调频场作用下双光子电离光电子谱特性

应用微扰理论和数值计算方法,研究了调频光场作用下激发与电离模型中双光子电离光电子谱的相干特性.分析了调频光场的调制振幅、调制频率以及初相位对双光子电离光电子谱的影响.结果表明,调制振幅、调制频率以及初相位对双光子电离光电子谱有调制作用.选取合适的参量,可以实现对双光子电离光电子谱的量子控制.这一相干量子控制的机理是强场作用下激发态的粒子在两个缀饰态之间的选择性布局所致.

双原子分子多光子电离强场效应的含时波包动力学研究

强激光非线性条件下分子的多光子电离过程呈现出较为明显的强场效应.由于这种效应不能用传统的量子微扰论来处理,“缀饰态”模型方法提供了物理图象清晰的处理光与物质相互作用的方案.本文基于含时波包动力学的基本理论,将激光场看作经典场,利用“缀饰态”模型研究了强场下双原子分子(NO、RbI等)的多光子电离过程.研究表明,激光场的强度、泵浦-探测脉冲延迟时间等对多光子电离光电子能谱的形状有着重要的影响,而这种影响是由光诱导势引起的.另外,在研究具有两个连续态的RbI体系时,自电离现象的发生也与势能面的交叉密切相关,并受外场强度的影响.本文计算模拟外场中分子的光电子能谱时所得到的强场效应对理解和实现原子分子过程的激光操控具有重要的意义.

双原子分子多光子电离强场效应的含时波包动力学研究

强激光非线性条件下分子的多光子电离过程呈现出较为明显的强场效应．由于这种效应不能用传统的量子微扰论来处理。“缀饰态”模型方法提供了物理图象清晰的处理光与物质相互作用的方案．本文基于含时波包动力学的基本理论，将激光场看作经典场，利用“缀饰态”模型研究了强场下双原子分子（NO、RbI等）的多光子电离过程．研究表明，激光场的强度、泵浦-探测脉冲延迟时间等对多光子电离光电子能谱的形状有着重要的影响。而这种影响是由光诱导势引起的．另外，在研究具有两个连续态的Rbl体系时，自电离现象的发生也与势能面的交叉密切相关，并受外场强度的影响．本文计算模拟外场中分子的光电子能谱时所得到的强场效应对理解和实现原子分子过程的激光搛控具有重要的意义．

Ionization Energies and Dyson Orbials of Allyl Alcohol and Allyl Mercaptan Conformers

The conformers of allyl alcohol and allyl mercaptan were studied with B3LYP/aug-cc-pVTZ method. Their relative energies were calculated at MP3, MP4（SDQ）, and CCSD（T） levels. The most stable conformers for these two molecules are Gauche-gauche＇ （Gg＇）. The theo-retical photoelectron spectra simulated with the calculated ionization energies demonstrate that there are at least four conformers in allyl alcohol and four conformers in allyl mercaptan in the gas-phase experiments. The Dyson orbitals of the highest occupied molecular orbital （HOMO） and the next HOMO （HOMO-1） of allyl mercaptan Ggt conformer show strongly mixing ns and πc=c characteristics, which may be due to the resonance and inductive effects between πc=c and ns in HOMO-1 and HOMO.

Corona Discharge Ion Mobility Spectrometry of Ten Alcohols

Ion mobility spectra for ten alcohols have been studied in an ion mobility spectrometry apparatus equipped with a corona discharge ionization source. Using protonated water cluster ions as the reactant ions and clean air as the drift gas, the alcohols exhibit different product ion characteristic peaks in their ion mobility spectra. The detection limit for these alcohols is at low concentration pmol/L level according to the concentration calibration by exponential dilution method. Based on the measured ion mobilities, several chemical physics parameters of the ion-molecular interaction at atmosphere were obtained, including the ionic collision cross sections, diffusion coefficients, collision rate constants, and the ionic radii under the hard-sphere model approximation.

In situ Investigations of Interfacial Degradation and Ion Migration at CH3NH3PbI3 Perovskite/Ag Interfaces

Interfacial properties between perovskite layers and metal electrodes play a crucial role in the device performance and the long-term stability of perovskite solar cells.Here,we report a comprehensive study of the interfacial degradation and ion migration at the interface between CH3NH3PbI3 perovskite layer and Ag electrode.Using in situ photoemission spectroscopy measurements,we found that the Ag electrode could induce the degradation of perovskite layers,leading to the formation of PbI2 and AgI species and the reduction of Pb^2+ions to metallic Pb species at the interface.The unconventional enhancement of the intensities of I 3d spectra provides direct experimental evidences for the migration of iodide ions from CH3NH3PbI3 subsurface to Ag electrode.Moreover,the contact of Ag electrode and perovskite layers induces an interfacial dipole of 0.3 eV at CH3NH3PbI3/Ag interfaces,which may further facilitate iodide ion diffusion,resulting in the decomposition of perovskite layers and the corrosion of Ag electrode.

