六角对称Si2Ge和SiGe2的物理性质：第一性原理计算

本文通过第一性原理计算预测了P6₂22空间群中的两种新型第14族元素合金Si₂Ge和SiGe₂,系统研究了这两种合金的结构、稳定性、弹性各向异性、以及电子和热力学特性. P6₂22-Si₂Ge和P6₂22-SiGe₂具有六角对称结构,其声子谱和弹性常数表明这两种合金在常态环境压力下具有动力学和机械稳定性. P6₂22-Si₂Ge和P6₂22-SiGe₂的弹性各向异性通过杨氏模量的表面结构、剪切模量的等高面和泊松比的方向依赖性进行了详细的研究,同时也讨论和比较了与第14族元素同素异形体P6₂22-Si₃和P6₂22-Ge₃的相关差异. 此外,通过对德拜温度和声速的测算,研究了P6₂22-Si₂Ge和P6₂22-SiGe₂的热力学特性.     

离子液体凝胶聚合物电解质PP13TFSI-LiTFSI-P(VdF-HFP)的电化学性能 (cited: 1)

采用溶液浇铸法将N-甲基-N-丙基哌啶二(三氟甲基磺)亚胺(PP13TFSI)、二(三氟甲基磺)亚胺锂与偏氟乙烯-六氟丙烯共聚物(P(VdF-HFP))混合制备离子液体凝胶聚合物电解质(ILGPEs). 通过扫描电子显微镜观察发现,这种离子液体凝胶聚合物电解质由于液体相的均匀分布而具有疏松的结构. 采用电化学阻抗、计时电流法、线性扫描伏安法测试了电解质的离子电导率、锂离子迁移数和电化学窗口. 室温下离子液体凝胶聚合物电解质的离子电导率和锂离子迁移数分别是0.79 mS/cm和0.71,电化学窗口为0～5.1 Vvs. Li⁺/Li. 电池性能测试表明,这种离子液体凝胶聚合物电解质在Li/LiFePO₄电池中是稳定的,放电容量在30、75和150mA/g倍率下分别为135、117和100 mAh/g,电池经100个循环后容量保持在100%而几乎没有衰减.     

高性能的钛掺杂O3相O3-Na1-xCr1-xTixO2(x=0, 0.03, 0.05)用于钠离子电池正极材料的研究

本文通过凝胶热聚合路线合成了层状的O3相正极材料Na_1-xCr_1-xTi_xO₂(x=0, 0.03, 0.05),采用X射线衍射、扫描电子显微镜来分析其晶体结构和微观形貌. 研究发现,适量的钛掺杂有助于形成更均匀的颗粒并且会改变样品的颜色. 作为钠离子电池正极材料,Na//Na_0.97Cr_0.97Ti_0.03O₂具有非常高的库伦效率(首次高于96%),并且在2.0-3.6 V的电化学窗口下,用0.2 C的倍率循环100次,只有4%的容量衰减;在32 C倍率下有110 mAh/g的比容量.     

“无水”NiCo2O4纳米棒在电化学无酶葡萄糖传感中的应用

本文介绍了棒状NiCo₂O₄的制备,并将其修饰玻碳电极作为无酶葡萄糖传感器. 通过简单的水热反应合成了NiCo₂O₄,然后在商用微波炉中对NiCo₂O₄进行处理,以消除水热合成过程中可能引入的残存水. 扫描电镜、透射电镜、X射线衍射谱和X射线光电子能谱分析表明,微波处理前后结构无变化. 通过EDS对Ni,Co,O原子比例的分析,证明微波处理对残存水的消除作用. 微波处理的NiCo₂O₄(M-NiCo₂O₄)作为葡萄糖传感器的灵敏度高达431.29 μA mM^-1 cm^-2. 最后,将M-NiCo₂O₄在水中浸泡不同时间后,其对葡萄糖的感应性能下降. 结果表明,水热过程中引入的残存水对其电化学性能有很强的影响,微波预处理对其电化学性能也有着重要的影响.     

羟基自由基双光子激发解离动力学

本文利用高里德堡态氢原子飞行时间探测技术，研究了羟基自由基的双光子激发解离动力学. H(²S)+O(¹D)和H(²S)+O(¹S)解离通道是由于羟基在经由A²Σ⁺(v''=2, J''=0.5-2.5)中间态通过双光子激发最终到排斥性的激发态势能曲线2²Ⅱ和B²Σ⁺上产生. 这两种解离通道产物都具有各向异性的角向分布，其中H(²S)+O(¹D)产物角分布异向因子β为-0.97，H(²S)+O(¹S)产物角分布异向因子β为1.97. 各向异性的角向分布与OH自由基在排斥性的激发态势能曲线上直接解离机理相吻合. 此实验观测到羟基自由基的解离能为35580±15 cm^-1.     

