Metallization of the Ge(111) surface at high-temperature probed by energy-loss and Auger spectroscopies

We present new electron energy-loss spectroscopy (EELS) and Auger (AES) experiments aimed to study the structural transition of the Ge(111) surface taking place at high temperatures. Our advanced high-temperature set-up allowed us to collect accurate EELS spectra near the M_2,3 excitation edges and AES MMV and MVV spectra, corresponding to different probing depths ranging from 4 to 10 Å. The metallization of the surface has been clearly detected by the shift of the M_2,3 edge and of the MMV, MVV Auger energies. A detailed study of the transition has been performed using a fine temperature step under thermal equilibrium conditions. The AES and EELS experiments show that a sudden semiconductor-metal transition takes place at about 1000 K involving mainly the topmost layers. Deeper layers within 10 Å are also involved in the metallization process (in a range of 10 above 1010 K) and a smooth change in the topmost layers is also observed at higher temperatures up to 1070 K. These transitions are not fully reversible upon cooling (down to 870 K). Structural and electronic characteristics of the surface transition are discussed in light of available models.     

Electrochemical biosensing for dsDNA damage induced by PbSe quantum dots under UV irradiation

<正>An electrochemical sensor for the detection of the natural double-stranded DNA(dsDNA) damage induced by PbSe quantum dots(QDs) under UV irradiation was developed.The biosensing membranes were prepared by successively assembling 3- mercaptopropionic acid,polycationic poly(diallyldimethyl ammonium) and dsDNA on the surface of the gold electrode.Damage of dsDNA was fulfilled by immersing the sensing membrane electrode in PbSe QDs suspension and illuminating it with an UV lamp. Cyclic voltammetry was utilized to detect dsDNA damage with Co(phen)_3~(3+) as the electroactive probe.The UV irradiation,Pb~(2+) ions liberated from the PbSe QDs under the UV irradiation and the reactive oxygen species(ROS) generated in the presence of the PbSe QDs also under the UV irradiation were the three factors of inducing the dsDNA damage.The synergistic effect of the three factors might dramatically enhance the damage of dsDNA.This electrochemical sensor provided a simple method for detecting DNA damage,and may be used for investigating the DNA damage induced by other QDs.     

MAA修饰ZnO量子点及其发光特性

以ZnAc2·2H2O为原料,在乙醇中通过70℃回流4h,得到ZnO前驱物,与LiOH·H2O反应,制备出ZnO.采用巯基乙酸(mercaptoacetic acid,MAA)对所合成的ZnO进行表面修饰,修饰后的产物经SEM和XRD表征,证明获得了物相单一、近似球状、粒径为4.6nm的ZnO量子点.借助紫外-可见和荧光分析,研究了MAA对该量子点的修饰效果,探讨了设置条件下ZnO的发光机理和性质.发现该实验体系之所以产生荧光表面缺陷发射峰消失和激子发射峰明显增加的光学现象,是因为MAA有效地覆盖了ZnO的表面缺陷,并稳定包裹住ZnO粒子.同时还研究了MAA加量、温度、电解质对修饰产物发光性能的影响,发现经MAA修饰后的ZnO量子点具有较强的荧光发光性能、良好的长期陈放稳定性,以及一定的抗电解质影响能力.研究结果对ZnO量子点应用于生物分析具有重要参考价值.     

甲氧基在Rh(111)表面吸附的密度泛函研究

采用密度泛函理论(DFT)的B3LYP方法,以原子簇Rh13(9,4)为模拟表面,在6-31G(d,p)与Lanl2dz基组水平上,对甲氧基在Rh(111)表面的四种吸附位置(fcc、hcp、top、bridge)的吸附模型进行了几何优化、能量计算、Mulliken电荷布局分析以及前线轨道的计算。结果表明,当甲氧基通过氧与金属表面相互作用时,在bridge位的吸附能最大,吸附体系最稳定,在top位转移的电子数最多;吸附于Rh(111)面的过程中C—O键被活化,C—O键的振动频率发生红移。     

多功能两亲梳状聚合物的合成及包覆荧光量子点

利用溶液聚合和成酰胺反应合成了多功能梳状两亲性共聚物,聚(甲基丙烯酸-co-甲基丙烯酸十八酯)-(乙醇胺-乙二胺叶酸)(PSM-EE-FA).用红外光谱(FTIR),核磁共振(1H-NMR)及凝胶渗透色谱(GPC)表征了该聚合物的结构及分子量分布.实验结果证明合成了该聚合物,其数均分子量(Mn)为28600,多分散性为1.375.用该两亲梳状聚合物包覆油溶性CdSe/ZnS量子点,通过相转移作用,得到水溶性靶向量子点(PSM-EE-FA-QDs).该水溶性量子点溶液具有较好的稳定性.通过紫外-可见(UV-Vis)及荧光发射光谱分析对该量子点的光学性质进行研究.结果表明,PSM-EE-FA-QDs的紫外-可见光谱及荧光发射光谱峰形与原量子点基本一致.由于量子点表面聚合物层的形成,峰位发生少量红移.该量子点水溶液的荧光强度是原量子点氯仿溶液的98%,荧光产率是原量子点氯仿溶液的95%.动态光散射(DLS)及透射电镜(TEM)测试结果表明水溶性量子点分布均匀.合成的水溶性量子点不但光学性能稳定,而且聚合物及水溶性量子点的合成方法较为简便.     

Ce_3Rh_3Si_2和CeRh_3Si_2的磁性模拟和晶场效应研究

根据晶场理论,通过对D.Kaczorowski等人测量的磁化率倒数与温度关系曲线的模拟,得到了稀土化合物CeRh3Si2和Ce3Rh3Si2的晶场分裂能和相应波函数.对于CeRh3Si2和Ce3Rh3Si2,它们的第一激发能和总的激发能分别为176K,855K和77.5K,428K.计算表明,Kramers离子Ce3+在晶场效应的作用下,基态简并部分消除得到了三个双重态,模拟得到的化合物的磁化率倒数与温度关系曲线与实验曲线吻合较好.     

Effect of zero-point energy on the dielectric behavior of strontium titanate

Barrett formula has been obtained in the framework of the effective field approach by including the zero-point energy. By fitting with experimental data of dielectric constant of SrTiO₃, we find that they agree in the whole temperature range fairly well if the zero-point energy is assumed to change from a small value at low temperature to a large value at high temperature.     

Depth dependence of the anomalous thermal behavior of Cu(110)

We report the results of a mirror electron microscope low energy electron diffraction (MEM-LEED) study of anomalous thermal behavior caused by enhanced thermal vibrational motion on a clean Cu(110) surface. The enhanced vibrational amplitudes cause diffracted intensities to deviate from simple Debye-Waller behavior. These deviations become apparent between 550 K and 600 K; i.e. at about 0.45 of the bulk melting temperature. Because of the finite penetration of low energy electrons, LEED intensities contain information about both surface and subsurface order. Our LEED results are analyzed to extract this information using a kinematical model in which the electron attenuation and the depth and temperature dependent vibrational amplitudes are parametrized. For a large range of model parameters, we conclude that by 850 K large anharmonic vibrations are present in several layers and at least two subsurface layers may have melted.     

Phase transitions in metals on metals

Phase transitions in two-dimensional metal layers on metal surfaces are discussed, with emphasis on systems with attractive lateral interactions on densely packed surfaces. The experimental tools which give information on these transitions are described briefly and the results obtained with them are illustrated by examples of various metals on W and Mo surfaces.