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Ambient pressure photoelectron spectroscopy: a new tool for surface science and nanotechnology

Description: Progress in science often follows or parallels the development of new techniques. The optical microscope helped convert medicine and biology from a speculative activity in old times to today's sophisticated scientific disciplines. The telescope changed the study and interpretation of heavens from mythology to science. X-ray diffraction enabled the flourishing of solid state physics and materials science. The technique object of this review, Ambient Pressure Photoelectron Spectroscopy or APPES for short, has also the potential of producing dramatic changes in the study of liquid and solid surfaces, particularly in areas such as atmospheric, environment and catalysis sciences. APPES adds an important missing element to the host of techniques that give fundamental information, i.e., spectroscopy and microscopy, about surfaces in the presence of gases and vapors, as encountered in industrial catalysis and atmospheric environments. APPES brings electron spectroscopy into the realm of techniques that can be used in practical environments. Decades of surface science in ultra high vacuum (UHV) has shown the power of electron spectroscopy in its various manifestations. Their unique property is the extremely short elastic mean free path of electrons as they travel through condensed matter, of the order of a few atomic distances in the energy range from a few eV to a few thousand eV. As a consequence of this the information obtained by analyzing electrons emitted or scattered from a surface refers to the top first few atomic layers, which is what surface science is all about. Low energy electron diffraction (LEED), Auger electron spectroscopy (AES), X-ray photoelectron spectroscopy (XPS), Ultraviolet photoelectron spectroscopy (UPS), and other such techniques have been used for decades and provided some of the most fundamental knowledge about surface crystallography, composition and electronic structure available today. Unfortunately the high interaction cross section of electrons with matter also prevents them from traveling ...
Date: March 12, 2008
Creator: Salmeron, Miquel; Salmeron, Miquel & Schlogl, Robert
Partner: UNT Libraries Government Documents Department

The Nature of the Dissociation Sites of Hydrogen Molecules on Ru(001)

Description: Scanning tunneling microscopy (STM) was used to study the dissociative adsorption of H{sub 2} on Ru(001) near saturation coverage, when the number of residual hydrogen vacancies (i.e., unoccupied Ru sites) is small. We found that H{sub 2} dissociation takes place only on Ru sites where the metal atom is not bound to any H atom. Such active sites are formed when at least 3 H-vacancies aggregate by thermal diffusion. Sites formed by single H-vacancies or pairs of adjoining vacancies were found to be unreactive toward H{sub 2}. As a similar phenomenon was found previously on Pd(111), the present results indicate that the active sites for H2 dissociation share a common characteristic among catalytically active transition metals.
Date: March 12, 2008
Creator: Salmeron, Miquel; Rose, Franck; Tartakhanov, Mous; Fomin, Evgeni & Salmeron, Miquel
Partner: UNT Libraries Government Documents Department

In situ photoelectron spectroscopy study of water adsorption on model biomaterial surfaces

Description: Using in situ photoelectron spectroscopy at near ambient conditions, we compare the interaction of water with four different model biomaterial surfaces: self-assembled thiol monolayers on Au(111) that are functionalized with methyl, hydroxyl, and carboxyl groups, and phosphatidylcholine (POPC) lipid films on Silicon. We show that the interaction of water with biomaterial surfaces is mediated by polar functional groups that interact strongly with water molecules through hydrogen bonding, resulting in adsorption of 0.2-0.3 ML water on the polar thiol films in 700 mTorr water pressure and resulting in characteristic N1s and P2p shifts for the POPC films. Provided that beam damage is carefully controlled, in situ electron spectroscopy can give valuable information about water adsorption which is not accessible under ultra-high vacuum conditions.
Date: July 10, 2007
Creator: Salmeron, Miquel; Ketteler, Guido; Ashby, Paul; Mun, B.S.; Ratera, I.; Bluhm, Hendrik et al.
Partner: UNT Libraries Government Documents Department

