Monochromatic soft X-ray-induced reactions of CCl2F2 adsorbed on Si(111)-7 × 7 near the Si(2p) edge

Continuous-time photoelectron spectroscopy (PES) and continuous-time core-level photon-stimulated desorption (PSD) spectroscopy were used to study the monochromatic soft X-ray-induced reactions of CCl₂F₂ molecules adsorbed on Si(111)-7 × 7 at 30 K (CCl₂F₂ dose = 2.0 × 10¹⁴ molecules/cm², ~ 0.75 monolayer) near the Si(2p) core level. Evolution of adsorbed CCl₂F₂ molecules was monitored by using continuous-time photoelectron spectroscopy at two photon energies of 98 and 120 eV to deduce the photolysis cross section as a function of energy. It was found that the photolysis cross sections for 98 and 120 eV photons are _~1.4 × 10^? 18 and ~ 8.0 × 10^? 18 cm², respectively. Sequential F⁺ PSD spectra obtained by using continuous-time core-level photon-stimulated desorption spectroscopy in the photon energy range of 98–110 eV show the variation of their shapes with photon exposure and depict the formation of surface SiF species. The dissociation of CCl₂F₂ molecules adsorbed on Si(111)-7 × 7, irradiated by monochromatic soft X-ray in the photon energy range of 98–110 eV, is mainly due to dissociative electron attachment and indirect dipolar dissociation induced by photoelectrons emitted from the silicon surface.     

Direct Likelihood Evaluation for the Renewal Hawkes Process

An interesting extension of the widely applied Hawkes self-exiting point process, the renewal Hawkes (RHawkes) process, was recently proposed by Wheatley, Filimonov, and Sornette, which has the potential to significantly widen the application domains of the self-exciting point processes. However, they claimed that computation of the likelihood of the RHawkes process requires exponential time and therefore is practically impossible. They proposed two expectation–maximization (EM) type algorithms to compute the maximum likelihood estimator (MLE) of the model parameters. Because of the fundamental role of likelihood in statistical inference, a practically feasible method for likelihood evaluation is highly desirable. In this article, we provide an algorithm that evaluates the likelihood of the RHawkes process in quadratic time, a drastic improvement from the exponential time claimed by Wheatley, Filimonov, and Sornette. We demonstrate the superior performance of the resulting MLEs of the model relative to the EM estimators through simulations. We also present a computationally efficient procedure to calculate the Rosenblatt residuals of the process for goodness-of-fit assessment, and a simple yet efficient procedure for future event prediction. The proposed methodologies were applied on real data from seismology and finance. An R package implementing the proposed methodologies is included in the supplementary materials.     

高功率激光系统nm宽带激光脉冲传输特性

对高功率激光系统采用宽带激光消除菲涅耳衍射问题进行了研究,指出只有数百nm的宽带啁啾光脉冲才对近场衍射有一定的平滑作用,数nm的宽带啁啾光脉冲对近场衍射几乎没有平滑作用;同时,还对宽带啁啾光的B积分表征方式和最快增长频率问题进行了研究,并与原型装置上开展的窄带脉冲、宽带啁啾堆积脉冲的非线性实验结果进行了对比研究,指出以最大B积分或加权B积分反映非线性自聚焦更为准确。研究还表明,在数nm,ns情况下最快增长频率与窄带激光脉冲的差别不大。     

A thioester substrate binds to the enzyme Arthrobacter thioesterase in two ionization states: evidence from Raman difference spectroscopy

4‐Hydroxybenzoyl‐CoA (4‐HB‐CoA) thioesterase from Arthrobacter is the final enzyme catalyzing the hydrolysis of 4‐HB‐CoA to produce coenzyme A and 4‐hydroxybenzoic acid in the bacterial 4‐chlorobenzoate dehalogenation pathway. Using a mutation E73A that blocks catalysis, stable complexes of the enzyme and its substrate can be analyzed by Raman difference spectroscopy. Here we have used Raman difference spectroscopy, in the non‐resonance regime, to characterize 4‐HB‐CoA bound in the active site of the E73A thioesterase. In addition, we have characterized complexes of the wild‐type enzyme complexed with the unreactive substrate analog 4‐hydroxyphenacyl‐CoA (4‐HP‐CoA). Both sets of complexes show evidence for two forms of the ligand in the active site: one population has the 4‐hydroxy group protonated, 4‐OH; while the second has the group as the hydroxide, 4‐O⁻. For bound 4‐HP‐CoA, X‐ray data show that glutamate 78 is close to the 4‐OH in the complex and it is likely that this is the proton acceptor for the 4‐OH proton. Although the pK_a of the 4‐OH group on the free substrate in aqueous solution is 8.6, the relative populations of ionized and neutral 4‐HB‐CoA bound to E73A remain invariant between pH 7.3 and 9.8. The invariance with pH suggests that the 4‐OH and the ‐COO⁻ of E78 constitute a tightly coupled pair where their separate pK_a ‘s lose their individual qualities. Narrow band profiles are seen in the CO double bond and C‐S regions, suggesting that the hydrolyzable thioester group is rigidly bound in the active site in a syn gauche conformation. Copyright © 2011 John Wiley & Sons, Ltd.     

