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Nature Communications · 2020 ·Vol. 11 ·期 1 ·1-7 · IF 12.121

Cooperative excitonic quantum ensemble in perovskite-assembly superlattice microcavities

Zhou Chun,Zhong Yichi,Dong Hongxing,Zheng Weihao,Tan Jiqing,Jie Qi,Pan Anlian,Zhang Long,Xie Wei

Perovskites—compounds with the CaTiO 3 -type crystal structure—show outstanding performance in photovoltaics and multiparameter optical emitters due to their large oscillator strength, strong solar absorption, and excellent charge-transport properties. However, the ability to realize and control many-body quantum states in perovskites, which would extend their application from classical optoelectronic materials to ultrafast quantum operation, remains an open research topic. Here, we generate a cooperative quantum state of excitons in a quantum dot ensemble based on a lead halide perovskite, and we control the ultrafast radiation of excitonic quantum ensembles by introducing optical microcavites. The stimulated radiation of excitonic quantum ensemble in a superlattice microcavity is demonstrated to not be limited by the classical population-inversion condition, leading to a picosecond radiative duration time to dissipate all of the in-phase dipoles. Such a perovskite-assembly superlattice microcavity with a tunable radiation rate promises potential applications in ultrafast, photoelectric-compatible quantum processors.

研究领域: 材料科学 · 光学 · 量子物理
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International Journal of Extreme Manufacturing · 2024 ·Vol. 6 ·期 5 ·055002 · IF 16.1

Femtosecond laser ultrafast photothermal exsolution

Lurun Xu,Jingchao Tao,Zhuguo Li,Guo He,Dongshi Zhang

Exsolution, as an effective approach to constructing particle-decorated interfaces, is still challenging to yield interfacial films rather than isolated particles. Inspired by in vivo near-infrared laser photothermal therapy, using 3 mol% Y2O3 stabilized tetragonal zirconia polycrystals (3Y-TZP) as host oxide matrix and iron-oxide (Fe3O4/γ-Fe2O3/α-Fe2O3) materials as photothermal modulator and exsolution resource, femtosecond laser ultrafast exsolution approach is presented enabling to conquer this challenge. The key is to trigger photothermal annealing behavior via femtosecond laser ablation to initialize phase transition from monoclinic zirconia (m-ZrO2) to tetragonal zirconia (t-ZrO2) and induce t-ZrO2 columnar crystal growth. Fe-ions rapidly segregate along grain boundaries and diffuse towards the outmost surface, and become 'frozen', highlighting the potential to use photothermal materials and ultrafast heating/quenching behaviors of femtosecond laser ablation for interfacial exsolution. Triggering interfacial iron-oxide coloring exsolution is composition and concentration dependent. Photothermal materials themselves and corresponding photothermal transition capacity play a crucial role, initializing at 2 wt%, 3 wt%, and 5 wt% for Fe3O4/γ-Fe2O3/α-Fe2O3 doped 3Y-TZP samples. Due to different photothermal effects, exsolution states of ablated 5 wt% Fe3O4/γ-Fe2O3/α-Fe2O3-doped 3Y-TZP samples are totally different, with whole coverage, exhaustion (ablated away) and partial exsolution (rich in the grain boundaries in subsurface), respectively. Femtosecond laser ultrafast photothermal exsolution is uniquely featured by up to now the deepest microscale (10 μm from 5 wt%-Fe3O4-3Y-TZP sample) Fe-elemental deficient layer for exsolution and the whole coverage of exsolved materials rather than the formation of isolated exsolved particles by other methods. It is believed that this novel exsolution method may pave a good way to modulate interfacial properties for extensive applications in the fields of biology, optics/photonics, energy, catalysis, environment, etc.

