms have ingenious optical structures which can help them get high luminescent performances. These remarkable and efficient structures have been formed by natural selection from long-time evolution. Researchers keenly observed the enhanced luminescence phenomena and studied how these phenomena happen in order to learn the characteristics of bio-photonics. In this review, we summarize the optical structures for enhancing luminescence and their applications. The structures are classified according to their different functions. We focus on how researchers use these biological inspirations to enhance different luminescence processes, such as chemiluminescence (CL), photoluminescence (PL), and electroluminescence (EL). It lays a foundation for further research on the applications of luminescence enhancement. Furthermore, we give examples of luminescence enhancement by bio-inspired structures in information encryption, biochemical detection, and light sources. These examples show that it is possible to use bio-inspired optical structures to solve complex problems in optical applications. Our work will provide guidance for research on biomimetic optics, micro- and nano-optical structures, and enhanced luminescence.

Photochemically deoxygenating micelles for protecting TTA-UC against oxygen quenching.

Pluronic F127, P123 and cross-linked F127 diacrylate micelles are photochemically deoxygenating nanocapsules in which oxygen could be removed by photochemical reaction with a surfactant and efficient triplet-triplet annihilation photon upconversion (TTA-UC) can be achieved in air. The efficiency of TTA-UC under air is comparable to that under deoxygenated conditions.

Direct writing concave structure on viscoelastic substrate for loading and releasing liquid on skin surface.

Droplet deposition on deformable matrix has a broad application prospect. Regular deposition and diffusion of droplet on the substrate is the key to prepare flexible concave structure. Direct writing technique is an advanced method for depositing ink droplet on various substrates, which could produce a variety of deposition forms. Meanwhile, direct writing technique has the characteristics of simplicity, convenience and strong controllability. In this work, patterned concave structure was fabricated with viscoelastic substrate by direct writing technology, depositing behavior of ink droplet, formation condition and shape control of concave structure were studied with viscoelastic substrate, and practical application of the patterned concave structure was explored in loading and releasing liquid on skin surface. This study provides an efficient method for the preparation and application of controllable concave surface.

Bioinspired "cage traps" for closed-loop lead management of perovskite solar cells under real-world contamination assessment.

Despite the remarkable progress made in perovskite solar cells, great concerns regarding potential Pb contamination risk and environmental vulnerability risks associated with perovskite solar cells pose a significant obstacle to their real-world commercialization. In this study, we took inspiration from the ensnaring prey behavior of spiders and chemical components in spider web to strategically implant a multifunctional mesoporous amino-grafted-carbon net into perovskite solar cells, creating a biomimetic cage traps that could effectively mitigate Pb leakage and shield the external invasion under extreme weather conditions. The synergistic Pb capturing mechanism in terms of chemical chelation and physical adsorption is in-depth explored. Additionally, the Pb contamination assessment of end-of-life perovskite solar cells in the real-world ecosystem, including Yellow River water and soil, is proposed. The sustainable closed-loop Pb management process is also successfully established involving four critical steps: Pb precipitation, Pb adsorption, Pb desorption, and Pb recycling. Our findings provide inspiring insights for promoting green and sustainable industrialization of perovskite solar cells.

Multifunctional Perovskite Photodetectors: From Molecular-Scale Crystal Structure Design to Micro/Nano-scale Morphology Manipulation.

Multifunctional photodetectors boost the development of traditional optical communication technology and emerging artificial intelligence fields, such as robotics and autonomous driving. However, the current implementation of multifunctional detectors is based on the physical combination of optical lenses, gratings, and multiple photodetectors, the large size and its complex structure hinder the miniaturization, lightweight, and integration of devices. In contrast, perovskite materials have achieved remarkable progress in the field of multifunctional photodetectors due to their diverse crystal structures, simple morphology manipulation, and excellent optoelectronic properties. In this review, we first overview the crystal structures and morphology manipulation techniques of perovskite materials and then summarize the working mechanism and performance parameters of multifunctional photodetectors. Furthermore, the fabrication strategies of multifunctional perovskite photodetectors and their advancements are highlighted, including polarized light detection, spectral detection, angle-sensing detection, and self-powered detection. Finally, the existing problems of multifunctional detectors and the perspectives of their future development are presented.

Molecular Recognition-Modulated Hetero-Assembly of Nanostructures for Visualizable and Portable Detection of Circulating miRNAs.

