光子扫描隧道显微镜的探测场

通过修改光子扫描隧道显微镜探测场的计算模型，推导出比较符合实际的探测场及透射系数的计算公式，并利用这一新计算公式在微机上进行了模拟计算，得到了一些过去未曾发现的现象，对光子扫描隧道显微镜的实际探测具有一定的指导意义。     

Two-Dimensional Numerical Simulations of Photon Scanning Tunneling Microscopy: Fourier Modal Method and R-Matrix Algorithm

Numerical simulation of a two-dimensional probe–object system for photon scanning tunneling microscope is presented. The R-matrix propagation algorithm incorporated into the Fourier modal method was used to achieve an extended capability for modeling of a realistic system consisting of both a probe and a sample. The type of the mode guided through the dielectric probe and the coupling of the near-field to fundamental guiding mode in the probe are discussed. The influence of the probe parameters on the near-field images is investigated. Three different probe shapes were simulated in the constant height scanning mode. The transmitted flux intensity through the probe was found to be strongly dependent on the tip shape. The analysis shows a good agreement of the obtained results with the available theoretical works and confirming experimental results. The proposed numerical scheme can find applications for near-field probe characterization and provides an understanding of the degree of perturbation introduced by a probe tip in the experiment.     

多学科应用可大范围搜索的紧凑型扫描隧道显微镜

本文展示了结构紧凑的（高度为66 mm,直径为25 mm）扫描隧道显微镜,配备了一套拥有原子级分辨精度的三维压电马达。其中Z方向定位依靠的是自行发明的由轴向切割的压电扫描管驱动的摩擦型步进器。X-Y方向（即样品面方向）的移动是将Z向步进器作为一个惯性滑块垂直嵌入压电扫描管内同时一端平放在压电扫描管的顶部。其设计具有在极端条件下（低温、强磁场等）从宏观尺度样品区域（平方毫米级别）搜索微观靶向（缺陷位、掺杂位、边界及纳米器件等）的能力。在室温大气下对高定向热解石墨进行测量,得到了高分辨率的原子图像.     

利用扫描隧道显微镜表征和操纵单分子

扫描隧道显微镜（STM）提供给我们一种表征单分子的局域物理和化学特性的特殊方法，甚至还能帮助我们操纵单分子以构造分子尺度的新型器件。本文中我们采用了两种新型STM技术分别来表征封装在富勒烯笼里面的金属原子和构造一种具有较强Kondo效应的分子器件。空间dI/dV映像谱被用来探索单个Dy@C82分子中能量分辨的金属-笼杂化态，揭示了有关Dy原子在碳笼中的空间位置和Dy-碳笼之间相互作用的重要信息。我们也通过控制STM针尖诱导的高电压脉冲来诱导CoPc分子的边缘脱氢化，从而改变了这个分子在Au(111)表面的吸附构型，导致吸附在Au表面的完整CoPc分子所不具备的Kondo效应产生。     

利用扫描隧道显微镜在溶液中直接观测过渡族金属硫属化合物

本文利用自制的溶液扫描隧道显微镜在溶液环境下直接观测到TiSe₂、MoTe₂和TaS₂样品的原子分辨率图像. 通过将单晶样品在溶液中直接解理,可以保护解理过的新鲜样品表面在几个小时内不会被严重污染. 利用自行搭建的溶液扫描隧道显微镜,首先观察到了TiSe₂活泼样品的原子分辨率图像,并观察到了TiSe₂表面所特有的点缺陷和三角形缺陷结构. 此外,还观察到了MoTe₂的原子分辨率超结构和TaS₂表面的电荷密度波结构. 结果表明：在室温、溶液环境下能更高效的研究过渡族金属硫属化合物等活泼样品的表面电子态结构,同样适用于溶液环境下的电催化和电化学研究.     

Instrumentation and Measurement Issues for Nanometer Particles: Workshop Summary

Journal of Nanoparticle Research -     

Cross-Polarized Single Photon Emission from Single Semiconductor Quantum Dots with V-Type Level Driven by Pulse Field

The statistic properties of photon emissions from single semiconductor quantum dots with V-type level driven by pulses are investigated theoretically. Based on quantum regression theorem and master equations, the dynamic equations of the second-order correlation function of the photon emissions are deduced. The calculated results reveal that the efficiency of single photon emissions from two orthogonal polarization eigenstates （｜x） and ｜y） ） reaches the maximum when the input pulses area is about π, and the probability of the cross-polarized single photon emission from ｜x） and ｜y） decreases with increasing of pulse width.     

