bluuebunny/crossref_metadata_2025 huggingface dataset:
A Meta‐Device for Intelligent Depth Perception
Authors: Chen Mu Ku , Liu Xiaoyuan , Wu Yongfeng , Zhang Jingcheng , Yuan Jiaqi , Zhang Zhengnan , Tsai Din Ping
Published: August 2022

The optical illusion affects depth‐sensing due to the limited and specific light‐field information acquired by single‐lens imaging. The incomplete depth information or visual deception would cause cognitive errors. To resolve this problem, an intelligent and compact depth‐sensing meta‐device that is miniaturized, integrated, and applicable for diverse scenes in all light levels is demonstrated. The compact and multifunction stereo vision system adopts an array with 3600 achromatic meta‐lenses and a size of 1.2 × 1.2 mm2to measure the depth over a 30 cm range with deep‐learning support. The meta‐lens array can act as multiple imaging lenses to collect light field information. It can also work with a light source as an active optical device to project a structured light. The meta‐lens array can serve as the core functional component of a light‐field imaging system under bright conditions or a structured‐light projection system in the dark. The depth information in both ways can be analyzed and extracted by the convolutional neural network. This work provides a new avenue for the applications such as autonomous driving, machine vision, human–computer interaction, augmented reality, biometric identification, etc.
Universal Hopping Motion Protected by Structural Topology
Authors: Song Moojune , You Mujin , Yang Seungmo , Ju Tae‐Seong , Moon Kyoung‐Woong , Hwang Chanyong , Kim Kyoung‐Whan , Park Albert Min Gyu , Kim Kab‐Jin
Published: August 2022

A scaling law elucidates the universality in nature, presiding over many physical phenomena which seem unrelated. Thus, exploring the universality class of scaling law in a particular system enlightens its physical nature in relevance to other systems and sometimes unearths an unprecedented new dynamic phase. Here, the dynamics of weakly driven magnetic skyrmions are investigated, and its scaling law is compared with the motion of a magnetic domain wall (DW) creep. This study finds that the skyrmion does not follow the scaling law of the DW creep in 2D space but instead shows a hopping behavior similar to that of the particle‐like DW in 1D confinement. In addition, the hopping law satisfies even when a topological charge of the skyrmion is removed. Therefore, the distinct scaling behavior between the magnetic skyrmion and the DW stems from a general principle beyond the topological charge. This study demonstrates that the hopping behavior of skyrmions originates from the bottleneck process induced by DW segments with diverging collective lengths, which is inevitable in any closed‐shape spin structure in 2D. This work reveals that the structural topology of magnetic texture determines the universality class of its weakly driven motion, which is distinguished from the universality class of magnetic DW creep.
Charge Transport in Twisted Organic Semiconductor Crystals of Modulated Pitch
Authors: Yang Yongfan , Silva de Moraes Lygia , Ruzié Christian , Schweicher Guillaume , Geerts Yves Henri , Kennedy Alan R. , Zhou Hengyu , Whittaker St. John , Lee Stephanie S. , Kahr Bart , Shtukenberg Alexander G.
Published: August 2022

Many molecular crystals (approximately one third) grow as twisted, helicoidal ribbons from the melt, and this preponderance is even higher in restricted classes of materials, for instance, charge‐transfer complexes. Previously, twisted crystallites of such complexes present an increase in carrier mobilities. Here, the effect of twisting on charge mobility is better analyzed for a monocomponent organic semiconductor, 2,5‐bis(3‐dodecyl‐2‐thienyl)‐thiazolo[5,4‐d]thiazole (BDT), that forms twisted crystals with varied helicoidal pitches and makes possible a correlation of twist strength with carrier mobility. Films are analyzed by X‐ray scattering and Mueller matrix polarimetry to characterize the microscale organization of the polycrystalline ensembles. Carrier mobilities of organic field‐effect transistors are five times higher when the crystals are grown with the smallest pitches (most twisted), compared to those with the largest pitches, along the fiber elongation direction. A tenfold increase is observed along the perpendicular direction. Simulation of electrical potential based on scanning electron microscopy images and density functional theory suggests that the twisting‐enhanced mobility is mainly controlled by the fiber organization in the film. A greater number of tightly packed twisted fibers separated by numerous smaller gaps permit better charge transport over the film surface compared to fewer big crystallites separated by larger gaps.
Nondestructive Photopatterning of Heavy‐Metal‐Free Quantum Dots
Authors: Yang Jeehye , Lee Myeongjae , Park Se Young , Park Myoungjin , Kim Jonghoon , Sitapure Niranjan , Hahm Donghyo , Rhee Seunghyun , Lee Daeyeon , Jo Hyunwoo , Jo Yong Hyun , Lim Jaemin , Kim Jungwook , Shin Tae Joo , Lee Doh C. , Kwak Kyungwon , Kwon Joseph S. , Kim BongSoo , Bae Wan Ki , Kang Moon Sung
Published: August 2022

Electroluminescence from quantum dots (QDs) is a suitable photon source for futuristic displays offering hyper‐realistic images with free‐form factors. Accordingly, a nondestructive and scalable process capable of rendering multicolored QD patterns on a scale of several micrometers needs to be established. Here, nondestructive direct photopatterning for heavy‐metal‐free QDs is reported using branched light‐driven ligand crosslinkers (LiXers) containing multiple azide units. The branched LiXers effectively interlock QD films via photo‐crosslinking native aliphatic QD surface ligands without compromising the intrinsic optoelectronic properties of QDs. Using branched LiXers with six sterically engineered azide units, RGB QD patterns are achieved on the micrometer scale. The photo‐crosslinking process does not affect the photoluminescence and electroluminescence characteristics of QDs and extends the device lifetime. This nondestructive method can be readily adapted to industrial processes and make an immediate impact on display technologies, as it uses widely available photolithography facilities and high‐quality heavy‐metal‐free QDs with aliphatic ligands.
An Irradiance‐Adaptable Near‐Infrared Vertical Heterojunction Phototransistor
Authors: Zhang Mengyu , Chi Zhiguo , Wang Guoqing , Fan Zelong , Wu Honglei , Yang Ping , Yang Junbo , Yan Peiguang , Sun Zhenhua
Published: August 2022

