Marked adsorption irreversibility of graphitic nanoribbons for CO2 and H2O

Graphene and graphitic nanoribbons possess different types of carbon hybridizations exhibiting different chemical activity. In particular, the basal plane of the honeycomb lattice of nanoribbons consisting of sp(2)-hybridized carbon atoms is chemically inert. Interestingly, their bare edges could be more reactive as a result of the presence of extra unpaired electrons, and for multilayer graphene nanoribbons, the presence of terraces and ripples could introduce additional chemical activity. In this study, a remarkable irreversibility in adsorption of CO(2) and H(2)O on graphitic nanoribbons was observed at ambient temperature, which is distinctly different from the behavior of nanoporous carbon and carbon blacks. We also noted that N(2) molecules strongly interact with the basal planes at 77 K in comparison with edges. The irreversible adsorptions of both CO(2) and H(2)O are due to the large number of sp(3)-hybridized carbon atoms located at the edges. The observed irreversible adsorptivity of the edge surfaces of graphitic nanoribbons for CO(2) and H(2)O indicates a high potential in the fabrication of novel types of catalysts and highly selective gas sensors.     

Super flexibility of a 2D Cu-based porous coordination framework on gas adsorption in comparison with a 3D framework of identical composition: framework dimensionality-dependent gas adsorptivities

Selective synthetic routes to coordination polymers [Cu(bpy)(2)(OTf)(2)](n) (bpy = 4,4'-bipyridine, OTf = trifluoromethanesulfonate) with 2- and 3-dimensionalities of the frameworks were established by properly choosing each different solvent-solution system. They show a quite similar local coordination environment around the Cu(II) centers, but these assemble in a different way leading to the 2D and 3D building-up structures. Although the two kinds of porous coordination polymers (PCPs) both have flexible frameworks, the 2D shows more marked flexibility than the 3D, giving rise to different flexibility-associated gas adsorption behaviors. All adsorption isotherms for N(2), CO(2), and Ar on the 3D PCP are of type I, whereas the 2D PCP has stepwise gas adsorption isotherms, also for CH(4) and water, in addition to these gases. The 3D structure, having hydrophilic and hydrophobic pores, shows the size-selective and quadrupole-surface electrical field interaction dependent adsorption. Remarkably, the 2D structure can accommodate greater amounts of gas molecules than that corresponding to the inherent crystallographic void volume through framework structural changes. In alcohol adsorption isotherms, however, the 2D PCP changes its framework structure through the guest accommodation, leading to no stepwise adsorption isotherms. The structural diversity of the 2D PCP stems from the breathing phenomenon and expansion/shrinkage modulation.     

Analysis of nonlinear steady state vibration of a multi-degree-of-freedom system using component mode synthesis method

In this paper, an analytical approach for nonlinear forced vibration of a multi-degree-of-freedom system is proposed using the component mode synthesis method. The whole system is divided into some components and a nonlinear modal equation of each component is derived using the free-interface vibration modes. The modal equations of all components and the conjunction conditions are solved simultaneously, and then the modal responses of components are derived. Finally, the dynamic responses of the whole system can be obtained. The degrees of freedom of modal equations can be reduced when the lower vibration modes are only adopted in each component. As a numerical example, a nine-degree-of-freedom system is considered, in which all spring have cubic type nonlinearity. As a result, it is shown that when there are no rigid modes in components, the compliance by the proposed method agrees very well with the exact one even if the lower vibration modes of components are only adopted. The other hand, in the case with rigid modes in components, the compliance has a little error compared with the exact result. It is recognized that the method proposed is very effective in the case without rigid modes in components for the actual application.     

调制掺杂ZnSe/BeTe Ⅱ型量子阱结构中的内秉电场和新型带电激子

报道了调制掺杂的ZnSe/BeTe/ZnSe Ⅱ型量子阱(type-Ⅱ QW)在低温(2—5 K)条件下的光致发光(PL),光致发光激发(PLE)和磁性光致发光(magneto-PL)光谱的实验结果.　观察到非掺杂样品的PL有两个很强的主发光峰而掺杂样品只有一个的奇异发光.　PL直线偏振度和PLE的测量结果都表明了这些空间间接型跃迁PL是来自两个异质结界面的贡献,非掺杂样品的两个主发光峰的分离则是起因于QW结构中的内秉电场(built-in electric field).在平行于QW生长方向的强磁场中, 关键词： 光致发光 二维电子气 带电激子 Ⅱ型量子阱     

213 W average power of 2.4 GW pulsed thermally controlled Nd:glass zigzag slab laser with a stimulated Brillouin scattering mirror

We report a high-average-power and high-pulse-energy diode-pumped Nd:glass laser amplifier system consisting of two thermally-edge-controlled zigzag slab amplifiers and a stimulated Brillouin scattering mirror. This phase-conjugated system produces an average power of 213 W at 10 Hz in a 8.9 ns pulse (2.4 GW peak power) with an optical-to-optical conversion efficiency of 11.7% and a near-diffraction-limited beam. To the best of our knowledge, this is the highest performance from a Nd:glass-based laser amplifier system ever built.     

