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Full-Text Articles in Physics

Sulfur Adsorption On Coinage Metal (100) Surfaces: Propensity For Metal-Sulfur Complex Formation Relative To (111) Surfaces, Da-Jiang Liu, Peter M. Spurgeon, Jiyoung Lee, Theresa L. Windus, Patricia A. Thiel, James W. Evans Nov 2019

Sulfur Adsorption On Coinage Metal (100) Surfaces: Propensity For Metal-Sulfur Complex Formation Relative To (111) Surfaces, Da-Jiang Liu, Peter M. Spurgeon, Jiyoung Lee, Theresa L. Windus, Patricia A. Thiel, James W. Evans

Chemistry Publications

Experimental data from low-temperature Scanning Tunneling Microscopy (LTSTM) studies on coinage metal surfaces with very low coverages of S is providing new insights into metal-S interactions. A previous LTSTM study for Cu(100), and a new analysis reported here for Ag(100), both indicate no metal-sulfur complex formation, but an Au4S5 complex was observed previously on Au(100). In marked contrast, various complexes have been proposed and/or observed on Ag(111) and Cu(111), but not on Au(111). Also, exposure to trace amounts of S appears to enhance mass transport far more dramatically on (111) than on (100 ...


Characteristics Of Sulfur Atoms Adsorbed On Ag(100), Ag(110), And Ag(111) As Probed With Scanning Tunneling Microscopy: Experiment And Theory, Peter M. Spurgeon, Da-Jiang Liu, Holly Walen, Junepyo Oh, Hyun Jin Yang, Yousoo Kim, Patricia A. Thiel May 2019

Characteristics Of Sulfur Atoms Adsorbed On Ag(100), Ag(110), And Ag(111) As Probed With Scanning Tunneling Microscopy: Experiment And Theory, Peter M. Spurgeon, Da-Jiang Liu, Holly Walen, Junepyo Oh, Hyun Jin Yang, Yousoo Kim, Patricia A. Thiel

Chemistry Publications

In this paper, we report that S atoms on Ag(100) and Ag(110) exhibit a distinctive range of appearances in scanning tunneling microscopy (STM) images, depending on the sample bias voltage, VS. Progressing from negative to positive VS, the atomic shape can be described as a round protrusion surrounded by a dark halo (sombrero) in which the central protrusion shrinks, leaving only a round depression. This progression resembles that reported previously for S atoms on Cu(100). We test whether DFT can reproduce these shapes and the transition between them, using a modified version of the Lang–Tersoff–Hamann ...


Kinetics, Energetics, And Size Dependence Of The Transformation From Pt To Ordered Ptsn Intermetallic Nanoparticles, Minda Chen, Yong Han, Tian Wei Goh, Rong Sun, Raghu V. Maligal‐Ganesh, Yuchen Pei, Chia‐ Kuang Tsung, James W. Evans, Wenyu Huang Jan 2019

Kinetics, Energetics, And Size Dependence Of The Transformation From Pt To Ordered Ptsn Intermetallic Nanoparticles, Minda Chen, Yong Han, Tian Wei Goh, Rong Sun, Raghu V. Maligal‐Ganesh, Yuchen Pei, Chia‐ Kuang Tsung, James W. Evans, Wenyu Huang

Chemistry Publications

The outstanding catalytic activity and chemical selectivity of intermetallic compounds make them excellent candidates for heterogeneous catalysis. However, the kinetics of their formation at the nanoscale is poorly understood or characterized, and precise control of their size, shape as well as composition during synthesis remains challenging. Here, using well-defined Pt nanoparticles (5 nm and 14 nm) encapsulated in mesoporous silica, we study the transformation kinetics from monometallic Pt to intermetallic PtSn at different temperatures by a series of time-evolution X-ray diffraction studies. Observations indicate an initial transformation stage mediated by Pt surface-controlled intermixing kinetics, followed by a second stage with ...