Bioinspired artificial visual perception devices with the optical environment‐adaptable function have attracted significant attention for their promising potential in applications like robotics and machine vision. In this regard, a photodetector with in‐sensor adaptability is longed for in terms of complexity, efficiency, and cost. Here, a near‐infrared phototransistor with a benign light irradiance‐adaptability is presented. The phototransistor uses a vertically stacking graphene/lead sulfide quantum dots/graphene heterojunction as the conductive channel. Compared with ordinary lead sulfide quantum dots‐decorated graphene phototransistors, the present device demonstrates a faster photoresponse speed and an abnormal transfer characteristic. The latter characteristic is induced by the gate voltage‐tunable Fermi level in the heterojunction and the abundant electron trap states in the quantum dot film, which jointly results in an intense dependence of the photoresponse on the gate voltage. The dynamic trapping and de‐trapping processes in the quantum dot film enable the inhibition or potentiation of the photoresponse, based on which the photopic or scotopic adaptation behavior of the human retina is successfully mimicked, respectively. By providing an irradiance‐adaptable photodetector with a spectral response beyond visible light, this work should inspire future research on artificial environment‐adaptable perception devices.
Enhanced Competition at the Nano–Bio Interface Enables Comprehensive Characterization of Protein Corona Dynamics and Deep Coverage of Proteomes
Authors: Ferdosi Shadi , Stukalov Alexey , Hasan Moaraj , Tangeysh Behzad , Brown Tristan R. , Wang Tianyu , Elgierari Eltaher M. , Zhao Xiaoyan , Huang Yingxiang , Alavi Amir , Lee‐McMullen Brittany , Chu Jessica , Figa Mike , Tao Wei , Wang Jian , Goldberg Martin , O'Brien Evan S. , Xia Hongwei , Stolarczyk Craig , Weissleder Ralph , Farias Vivek , Batzoglou Serafim , Siddiqui Asim , Farokhzad Omid C. , Hornburg Daniel
Published: August 2022

Introducing engineered nanoparticles (NPs) into a biofluid such as blood plasma leads to the formation of a selective and reproducible protein corona at the particle–protein interface, driven by the relationship between protein–NP affinity and protein abundance. This enables scalable systems that leverage protein–nano interactions to overcome current limitations of deep plasma proteomics in large cohorts. Here the importance of the protein to NP‐surface ratio (P/NP) is demonstrated and protein corona formation dynamics are modeled, which determine the competition between proteins for binding. Tuning the P/NP ratio significantly modulates the protein corona composition, enhancing depth and precision of a fully automated NP‐based deep proteomic workflow (Proteograph). By increasing the binding competition on engineered NPs, 1.2–1.7× more proteins with 1% false discovery rate are identified on the surface of each NP, and up to 3× more proteins compared to a standard plasma proteomics workflow. Moreover, the data suggest P/NP plays a significant role in determining the in vivo fate of nanomaterials in biomedical applications. Together, the study showcases the importance of P/NP as a key design element for biomaterials and nanomedicine in vivo and as a powerful tuning strategy for accurate, large‐scale NP‐based deep proteomic studies.
Zn‐Metal–Organic Framework Derived Ordered Mesoporous Carbon‐Based Nanostructure for High‐Performance and Universal Multivalent Metal Ion Storage
Authors: Zhang Hong , Wang Haozhi , Pan Zhenghui , Wu Zhong , Deng Yida , Xie Jianping , Wang John , Han Xiaopeng , Hu Wenbin
Published: August 2022

Metal–organic framework (MOF) derivatives promise great potential in energy storage and conversion because of their excellent tunability in both the active metal sites, organic links, and the overall structures down to atomic and up to mesoscale. Nevertheless, a big challenge is to precisely control and thoroughly understand the actual MOF‐to‐derivative conversion process to realize the template‐free synthesis of the MOF‐derived ordered mesoporous materials. Here, a class of ordered mesoporous N‐doped carbon nanoflakes is presented with slit‐shaped pores synthesized by one‐step pyrolysis of Zn1Cux–MOF, where the Cu doping plays a critically important direction‐inducing function on the dissociation of organic ligands during the pyrolysis. Benefiting from the uniquely ordered mesoporous structure and large specific surface area (910 m2 g−1), the Zn1Cux–MOF‐derived ordered mesoporous carbon nanoflakes present outstanding electrochemical storage performance for multivalent metal ions, such as Mg2+, Ca2+, Co2+, Ni2+, Al3+, and Zn2+, demonstrating the universal nature of the slit‐shaped pores in enabling the multivalent metal ions for energy storage. Moreover, the assembled flexible Zn‐ion hybrid supercapacitor (ZHSC) delivers a high specific capacity of 134 mAh g−1 at 0.5 A g−1, excellent cycling and mechanical stability, showing great application potential in the new generation energy storage devices.
Ultrasound‐Controlled Swarmbots Under Physiological Flow Conditions
Authors: Fonseca Alexia Del Campo , Kohler Tobias , Ahmed Daniel
Published: August 2022

