Publications by authors named "Wenping Hu"

378 Publications

Organic Semiconductor Single Crystals for X-ray Imaging.

Adv Mater 2021 Sep 20:e2104749. Epub 2021 Sep 20.

Department of Chemistry & Biochemistry, University of California at Los Angeles, Los Angeles, CA 90095, USA.

Low-dose, high-resolution X-ray imaging is vital for medical diagnostics and material/device analyses. Current X-ray imagers are dominated by expensive inorganic materials via high-temperature solid processes (up to 1700 °C, e.g., CsI:Tl) with heavy metal elements. It is essential to search for new materials as X-ray imagers with low growth temperature, low cost, high sensitivity, along with high chemical and environmental stability. Here, 9,10-diphenylanthracene (9,10-DPA) single crystals are used as a representative model, which are grown via low-temperature solution processes, exhibiting intense X-ray radioluminescence with ultrahigh photon-conversion efficiency, ultrafast response and high sensitivity. The resolution of devices based on organic crystals exceeds 20.00 lp mm . Meanwhile the crystals exhibit high cycle performance under X-ray irradiation and environmental stability. This study demonstrates that organic semiconductors have potential use in low-cost, high-sensitivity and low-dose X-ray imaging systems.
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http://dx.doi.org/10.1002/adma.202104749DOI Listing
September 2021

Retraction: Polymer nanodots of graphitic carbon nitride as effective fluorescent probes for the detection of Fe and Cu ions.

Nanoscale 2021 Sep 23;13(36):15481. Epub 2021 Sep 23.

Beijing National Laboratory for Molecular Sciences, Key Laboratory of Organic Solids, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, PR China.

Retraction of 'Polymer nanodots of graphitic carbon nitride as effective fluorescent probes for the detection of Fe and Cu ions' by Shouwei Zhang , , 2014, , 4157-4162, DOI: 10.1039/C3NR06744K.
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http://dx.doi.org/10.1039/d1nr90195hDOI Listing
September 2021

When graphene meets white graphene - recent advances in the construction of graphene and h-BN heterostructures.

Nanoscale 2021 Aug 28;13(31):13174-13194. Epub 2021 Jul 28.

Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University and Collaborative Innovation Center of Chemical Science and Engineering, Tianjin, 300072 P. R. China.

2D heterostructures have very recently witnessed a boom in scientific and technological activities owing to the customized spatial orientation and tailored physical properties. A large amount of 2D heterostructures have been constructed on the basis of the combination of mechanical exfoliation and located transfer method, opening wide possibilities for designing novel hybrid systems with tuned structures, properties, and applications. Among the as-developed 2D heterostructures, in-plane graphene and h-BN heterostructures have drawn the most attention in the past few decades. The controllable synthesis, the investigation of properties, and the expansion of applications have been widely explored. Herein, the fabrication of graphene and h-BN heterostructures is mainly focused on. Then, the spatial configurations for the heterostructures are systematically probed to identify the highly related unique features. Moreover, as a most promising approach for the scaled production of 2D materials, the in situ CVD fabrication of the heterostructures is summarized, demonstrating a significant potential in the controllability of size, morphology, and quality. Further, the recent applications of the 2D heterostructures are discussed. Finally, the concerns and challenges are fully elucidated and a bright future has been envisioned.
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http://dx.doi.org/10.1039/d1nr03733aDOI Listing
August 2021

Dual-functional porous MOFs with hierarchical guest encapsulation for room-temperature phosphorescence and white-light-emission.

Nanoscale 2021 Aug 21;13(29):12466-12474. Epub 2021 Jul 21.

Department of Chemistry, School of Science & Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin University, Tianjin 300072, China.

The development of optical materials with room temperature phosphorescence (RTP) and white light emission (WLEDs) is highly desirable and remains a challenging task. Herein, a porous metal-organic framework PCN-921 with a high quantum yield (Φ = 93.6%) was achieved. To make full use of the advantages of the high porosity of PCN-921, we hierarchically encapsulated different guest molecules coronene and rhodamine B (RhB) into the framework. Unsurprisingly, the hybrid material [email protected] was obtained after in situ encapsulation of the guest coronene into the framework, and it exhibits obvious RTP behavior with a long phosphorescence lifetime of 62.5 ns. Subsequently, second guest RhB molecules were introduced after soaking in RhB solution and the material [email protected]@PCN-921 was achieved. Interestingly, it exhibits white light emission with the CIE coordinates of (0.29, 0.34), and can be used as a high performance WLED lamp. This is the first work on dual-functional hybrid [email protected] with hierarchical guest encapsulation for RTP and white light emission, which suggests the potential applications of MOFs in multifunctional optical devices.
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http://dx.doi.org/10.1039/d1nr03006jDOI Listing
August 2021

Inactivated influenza vaccine effectiveness among department of defense beneficiaries aged 6 months-17 years, 2016-2017 through 2019-2020 influenza seasons.

PLoS One 2021 27;16(8):e0256165. Epub 2021 Aug 27.

The Department of Defense Global Emerging Infections Surveillance Branch, Armed Forces Health Surveillance Division, WPAFB, OH, United States of America.

