Simple algorithm for quantitative analysis of reflection electron energy loss spectra (REELS)

A detailed comparison of two different physical approaches for quantitative analysis of reflection electron energy loss spectra (REELS) is presented. The Tougaard–Chorkendorff (TC) algorithm [S. Tougaard, I. Chorkendorff, Phys. Rev. B35 (1987) 6570] is analyzed theoretically and applied to experimental spectra of four elemental solids (Si, Cu, Ag, and Au). A closed expression is derived for the quantity retrieved by the TC-algorithm, the so-called “effective” cross section, which was originally only given as a recursive procedure. Single scattering loss distributions are derived from the experimental spectra using the bivariate reversal method [W.S.M. Werner, Phys. Rev. B74 (2006) 075421]. The latter agree satisfactorily with density functional theory (DFT) calculations and other data found in the literature. Using these single scattering loss distributions, the TC “effective” cross section can be perfectly reproduced if the fact is taken into account that the effective cross section is not a single scattering loss distribution and is governed to a significant extent by elastic scattering. On the basis of the above results, a dramatically simplified deconvolution scheme for quantitative analysis of REELS is developed.     

Theoretical determination of the surface excitation parameter for Ti, Fe, Cu, Pd, Ag, and Au

The angular dependence of the surface excitation parameter (SEP) is theoretically determined for different materials (Ti, Fe, Cu, Pd, Ag, and Au) for angles to the surface normal between 10° and 70° and for energies between 300 and 3400 eV. The method is based on analysis of energy-differential inelastic electron scattering cross sections calculated from the dielectric function with the software QUEELS (quantitative analysis of electron energy losses at surfaces) valid for reflection-electron-energy-loss spectroscopy (REELS). The calculations presented here are closely related to a method previously developed [N. Pauly, S. Tougaard, F. Yubero, Surf. Interf. Anal. 37 (2005) 1151] for materials (like Al and Si) with a clear surface plasmon peak. However, for the materials studied here the excitations are broad and there is no clear visual distinction between surface and bulk excitations. It is therefore not possible, as in the previous studies of Al and Si, to isolate the intensity of the surface excitation directly. Therefore the volume component for an infinite medium is subtracted from the calculated cross section and in this way the surface excitation component of the cross section is determined and the SEP calculated.     

掺镱硅酸盐激光玻璃的制备与光谱特性分析

采用高温熔融工艺制备了两块组分差别不大的掺镱(Yb3+)硅酸盐激光玻璃.测试出两块玻璃样品的吸收光谱和荧光光谱;计算了Yb3+掺杂玻璃的积分吸收截面、受激发射截面、荧光线宽、能级寿命、最小粒子数、饱和泵浦强度、最小泵浦强度等参数,比较发现样品的吸收截面图与倒易法计算所得的受激发射截面图线型相似,而与F-L法计算所得的受激发射截面图筹别较大,这与理论分析相吻合.两块玻璃样品的吸收光谱的线型基本一致,吸收主峰位于975 nm,次峰位于908 nm,这就说明影响激光玻璃吸收光谱线型的主要因素足玻璃基质的组成.两块玻璃样晶的荧光光谱差别比较大,样品1主峰位于993 nm,次峰位于1 029 nm;样品2主峰位于1 035 nm,次峰位于994nm,差别原因主要在于Yb3+离子的掺杂浓度不同.     

(Au,Ag)/Si复合纳米颗粒薄膜的微结构与光谱特性

采用复合靶共溅射方法制备了(Au,Ag)/Si复合纳米颗粒薄膜,分别采用Maxwell-Garnett理论和微分有效媒质(DEM)理论计算了Ag/Si复合薄膜的吸收光谱,实验测量结果与DEM理论计算更接近,讨论了(Au,Ag)/Si体系复合薄膜共振吸收峰宽化的微观机制. 关键词：     