Nano-scale gap filling and mechanism of deposit-etch-deposit process for phase-change material

Ge2Sb2Te5 gap filling is one of the key processes for phase-change random access memory manufacture.Physical vapor deposition is the mainstream method of Ge2Sb2Te5 film deposition due to its advantages of film quality,purity,and accurate composition control.However,the conventional physical vapor deposition process cannot meet the gapfilling requirement with the critical device dimension scaling down to 90 nm or below.In this study,we find that the deposit-etch-deposit process shows better gap-filling capability and scalability than the single-step deposition process,especially at the nano-scale critical dimension.The gap-filling mechanism of the deposit-etch-deposit process was briefly discussed.We also find that re-deposition of phase-change material from via the sidewall to via the bottom by argon ion bombardment during the etch step was a key ingredient for the final good gap filling.We achieve void-free gap filling of phase-change material on the 45-nm via the two-cycle deposit-etch-deposit process.We gain a rather comprehensive insight into the mechanism of deposit-etch-deposit process and propose a potential gap-filling solution for over 45-nm technology nodes for phase-change random access memory.     

Density functional calculations on 13-atom Pd12M （M= Sc-Ni） bimetallic clusters

The geometric structures,electronic and magnetic properties of the 3d transition metal doped clusters Pd12M(M=Sc-Ni) are studied using the semi-core pseudopots density functional theory.The groundstate geometric structure of the Pd12M cluster is probably of pseudoicosahedron.The Ih-Pd12M cluster has the most thermodynamic stability in five different symmetric isomers.The energy gap shows that Pd12M cluster is partly metallic.Both the absolutely predominant metal bond and very weak covalent bond might exist in the Pd12M cluster.The magnetic moment of Pd12M varies from 0 to 5 μB,implying that it has a potential application in new nanomaterials with tunable magnetic properties.     

纯锆上离子注入钇和镧后的表面分析

用金属蒸汽真空弧源，以40kV加速电压对纯锆样品分别进行了10¹⁶—10¹⁷/cm²的钇、镧离子注入，注入温度约为130℃.然后对注入样品进行表面分析.x射线光电子能谱分析表明，注入的钇以Y₂O₃形式存在，镧以La₂O₃形式存在.俄歇电子能谱表明，纯锆基体表面的氧化膜厚度随着离子注入剂量的增加而增加，当离子注入剂量达到10¹⁷/cm²时，氧化膜的厚度达到了最大值.卢瑟福背散射显示镧层的厚度约为30nm，同时直接观察到当离子注入剂量为(La+Y)10¹⁷/cm²时，纯锆样品表面发生了严重的溅射. 关键词： 纯锆 钇和镧离子共注入 卢瑟福背散射 x射线光电子能谱     

飞秒激光作用下全向高反膜破坏的激发过程

设计和制备了全向高反膜SiO₂/TiO₂，研究了它在不同脉冲宽度、不同脉冲能量的飞秒激光作用下的破坏阈值和烧蚀深度.利用发展的抽运-探针方法，研究了抽运脉冲作用下材料中导带电子的超快激发和能量沉积过程，建立并求解了飞秒激光激发材料和材料的激发对抽运光自身反作用的耦合动力学模型.模型较好地揭示了材料破坏的激发过程. 关键词： 飞秒激光 全向高反膜 激发过程 破坏机制     

Br2+分子离子[1+1]双光子解离动力学

本文利用最近研制的低温离子阱-离子速度成像谱仪在冷离子束中研究了同位素质量分辨的⁷⁹Br₂⁺分子离子的[1+1]双光子激光解离动力学. 借助其1⁴Σ^-_u,3/2态为中间态使⁷⁹Br₂⁺共振吸收两个光子至4∽5 eV区域的高激发态并发生解离. 利用离子速度成像技术获得了光解产物⁷⁹Br⁺的二维速度分布和平动能释放谱. 通过平动能释放谱确定了不同解离能量处量子态分辨的解离产物通道分支比. 光碎片产物的角分布表明⁷⁹Br₂⁺分子离子的双光子解离是1⁴Σ^-_u,3/2态的ΔΩ=0平行跃迁至一个Ω=3/2高解离态发生的. 由于分子激发态中的强自旋-轨道耦合作用,高激发的四重态很可能参与到实验观测的光解过程.     

小型荧光激光雷达测量六种典型生物战剂模拟物二维荧光光谱

对成团泛菌(Pan)、金黄色葡萄球菌金黄亚种(Sta)、球芽孢杆菌(BG)和大肠杆菌(EH)四种生物战剂模拟物进行了培养和生长曲线测定,四种菌的代时分别为0.99,0.835,1.07和1.909 h;设计研制了近场小型荧光测量激光雷达,266和355 nm波长分别用于测量生物战剂模拟物氨基酸段和NADH段二维荧光谱;在可控的荧光测量腔室,测得了分辨率为4 nm的营养态细菌液态气溶胶以及牛血清(BSA)、卵清蛋白(OVA)两种毒素类模拟物液态气溶胶的二维荧光谱;二维荧光谱数据表明,Pan,Sta,BG,EH,BSA和OVA气溶胶,在氨基酸段的荧光谱形与标准荧光组分色氨酸较为一致,FWHM为60 nm,受培养生化环境、细菌内部荧光组分及比例的影响,荧光分子激发态与基态间的能量差增大,荧光谱带均存在不同程度的蓝/紫移;在Pan,Sta,BG和EH营养细菌气溶胶中均检出了较弱的NADH荧光组分,且水、氮等的拉曼散射不能完全扣除,光谱锯齿严重,FWHM为100 nm;二阶求导后的二维荧光谱表明,荧光谱的高阶处理和分辨识别是可行的。