Showing papers in "Materials horizons in 2022"

Heterointerface optimization in a covalent organic framework-on-MXene for high-performance capacitive deionization of oxygenated saline water.

Abstract: Capacitive deionization (CDI) provides a promising option for affordable freshwater while simultaneously storing energy, but its large-scale application is usually limited owing to the poor performance of conventional materials in natural (oxygenated) saline water. Herein, we report heterointerface optimization in a covalent organic framework (COF)-on-MXene heterostructure achieving a high CDI performance for desalination of oxygenated saline water. The 2D heterostructure with the optimal core-shell architecture inherits the high conductivity and reversible ion intercalation/deintercalation ability of MXene, and the hierarchical porous structure, large porosity, and extraordinary redox capacity of COFs. Thanks to the heterointerface optimization, the MXene@COF heterostructure exhibits a very stable cycling performance over 100 CDI cycles with a maximum NaCl adsorption capacity of 53.1 mg g-1 in oxygenated saline water, among the state-of-the-art values for CDI electrodes and also exceeding those of most MXene-based or 2D materials. This study highlights the importance of heterointerface optimization in MXene-organic 2D heterostructures to promote CDI of natural (oxygenated) saline water.

Printing fabrication of large-area non-fullerene organic solar cells

Abstract: Organic solar cells (OSCs) based on a bulk heterojunction structure exhibit inherent advantages, such as low cost, light weight, mechanical flexibility, and easy processing, and they are emerging as a potential renewable energy technology. However, most studies are focused on lab-scale, small-area ( 1 cm2) OSCs still exhibit considerable efficiency loss during upscaling from small-area to large-area, which is a big challenge. In recent years, along with the rapid development of high-performance non-fullerene acceptors, many researchers have focused on developing large-area non-fullerene-based devices and modules. There are three essential issues in upscaling OSCs from small-area to large-area: fabrication technology, equipment development, and device component processing strategy. In this review, the challenges and solutions in fabricating high-performance large-area OSCs are discussed in terms of the abovementioned three aspects. In addition, the recent progress of large-area OSCs based on non-fullerene electron acceptors is summarized.

Narrowband organic photodetectors - towards miniaturized, spectroscopic sensing.

Abstract: Omnipresent quality monitoring in food products, blood-oxygen measurement in lightweight conformal wrist bands, or data-driven automated industrial production: Innovation in many fields is being empowered by sensor technology. Specifically, organic photodetectors (OPDs) promise great advances due to their beneficial properties and low-cost production. Recent research has led to rapid improvement in all performance parameters of OPDs, which are now on-par or better than their inorganic counterparts, such as silicon or indium gallium arsenide photodetectors, in several aspects. In particular, it is possible to directly design OPDs for specific wavelengths. This makes expensive and bulky optical filters obsolete and allows for miniature detector devices. In this review, recent progress of such narrowband OPDs is systematically summarized covering all aspects from narrow-photo-absorbing materials to device architecture engineering. The recent challenges for narrowband OPDs, like achieving high responsivity, low dark current, high response speed, and good dynamic range are carefully addressed. Finally, application demonstrations covering broadband and narrowband OPDs are discussed. Importantly, several exciting research perspectives, which will stimulate further research on organic-semiconductor-based photodetectors, are pointed out at the very end of this review.

Design strategies for improving the crystallinity of covalent organic frameworks and conjugated polymers: a review

Abstract: Highly crystalline covalent organic frameworks (COFs) or conjugated polymers (CPs) are very important and highly desirable because these materials would display better performance in diverse devices and provide more structure–property related information. However, how to achieve highly crystalline or single-crystal COFs and CPs is very challenging. Recently, many research studies have demonstrated the possibility of enhancing the crystallinity of COFs and CPs. Thus, it is timely to offer an overview of the important progress in improving the crystallinity of COFs and CPs from the viewpoint of design strategies. These strategies include polycondensation reaction optimization, improving the planarity, fluorine substitution, side chain engineering, and so on. Furthermore, the challenges and perspectives are also discussed to promote the realization of highly crystalline or single-crystal COFs and CPs.

