Likelihood and conditional likelihood inference for generalized additive mixed models for clustered data

Lin and Zhang (J. Roy. Statist. Soc. Ser. B 61 (1999) 381) proposed the generalized additive mixed model (GAMM) as a framework for analysis of correlated data, where normally distributed random effects are used to account for correlation in the data, and proposed to use double penalized quasi-likelihood (DPQL) to estimate the nonparametric functions in the model and marginal likelihood to estimate the smoothing parameters and variance components simultaneously. However, the normal distributional assumption for the random effects may not be realistic in many applications, and it is unclear how violation of this assumption affects ensuing inferences for GAMMs. For a particular class of GAMMs, we propose a conditional estimation procedure built on a conditional likelihood for the response given a sufficient statistic for the random effect, treating the random effect as a nuisance parameter, which thus should be robust to its distribution. In extensive simulation studies, we assess performance of this estimator under a range of conditions and use it as a basis for comparison to DPQL to evaluate the impact of violation of the normality assumption. The procedure is illustrated with application to data from the Multicenter AIDS Cohort Study (MACS).     

Characterization of host-lattice emission and energy transfer in BaMgAl10O17:Eu

Host-lattice emission, energy transfer and degradation processes are characterized in undoped and Eu-doped BaMgAl₁₀O₁₇. Undoped BaMgAl₁₀O₁₇ exhibits a broad emission centered at 265 nm when excited at wavelengths shorter than 190 nm. This emission is assigned to exciton recombination at Ba-O groups in the cation layer of the lattice. The emission exhibits excellent overlap with the excitation band of Eu²⁺ in this host, providing a means of host-to-activator energy transfer in the doped phosphor. The exciton emission is relatively stable to thermal damage, but undergoes a peak shift and significant decrease in intensity after exposure to VUV radiation. Heating of VUV-damaged materials in air leads to some repair of the spectral properties.     

Gravitational Collapse of Self-Similar Perfect Fluid in 2 + 1 Gravity

Perfect fluid with kinematic self-similarity is studied in 2+1 dimensional spacetimes with circular symmetry, and various exact solutions to the Einstein field equations are given. These include all the solutions of dust and stiff perfect fluid with self-similarity of the first kind, and all the solutions of perfect fluid with a linear equation of state and self-similarity of the zeroth and second kinds. It is found that some of these solutions represent gravitational collapse, and the final state of the collapse can be either a black hole or a null singularity. It is also shown that one solution can have two different kinds of kinematic self-similarity.     

Does the beam width affect the generalized M factor of hard-edged diffracted beams?

A detailed study of the generalized M² factor of hard-edged diffracted beams based on the truncated second-order moments method, asymptotic analysis and self-convergent beam width approach is performed. The dependence of the generalized M² factor on the parameters characterizing the spatial profile, and beam truncation, etc. is analyzed.     

2‐connected 7‐coverings of 3‐connected graphs on surfaces

An m‐covering of a graph G is a spanning subgraph of G with maximum degree at most m. In this paper, we shall show that every 3‐connected graph on a surface with Euler genus k ≥ 2 with sufficiently large representativity has a 2‐connected 7‐covering with at most 6k ? 12 vertices of degree 7. We also construct, for every surface F² with Euler genus k ≥ 2, a 3‐connected graph G on F² with arbitrarily large representativity each of whose 2‐connected 7‐coverings contains at least 6k ? 12 vertices of degree 7. © 2003 Wiley Periodicals, Inc. J Graph Theory 43: 26–36, 2003     

Electrochemical characterization of poly(vinylidenefluoride)-zinc triflate gel polymer electrolyte and its application in solid-state zinc batteries

Gel polymer electrolyte (GPE) films comprising of poly(vinylidenefluoride), propylene carbonate, ethylene carbonate and zinc trifluoromethane sulfonate are prepared and characterized. The composition of GPE is optimized to contain minimum liquid components with a maximum specific conductivity of 3.94×10⁻³ S cm⁻¹ at (25±1) °C. A detailed investigation on the properties such as ionic conductivity, transport number, electrochemical stability window, reversibility of Zn/Zn²⁺ couple and Zn/gel electrolyte interfacial stability have been carried out. The ionic conductivity follows a VTF behaviour with an activation energy of about 0.0014 eV. Cationic transport number varies from 0.51 at 25 °C to 0.18 at 70 °C. Several cells have been assembled with GPE as the electrolyte, zinc as the anode, γ-MnO₂ as the cathode and their charge–discharge behaviour followed. Capacity values of 105, 82, 64 and 37 mAh/g of MnO₂ have been achieved at 10, 50, 100 and 200 μA/cm² discharge current densities, respectively. The discharge capacity values are almost constant for about 55 cycles for all values of current densities. Cyclic voltammetric study of MnO₂ electrode in Zn/GPE/MnO₂ cell clearly shows intercalation/deintercalation of Zn²⁺.     

二氧化碳和丙烯直接合成甲基丙烯酸的NiPMo/TiO2催化剂的研究

用溶胶 凝胶法以磷钼酸 (MPA)的镍盐溶液水解钛酸四丁酯制备了NiPMo/TiO2 催化剂 .使用ICP、XRD、TG DTA、IR、TPD MS和微反应技术研究了催化剂的化学组成、热稳定性、化学吸附性质和催化反应性能 .杂多钼酸盐与TiO2 通过O2 -在TiO2 表面发生了键合 .在 6 2 3K下 ,杂多阴离子仍保持原有的Keggin结构 .CO2 在Lewis酸位Ni(Ⅱ )和Lewis碱位Ni-O -Mo的桥氧协同作用下生成CO2 卧式吸附态Ni(Ⅱ )←O - (CO)← (O--Ni) .丙烯有多种吸附态在催化剂上吸附 .在 5 6 3K、1MPa和空速 15 0 0h-1的反应条件下 ,丙烯的摩尔转化率为 3.2 % ,产物MAA选择性为 95 % .     

Total synthesis of (±) maculalactone A, maculalactone B and maculalactone C and the determination of the absolute configuration of natural (+) maculalactone A by asymmetric synthesis

Maculalactones A, B and C from the marine cyanobacterium Kyrtuthrix maculans are amongst the only compounds based on the tribenzylbutyrolactone skeleton known in nature and (+) maculalactone A from the natural source possesses significant biological activity against various marine herbivores and marine settlers. We now report a concise synthesis of racemic maculalactone A in five steps from inexpensive starting materials. Maculalactones B and C were synthesized by a minor modification to this procedure, and the synthetic design also permitted an asymmetric synthesis of maculalactone A to be achieved in around 85% ee. The (+) and (−) enantiomers of maculalactone A were assigned, respectively, to the S and R configurations on the basis of the chiral selectivity expected for catecholborane reduction of an unsymmetrical ketone in the presence of Corey's oxazoborolidine catalyst. Surprisingly, it appeared that natural (+) maculalactone A was biosynthesized in K. maculans in a partially racemic form, comprising ca. 90-95% of the (S) enantiomer and 5-10% of its (R) enantiomer. Coincidentally therefore, the percentage enantiomeric excess of the product obtained from asymmetric synthesis almost exactly matched that found in nature.