不同Ag壳厚度Au@Ag纳米粒子的调控制备表征及表面增强拉曼光谱的效应

采用化学还原法制备了以Au为核、包覆Ag的双金属核壳Au@Ag纳米粒子,并成功地用于表面增强拉曼光谱(SERS)分析测试。通过改变制备液中Ag/Au的量比来调控Ag壳包覆厚度。采用透射电子显微镜(TEM)和紫外-可见光谱仪(UV-Vis)对Au@Ag纳米粒子的构貌进行表征。TEM显示明显存在核壳结构,且Ag壳层随Ag/Au的量比的增加而逐渐变厚;UV-Vis表明随着Ag/Au的量比的增加,Au@Ag纳米粒子出现了Au核与Ag壳吸收峰的2个等离子体共振峰,同时伴随着Au峰的蓝移和Ag峰的红移。以双甲脒为分析物,考察了不同Ag/Au的量比时的Au@Ag纳米粒子的SERS活性。结果表明,SERS活性随Ag/Au的量比的增加先增大后减小,在6∶5时其SERS增强效应最佳,此时Ag壳厚度约为6 nm。以对巯基苯胺(4-ATP)、结晶紫(CV)和双甲脒为分析测试对象,对比了Au@Ag、Ag、Au 3种基底的SERS活性。结果表明,所制备的Au@Ag纳米粒子的SERS活性要明显优于单纯的Au、Ag纳米粒子。     

Electronic and optical properties of Cu, CuO and Cu2O studied by electron spectroscopy

The electronic and optical properties of Cu, CuO and Cu(2)O were studied by x-ray photoelectron spectroscopy (XPS) and reflection electron energy-loss spectroscopy (REELS). We report detailed Cu 2p, Cu LVV, O 1s and O KLL spectra which are in good agreement with previous results. REELS spectra, recorded for primary energies in the range from 150 to 2000 eV, were corrected for multiple inelastically scattered electrons to determine the effective inelastic scattering cross section. The dielectric functions and optical properties were determined by comparing the experimental inelastic electron scattering cross section with a simulated cross section calculated within the semi-classical dielectric response model in which the only input is Im(-1/ε) by using the QUEELS-ε(k,ω)-REELS software package. By Kramers-Kronig transformation of the determined Im(-1/ε), the real and imaginary parts (ε(1) and ε(2)) of the dielectric function, and the refractive index n and extinction coefficient k were determined for Cu, CuO, and Cu(2)O in the 0-100 eV energy range. Observed differences between Cu, CuO and Cu(2)O are mainly due to modifications of the 3d and O 2p electron configurations.     

没食子酸还原法制备金银合金纳米粒子及其吸收光谱研究

用没食子酸一步液相还原制备粒度均匀和性质稳定的Au-Ag合金纳米粒子,研究在不同反应温度和Au／Ag摩尔比下Au-Ag合金纳米粒子的吸收光谱特性。实验结果表明Au-Ag合金纳米粒子仅有1个吸收峰,介于纯Ag和纯Au纳米粒子的吸收峰之间,且随着反应温度的提高,合金纳米粒子的最大吸收峰位逐渐蓝移,吸光度增加,半峰宽变窄。随着Au/Ag摩尔比的增加,合金纳米粒子的最大吸收峰位红移,且与其所含Au摩尔百分数呈线性关系。HRTEM表征结果说明制备的Au/Ag合金纳米粒子近球形、粒度均匀、无包覆现象。EDX分析结果证实单个纳米粒子由Au和Ag组成,其元素组成比与参加反应的Au/Ag摩尔比接近。     

Yb2.75C60同步辐射光电子能谱

在超高真空系统中制备了Yb275C60薄膜.对样品进行了同步辐射光电子能谱研究.在费米能级以下约5 eV范围内的谱数据由Yb275C60价带（C60分子轨道LUMO，HOMO和HOMO 1导出的能带）和芯态（Yb 4f7/2，4f5/2）能级构成.用紫外能区不同能量的入射光子，用C 2p和Yb 4f光电离截面随光子能量的不同变化规律，通过定量拟合，得到了对谱线有贡献的上述各个组分的峰位、峰宽和强度.结果表明，光子能量高于约300 eV时，芯态4f的贡献使得实验结果远远偏离价带的本征态密度分布.因此，研究Yb275C60价态时，应使用能量低于300 eV的光子.对实验和拟合结果分析，发现了类似纯C60的光电离截面振荡现象.振荡幅度相对于纯C60较小，反映了化合物中C60分子的化学环境对光电离截面振荡现象起着不可忽略的作用. 关键词： Yb275C60 同步辐射光电子能谱 光电离截面振荡     