Spatial–Temporal Spectroscopy Characterizations And Electronic Structure Of Methylammonium Perovskites, Zhaoyu Liu, K. C. Bhamu, Liang Luo, Satvik Shah, Joong-Mok Park, Di Cheng, Men Long, Rana Biswas, F. Fungara, Ruth Shinar, Joseph Shinar, Javier Vela, Jigang Wang Jul 2018

Spatial–Temporal Spectroscopy Characterizations And Electronic Structure Of Methylammonium Perovskites, Zhaoyu Liu, K. C. Bhamu, Liang Luo, Satvik Shah, Joong-Mok Park, Di Cheng, Men Long, Rana Biswas, F. Fungara, Ruth Shinar, Joseph Shinar, Javier Vela, Jigang Wang

Chemistry Publications

Using time-resolved laser-scanning confocal microscopy and ultrafast optical pump/THz probe spectroscopy, we measure photoluminescence and THz-conductivity in perovskite micro-crystals and films. Photoluminescence quenching and lifetime variations occur from local heterogeneity. Ultrafast THz-spectra measure sharp quantum transitions from excitonic Rydberg states, providing weakly bound excitons with a binding energy of ~13.5 meV at low temperatures. Ab-initio electronic structure calculations give a direct band gap of 1.64 eV, a dielectric constant ~18, heavy electrons, and light holes, resulting in weakly bound excitons, consistent with the binding energies from experiment. The complementary spectroscopy and simulations reveal fundamental insights into perovskite ...


Pore Diameter Dependence Of Catalytic Activity: P-Nitrobenzaldehyde Conversion To An Aldol Product In Amine-Functionalized Mesoporous Silica, Andres Garcia, Igor I. Slowing, James W. Evans Jul 2018

Pore Diameter Dependence Of Catalytic Activity: P-Nitrobenzaldehyde Conversion To An Aldol Product In Amine-Functionalized Mesoporous Silica, Andres Garcia, Igor I. Slowing, James W. Evans

Chemistry Publications

The reaction yield for conversion of p-nitrobenzaldehyde (PNB) to an aldol product in amine-functionalized mesoporous silica nanoparticles (MSN) exhibits a 20-fold enhancement for a modest increase in pore diameter, d. This enhanced catalytic activity is shown to reflect a strong increase in the “passing propensity,” 𝒫, of reactant and product species inside the pores. We find that 𝒫 ≈ 0, corresponding to single-file diffusion, applies for the smallest d which still significantly exceeds the linear dimensions of PNB and the aldol product. However, in this regime of narrow pores, these elongated species must align with each other and with the pore ...


Theoretical Prediction Of Crystallization Kinetics Of A Supercooled Lennard-Jones Fluid, K. G. S. H. Gunawardana, Xueyu Song May 2018

Theoretical Prediction Of Crystallization Kinetics Of A Supercooled Lennard-Jones Fluid, K. G. S. H. Gunawardana, Xueyu Song

Chemistry Publications

The first order curvature correction to the crystal-liquid interfacial free energy is calculated using a theoretical model based on the interfacial excess thermodynamic properties. The correction parameter (δ), which is analogous to the Tolman length at a liquid-vapor interface, is found to be 0.48 ± 0.05 for a Lennard-Jones (LJ) fluid. We show that this curvature correction is crucial in predicting the nucleation barrier when the size of the crystal nucleus is small. The thermodynamic driving force (Δμ) corresponding to available simulated nucleation conditions is also calculated by combining the simulated data with a classical density functional theory ...


Defect-Mediated, Thermally-Activated Encapsulation Of Metals At The Surface Of Graphite, Yinghui Zhou, Ann Lii-Rosales, Minsung Kim, Mark Wallingford, Dapeng Jing, Michael C. Tringides, Cai-Zhuang Wang, Patricia A. Thiel Feb 2018

Defect-Mediated, Thermally-Activated Encapsulation Of Metals At The Surface Of Graphite, Yinghui Zhou, Ann Lii-Rosales, Minsung Kim, Mark Wallingford, Dapeng Jing, Michael C. Tringides, Cai-Zhuang Wang, Patricia A. Thiel

Chemistry Publications

We show that 3 metals – Dy, Ru, and Cu – can form multilayer intercalated (encapsulated) islands at the graphite (0001) surface if 2 specific conditions are met: Defects are introduced on the graphite terraces to act as entry portals, and the metal deposition temperature is well above ambient. Focusing on Dy as a prototype, we show that surface encapsulation is much different than bulk intercalation, because the encapsulated metal takes the form of bulk-like rafts of multilayer Dy, rather than the dilute, single-layer structure known for the bulk compound. Carbon-covered metallic rafts even form for relatively unreactive metals (Ru and Cu ...