A test-negative case-control study was conducted to assess inactivated influenza vaccine effectiveness (VE) in children aged 6 months-17 years. The database was developed from the US Department of Defense Global Respiratory Pathogen Surveillance Program over four consecutive influenza seasons from 2016 to 2020. A total of 9,385 children including 4,063 medically attended, laboratory-confirmed influenza-positive cases were identified for VE analysis. A generalized linear mixed model with logit link and binomial distribution was used to estimate the VE. The adjusted VE for children was 42% [95% confidence interval (CI): 37-47%] overall, including 55% (95% CI: 47-61%) for influenza A(H1N1)pdm09, 37% (95% CI: 28-45%) for influenza A(H3N2), and 49% (95% CI: 41-55%) for influenza B. The analysis by age groups indicated that the adjusted VE in children aged 6 months-4 years was higher against influenza A(H1N1)pdm09 and influenza B, and comparable against influenza A(H3N2), compared to those in children aged 5-17 years. Further age-stratified analysis showed that the VE against any types of influenza was low and non-significant for children aged 6-11 months (33%; 95% CI:-2-56%), but it was high (54%; 95% CI: 34-67%) in children aged 12-23 months, and then declined linearly with increasing age. In conclusion, the inactivated influenza vaccination was moderately effective against influenza infection, based on the analysis from a large number of children aged 6 months-17 years over multiple influenza seasons.
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http://journals.plos.org/plosone/article?id=10.1371/journal.pone.0256165PLOS
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8397503PMC
August 2021

Organic Semiconductor Crystal Engineering for High-Resolution Layer-Controlled 2D Crystal Arrays.

Adv Mater 2021 Aug 20:e2104166. Epub 2021 Aug 20.

Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University & Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin, 300072, China.

2D organic semiconductor crystals (2DOSCs) have extraordinary charge transport capability, adjustable photoelectric properties, and superior flexibility, and have stimulated continuous research interest for next-generation electronic and optoelectronic applications. The prerequisite for achieving large-area and high-throughput optoelectronic device integration is to fabricate high-resolution 2DOSC arrays. Patterned substrate- and template-assisted self-assembly is an effective strategy to fabricate OSC arrays. However, the film thickness is difficult to control due to the complicated crystallization process during solvent evaporation. Therefore, the manufacturing of 2DOSC arrays with high-resolution and controllable molecular-layer numbers through solution-based patterning methods remains a challenge. Herein, a two-step strategy to produce high-resolution layer-controlled 2DOSC arrays is reported. First, large-scale 2DOSCs with well-defined layer numbers are obtained by a solution-processed organic semiconductor crystal engineering method. Next, the high-resolution layer-controlled 2DOSC arrays are fabricated by a polydimethylsiloxane mold-assisted selective contact evaporation printing technique. The organic field-effect transistors (OFETs) based on 2DOSC arrays have high electrical performance and excellent uniformity. The 2,6-bis(4-hexylphenyl)anthracene 2DOSC arrays-based OFETs have a small variation of 12.5% in mobility. This strategy can be applied to various organic semiconductors and pattern arrays. These demonstrations will offer more opportunities for 2DOSCs for integrated optoelectronic devices.
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http://dx.doi.org/10.1002/adma.202104166DOI Listing
August 2021

Tamsulosin attenuates high glucose- induced injury in glomerular endothelial cells.

Bioengineered 2021 12;12(1):5184-5194

Department of Nephrology, The Fourth Affiliated Hospital of Harbin Medical University, Harbin, Heilongjiang, China.

Diabetic nephropathy (DN) is a common complication of diabetes. Tamsulosin is a selective α1-AR antagonist. α1-AR is expressed widely in kidney tissues and has displayed its various physiological functions. However, whether Tamsulosin has affects DN is unknown. To our knowledge, this is the first time it has been examined whether Tamsulosin possesses a beneficial effect in high glucose-challenged glomerular endothelial cells (GECs). Firstly, we found that Tamsulosin reduced high glucose-induced expressions of TNF-α, IL-6, and IL-8. Secondly, Tamsulosin alleviated high glucose-induced expressions of MMP-2 and MMP-9. Thirdly, Tamsulosin inhibited the expressions of VCAM-1 and ICAM-1. Importantly, our results indicate that Tamsulosin inhibited high glucose-induced expressions of fibrosis factors such as Col-1 and TGF-β1. Additionally, we found that Tamsulosin ameliorated oxidative stress via reducing the generation of ROS and preventing the activation of p38. Mechanistically, we found that Tamsulosin attenuated high glucose-induced activation of NF-κB. Based on these findings, we conclude that Tamsulosin could attenuate high glucose-induced injury in GECs through alleviating oxidative stress and inflammatory response.
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http://dx.doi.org/10.1080/21655979.2021.1955527DOI Listing
December 2021

shRNA transgenic swine display resistance to infection with the foot-and-mouth disease virus.

Sci Rep 2021 Aug 12;11(1):16377. Epub 2021 Aug 12.

State Key Laboratory of AgroBiotechnology, China Agricultural University, Beijing, China.

