Search

Passive daytime radiative cooling (PDRC) textiles hold substantial potential for localized outdoor cooling of the human body without additional energy consumption, but their limited multifunctional integration severely hinders their practical application. Herein, aluminum-doped zinc oxide (AZO) nanoparticles were purposefully introduced into poly(vinylidene fluoride) (PVDF) nanofibers via a facile electrospinning process, forming a large-scale and flexible PDRC textile with the desired antibacterial, UV-shielding, and self-cleaning capabilities. These prepared PDRC textiles present a weighted sunlight reflection rate of 92.3% and a weighted emissivity of 89.5% in the mid-infrared region. Furthermore, outdoor tests with an average solar intensity of ∼715 W/m 2 demonstrated that a skin simulator temperature could be cooled by ∼16.1 °C below the ambient temperature, outperforming cotton fabric by ∼6.3 °C. Owing to the outstanding photocatalytic properties of the AZO nanoparticles, these prepared PVDF textiles exhibit antibacterial properties ( Escherichia coli : 99.99%), UV-shielding performance (UPF > 50 + ), and superior self-cleaning capabilities, providing a cost-effective and eco-friendly avenue for daytime personal thermal management.

Smart materials demonstrate fascinating responses to environmental physical/chemical stimuli, including thermal, photonic, electronic, humidity, or magnetic stimuli, which have attracted intensive interest in material chemistry. However, their limited/harsh stimuli-responsive behavior or sophisticated postprocessing leads to enormous challenges for practical applications. Herein, we rationally designed and synthesized thermochromic Ni(II) organometallic [(C 2 H 5 ) 2 NH 2 ] 2 NiCl 4- x Br x via a facile mechanochemical strategy, which demonstrated a reversible switch from yellow to blue color with a tunable phase-transition temperature from 75.6 to 61.7 °C. The simple electrospinning technology was applied to fabricate thermochromic Ni(II) organometallic-based nanofiber membranes for temperature monitoring. Furthermore, the organic charge-transfer cocrystal with a wide spectral absorption of 300-1950 nm and a high-efficiency photothermal conversion was combined with thermochromic Ni(II) organometallics for the desired dual-stimuli photo/thermochromism. This work supplies a new strategy for realizing multiple stimuli-responsive applications, such as thermal/light sensor displays and information storage.

Flexible hydroelectric generators (HEGs) are promising self-powered devices that spontaneously derive electrical power from moisture. However, achieving the desired compatibility between a continuous operating voltage and superior current density remains a significant challenge. Herein, a textile-based van der Waals heterostructure is rationally designed between conductive 1T phase tungsten disulfide@carbonized silk (1T-WS 2 @CSilk) and carbon black@cotton (CB@Cotton) fabrics with an asymmetric distribution of oxygen-containing functional groups, which enhances the proton concentration gradients toward high-performance wearable HEGs. The vertically staggered 1T-WS 2 nanosheet arrays on the CSilk fabric provide abundant hydrophilic nanochannels for rapid carrier transport. Furthermore, the moisture-induced primary battery formed between the active aluminum (Al) electrode and the conductive textiles introduces the desired electric field to facilitate charge separation and compensate for the decreased streaming potential. These devices exhibit a power density of 21.6 µW cm -2 , an open-circuit voltage (V oc ) of 0.65 V sustained for over 10 000 s, and a current density of 0.17 mA cm -2 . This performance makes them capable of supplying power to commercial electronics and human respiratory monitoring. This study presents a promising strategy for the refined design of wearable electronics., (© 2024 Wiley‐VCH GmbH.)

Organic heterostructures (OHTs) with the desired geometry organization on micro/nanoscale have undergone rapid progress in nanoscience and nanotechnology. However, it is a significant challenge to elucidate the epitaxial-growth process for various OHTs composed of organic units with a lattice mismatching ratio of > 3%, which is unimaginable for inorganic heterostructures. Herein, we have demonstrated a vivid visualization of the morphology evolution of epitaxial-growth based on a doped interfacial-layer, which facilitates the comprehensive understanding of the hierarchical self-assembly of core-shell OHT with precise spatial configuration. Significantly, the barcoded OHT with periodic shells obviously illustrate the shell epitaxial-growth from tips to center parts along the seeded rods for forming the core-shell OHT. Furthermore, the diameter, length, and number of periodic shells were modulated by finely tuning the stoichiometric ratio, crystalline time, and temperature, respectively. This epitaxial-growth process could be generalized to organic systems with facile chemical/structural compatibility for forming the desired OHTs., (© 2024. The Author(s).)