Polar Intermetallics Pr5co2ge3 And Pr7co2ge4 With Planar Hydrocarbon‐Like Metal Clusters, Qisheng Lin, Kaiser Aguirre, Scott M. Saunders, Timothy A. Hackett, Yong Liu, Valentin Taufour, Durga Paudyal, Sergey L. Bud’Ko, Paul C. Canfield, Gordon J. Miller Aug 2017

Polar Intermetallics Pr5co2ge3 And Pr7co2ge4 With Planar Hydrocarbon‐Like Metal Clusters, Qisheng Lin, Kaiser Aguirre, Scott M. Saunders, Timothy A. Hackett, Yong Liu, Valentin Taufour, Durga Paudyal, Sergey L. Bud’Ko, Paul C. Canfield, Gordon J. Miller

Chemistry Publications

Planar hydrocarbon‐like metal clusters may foster new insights linking organic molecules with conjugated π–π bonding interactions and inorganic structures in terms of their bonding characteristics. However, such clusters are uncommon in polar intermetallics. Herein, we report two polar intermetallic phases, Pr5Co2Ge3 and Pr7Co2Ge4, both of which feature such planar metal clusters, namely, ethylene‐like [Co2Ge4] clusters plus the concatenated forms and polyacene‐like [Co2Ge2]n ribbons in Pr5Co2Ge3, and 1,2,4,5‐tetramethylbenzene‐like [Co4Ge6] cluster in Pr7Co2Ge4. Just as in the related planar organic structures, these metal–metalloid species are dominated by covalent bonding interactions. Both ...


Crystal Structure, Homogeneity Range And Electronic Structure Of Rhombohedral Γ-Mn5al8, Srinivasa Thimmaiah, Zachary Tener, Tej N. Lamichhane, Paul C. Canfield, Gordon J. Miller Jul 2017

Crystal Structure, Homogeneity Range And Electronic Structure Of Rhombohedral Γ-Mn5al8, Srinivasa Thimmaiah, Zachary Tener, Tej N. Lamichhane, Paul C. Canfield, Gordon J. Miller

Chemistry Publications

The γ-region of the Mn–Al phase diagram between 45 and 70 at.% Al was re-investigated by a combination of powder and single crystal X-ray diffraction as well as EDS analysis to establish the distribution of Mn and Al atoms. Single crystals of γ-Mn5–x Al8+x were grown using Sn-flux at 650 °C. The crystal structure, atomic coordinates and site occupancy parameters of γ-Mn5−x Al8+x phases were refined from single crystal X-ray data. The γ-Mn5-x Al8+x phase adopts the rhombohedral Cr5Al8-type structure rather than a cubic γ-brass structure. The refined compositions from two crystals extracted ...


A Molecular Debye-Hückel Theory And Its Applications To Electrolyte Solutions: The Size Asymmetric Case, Tiejen Xiao, Xueyu Song Mar 2017

A Molecular Debye-Hückel Theory And Its Applications To Electrolyte Solutions: The Size Asymmetric Case, Tiejen Xiao, Xueyu Song

Chemistry Publications

A molecular Debye-Hückel theory for electrolyte solutions with size asymmetry is developed, where the dielectric response of an electrolyte solution is described by a linear combination of Debye-Hückel-like response modes. As the size asymmetry of an electrolyte solution leads to a charge imbalanced border zone around a solute, the dielectric response to the solute is characterized by two types of charge sources, namely, a bare solute charge and a charge distribution due to size asymmetry. These two kinds of charge sources are screened by the solvent differently, our theory presents a method to calculate the mean electric potential as well ...