Foot-and-mouth disease virus (FMDV) is one of the most important animal pathogens in the world. FMDV naturally infects swine, cattle, and other cloven-hoofed animals. FMD is not adequately controlled by vaccination. An alternative strategy is to develop swine that are genetically resistant to infection. Here, we generated FMDV-specific shRNA transgenic cells targeting either nonstructural protein 2B or polymerase 3D of FMDV. The shRNA-positive transgenic cells displayed significantly lower viral production than that of the control cells after infection with FMDV (P < 0.05). Twenty-three transgenic cloned swine (TGCS) and nine non-transgenic cloned swine (Non-TGCS) were produced by somatic cell nuclear transfer (SCNT). In the FMDV challenge study, one TGCS was completely protected, no clinical signs, no viremia and no viral RNA in the tissues, no non-structural antibody response, another one TGCS swine recovered after showing clinical signs for two days, whereas all of the normal control swine (NS) and Non-TGCS developed typical clinical signs, viremia and viral RNA was determined in the tissues, the non-structural antibody was determined, and one Non-TGCS swine died. The viral RNA load in the blood and tissues of the TGCS was reduced in both challenge doses. These results indicated that the TGCS displayed resistance to the FMDV infection. Immune cells, including CD3, CD4, CD8, CD21, and CD172 cells, and the production of IFN-γ were analyzed, there were no significant differences observed between the TGCS and NS or Non-TGCS, suggesting that the FMDV resistance may be mainly derived from the RNAi-based antiviral pathway. Our work provides a foundation for a breeding approach to preventing infectious disease in swine.
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http://dx.doi.org/10.1038/s41598-021-95853-3DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8361160PMC
August 2021

Facile Functionalization Strategy for Ultrasensitive Organic Protein Biochips in Multi-Biomarker Determination.

Anal Chem 2021 08 29;93(32):11305-11311. Epub 2021 Jul 29.

Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University, Tianjin 300072, China.

In recent years, organic field-effect transistors (OFETs) have shown great potential for advanced protein biochips due to their inherent biocompatibility and high-throughput detectability. However, the development of OFET-based protein biochips is still at an early stage. On the one hand, single-biomarker determination is not sufficient for the diagnosis of cancer; thus, simultaneous monitoring of electrical signals toward multi-biomarkers is widely concerned and explored. On the other hand, an optimized functionalization strategy for efficient protein immobilization is another key to make OFET-based protein biochips accessible with improved detection performance. Herein, a facile functionalization strategy is developed for excellent charge-transport thin films by suppressing the gelation of diketopyrrolopyrrole (DPP)-based polymer semiconductors with the addition of the glutaraldehyde cross-linking agent. Besides, functional groups are introduced on the device surface for efficient attachment of antibodies as receptors a condensation reaction, enabling simultaneous determination of α-fetoprotein biomarker and carcinoembryonic antigen biomarker with improved sensitivity and reliability. Therefore, the proposed high-throughput OFET-based protein biochip has the potential to be widely utilized in early liver cancer diagnosis.
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http://dx.doi.org/10.1021/acs.analchem.1c02601DOI Listing
August 2021

Ternary Conductance Switching Realized by a Pillar[5]arene-Functionalized Two-Dimensional Imine Polymer Film.

Chemistry 2021 Sep 24;27(54):13605-13612. Epub 2021 Aug 24.

Tianjin Key Laboratory of Molecular Optoelectronic Science, Department of Chemistry, School of Science &, Collaborative Innovation Center of Chemical Science and Engineering, Tianjin University, Tianjin, 300072, P. R. China.

Nowadays, most manufacturing memory devices are based on materials with electrical bistability (i. e., "0" and "1") in response to an applied electric field. Memory devices with multilevel states are highly desired so as to produce high-density and efficient memory devices. Herein, we report the first multichannel strategy to realize a ternary-state memristor. We make use of the intrinsic sub-nanometer channel of pillar[5]arene and nanometer channel of a two-dimensional imine polymer to construct an active layer with multilevel channels for ternary memory devices. Low threshold voltage, long retention time, clearly distinguishable resistance states, high ON/OFF ratio (OFF/ON1/ON2=1 : 10 : 10 ), and high ternary yield (75 %) were obtained. In addition, the flexible memory device based on 2DP can maintain its stable ternary memory performance after being bent 500 times. The device also exhibits excellent thermal stability and can tolerate a temperature as high as 300 °C. It is envisioned that the results of this work will open up possibilities for multistate, flexible resistive memories with good thermal stability and low energy consumption, and broaden the application of pillar[n]arene.
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http://dx.doi.org/10.1002/chem.202101772DOI Listing
September 2021

High Mobility Organic Lasing Semiconductor with Crystallization-Enhanced Emission for Light-Emitting Transistors.

Angew Chem Int Ed Engl 2021 Sep 11;60(37):20274-20279. Epub 2021 Aug 11.

Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Sciences, Tianjin University&Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin, 300072, China.