3D printing of artificial skin patches with bioactive and optically active polymer materials for anti-infection and augmenting wound repair.

Abstract: A printable ink composed of a photoactive cationic conjugated poly(phenylene vinylene) derivative (PPV) and gelatin/alginate/hyaluronic acid is developed for 3D printing artificial skin patches. This patch shows excellent photodynamic therapy-based anti-infection superiority and outstanding bioactivity to facilitate wound repair. This study contributes to design new conjugated polymer inks for manufacturing functional skin patches.

A bioinspired antibacterial and photothermal membrane for stable and durable clean water remediation.

Abstract: Solar-driven steam generation has been considered as a prevalent and sustainable approach to obtain clean fresh water. However, the presence of microorganisms in seawater may cause the biofouling and degradation of polymeric photothermal materials and clog the channels for water transportation, leading to a decrease in solar evaporation efficiency during long-term usage. Herein, we have reported a facile strategy to construct a robust cellulose membrane device coated by tobramycin-doped polydopamine nanoparticles (PDA/TOB@CA). The PDA/TOB@CA membrane not only exhibited synergistic antibacterial behaviors with long-term and sustained antibiotic release profiles, but also achieved a high water evaporation rate of 1.61 kg m-2 h-1 as well as an evaporation efficiency of >90%. More importantly, the high antibacterial activity endowed the PDA/TOB@CA membrane with superb durability for stable reuse over 20 cycles, even in microbe-rich environments. Therefore, we envision that this study could pave a new pathway towards the design and fabrication of robust antibacterial and photothermal materials for long-term and stable clean water production.

Regiospecific N-alkyl substitution tunes the molecular packing of high-performance non-fullerene acceptors

Abstract: The rapid development of non-fullerene acceptors (NFAs) with strong near-infrared absorption has led to remarkably enhanced short-circuit current density (Jsc) values in organic solar cells (OSCs). NFAs based on the benzotriazole (Bz) fused-ring π-core have great potential in delivering both high Jsc and decent open-circuit voltage values due to their strong intramolecular charge transfer with reasonably low energy loss. In this work, we have designed and synthesized a series of Bz-based NFAs, PN6SBO-4F, AN6SBO-4F and EHN6SEH-4F, via regiospecific N-alkyl engineering based on the high-performance NFA mBzS-4F that was reported previously. The molecular packing of mBzS-4F, AN6SBO-4F, and EHN6SEH-4F single crystals was analyzed using X-ray crystallography in order to provide a comprehensive understanding of the correlation between the molecular structure, the charge-transporting properties, and the solar cell performance. Compared with the typical honeycomb single-crystal structure of Y6 derivatives, these NFAs exhibit distinctly different molecular packing patterns. The strong interactions of terminal indanone groups in mBzS-4F and the J-aggregate-like packing in EHN6SEH-4F lead to the formation of ordered 3D networks in single-crystals with channels for efficient charge transport. Consequently, OSCs based on mBzS-4F and EHN6SEH-4F show efficient photon-to-current conversions, achieving the highest power conversion efficiency of 17.48% with a Jsc of 28.83 mA cm−2.

Design and synthesis of chromophores with enhanced electro-optic activities in both bulk and plasmonic–organic hybrid devices

Abstract: This study demonstrates enhancement of in-device electro-optic activity via a series of theory-inspired organic electro-optic (OEO) chromophores based on strong (diarylamino)phenyl electron donating moieties. These chromophores are tuned to minimize trade-offs between molecular hyperpolarizability and optical loss. Hyper-Rayleigh scattering (HRS) measurements demonstrate that these chromophores, herein described as BAH, show >2-fold improvement in β versus standard chromophores such as JRD1, and approach that of the recent BTP and BAY chromophore families. Electric field poled bulk devices of neat and binary BAH chromophores exhibited significantly enhanced EO coefficients (r33) and poling efficiencies (r33/Ep) compared with state-of-the-art chromophores such as JRD1. The neat BAH13 devices with charge blocking layers produced very large poling efficiencies of 11.6 ± 0.7 nm2 V−2 and maximum r33 value of 1100 ± 100 pm V−1 at 1310 nm on hafnium dioxide (HfO2). These results were comparable to that of our recently reported BAY1 but with much lower loss (extinction coefficient, k), and greatly exceeding that of other previously reported OEO compounds. 3 : 1 BAH-FD : BAH13 blends showed a poling efficiency of 6.7 ± 0.3 nm2 V−2 and an even greater reduction in k. 1 : 1 BAH-BB : BAH13 showed a higher poling efficiency of 8.4 ± 0.3 nm2 V−2, which is approximately a 2.5-fold enhancement in poling efficiency vs. JRD1. Neat BAH13 was evaluated in plasmonic–organic hybrid (POH) Mach–Zehnder modulators with a phase shifter length of 10 μm and slot widths of 80 and 105 nm. In-device BAH13 achieved a maximum r33 of 208 pm V−1 at 1550 nm, which is ∼1.7 times higher than JRD1 under equivalent conditions.