Tailoring Nanoscale Morphology Of Polymer: Fullerene Blends Using Electrostatic Field, Moneim Elshobaki, Ryan S. Gebhardt, John Carr, William Lindemann, Wenjie Wang, Eric Grieser, Swaminathan Venkatesan, Evan Ngo, Ujjal Bhattacharjee, Joseph Strzalka, Zhang Jiang, Qiquan Qiao, Jacob W. Petrich, David Vaknin, Sumit Chaudhary Jan 2017

Tailoring Nanoscale Morphology Of Polymer: Fullerene Blends Using Electrostatic Field, Moneim Elshobaki, Ryan S. Gebhardt, John Carr, William Lindemann, Wenjie Wang, Eric Grieser, Swaminathan Venkatesan, Evan Ngo, Ujjal Bhattacharjee, Joseph Strzalka, Zhang Jiang, Qiquan Qiao, Jacob W. Petrich, David Vaknin, Sumit Chaudhary

Chemistry Publications

To tailor the nanomorphology in polymer/fullerene blends, we study the effect of electrostatic field (E-field) on the solidification of poly(3-hexylthiophene-2, 5-diyl) (P3HT):[6,6]-phenyl-C61-butyric acid methyl ester (PC60BM) bulk heterojunction (BHJ). In addition to control; wet P3HT:PC60BM thin films were exposed to E-field of Van de Graaff (VDG) generator at three different directions—horizontal (H), tilted (T), and vertical (V)—relative to the plane of the substrate. Surface and bulk characterizations of the field-treated BHJs affirmed that fullerene molecules can easily penetrate the spaghetti-like P3HT and move up and down following the E-field. Using E-field treatment ...


Enhancement Of The Superconducting Gap By Nesting In Cakfe4as4: A New High Temperature Superconductor, Daixiang Mou, Tai Kong, William R. Meier, Felix Lochner, Lin-Lin Wang, Qisheng Lin, Yun Wu, S. L. Bud’Ko, Ilya Eremin, Duane D. Johnson, Paul C. Canfield, Adam Kaminski Dec 2016

Enhancement Of The Superconducting Gap By Nesting In Cakfe4as4: A New High Temperature Superconductor, Daixiang Mou, Tai Kong, William R. Meier, Felix Lochner, Lin-Lin Wang, Qisheng Lin, Yun Wu, S. L. Bud’Ko, Ilya Eremin, Duane D. Johnson, Paul C. Canfield, Adam Kaminski

Chemistry Publications

We use high resolution angle resolved photoemission spectroscopy and density functional theory with measured crystal structure parameters to study the electronic properties of CaKFe4As4. In contrast to the related CaFe2As2 compounds, CaKFe4As4 has a high Tc of 35 K at stochiometric composition. This presents a unique opportunity to study the properties of high temperature superconductivity in the iron arsenides in the absence of doping or substitution. The Fermi surface consists of several hole and electron pockets that have a range of diameters. We find that the values of the superconducting gap are nearly isotropic (within the explored portions of the ...


The Transition From The Open Minimum To The Ring Minimum On The Ground State And On The Lowest Excited State Of Like Symmetry In Ozone: A Configuration Interaction Study, Theresa Lynn Windus, Daniel Theis, Joseph Ivanic, Klaus Ruedenberg Jan 2016

The Transition From The Open Minimum To The Ring Minimum On The Ground State And On The Lowest Excited State Of Like Symmetry In Ozone: A Configuration Interaction Study, Theresa Lynn Windus, Daniel Theis, Joseph Ivanic, Klaus Ruedenberg

Chemistry Publications

The metastable ring structure of the ozone 11A1 ground state, which theoretical calculations have shown to exist, has so far eluded experimental detection. An accurate prediction for the energy difference between this isomer and the lower open structure is therefore of interest, as is a prediction for the isomerization barrier between them, which results from interactions between the lowest two 1A1 states. In the present work, valence correlated energies of the 11A1 state and the 21A1 state were calculated at the 11A1 open minimum, the 11A1 ring minimum, the transition state between these two minima, the minimum of the 21A1 ...