Validity of the semi-classical approach for calculation of the surface excitation parameter

The problem of surface plasmon excitation by moving charges has been elaborated by several different approaches, mainly based on dielectric response theory within either semi-classical or quantum mechanical frameworks. In this work, a comparison of the surface excitation effect between two different frameworks is made by calculation of the differential inverse inelastic mean free path (DIIMFP) and a Monte Carlo simulation of reflection electron energy loss spectroscopy (REELS) spectra. A semi-classical modeling of the interaction between electrons and a solid surface is based on analyzing the work done by moving electrons; the stopping power and inelastic cross section are derived with the induced potential. On the other hand, a quantum mechanical approach is based on derivation of the complex inhomogeneous self-energy of the electrons. The numerical calculation shows that the semi-classical model presents almost the same values of DIIMFP as by the quantum model except at the glancing condition. The simulation of REELS spectra for Ag and SiO(2) as well as a comparison with experimental spectra also confirms that a good agreement with the spectral shape is found among the two simulation results and the experimental data.     

一种稀土离子发射截面的计算方法

介绍一种将McCumber理论和Judd-Oflet理论结合起来计算稀土离子从激光发态跃迁回基态的发射截面的方法,这种方法非常简单,只需要测量离子的吸收光谱。计算了氟化物玻璃中稀土离子Tm3 ,Yb^3 和Er^3 第一激发态的发射截面,其结果表明这种方法是很实用的。     

n-Si(As):Yb1130nm四能级发光研究

在n-Si(As):Yb中首次观察到1130nm的尖锐发光.通过掺入Yb的剂量与发光强度的关系以及红外吸收、透射光谱的测量,讨论了敏化剂Yb与激活剂As之间能量传递过程.适当选取Yb与As的浓度比可提高发光效率.     

Study of Spectroscopic Properties of Yb-doped Calcium Fluorapatite

The spectroscopic performance of Yb-doped calcium fluorapatite (Yb:FAP) was assessed by measuring polarization absorption spectra, polarization emission spectra and fluorescence lifetime. The emission cross section has been evaluated using the absorption cross section and principle of reciprocity. The π polarization absorption and emission cross sections of Yb3+ in FAP are found to be substantially larger than those of other Yb-doped media. Favorable spectroscopic parameters show that Yb:FAP crystal is more desirable for many diode-pumped solid state laser application with low- and medium-power in the near future.     

Study of Spectroscopic Properties of Yb-doped Calcium Fluorapatite

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Delayed onset of 4d photoemission relative to the giant 4d photoabsorption of La

For the giant 4d photoabsorption of La, both the total photoabsorption spectrum and the N_4.5-derived Auger emission intensity spectrum increase significantly above hν ? 112 eV, with spectral peaks at hν = 118 and 119 eV, respectively. However, the predominant 4d photoemission partial cross section shows a delayed onset of ～ 4 eV, with a peak at hν = 121 eV, while the 5s, 5p, and 5d partial cross sections all show a strong resonant enhancement at lower energies, with spectral peaks at hν = 116.6 eV. These results are compared with a recent many-body calculation for Ce. The photon energy dependence of the La 4d_{$\text{5}\text{2}$}/4d_{$\text{3}\text{2}$} photo-emission branching ratio is consistent with a “final-state model.”     

Au/Ag合金溶胶与HCuCl4反应过程的紫外光谱研究

采用柠檬酸根为保护剂,通过水合肼还原的方法,在水相中合成了Au/Ag合金纳米粒子,UV-Vis光谱中只观察到一个位于单金属Ag和Au之间的等离子体共振峰,并且合金溶胶的最大吸收峰随着溶胶中Au的物质的量分数变化呈线性变化.通过紫外-可见吸收光谱研究了不同组分的溶胶与HCuCl4溶液的反应过程.结果显示,溶胶的紫外-可见吸收峰随着HCuCl4的加入量的改变而呈规律性变化,其中有一紫外吸收峰随着HCuCl4的加入而呈线性变化的区间,分析后认为这一过程为合金的去合金过程.     