Facilitating the acidic oxygen reduction of Fe-N-C catalysts by fluorine-doping.

Abstract: As the alternatives to expensive Pt-based materials for the oxygen reduction reaction (ORR), iron/nitrogen co-doped carbon catalysts (FeNC) with dense FeNx active sites are promising candidates to promote the commercialization of proton exchange membrane fuel cells. Herein, we report a synthetic approach using perfluorotetradecanoic acid (PFTA)-modified metal–organic frameworks as precursors for the synthesis of fluorine-doped FeNC (F-FeNC) with improved ORR performance. The utilization of PFTA surfactants causes profound changes of the catalyst structure including F-doping into graphitic carbon, increased micropore surface area and Brunauer–Emmett–Teller (BET) surface area (up to 1085 m2 g−1), as well as dense FeNx sites. The F-FeNC catalyst exhibits an improved ORR activity with a high E1/2 of 0.83 V (VS. RHE) compared to the pristine FeNC material (E1/2 = 0.80 V). A fast decay occurs in the first 10 000 potential cycles for the F-FeNC catalyst, but high durability is still maintained up to another 50 000 cycles. Density functional theory calculations reveal that the strongly withdrawing fluorine atoms doped on the graphitic carbon can optimize the electronic structure of the FeNx active center and decrease the adsorption energy of ORR intermediates.

Aggregation-induced emission luminogen with excellent triplet-triplet upconversion efficiency for highly efficient non-doped blue organic light-emitting diodes.

Abstract: By combining aggregation-induced emission (AIE) effect and a triplet–triplet upconversion (TTU) process, a blue emitter with excellent photoluminescence quantum efficiency and high upconversion efficiency in the film state is developed, from which a highly efficient non-doped blue TTU organic light-emitting diode (TTU-OLED) was realized.

Substituent-dependent absorption and fluorescence properties of perylene bisimide radical anions and dianions.

Abstract: Perylene-3,4:9,10-bis(dicarboximides) (PBIs) rank among the most important functional dyes and organic semiconductors, but only recently have their radical anions and dianions attracted interest for a variety of applications. Here, we systematically elucidate the functional properties (redox, absorption, and emission) of five PBI anions and dianions bearing different bay-substituents attached to the chromophore core. Cyclic voltammetry measurements reveal the influence of the substituents ranging from electron-withdrawing cyano to electron-donating phenoxy groups on the oxidation and reduction potentials that relate to the HOMO and LUMO levels ranging from −7.07 eV to −6.05 eV and −5.01 eV to −4.05 eV, respectively. Spectroelectrochemical studies reveal a significant number of intense absorption bands in the NIR-spectral range (750–1400 nm) for the radical anions, whereas the dianionic species are characterized by similar spectra to those for the neutral dyes, however being bathochromically shifted and with increased molar extinction coefficients of approximately 100 000 M−1 cm−1. The increase of the transition dipole moment is up to 56% and accompanied by an almost cyanine-like red-shifted (by 300 nm) absorption spectrum for the most electron-poor tetracyanotetrachloro PBI. Whilst the outstanding fluorescence properties of the neutral PBIs are lost for the radical anions, an appreciable near-infrared (NIR) fluorescence with a quantum yield of up to 18% is revealed for the dianions by utilizing a custom-built flow-cell spectroelectrochemistry setup. Time-dependent density functional theory calculations help to assign the absorption bands to the respective electronic transitions.