Sensing Current and Forces with SPM

Description: Atomic force microscopy (AFM) and scanning tunneling microscopy (STM) are well established techniques to image surfaces and to probe material properties at the atomic and molecular scale. In this review, we show hybrid combinations of AFM and STM that bring together the best of two worlds: the simultaneous detection of atomic scale forces and conduction properties. We illustrate with several examples how the detection of forces during STM and the detection of currents during AFM can give valuable additional information of the nanoscale material properties.
Date: July 2, 2010
Creator: Park, Jeong Y.; Maier, Sabine; Hendriksen, Bas & Salmeron, Miquel
Partner: UNT Libraries Government Documents Department

Structure and Reactions of Carbon and Hydrogen on Ru(0001): A Scanning Tunneling Microscopy Study

Description: The interaction between carbon and hydrogen atoms on a Ru(0001) surface was studied using scanning tunneling microscopy (STM), Density Functional Theory (DFT) and STM image calculations. Formation of CH species by reaction between adsorbed H and C was observed to occur readily at 100 K. When the coverage of H increased new complexes of the form CH+nH (n = 1, 2 and 3) were observed. These complexes, never observed before, might be precursors for further hydrogenation reactions. DFT analysis reveals that a considerable energy barrier exists for the CH+H {yields} CH{sub 2} reaction.
Date: September 9, 2008
Creator: Shimizu, Tomoko K.; Mugarza, Aitor; Cerda, Jorge & Salmeron, Miquel
Partner: UNT Libraries Government Documents Department

Electronic contribution to friction on GaAs

Description: The electronic contribution to friction at semiconductor surfaces was investigated by using a Pt-coated tip with 50nm radius in an atomic force microscope sliding against an n-type GaAs(100) substrate. The GaAs surface was covered by an approximately 1 nm thick oxide layer. Charge accumulation or depletion was induced by the application of forward or reverse bias voltages. We observed a substantial increase in friction force in accumulation (forward bias) with respect to depletion (reverse bias). We propose a model based on the force exerted by the trapped charges that quantitatively explains the experimental observations of excess friction.
Date: April 15, 2008
Creator: Applied Science and Technology Graduate Group, UC Berkeley; Dept. of Materials Sciences and Engineering, UC Berkeley; Salmeron, Miquel; Qi, Yabing; Park, J.Y.; Hendriksen, B.L.M. et al.
Partner: UNT Libraries Government Documents Department

Structure and dynamics of dense monolayers of NO adsorbed on Rh(111) in equilibrium with the gas phase in the Torr pressure range

Description: Using Scanning Tunneling Microscopy, we show the phase transition between new structures of NO on Rh(111) in equilibrium with the gas phase near 300K, in the Torr pressure range. Two phases with (2x2)and (3x3) periodicity transform into each other as the pressure and temperature change around the equilibrium P-T line. By measuring P and T at coexistence, we determined the heat of adsorption in the(3x3) structure. From the phase boundary dynamics, the activation energy barrier between phases was estimated. The results demonstrate that unique information can be obtained from high-pressure and high-temperature studies.
Date: November 1, 2000
Creator: Rider, Keith B.; Hwang, Kevin S.; Salmeron, Miquel & Somorjai, Gabor A.
Partner: UNT Libraries Government Documents Department

Water Induced Surface Reconstruction of the Oxygen (2x1) covered Ru(0001)

Description: Low temperature scanning tunneling microscopy (STM) and density functional theory (DFT) were used to study the adsorption of water on a Ru(0001) surface covered with half monolayer of oxygen. The oxygen atoms occupy hcp sites in an ordered structure with (2x1) periodicity. DFT predicts that water is weakly bound to the unmodified surface, 86 meV compared to the ~;;200 meV water-water H-bond. Instead, we found that water adsorption causes a shift of half of the oxygen atoms from hcp sites to fcc sites, creating a honeycomb structure where water molecules bind strongly to the exposed Ru atoms. The energy cost of reconstructing the oxygen overlayer, around 230 meV per displaced oxygen atom, is more than compensated by the larger adsorption energy of water on the newly exposed Ru atoms. Water forms hydrogen bonds with the fcc O atoms in a (4x2) superstructure due to alternating orientations of the molecules. Heating to 185 K results in the complete desorption of the water layer, leaving behind the oxygen honeycomb structure, which is metastable relative to the original (2x1). This stable structure is not recovered until after heating to temperatures close to 260K.
Date: August 6, 2010
Creator: Maier, Sabine; Cabrera-Sanfelix, Pepa; Stass, Ingeborg; Sanchez-Portal, Daniel; Arnau, Andres & Salmeron, Miquel
Partner: UNT Libraries Government Documents Department