Navigation of microrobots in living vasculatures is essential in realizing targeted drug delivery and advancing non‐invasive surgeries. Acoustically‐controlled “swarmbots” are developed based on the self‐assembly of clinically‐approved microbubbles (MBs). Ultrasound is noninvasive, penetrates deeply into the human body, and is well‐developed in clinical settings. This propulsion strategy relies on two forces: the primary radiation force and the secondary Bjerknes force. Upon ultrasound activation, the MBs self‐assemble into microswarms, which migrate toward and anchor at the containing vessel's wall. A second transducer, which produces an acoustic field parallel to the channel, propels the swarms along the wall. Noting that human arteries have a blood flow 5–19 cm s−1, powerful features of cross‐ and upstream swarmbot navigation are demonstrated against physiologically‐relevant flow rates that reach 16.7 cm s−1. Additionally, controlled navigation of swarmbots is shown within mice blood and under pulsatile flow conditions of 100 beats per minute (bpm); an adult human heart at rest executes between 60 and 100 bpm. This capability represents a much‐needed pathway for advancing preclinical research.
In Situ Raman Observation of Dynamically Structural Transformation Induced by Electrochemical Lithium Intercalation and Deintercalation from Multi‐Electrochromic V2O5 Thin Films
Authors: Zhang Zhuohui , Xie Weiping , Li Jia , Zhang Hongliang , Wang Qiang , Zhang Chengli , Xu Guanglong , Gao Junhua , Rogachev A. A. , Cao Hongtao
Published: August 2022

Understanding the dynamic nature of electrochemical interface induced by ion transfer is of great significance. Herein, in situ Raman spectroscopy combined with electrochemistry has been developed to real‐time monitor the transfer of lithium ions at electrode‐electrolyte interface and reveal the associated structure and performance variation of the vanadium pentoxide (V2O5) thin films on the indium tin oxide/silver/aluminum zinc oxide/poly(ethylene terephthalate) (ITO/Ag/AZO/PET) substrates. It is demonstrated that the Raman active/silent states of the vibrational modes of VO, V3O, and VO bonds, as well as the transformation of the V2O5 thin films from V2O5 to lithium vanadate (LixV2O5), can be reversibly changed with reversible extraction/insertion of lithium ions. In situ UV‐vis spectroscopy in combination with in situ Raman analysis is applied to show that the reversible evolutions involving V2O5/LixV2O5 and VO bonding characteristic contribute to the multi‐color electrochromic characteristic of the V2O5 thin films enabling a superior optical modulation of up to 75.41%. This experimental approach establishes a significative guideline for the more elaborate research on the dynamic nature of electrochemical interface.
Electrolyte‐Controlled Permeability in Nanocellulose‐Stabilized Emulsions
Authors: Heise Katja , Jonkergouw Christopher , Anaya‐Plaza Eduardo , Guccini Valentina , Pääkkönen Timo , Linder Markus B. , Kontturi Eero , Kostiainen Mauri A.
Published: August 2022

Particle‐stabilized emulsions, so‐called Pickering emulsions (PEs), are a promising low‐tech avenue to precisely engineered materials for applications in drug delivery, catalysis, or water remediation. The particle assembly at the liquid–liquid interface provides superior stability and an adjustable permeability, which is a key parameter for controllable compound capture and release. However, understanding the complex factors that control the particle assembly in detail is a still‐remaining challenge limiting practical applications of PEs in an industrial framework. In this study, the properties of oil‐in‐water emulsions, stabilized by cellulose nanocrystals (CNCs), are investigated. It is shown how high ionic strength leads to low polydispersity droplets, with restricted permeability across the oil‐water interface due to the dense packing of the CNC layer. In contrast, lower electrolyte concentration enables enhanced uptake through the interface, while providing the required stability for the reusability of the material. The authors continue to study the impact of the electrolyte content on the dynamic responses of the emulsions, leading to a liquid–liquid system with tunable cyclic uptake and release levels. Overall, the results highlight the potential of nanocellulose‐stabilized emulsions as tunable and robust material platform with well‐defined permeability characteristics—made in a simple way.
High‐Performance Full‐Solution‐Processed Oxide Thin‐Film Transistor Arrays Fabricated by Ultrafast Scanning Diode Laser
Authors: Xu Meng , Hu Sunjie , Peng Cong , Jing Bin , Chen Longlong , Li Xifeng , Zhang Jianhua
Published: August 2022

The full‐solution‐processed oxide thin‐film transistor (TFT) array is successfully realized by using ultrafast scanning diode laser annealing (USDLA). It integrates all solution‐processed functional thin films well, including low‐electrical‐resistivity transparent conductive indium‐tin‐oxide (ITO) thin film, high‐k dielectric hafnium‐aluminum‐oxide (HAO) thin film, and high‐quality semiconductor tungsten‐zinc‐tin‐oxide (WZTO) thin film. And the stacked multilayer thin films as a whole exhibit a smooth surface with the root mean square (RMS) roughness of 0.293 nm. The full‐solution‐processed TFT array exhibits a uniform overall TFT device performance, the average values including subthreshold swing of 118 mV dec−1, threshold voltage of −0.45 V, and mobility of 12 cm2 V−1 s−1. Moreover, the full‐solution‐processed TFTs have good bias illumination stability, especially the VT shift of the PBIS and NBIS are only 0.09 and 0.4 V, respectively. The result implies that the USDLA technique can meet the large‐scale fabrication of full‐solution‐processed TFTs and provide a solid path to low‐cost high‐performance and large‐scale electronics.
Bromide‐Mediated Reduction Kinetics and Oxidative Etching for Manipulating the Twin Structure and Facet of Pd Nanocrystals for Catalysis
Authors: Hsieh Chia‐Jui , Liu Yi‐Hong , Tsao Chi‐Yen , Lin Jui‐Tai , Chi Chong‐Chi , Chang Chun‐Wei , Hsiao Yueh‐Chun , Wu Cheng‐Yu , Yang Tung‐Han
Published: August 2022