CAS / MDL: 1309-37-1 1317-61-9
研究领域: 材料科学 · 光学 · 生物医学工程
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Metals · 2023 ·Vol. 13 ·期 4 ·677 · IF 2.9

Preparation of Porous Composite Phase Na Super Ionic Conductor Adsorbent by In Situ Process for Ultrafast and Efficient Strontium Adsorption from Wastewater

Yuliang Chen,Xiangbiao Yin,Hao Fu,Zheyang Lin,Guangcan Ma,Xinpeng Wang,Qingsong Wang,Fangqiang Chen

Strontium, the main component of radioactive nuclear wastewater, is characterized by a high fission yield and an extended half-life. It is easily absorbed by the human body, thus greatly threatening the environment and the human body. In this study, a mesoporous composite phase sodium superionic conductor (NVP@NMP) was synthesized by the droplet template method, and the rapid capture of Sr2+from wastewater was achieved by constructing a nano-heterogeneous interface to increase the ion diffusion rate. NVP@NMP showed efficient and rapid removal of strontium ions in adsorption kinetics, isothermal adsorption, solution pH, and interfering ions concentration tests, especially using the equilibrium time of 2 min for strontium absorption by NVP@NMP and a maximum theoretical adsorption capacity of 361.36 mg/g. The adsorption process was spontaneous, endothermic, and feasible. At higher concentrations of other competing ions (Na, K, Ca, Mg, and Cs), the adsorbent exhibited higher selectivity towards Sr2+.TEM, XPS, and XRD analyses revealed that ion exchange was the main mechanism for the NVP@NMP ultrafast adsorption of Sr2+. In this research, we investigated the feasibility of ultrafast strontium capture by sodium superionic conductor structured phosphates and explained the ultrafast strontium adsorption mechanism of NASICON materials through XPS.Keywords:NASICON;ultrafast adsorption;strontium;ion exchange;wastewater

研究领域: 环境科学 · 材料科学
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Nature Communications · 2023 ·Vol. 14 ·期 1 ·1-9 · IF 16.6

Simultaneously ultrafast and robust two-dimensional flash memory devices based on phase-engineered edge contacts

Yu Jun,Wang Han,Zhuge Fuwei,Chen Zirui,Hu Man,Xu Xiang,He Yuhui,Ma Ying,Miao Xiangshui,Zhai Tianyou

As the prevailing non-volatile memory (NVM), flash memory offers mass data storage at high integration density and low cost. However, due to the ‘speed-retention-endurance’ dilemma, their typical speed is limited to ~microseconds to milliseconds for program and erase operations, restricting their application in scenarios with high-speed data throughput. Here, by adopting metallic 1T-Li x MoS 2 as edge contact, we show that ultrafast (10–100 ns) and robust (endurance>10 6 cycles, retention>10 years) memory operation can be simultaneously achieved in a two-dimensional van der Waals heterostructure flash memory with 2H-MoS 2 as semiconductor channel. We attribute the superior performance to the gate tunable Schottky barrier at the edge contact, which can facilitate hot carrier injection to the semiconductor channel and subsequent tunneling when compared to a conventional top contact with high density of defects at the metal interface. Our results suggest that contact engineering can become a strategy to further improve the performance of 2D flash memory devices and meet the increasing demands of high speed and reliable data storage.

研究领域: 材料科学 · 电子工程
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JOURNAL OF CHEMICAL PHYSICS · 2024 ·Vol. 160 ·期 24 · IF 3.1

Ultrafast excited state intramolecular proton transfer and isomerization of long-chain linked Schiff bases

