Facile synthesis of N-doped carbon-coated Li<Subscript>4</Subscript>Ti<Subscript>5</Subscript>O<Subscript>12</Subscript> anode for application in high-rate lithium ion batteries

A facile sol-gel approach for the synthesis of lithium titanate composite decorated with N-doped carbon material (LTO/NC) is proposed. Urea is used as a nitrogen source in the proposed approach. The LTO/NC exhibits superior electrochemical performances as an electrode material for lithium-ion batteries, delivering a discharge capacity of as high as 103 mAh g^?1 at a high rate of 20 C and retaining a stable reversible capacity of 90 mAh g^?1 after 1000 cycles, corresponding to 100% capacity retention. These excellent electrochemical performances are proved by the nanoscale structure and N-doped carbon coating. NC layers were uniformly dispersed on the surface of LTO, thus preventing agglomeration, favoring the rapid migration of the inserted Li ion, and increasing the Li⁺ diffusion coefficient and electronic conductivity. LTO with the appropriate amount of NC coating is a promising anode material with applications in the development of high-powered and durable lithium-ion batteries.     

利用相干光照明的纹影成像装置研究飞秒激光脉冲烧蚀铝靶喷射物相位的超快时间演化

本文提出了一种基于纹影成像装置的新型相位检测方法, 并使用该方法对飞秒激光烧蚀铝靶产生的喷射物的超快相位演化过程进行了实验研究. 与传统的纹影法不同, 本文的相位检测方法使用相干光作为成像照明光, 利用未透过样品的背景光作为参考光, 借助透过样品后在纹影装置刀口处衍射的照明光与背景照明光的干涉, 检测样品的相位; 其最显著的优点是能够清晰反映被测样品mπ或2mπ (m为整数) 的相位改变. 利用该方法, 结合抽运-探测技术, 研究了激光流量为5.4 J/cm²的50 fs脉冲激光烧蚀铝靶产生的喷射物的超快相位演化. 实验发现, 烧蚀过程中形成的喷射物可分为三个相位不同的区域, 分别对应等离子体态的喷射物、后续的垂直靶面喷射的物质和冲击波. 其中, 等离子体态的喷射物在0–9.0 ns的时间延迟内, 由于膨胀和电子复合作用, 相位变化超过π; 而后续的垂直靶面的喷射物在此时间内的相位变化没有超过π. 关键词： 相位检测方法 纹影成像技术 相干光照明 抽运-探测技术     

Facile fabrication of highly flexible,porous PEDOT: PSS/SWCNTs films for thermoelectric applications

High-performance organic composite thermoelectric(TE)materials are considered as a promising alternative for harvesting heat energy.Herein,composite films of poly(3,4-ethyienedioxythiophene):poly(styrene sulfonate)/single-walled carbon nanotubes(PEDOT:PSS/SWCNTs)were fabricated by utilizing a convenient solution mixing method.Thereafter,the as-prepared hybrid films were treated using sulfuric acid(H₂SO₄)to further optimize the TE performance.Film morphological studies revealed that the sulfuric acid treated PEDOT:PSS/SWCNTs composite samples all possessed porous structures.Due to the successful fabrication of highly conductive networks,the porous nano-architecture also exhibited much more excellent TE properties when compared with the dense structure of the pristine samples.For the post-treated sample,a high power factor of 156.43μW·m^-1·K^-2can be achieved by adjusting the content of CNTs,which is approximately 3 orders of magnitude higher than that of the corresponding untreated samples(0.23μW·m^-1·K^-2).Besides,the obtained films also showed excellent mechanical flexibility,owing to the porous nanostructure and the strong p–p interactions between the two components.This work indicates that the H₂SO₄ treatment could be a promising strategy for fabricating highly-flexible and porous PEDOT:PSS/SWCNTs films with high TE performances.     