Chemical reactions of water molecules on Ru(0001) induced by selective excitation of vibrational modes

Description: Tunneling electrons in a scanning tunneling microscope were used to excite specific vibrational quantum states of adsorbed water and hydroxyl molecules on a Ru(0 0 0 1) surface. The excited molecules relaxed by transfer of energy to lower energy modes, resulting in diffusion, dissociation, desorption, and surface-tip transfer processes. Diffusion of H{sub 2}O molecules could be induced by excitation of the O-H stretch vibration mode at 445 meV. Isolated molecules required excitation of one single quantum while molecules bonded to a C atom required at least two quanta. Dissociation of single H{sub 2}O molecules into H and OH required electron energies of 1 eV or higher while dissociation of OH required at least 2 eV electrons. In contrast, water molecules forming part of a cluster could be dissociated with electron energies of 0.5 eV.
Date: May 7, 2009
Creator: Mugarza, Aitor; Shimizu, Tomoko K.; Ogletree, D. Frank & Salmeron, Miquel
Partner: UNT Libraries Government Documents Department

Photoelectron Spectroscopy under Ambient Pressure and Temperature Conditions

Description: We describe the development and applications of novel instrumentation for photoemission spectroscopy of solid or liquid surfaces in the presence of gases under ambient conditions or pressure and temperature. The new instrument overcomes the strong scattering of electrons in gases by the use of an aperture close to the surface followed by a differentially-pumped electrostatic lens system. In addition to the scattering problem, experiments in the presence of condensed water or other liquids require the development of special sample holders to provide localized cooling. We discuss the first two generations of Ambient Pressure PhotoEmission Spectroscopy (APPES) instruments developed at synchrotron light sources (ALS in Berkeley and BESSY in Berlin), with special focus on the Berkeley instruments. Applications to environmental science and catalytic chemical research are illustrated in two examples.
Date: February 27, 2009
Creator: Ogletree, D. Frank; Bluhm, Hendrik; Hebenstreit, Eleonore B. & Salmeron, Miquel
Partner: UNT Libraries Government Documents Department

A New Scanning Tunneling Microscope Reactor Used for High Pressure and High Temperature Catalysis Studies

Description: We present the design and performance of a home-built high-pressure and high-temperature reactor equipped with a high-resolution scanning tunneling microscope (STM) for catalytic studies. In this design, the STM body, sample, and tip are placed in a small high pressure reactor ({approx}19 cm{sup 3}) located within an ultrahigh vacuum (UHV) chamber. A sealable port on the wall of the reactor separates the high pressure environment in the reactor from the vacuum environment of the STM chamber and permits sample transfer and tip change in UHV. A combination of a sample transfer arm, wobble stick, and sample load-lock system allows fast transfer of samples and tips between the preparation chamber, high pressure reactor, and ambient environment. This STM reactor can work as a batch or flowing reactor at a pressure range of 10{sup -13} to several bars and a temperature range of 300-700 K. Experiments performed on two samples both in vacuum and in high pressure conditions demonstrate the capability of in situ investigations of heterogeneous catalysis and surface chemistry at atomic resolution at a wide pressure range from UHV to a pressure higher than 1 atm.
Date: May 12, 2008
Creator: Tao, Feng; Tang, David C.; Salmeron, Miquel & Somorjai, Gabor A.
Partner: UNT Libraries Government Documents Department

Water adsorption, solvation and deliquescence of alkali halide thin films on SiO2 studied by ambient pressure X-ray photoelectron spectroscopy