Wang Ye,Wang Dongdong,Hu Xiao,Zhang Song

The ultrafast proton transfer and the following dynamics for aromatic Schiff bases N , N ′-bis(salicylidene)ethylenediamine (salen) and N , N ′-bis(salicylidene)-1,4-butylenediamine (salbn) were investigated with experimental and theoretical methods. A dual emission property with a large Stokes shift in salen and salbn indicates that excited state intramolecular proton transfer occurs with photoexcitation. An efficient single proton transfer was confirmed within 200 fs for both molecules. Subsequently, a fast twisted motion of the keto moiety carries cis -keto to a relaxed stable geometry in the S 1 state. Following the twisted motion, the phenol ring at keto moiety further rotates to a conical intersection with the ground state and a cis – trans isomerization occurs. The isomerization rate is high, which dominates the competition with the radiative transition, resulting in weak emission intensity. It is confirmed that the length of alkyl chain affects the direction of phenol ring twisting and rotation during the whole subsequent relaxation of excited cis -keto tautomer. Compared with polar solvent acetonitrile, the barrier of isomerization is higher and the hydrogen bond on keto moiety is stronger in nonpolar solvent toluene. It makes fluorescence radiation channels competing with isomerism more likely to occur, contributing to the observed difference of enol/keto emission ratios of salen and salbn in toluene and acetonitrile.

研究领域: 物理化学 · 理论化学 · 光化学
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ANALYTICAL CHEMISTRY · 2024 · IF 6.7

Target-Triggered Ultrafast Chondroitin Gelation Enabled Power-Free and Point-of-Care Bioassays

Chunjiao Qi,Jintao Chen,Yuhui Shang,Yu Yang,Kangyan Wang,Jinyang Chen

Point-of-care (POC) tests increasingly highlight the importance of portable, cost-effective, and visually quantitative detection of biomarkers. Herein, we developed a power-free and visual signal-readout POC sensor based on the target-triggered ultrafast gelation process. In the gelation process, the target triggered the cascade reaction catalyzed by oxidase and ferrous glycinate to produce carbon radicals that immediately initiated the rapid polymerization and cross-linking of acryloylated chondroitin sulfate and dimethylacrylamide. This highly efficient enzymatic polymerization process contributed to the ultrafast generation of chondroitin hydrogel within 1 min at 25 °C. The increase in viscosity of aqueous solution resulted from hydrogel formation was then visually measured according to the distance of solution migration on a tick-labeled pH test strip, which thus realized the quantification of a target. By utilizing glucose oxidase as an oxidase model during the gelation process, this POC sensor was successfully employed in the rapid quantitative detection of glucose without the need for any auxiliary instruments. Benefiting from the specificity and stability of the enzymatic polymerization reaction, the sensor exhibited excellent performance in the detection of glucose in clinical blood samples. Moreover, the sensor was further extended to uric acid detection and enabled accurate assay in clinical urine samples, which indicated the versatility and practicability of this sensor in the POC test.

研究领域: 生物化学 · 医学诊断 · 材料科学
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2018 · IF 2.88

Ultra-fast zinc ion detection in living cells and zebrafish by a light-up fluorescent probe

Zhengliang Lu,Yanan Lu,Wenlong Fan,Chunhua Fan,Yanan Li

As the second most abundant transition metal after iron in biological systems, Zn 2+ takes part in various fundamental life processes such as cellular metabolism and apoptosis, neurotransmission. Thus, the development of analytical methods for fast detection of Zn 2+ in biology and medicine has been attracting much attention but still remains a huge challenge. In this report, we develop a novel Zn 2+ -specific light-up fluorescent probe based on intramolecular charge transfer combined with chelation enhanced fluorescence induced by structural transformation. Addition of Zn 2+ in vitro can induce a remarkable color change from colorless to green and a strong fluorescence enhancement with a red shift of 43 nm. Moreover, the probe shows an extremely low detection limit of 13 nM and ultra-fast response time of less than 1 s. The Zn 2+ sensing mechanism was fully supported by TDDFT calculations as well as HRMS and 1 H NMR titrations . The recognition of Zn 2+ in living Hela cells as well as the MTT assay demonstrate that the probe can rapidly light-up detect Zn 2+ in vivo with low cytotoxicity and good cell-permeability. Furthermore, the probe can also be successfully applied to bioimaging Zn 2+ in living zebrafish.