With Pd as an example, a set of quantitative analyses is designed to shed light on the bromide‐mediated reduction kinetics and oxidative etching in determining the twin structure and facet of Pd nanocrystals. The success of this work relies on the kinetic measurements of Pd(II) precursor reduction and the close examinations of resultant Pd seeds and nanocrystals at different stages of synthesis. We observe there is a clear trend where low, moderate, and high initial Pd(II) reduction rates regulated by Br− ions correspond to the formation of Pd seeds with singly‐twinned, multiply‐twinned, and single‐crystal structures in the nucleation stage, respectively. Our quantitative analyses also suggest the oxidative etching induced by oxygen/Br− pair can selectively remove the multiply‐twinned Pd seeds from the products in the growth stage while leaving behind singly‐twinned or single‐crystal Pd seeds for the evolution into Pd nanocrystals with well‐defined facets in high purity. The mechanistic insights obtained in this work can be extended to the synthesis of Pd@Pd−Pt core−shell nanocubes with high‐index facets, which can be used as excellent electrocatalysts and photocatalysts for hydrogen generation.
Core‐Shell Se‐Doped TiO2@Carbon Nanotubes for High‐Performance Sodium‐Ion Batteries
Authors: Yao Menglong , Gao Ang , Chen Ruochen , He Qiangrui , Yao Tianhao , Wang Hongkang
Published: August 2022

Titanium dioxide (TiO2) has been considered as a promising anode material for sodium‐ion batteries (SIBs), because of its abundance, safety and eco‐friendliness. However, the inferior electronic conductivity and low sodium ion diffusion rate of TiO2 hinder its improvement of electrochemical performance. To overcome these drawbacks, herein, core‐shell Se‐doped TiO2@carbon nanotubes (denoted as Se‐TiO2@CNTs) are successfully designed and fabricated, in which the TiO2 nanoparticle aggregated shells are conformally coated on the carbon nanotubes, while the metallic Se species are physically confined within the meso/micropores. When examined as a SIB anode, the Se‐TiO2@CNTs electrode demonstrates excellent sodium storage performance, correspondingly delivering high reversible capacities of 222.7/208.5 mA h g−1 after 200/1000 cycles at current densities of 0.2/1.0 A g−1, and even a capacity of 140.2 mA h g−1 after 4500 cycles at a high‐rate of 5.0 A g−1. The high reversible capacity, long‐term cycling stability, and high‐rate capability of the Se‐TiO2@CNTs can be owing to the unique structure characteristics, as the hollow/porous structure with high specific surface area of 335.4 m2 g−1 efficiently shortens the Na+ diffusion length and facilitates the electrolyte penetration, while Se‐doping and carbon supporting greatly enhance the electronic conductivity of the Se‐TiO2@CNTs electrode.
Synergetic Pt Atoms and Nanoparticles Anchored in Standing Carbon‐Derived from Covalent Organic Frameworks for Catalyzing ORR
Authors: Zhou Mingan , Liu Minghao , Miao Qiyang , Shui Hengfu , Xu Qing
Published: August 2022

Oxygen reduction reaction (ORR) plays key roles in fuel cells and metal air batteries. Covalent organic frameworks (COFs)‐derived carbons have been utilized for catalyzing ORR. However, the activity and selectivity for these catalysts in the acidic medium is still under improved. In this work, Pt atoms and uniform Pt nanoparticles supported by standing carbons are derived from a three‐dimensional COF. With increasing the contents of Pt ions, the corresponding particle sizes show obvious decrease, and thus resulting in higher catalytic activity. The synergetic roles between Pt atoms and nanoparticles with average sizes of 6.19 nm make catalyst show remarkable activity toward ORR, with onset potential and half‐wave potential of 0.98 and 0.85 V (vs RHE) in the acidic medium, which are 70 and 40 mV more positive than those of Pt/C, respectively. This work provides a new insight for developing COFs in energy storage and conversion systems.
Active Buffer Matrix in Nanoparticle‐Based Silicon‐Rich Silicon Nitride Anodes Enables High Stability and Fast Charging of Lithium‐Ion Batteries
Authors: Kilian Stefan O. , Wankmiller Björn , Sybrecht Anna Margarete , Twellmann Jonas , Hansen Michael Ryan , Wiggers Hartmut
Published: August 2022

A very promising way to improve the stability of silicon in lithium‐ion battery (LIB) anodes is the use of nanostructured silicon‐rich silicon nitride (SiNx), known as a conversion‐type anode material. To investigate the conversion mechanism in this material in detail, SiN0.5 nanoparticles are synthesized and examined as LIB anodes using a combination of ex situ X‐ray photoelectron spectroscopy and solid‐state 7Li MAS NMR measurements. During the initial cycle, the conversion of SiN0.5 nanoparticles results in the formation of lithium silicides and a buffer matrix consisting of different lithium nitridosilicates and lithium nitride. These phases can be reversibly lithiated and contribute to the total reversible capacity of the silicon nitride active material. The structure of the material after conversion is best described by an amorphous solid solution. Further, it is shown that silicon‐rich silicon nitrides possess improved rate capability because of the higher ionic conductivity of the buffer matrix compared to pure silicon, and very fine dispersion of silicon clusters throughout the buffer matrix. Thus, unlike most conversion materials, the silicon‐rich silicon nitride exhibits an additional intrinsic active functionality of the buffer matrix that goes far beyond the mere reduction of electrolyte contact area and volume expansion.
One‐Dimensional Photonic Crystal for Surface Mode Polarization Control
Authors: Mogni Erika , Pellegrini Giovanni , Gil‐Rostra Jorge , Yubero Francisco , Simone Giuseppina , Fossati Stefan , Dostálek Jakub , Martínez Vázquez Rebeca , Osellame Roberto , Celebrano Michele , Finazzi Marco , Biagioni Paolo
Published: August 2022