Cross-Polarized Single Photon Emission from Single Semiconductor Quantum Dots with V-Type Level Driven by Pulse Field

The statistic properties of photon emissions from single semiconductor quantum dots with V-type level driven by pulses are investigated theoretically. Based on quantum regression theorem and master equations, the dynamic equations of the second-order correlation function of the photon emissions are deduced. The calculated results reveal that the efficiency of single photon emissions from two orthogonal polarization eigenstates |x〉and |y〉) reaches the maximum when the input pulses area is about π, and the probability of the cross-polarized single photon emission from |x 〉 and |y 〉decreases with increasing of pulse width.     

Scanning tunneling spectroscopy and break junction spectroscopy on iron-oxypnictide superconductor NdFeAs(O0.9F0.1)

Iron-oxypnictide superconductor NdFeAs(O_0.9F_0.1) was studied using both low-temperature scanning tunneling microscopy/spectroscopy (STM/STS) and tunnel break junction (BJ) methods. STM topography showed granular and spot structures with a typical size of several nanometers, most probably governed by fluorine atom distribution. The majority of STS conductance, G, versus voltage, V, curves revealed V-shaped structures, whereas some of G(V) dependences possessed coherent gap peaks or kinks at gap energies. At the same time, G(V) dependences obtained by the BJ technique showed clear-cut coherence peaks with peak-to-peak distances V_pp = 4Δ/e ∼ 25 mV at 4.2 K, where Δ is the superconducting energy gap, e > 0 is the elementary charge. This yields Δ(0) = 6–7 meV, so that the ratio 2Δ(0)/k_BT_c is about 3–4, k_B being the Boltzmann constant. This value is consistent with the conventional weak-coupling s-wave Bardeen–Cooper–Schrieffer theory.     

量子点操控的光子探测和圆偏振光子发射

半导体量子点是研究光子与电子态相互作用的优选固态体系,并在光子探测和发射两个方向上展现出独特的技术机遇.其中基于量子点的共振隧穿结构被认为在单光子探测方面综合性能最佳,但受到光子数识别、工作温度两个关键性能的制约.利用腔模激子态外场耦合效应,有望获得圆偏振态可控的高频单光子发射.本文介绍作者提出的量子点耦合共振隧穿（QD-cRTD）的光子探测机理,利用量子点量子阱复合电子态的隧穿放大,将QD-cRTD光子探测的工作温度由液氦提高至液氮条件,光电响应的增益达到10⁷以上,并具备双光子识别能力;同时,由量子点能级的直接吸收,原型器件获得了近红外的光子响应.在量子点光子发射机理的研究方面,作者实现了量子点激子跃迁和微腔腔模共振耦合的磁场调控,在Purcell效应的作用下增强激子自旋态的自发辐射速率,从而增强量子点中左旋或右旋圆偏振光的发射强度,圆偏度达到90%以上,形成一种光子自旋可控发射的新途径.     

Near-Field Fluorescence and Topography Characterization of a Single Nanometre Fluorophore by Apertureless Tip-Enhanced Scanning Near-Field Microscopy

Tip-enhanced near-field fluorescence and topography characterization of a single nanometre fluorophore is conducted by using an apertureless scanning near-field microscopy system. A fluorophore with size 80hm is mapped with a spatial resolution of 10hm. The corresponding near-field fluorescence data shows significant signal enhancement due to the apertureless tip-enhanced effect. With the nanometre spatial resolution capability and nanometre local tip-enhanced effect, the apertureless tip-enhanced scanning near-field microscopy may be further used to characterize a single molecule by realizing the local near-field spectrum assignment corresponding to topography at nanometre scale.     