研究领域: 生物化学 · 医学 · 分析化学
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JOURNAL OF CHEMICAL PHYSICS · 2024 ·Vol. 160 ·期 16 · IF 3.1

Photogenerated carrier dynamics of Mn2+ doped CsPbBr3 assembled with TiO2 systems: Effect of Mn doping content

Du Luchao,An Jie,Katayama Tetsuro,Duan Menghan,Shi XiaoPing,Wang Yunpeng,Furube Akihiro

In recent years, all-inorganic perovskite materials have become an ideal choice for new thin film solar cells due to their excellent photophysical properties and have become a research hotspot. Studying the ultrafast dynamics of photo-generated carriers is of great significance for further improving the performance of such devices. In this work, we focus on the transient dynamic process of CsPbBr 3 /TiO 2 composite systems with different Mn 2+ doping contents using femtosecond transient absorption spectroscopy technology. We used singular value decomposition and global fitting to analyze the transient absorption spectra and obtained three components, which are classified as hot carrier cooling, charge transfer, and charge recombination processes, respectively. We found that the doping concentration of Mn 2+ has an impact on all three processes. We think that the following two factors are responsible: one is the density of defect states and the other is the bandgap width of perovskite. As the concentration of doped Mn 2+ increases, the charge transfer time constant shows a trend of initially increasing, followed by a subsequent decrease, reaching a turning point. This indicates that an appropriate amount of Mn 2+ doping can effectively improve the photoelectric performance of solar cell systems. We proposed a possible charge transfer mechanism model and further elucidated the microscopic mechanism of the effect of Mn 2+ doping on the interface charge transfer process of the CsPbBr 3 /TiO 2 solar cell system.

研究领域: 材料科学 · 物理化学
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Ultrafast Laser-Induced Thickness-Limited Sintering of Metal Nanoparticle Film for Ultrathin Flexible Microelectronic Devices

Junde Ji,Luchan Lin,Yifan Hu,Weiqing Wu,Xinde Zuo,Zhuguo Li

Laser sintering of metal nanoparticles (NPs) has been widely used in flexible microelectronic device fabrication, wherein the sintered layer thickness is a key factor affecting the mechanical stability and conductivity. In this work, ultrathin flexible electronic circuits on flexible substrates with robust bonds and excellent conductivity have been fabricated through ultrafast laser-induced thickness-limited sintering of the metal NP film. When the laser fluence is below the damage threshold of the metal NP film, sintered layer thickness can be controlled by the laser parameters. The maximum thickness of the dense sintered NP layer is limited to 355, 421, 491, 527, and 647 nm at laser pulse durations of 0.3, 5, 10, 15, and 20 ps, respectively. This thickness-limited sintered layer is mainly determined by the plasmonic photothermal absorption of metal NPs and heat transfer within the NP layer. Due to the nonthermal process under intense ultrafast laser irradiation, the metal–polymer interaction can be further enhanced with minimal damage on substrates. The resistivity of the as-received Ag NP film decreases to 6.32 μΩ·cm after laser sintering at a pulse duration of 20 ps. Meanwhile, the relative resistance of the NP film increases to 2.7, 1.7, and 1.03 after 105 bending cycles, 500 tape peeling cycles, and water flow impinging for 60 min, respectively. This thickness-controlled ultrathin Ag NP film fabricated by ultrafast laser sintering exhibits excellent mechanical robustness and electrical conductivity, which shows great promise in ultrathin flexible microelectronic devices.

研究领域: 材料科学 · 微电子学 · 光学工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Synthesis and applications of phase-change recyclable microgels with ultrafast adsorbing performance towards U(Ⅵ)