Bloch surface waves sustained by truncated 1D photonic crystals (1DPCs) are well known tools for surface‐enhanced spectroscopy. They provide strongly confined fields with uniform distribution over a large surface area, a characteristic exploited in standard refractometric sensing. However, their application to polarization‐sensitive investigations is not straightforward because the transverse electric (TE) and magnetic (TM) surface modes possess distinct dispersion relations, therefore their relative phase is not conserved along propagation and the polarization state of any wave obtained by combining these modes is ill‐defined. In this work, a novel design of a 1DPC is realized in which the TE and TM modes exhibit the same phase velocity over a broadband spectral range and thus their dispersion relations overlap. The capability to simultaneously excite TE and TM modes with a well‐defined phase relation allows the generation of surface waves with a controlled polarization state. This paves the way to polarization‐resolved surface‐enhanced analysis, including, for example, linear and circular dichroism spectroscopy of grafted molecular layers at the photonic crystal surface.
Non‐Interleaved Polarization‐Frequency Multiplexing Metasurface for Multichannel Holography
Authors: Gou Yue , Ma Hui Feng , Wu Liang Wei , Sun Shi , Wang Zheng Xing , Cui Tie Jun
Published: August 2022

In order to enhance channel capacity in modern wireless communications, diverse multiplexing techniques, such as polarization, frequency, and spatial multiplexing, are proposed and implemented. Here, a non‐interleaved polarization‐frequency multiplexing metasurface is proposed, which can realize independent controls of orthogonal linearly polarized or circularly polarized waves in two frequency bands to achieve four independent information channels. As a proof of concept, the metasurfaces that can independently realize four different polarized holographic images in two frequency bands are designed, simulated, and measured. The results show that two orthogonally polarized holographic images are achieved in each frequency band, respectively, which can be either linear or circular polarization. Benefitting from the advantages of non‐interleaved design, the proposed metasurfaces can reach not only high information capacity but also high information density by taking full use of the metasurface apertures.
Binary Ligand‐Mediated Photochromic Tuning of Lanthanide‐Doped Upconversion Nanoparticle Conjugates
Authors: Peng Chenxi , Chen Xue , Suh Yung Doug , Liu Xiaowang
Published: August 2022

The ability to tune photochromic features of nanoparticle (NP)‐ligand conjugates can vastly extend the utility of dynamic materials in the fields of drug delivery, bioimaging, and data storage. Herein, the photochromic tuning of lanthanide‐doped upconversion nanoparticle (UCNP)‐spiropyran (SP) conjugates through a binary ligand strategy is reported. It is found that the content of SP ligand on the surface of UCNPs can be rationally controlled by an SP‐to‐oleate ligand exchange reaction, allowing for regulating the steric congestion in the ligand layer. A highly congested SP layer not only leads to an ultralong lifetime for the purple open‐ring state but also results in improved red fluorescence under UV excitation. The enhancement in steric congestion further enables increased activation energy for the ring‐opening reaction for the bound SP ligand, permitting the generation of high‐resolution self‐erasing patterns in a UCNP‐SP conjugate‐doped polydimethylsiloxane film by local irradiation with either UV or near‐infrared light. The findings provide new insights into the optical tuning of nanoconjugates by controlling the conformational dynamics of their mixed ligand layers.
Near‐Infrared Optical Sensing of Biomacromolecules with Upconversion Nanoplatforms
Authors: Yan Liben , Wang Zhimin
Published: August 2022

Optical sensing and imaging have perceived massive success in biomedical analysis and disease diagnosis in terms of minimal invasiveness, good sensitivity, high accuracy, and time‐/cost‐effectiveness. Upconversion nanoparticles (UCNPs) as a kind of promising luminescent material hold many merits like unique frequency‐converting capability, emission fine‐tuning, low auto‐fluorescence interference, good tissue‐penetration ability, high photostability, and excellent biocompatibility, which are widely applied for optical sensing of diverse chemically or biologically derived analytes. Extensive efforts are dedicated to the rational fabrication of reliable upconversion nanoplatforms (UCNs) through ingenious modulation of the luminescent energy transfer process for various optical biosensing applications. Herein, the advancement of biomacromolecules (e.g., nucleic acids, proteins, and enzymes) detection using multiplex UCNs from on‐paper platforms to in‐solution as well in living systems is specifically focussed. Detailed summarizations of the probe design strategy, responsive mechanisms, and sensing performance have been presented. In addition, based on the current research achievements, the challenges and future perspectives are emphasized to facilitate further clinical sensing utilizations with upconversion photonic technology.
Synthesis of Substituted Pyrimido[1,2‐b]indazoles through (3+2+1) Cyclization of 3‐Aminoindazoles, Ketones, and N,N‐Dimethylaminoethanol as One‐Carbon Synthon
Authors: Qin Zemin , Ma Renchao , Ying Shenpeng , Li Fanzhu , Ma Yongmin
Published: August 2022

2‐Mono‐ or 2,3‐disubstituted pyrimido[1,2‐b]indazoles are synthesized by a (3+2+1) three‐component cyclization of 3‐aminoindazoles, ketones, and N,N‐dimethylaminoethanol as a methine source. The reaction demonstrates good tolerance of both aromatic and aliphatic ketones, as well as various substitution patterns in air. A plausible mechanism is discussed.