On the Thermal Decomposition of Dipyridamole: Thermogravimetric,Differential Scanning Calorimetric and Spectroscopic Studies

Thermal decomposition of dipyridamole was followed by analysis of the residue by spectroscopic methods. The loss of mass observed in thermogravimetric (TG) experiments in N₂ atmosphere occurs in essentially three steps. The first step, corresponding to 35% of mass loss, was monitored in an isothermal process, and the solid residue was analyzed by proton and carbon NMR, optical absorption, and fluorescence emission. Heating at 305°C leads to new products with optical absorption bands shifted to lower wavelengths relative to dipyridamole. The broad emission band is also shifted to lower wavelengths. NMR analysis demonstrates that the piperidine groups are probably one of the sites of modification because the corresponding resonance peaks are not present in proton or carbon spectra. Preliminary high‐pressure chromatography shows that two main compounds appear at significantly higher polarity as compared with dipyridamole. Isothermal decomposition leaves the pyrimido‐pyrimidine central ring essentially unchanged, and the products involve changes at the peripheral substituent positions. Our results further contribute to elucidate the chemistry of this class of compounds.     

Structural and Optical Properties of Gold/Silica “Mushroom” Particles Prepared by Interfacial Templating

Complex shaped nanoparticles featuring structural or surface chemical patchiness are of special interest in both fundamental and applied research areas. This study reports the preparation and optical properties of gold/silica “mushroom” nanoparticles, where a gold particle is only partially covered by the silica cap. The synthetic approach allows precise control over the particle structure. The interfacial preparation method relies on partially embedding the gold particles in a polystyrene layer that masks the immersed part of the gold particle during silica shell growth from an aqueous solution. By adjusting sacrificial polystyrene film thickness and silica growth time, precise control over the coverage and cap thickness can be achieved. Correlative electron microscopy and single particle scattering spectroscopy measurements underline the high precision and reproducibility of the method. The good agreement between the measured and simulated single particle spectra supported by near‐field calculations indicates that the observed changes in the dipolar plasmon resonance are influenced by the extent of coverage of the gold core by the silica cap. The straightforward methods readily available for gold and silica surface modification using range of different (bio)molecules make these well‐defined nanoscale objects excellent candidates to study fundamental processes of programmed self‐assembly or application as theranostic agents.     

Si衬底上生长的MnSi薄膜和MnSi1．7纳米线的STM和XPS分析

本文采用分子束外延方法制备出MnSi薄膜和MnSi1．7纳米线,利用扫描隧道显微镜进行观察,采用X射线光电子能谱仪系统地分析了MnSi薄膜和MnSi1．7纳米线的Mn2p和Si2p．结果表明厚度为-0．9nm的MnSi薄膜表面为／3×／3重构,MnSi1．7纳米线长50ff--1500nm,宽16—18nm,高-3nm．MnSi薄膜的Mn2p1／2和Mn2p3／2峰位与MnSil．7纳米线相同,均分别为649．7eV和638．7ev结合能在640-645eV和-653．8eV处的锰氧化合物的Mn2ps／2和Mn2p1／2峰证明在短暂暴露于空气中后MnSi薄膜和MnSi1．7纳米线表面有氧化层形成．相对于纯si的si2p谱,两种锰硅化合物的Si2p谱向低结合能方向发生了位移,表明随着锰硅化合物的形成Si的化学环境发生了变化．     

近场显微干涉成像中的探测角度和偏振问题研究

用偶极子耦合系统来模拟近场干涉测量中的探针样品关系,并利用各电场分量之间的组合方程组精确计算出其可能探测到的强度和相位像。结果显示,近场干涉所测量到的近场像的分辨力和探测器的方位及参考光的偏振方向之间有较强的依赖关系,随着探测器位置不同或者参考光偏振方向的变化,同一样品在同一照明条件下所得到的图像也会发生明显的改变。在倏逝波照明的情况下,近场像的精确度随着探测器相对于样品视角的增大而改善,且在不同偏振方向的近场像中,只有偏振方向垂直于样品表面的像能真实反映样品的细节分布,且同时具有足够的强度分布。     

Self‐Assemble Polymeric Nanoparticle with GSH Exhaustion for SPECT Imaging–Guided Enhanced Radioisotope Therapy