Description: The adsorption of water on KBr thin films evaporated onto SiO2 was investigated as a function of relative humidity (RH) by ambient pressure X-ray photoelectron spectroscopy. At 30percent RH adsorbed water reaches a coverage of approximately one monolayer. As the humidity continues to increase, the coverage of water remains constant or increases very slowly until 60percent RH, followed by a rapid increase up to 100percent RH. At low RH a significant number of the Br atoms are lost due to irradiation damage. With increasing humidity solvation increases ion mobility and gives rise to a partial recovery of the Br/K ratio. Above 60percent RH the increase of the Br/K ratio accelerates. Above the deliquescence point (85percent RH), the thickness of the water layer continues to increase and reaches more than three layers near saturation. The enhancement of the Br/K ratio at this stage is roughly a factor 2.3 on a 0.5 nm KBr film, indicating a strong preferential segregation of Br ions to the surface of the thin saline solution on SiO2.
Date: March 31, 2010
Creator: Arima, Kenta; Jiang, Peng; Deng, Xingyi; Bluhm, Henrik & Salmeron, Miquel
Partner: UNT Libraries Government Documents Department

Hydrogen adsorption on Ru(001) studied by Scanning TunnelingMicroscopy

Description: The adsorption of hydrogen on Ru(001) was studied by scanning tunneling microscopy at temperatures around 50 K. Hydrogen was found to adsorb dissociatively forming different ordered structures as a function of coverage. In order of increasing coverage {theta} in monolayers (ML) these were ({radical}3 x {radical}3)r30{sup o} at {theta} = 0.3 ML; (2 x 1) at {theta} = 0.50 ML, (2 x 2)-3H at {theta} = 0.75, and (1 x 1) at {theta} = 1.00. Some of these structures were observed to coexist at intermediate coverage values. Close to saturation of 1 ML, H-vacancies (unoccupied three fold fcc hollow Ru sites) were observed either as single entities or forming transient aggregations. These vacancies diffuse and aggregate to form active sites for the dissociative adsorption of hydrogen.
Date: January 18, 2008
Creator: Tatarkhanov, Mous; Rose, Franck; Fomin, Evgeny; Ogletree, D.Frank & Salmeron, Miquel
Partner: UNT Libraries Government Documents Department

The surface chemistry of Cu in the presence of CO2 and H2O

Description: The chemical nature of copper and copper oxide (Cu{sub 2}O) surfaces in the presence of CO{sub 2} and H{sub 2}O at room temperature was investigated using ambient pressure x-ray photoelectron spectroscopy. The studies reveal that in the presence of 0.1 torr CO{sub 2} several species form on the initially clean Cu, including carbonate CO{sub 3}{sup 2}, CO{sub 2}{sup {delta}-} and C{sup 0}, while no modifications occur on an oxidized surface. The addition of 0.1 ML Zn to the Cu results in the complete conversion of CO{sub 2}{sup {delta}-} to carbonate. In a mixture of 0.1 torr H{sub 2}O and 0.1 torr CO{sub 2}, new species are formed, including hydroxyl, formate and methoxy, with H{sub 2}O providing the hydrogen needed for the formation of hydrogenated species.
Date: July 16, 2008
Creator: Deng, Xingyi; Verdaguer, Albert; Herranz, Tirma; Weis, Christoph; Bluhm, Hendrik & Salmeron, Miquel
Partner: UNT Libraries Government Documents Department

Electrical transport and mechanical properties of alkylsilane self-assembled monolayers on silicon surfaces probed by atomic force microscopy

Description: The correlation between molecular conductivity and mechanical properties (molecular deformation and frictional responses) of hexadecylsilane self-assembled monolayers was studied with conductive probe atomic force microscopy/friction force microscopy in ultrahigh vacuum. Current and friction were measured as a function of applied pressure, simultaneously, while imaging the topography of self-assembled monolayer molecule islands and silicon surfaces covered with a thin oxide layer. Friction images reveal lower friction over the molecules forming islands than over the bare silicon surface, indicating the lubricating functionality of alkylsilane molecules. By measuring the tunneling current change due to changing of the height of the molecular islands by tilting the molecules under pressure from the tip, we obtained an effective conductance decay constant ({beta}) of 0.52/{angstrom}.
Date: February 6, 2009
Creator: Park, Jeong Young; Qi, Yabing; Ashby, Paul D.; Hendriksen, Bas L.M. & Salmeron, Miquel
Partner: UNT Libraries Government Documents Department