Flexible moisture-electric generators (MEGs) capture chemical energy from atmospheric moisture for sustainable electricity, gaining attention in wearable electronics. However, challenges persist in the large-scale integration and miniaturization of MEGs for long-term, high-power output. Herein, a vertical heterogeneous phase-engineering MoS 2 nanosheet structure based silk and cotton were rationally designed and successfully applied to construct wearable MEGs for moisture-energy conversion. The prepared METs exhibit ∼0.8 V open-circuit voltage, ∼0.27 mA/cm 2 current density for >10 h, and >36.12 μW/cm 2 peak output power density, 3 orders higher than current standards. And the large-scale device realizes a current output of 0.145 A. An internal phase gradient between the 2H semiconductor MoS 2 in carbonized silks and 1T metallic MoS 2 in cotton fibers enables a phase-engineering-based heterogeneous electric double layer functioning as an equivalent parallel circuit, leading to enhanced high-power output. Owing to their facile customization for seamless adaptation to the human body, we envision exciting possibilities for these wearable METs as integrated self-power sources, enabling real-time monitoring of physiological parameters in wearable electronics.

Harvesting sunlight into cost-effective electricity presents an enticing prospect for self-powered wearable applications. The photothermal materials with an extensive absorption are fundamental to achieve optical and thermal concentration of the sunlight for efficiency output electricity of wearable solar thermoelectric generators (STEGs). Here, we synthesize an organic charge-transfer (CT) cocrystal with a flat absorption from ultraviolet to second near-infrared region (200 to 1950 nanometers) and a high photothermal conversion efficiency (PCE) of 80.5%, which is introduced into polyurethane toward large-area nanofiber membrane by electrospinning technology. These corresponding membranes demonstrate a high PCE of 73.7% under the strain more than 80%. Sandwiched with carbon nanotube-based thermoelectric fibers, the membranes as stretchable solar absorbers of STEGs could supply a notably increase temperature gradient, processing a maximum output voltage density of 23.4 volts per square meter at 1:00 p.m. under sunlight. This strategy presents an important insight in heat management for wearable STEGs with a desired electricity output.

Organic multilayer heterostructures with accurate spatial organization demonstrate strong light-matter interaction from excitonic responses and efficient carrier transfer across heterojunction interfaces, which are considered as promising candidates toward advanced optoelectronics. However, the precise regulation of the heterojunction surface area for finely adjusting exciton conversion and energy transfer is still formidable. Herein, organic bilayer heterostructures (OBHs) with controlled face-to-face heterojunction via a stepwise seeded growth strategy, which is favorable for efficient exciton propagation and conversion of optical interconnects are designed and synthesized. Notably, the relative position and overlap length ratio of component microwires (L DSA /L BPEA = 0.39-1.15) in OBHs are accurately regulated by modulating the crystallization time of seeded crystals, resulting into a tailored heterojunction surface area (R = L overlap /L BPEA = 37.6%-65.3%). These as-prepared OBHs present the excitation position-dependent waveguide behaviors for optical outcoupling characteristics with tunable emission colors and intensities, which are applied into two-dimensional (2D) photonic barcodes. This strategy opens a versatile avenue to purposely design OBHs with tailored heterojunctions for efficient energy transfer and exciton conversion, facilitating the application possibilities of advanced integrated optoelectronics., (© 2023 Wiley-VCH GmbH.)

Desalination and power generation through solar energy harvesting is a crucial technology that can effectively address freshwater shortages and energy crises. However, owing to the complexity of the actual water environment, the thermal output capability of the photothermal material and the functional integration of the evaporation system need urgent improvement, to obtain high-quality fresh water and sufficient electricity. Herein, a 2D/2D cesium tungsten bronze/copper sulfide (2D/2D Cs 0.32 WO 3 /CuS) nano-heterojunction is developed and it is loaded into a cellulose-based hybrid hydrogel to construct a multifunctional evaporator. Benefiting from the more nonradiative recombination centers from deep-level defects, as well as shorter carrier migration distances and higher redox potentials in the Cs 0.32 WO 3 /CuS nano-heterojunction, this evaporator has a significant improvement in thermal output capacity, enabling both super-efficient seawater evaporation (4.22 kg m -2 h -1 ) and photodegradation of organic pollutants (removal rate ≈ 99%). Moreover, the evaporator exhibits long-term stability and sustainable self-cleaning property against salt accumulation. Remarkably, the thermoelectric module based on the Cs 0.32 WO 3 /CuS nano-heterojunction shows promising electricity generation performance (4.85 W m -2 ), which can power small appliances durably and stably, exceeding previously reported similar devices. This 2D/2D heterojunction-based solar evaporation system will provide a more reliable solution for efficient and sustainable freshwater-electricity co-generation in resource-limited areas., (© 2023 Wiley-VCH GmbH.)

