Structural effects on water formation from coadsorbed H + O on Rh(100)

The effect of adsorbate coverage, adsorption sequence and temperature on the structure, composition and reactivity of coadsorbed layers, produced by dissociative adsorption of O₂ and H₂ at 200 K on a Rh(100) surface, has been studied by combined TPD, XPS and LEED measurements. The emphasis is on the impact of the structure and composition of the mixed O + H layers on the synthesis of hydroxyl and water as a result of the O + H surface reaction. The difference in the O 1s binding energies of adsorbed O (529.9 eV) and OH species (530.8 eV) was used as a fingerprint to monitor the formation of the OH species. The H₂O TPD spectra show substantial variations of the desorption temperature range and the amount of water evolved with coadsorbate coverage and structure: from 270 to 350 K and from 0 to 0.08 ML, respectively. It has been found that dense O + H adlayers, where the O coverage is in the range 0.25-0.4 ML, favor the formation of stable OH species. The maximum amount of stable hydroxyl OH species ( 0.16 ML) can be produced by heating of these dense adlayers to 260 K. This results in reordering of the adspecies to form a new O + OH − (2 × 6) structure, where hydroxyls react readily to evolve 0.08 ML of water in a sharp desorption peak at 280 K. The effect of the adlayer density and restructuring on the production of OH and H₂O is discussed.     

Experimental and theoretical evidence for the chemical mechanism in SERRS of rhodamine 6G adsorbed on colloidal silver excited at 1064 nm

The evidence for the existence of a chemical mechanism in surface‐enhanced resonance Raman scattering (SERRS) of rhodamine 6G (R6G) adsorbed on colloidal silver excited at 1064 nm is reported on the basis of experimental and theoretical analyses. A weak absorption peak at around 1060 nm for R6G‐functionalized silver nanoparticles was observed, which is not present in the individual spectra of R6G or silver nanoparticles. Theoretically, the charge difference density reveals that this weak absorption is a metal‐to‐molecule charge transfer excited state. Copyright © 2010 John Wiley & Sons, Ltd.     

Interplay of superconductivity and d-f correlation in CeFeAs_(1-x)P_xO_(1-y)F_y

The recent discovery of high-temperature superconductivity in iron-based pnictides (chalcogenides) not only triggers tremendous enthusiasm in searching for new superconducting materials, but also opens a new avenue to the study of the Kondo physics. CeFeAsO is a parent compound of the 1111-type iron-based superconductors. It shows 3d-antiferromagnetic (AFM) ordering below ～ 139 K and 4f-AFM ordering below ～ 4 K. On the other hand, the phosphide CeFePO is a ferromagnetically correlated heavy-fermion (HF) metal with Kondo scale T K ～ 10 K. These properties set up a new platform for research of the interplay among magnetism, Kondo effect, and superconductivity (SC). In this review, we present the recent progress in the study of chemical pressure effect in CeFeAsO 1-y F y (y = 0 and 0.05). This P/As-doping in CeFeAsO serves as an effective controlling parameter which leads to two magnetic critical points, x c1 0.4 and x c2 0.92, associated with suppression of 3d and 4f magnetism, respectively. We also observe a turning point of AFM-FM ordering of Ce 3+ moment at x c3 0.37. The SC is absent in the phase diagram, which is attributed to the destruction to Cooper pair by Ce-FM fluctuations in the vicinity of x c1 . We continue to investigate CeFeAs 1-x P x O 0.95 F 0.05 . With the separation of x c1 and x c3 , this chemical pressure results in a broad SC region 0≤ x ≤ 0.53, while the original HF behavior is driven away by 5% F doping. Different roles of P and F dopings are addressed, and the interplay between SC and Ce-4f magnetism is also discussed.     

Mechanistic study of the reaction of methyl peroxy radical (CH3O2) with formaldehyde (CH2O)

ABSTRACT

A direct dynamic study on the reactions of CH₃O₂?+?CH₂O was carried out over the temperature range of 300–1500?K. All stationary points were calculated with the M06-2X/6-311++G(d,p) level of theory and identified for local minimum. The energetic parameters were refined at QCISD (T)/cc-pVTZ and CCSD (T)/cc-pVTZ levels of theory. Three channels were explored and a reaction of hydrogen abstraction from CH₂O by CH₃O₂ was identified as dominant channel which involves the formation of a prereactive complex in the entrance channel. The rate coefficient of the dominant channel was calculated with TST and TST/Eck and the Eckart tunnelling effect is only important over the lower temperature region. The calculated rate coefficient of the dominant channel has positive temperature dependence and agrees reasonably with the available literature data.     