Recent advances of metal telluride anodes for high-performance lithium/sodium-ion batteries.

Abstract: Metal tellurides (MTs) have emerged as highly promising candidate anode materials for state-of-the-art lithium-ion batteries (LIBs) and sodium ion batteries (SIBs). This is owing to the unique crystal structure, high intrinsic conductivity, and high trap density of such materials. The present work delivers a detailed discussion on the latest research and progress associated with the use of MTs for LIBs/SIBs with a focus on reaction mechanisms, challenges, electrochemical performance, and synthesis strategies. Further, the prospects and future development of MT anode materials are discussed in terms of strategies to overcome the existing limitations. This review provides both an in-depth understanding of MTs and provides the driving force for expanding research on MTs for energy storage and conversion applications.

Enhancing of broadband sound absorption through soft matter.

Abstract: This paper proposed a metamaterial design method that uses soft matter for constructing a unique soft acoustic boundary to effectively improve broadband sound absorption performance. Specifically, attaching a flexible polyvinyl chloride (PVC) gel layer with an elastic modulus as low as a few kilopascals and a thickness of a few millimeters to the inner wall of a cavity-type sound-absorbing metamaterial structure significantly improved the absorption performance of the composite structure in low-frequency broadband ranges. The sound absorption enhancement mechanism differed from those proposed in previous research. On the one hand, the soft PVC gel layer acted as a soft acoustic boundary, substantially reducing the sound speed and reflection and producing considerable elastic strain energy at the interface between two different media to improve the sound absorption performance. On the other hand, this PVC gel layer displayed extremely low stiffness and high damping, producing an abundance of plasmon-like resonance modes in low-frequency broadband ranges, achieving a resonance absorption effect. Since this sound absorption enhancement method did not require an increase in the external dimensions or a change in the structural parameters of the original absorber and achieved robust enhancement in a wide frequency band, it displayed potential application value in various engineering fields.

Biomimetic Janus photonic soft actuator with structural color self-reporting.

Abstract: Soft actuators with variable signal/color play an important role in the fields of targeted locomotion, artificial phototropism, drug screening, cargo transportation, and interactive sensing. The ability to achieve rapid response, large curvature, wide bending angle, and full-color display continues to be an unresolved challenge for artificial actuating materials. Inspired by the angle-dependent structural color of broad-tailed hummingbird and the Janus wettability of the lotus leaf, a Janus photonic soft actuator (JPSA) was fabricated by integrating an underwater super-oleophilic copper micro-nano array and oil-phobic inverse opal through a Laplace channel. The JPSA exhibits unidirectional permeability to underwater oil droplets. Attractively, with the combination of a swellable super-oleophilic surface and photonic crystals, JPSAs were endowed with oil-controlled reversible bending behavior with self-reporting angle-dependent color indication. We described for the first time the directional actuating mechanism induced by underwater oil unidirectional penetration and revealed the corresponding actuating kinetics and the inner-stress distribution/transfer by using structural color. As an extension of such theory, a rapid responsive JPSA with a wide bending angle and full-color self-reporting is further fabricated. This work provides an efficient strategy for oil directional transportation and separation in aqueous media and inspires the fabrication of a soft actuator/sensor with structural color self-reporting.

Boosting sluggish photocatalytic hydrogen evolution through piezo-stimulated polarization: a critical review.

Abstract: To address the growing energy demand, remarkable progress has been made in transferring the fossil fuel-based economy to hydrogen-based environmentally friendly photocatalytic technology. However, the sluggish production rate due to the quick charge recombination and slow diffusion process needs careful engineering to achieve the benchmark photocatalytic efficiency. Piezoelectric photocatalysis has emerged as a promising field in recent years due to its improved catalytic performance facilitated by a built-in electric field that promotes the effective separation of excitons when subjected to mechanical stimuli. This review discusses the recent progress in piezo-photocatalytic hydrogen evolution while elaborating on the mechanistic pathway, effect of piezo-polarization and various strategies adopted to improve piezo-photocatalytic activity. Moreover, our review systematically emphasizes the fundamentals of piezoelectricity and piezo-phototronics along with the operational mechanism for designing efficient piezoelectric photocatalysts. Finally, the summary and outlooks provide insight into the existing challenges and outline the future prospects and roadmap for the development of next-generation piezo-photocatalysts towards hydrogen evolution.

