Structure and peculiarities of the (8 x n)-type Si(001) surface prepared in a molecular-beam epitaxy chamber: a scanning tunneling microscopy study

A clean Si(001) surface thermally purified in an ultrahigh vacuum molecular-beam epitaxy chamber has been investigated by means of scanning tunneling microscopy. The morphological peculiarities of the Si(001) surface have been explored in detail. The classification of the surface structure elements has been carried out, the dimensions of the elements have been measured, and the relative heights of the surface relief have been determined. A reconstruction of the Si(001) surface prepared in the molecular-beam epitaxy chamber has been found to be (8 x n). A model of the Si(001)-(8 x n) surface structure is proposed.Comment: 4 pages, 8 figures. Complete versio

STM and RHEED study of the Si(001)-c(8x8) surface

The Si(001) surface deoxidized by short annealing at T~925C in the ultrahigh vacuum molecular beam epitaxy chamber has been in situ investigated by high resolution scanning tunnelling microscopy (STM) and reflected high energy electron diffraction (RHEED). RHEED patterns corresponding to (2x1) and (4x4) structures were observed during sample treatment. The (4x4) reconstruction arose at T<600C after annealing. The reconstruction was observed to be reversible: the (4x4) structure turned into the (2x1) one at T>600C, the (4x4) structure appeared again at recurring cooling. The c(8x8) reconstruction was revealed by STM at room temperature on the same samples. A fraction of the surface area covered by the c(8x8) structure decreased as the sample cooling rate was reduced. The (2x1) structure was observed on the surface free of the c(8x8) one. The c(8x8) structure has been evidenced to manifest itself as the (4x4) one in the RHEED patterns. A model of the c(8x8) structure formation has been built on the basis of the STM data. Origin of the high-order structure on the Si(001) surface and its connection with the epinucleation phenomenon are discussed.Comment: 26 pages, 12 figure

Hidden correlations in stochastic photoinduced dynamics of a solid-state electrolyte

Photoexcitation by ultrashort laser pulses plays a crucial role in controlling reaction pathways, creating nonequilibrium material properties, and offering a microscopic view of complex dynamics at the molecular level. The photo response following a laser pulse is, in general, non-identical between multiple exposures due to spatiotemporal fluctuations in a material or the stochastic nature of dynamical pathways. However, most ultrafast experiments using a stroboscopic pump-probe scheme struggle to distinguish intrinsic sample fluctuations from extrinsic apparatus noise, often missing seemingly random deviations from the averaged shot-to-shot response. Leveraging the stability and high photon-flux of time-resolved X-ray micro-diffraction at a synchrotron, we developed a method to quantitatively characterize the shot-to-shot variation of the photoinduced dynamics in a solid-state electrolyte. By analyzing temporal evolutions of the lattice parameter of a single grain in a powder ensemble, we found that the sample responses after different shots contain random fluctuations that are, however, not independent. Instead, there is a correlation between the nonequilibrium lattice trajectories following adjacent laser shots with a characteristic "correlation length" of approximately 1,500 shots, which represents an energy barrier of 0.38~eV for switching the photoinduced pathway, a value interestingly commensurate with the activation energy of lithium ion diffusion. Not only does our nonequilibrium noise correlation spectroscopy provide a new strategy for studying fluctuations that are central to phase transitions in both condensed matter and molecular systems, it also paves the way for discovering hidden correlations and novel metastable states buried in oft-presumed random, uncorrelated fluctuating dynamics

Alternative catalyst and exhaust gas sensor work at Argonne National Laboratory

Research programs at Argonne National Laboratory in the areas of automobile emissions monitoring and control are described. The mandate to improve automobile efficiency while reducing Pollution requires the development of new catalysts for exhaust emissions control that are capable of functioning efficiently under lean-burn engine operating conditions. It is also desirable that the use of expensive noble metal catalysts be avoided. NO{sub x} emissions will not be efficiently controlled by the current three-way, supported noble metal catalysts under lean-burn conditions. New catalysts are being sought that could effect the selective catalytic reduction (SCR) of NO{sub x} by exhaust hydrocarbons in the presence of oxygen. Molecular sieve zeolites of the ZSM-5 and ferrierite types, ion-exchanged with copper ions, are the best of the catalysts known to effect this chemistry, but the mechanism of the SCR is still not understood. In this project the authors will first undertake the investigation of the SCR of NO using model reactions to test postulated mechanistic pathways. Initial experiments have been devised to investigate the possible participation of metal alkyl complexes, metal oxime complexes, N-alkyl-N-nitroso-alkylaminato-metal complexes, and metal nitrile complexes in the zeolites. ANL will also develop microsensors, based on surface acoustic wave (SAW) chemical sensing techniques, and a micro mass-spectrometer (MS) for tailpipe or engine-out emission monitoring. The sensor configurations and sensing techniques of the proposed SAW and micro-MS are described