OCS经由F 31Π里德堡态生成CO(X1Σ+)+S(1D2)产物的波长相关性光解离

本文利用时间切片离子速度成像技术在134∽140 nm波段研究了OCS分子经由F 3¹Π里德堡态的真空紫外光解离动力学. 在选取的5个分别对应OCS(F 3¹Π, v₁=0∽4)的伸缩振动激发的光解波长，实验测得了来自CO(X¹Σ⁺)+S(¹D₂)产物通道的SS(¹D₂))实验影像，并获得了总平动能谱和CO(X¹Σ⁺, v)共生产物的振动布居及角分布. 结果分析表明OCS分子解离生成CO(X¹Σ⁺)+S(¹D₂)产物的过程经历了上态F 3¹Π 与C_?v和C_s构型的下电子态间非绝热耦合过程. 实验结果显示了很强的波长相关性：OCS (F 3¹Π, v₁)的较低转动激发态(v₁=0∽2)和较高转动激发态(v₁=3, 4)的CO(X¹Σ⁺)产物的振动布居和角分布具有显著差异，表明该解离过程中具有不同的解离机理. 本结果提供了振动耦合可能对真空紫外光解离动力学产生关键作用的相关证据.     

He-H2S复合物的六维从头算势能面和束缚态

采用[CCSD(T)]-F12a/aug-cc-pVTZ方法，同时在基组中引入中心键函数(3s3p2d1f1g)构建了He-H$_2$S复合物的高精度六维势能面. 除分子间振动坐标，同时考虑了H₂S分子内的v₁对称伸缩振动Q₁正则模、v₂弯曲振动Q₂正则模和v₃反对称伸缩振动Q₃正则模三种振动模式. 将计算得到的六维势能面在Q₁，Q₂和Q₃方向上分别做积分得到H₂S单体分别处于振动基态、v和v₃激发态下的He-H₂S的三个振动平均势能面. 计算结果表明，每个平均势能面都有一个T形全局极小值、一个平面局部极小值、两个平面内鞍点和一个平面外鞍点. 全局极小值的几何构型位于R=3.46 ?，θ=109.9°和φ=0.0°，势阱深度为35.301 ^-1. 在径向部分采用离散变量表象法和角度部分采用有限基组表象法并结合Lanczos循环算法计算了He-H₂S的振转能级和束缚态. 计算发现He-(para-H₂S)在H₂S的v₂和v₃区域的带心位移分别为0.025 cm^-1和0.031 cm^-1，而He-(ortho-H₂S)的带心位移分别为0.041 cm^-1和0.060 cm^-1，都表现为蓝移.     

MgF自由基A2π-X2Σ+跃迁的高分辨激光诱导荧光光谱和Franck-Condon因子

MgF自由基被认为是适用于直接激光冷却的候选分子之一. 本文利用激光诱导荧光技术研究了MgF A²π-X²Σ⁺电子跃迁系统的转动分辨光谱. 在超声射流膨胀条件下利用两个镁针对SF₆/Ar气体混合放电产生MgF自由基. 在348∽370 nm范围内,实验记录了属于Δv=0,±1三个序的19个振动带. 通过对实验光谱的转动分析,确定了X²Σ⁺和A²π态的精确光谱常数. 利用实验结果结合和Rydberg-klein-rees方法计算了包括Franck-Condon因子(FCFs)在内的光谱常数. 实验结果和理论计算的FCFs之间存在显著差异,表明FCFs几乎不依赖于A²π态自旋-轨道耦合效应. 本文确定的势能曲线和FCFs为MgF分子激光冷却方案的理论模拟提供了必要的光谱数据.     

理解O(3P)+CHD3→OH+CD3反应的转动模式特异性: 反应物排列图像

本文采用含时波包方法和七维约化量子模型研究了典型碳氢氧化反应O(³P)+CHD₃→OH+CD₃中反应分子CHD₃的转动模式特异性. 发现理论计算反应几率依赖于CHD₃转动量子数J在分子对称轴上的投影$K$和在O-CHD₃分子间轴上的投影K_tot,即P_Ktot=K=0>P_Ktot=K=J>P_Ktot=J,K=0=P_Ktot=0,K=J. 这种关系可以用反应物分子相对取向进行解释. 另外,反应物CHD₃的转动激发(J≤4)表现出比较弱的促进作用,但是K=0转动态激发的促进作用比K=J的强,主要得益于K=K_tot=0分量的贡献. 该分量对应于CHD₃的滚动转动,这种运动形式可以增大初始有效反应碰撞角度的范围.     