Thermochromic smart windows with rational modulation in indoor temperature and brightness draw considerable interest in reducing building energy consumption, which remains a huge challenge to meet the comfortable responsive temperature and the wide transmittance modulation range from visible to near-infrared (NIR) light for their practical application. Herein, a novel thermochromic Ni(II) organometallic of [(C 2 H 5 ) 2 NH 2 ] 2 NiCl 4 for smart windows is rationally designed and synthesized via an inexpensive mechanochemistry method, which processes a low phase-transition temperature of 46.3 °C for the reversible color evolution from transparent to blue with a tunable visible transmittance from 90.5% to 72.1%. Furthermore, cesium tungsten bronze (CWO) and antimony tin oxide (ATO) with excellent NIR absorption in 750-1500 and 1500-2600 nm are introduced in the [(C 2 H 5 ) 2 NH 2 ] 2 NiCl 4 -based smart windows, realizing a broadband sunlight modulation of a 27% visible light modulation and more than 90% of NIR shielding ability. Impressively, these smart windows demonstrate stable and reversible thermochromic cycles at room temperature. Compared with the conventional windows in the field tests, these smart windows can significantly reduce the indoor temperature by 16.1 °C, which is promising for next-generation energy-saving buildings., (© 2023 Wiley-VCH GmbH.)

Organic hierarchical branch micro/nanostructures constituted by single crystals with inherent multichannel characteristics exhibit superior potential in regulating photon transmission for photonic circuits. However, organic branch micro/nanostructures with precise branch positions are extremely difficult to achieve due to the randomness of the nucleation process. Herein, by taking advantage of the dislocation stress field-impurity interaction that solute molecules deposit preferentially along the dislocation line, twinning deformation was introduced into microcrystals to induce oriented nucleation sites, and ultimately organic branch microstructures with controllable branch sites were fabricated. The growth mechanism of these controllable single crystals with an angle of 140° between trunk and branch is attributed to the low lattice mismatching ratio (η) of 4.8%. These as-prepared hierarchical branch single crystals with asymmetrical optical waveguide characteristics have been demonstrated as an optical logic gate with multiple input/out channels, which provides a route to command the nucleation sites and offers potential applications in the organic optoelectronics at the micro/nanoscale.

Organic photothermal cocrystals, integrating the advantages of intrinsic organic cocrystals and the fascinating photothermal conversion ability, hold attracted considerable interest in both basic science and practical applications, involving photoacoustic imaging, seawater desalination, and photothermal therapy, and so on. However, these organic photothermal cocrystals currently suffer individual cases discovered step by step, as well as the deep and systemic investigation in the corresponding photothermal conversion mechanisms is rarely carried out, suggesting a huge challenge for their further developments. Therefore, it is urgently necessary to investigate and explore the rational design and synthesis of high-performance organic photothermal cocrystals for future applications. This review first and systematically summarizes the organic photothermal cocrystal in terms of molecular classification, the photothermal conversion mechanism, and their corresponding applications. The timely interpretation of the cocrystal photothermal effect will provide broad prospects for the purposeful fabrication of excellent organic photothermal cocrystals toward great efficiency, low cost, and multifunctionality., (© 2023 The Authors. Advanced Science published by Wiley-VCH GmbH.)

Multifunctional and long-term stable wearable heating systems have attracted extensive attention from experts, yet smart textiles that only rely on harvesting the body's heat without additional energy still face huge challenges in practical applications. Herein, we rationally prepared the monolayer MXene Ti 3 C 2 T x nanosheets via an in situ hydrofluoric acid generation method, which was further employed to construct a wearable heating system of MXene @ polyester polyurethane blend fabrics (MP textile) for the passive personal thermal management through a simple spraying process. Owing to the unique two-dimensional (2D) structure, the MP textile presents the desired mid-infrared emissivity, which could efficiently suppress the thermal radiation loss from the human body. Notably, the MP textile with an MXene concentration of 28 mg/mL exhibits a low mid-infrared emissivity of 19.53% at 7-14 μm. Significantly, these prepared MP textiles demonstrate an enhanced temperature of more than 6.83 °C compared with those of favorably traditional fabrics, involving the black polyester fabric, pristine polyester polyurethane blend fabric (PU/PET), and cotton, suggesting a charming indoor passive radiative heating performance. The temperature of real human skin covered by MP textile is 2.68 °C higher than that covered by cotton fabric. Impressively, these prepared MP textiles simultaneously possess attractive breathability, moisture permeability, mechanical strength, and washability, which provide new insight into human body temperature regulation and physical health.