Steered coherence and entanglement in the Heisenberg XX chain under twisted boundary conditions

We study steered coherence(SC) and entanglement in a three-spin Heisenberg XX model under twisted boundary conditions and show that their strengths can be significantly enhanced by tuning the twist angle. The optimal twist angle θ_(opt) for achieving the maximum l_1 norm of SC is π in the region of weak field B and decreases gradually from π to 0 when B increases after a critical value, while for the relative entropy of SC, θ_(opt) equals π in the weak field region and 0 otherwise.The entanglement and the critical temperature above which the entanglement vanishes can also be significantly enhanced by tuning the twist angle from 0 to π.     

基于动态最小生成树路由协议的数据聚融算法

大规模的地理环境监测,以及用来传输与处理数据的物理基础设施无法和监测区域的规模保持同样的增速,使得不可靠链路下的数据采集与处理呈现出一种饱和流状态,无线传感器网络的能力看似难以稳定.另一方面,尽管理想网络模型的计算结果足够精确,然而,由于与实际应用偏差甚大,使得网络用户无法充分地分析和利用从工业现场所获得到的网络感知数据,并且没有针对网络规模和性能对数据聚融的影响进行分析.为此,本文提出以"过渡区"作为工业现场仿真的假设条件,并在此基础上提出了一种面向实际应用的数据聚融算法,即基于可信度的数据聚融算法(R算法).在具体设计R算法过程中,选用聚集和操作符SUM为例,通过对网络提供出的近似聚集和加以自动分析、综合,针对相对误差界限ε,计算出近似聚集和的可信度的下限η;并将近似聚集和、参数η一同提供给用户,在为用户提供网络概要信息的同时,还提供了参数η作为对信息可信度的判断,以便指导用户对数据聚集结果进行深度处理和提高网络的感知性能.仿真实验描述了过渡区内由于信噪比导致的链路不可靠所引起的η的变化规律;讨论了网络性能和规模对η的影响,随着网络运行周期的增加和网络规模的增大,η的值将逐渐靠近0;从而为WSNs从理论模型投入实际工业应用提供了理论依据和经验公式.     

Laser phase effect on asymmetric harmonic distribution in H_2~+

The laser phase effect on the spatial distribution of the molecular high-order harmonic generation(MHHG) spectrum from H_2~+ is theoretically investigated through solving the Non-Bohn-Oppenheimer(NBO) time-dependent Schrodinger equation(TDSE).The results are shown as follows,(i) The generated harmonics from the two nuclei each present an asymmetric distribution.Particularly,when the laser phases are chosen from 0.0π to 0.6π and from 1.7π to 2.0π,the contribution from the negative-H plays a main role in harmonic generation.When the laser phases are chosen from 0.7πto 1.6k,the contribution from the positive-H to the harmonic generation is remarkably enhanced and becomes greater than that from the negative-H.The electron localization,the time-frequency analyses of the harmonic spectrum and the time-dependent wave function are shown to explain the asymmetric harmonic distribution in H_2~+,which provides us with a method to control the electron motion in molecules,(ⅱ) As the pulse duration increases,the asymmetric distributions of the MHHG in two H nuclei decrease,(ⅲ) Isotope investigation shows that the asymmetric harmonic distribution can be reduced by introducing the heavy nucleus(i.e.,D_2~+).     

Elastic electron scattering with formamide-(H2O)n complexes (n=1, 2): Influence of microsolvation on the π* and σ* resonances

We report elastic cross sections for low-energy electron scattering with formamide-(H₂O)_n complexes (n=1, 2) in the energy region of 0.01-8 eV. The scattering calculations are performed using the R-matrix method in the static-exchange (SE) approximation. We consider three structures of formamide-H₂O and six structures of formamide-(H₂O)₂ in the present work. Our purpose is to investigate effects of water molecules hydrogen-bonding to formamide. We focus on the influence of microsolvation on the π^* and σ^* resonances of formamide. The scattering result for complexes shows that the position of π^* resonance appears at lower or higher energies in the cluster than in the isolated formamide depending on the complex structure and the water role in the hydrogen bonding. We explain this behavior according to the net charge of the solute. It is found that the microsolvation environment has a substantial effect on the width of π^* resonance. Our results indicate that surrounding water molecules may affect the lifetime of the resonances, and hence the process is driven by the anion state, such as the dissociative electron attachment.     