The development of high mobility organic laser semiconductors with strong emission is of great scientific and technical importance, but challenging. Herein, we present a high mobility organic laser semiconductor, 2,7-diphenyl-9H-fluorene (LD-1) showing unique crystallization-enhanced emission guided by elaborately modulating its crystal growth process. The obtained one-dimensional nanowires of LD-1 show outstanding integrated properties including: high absolute photoluminescence quantum yield (PLQY) approaching 80 %, high charge carrier mobility of 0.08 cm  V  s , Fabry-Perot lasing characters with a low threshold of 86 μJ cm and a high-quality factor of ≈2400. Furthermore, electrically induced emission was obtained from an individual LD-1 crystal nanowire-based light-emitting transistor due to the recombination of holes and electrons simultaneously injected into the nanowire, which provides a good platform for the study of electrically pumped organic lasers and other related ultrasmall integrated electrical-driven photonic devices.
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http://dx.doi.org/10.1002/anie.202108224DOI Listing
September 2021

Successive Storage of Cations and Anions by Ligands of π-d-Conjugated Coordination Polymers Enabling Robust Sodium-Ion Batteries.

Angew Chem Int Ed Engl 2021 Aug 16;60(34):18769-18776. Epub 2021 Jul 16.

Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Sciences, Tianjin University, Tianjin, 300072, China.

The oxidation of π-d-conjugated coordination polymers (CCPs) accompanied with anion insertion has the merits of increasing the capacity and elevating the discharge voltages. However, previous reports on this mechanism either required more investigations or showed low capacity and poor cyclablity. Herein, triphenylene-catecholate-based two-dimensional CCPs are constructed by employing inactive transition-metal ions (Zn ) as nodes, forming Zn-HHTP. Substantial characterizations and theoretical calculations indicate the successive storage of cations and anions by redox reactions of only ligands, leading to a high reversible capacity of ≈150 mAh g at 100 mA g and a remarkable capacity retention of 90 % after 1000 cycles. On the contrary, as a control experiment, the analogous CCPs (Cu-HHTP) with Cu nodes, where both ligands and metal ions undergo redox reactions, accompanied by the storage of only Na cations, show a much poorer cyclability. These results highlight the importance of redox reactions of only ligands for long-term cycle life and the insight into the storage mechanisms deepens our understanding on CCPs for the further design of CCPs with high performance.
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http://dx.doi.org/10.1002/anie.202106055DOI Listing
August 2021

Bandgap Engineering of an Aryl-Fused Tetrathianaphthalene for Visible-Blind Organic Field-Effect Transistors.

Front Chem 2021 28;9:698246. Epub 2021 May 28.

Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University and Collaborative Innovation Center of Chemical Science and Engineering, Tianjin, China.

Stability problem of organic semiconductors (OSCs) because of photoabsorption has become a major barrier to large scale applications in organic field-effect transistors (OFETs). It is imperative to design OSCs which are insensitive to visible and near-infrared (VNIR) light to obtain both environmental and operational stability. Herein, taking a 2,3,8,9-tetramethoxy [1,4]benzodithiino[2,3-b][1,4]benzodithiine (TTN2) as an example, we show that controlling molecular configuration is an effective strategy to tune the bandgaps of OSCs for visible-blind OFETs. TTN2 adopts an armchair-like configuration, which is different from the prevailing planar structure of common OSCs. Because of the large bandgap, TTN2 exhibits no photoabsorption in the VNIR region and OFETs based on TTN2 show high environmental stability. The devices worked well after being stored in ambient air, (i.e. in the presence of oxygen and water) and light for over two years. Moreover, the OFETs show no observable response to light irradiation from 405-1,020 nm, which is also favorable for high operational stability.
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http://dx.doi.org/10.3389/fchem.2021.698246DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8193678PMC
May 2021

Spatially Selective Imaging of Mitochondrial MicroRNAs via Optically Programmable Strand Displacement Reactions.

Angew Chem Int Ed Engl 2021 08 5;60(33):17937-17941. Epub 2021 Jul 5.

CAS Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety and CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing, 100190, China.

MicroRNA (miRNA) functions are tightly regulated by their sub-compartmental location in living cells, and the ability to imaging of mitochondrial miRNAs (mitomiRs) is essential for understanding of the related pathological processes. However, most existing DNA-based methods could not be used for this purpose. Here, we report the development of a DNA nanoreporter technology for imaging of mitomiRs in living cells through near-infrared (NIR) light-controlled DNA strand displacement reactions. The sensing function of the DNA nanoreporters are silent (OFF) during the delivery process, but can be photoactivated (ON) with NIR light after targeted mitochondrial localization, enabling spatially-restricted imaging of two types of cancer-related mitomiRs with improved detection accuracy. Furthermore, we demonstrate imaging of mitomiRs in vivo through spatiotemporally-controlled delivery and activation. Therefore, this study illustrates a simple methodology that may be broadly applicable for investigating the mitomiRs-associated physiological events.
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http://dx.doi.org/10.1002/anie.202105696DOI Listing
August 2021

An intermolecular hydrogen bond plays a determining role in product selection of a surface confined Schiff-base reaction.

Chem Commun (Camb) 2021 Jul;57(53):6495-6498

Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science & Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin University, Tianjin 300072, China.

Herein, we illustrate how the cooperation of intermolecular hydrogen bonds and conformation flexibility leads to the formation of diverse complex covalent nanostructures on the surface, while the relative abundance of the final products can be further tuned by adjusting the molar ratio and concentration of monomers.
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http://dx.doi.org/10.1039/d1cc01801aDOI Listing
July 2021

Organic Light-Emitting Transistors Entering a New Development Stage.