Peiyan He,Xianshuang Zhu,Danqing Shen,Yue Ma,Xue Bai,Jianming Pan

Rapid treatment of uranium in seawater is an important topic that needs to be addressed urgently. Microgel materials are considered ideal for rapid adsorption due to their ability to absorb water quickly. In a seawater environment, amidoxime materials exhibit superior selectivity for uranium enrichment. However, the modification of amidoxime groups onto microgels must be conducted in organic solvents. These solvents are unable to sufficiently swell and dissolve common microgels, leading to shrinkage that nearly blocks all modification reactions. Here, the thermo-responsive N'N -diethylpropionamide (DEA) was chose as the skeleton monomer to synthesize microgels, which showed both good hydrophilicity and oleophilicity properties The difference between the particle size of synthesized microgels in water and ethanol was not obvious. Due to the integration of microgels and kairamidoxime materials, the AO-Microgels demonstrate a maximum adsorption capacity of 79.29% within just 3 min. Additionally, their selective adsorption capacity for uranium in simulated seawater is remarkable. Furthermore, it simplifies the recycling process because of its intelligent temperature responsiveness.

研究领域: 材料科学 · 环境科学
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Journal of the Taiwan Institute of Chemical Engineers · 2021 · IF 5.876

Method to fabricate porous multifunction β-cyclodextrin modified resin for ultrafast and efficient removal of Cu(II) and bisphenol A

Wei Zhang,Ping Sun,Desheng Liu,Quanlin Zhao,Binze Zou,Lincheng Zhou,Zhengfang Ye

Herein, a simple and green method to fabricate β-cyclodextrin (β-CD) porous cross-linked polymer modified poly(chloromethylstyrene) (PS-Cl) resin, namely, PS@CM-CDP, for ultrafast and efficient removal of heavy metal ions and organic pollutants from aqueous solution was reported. The selected (PS-Cl) was used as a matrix; meanwhile, the β-CD was formed on the surface of PS-Cl under a rigid cross-linking agent of tetrafluoroterephthalonitrile nitrile. The structure and surface elements distribution of PS@CM-CDP were characterized using FT-IR, TG, SEM, XPS, and BET. The resultant PS@CM-CDP with a relatively high maximum adsorption capacity for Cu(II) and BPA can reach 121.88 and 8.25 mg g −1 , respectively, and the spherical nature of the resin makes conventional β-CD polymers easy to recycle 6 times without significantly decreased. The possible adsorption mechanism was also proposed. Industrial wastewater adsorption methods have been used into practice, and the practice presents considerable prospects in the aspects of column for water treatment.

研究领域: 环境科学 · 材料科学
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2021 · IF 4.539

Blue-emitting carbon quantum dots: Ultrafast microwave synthesis, purification and strong fluorescence in organic solvents

Jie Zhu,Chunxing Wu,Yongmei Cui,Dongxiang Li,Yaojun Zhang,Jie Xu,Chunfang Li,Shahid Iqbal,Meiwen Cao

The impurity of unpurified carbon quantum dots (CQDs) severely limits their application. In this paper, CQDs synthesized by ultrafast microwave hydrothermal method from L -cystine were purified by both dialysis and direct phase-transfer. The as-obtained CQDs in basic aqueous reaction mixture show excitation-independent fluorescence around 505 nm with a maximum excitation at 421 nm and pH-responsive emission intensity. However, after purification by dialysis the CQDs display excitation-dependent blue fluorescence from 410 to 500 nm with respect to the excitation from 310 to 430 nm. Particularly, the CQDs purified by direct phase-transfer into various organic solvents show two strong blue fluorescence peaks respectively focusing on 422–434 nm and 400–410 nm with a maximum excitation at 370–372 nm. The quantum yield of the CQDs decreases to 45.1% after a purification by dialysis from the original 82.7%, while it decreases to 57.5% after a purification of phase-transfer. The CQDs extracted in organic solvents are demonstrated to be pure small crystalline-carbon nanoparticles with chemically surface-grafted groups, while the dialyzed CQDs will physically adsorb additional L -cystine, sodium and by-product nitrate ions. The difference of surface state and solvent environment of these CQDs shall contribute to the different fluorescence property. Such strong luminescent , pure CQDs in organic solvents should have obvious advantages in further applications.

CAS / MDL: 56-89-3
研究领域: 材料科学 · 化学
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