Azobenzene mesogens mediated preparation of Sn S nanocrystals encapsulated with in-situ N-doped carbon and their enhanced electrochemical performance for lithium ion batteries application

In this work,azobenzene mesogen-containing tin thiolates have been synthesized,which possess ordered lamellar structures persistent to higher temperature and serve as liquid crystalline precursors.Based on the preorganized tin thiolate precursors,Sn S nanocrystals encapsulated with in-situ N-doped carbon layer have been achieved through a simple solventless pyrolysis process with the azobenzene mesogenic thiolate precursor served as Sn,S,N,and C sources simultaneously.Thus prepared nanocomposite materials as anode of lithium ion batteries present a large specific capacity of 604.6 m Ah·g~(-1)at a current density of 100 m A·g~(-1),keeping a high capacity retention up to 96% after 80 cycles,and display high rate capability due to the synergistic effect of well-dispersed Sn S nanocrystals and N-doped carbon layer.Such encouraging results shed a light on the controlled preparation of advanced nanocomposites based on liquid crystalline metallomesogen precursors and may boost their novel intriguing applications.     

N-doped graphene as a nanostructure adsorbent for carbon monoxide: DFT calculations

ABSTRACT

This work reports the physisorption of carbon monoxide (CO) on the surface of N-doped graphene. To study the adsorption of CO on N-doped graphene, some quantum chemical calculations were used through density functional theory. Based on our results, it can be found that the CO molecule could be adsorbed on the surface of N-doped graphene physically with the adsorption energies (E_ads) of ?2.9 and ?0.8 kcal mol^?1 (depends on the kind of configuration) while positive adsorption energies were calculated upon adsorption of CO on pristine graphene. We used the charge analysis for calculation of the net transferred charge of adsorbed CO on pristine and N-doped graphene sheets to evaluate the sensing ability of surface. The global indices of reactivity were calculated from the differences of the lowest unoccupied molecular orbital and highest occupied molecular orbital energies. Graphs for density of states point to some orbital hybridisation between CO molecule and N-doped graphene. Consequently, the N-doped graphene transforms the existence of CO molecules into electrical signal, and it may be potentially used as a sensor for CO.     

二维旋转边带分解实验

描述了一类新的二维旋转边带分解实验,准备期包括交叉极化、若干个以TOSS序列的延迟加上的π脉冲和一个π/2脉冲,混合期包括一个π/2脉冲和一个TOSS序列,在演化期内,磁化矢量位于z方向。本实验能给出完全分解的各向同性化学位移与各向异性化学位移,它与Kolbert等人^[5]的实验方法相互补充。     

Phase-and spin-dependent manipulation of leakage of Majorana mode into double quantum dot

We present a phase-and spin-dependent manipulation of leakage of a Majorana mode into a double quantum dot. We study the density of states(DOS) to show the effect of phase change factor on the Majorana leakage into(out) of a double quantum dot. The DOS is derived from the Green's function of the quantum dot by the equation of motion method, and exhibits a formant structure when φ = 0, 2π and a resonance shape when φ = 0.5π and 1.5π. Also, it changes more strongly under the spin-polarized coefficient than the non-polarized lead. Such a theoretical model can be modified to explore the spin-dependent effect in the hybrid Majorana quantum dot system.     

Novel 0–π transitions in Josephson junctions between noncentrosymmetric superconductors

We study the Josephson effect between two noncentrosymmetric superconductors(NCSs) with opposite polarization vectors of Rashba spin–orbit coupling(RSOC).We find a 0–π transition driven by the triplet–singlet ratio of NCSs.Different from conventional 0–π transitions,the Andreev bound states change their energy range instead of phase shift in the 0–π transition found here.This novel property results in a feature that the critical current becomes almost zero at the transition point,not only a minimum.Furthermore,when the directions of RSOC polarization vectors are the same in two NCSs,the similar effect can also be found in the presence of a perpendicular exchange field or a Dresselhause spin–orbit coupling in the interlayer.We find novel oscillations of critical current without 0–π transition.These novel 0–π transitions or oscillations of critical current present new understanding of the Josephson effect and can also serve as a tool to determine the unknown triplet–singlet ratio of NCSs.     