Adv Mater 2021 Aug 22;33(31):e2007149. Epub 2021 May 22.

Beijing National Laboratory for Molecular Sciences, Key Laboratory of Organic Solids, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China.

Organic light-emitting transistors (OLETs) are possibly the smallest integrated optoelectronic devices that combine the switching and amplification mechanisms of organic field-effect transistors (OFETs) and the electroluminescent characteristic of organic light-emitting diodes (OLEDs). Such a unique architecture of OLETs makes them ideal for developing the next-generation display technology and electrically pumped lasers for miniaturized photonic devices and circuits. However, the development of OLETs has been slow. Recently, some exciting progress has been made with breakthroughs in high mobility emissive organic semiconductors, construction of high-performance OLETs, and fabrication of novel multifunctional OLETs. This recent slew of advances may represent the advent of a new development stage of OLETs and their related devices and circuits. In this paper, a detailed review of these fantastic advances is presented, with a special focus on the key points for developing high-performance OLETs. Finally, a brief conclusion is provided with a discussion on the challenges and future perspectives in this field.
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http://dx.doi.org/10.1002/adma.202007149DOI Listing
August 2021

Recent Advances of Nanospheres Lithography in Organic Electronics.

Small 2021 07 21;17(28):e2100724. Epub 2021 May 21.

Physikalisches Institut, Westfälische Wilhelms-Universität, Wilhelm-Klemm-Straße 10, 48149, Münster, Germany.

Nanospheres lithography (NSL) is an economical technique, which makes use of highly monodispersed nanospheres such as deposition or etch masks for generating patterns with nanoscale features. Embedding nanostructures into organic electronic devices can endow them with unique capabilities and enhanced performance, which have greatly advanced the development of organic electronics. In this review, a brief summary of the methods for the preparation of monodispersed nanospheres is presented. Afterward, the authors highlight the recent advances of a wide variety of applications of nanospheres lithography in organic electronic devices. Finally, the challenges in this field are pointed out, and the future development of this field is discussed.
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http://dx.doi.org/10.1002/smll.202100724DOI Listing
July 2021

Isomeric Dibenzoheptazethrenes for Air-Stable Organic Field-Effect Transistors.

Angew Chem Int Ed Engl 2021 Jul 15;60(29):16230-16236. Epub 2021 Jun 15.

Institute of Molecular Plus, Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Tianjin university, 92 Weijin Road, Tianjin, 300072, China.

Singlet diradicaloids hold great potential as semiconductors for organic field-effect transistors (OFETs). However, their relative low material and device stabilities impede the practical applications. Here, to achieve balanced stability and performance, two isomeric dibenzoheptazethrene derivatives with singlet diradical character were synthesized in a concise manner. Benefitting from the aromatic stabilization, both compounds display a small diradical character and large singlet-triplet gap, as corroborated by variable-temperature electron paramagnetic resonance spectra, single-crystal analysis, and theoretical calculations. OFET devices based on single crystals showed a high hole mobility of 0.15 cm  V  s , which is the highest for zethrene-based semiconductors. Both isomers exhibited remarkable material stability in air-saturated solutions as well as excellent bias-stress and storage stability in device under ambient air.
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http://dx.doi.org/10.1002/anie.202105872DOI Listing
July 2021

Sub-5 nm single crystalline organic p-n heterojunctions.

Nat Commun 2021 May 13;12(1):2774. Epub 2021 May 13.

Beijing National Laboratory for Molecular Sciences, Institute of Chemistry Chinese Academy of Sciences, Beijing, China.

The cornerstones of emerging high-performance organic photovoltaic devices are bulk heterojunctions, which usually contain both structure disorders and bicontinuous interpenetrating grain boundaries with interfacial defects. This feature complicates fundamental understanding of their working mechanism. Highly-ordered crystalline organic p-n heterojunctions with well-defined interface and tailored layer thickness, are highly desirable to understand the nature of organic heterojunctions. However, direct growth of such a crystalline organic p-n heterojunction remains a huge challenge. In this work, we report a design rationale to fabricate monolayer molecular crystals based p-n heterojunctions. In an organic field-effect transistor configuration, we achieved a well-balanced ambipolar charge transport, comparable to single component monolayer molecular crystals devices, demonstrating the high-quality interface in the heterojunctions. In an organic solar cell device based on the p-n junction, we show the device exhibits gate-tunable open-circuit voltage up to 1.04 V, a record-high value in organic single crystalline photovoltaics.
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http://dx.doi.org/10.1038/s41467-021-23066-3DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8119440PMC
May 2021

Molecular Weight Engineering in High-Performance Ambipolar Emissive Mesopolymers.

Angew Chem Int Ed Engl 2021 Jun 1;60(27):14902-14908. Epub 2021 Jun 1.

Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University, Tianjin, 300072, China.