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Photoredox and Copper‐Catalyzed Sulfonylphosphorothiolation of Alkenes toward β‐Sulfonyl Phosphorothioates
Authors: Zhang Pengbo , Li Wenwu , Zhu Xianglong , Li Ying , Zhao Xiangmei , Shi Saige , Zhu Fengxiang , Lin Jinming , Gao Xia
Published: August 2022

A photoredox and copper‐catalyzed sulfonylphosphorothiolation of alkenes has been developed. With the use of readily available aryl or alkyl sulfonyl chlorides as radical precursors and (RO)2P(O)SH as coupling partners, a wide range of decorated β‐sulfonyl phosphorothioates could be obtained in 37–98% yields with good functional group tolerance. Importantly, this three‐component reaction can be conveniently extended to late‐stage modification of bioactive molecules and gram‐scale synthesis.

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A Many‐Body Perturbation Theory Approach to Energy Band Alignment at the Crystalline Tetracene–Silicon Interface
Authors: Klymenko Mykhailo V. , Tan Liang Z. , Russo Salvy P. , Cole Jared H.
Published: August 2022

Hybrid inorganic–organic semiconductor (HIOS) interfaces are of interest for new photovoltaic devices operating above the Shockley–Queisser limit. Predicting energy band alignment at the interfaces is crucial for their design, but represents a challenging problem due to the large scales of the system, the energy precision required and a wide range of physical phenomena that occur at the interface. To tackle this problem, many‐body perturbation theory in the non‐self‐consistent GW approximation, orbital relaxation corrections for organic semiconductors, and line‐up potential method for inorganic semiconductors which allows for tractable and accurate computing of energy band alignment in crystalline van‐der‐Waals hybrid inorganic–organic semiconductor interfaces are used. In this work, crystalline tetracene physisorbed on the clean hydrogen‐passivated 1 × 2 reconstructed (100) silicon surface is studied. Using this computational approach, it is found that the energy band alignment is determined by an interplay of the mutual dynamic dielectric screening of two materials and the formation of a dipole layer due to a weak hybridization of atomic/molecular orbitals at the interface. The significant role of the exchange‐correlation effects in predicting band offsets for the hybrid inorganic–organic semiconductor interfaces is also emphasized.
First‐Principles Investigation of Phase Stability in Substoichiometric Zirconium Carbide under High Pressure
Authors: Thiel Scott D. , Walsh James P. S.
Published: August 2022

NaCl‐type carbides of the early transition metals can exhibit a substantial sub‐stoichiometry at the carbon site, impacting a host of bulk properties that depend upon carbon concentration including melting points, mechanical and elastic properties, and superconducting transition temperatures. Unfortunately, control over vacancies remains challenging with current preparation methods, motivating the search for new synthetic approaches that will allow for the prescription of specific vacancy configurations. Here, density functional theory is augmented with alloy cluster expansion to examine the structure and zero kelvin enthalpy of millions of structures across composition and pressure space. The results are used to examine how extreme pressures might be used to access novel ordered and disordered phases of ZrC, many of which have been calculated to be thermodynamically stable yet remain synthetically elusive. High pressure is shown to significantly reduce sub‐stoichiometry and drive the system toward fully stoichiometric ZrC. They examine the root of these changes and find that pressure exerts an influence over the distribution and abundance of specific nearest‐neighbor vacancy pairs. These results suggest that pressure is a powerful tool for the control of vacancies, and can offer a new synthetic handle on the bulk properties exhibited in this industrially important class of materials.
Tuning Ambipolarity of the Conjugated Polymer Channel Layers of Floating‐Gate Free Transistors: From Volatile Memories to Artificial Synapses
Authors: Yang Yu‐Ting , Wu Ying‐Sheng , He Waner , Tien Hsin‐Chiao , Yang Wei‐Chen , Michinobu Tsuyoshi , Chen Wen‐Chang , Lee Wen‐Ya , Chueh Chu‐Chen
Published: August 2022

Three‐terminal synaptic transistor has drawn significant research interests for neuromorphic computation due to its advantage of facile device integrability. Lately, bulk‐heterojunction‐based synaptic transistors with bipolar modulation are proposed to exempt the use of an additional floating gate. However, the actual correlation between the channel's ambipolarity, memory characteristic, and synaptic behavior for a floating‐gate free transistor has not been investigated yet. Herein, by studying five diketopyrrolopyrrole–benzotriazole dual‐acceptor random conjugated polymers, a clear correlation among the hole/electron ratio, the memory retention characteristic, and the synaptic behavior for the polymer channel layer in a floating‐gate free transistor is described. It reveals that the polymers with balanced ambipolarity possess better charge trapping capabilities and larger memory windows; however, the high ambipolarity results in higher volatility of the memory characteristics, namely poor memory retention capability. In contrast, the polymer with a reduced ambipolarity possesses an enhanced memory retention capability despite showing a reduced memory window. It is further manifested that this enhanced charge retention capability enables the device to present artificial synaptic characteristics. The results highlight the importance of the channel's ambipolarity of floating‐gate free transistors on the resultant volatile memory characteristics and synaptic behaviors.
Implementing Complex Oxides for Efficient Room‐Temperature Spin–Orbit Torque Switching
Authors: Tang Aihua , Xu Teng , Liu Shengsheng , Liang Yuhan , Chen Hetian , Yan Dayu , Shi Youguo , Yu Pu , Yu Rong , Lin Yuanhua , Nan Tianxiang , Jiang Wanjun , Yi Di
Published: August 2022