B-X and C-X Band Systems of CuCl Revisited: Laser-induced Fluorescence Study in 465−490 nm

通过20400～21800 cm^-1的激光诱导荧光激发谱,重新研究了CuCl的B～X和C～X带系,洪特情形(a)的转动分析揭示出明显的单重态到单重态的跃迁特征. 测量的寿命(分别为4.670和4.667 μs)对于纯的单重态明显太长, 表明CuCl的B态和C态应该位于单重态(¹П和¹∑⁺)和三重态(³П_0,1,2)的混合区,光谱所观测到的这两个激发态可能是被临近三重态严重微扰的单重态.     

Insulating method using cataphoretic paint for tungsten tips for electrochemical scanning tunnelling microscopy (ECSTM)

A new tip insulating process for active metal tips allowing atomic resolution ECSTM imaging has been developed. This new method using cathodic cataphoretic paint deposition has been tested successfully. The insulating deposited film appears homogeneous under optical microscopy and it has been characterised by infra red and SEM analysis. The depositing layer of the paint is sufficiently dense to effectively resist electrolyte ion penetration and resists corrosion in various acidic, basic aqueous or non-aqueous media. The coating film does not reduce the imaging capability of the ECSTM even to atomic resolution. This new insulating method adds to the approaches available to those preparing tips for ECSTM. This approach would also be of great utility for the preparation of microelectrodes using active metals.     

Scalable Formation of Concentrated Monodisperse Lignin Nanoparticles by Recirculation-Enhanced Flash Nanoprecipitation

A highly controllable and scalable process for fabrication of large amounts of concentrated lignin nanoparticles (LNPs) is reported. These lignin core nanoparticles are formed through flash nanoprecipitation, however, scaling up of the fabrication process requires fundamental understanding of their operational formation mechanism and surface properties. It is shown how a semicontinuous synthesis system with a recirculation loop makes it possible to produce flash precipitated lignin nanoparticles in large amounts for practical applications. The roles of the process parameters, including flow rates and lignin concentration, are investigated and analyzed. The results indicate that the LNPs are formed by a process of continuous burst nucleation at the point of mixing without diffusive growth, which yields nanoparticles of highly uniform size following a modified LaMer nucleation and growth mechanism. This mechanism makes possible facile process control and scale-up. Effective control of the resulting nanoparticle size is achieved through the initial concentration of lignin in the injected solution. The impressive capability to produce suspensions of any predesigned multimodal distribution is demonstrated. The resulting nanofabrication technique can produce large volumes of concentrated LNP suspensions of high stability and tightly controlled size distributions for biological or agricultural applications.     

Peripheral collisions of highly charged ions with metal clusters

Within the framework of the dynamical classical over-barrier model,the soft collisions between slow highly charged ions(SHCIs) Ar 17+ and the large copper clusters under large impact parameters have been studied in this paper.We present the dominant mechanism of the electron transfer between SHCIs and a large metal cluster by computational simulation.The evolution of the occupation of projectile ions,KL x satellite lines,X-ray yields,Auger electron spectrum and scattering angles are provided.     

Overstretching of a 30 bp DNA duplex studied with steered molecular dynamics simulation: Effects of structural defects on structure and force-extension relation

Single-molecule experiments on polymeric DNA show that the molecule can be overstretched at nearly constant force by about 70% beyond its relaxed contour length. In this publication we use steered molecular dynamics (MD) simulation to study the effect of structural defects on force-extension curves and structures at high elongation in a 30 base pair duplex pulled by its torsionally unconstrained 5' -5' ends. The defect-free duplex shows a plateau in the force-extension curve at 120pN in which large segments with inclined and paired bases (“S-DNA”) near both ends of the duplex coexist with a central B-type segment separated from the former by small denaturation bubbles. In the presence of a base mismatch or a nick, force-extension curves are very similar to the ones of the defect-free duplex. For the duplex with a base mismatch, S-type segments with highly inclined base pairs are not observed; rather, the overstretched duplex consists of B-type segments separated by denaturation bubbles. The nicked duplex evolves, via a two-step transition, into a two-domain structure characterized by a large S-type segment coexisting with several short S-type segments which are separated by short denaturation bubbles. Our results suggest that in the presence of nicks the force-extension curve of highly elongated duplex DNA might reflect locally highly inhomogeneous stretching.     