Oxygen Trapped By Rare Earth Tetrahedral Clusters In Nd4feos6: Crystal Structure, Electronic Structure, And Magnetic Properties, Qisheng Lin, Valentin Taufour, Yuemei Zhang, Max Wood, Thomas Drtina, Sergey L. Bud’Ko, Paul C. Canfield, Gordon J. Miller Sep 2015

Oxygen Trapped By Rare Earth Tetrahedral Clusters In Nd4feos6: Crystal Structure, Electronic Structure, And Magnetic Properties, Qisheng Lin, Valentin Taufour, Yuemei Zhang, Max Wood, Thomas Drtina, Sergey L. Bud’Ko, Paul C. Canfield, Gordon J. Miller

Chemistry Publications

Single crystals of Nd4FeOS6 were grown from an Fe–S eutectic solution. Single crystal X-ray diffraction analysis revealed a Nd4MnOSe6-type structure (P63mc, a=9.2693(1) Å, c=6.6650(1)Å, V=495.94(1) Å3, Z=2), featuring parallel chains of face-sharing [FeS6×1/2]4− trigonal antiprisms and interlinked [Nd4OS3]4+ cubane-like clusters. Oxygen atoms were found to be trapped by Nd4 clusters in the [Nd4OS3]4+ chains. Structural differences among Nd4MnOSe6-type Nd4FeOS6and the related La3CuSiS7− and Pr8CoGa3-type structures have been described. Magnetic susceptibility measurements on Nd4FeOS6 suggested the dominance of antiferromagnetic interactions at low ...


Β-Mn-Type Co8+Xzn12–X As A Defect Cubic Laves Phase: Site Preferences, Magnetism, And Electronic Structure, Weiwei Xie, Srinvasa Timmaiah, Jagat Lamal, Jing Liu, Thomas W. Heitmann, Dante Quirinale, A. I. Goldman, Vitalij K. Pecharsky, Gordon J. Miller Jan 2013

Β-Mn-Type Co8+Xzn12–X As A Defect Cubic Laves Phase: Site Preferences, Magnetism, And Electronic Structure, Weiwei Xie, Srinvasa Timmaiah, Jagat Lamal, Jing Liu, Thomas W. Heitmann, Dante Quirinale, A. I. Goldman, Vitalij K. Pecharsky, Gordon J. Miller

Chemistry Publications

The results of crystallographic analysis, magnetic characterization, and theoretical assessment of β-Mn-type Co–Zn intermetallics prepared using high-temperature methods are presented. These β-Mn Co–Zn phases crystallize in the space group P4132 [Pearson symbol cP20; a = 6.3555(7)–6.3220(7)], and their stoichiometry may be expressed as Co8+xZn12–x [1.7(2) < x < 2.2(2)]. According to a combination of single-crystal X-ray diffraction, neutron powder diffraction, and scanning electron microscopy, atomic site occupancies establish clear preferences for Co atoms in the 8c sites and Zn atoms in the 12d sites, with all additional Co atoms replacing some Zn atoms, a result that can be rationalized by electronic structure calculations. Magnetic measurements and neutron powder diffraction of an equimolar Co:Zn sample confirm ferromagnetism in this phase with a Curie temperature of ∼420 K. Neutron powder diffraction and electronic structure calculations using the local spin density approximation indicate that the spontaneous magnetization of this phase arises exclusively from local moments at the Co atoms. Inspection of the atomic arrangements of Co8+xZn12–x reveals that the β-Mn aristotype may be derived from an ordered defect, cubic Laves phase (MgCu2-type) structure. Structural optimization procedures using the Vienna ab initio simulation package (VASP) and starting ...