Exploiting biocompatible nanomaterials for cancer theranostics has attracted great attention in recent years. Herein, a multifunctional self‐assembled nanoparticle based on a biocompatible polymer that contains 3‐(4‐hydroxyphenyl) propionic acid N‐hydroxysuccinimide ester (HOPA) for radiolabeling and piperlongumine (PL) for exhausting endogenous glutathione (GSH) (HOPA‐C18PMH‐PEG/PL) is successfully synthesized. With radionuclide ¹²⁵I labeling, SPECT imaging shows high tumor uptake of HOPA‐C18PMH‐PEG/PL after intravenous injection. The in vitro and in vivo combined radioisotope therapy (RIT) and chemotherapy using ¹³¹I‐labeled HOPA‐C18PMH‐PEG/PL is then carried out, achieving synergistic antitumor effect. This is because the reactive oxygen species (ROS) level in the tumor sites of mice treated with ¹³¹I‐labeled HOPA‐C18PMH‐PEG/PL is increased after the exhaustion of GSH by PL. Additionally, such a strategy (exhausting GSH and increasing ROS) induces no obvious toxicity to normal tissue. Therefore, as‐made polymeric nanoparticles exhibit multifunctional properties for SPECT imaging–guided combined RIT and chemotherapy in one system. This finding will further promote polymeric nanoparticle–based RIT of cancer and is expected to be used for future clinical transformation.     

Synthesis and Characterization of CdS Nanoparticles with Strong Electrolyte Behavior

The CdS nanoparticles whose structure is similar to a strong electrolyte were synthesized by the colloidal chemical method. The CdS nanoparticles with Cd²⁺-rich surface are capped by the electrically neutral ligand of 2,2-bipyridine (bpy), and the counterion, BPh₄ ^-, is adsorbed around the particle as balance charge. The donation from 2,2-bipyridine at 2-position to the Cd²⁺-rich surface of the CdS nanoparticles was characterized by X-ray photoelectron spectroscopy (XPS). These CdS nanoparticles can redisperse in pyridine (py) or DMF, and have high stability. The determination of electroconductivity and the electrophoresis deposition in dilute solution containing the CdS nanoparticles further prove the rationality of the above electrolyte structure of the CdS nanoparticles.     

Probing droplets with biological colloidal suspensions on smart surfaces by synchrotron radiation micro- and nano-beams

Droplets with colloidal biological suspensions evaporating on substrates with defined wetting properties generate confined environments for initiating aggregation and self-assembly processes. We describe smart micro- and nanostructured surfaces, optimized for probing single droplets and residues by synchrotron radiation micro- and nanobeam diffraction techniques. Applications are presented for Ac-IVD and β-amyloid (1–42) peptides capable of forming cross-β sheet structures. Complementary synchrotron radiation FTIR microspectroscopy addresses secondary structure formation. The high synchrotron radiation source brilliance enables fast raster-scan experiments.     

Recent Notable Approaches to Study Self-Assembly of Nanoparticles with X-Ray Scattering and Electron Microscopy

Self-assembly of nanoparticles (NPs) has evolved into a powerful tool for the synthesis of superstructures with tailored properties. The quality, diversity, and complexity of synthesized structures are continuously improving and fascinating new collective properties are demonstrated. At the same time, the rapid development of electron microscopy and synchrotron sources for X-rays has enabled new exciting experimental approaches to study structure and structure formation in the context of NP self-assembly. In this review, some recent studies and what can be learned from them are highlighted and discussed. It is started with a general introduction covering important concepts, experimental approaches, commonly obtained structures, the ideas of artificial atoms, and emerging properties are discussed. Recent experimental in situ and ex situ approaches with state-of-the-art electron microscopy and X-ray diffraction and scattering that helped to obtain a detailed picture of NP self-assembly processes and resulting structures are then presented.     

Spherical gravitational collapse with photon emission and a generalized Schwarzchild interior solution

The general dynamical equations for perfect fluid filled spheres with an outward flux of photons are derived. The vital role played by the energy density of the free gravitational field in accelerating photon production has been emphasized. It is pointed out that even when the material energy density is finite, the energy density of the free gravitational field can take infinitely large values resulting in vanishing surface area of the star. A generalized Schwarzschild interior solution with conformally flat geometry but with photon emission has been obtained. It is pointed out that the interior conformal coordinate system bears a strong resemblance to the exterior Krushkal coordinates. It is shown that for spherical star the invariant velocity of the fluid particles, falling towards the centre, is proportional to its radius suggesting that the outer envelopes collapse at a faster rate than the core part. It is shown that the interior radiating solution can be matched with generalized Schwarzchild exterior solution.