Rationally Designed Self-assembling DNA Biomolecules as a Defined Biomaterial for 3D Bioprinting

Abstract: DNA has excellent features such as the presence of functional and targeted molecular recognition motifs, tailorable, defined material source, multifunctionality, high–precision molecular self–assembly, synthetic preparation, hydrophilicity and outstanding biocompatibility. Due...

Designer DNA biomolecules as a defined biomaterial for 3D bioprinting applications.

Abstract: DNA has excellent features such as the presence of functional and targeted molecular recognition motifs, tailorability, multifunctionality, high-precision molecular self-assembly, hydrophilicity, and outstanding biocompatibility. Due to these remarkable features, DNA has emerged as a leading next-generation biomaterial of choice to make hydrogels by self-assembly. In recent times, novel routes for the chemical synthesis of DNA, advances in tailorable designs, and affordable production ways have made DNA as a building block material for various applications. These advanced features have made researchers continuously explore the interesting properties of pure and hybrid DNA for 3D bioprinting and other biomedical applications. This review article highlights the topical advancements in the use of DNA as an ideal bioink for the bioprinting of cell-laden three-dimensional tissue constructs for regenerative medicine applications. Various bioprinting techniques and emerging design approaches such as self-assembly, nucleotide sequence, enzymes, and production cost to use DNA as a bioink for bioprinting applications are described. In addition, various types and properties of DNA hydrogels such as stimuli responsiveness and mechanical properties are discussed. Further, recent progress in the applications of DNA in 3D bioprinting are emphasized. Finally, the current challenges and future perspectives of DNA hydrogels in 3D bioprinting and other biomedical applications are discussed.

A computational scheme for evaluating the phosphorescence quantum efficiency: applied to blue-emitting tetradentate Pt(II) complexes.

Abstract: Phosphorescent organic light-emitting diodes (PhOLEDs) are leading candidates for displays or lighting technologies. Recently, blue phosphorescent tetradentate Pt(II) complexes have been attracting extensive attention due to their high phosphorescence quantum efficiency and numerous chemical structures on account of flexible ligand frames and modifications. Using quantum chemistry coupled with our thermal vibration correlation function (TVCF) formalism, we investigated the triplet excited state energy surface and the decay processes involving both direct vibrational relaxation and minimum energy crossing point (MECP) via the transition state (3TS) to the ground state (S0) for 16 recently experimentally reported blue-emitting tetradentate Pt(II) emitters containing fused 5/6/6 metallocycles. We found that (i) in most cases, the direct vibrational relaxation deactivations dominated the triplet non-radiative decay because either the 3TS is too high or the MECP is not reachable. Hence, results from the TVCF formalism agreed well with the experiments for the phosphorescence quantum efficiency; (ii) only when both 3TS and MECP are low, for instance, for PtON1-oMe, deactivations via MECP dominated the triplet non-radiative decay.

Multifunctionally wearable monitoring with gelatin hydrogel electronics of liquid metals.

Abstract: Hydrogel-based flexible electronics have been of widespread interest in recent years. However, current hydrogel electronics have limitations, such as poor biocompatibility, non-reusability, low electrical response to deformation and being single-function. GelMA is a gelatin-based hydrogel that has been widely used in the biological field, such as in tissue repair and drug delivery. Could it be a good choice for high biocompatibility wearable electronics? Here, by controlling the replacement rate of amine and hydroxy functionalities, we made the common brittle GelMA into a highly stretchable hydrogel. And we report for the first time GelMA hydrogel electronics with liquid metals (LMGE), which could be fabricated by simply injecting liquid metals into the internal microchannels of the GelMA hydrogels (GelMA-30). With the unique biocompatibility, outstanding air and ion permeability, and great mechanical properties of GelMA-30, as well as the low toxicity, high conductivity and high rheology of liquid metals, LMGE can not only monitor movement changes and even the heartbeat of rats, but can also be used as a wireless monitor to supervise secretions produced during human exercise. The design of LMGE provides a general strategy for the manufacture of bio-flexible hydrogel electronics, which opens the way for the development of multi-functional biomimetic materials for integrated monitoring and repair for biomedical applications.