Reactivity of Ozone with Solid Potassium Iodide Investigated by Atomic Force Microscopy

Description: The reaction of ozone with the (100) plane of solid potassium iodide (KI) was investigated using atomic force microscopy (AFM). The reaction forming potassium iodate (KIO{sub 3}) initiates at step edges prior to reacting on the flat terraces. Small domains of KIO{sub 3}, initially 3.8 {angstrom} in height are formed on the top of step edges. Following reaction at the step edge, domains of KIO{sub 3} are formed across the terraces. With prolonged exposure to ozone, KIO{sub 3} domains nucleate further growth until the surface is evenly covered with KIO{sub 3} particles that are 4-6 nm in height, at which point the surface is passivated and the reaction terminates.
Date: April 14, 2008
Creator: Mulleregan, Alice; Brown, Matthew A.; Ashby, Paul D.; Ogletree, D. Frank; Salmeron, Miquel & Hemminger, John C.
Partner: UNT Libraries Government Documents Department

Autocatalytic water dissociation on Cu(110) at near ambient conditions

Description: Autocatalytic dissociation of water on the Cu(110) metal surface is demonstrated based on X-ray photoelectron spectroscopy studies carried out in-situ under near ambient conditions of water vapor pressure (1 Torr) and temperature (275-520 K). The autocatalytic reaction is explained as the result of the strong hydrogen-bond in the H{sub 2}O-OH complex of the dissociated final state, which lowers the water dissociation barrier according to the Broensted-Evans-Polanyi relations. A simple chemical bonding picture is presented which predicts autocatalytic water dissociation to be a general phenomenon on metal surfaces.
Date: May 16, 2007
Creator: Mulleregan, Alice; Andersson, Klas; Ketteler, Guido; Bluhm, Hendrik; Yamamoto, Susumu; Ogasawara, Hirohito et al.
Partner: UNT Libraries Government Documents Department

In situ spectroscopic detection of SMSI effect in a Ni/CeO2 system: hydrogen-induced burial and dig out of metallic nickel

Description: In situ APPES technique demonstrates that the strong metal support interaction effect (SMSI) in the Ni-ceria system is associated with the decoration and burial of metallic particles by the partially reduced support, a phenomenon reversible by evacuation at high temperature of the previously absorbed hydrogen.
Date: June 29, 2010
Creator: Caballero, Alfonso; Holgado, Juan P.; Gonzalez-delaCruz, Victor M.; Habas, Susan e.; Herranz, Tirma & Salmeron, Miquel
Partner: UNT Libraries Government Documents Department

In-situ X-ray photoelectron spectroscopy studies of water on metals and oxides at ambient conditions

Description: X-ray photoelectron spectroscopy (XPS) is a powerful tool for surface and interface analysis, providing the elemental composition of surfaces and the local chemical environment of adsorbed species. Conventional XPS experiments have been limited to ultrahigh vacuum (UHV) conditions due to a short mean free path of electrons in a gas phase. The recent advances in instrumentation coupled with third-generation synchrotron radiation sources enables in-situ XPS measurements at pressures above 5 Torr. In this review, we describe the basic design of the ambient pressure XPS setup that combines differential pumping with an electrostatic focusing. We present examples of the application of in-situ XPS to studies of water adsorption on the surface of metals and oxides including Cu(110), Cu(111), TiO2(110) under environmental conditions of water vapor pressure. On all these surfaces we observe a general trend where hydroxyl groups form first, followed by molecular water adsorption. The importance of surface OH groups and their hydrogen bonding to water molecules in water adsorption on surfaces is discussed in detail.
Date: October 29, 2007
Creator: Salmeron, Miquel; Yamamoto, S.; Bluhm, H.; Andersson, K.; Ketteler, G.; Ogasawara, H. et al.
Partner: UNT Libraries Government Documents Department

Adsorption of water on O(2x2)/Ru(0001): thermal stability and inhibition of dissociation by H2O-O bonding