Complex oxides hosting 4d and 5d cations with significant spin–orbit coupling have recently been shown as promising materials for efficient spin‐charge interconversion. Through interfacing 4d and 5d oxides with magnet layers, a large spin–orbit torque (SOT) is reported. However, a room‐temperature SOT switching of perpendicular magnetization by using these oxides, which is essential for spintronic devices, is not demonstrated. Here, this is addressed yet missing aspect by studying heterostructures comprised of two representative complex oxides (4d SrRuO3 and 5d SrIrO3) and a compensated ferrimagnet FeGd with perpendicular magnetic anisotropy. A room temperature current‐induced SOT switching of perpendicular magnetization in both SrRuO3/FeGd and SrIrO3/FeGd bilayers, with the critical switching current density on the order of 106 A cm−2 is demonstrated. The SOT efficiencies of SrRuO3 and SrIrO3 are further quantified by using harmonic Hall voltage measurements. The results suggest that the strongly correlated oxides could be another promising platform for enabling energy‐efficient spin‐orbitronic applications.
Impact of the COVID‐19 pandemic on colorectal cancer surgery in Japan: Clinical Study Group of Osaka University―A multicenter retrospective study
Authors: Miyo Masaaki , Mizushima Tsunekazu , Nishimura Junichi , Hata Taishi , Tei Mitsuyoshi , Miyake Yuichiro , Kagawa Yoshinori , Noura Shingo , Ikenaga Masakazu , Danno Katsuki , Ogawa Atsuhiro , Chinen Yoshinao , Hata Tsuyoshi , Miyoshi Norikatsu , Takahashi Hidekazu , Uemura Mamoru , Yamamoto Hirofumi , Murata Kohei , Doki Yuichiro , Eguchi Hidetoshi ,   Clinical Study Group of Osaka University Colorectal Group
Published: August 2022

Aim

Due to the overwhelming spread of SARS‐CoV‐2 and its disruption of the healthcare system, delays and reduced numbers were reported for colorectal cancer screening, colonoscopies, and surgery during the COVID‐19 pandemic. This multicenter retrospective study investigated the still poorly understood impact of the COVID‐19 pandemic on colorectal cancer treatment in Japan.

Methods

This study was organized by the Clinical Study Group of Osaka University, which comprised 32 major institutions in Osaka. We retrospectively analyzed the number of surgeries and colonoscopies performed and the characteristics of patients who underwent surgery for colorectal cancer between March 2019 and February 2021. We compared data collected before and during the COVID‐19 pandemic. We also assessed the methods used for detecting colorectal cancer, including fecal occult blood test, abdominal symptoms, and anemia.

Results

The COVID‐19 pandemic caused reductions in the annual numbers of surgeries (3569 vs 3198) and colonoscopies (67 622 vs 58 183) performed in the 2020 fiscal year, compared to the 2019 fiscal year. During the COVID‐19 pandemic, a significantly lower proportion of patients were treated for clinical stages ≤I (24.2% vs 26.9%; P = .011), compared to the proportion treated before the pandemic. Fecal occult blood tests for detecting colorectal cancer were used significantly less frequently during the COVID‐19 pandemic (26.2% vs 29.6%; P = .002). These trends were more significant in larger institutions.

Conclusion

The COVID‐19 pandemic reduced the number of colonoscopies and surgeries performed for colorectal cancer and hindered the detection of asymptomatic early‐stage cancers, and its impact varied by hospital size.
Objective evaluation of facial features in Congolese newborns by facial measurements. The need for population‐specific measurements
Authors: Mubungu Gerrye , Roelants Mathieu , Lumaka Aimé , Makay Prince , Tshika Dahlie , Lubala Toni , Tshilobo Lukusa Prosper , Devriendt Koenraad
Published: August 2022

The evaluation of dysmorphism is often subjective because many continuous traits are not easily measured or lack normal values. Because many common morphologic profiles vary between populations, population‐specific reference ranges of relevant traits are needed. We aim to evaluate the objective assessment of facial dysmorphism in 553 Congolese newborns based on facial measurements. Measurements taken with a ruler were on average larger compared to those with a caliper, but the bias did not depend on the size of the measurement. We therefore introduced a correction factor that allows to use both techniques for facial measurements interchangeably in future studies. The outer canthal distance, palpebral fissure length, and mouth width were significantly larger in Congolese newborns (respectively mean 6.59 [SD 0.48]; mean 2.20 [SD 0.24]; mean 2.78 [SD 0.26]) when compared to references based on European newborns (respectively mean 3.59 [SD 1.76]; mean 4.20 [SD 2.26]; mean 0.47 [SD 1.21]), while the rest of measurements were significantly smaller. The interpupillary distance (IPD) calculated from inner canthal distance and outer canthal distance was not significantly different. We observed a poor agreement between clinical evaluation and measured features (kappa of 0.432). Clinicians were more likely to recognize a face as having wide‐spaced eyes when it had been recognized as such during the clinical examination, more than if the child had a high interpupillary distance. This suggests that the measured IPD is not precisely reflecting what is clinically evaluated as wide‐spaced eyes.
Expanding the genotypic and phenotypic landscapes of rhizomelic chondrodysplasia punctata type 3 (RCDP3) with two novel families, and a review of the literature
Authors: İli Ezgi Gökpınar , Gezdirici Alper , Di Pietro Erminia , Yergeau Christine , Braverman Nancy
Published: August 2022