High tap density of Ni_3(PO_4)_2 coated LiNi_(1/3)Co_(1/3)Mn_(1/3)O_2 with enhanced cycling performance at high cut-off voltage

The Li Ni1/3Co1/3Mn1/3O2 is first obtained by the controlled crystallization method and then coated with Ni3(PO4)2particles. The effects of the coating on rate capability and cycle life at high cut-off voltage are investigated by electrochemical impedance spectroscopy and galvanostatic measurements. The element ratio of Ni:Mn:Co is tested by inductively-coupled plasma spectrometer(ICP) analysis and it testified to be 1:1:1. It is indicated that Ni3(PO4)2-coated Li Ni1/3Co1/3Mn1/3O2 has an outstanding capacity retention, where 99% capacity retention is maintained after 10 cycles at 5C discharge rate between 2.7 V and 4.6 V. The electrochemical impedance spectroscopy(EIS) results show that the current exchange density i0 of the coated sample is higher than that of Li Ni1/3Co1/3Mn1/3O2, which is beneficial to its electrochemical performances. All the conclusions show that the Ni3(PO4)2coating can prominently enhance the high rate performance of the Li Ni1/3Co1/3Mn1/3O2, especially at high cut-off voltage.

The Pulsed Plasma-Liquid Systems at Cylindrical Geometry with Possibility of Convergent Acoustic Waves Efficient Generation

This research investigates the possibility of convergent acoustic waves generation in the liquid by means of the sotmd waves reflection from the solid cylindrical surface, emerged in the pulsed electric discharge. The spectra of pulse discharge plasma emission in the water and in the air-water mixture were obtained. The temperature of cuprum and oxygen atoms electronic excitation levels and the temperature tendencies during the discharge current existence were calculated.

Carbon electrodes with ionophobic characteristics in organic electrolyte for high-performance electric double-layer capacitors

Activated carbon(AC)in organic electrolytebased electric double-layer capacitors(EDLCs)usually suffers from low specific capacitance.Most studies on AC focus on improving its surface area and optimizing pore structures to enhance its electrochemical performance in EDLCs.Unfortunately,the interfacial microenvironment,which is composed of nanoporous carbon and the organic electrolyte confined in it,is always ignored.Herein,a simple and powerful strategy to create AC with an ionophobic surface is proposed to address the poor efficiency of the electric doublelayer process.The polar C±F bonds formed in the AC material are characterized through near-edge X-ray absorption fine structure and X-ray photoelectron spectroscopy.The ionophobic characteristic of YP-F60 s in an organic electrolyte is extensively studied via contact angle measurements and smallangle X-ray scattering spectroscopy.An EDLC constructed with YP-F60 s as the electrode and 1 mol L^(-1) tetraethylammonium tetrafluoroborate/propylene carbonate as the electrolyte demonstrates high specific capacitance,low internal resistance,and excellent cycling stability.Our results successfully demonstrate the importance of the interfacial microenvironment of AC and its confined electrolyte to the electrochemical performance of EDLCs.Our work also offers new perspectives on the use of the CF;plasma technique to fabricate low-cost superior carbon for EDLCs.

Self-organized metal-semiconductor epitaxial graphene layer on off-axis 4H-SiC（0001）

The remarkable properties of graphene have shown promise for new perspectives in future electronics, notably for nanometer scale devices. Here we grow graphene epitaxially on an off-axis 4H-SiC（0001） substrate and demonstrate the formation of periodic arrangement of monolayer graphene on planar （0001） terraces and Bernal bilayer graphene on （1120） nanofacets of SiC. We investigate these lateral superlattices using Raman spectroscopy, atomic force microscopy/ electrostatic force microscopy （AFM/EFM） and X-ray and angle resolved photoemission spectroscopy （XPS/ARPES）. The correlation of EFM and ARPES reveals the appearance of permanent electronic band gaps in AB-stacked bilayer graphene on （1120） SiC nanofacets of 150 meV. This feature is confirmed by density functional theory （DFT） calculations. The charge transfer between the substrate and graphene bilayer results in an asymmetric charge distribution between the top and the bottom graphene layers opening an energy gap. This surface organization can be thus defined as self-organized metal-semiconductor graphene.

Electrochemical synthesis and the functionalization of few layer graphene in ionic liquid and redox ionic liquid

Electrochemical reductive exfoliation of graphite to few layered graphene(FLG) in presence of 1-ethyl-2,3-dimethyl imidazolium bis(trifluoromethylsulfonyl) imide ionic liquid and redox ionic liquid based ferrocene has been investigated. Thus, by applying a mild negative potential(-2.7 V vs. Fc/Fc^+) to carbon electrode in ionic liquid graphene flakes could be generated. The generated materials have been characterized by X-ray photoelectron spectroscopy, Raman spectroscopy, high resolution transmission electron microscopy and atomic force microscopy. XPS and Raman analysis show that the electrochemical reductive exfoliation provides the formation of FLG. The thickness of the resulting FLG was found to be ranged between 4 and1 nm. HR-TEM images reveal the formation of few graphene layers and in some cases single graphene layer was observed.Moreover, this electrochemical route conduces to the formation of ionic liquid functionalized FLG. Finally, the reductive exfoliation was further investigated in the presence of redox ionic liquid. XPS and electrochemical measurements confirm the presence of ferrocene.