Electronic properties of metal halide perovskites and their interfaces: the basics.

Abstract: We have witnessed tremendous progress of metal halide perovskite (MHP)-based optoelectronic devices, especially in the field of photovoltaics. Despite intensive research in the past few years, questions still remain regarding their fundamental optoelectronic properties, among which the electronic properties exhibit an interplay of numerous phenomena that deserve serious scrutiny. In this Focus article, we aim to provide a contemporary understanding of the unique electronic properties that has been resolved by the community. First introducing some of the basic concepts established in semiconductor physics, the intrinsic and extrinsic electronic properties of the MHPs are disentangled and explained. With this, the complex interplay of interface-, dopant-, and surface state-induced electronic states in determining the electrostatic landscape in the material can be comprehended, and the energy level alignment in device architectures more reliably assessed.

Multi-photoresponsive triphenylethylene derivatives with photochromism, photodeformation and room temperature phosphorescence.

Abstract: A series of triphenylethylene derivatives exhibited multi-photoresponsive properties, including photochromism, photodeformation and room temperature phosphorescence (RTP), which are strongly related to molecular conformations and packing in the aggregated states. Accordingly, these properties can be subtly adjusted by substituents to the center double bond and/or peripheral phenyl moieties. The introduction of bromine atom was beneficial to photochromism and photodeformation properties as a result of the additional C–H⋯Br interactions and electron-withdrawing property. Also, it can promote the RTP effect via heavy atom effect, resulting in persistent afterglow lasting up to 150 min as detected by chemiluminescent imaging system.

Molecular bases for temperature sensitivity in supramolecular assemblies and their applications as thermoresponsive soft materials.

Abstract: Thermoresponsive supramolecular assemblies have been extensively explored in diverse formats, from injectable hydrogels to nanoscale carriers, for a variety of applications including drug delivery, tissue engineering and thermo-controlled catalysis. Understanding the molecular bases behind thermal sensitivity of materials is fundamentally important for the rational design of assemblies with optimal combination of properties and predictable tunability for specific applications. In this review, we summarize the recent advances in this area with a specific focus on the parameters and factors that influence thermoresponsive properties of soft materials. We summarize and analyze the effects of structures and architectures of molecules, hydrophilic and lipophilic balance, concentration, components and external additives upon the thermoresponsiveness of the corresponding molecular assemblies.

Crystalline tetra-aniline with chloride interactions towards a biocompatible supercapacitor.

Abstract: Recent advances in wearable and implantable electronics have increased the demand for biocompatible integrated energy storage systems. Conducting polymers, such as polyaniline (PANi), have been suggested as promising electrode materials for flexible biocompatible energy storage systems, based on their intrinsic structural flexibility and potential polymer chain compatibility with biological interfaces. However, due to structural disorder triggering insufficient electronic conductivity and moderate electrochemical stability, PANi still cannot fully satisfy the requirements for flexible and biocompatible energy storage systems. Herein, we report a biocompatible physiological electrolyte activated flexible supercapacitor encompassing crystalline tetra-aniline (c-TANi) as the active electrode material, which significantly enhances the specific capacitance and electrochemical cycling stability with chloride electrochemical interactions. The crystallization of TANi endows it with sufficient electronic conductivity (8.37 S cm-1) and a unique Cl- dominated redox charge storage mechanism. Notably, a fully self-healable and biocompatible supercapacitor has been assembled by incorporating polyethylene glycol (PEG) with c-TANi as a self-healable electrode and a ferric-ion cross-linked sodium polyacrylate (Fe3+-PANa)/0.9 wt% NaCl as a gel electrolyte. The as-prepared device exhibits a remarkable capacitance retention even after multiple cut/healing cycles. With these attractive features, the c-TANi electrode presents a promising approach to meeting the power requirements for wearable or implantable electronics.