Rhizomelic chondrodysplasia punctata (RCDP) are a group of peroxisomal disorders caused by plasmalogen synthesis defects. Patients with RCDP present with rhizomelic short stature, characteristic punctate epiphyseal calcifications, congenital cataracts, severe intellectual disability, seizures, and facial dysmorphism. Pathogenic variants in AGPS result in RCDP type 3 (RCDP3) which is an extremely rare disorder characterized by isolated ADHAPS deficiency. Six patients with RCDP3 have been identified, upto‐date. We report two new patients with RCDP3 and their novel variants, c.154dupG (p.Ala52GlyfsTer6) and c.637+1G>A, in the AGPS gene. We also present a review of previously reported RCDP3 patients.
Polycyclic Hydrocarbons from [4n]Annulenes: Correlation versus Hybridization Forces in the Formation of Diradicaloids
Authors: Moles Quintero Sergio , Haley Michael M. , Kertesz Miklos , Casado Juan
Published: August 2022

The conceptual connections between [4n] Hückel antiaromaticity, disjoint orbitals, correlation energy, pro‐aromaticity and diradical character for a variety of extended π‐conjugated systems, including some salient recent examples of nanographenes and polycyclic aromatic radicals, are provided based on their [4n]annulene peripheries. The realization of such structure–property relationships has led to a beneficial pedagogic exercise establishing design guidelines for diradicaloids. The antiaromatic fingerprint of the [4n]annulene peripheries upon orbital interactions due to internal covalent connectors gives insights into the diradicaloid property of a diversity of π‐conjugated molecules that have fascinated chemists recently.
New polyimides containing methyl benzamidobenzoate or dimethyl benzamidoisophthalate as bulky pendant groups. Effects on solubility, thermal and gas transport properties
Authors: Terraza Claudio A. , Cruz Yennier , Rodríguez Ary , Velázquez‐Tundidor María Victoria , Hauyon René A. , Rodríguez‐González Fidel E. , Niebla Vladimir , Aguilar‐Vega Manuel , Sulub‐Sulub Rita , Coll Deysma , Ortiz Pablo A. , Pérez Yasmín P. , Comesaña‐Gándara Bibiana , Tundidor‐Camba Alain
Published: August 2022

This work reports the synthesis of six new polyimides obtained by the reaction of two novel diamine monomers: methyl 4‐(3,5‐diaminobenzamido)benzoate and dimethyl 5‐(3,5‐diaminobenzamido)isophthalate, bearing one or two methyl ester groups in their phenyl rings, respectively, with three known dianhydrides, 4,4′‐(hexafluoroisopropylidene) diphatalic anhydride (6FDA), 4,4′‐(dimethylsilanediyl) dipthalic anhydride (SiDA) and 4,4′‐oxydiphthalic anhydride (ODPA). The polyimides were synthesized using the “two‐step” method, which first involves forming a poly(amic acid) precursor that is subsequently cyclodehydrated to form the imide linkage. The yields were higher than 95% in all cases, and the structural characterization was performed by spectroscopic techniques like FT‐IR, 1H, 13C, and 29Si NMR. In addition, the effect on the solubility in common organic solvents and thermal and gas transport properties of these polyimides were studied as a function of the nature of the respective side group and the dianhydride used.
Influence of different stirring setups on mass transport, gas hydrate formation, and scale transfer concepts for technical gas hydrate applications
Authors: Filarsky Florian , Hagelstein Maurice , Schultz Heyko J.
Published: August 2022

This contribution describes the influence of turbulent flow conditions in the liquid and/or gas phase and directly in the phase interface, different flow patterns (axial/radial), volume‐specific power inputs, mass‐specific energy consumptions, as well as volume‐specific mass transfer coefficients on the gas hydrate formation, derived from an experimental investigation of five different reactor setups. The results correspond to all fields of gas hydrate research, especially actually discussed technical hydrate applications, like hydrate‐based desalination, gas storage, gas separation, biogas and green hydrogen handling, carbon dioxide deposition, new phase transfer materials, and even electrical power supply. Two main objectives, first, to determine favorable hydrate forming conditions in stirred systems to provide competitive hydrate formation processes, and second, the search for a concept to enable the transfer of experimental results, for example, from a stirred reactor to a pipeline system for inhibitor research, through the targeted adjustment of similar and comparable turbulent flow conditions in different reactor setups could be achieved. So far, the targeted formation of gas hydrates has been investigated essentially from the point of view of optimizing the formation conditions with regard to pressure and temperature as well as the addition of auxiliary materials and promoters. In addition, some studies consider different reactor types and setups, for example, spray reactors or bubble columns. In many publications, stirred and cooled pressure autoclaves are described, whereby the gas and the liquid phase are brought into contact with each other by mixing to a greater or lesser extent by an agitator, then forming a solid gas hydrate phase. Often missing in previous research work is a systematic approach for determining the influence of flow conditions on gas hydrate formation. Many different influencing factors in a stirred reactor system can strongly affect the kinetics and formation of gas hydrates, for example, stirrer type, rotational frequency, stirrer and reactor geometry, and filling level. This is the starting point of the present investigation that deals with the influence of the flow conditions on the formation of gas hydrates. Tests were performed in a stirred autoclave to measure the effects of different stirrer configurations. The results obtained contribute to the explanation of the hydrate formation mechanism and can be used to optimize the targeted production of gas hydrates in technical hydrate applications. A rapid, immediate, hydrate formation is advantageous and can be achieved by suitable flow conditions in stirred reactors, which is successfully proven within this study contribution.