Mesopolymers with high solubility, free of structural defects, and negligible batch-to-batch variation open a new avenue for organic optoelectronics. Organic light emitting transistors that combine the functions of organic light-emitting diodes and organic field-effect transistors. However, charge transport ability and light emitting strength are contradictory within one conjugated polymer. Herein, three low-molecular-weight mesopolymers with thienopyrroledione-benzothiadiazole repeating units (meso-TBTF) were obtained. The mesopolymers show strong solid-state emission and high ambipolar carrier mobility. The molecular weights of meso-TBTF can be tuned by polymerization temperature. The mesopolymers have photoluminescence quantum yields (PLQY) of about 50 % in solution and 10 % in solid state. Polymer light emitting diodes of this material are fabricated to explore its potential use in optoelectronic devices.
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http://dx.doi.org/10.1002/anie.202105036DOI Listing
June 2021

Revealing molecular conformation-induced stress at embedded interfaces of organic optoelectronic devices by sum frequency generation spectroscopy.

Sci Adv 2021 Apr 14;7(16). Epub 2021 Apr 14.

Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, Institute of Molecular Aggregation Science, Tianjin University, Tianjin 300072, China.

Interface stresses are pervasive and critical in conventional optoelectronic devices and generally lead to many failures and reliability problems. However, detection of the interface stress embedded in organic optoelectronic devices is a long-standing problem, which causes the unknown relationship between interface stress and organic device stability (one key and unsettled issue for practical applications). In this study, a kind of previously unknown molecular conformation-induced stress is revealed at the organic embedded interface through sum frequency generation (SFG) spectroscopy technique. This stress can be greater than 10 kcal/mol per nm and is sufficient to induce molecular disorder in the organic semiconductor layer (with energy below 8 kcal/mol per nm), finally causing instability of the organic transistor. This study not only reveals interface stress in organic devices but also correlates instability of organic devices with the interface stress for the first time, offering an effective solution for improving device stability.
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http://dx.doi.org/10.1126/sciadv.abf8555DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8050595PMC
April 2021

2D MXene-Molecular Hybrid Additive for High-Performance Ambipolar Polymer Field-Effect Transistors and Logic Gates.

Adv Mater 2021 May 12;33(20):e2008215. Epub 2021 Apr 12.

Institut de Science et d'Ingénierie Supramoléculaires, University of Strasbourg & CNRS, 8 allée Gaspard Monge, Strasbourg, 67000, France.

MXenes are highly conductive layered materials that are attracting a great interest for high-performance opto-electronics, photonics, and energy applications.. Their non-covalent functionalization with ad hoc molecules enables the production of stable inks of 2D flakes to be processed in thin-films. Here, the formation of stable dispersions via the intercalation of Ti C T with didecyldimethyl ammonium bromide (DDAB) yielding Ti C T -DDAB, is demonstrated. Such functionalization modulates the properties of Ti C T , as evidenced by a 0.47 eV decrease of the work function. It is also shown that DDAB is a powerful n-dopant capable of enhancing electron mobility in conjugated polymers and 2D materials. When Ti C T -DDAB is blended with poly(diketopyrrolopyrrole-co-selenophene) [(PDPP-Se)], a simultaneous increase by 170% and 152% of the hole and electron field-effect mobilities, respectively, is observed, compared to the neat conjugated polymer, with values reaching 2.0 cm V s . By exploiting the balanced ambipolar transport of the Ti C T -DDAB/PDPP-Se hybrid, complementary metal-oxide-semiconductor (CMOS) logic gates are fabricated that display well-centered trip points and good noise margin (64.6% for inverter). The results demonstrate that intercalant engineering represents an efficient strategy to tune the electronic properties of Ti C T yielding functionalized MXenes for polymer transistors with unprecedented performances and functions.
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http://dx.doi.org/10.1002/adma.202008215DOI Listing
May 2021

Directly Patterning Conductive Polymer Electrodes on Organic Semiconductor via In Situ Polymerization in Microchannels for High-Performance Organic Transistors.

ACS Appl Mater Interfaces 2021 Apr 7;13(15):17852-17860. Epub 2021 Apr 7.

Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, Institute of Molecular Aggregation Science, Tianjin University, 300072 Tianjin, China.

Conductive polymers are considered promising electrode materials for organic transistors, but the reported devices with conductive polymer electrodes generally suffer from considerable contact resistance. Currently, it is still highly challenging to pattern conductive polymer electrodes on organic semiconductor surfaces with good structure and interface quality. Herein, we develop an in situ polymerization strategy to directly pattern the top-contacted polypyrrole (PPy) electrodes on hydrophobic surfaces of organic semiconductors by microchannel templates, which is also applicable on diverse hydrophobic and hydrophilic surfaces. Remarkably, a width-normalized contact resistance as low as 1.01 kΩ·cm is achieved in the PPy-contacted transistors. Both p-type and n-type organic field-effect transistors (OFETs) exhibit ideal electrical characteristics, including almost hysteresis-free, low threshold voltage, and good stability under long-term test. The facile patterning method and high device performance indicate that the polymerization strategy in confined microchannels has application prospects in all-organic, transparent, and flexible electronics.
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http://dx.doi.org/10.1021/acsami.1c01386DOI Listing
April 2021

1D Mixed-Stack Cocrystals Based on Perylene Diimide toward Ambipolar Charge Transport.

Small 2021 Apr 6:e2006574. Epub 2021 Apr 6.

Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Sciences Tianjin University, Collaborative Innovation Center of Chemical Science, and Engineering, Tianjin, 300072, China.