掺镱硅酸盐玻璃的光谱性质

采用高温熔融工艺制备了掺Yb^3＋硅酸盐玻璃。测试了玻璃的吸收光谱和荧光光谱,计算并分析了Yb^3＋离子在975nm附近的吸收截面和积分吸收截面随掺杂浓度的变化趋势。玻璃光谱曲线表明：吸收主峰位于975nm,在900—960nm范围内有一个弥散的吸收峰,中心波长为930nm;荧光主峰位于975nm,荧光次峰位于1010nm。综合其性能表明实验中硅酸盐玻璃的最佳Yb^3＋掺杂浓度为4mol%。     

五边形截面的Ag纳米线局域表面等离子体共振模式

五边形截面的单晶Ag纳米线对ZnO量子点荧光具有增强的现象. 为解释这一现象, 利用时域有限差分法对五边形截面的Ag纳米线的局域表面等离子体共振模式进行了理论模拟. 结果表明, 五边形截面的Ag纳米线在紫外区域存在两个消光峰, 分别由Ag纳米线的横向偶极共振(340 nm)和四极共振(375 nm)引起; 这两个消光峰与ZnO量子点荧光增强峰相一致, 而且随着Ag纳米线的半径增大而红移; 消光峰对应的共振模式取决于Ag纳米线的截面形状; 根据Ag纳米线电场增强倍数与激发光波长变化关系曲线可知, 最大增强电场位于五边形截面的顶点处, 而边线处电场增强较小. 理论模拟的结果较好地解释了Ag纳米线/ZnO量子点体系的荧光增强现象, 也为Ag纳米线在提高半导体材料发光效率、生物探测等方面的应用提供有益的参考.     

Nuclear and Coulomb interactions in coherent fragmentation of relativistic nuclei in a photoemulsion

The role of the nuclear and Coulomb interactions in coherent fragmentation of relativistic nuclei is discussed with the cluster-model analysis of the experimental data on the fragmentation of ⁷Li (P = 3A GeV/c) via the ³H + ⁴He channel in photoemulsion used as an example. The calculated electromagnetic contribution of ～10% to the cross section is not in conflict with the photoemulsion data and the upper estimate of ～40% derived from the earlier measurements of total cross sections for fragmentation of light nuclei using the counter technique. The observed irregularities in the differential cross section for ⁷Li fragmentation with a separated Coulomb peak at a very small momentum transfer Q are ascribed to the overlap of nuclear diffraction patterns arising from light (C, N, O) and heavy (Ag, Br) photoemulsion nuclei. The predicted diffraction cross sections in the inelastic channel drastically differ from the usual shape of nuclear diffraction in an elastic channel. For pure targets, they have a shape of oscillations with a few peaks of comparable intensity and show strong dependence on the form of the surface nuclear density and radii of the intranuclear cluster and target nucleus. The probability for two-body clustering in ⁷Li is estimated at about 0.7.     

高发射截面掺镱氧化物玻璃

在国外报道的一些掺镱(Yb^3 )激发玻璃基上,实验研究得到发射截面更大的掺Yb^3 玻璃.其中掺Yb^3 锗碲酸盐`硼酸盐和硅铌酸盐玻璃的发射截面大于1.9pm^2;磷酸盐玻璃的发射截面较小但有较长的荧光寿命.优良的光谱性质使这些玻璃有望成为高平均功率和高峰值功率激光器增益介质的候选基质.     

Spin-resolved photoemission by circularly polarized light from Au on Ag(111): experiment and theory

The electronic structure of 1 ML and 2 ML Au on Ag(111) has been studied experimentally and theoretically by spin-, angle- and energy-resolved photoemission in the highly symmetrical set-up of normally incident circularly polarized VUV radiation and normal electron emission. The measured spectra agree rather well with their relativistically calculated counterparts and can be consistently interpreted with the aid of spin- and layer-resolved densities of states. The spin polarization of spectral peaks directly reflects the double group symmetry type of the the corresponding initial states. For 1 ML (2 ML) Au on Ag(111) there are two (four) Au-derived states, which are confined to the adlayers (“film states”). For 2 ML Au, the “film-state” photoemission intensity depends strongly on the photon energy, which is understood as an interference effect. Since the agreement with the experimental photoemission spectra is improved by calculations assuming an additional Ag layer on top, and since the Au-derived experimental features are substantially broadened, an intermixing of Au and Ag is very likely.