Low-molecular-weight supramolecular adhesives based on non-covalent self-assembly of a small molecular gelator.

Abstract: Currently developed adhesives are overwhelmingly polymeric in nature. Herein, we highlight for the first time the potential of supramolecular eutectogels assembled from small molecules as robust low-molecular-weight (LMW) supramolecular adhesives in air, water and organic solvents, and under low temperatures. These supramolecular eutectogels were produced from commercial alkyl trimethyl ammonium bromide (CnTAB) in emerging deep eutectic solvents (DESs), which demonstrated rapid (∼2 min), robust, and tunable adhesion to both hydrophilic and hydrophobic surfaces at room temperature in air. Moreover, high adhesion performance was maintained even in liquid nitrogen (-196 °C), underwater, and in organic solvents. A study of the structure-property relationship of these adhesives and molecular dynamics (MD) simulations further clarified the assembly and adhesion mechanism of the C12TAB molecules in DESs. Compared with traditional polymer adhesives and several existing examples of LMW supramolecular adhesives with solvent-free dry network structures, the spontaneous self-assembly of LMW gelators in versatile DESs provides a new strategy for the facile construction of high-strength supramolecular adhesives with gel network structures for a diverse range of harsh environments.

Two-dimensional magnetic atomic crystals.

Abstract: Two-dimensional (2D) magnetic crystals show many fascinating physical properties and have potential device applications in many fields. In this paper, the preparation, physical properties and device applications of 2D magnetic atomic crystals are reviewed. First, three preparation methods are presented, including chemical vapor deposition (CVD) molecular beam epitaxy (MBE) and single-crystal exfoliation. Second, physical properties of 2D magnetic atomic crystals, including ferromagnetism, antiferromagnetism, magnetic regulation and anomalous Hall effect are presented. Third, the application of 2D magnetic atomic crystals in heterojunctions reluctance and other aspects are briefly introduced. Finally, the future development direction and possible challenges of 2D magnetic atomic crystals are briefly addressed.

Singlet Fission and Triplet Pair Recombination in Bipentacenes with a Twist

Abstract: We investigate triplet pair dynamics in pentacene dimers that have varying degrees of coplanarity (pentacene-pentacene twist angle). The fine-tuning of the twist angle was achieved by alternating connectivity at the 1-position or 2-positions of pentacene. This mix-and-match connectivity leads to tunable twist angles between the two covalently linked pentacenes. These twisted dimers allow us to investigate the subtle effects that the dihedral angle between the covalently linked pentacenes imparts on singlet fission and triplet pair recombination dynamics. We observe that as the dihedral angle between the two bonded pentacenes is increased, the rates of singlet fission decrease, while the accompanying decrease in triplet recombination rates is stark. Temperature-dependent transient optical studies combined with theoretical calculations show that the triplet pair recombination proceeds primarily through a direct multiexciton internal conversion process. Calculations further show that the significant decrease in recombination rates can be directly attributed to a corresponding decrease in the magnitude of the nonadiabatic coupling between the singlet multiexcitonic state and the ground state. These results highlight the importance of the twist angle in designing systems that exhibit rapid singlet fission, while maintaining long triplet pair lifetimes in pentacene dimers.

Lower limits for non-radiative recombination loss in organic donor/acceptor complexes

Abstract: Understanding the factors controlling radiative and non-radiative transition rates for charge transfer states in organic systems is important for applications ranging from organic photovoltaics (OPV) to lasers and LEDs. We explore the role of charge-transfer (CT) energetics, lifetimes, and photovoltaic properties in the limit of very slow non-radiative rates by using a model donor/acceptor system with photoluminescence dominated by thermally activated delayed fluorescence (TADF). This blend exhibits an extremely high photoluminescence quantum efficiency (PLQY = ∼22%) and comparatively long PL lifetime, while simultaneously yielding appreciable amounts of free charge generation (photocurrent external quantum efficiency EQE of 24%). In solar cells, this blend exhibits non-radiative voltage losses of only ∼0.1 V, among the lowest reported for an organic system. Notably, we find that the non-radiative decay rate, knr, is on the order of 105 s−1, approximately 4–5 orders of magnitude slower than typical OPV blends, thereby confirming that high radiative efficiency and low non-radiative voltage losses are achievable by reducing knr. Furthermore, despite the high radiative efficiency and already comparatively slow knr, we find that knr is nevertheless much faster than predicted by Marcus–Levich–Jortner two-state theory and we conclude that CT-local exciton (LE) hybridization is present. Our findings highlight that it is crucial to evaluate how radiative and non-radiative rates of the LE states individually influence the PLQY of charge-transfer states, rather than solely focusing on the PLQY of the LE. This conclusion will guide material selection in achieving low non-radiative voltage loss in organic solar cells and high luminescence efficiency in organic LEDs.