Highly spatial and angular precision in epitaxial-growth process is crucial for constructing organic low-dimensional heterostructures (OLDHs) with the desired substructures, which remains significant challenge owing to the unpredicted location of complex heterogeneous nucleation. Herein, a dynamic epitaxial-growth approach is developed along the tailored longitudinal/horizontal directions to create diverse OLDHs with hierarchical architectures. The controlled morphology evolution of seed crystals from kinetic to thermodynamic species is achieved via incrementally increasing the crystallization time from 0 to 600 s. Accordingly, the kinetic and thermodynamic seed crystals respectively present the specific lattice-matching crystal-planes of (100) and (011), which facilitates the longitudinal epitaxial-growth (LG) process for triblock heterostructures, and the horizontal epitaxial-growth (HG) process for axial-branch heterostructures. The dominant core/shell heterostructures are prepared via both LG and HG processes with a crystallization time of ≈30 s. Significantly, these prepared OLDHs realize the rationally polarized exciton conversion for optical logic gate application through the exciton conversion and photon propagation at the heterojunction. This strategy provides an avenue for the precise synthesis of OLDHs with anisotropy optical characters for integrated optoelectronics., (© 2022 Wiley-VCH GmbH.)

Organic photothermal materials integrating a high-efficiency light-heat conversion effect and high flexibility have generated immense interest in fundamental research and practical applications. Nevertheless, their practical applications still remain a challenge, owing to the complicated design, tedious synthesis, and limited programmable substrates. Herein, an organic charge-transfer cocrystal with a narrow energy gap of 0.33 eV and a high photothermal conversion efficiency (PCE) of 69.3% was rationally designed and synthesized via a facile self-assembly process, which was introduced into polyurethane for forming a large-area photothermal nanofiber membrane via electrospinning technology. Femtosecond transient absorption spectroscopy elucidates that the excellent PCE is attributed to the nonradiation transition process, including internal conversion and charge dissociation processes. Furthermore, the temperature of the as-prepared photothermal nanofiber membrane could quickly rise to 52 °C under laser irradiation with a power density of 0.183 W/cm 2 , suggesting a high PCE of 53.7%. This work successfully achieves the fabrication of a large-area photothermal membrane and the development of photothermal imaging.

Organic heterostructure nanowires, such as multiblock, core/shell, branch-like and related compounds, have attracted chemists' extensive attention because of their novel physicochemical properties. However, owing to the difficulty in solving the lattice mismatch of distinct molecules, the construction of organic heterostructures at large scale remains challenging, which restricts its wide use in future applications. In this work, we define a concept of lattice-mismatch-free for hierarchical self-assembly of organic semiconductor molecules, allowing for the large-scale synthesis of organic heterostructure nanowires composed of the organic alloys and cocrystals. Thus, various types of organic triblock nanowires are prepared in large scale, and the length ratio of different segments of the triblock nanowires can be precisely regulated by changing the stoichiometric ratio of different components. These results pave the way towards fine synthesis of heterostructures in a large scale and facilitate their applications in organic optoelectronics at micro/nanoscale., (© 2022. The Author(s).)

Optical interconnects exhibit superior potential in the precise regulation of photon transmission for organic photonic circuits. However, the rational design of well-defined organic heterostructures toward active optoelectronics remains challenging. Herein, we designed organic branched heterostructures (OBHs) with accurate spatial organization for optical interconnection. Notably, the precise regulation of OBHs has been controllably achieved including the trunk morphologies and the branched microwire number. Significantly, these as-prepared OBHs inherently exhibit the multichannel coupling outputs and the excitation position-dependent waveguide characteristics, leading to various outcoupling signals with tunable intensity and emission colors. The optical interconnects are realized due to the occurrence of exciton conversion and photon propagation between branch and trunk at the heterojunction, benefiting the application possibilities of two-dimensional (2D) optical barcodes., (© 2022 Wiley-VCH GmbH.)