Large scale highly organized single-walled carbon nanotube networks for electrical devices

Large-scale room-temperature liquid-phase directed assembly of highly organized single-walled carbon nanotubes (SWNT) over large areas is demonstrated. The presented process utilizes lithographically patterned template to guide the fluidic self-assembly of SWNTs on a silicon-dioxide substrate. The width of these highly organized SWNT structures are in the micron range while their heights are in orders of nanometers. Room temperature electrical I–V characterization of these fabricated high coverage SWNT wires show linear ohmic behavior. The resistivity of these assembled SWNT network is in the order of 10⁻⁶ Ω m demonstrating their metallic characteristics during conductance. Scaling of the assembly processes on a wafer level with high yield is demonstrated. Our developed assembly process is compatible with complimentary metal oxide semiconductor (CMOS) processes and provides a simple and flexible way of building SWNT nanotube-based electronics in a large scale.     

WIMPs search by scintillators: possible strategy for annual modulation search with large-mass highly-radiopure NaI(TI)

The DAMA experiments are running deep underground in the Gran Sasso National Laboratory. Several interesting results have been achieved so far. Here a maximum likelihood method to search for the WIMP annual modulation signature is discussed and applied to a set of preliminary test data collected with large mass highly radiopure NaI(Tl) detectors. Various related technical arguments are briefly addressed.     

Clustering aspects of nuclei in highly deformed states

The potential energies, the moments of inertia, and the quadrupole and octupole moments of dinuclear systems are compared with corresponding values for the highly deformed nuclear states. The idea is advocated that hyperdeformed states of nuclei are close to near-symmetric dinuclear systems. The superdeformed states are considered as asymmetric dinuclear systems. The cluster superdeformed and hyperdeformed states have quite a large octupole deformation. Measurement of octupole deformations of highly deformed nuclei can answer the question of whether these nuclei exist in cluster configurations.     

Numerical investigations on resistive cooling of trapped highly charged ions

The investigation of simple atomic systems in extreme electromagnetic fields with highest precision demands intense beams of heavy and highly charged ions to be decelerated and cooled to extremely low energies for long-time observation. Resistive cooling, i.e., the electronic dissipation of energy of a stored ion cloud on an external impedance, seems to be a good candidate for in-trap cooling of highly charged ions and has been chosen for the upcoming HITRAP (Highly charged Ion TRAP) facility at GSI, Darmstadt. Nevertheless, resistive cooling of large ensembles of ions confined in a Penning trap has never been thoroughly studied until now and the understanding of this highly nonlinear phenomenon is far from complete. Through the use of systematic simulations we give a proof of the feasibility of resistive cooling of large numbers of highly charged ions as well as the interpretation of some specific features observed experimentally.     

Two-dimensional metal inclusions in a dielectric crystal

Highly aggregated color centers in crystals of a wide-band-gap calcium fluoride insulator heated in a reducing atmosphere of vapors of calcium metal cation (“additive coloration” of crystals) have been studied using spectroscopy and atomic-force microscopy methods. These centers are large aggregates of anion vacancies and electrons, which transform into metal structures. The evolution of these structures with increasing number of such components has been traced from individual particles with two-dimensional structure to large film fragments. It has been shown that fragments are concentrated in isolated planes {111}, which are cleavage planes of the crystal with high contents of highly aggregated centers.     

场发射冷阴极微栅孔阵列制备技术

实现了一种采用聚苯乙烯纳米球自组装技术和微机械制造技术加工的场发射阴极用亚微米栅极微孔阵列。设计了一套完整的工艺实验方案,首先采用微球自组装技术获得了亚微米级金属网孔掩膜,然后通过反应离子刻蚀技术获得了亚微米栅极孔阵列,从而实现了集成度高、分布均匀的周期性亚微米孔洞阵列的制备,微孔集成度达到108cm-2。实验研究了氧气刻蚀聚苯乙烯微球的规律。采用金属掩膜,四氟化碳干法刻蚀二氧化硅,获得了深度为500 nm的微孔。实验结果证明该工艺方案是一种获得大面积、均匀分布、集成度高的场发射冷阴极栅孔阵列的有效方法。