PCDTBT作为发光层的有机电致发光器件研究

使用PCDTBT作为发光层材料,制备了发光波长为705 nm的红色有机电致发光器件,其结构为ITO/PEDOT:PSS/PCDTBT/BCP/LiF/Al.器件启亮电压为2 V,在9 V时器件达到最高亮度,为29000 cd/m2,最大电流效率为3.5 cd/A.还研究了不同退火温度对器件发光性能的影响.实验结果表明,退火温度为50?C时器件的性能最佳,其原因是此时既有利于溶剂挥发,又保持了分子结构的稳定性,而高温退火降低了PCDTBT的π-π堆积的有序性,从而使得器件性能下降.     

Round-robin differential quadrature phase-shift quantum key distribution

Recently,a round-robin differential phase-shift(RRDPS) protocol was proposed[Nature 509,475(2014)],in which the amount of leakage is bounded without monitoring the signal disturbance.Introducing states of the phase-encoded Bennett-Brassard 1984 protocol(PE-BB84) to the RRDPS,this paper presents another quantum key distribution protocol called round-robin differential quadrature phase-shift(RRDQPS) quantum key distribution.Regarding a train of many pulses as a single packet,the sender modulates the phase of each pulse by one of {0,π/2,π,3π/2},then the receiver measures each packet with a Mach-Zehnder interferometer having a phase basis of 0 or π/2.The RRDQPS protocol can be implemented with essential similar hardware to the PE-BB84,so it has great compatibility with the current quantum system.Here we analyze the security of the RRDQPS protocol against the intercept-resend attack and the beam-splitting attack.Results show that the proposed protocol inherits the advantages arising from the simplicity of the RRDPS protocol and is more robust against these attacks than the original protocol.     

O-乙基O-芳基N-异丙基硫代磷酰胺酯类化合物的除草活性与其31P化学位移的关系

本文测定了标题所示一类化合物的³¹P的化学位移,并讨论了它与取代基电子性间存在如下的关系δP=-0.9193σ+3.5891F+66.5385提出了³¹P化学位移与此类化合物的除草活性间存在一定的相关性,其关系如下PI₅₀=-0.9025π²+0.9017π-0.5600E_s-0.1620△δP+0.8445I+4.2514并对此关系的适用性及存在偏差作了初步讨论。     

Theoretical study of stereodynamics for the D'+DS(ν = 0,j = 0)→D'D+S abstraction reaction

Quasiclassical trajectory (QCT) calculations have been performed for the abstraction reaction, D' +DS(v = 0, j = 0)→D'D+S on a new LZHH potential energy surface (PES) of the adiabatic 3A' electronic state [Lü et al. 2012 J. Chem. Phys. 136 094308]. The collision energy effect on the integral cross section and product polarization are studied over a wide collision energy range from 0.1 to 2.0 eV. The cross sections calculated by the QCT procedure are in good accordance with previous quantum wave packet results. The three angular distribution functions, P(θ_r), P(φ_r), and P(θ_r,φ_r), together with the four commonly used polarization-dependent differential cross sections ((2π/σ)(ds₀₀/dω_t), (2π/σ)(ds₂₀/dω_t), (2π/σ)(ds₂₂₊/dω_t), (2π/σ)(ds_21-/dω_t)) are obtained to gain insight into the chemical stereodynamics of the title reaction. Influences of the collision energy on the product polarization are exhibited and discussed.     