There is very limited repertoire of organic ambipolar semiconductors to date. Electron donor-acceptor alternative stacking is a unique and important binary motif for 1D mixed-stack cocrystals, opening up possibilities for the development of organic ambipolar semiconductors. Herein, four 1D mixed-stack cocrystals using N,N'-bis(perfluorobutyl)-1,7-dicyanoperylene-3,4:9,10-bis(dicarboximide) (PDICNF) as the acceptor and anthracene, pyrene, perylene, and meso-diphenyl tetrathia[22]annulene[2,1,2,1] (DPTTA) as the donors are achieved in a stoichiometric ratio (D:A = 1:1) through solution or vapor processed methods. Their packing structures, energy levels, charge transfer interactions, coassembling behaviors, and molecular orientations are systematically investigated by single-crystal X-ray analysis, absorption spectra, fluorescence quenching, Job's curve plot, and polarized photoluminescence measurements with the help of theoretical calculations. The donor-acceptor alternative stacking direction coincides with the long axis for all the four cocrystals. The field-effect transistors based on Pyrene-PDICNF show the electron mobility up to 0.19 cm V s , which is the highest value among perylene diimide-based cocrystals. Moreover, DPTTA-PDICNF cocrystals possess well-balanced electron and hole mobility with 1.7 × 10 and 2.0 × 10  cm V s respectively due to both hole and electron strong superexchange interactions, shedding light on the design of 1D mixed-stack cocrystals with excellent ambipolar transport behaviors.
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http://dx.doi.org/10.1002/smll.202006574DOI Listing
April 2021

Ultrasensitive and Reliable Organic Field-Effect Transistor-Based Biosensors in Early Liver Cancer Diagnosis.

Anal Chem 2021 04 29;93(15):6188-6194. Epub 2021 Mar 29.

Department of Chemistry, Tianjin Key Laboratory of Molecular Optoelectronic Sciences, School of Science, Tianjin University, Tianjin 300072, China.

Organic field-effect transistors (OFETs) are considered as one of the cost-effective biosensor devices with rapid detection capabilities and multiparameter responses. However, the functionalization processes on normal organic devices might impact the device performance for its further sensitive and reliable sensing applications. Herein, we develop a novel organic material, 2,6-bis(4-formylphenyl)anthracene (BFPA) for use as the protective and functional layer of OFET-based biosensors, enabling ultrasensitive determination of alpha-fetoprotein (AFP) with femtomolar accuracy in human serum. By monitoring changes of the source-drain current () and threshold voltage () electrical signals, the device exhibits improved reliability in detecting AFP biomarkers and is able to differentiate between liver cancer patients and healthy individuals. Featuring label-free determination, shorter analysis time, and lower sample volume, this ultrasensitive and reliable OFET-based biosensor displays numerous advantages over traditional strategies such as enzyme-linked immunosorbent assay and electrochemiluminescence immunoassay, demonstrating that the proposed OFET-based biosensors have broader analytical and clinical applications for early liver cancer diagnosis.
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http://dx.doi.org/10.1021/acs.analchem.1c00372DOI Listing
April 2021

Influenza Surveillance Trends and Influenza Vaccine Effectiveness Among Department of Defense Beneficiaries During the 2019-2020 Influenza Season.

MSMR 2021 Mar;28(3):2-8

Laboratory-based influenza surveillance was conducted in the 2019-2020 influenza season among Department of Defense (DoD) beneficiaries through the DoD Global Respiratory Pathogen Surveillance Program (DoDGRS). Sentinel and participating sites submitted 28,176 specimens for clinical diagnostic testing. A total of 5,529 influenza-positive cases were identified. Starting at surveillance week 45 (3-9 November 2019), influenza B was the predominant influenza type, followed by high activity of influenza A(H1N1)pdm09 three weeks thereafter. Both influenza B and influenza A(H1N1)pdm09 were then highly co-circulated through surveillance week 13 (22-28 March 2020). End-of-season influenza vaccine effectiveness (VE) was estimated using a test-negative case-control study design. The adjusted end-of-season VE for all beneficiaries, regardless of influenza type or subtype, was 46% (95% confidence interval: 40%-52%). The influenza vaccine was moderately effective against influenza viruses during the 2019-2020 influenza season.
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March 2021

Expression, structure and function analysis of the sperm-oocyte fusion genes Juno and Izumo1 in sheep (Ovis aries).

J Anim Sci Biotechnol 2021 Mar 12;12(1):37. Epub 2021 Mar 12.

Key Laboratory of Animal Genetics and Breeding and Reproduction of Ministry of Agriculture and Rural Affairs, Institute of Animal Sciences, Chinese Academy of Agricultural Sciences, Beijing, 100193, China.

Background: JUNO and IZUMO1 are the first receptor-ligand protein pairs discovered to be essential for sperm-oocyte fusion; their interaction is indispensable for fertilization.