Widely tunable ring-cavity tellurite fiber Raman laser

We report a widely tunable ring-cavity tellurite fiber Raman laser covering the S+C+L+U band. A tunable range (1495-1600 nm, limited by the tunable optical bandpass filter) over 100 nm is obtained by using a single-mode tellurite fiber with high Raman gain coefficients (55 W(-1)km(-1)) and large Raman shift (~22.3 THz) as the gain medium. Furthermore, the free-running 1665 nm Raman fiber laser is achieved from the ring cavity by removing the tunable optical bandpass filter, which shows that such a tellurite fiber has potential for constructing a widely tunable fiber Raman laser covering the S+C+L+U band. A high optical signal-to-noise ratio of over 60 dB for almost all of the tunable range is also demonstrated.     

Pressure-induced valence anomaly in TmTe probed by resonant inelastic X-ray scattering

The pressure-induced valence transition in TmTe was investigated by resonant inelastic x-ray scattering at the Tm L3 edge, a powerful probe of the rare-earth valent state. The data are analyzed within the Anderson impurity model which yields key parameters such as the Tm 4f-5d hybridization. In addition to the general tendency of the f electrons towards delocalization, we find a plateau in both the Tm valence and hybridization pressure dependences between 4.3 and 6.5 GPa which is interpreted in terms of an n-channel Kondo (NCK) screening process. This behavior is at odds with the usually continuous, single-channel Kondo-like f delocalization while being supported by the seminal calculations of the NCK temperature in Tm ion by Saso et al. Our study raises the interesting possibility that an NCK effect realized in a compressed mixed-valent f system could impede the concomitant electron delocalization.     

Optimal control of nonadiabatic alignment of rotationally cold N2 molecules with the feedback of degree of alignment

Nonadiabatic alignment of rotationally cold N2 molecules is optimally controlled by shaping femtosecond pump pulses with the feedback of degree of alignment evaluated by an ion imaging technique. The alignment is optimized by doubly peaked pulses with approximately equal intensities. A doubly peaked pulse with an appropriate interval can be regarded as a single pulse with a center trough based on the considerations from both time and frequency domains, suggesting that the effective duration of a doubly peaked pulse rather than its structure is crucial to nonadiabatic molecular alignment.     

Evidence for strong Breit interaction in dielectronic recombination of highly charged heavy ions

Resonant strengths have been measured for dielectronic recombination of Li-like iodine, holmium, and bismuth using an electron beam ion trap. By observing the atomic number dependence of the state-resolved resonant strength, clear experimental evidence has been obtained that the importance of the generalized Breit interaction (GBI) effect on dielectronic recombination increases as the atomic number increases. In particular, it has been shown that the GBI effect is exceptionally strong for the recombination through the resonant state [1s2s(2)2p(1/2)](1).     

RISM-SCF study of the free-energy profile of the Menshutkin-type reaction NH3+CH3Cl→NH3CH3++Cl− in aqueous solution

The free-energy profile for the Menshutkin-type reaction NH₃ + CH₃Cl → NH₃CH₃ ⁺ + Cl⁻ in aqueous solution is studied using the RISM-SCF method. The effect of electron correlation on the free-energy profile is estimated by the RISM-MP2 method at the HF optimized geometries along the reaction coordinate. Solvation was found to have a large influence on the vibrational frequencies at the reactant, transition state and product; these vibrational frequencies are utilized to calculate the zero-point energy correction of the free-energy profile. The computed barrier height and reaction exothermicity are in reasonable agreement with those of experiment and previous calculations. The change of solvation structure along the reaction path is represented by radial distribution functions between solute-solvent atomic sites. The mechanisms of the reaction are discussed from the view points of solute electronic and solvation structures. Received: 26 June 1998/Accepted: 28 August 1998 / Published online: 2 November 1998