Harvesting the narrow bandgap excitons of charge-transfer (CT) complexes for the achievement of near-infrared (NIR) emission has attracted intensive attention for its fundamental importance and practical application. Herein, the triphenylene (TP)-2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F 4 TCNQ) CT organic complex is designed and fabricated via the supramolecular self-assembly process, which demonstrates the NIR emission with a maximum peak of 770 nm and a photoluminescence quantum yield (PLQY) of 5.4%. The segregated stacking mode of TP-F 4 TCNQ CT complex based on the multiple types of intermolecular interaction has a low CT degree of 0.00103 and a small counter pitch angle of 40° between F 4 TCNQ and TP molecules, which breaks the forbidden electronic transitions of CT state, resulting in the effective NIR emission. Acting as the promising candidates for the active optical waveguide in the NIR region beyond 760 nm, the self-assembled TP-F 4 TCNQ single-crystalline organic microwires display an ultralow optical-loss coefficient of 0.060 dB µm -1 . This work holds considerable insights for the exploration of novel NIR-emissive organic materials via an universal "cocrystal engineering" strategy., (© 2022 Wiley-VCH GmbH.)

Two-dimensional transition metal dichalcogenides are of particular interest in high-performance photothermal conversion, yet there remains a huge challenge in their practical application in smart textiles for healthcare, energy, and personal protection. Herein, we controllably prepared MoS 2 hollow nanospheres with a high photothermal conversion efficiency of 36% via a microemulsion-hydrothermal method, which was further applied to construct photothermal fibers for personal thermal management after a hot-blast dip-drying process. Because of the prominent photothermal effect, the temperature of the photothermal fibers sharply increases from the room temperature value of 25.0 to 55.5 °C in 60 s under near-infrared illumination with a power density of 500 W/cm 2 . Furthermore, the photothermal fiber pad demonstrated an obvious temperature enhancement of 38.0 °C from a skin temperature of 22.0 °C after it was irradiated by natural sunlight for 60 s. Significantly, the antibacterial elimination rates of the photothermal fibers for Escherichia coli and Staphylococcus aureus are ∼99.9 and ∼99.8%, respectively. This strategy affords an avenue toward the practical application of photothermal materials in smart fibers for personal thermoregulation.

White-light-emissive organic micro/nanostructures hold exotic potential applications in full-color displays, on-chip wavelength-division multiplexing, and backlights of portable display devices, but are rarely realized in organic core/shell heterostructures. Herein, through regulating the noncovalent interactions between organic semiconductor molecules, a hierarchical self-assembly approach of horizontal epitaxial-growth is demonstrated for the fine synthesis of organic core/mono-shell microwires with multicolor emission (red-green, red-blue, and green-blue) and especially organic core/double-shell microwires with radial red-green-blue (RGB) emission, whose components are dibenzo[g,p]chrysene (DgpC)-based charge-transfer (CT) complexes. In fact, the desired lattice mismatching (≈2%) and the excellent structure compatibility of these CT complexes facilitate the epitaxial-growth process for the facile synthesis of organic core/shell microwires. With the RGB-emissive substructures, these core/double-shell organic microwires are microscale white-light sources (CIE [0.34, 0.36]). Besides, the white-emissive core/double-shell microwires demonstrate the fascinating full-spectrum light transportation from 400 to 700 nm. This work indeed opens up a novel avenue for the accurate construction of organic core/shell heterostructures, which provides an attractive platform for the organic integrated optoelectronics., (© 2021 Wiley-VCH GmbH.)

Rationally designing and precisely constructing the dimensions, configurations and compositions of organic nanomaterials are key issues in material chemistry. Nevertheless, the precise synthesis of organic heterostructure nanomaterials remains challenging owing to the difficulty of manipulating the homogeneous/heterogeneous-nucleation process and the complex epitaxial relationships of combinations of dissimilar materials. Herein, we propose a hierarchical epitaxial-growth approach with the combination of longitudinal and horizontal epitaxial-growth modes for the design and synthesis of a variety of organic superstructure microwires with accurate spatial organisation by regulating the heterogeneous-nucleation crystallisation process. The lattice-matched longitudinal and horizontal epitaxial-growth modes are separately employed to construct the primary organic core/shell and segmented heterostructure microwires. Significantly, these primary organic core/shell and segmented microwires are further applied to construct the core/shell-segmented and segmented-core/shell type's organic superstructure microwires through the implementation of multiple spatial epitaxial-growth modes. This strategy can be generalised to all organic microwires with tailored multiple substructures, which affords an avenue to manipulate their physical/chemical features for various applications.