Oxidation degree dependent adsorption of ssDNA onto graphene-based surface

DNA/GO composite plays a significant role in the research field of biotechnology and nanotechnology, and attracts a great deal of interest. However, it is still unclear how the oxidation degree of the graphene-based surface affects the adsorption process of single-strand DNA(ss DNA). In this paper, based on the molecular dynamics simulations, we find that ss DNA molecule is absorbed on the GO surface in the most stable state with the oxidation degree around 15%. The microscopic mechanism is attributed to the van Der Walls and the electrostatic interactions between the ss DNA molecule and the graphene-based surface, which is accompanied with the π–π stacking and hydrogen bond formation. The number of π–π stacking between ss DNA and GO reaches the maximum value when the oxidation degree is around 15% among all the GO surfaces. Our simulation results also reveal the coexistence of stretched and curved configurations as well as the adsorption orientation of ss DNA on the GO surface. Furthermore, it is found that the absorbed ss DNA molecules are more likely to move on the graphene-based surface of low oxidation degree, especially on pristine graphene. Our work provides the physics picture of ss DNA's physisorption dynamics onto graphene-based surface and it is helpful in designing DNA/GO nanomaterials.     

Highly Strong Interaction between Fe/Fe3C Nanoparticles and N-Doped Carbon toward Enhanced Oxygen Reduction Reaction Performance

Transition metal compounds anchored on N-doped carbon (NC) show intrinsic activity and stability for oxygen reduction reaction (ORR). However, the interaction between the transition metal compounds and NC still needs to be strengthened for electron transfer at the compounds/carbon interface. Herein, Fe/Fe₃C hybrid nanoparticles encapsulated into N-doped carbon (Fe@NC) are used as high-performance ORR catalysts. Benefiting from the strong interaction at Fe/Fe₃C nanoparticles/NC interface, the electrons can transfer from Fe/Fe₃C hybrid nanoparticles to NC, redistributing the electron density of active sites and promoting the ORR process. The as-synthesized Fe@NC exhibits outstanding ORR catalytic activity with an onset potential of 1.01 V and a half-wave potential of 0.92 V in alkaline media. It also shows prominent cycling stability and tolerance to methanol crossover, superior to Pt/C catalyst. The theoretical analysis reveals that the Fe nanoparticles have regulated the electron distributions at the heterojunction interface. The Gibbs free energy diagrams for ORR illustrate that the rate-determining step is the conversion of OH* to OH⁻. In situ Raman spectra give evidence of O-containing intermediates to prove the ORR process.     

Geometrically induced π-band splitting in graphene superlattices

According to band folding analyses, the graphene superlattices can be differed by whether the Dirac points are folded to Γ point or not. In previous studies, the inversion symmetry preserved defects open bandgap in the former superlattices while they cannot in the latter ones. In this paper, by using density functional theory with generalized gradient approximation, we have carefully studied the electronic properties of the latter graphene superlattices, in which the defects would induce π-band splitting to get the π_a1–π_a2 and π_z1–π_z2 band sets. Based on our detailed studies, such splitting could be attributed to the geometrically induced bond-symmetry breaking. In addition, these band sets could be shifted toward each other by the methodology of strain engineering. A bandgap would be opened once the band sets start to overlap. Then,its gap width could be continuously enlarged by enhancing strain until reaching the maximum value determined by the defect density. These studies contribute to the bandstructure engineering of graphene-based nanomaterials, which would be interesting to call for further investigations on both theory and experiment.     

Insight into influence of thermodynamic coefficients on transient negative capacitance in Zr-doped HfO2 ferroelectric capacitors

We study the influence of the thermodynamic coefficients on transient negative capacitance for the Zr-doped HfO₂ (HZO) ferroelectric capacitors by the theoretical simulation based on the Landau-Khalatnikov (L-K) theory and experimental measurement of electrical properties in the resistor-ferroelectric capacitor (R-FEC) circuit. Our results show that the thermodynamic coefficients α, β and γ also play a key role for the transient NC effect besides the viscosity coefficient and series resistor. Moreover, the smaller coefficients α and β, the more significant the transient NC effect. In addition, we also find that the thermodynamic process of transient NC does not obey the generally accepted viewpoint of Gibbs free energy minimization.