Biomolecular markers, particularly circulating microRNAs (miRNAs) play an important role in diagnosis, monitoring, and therapeutic intervention of cancers. However, existing detection strategies remain intricate, laborious, and far from being developed for point-of-care testing. Here, we report a portable colorimetric sensor that utilizes the hetero-assembly of nanostructures driven by base pairing and recognition for direct detection of miRNAs. Following hybridization, two sizes of nanoparticles modified with single-strand DNA can be robustly assembled into heterostructures with strong optical resonance, exhibiting distinct structure colors. Particularly, the large nanoparticles are first arranged into nanochains to enhance scattering signals of small nanoparticles, which allows for sensitive detection and quantification of miRNAs without the requirement of target extraction, amplification, and fluorescent labels. Furthermore, we demonstrate the high specificity and single-base selectivity of testing different miRNA samples, which shows great potential in the diagnosis, staging, and monitoring of cancers. These heterogeneous assembled nanostructures provide an opportunity to develop simple, fast, and convenient tools for miRNAs detection, which is suitable for many scenarios, especially in low-resource setting.

FP(µ-N)2 S: A Sulfur-Pnictogen Four-Membered Ring with 6π Electrons.

The new 6π-electron four-membered ring compound 3-fluoro-1λ2 ,2,4,3λ3 -thiadiazaphosphetidine, FP(µ-N)2 S, has been generated in the gas phase through high-vacuum flash pyrolysis (HVFP) of thiophosphoryl diazide, FP(S)(N3 )2 , at 1000 K. Subsequent isolation of FP(µ-N)2 S in cryogenic matrices (Ar, Ne, and N2 ) allows its characterization with matrix-isolation IR and UV-vis spectroscopy by combination with 15 N-isotope labeling and computations at the CCSD(T)-F12a/VTZ-F12 level of theory. Upon visible-light irradiation at 550 nm, this cyclic compound undergoes ring-opening to the thiazyl isomer FPNSN, followed by dissociation to FP and SN2 under subsequent UV-irradiation at 365 nm. In sharp contrast to the square planar structure for the isolobal four-membered ring S2 N2 , a puckered structure with significant biradical character has been found for FP(µ-N)2 S.

Heterogeneous Self-Assembly of a Single Type of Nanoparticle Modulated by Skin Formation.

Self-assembly of colloidal nanoparticles has generated tremendous interest due to its widespread applications in structural colorations, sensors, and optoelectronics. Despite numerous strategies being developed to fabricate sophisticated structures, the heterogeneous self-assembly of a single type of nanoparticle in one step remains challenging. Here, facilitated by spatial confinement induced by a skin layer in a drying droplet, we achieve the heterogeneous self-assembly of a single type of nanoparticle by quickly evaporating a colloid-poly (ethylene glycol) (PEG) droplet. During the drying process, a skin layer forms at the droplet surface. The resultant spatial confinement assembles nanoparticles into face-centered-cubic (FCC) lattices with (111) and (100) plane orientations, generating binary bandgaps and two structural colors. The self-assembly of nanoparticles can be regulated by varying the PEG concentration so that FCC lattices with homo- or heterogeneous orientation planes can be prepared on demand. Besides, the approach is applicable for diverse droplet shapes, various substrates, and different nanoparticles. The one-pot general strategy breaks the requirements for multiple types of building blocks and predesigned substrates, extending the fundamental understanding underlying colloidal self-assembly.

Tailoring vapor film beneath a Leidenfrost drop.

For a drop on a very hot solid surface, a vapor film will form beneath the drop, which has been discovered by Leidenfrost in 1756. The vapor escaping from the Leidenfrost film causes uncontrollable flows, and actuates the drop to move around. Recently, although numerous strategies have been used to regulate the Leidenfrost vapor, the understanding of surface chemistry for modulating the phase-change vapor dynamics remains incomplete. Here, we report how to rectify vapor by "cutting" the Leidenfrost film using chemically heterogeneous surfaces. We demonstrate that the segmented film cut by a Z-shaped pattern can spin a drop, since the superhydrophilic region directly contacts the drop and vaporizes the water, while a vapor film is formed on the superhydrophobic surrounding to jet vapor and reduce heat transfer. Furthermore, we reveal the general principle between the pattern symmetry design and the drop dynamics. This finding provides new insights into the Leidenfrost dynamics modulation, and opens a promising avenue for vapor-driven miniature devices.

Volatile Dual-Solvent Assisted Intermediate Phase Regulation for Anti-Solvent-Free Perovskite Photovoltaics.