Many-body effects in hyperfine interactions in <Superscript>205</Superscript>Pb<Superscript>+</Superscript>

Ab initio calculations have been carried out to study the magnetic dipole and electric quadrupole hyperfine structure constants of ²⁰⁵Pb⁺. Many-body effects have been considered to all orders using the relativistic coupled-cluster theory in the singles, doubles and partial triples approximation. The trends of these effects are found to be different from atomic systems that have been studied earlier.     

低温太阳热与甲醇化学链整合能量释放机理实验初探

本文在低温太阳热能与CH3OH-Fe2O3化学链燃烧相结合控制CO2分离动力系统的基础上,进一步探讨了低温太阳热能品位提升的内在规律,分别揭示出辐照强度与CH3OH-Fe2O3反应特性、低温太阳热能品位提升的关联关系.本文采用溶胶凝胶法制作了Fe2O3反应颗粒,在热重反应器中进行了模拟太阳热能与甲醇化学链实验的初步研究,通过电镜,分析了反应前后金属氧化物的表面形貌特征.研究成果将为低温太阳热能与化学链燃烧整合能量释放新机理的研究提供理论依据和基础实验数据.     

Light propagation and oscillations in two-dimensional graded square photonic lattices

We have studied the optical oscillations and transitions in two-dimensional graded square photonic lattices (GSPL) formed by evanescently coupled optical waveguide arrays with parabolic confinements in all transverse directions. When we retain only the orthogonal couplings, decoupled one-dimensional models can be used to obtain the various normal modes, which correspond to a variety of optical oscillations. Six different combinations of Bloch oscillation (BO), dipole oscillation (DO), and reflections from the boundaries of finite lattice are classified on the phase diagram. If we include the diagonal couplings, transitions among various oscillations are obtained with the Hamiltonian optics approach and confirmed by the field-evolution analysis. We studied in detail a typical example in which a switching occurs from the constituent BO and DO to both DOs in the two orthogonal directions. The method to analyze the complex field evolution in GSPL can be extended to similar systems with different types of lattices and/or confinements.     

Preparation and photocatalytic property of CeO2 lamellar

A novel room temperature solid-state chemical synthesis was introduced to successfully fabricate CeO₂ samples, coupled by a polyethylene glycol 400 (PEG 400)/cetyl trimethylammonium bromide (CTAB)/sodium dodecyl sulfate (SDS). The as-prepared products were characterized by XRD, TEM, SEM, BET and UV. A study of photocatalytic degradation of the methylene blue MB under UV illumination has been carried out. It is indicated that the samples exhibit excellent photocatalytic activity. Besides, the samples assisted with surfactants possess higher photocatalytic activity than the sample without any surfactants, wherein the sample with SDS as an additive shows the highest photocatalytic activity, which is able to reach 89.6% MB degradation ratio within 60 min illumination. Moreover, the effects of important operational parameters such as initial MB concentration, catalyst loading and pH were also investigated. The above sample under the optimum conditions obtained the maximum MB degradation ratio up to 96.5%, which is higher than that of the commercial TiO₂ P25 under the same conditions. It can be concluded that CeO₂ will be a potential photocatalyst in the application of organic pollutant.     

Effect of the thickness of InGaN interlayer on a-plane GaN epilayer

In this paper,we use the a-plane InGaN interlayer to improve the property of a-plane GaN.Based on the a-InGaN interlayer,a template exhibits that a regular,porous structure,which acts as a compliant effect,can be obtained to release the strain caused by the lattice and thermal mismatch between a-GaN and r-sapphire.We find that the thickness of InGaN has a great influence on the growth of a-GaN.The surface morphology and crystalline quality both are first improved and then deteriorated with increasing the thickness of the InGaN interlayer.When the InGaN thickness exceeds a critical point,the a-GaN epilayer peels off in the process of cooling down to room temperature.This is an attractive way of lifting off a-GaN films from the sapphire substrate.