High-Precision Tracking With Non-Blinking Quantum Dots Resolves Nanoscale Vertical Displacement, Kyle Marchuk, Yijun Guo, Wei Sun, Javier Vela, Ning Fang Mar 2012

High-Precision Tracking With Non-Blinking Quantum Dots Resolves Nanoscale Vertical Displacement, Kyle Marchuk, Yijun Guo, Wei Sun, Javier Vela, Ning Fang

Chemistry Publications

Novel non-blinking quantum dots (NBQDs) were utilized in three-dimensional super-localization, high-precision tracking applications under an automated scanning-angle total internal reflection fluorescence microscope (SA-TIRFM). NBQDs were randomly attached to stationary microtubules along the radial axis under gliding assay conditions. By automatically scanning through a wide range of incident angles with different evanescent-field layer thicknesses, the fluorescence intensity decay curves were obtained. Fit with theoretical decay functions, the absolute vertical positions were determined with sub-10-nm localization precision. The emission intensity profile of the NBQDs attached to kinesin-propelled microtubules was used to resolve the self-rotation of gliding microtubules within a small vertical distance ...


Destabilization Of Ag Nanoislands On Ag(100) By Adsorbed Sulfur, Mingmin Shen, Selena M. Russell, Da-Jiang Liu, Patricia A. Thiel Jan 2011

Destabilization Of Ag Nanoislands On Ag(100) By Adsorbed Sulfur, Mingmin Shen, Selena M. Russell, Da-Jiang Liu, Patricia A. Thiel

Chemistry Publications

Sulfur accelerates coarsening of Ag nanoislands on Ag(100) at 300 K, and this effect is enhanced with increasing sulfur coverage over a range spanning a few hundredths of a monolayer, to nearly 0.25 monolayers. We propose that acceleration of coarsening in this system is tied to the formation of AgS2 clusters primarily at step edges. These clusters can transport Ag more efficiently than can Ag adatoms (due to a lower diffusion barrier and comparable formation energy). The mobility of isolated sulfur on Ag(100) is very low so that formation of the complex is kinetically limited at ...


Adsorbate-Enhanced Transport Of Metals On Metal Surfaces: Oxygen And Sulfur On Coinage Metals, Patricia A. Thiel, Mingmin Shen, Da-Jiang Liu, James W. Evans Jan 2010

Adsorbate-Enhanced Transport Of Metals On Metal Surfaces: Oxygen And Sulfur On Coinage Metals, Patricia A. Thiel, Mingmin Shen, Da-Jiang Liu, James W. Evans

Chemistry Publications

Coarsening (i.e., ripening) of single-atom-high, metal homoepitaxial islands provides a useful window on the mechanism and kinetics of mass transport at metal surfaces. This article focuses on this type of coarsening on the surfaces of coinage metals (Cu, Ag, Au), both clean and with an adsorbed chalcogen (O, S) present. For the clean surfaces, three aspects are summarized: (1) the balance between the two major mechanisms—Ostwald ripening (the most commonly anticipated mechanism) and Smoluchowski ripening—and how that balance depends on island size; (2) the nature of the mass transport agents, which are metal adatoms in almost all ...


Islands And Holes As Measures Of Mass Balance In Growth Of The (√3×√3)R30° Phase Of Ag On Si(111), Alex Belianinov, Barış Ünal, Ning Lu, Min Ji, Kai-Ming Ho, Cai-Zhuang Wang, Michael C. Tringides, Patricia A. Thiel Jan 2010

Islands And Holes As Measures Of Mass Balance In Growth Of The (√3×√3)R30° Phase Of Ag On Si(111), Alex Belianinov, Barış Ünal, Ning Lu, Min Ji, Kai-Ming Ho, Cai-Zhuang Wang, Michael C. Tringides, Patricia A. Thiel

Chemistry Publications

It is well known that conversion of Si(111)-(7×7) into the (√3×√3)R30° phase of adsorbed Ag requires a change in the Si density, and causes formation of islands and holes at the surface. By mass balance, the ratio of areas of islands and holes (RIH) should be approximately 1. However, we find that the ratio is significantly higher, depending on preparation conditions. A possible explanation would be that there are different types of (√3×√3)R30° structures. However, neither scanning tunneling microscopy nor density-functional theory (implemented as a genetic algorithm search) supports this explanation. We ...