The unprecedented development of perovskite solar cells (PSCs) makes them one of the most promising candidates for terawatt-scale green energy production with low cost. However, the high boiling point solvents during the solution-processed film deposition cause anisotropic crystal growth and toxic solvent vapor during high-throughput manufacturing. Here, a dual-component green solvent consisting of isopropyl acetate and acetonitrile is proposed to form a volatile perovskite precursor, which can realize the high-quality perovskite thin film deposition by intermediate phase regulation. A room-temperature stable perovskite intermediate phase is constructed with the engagement of isopropyl acetate as co-solvent, which suppresses the exploding nucleation rate in volatile perovskite precursor, providing a fine grain growth rate and wide processing window in scalable film deposition. The corresponding PSCs fabricated by blade coating without anti-solvents or gas quenching achieve power conversion efficiency (PCE) of 16.37 % and 15.29 % for the areas of 14.08 cm2 and 37.83 cm2 , respectively.

Nonpolar Solvent Modulated Inkjet Printing of Nanoparticle Self-Assembly Morphologies.

Patterning of luminescent nanomaterials is critical in the fields of display and information encryption, and inkjet printing technology have shown remarkable significance with the advantage of fast, large-scalable and integrative. However, inkjet printing nanoparticle deposits with high-resolution and well controlled morphology from nonpolar solvent droplets is still challenging. Herein, a facile approach of nonpolar solvent modulated inkjet printing of nanoparticles self-assembly patterns driven by the shrinkage of the droplet and inner solutal convection is proposed. Through regulating the solvent composition and nanoparticle concentration, multicolor light-emissive upconversion nanoparticle self-assembly microarrays with tunable morphologies are achieved, showing the integration of designable microscale morphologies and photoluminescences for multimodal anti-counterfeit. Furthermore, inkjet printing of nanoparticles self-assembled continuous lines with adjustable morphologies by controlling the coalescence and drying of the ink droplets is achieved. The high resolution of inkjet printing microarrays and continuous lines' width < 5 and 10 µm is realized, respectively. This nonpolar solvent-modulated inkjet printing of nanoparticle deposits approach facilitates the patterning and integration of different nanomaterials, and is expected to provide a versatile platform for fabricating advanced devices applied in photonics integration, micro-LED, and near-field display.

Humidity-Controlled Molecular Assembly and Photoisomerization Behavior with a Bubble-Assisted Patterning Approach.

Precise control of molecular assembly is of great significance in the application of functional molecules. This work has systematically investigated the humidity effect in bubble-assisted molecular assembly. This work finds humidity is critical in the evolution of the soft confined space, leading to the formation of microscale liquid confined space under high humidity, and nanoscale liquid confined space under low humidity. It is also revealed that the differences in surface wettability and adhesion play the key role. Consequently, a flat pattern with thermodynamically favorable ordered structure and a sharp pattern with dynamically favorable disordered structure are achieved, which show different solid-state photoisomerization behaviors and photoresponsiveness. Interestingly, conductivity of sharp pattern with disordered structure is higher than that of flat pattern with layered ordered structure due to electronic transport mechanism of different spatial dimensions. This work opens a new way for manipulating the molecular self-assembly to control the morphology and function of molecular patterns.

Regulation of Quantum Wells Width Distribution in Quasi-2D Perovskite Films for High-Performance Photodetectors.

Dynamic optimization of the quantum-well (QW) width distribution in quasi-2D halide perovskite thin films is an effective approach for tuning the properties of photoelectric devices. Here, that the QWs width distribution in quasi-2D perovskite films can be controlled only by using hydroiodic acid (HI) as an additive is demonstrated. A uniform distribution of the colloidal particle size in the quasi-2D perovskite precursor solution is achieved through the formation of soluble iodoplumbate coordination complexes, PbI3 - from the reaction of HI with PbI2 , resulting in an improved phase purity in the final film. Density functional theory calculations indicate that the ideal n value quasi-2D perovskite reaction pathway through the PbI3 - complex has a lower enthalpy of formation than the random nucleation pathway without the HI additive. Benefiting from this merit, a high-quality quasi-2D perovskite film with optimized phase purity delivered a balanced carrier diffusion length and improved carrier mobility. The resultant photodetectors exhibited a light on/off ratio of 50 000, a responsivity of 0.96 A W-1 , and a detectivity of 5.7 × 1012 Jones at 532 nm. In addition, the state-of-the-art device maintained more than 80% of its initial photocurrent after 720 h of storage at 30% relative humidity.