Near-infrared (NIR) organic solid-state lasers play an essential role in applications ranging from laser communication to infrared night vision, but progress in this area is restricted by the lack of effective excited-state gain processes. Herein, we originally proposed and demonstrated the cascaded occurrence of excited-state intramolecular proton transfer for constructing the completely new energy-level systems. Cascading by the first ultrafast proton transfer of <430 fs and the subsequent irreversible second proton transfer of ca. 1.6 ps, the stepwise proton transfer process favors the true six-level photophysical cycle, which supports efficient population inversion and thus NIR single-mode lasing at 854 nm. This work realizes longest wavelength beyond 850 nm of organic single-crystal lasing to date and originally exploits the cascaded excited-state molecular proton transfer energy-level systems for organic solid-state lasers., (© 2021 Wiley-VCH GmbH.)

The rational design and the fine synthesis of organic heterostructures (OHSs) are the key steps toward integrated organic optoelectronics. Herein we have demonstrated a self-assembly approach of combining a molecular-level heterostructure with a structural-level heterostructure and regulating the noncovalent intermolecular interactions for the precise construction of OHSs: a vertical type of anthracene-TCNB heterostructure and a horizontal type of benzopyrene-TCNB heterostructure. The excellent structural compatibility and the low lattice mismatch rate of ∼5.8% between single-component microplates and cocrystal microwires allow anthracene and benzopyrene molecules to grow epitaxially on the cocrystal. Significantly, integrating the multicolor emission and the distinctive dimensional-dependent photon transportation properties of low-dimensional micro/nanostructures, the multicolor optical outputs are achieved via modulating the active/passive optical waveguides in OHSs. Our work exhibits the utilization of the multilevel heterostructure strategy, which boosts the rational design of OHSs for organic photonics.

The realization of high-performance optoelectronic devices requires excellent charge-transporting layers and efficient carrier recombination. Herein, we synthesized cesium tungsten bronze (Cs 0.32 WO 3 ) nanocrystals and utilized them as the hole-transporting material to fabricate all-inorganic perovskite light-emitting diodes (PeLEDs). Due to the excellent carrier balance characteristics via comparison between the hole-only device and electron-only device, the all-inorganic PeLEDs with CsPbBr 3 as the light-emitting layer present the maximum current efficiency of 31.51 cd/A and external quantum efficiency (EQE) of 8.48%, which are self-evidently enhanced compared with the PEDOT:PSS (14.78 cd/A, 4.03%) and WO 3 (24.75 cd/A, 6.18%) based devices. Considering the remarkably improved device performance, the proposed HTL of Cs 0.32 WO 3 is promising, acting as a favorable building block for high-efficiency light-emitting devices.

Organic-inorganic halide perovskite solar cells (PSCs) still suffer from stability issues which are caused by possible erosions from moisture, ultraviolet (UV) light, heat, and so forth. An electron-transporting layer (ETL), that is, TiO 2 , is a key component for state-of-the-art PSCs. However, UV-caused desorption of O 2- in TiO 2 would accelerate the degradation of PSCs. Herein, we explored perovskite oxide, NaTaO 3 , for the first time as an alternative ETL in PSCs. NaTaO 3 as an ETL can effectively avoid the damage from UV irradiation, inhibit the degradation of the perovskite layer, and improve the overall stability of the PSC. PSCs fabricated with NaTaO 3 yielded a power conversion efficiency (PCE) of 21.07% with a retention of more than 80% of this initial PCE after 240 min UV irradiation in air while the reference device with a PCE of 20.16% can only retain about 53% of its initial PCE after the same testing condition. The developed stable perovskite oxide material of NaTaO 3 provides the diversification of electron-selective contact for highly efficient and stable PSCs.

Organic heterostructures (OHSs) integrating the intrinsic heterostructure characters as well as the organic semiconductor properties have attracted intensive attention in material chemistry. However, the precise bottom-up synthesis of OHSs is still challenging owing to the general occurrence of homogeneous-nucleation and the difficult manipulation of noncovalent interactions. Herein, we present the rational synthesis of the longitudinally/horizontally-epitaxial growth of one-dimensional OHSs including triblock and core/shell nanowires with quantitatively-manipulated microstructure via a hierarchical self-assembly method by regulating the noncovalent interactions: hydrogen bond (-15.66 kcal mol -1 ) > halogen bond (-4.90 kcal mol -1 ) > π-π interaction (-0.09 kcal mol -1 ). In the facet-selective epitaxial growth strategy, the lattice-matching and the surface-interface energy balance respectively facilitate the realization of triblock and core/shell heterostructures. This hierarchical self-assembly approach opens up avenues to the fine synthesis of OHSs. We foresee application possibilities in integrated optoelectronics, such as the nanoscale multiple input/out optical logic gate with high-fidelity signal.