Two-photon absorption in halide perovskites and their applications.

Abstract: Active research on halide perovskites has given us a deep understanding of this family of materials and their potential for applications in advanced optoelectronic devices. One of the prominent outcomes is the use of perovskite materials for nonlinear optical applications. Two-photon absorption in perovskites, in particular their nanostructures, has been extensively studied and shows huge promise for many applications. However, we are still far from a thorough understanding of two-photon absorption in halide perovskites from a micro to macro perspective. Here we summarize different techniques for studying the two-photon absorption in nonlinear optical materials. We discuss the in-depth photophysics in two-photon absorption in halide perovskites. A comprehensive summary about the factors which influence two-photon absorption provides the direction to improve the two-photon absorption properties of halide perovskites. A summary of the recent applications of two-photon absorption in halide perovskites provides inspirations for engineers to utilize halide perovskites in two-photon absorption device development. This review will help readers to have a comprehensive and in-depth understanding of the research field of two-photon absorption of halide perovskites from microscopic mechanisms to applications. The article can serve as a manual and give inspiration for future researchers.

Suppressing singlet-triplet annihilation processes to achieve highly efficient deep-blue AIE-based OLEDs.

Abstract: Aggregation-induced emission (AIE) materials are attractive for the fabrication of high efficiency organic light-emitting diodes (OLEDs) by harnessing "hot excitons" from the high-lying triplet exciton states (Tn, n ≥ 2) and high photoluminescence (PL) quantum efficiency in solid films. However, the electroluminescence (EL) efficiency of most AIE-based OLEDs does not meet our expectation due to some unrevealed exciton loss processes. Herein, we further enhance the efficiency of blue AIE-based OLEDs, and find experimentally and theoretically that the serious exciton loss is caused by the quenching of radiative singlet excitons and long-lived triplet excitons [singlet-triplet annihilation (STA)]. In order to suppress the STA process, 1-(2,5-dimethyl-4-(1-pyrenyl)phenyl)pyrene (DMPPP) with triplet-triplet annihilation up-conversion was doped in two AIE emitters to reduce the triplet excitons on the lowest triplet excited state (T1) of AIE molecules. It can be seen that the external quantum efficiency (EQE) of the resulting blue OLEDs was enhanced to 11.8% with CIE coordinates of (0.15, 0.07) and a negligible efficiency roll-off, realizing the efficiency breakthrough of deep-blue AIE-based OLEDs. This work establishes a physical insight in revealing the exciton loss processes and the fabrication of high-performance AIE-based OLEDs.

Continuous-flow syntheses of alloy nanoparticles.

Abstract: Alloy nanoparticles (NPs), including core-shell, segregated and solid-solution types, show a variety of attractive properties such as catalytic and optical properties and are used in a wide range of applications. Precise control and good reproducibility in the syntheses of alloy NPs are highly demanded because these properties are tunable by controlling alloy structures, compositions, particle sizes, and so on. To improve the efficiency and reproducibility of their syntheses, continuous-flow syntheses with various types of reactors have recently been developed instead of the current mainstream approach, batch syntheses. In this review, we focus on the continuous-flow syntheses of alloy NPs and first overview the flow syntheses of NPs, especially of alloy NPs. Subsequently, the details of flow reactors and their chemistry to synthesize core-shell, segregated, solid-solution types of alloy NPs, and high-entropy alloy NPs are introduced. Finally, the challenges and future perspectives in this field are discussed.