Description: The effect of preadsorbed oxygen on the subsequent adsorption and reactions of water on Ru(0001) has been studied using low temperature scanning tunneling microscopy and DFT calculations. Experiments were carried out for O coverages close to 0.25 ML. It was found that no dissociation of water takes place up to the desorption temperature of {approx}180-230 K. DFT calculations show that intact water on O(2x2)/Ru(0001) is {approx} 0.49 eV more stable than the dissociation products, H and OH, at their preferred fcc and top adsorption sites.
Date: August 1, 2008
Creator: Mugarza, Aitor; Shimizu, Tomoko; Cabrera-Sanfelix, Pepa; Sanchez-Portal, Daniel; Arnau, Andres & Salmeron, Miquel
Partner: UNT Libraries Government Documents Department

Decisive role of the energetics of dissociation products in the adsorption of water on O/Ru(0001)

Description: Using density-functional theory they found that, depending on coverage, coadsorbed oxygen can act both as a promoter and as an inhibitor of the dissociation of water on Ru(0001), the transition between these two behaviors occurring at (0.2 M). The key factor that determines this transition is the adsorption energy of the reaction products, OH in particular. The chemistry of this coadsorbed system is dictated by the effective coordination of the Ru atoms that participate in the bonding of the different species. In particular, they observed that a low coverage of oxygen increases the adsorption energy of the OH fraction on the Ru surface. This surprising extra stabilization of the OH with the coadsorption of oxygen can be understood in the context of the metallic bonding and could well correspond to a general trend for the coadsorption of electronegative species on metallic surfaces.
Date: October 15, 2008
Creator: Cabrera-Sanfelix, Pepa; Arnau, Andres; Mugarza, Aitor; Shimizu, Tomoko K.; Salmeron, Miquel & Sánchez-Portal, Daniel
Partner: UNT Libraries Government Documents Department

Friction Anisotropy: A unique and intrinsic property of decagonal quasicrystals

Description: We show that friction anisotropy is an intrinsic property of the atomic structure of Al-Ni-Co decagonal quasicrystals and not only of clean and well-ordered surfaces that can be prepared in vacuum [J.Y. Park et al., Science (2005)]. Friction anisotropy is manifested both in nanometer size contacts obtained with sharp atomic force microscope (AFM) tips as well as in macroscopic contacts produced in pin-on-disc tribometers. We show that the friction anisotropy, which is not observed when an amorphous oxide film covers the surface, is recovered when the film is removed due to wear. Equally important is the loss of the friction anisotropy when the quasicrystalline order is destroyed due to cumulative wear. These results reveal the intimate connection between the mechanical properties of these materials and their peculiar atomic structure.
Date: June 25, 2008
Creator: Mulleregan, Alice; Park, Jeong Young; Salmeron, Miquel; Ogetree, D.F.; Jenks, C.J.; Thiel, P.A. et al.
Partner: UNT Libraries Government Documents Department

Graphene Growth by Metal Etching on Ru (0001)

Description: Low-energy electron microscopy (LEEM) reveals a new mode of graphene growth on Ru(0001) in which Ru atoms from a step edge are injected under a growing graphene sheet. The injected atoms can form under-graphene islands, or incorporate into the topmost Ru layer, thereby increasing its density and forming dislocation networks. Density functional calculations imply that Ru islands nucleated between the graphene layer and the substrate are energetically stable; scanning tunneling microscopy (STM) reveals that dislocation networks exist near step edges.
Date: September 14, 2009
Creator: Loginova, Elena; Maier, Sabine; Stass, Ingeborg; Bartelt, Norman; Feibelman, Peter; Salmeron, Miquel et al.
Partner: UNT Libraries Government Documents Department

Nonlinear broadband photoluminescence of graphene induced by femtosecond laser irradiation

Description: Upon femtosecond laser irradiation, a bright, broadband photoluminescence is observed from graphene at frequencies well above the excitation frequency. Analyses show that it arises from radiative recombination of a broad distribution of nonequilibrium electrons and holes, generated by rapid scattering between photoexcited carriers within tens of femtoseconds after the optical excitation. Its highly unusual characteristics come from the unique electronic and structural properties of graphene.
Date: July 1, 2010
Creator: Liu, Wei-Tao; Wu, S.W.; Schuck, P.J.; Salmeron, Miquel; Shen, Y.R. & Wang, F.
Partner: UNT Libraries Government Documents Department