Solid-state lasers (SSLs) play an important role in developing optoelectronic devices, optical communication, and modern medicine fields. As compared with inorganic SSLs, the electrically pumped organic SSLs (OSSLs) still remain unrealized because of the high lasing threshold and low carrier mobility. Herein, we first demonstrate the laser action at ∼520 nm based on the self-assembled single-crystalline organic microribbons of the aggregation-induced emission (AIE) molecules of 1,4-bis(( E)-4-(1,2,2-triphenylvinyl)styryl)-2,5-dimethoxybenzene (TPDSB). Moreover, these as-prepared organic microribbons exhibit an effective optical waveguide with a low optical loss of 0.012 dB μm -1 , indicating good light confinement for laser resonator feedback. Impressively, the multiple mode and the single mode lasing are both achieved from individual organic microribbons, whose lasing threshold is as low as 653 nJ cm -2 . These "bottom-up" synthesized organic microribbons based on AIE-active molecules offer a new strategy for the realization of the ultralow threshold OSSLs, which would eventually contribute to the realization of electrically pumped OSSLs.

The core/shell micro-/nanostructures with versatility, tunability, stability, dispersibility, and biocompatibility are widely applied in optics, biomedicine, catalysis, and energy. Organic micro-/nanocrystals have significant applications in miniaturized optoelectronics because of their controllable self-assembly behavior, tunable optical properties, and tailor-made molecular structure. Nevertheless, the advanced organic core/shell micro-/nanostructures, which possess multifunctionality, flexibility, and higher compatibility, are rarely demonstrated because of the dynamic nature of molecular self-assembly and the complex epitaxial relationship of material combination. Herein, we demonstrate the one-dimensional organic core/shell micro-/nanostructures with component interchange, which originates from the 4,4'-((1 E,1' E)-(2,5-dimethoxy-1,4-phenylene)bis(ethene-2,1-diyl))dipyridine (DPEpe) single-crystal microrods or the DPEpe-HCl single-crystal microrods after a reversible protonation or deprotonation process. Notably, the DPEpe/DPEpe-HCl core/shell microrods display vivid visualizations of tunable emission color via an efficient energy-transfer process during the stepwise formation of a shell layer. More significantly, these DPEpe/DPEpe-HCl and DPEpe-HCl/DPEpe core/shell microrods cooperatively demonstrate the multicolor optical waveguide properties continuously adjusted from green [CIE (0.326, 0.570)], to yellow [CIE (0.516, 0.465)], and to red [CIE (0.614, 0.374)]. Our investigation provides a new strategy to fabricate the organic core/shell micro-/nanostructures, which can eventually contribute to the advanced organic optoelectronics at the micro-/nanoscale.

Full inorganic cesium lead halide perovskites (IOPs) are regarded as attractive candidates for light-emitting diodes (LEDs) by their excellent luminescent conversion. However, unsatisfactory efficiency and stability are still the main drawbacks that hinder the commercialization progress of perovskite LEDs (PeLEDs). Here, we report an extremely uniform and flat CsPbBr 3 film composing of self-assembly core-shell structured quantum dots (SCQDs) based on one-step precursor coating. The QDs size in the CsPbBr 3 film is around 4.5 nm (smaller than the Bohr radius), which significantly confines injected carriers and leads to a ultrahigh exciton binding energy ( E b ) of 198 meV. In addition, unfavorable surfacial defects are dramatically passivated by a thin surfacial-capping layer composed of long-chain ammonium groups (phenylalanine bromide, PPABr), resulting in an ultralow nonradiative recombination rate. Consequently, the CsPbBr 3 SCQDs film presents a high photoluminescence quantum yield (PLQY) of 85%. It enables the resulting green PeLEDs to deliver a recorded external quantum efficiency (EQE) over 15% with ideal operational stability. Furthermore, the developed CsPbBr 3 SCQDs film also demonstrates promising potential in multifunctional lighting sources such as flexible and smart devices.