Methods: PCR was used to clone the full-length DNA sequence of the Juno gene in sheep. The single nucleotide polymorphism (SNP) loci of Juno were genotyped by Sequenom MassARRAY®. PCR combined with rapid amplification of cDNA Ends were used to clone the full-length cDNA sequence of Juno and Izumo1. Reverse transcriptase-PCR (RT-PCR) and real time-quantitative-PCR (RT-qPCR) were used to analyze the genes' expression in tissues of sheep, and single cell RNA-seq was used to analyze the genes' expression in oocytes, granulosa cells and follicular theca of polytocous and monotocous Small Tail Han ewes. Bioinformatics was used to analyze advanced structure and phylogeny of JUNO and IZUMO1 proteins.

Results: The full-length DNA sequence of the Juno gene in sheep was cloned and nine SNPs were screened. We found a significant association between the g.848253 C > A locus of Juno and litter size of Small Tail Han sheep (P < 0.05). The full-length cDNA sequence of Juno and Izumo1 genes from Small Tail Han sheep were obtained. We found a new segment of the Izumo1 CDS consisting of 35 bp, and we confirmed the Izumo1 gene has 9 exons, not 8. RT-qPCR showed that Juno and Izumo1 genes were highly expressed in ovarian and testicular tissues, respectively (P < 0.01). Single cell RNA-seq showed Juno was specifically expressed in oocytes, but not in granulosa cells or follicular theca, while Izumo1 displayed little to no expression in all three cell types. There was no difference in expression of the Juno gene in oocyte and ovarian tissue in sheep with different litter sizes, indicating expression of Juno is not related to litter size traits. Bioinformatic analysis revealed the g.848253 C > A locus of Juno results in a nonconservative missense point mutation leading to a change from Phe to Leu at position 219 in the amino acid sequence.

Conclusions: For the first time, this study systematically analyzed the expression, structure and function of Juno and Izumo1 genes and their encoded proteins in Small Tail Han sheep, providing the basis for future studies of the regulatory mechanisms of Juno and Izumo1 genes.
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http://dx.doi.org/10.1186/s40104-021-00548-4DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7953763PMC
March 2021

Regulating the Solvation Sheath of Li Ions by Using Hydrogen Bonds for Highly Stable Lithium-Metal Anodes.

Angew Chem Int Ed Engl 2021 May 6;60(19):10871-10879. Epub 2021 Apr 6.

Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Sciences, Tianjin University, Tianjin, 300072, China.

The performance of Li anodes is extremely affected by the solvation of Li ions, leading to preferential reduction of the solvation sheath and subsequent formation of fragile solid-electrolyte interphase (SEI), Li dendrites, and low coulombic efficiency (CE). Herein, we propose a novel strategy to regulate the solvation sheath, through the introduction of intermolecular hydrogen bonds with both the anions of Li salt and the solvent by small amount additives. The addition of such hydrogen bonds reduced the LUMO energy level of anions in electrolyte, promoted the formation of a robust SEI, reduced the amount of free solvent molecules, and enhanced stability of electrolytes. Based on this strategy, flat and dense lithium deposition was obtained. Even under lean electrolytes, at a current density of 1 mA cm with a fixed capacity of 3 mAh cm , the Li-Cu cells showed an impressive CE value of 99.2 %. The Li-LiFePO full cells showed long-term cycling stability for more than 1000 cycles at 1 C, with a total capacity loss of only 15 mAh g .
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http://dx.doi.org/10.1002/anie.202101976DOI Listing
May 2021

Ultra-thin two-dimensional molecular crystals grown on a liquid surface for high-performance phototransistors.

Chem Commun (Camb) 2021 Mar 17;57(21):2669-2672. Epub 2021 Feb 17.

Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University & Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin 300072, China.

A novel strategy for the growth of molecularly thin two-dimensional molecular crystals (2DMCs) of organic semiconductors with poor solubility was developed. Large-area bilayer 2DMCs were grown on a liquid surface at elevated temperatures, with record mobility and superior photoresponse.
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http://dx.doi.org/10.1039/d0cc07545kDOI Listing
March 2021

Electrically Conductive Coordination Polymers for Electronic and Optoelectronic Device Applications.

J Phys Chem Lett 2021 Feb 8;12(6):1612-1630. Epub 2021 Feb 8.

Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University and Collaborative Innovation Center of Chemical Science and Engineering, Tianjin 300072, China.

Electrically conductive coordination polymers (generally known as metal-organic frameworks, MOFs) are a class of crystalline hybrid materials produced by the reasonable self-assembly of metal nodes and organic linkers. The unique and intriguing combination of inorganic and organic components endows coordination polymers with superior optical and electrical properties, which have recently aroused much attention in several electronic and optoelectronic technological applications. However, there are many challenging obstacles and issues that need to be addressed in this burgeoning field. In this Perspective, we first provide a fundamental understanding about the electronic design strategies that provide better guidance for realizing high conductivities and good mobilities in coordination polymers. We then examine the current established synthetic approaches to construct high-quality working samples of electrically conductive coordination polymers for device integration. This is followed by a discussion of the current state-of-the-art progress toward the preliminary achievements in (opto)electronic devices spanning chemiresistive sensors, field-effect transistors, organic photovoltaics, photodetectors, . Finally, we conclude this Perspective with the existing hurdles and limitations in this area, along with the critical directions and opportunities for future research.
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http://dx.doi.org/10.1021/acs.jpclett.0c02988DOI Listing
February 2021
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