Anisotropic organic molecular construction and packing are crucial for the optoelectronic properties of organic crystals. Two-dimensional (2D) organic crystals with regular morphology and good photon confinement are potentially suitable for a chip-scale planar photonics system. Herein, through the bottom-up process, 2D halogen-bonded DPEpe-F 4 DIB cocrystals were fabricated that exhibit an asymmetric optical waveguide with the optical-loss coefficients of R Backward =0.0346 dB μm -1 and R Forward =0.0894 dB μm -1 along the [010] crystal direction, which can be attributed to the unidirectional total internal reflection caused by the anisotropic molecular packing mode. Based on this crystal direction-oriented asymmetric photon transport, these as-prepared 2D cocrystals have been demonstrated as a microscale optical logic gate with multiple input/out channels, which will offer potential applications as the 2D optical component for the integrated organic photonics., (© 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Exploiting organic/inorganic hybrid perovskite solar cells (PSCs) with reduced Pb content is very important for developing environment-friendly photovoltaics. Utilizing of Pb-Sn alloying perovskite is considered as an efficient route to reduce the risk of ecosystem pollution. However, the trade-off between device performance and Sn substitution ratio due to the instability of Sn 2+ is a current dilemma. Here, for the first time, the highly efficient Pb-Sn-Cu ternary PSCs are reported by partial replacing of PbI 2 with SnI 2 and CuBr 2 . Sn 2+ substitution results in a redshift of the absorption onset, whereas worsens the film quality. Interestingly, Cu 2+ introduction can passivate the trap sites at the crystal boundaries of Pb-Sn perovskites effectively. Consequently, a power conversion efficiency as high as 21.08% in inverted planar Pb-Sn-Cu ternary PSCs is approached. The finding opens a new route toward the fabrication of high efficiency Pb-Sn alloying perovskite solar cells by Cu 2+ passivation., (© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The controlled fabrication of organic single-crystalline nanowires (OSCNWs) with a uniform diameter in the nanoscale via the bottom-up approach, which is just based on weak intermolecular interaction, is a great challenge. Herein, we utilize the synergy approach of the bottom-up and the top-down processes to fabricate OSCNWs with diameters of 120 ± 10 nm through stepwise evolution processes. Specifically, the evolution processes vary from the self-assembled organic micro-rods with a quadrangular pyramid-like end-structure bounded with {111}s and {11-1}s crystal planes to the "top-down" synthesized organic micro-rods with the flat cross-sectional {002}s plane, to the organic micro-tubes with a wall thickness of ∼115 nm, and finally to the organic nanowires. Notably, the anisotropic etching process caused by the protic solvent molecules (such as ethanol) is crucial for the evolution of the morphology throughout the whole top-down process. Therefore, our demonstration opens a new avenue for the controlled-fabrication of organic nanowires, and also contributes to the development of nanowire-based organic optoelectronics such as organic nanowire lasers.

Efficient electron-injection into the emitting layer (EML) plays a pivotal role in the fabrication of high performance blue quantum dot light-emitting diodes (QLEDs). Herein, we reduce the electron-transporting barrier at the ITO/ETL (electron-transporting layer) interface from 0.7 eV to 0.4 eV by spin-coating a polyethylenimine ethoxylated (PEIE) film (8 nm) on the ITO substrate. Meanwhile, the electron-injection barrier was reduced from 0.5 to 0.1 eV at the ETL/QD interface by employing the incorporation of PEIE (0.1 wt%) into a ZnO layer. These above two interfacial modifications jointly decrease the electron barrier and make the electron transportation easier. As a result, the optimized QLEDs with the 460 nm emission peak exhibit a maximum external quantum efficiency (EQE) of 7.85%, which is enhanced by 1.4 fold compared with the reference device (5.68%). It is demonstrated that the facile interfacial modification by the organic polymer PEIE contributes to the fabrication of high-efficiency blue QLEDs.

Organic semiconductor micro-/nanocrystals with regular shapes have been demonstrated for many applications, such as organic field-effect transistors, organic waveguide devices, organic solid-state lasers, and therefore are inherently ideal building blocks for the key circuits in the next generation of miniaturized optoelectronics. In the study, blue-emissive organic molecules of 1,4-bis(2-methylstyryl)benzene (o-MSB) can assemble into rectangular microcrystals at a large scale via the room-temperature solution-exchange method. Because of the Förster resonance energy transfer, the energy of the absorbed photons by the host matrix organic molecules of o-MSB can directly transfer to the dopant organic molecules of tetracene or 1,2:8,9-dibenzopentacene (DBP), which then emit visible photons in different colors from blue to green, and to yellow. More impressively, by modulating the doping molar ratios of DBP to o-MSB, bright white-emissive organic microcrystals with well-preserved rectangular morphology can be successfully achieved with a low doping ratio of 1.5%. These self-assembled organic semiconductor microcrystals with multicolor emissions can be the white-light sources for the integrated optical circuits at micro-/nanoscale., (© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)