Periodic Step Arrays On The Aperiodic I-Al-Pd-Mn Quasicrystal Surface At High Temperature, Y. Sato, Barış Ünal, Thomas A. Lograsso, Patricia A. Thiel, A. K. Schmid, T. Duden, N. C. Bartelt, K. F. Mccarty Jan 2010

Periodic Step Arrays On The Aperiodic I-Al-Pd-Mn Quasicrystal Surface At High Temperature, Y. Sato, Barış Ünal, Thomas A. Lograsso, Patricia A. Thiel, A. K. Schmid, T. Duden, N. C. Bartelt, K. F. Mccarty

Chemistry Publications

We have observed the configuration and motion of surface steps on the aperiodic icosahedral (i-) Al-Pd-Mn quasicrystal using low-energy electron microscopy and scanning tunneling microscopy. As the quasicrystal is cooled from high temperature, bulk vacancies migrate to the surface causing the surface to be etched. Surprisingly, this etching occurs by two types of steps with different heights moving in different directions with different velocities. The steady-state surface morphology is a uniformly spaced rhomboidal step network. This network requires that the layer stacking near the surface deviates from the bulk quasicrystal stacking.


Rhombohedrally Distorted Γ-Brasses Cr1−Xfexga, Hyujin Ko, Olivier Gourdon, Delphine Gout, Eun-Deok Mun, Srinivasa Thimmaiah, Gordon J. Miller Jan 2010

Rhombohedrally Distorted Γ-Brasses Cr1−Xfexga, Hyujin Ko, Olivier Gourdon, Delphine Gout, Eun-Deok Mun, Srinivasa Thimmaiah, Gordon J. Miller

Chemistry Publications

A series of rhombohedrally distorted γ-brass structures containing a mixture of magnetically active 3d elements, Cr and Fe, Cr1−xFexGa, is investigated crystallographically. These structures consist of chains of trans-face-sharing Ga-centered transition metal icosahedra. Neutron powder diffraction specifically on Cr0.5Fe0.5Ga, which could be prepared as a single phase material, gave lattice constants (11 K) a = 12.5172(2) Å and c = 7.8325(2) Å and a refined composition of Cr0.502(6)Fe0.498Ga = Cr6.523Fe6.477Ga13 and revealed partial ordering ...


Low-Temperature Adsorption Of H2s On Ag(111), Selena M. Russell, Da-Jiang Liu, Maki Kawai, Yousoo Kim, Patricia A. Thiel Jan 2010

Low-Temperature Adsorption Of H2s On Ag(111), Selena M. Russell, Da-Jiang Liu, Maki Kawai, Yousoo Kim, Patricia A. Thiel

Chemistry Publications

H2S forms a rich variety of structures on Ag(111) at low temperature and submonolayer coverage. The molecules decorate step edges, exist as isolated entities on terraces, and aggregate into clusters and islands, under various conditions. One type of island exhibits a (×)R25.3° unit cell. Typically, molecules in the clusters and islands are separated by about 0.4 nm, the same as the S–S separation in crystalline H2S. Density functional theory indicates that hydrogen-bonded clusters contain two types of molecules. One is very similar to an isolated adsorbed H2S molecule, with both ...


Variation Of Growth Morphology With Chemical Composition Of Terraces: Ag On A Twofold Surface Of A Decagonal Al-Cu-Co Quasicrystal, T. Duguet, Barış Ünal, Yong Han, James W. Evans, J. Ledieu, Cynthia J. Jenks, J.-M. Dubois, V. Fournée, Patricia A. Thiel Jan 2010

Variation Of Growth Morphology With Chemical Composition Of Terraces: Ag On A Twofold Surface Of A Decagonal Al-Cu-Co Quasicrystal, T. Duguet, Barış Ünal, Yong Han, James W. Evans, J. Ledieu, Cynthia J. Jenks, J.-M. Dubois, V. Fournée, Patricia A. Thiel

Chemistry Publications

Growth of Ag thin films on the twofold surface of a decagonal Al-Cu-Co quasicrystal is characterized by scanning tunneling microscopy, at different temperatures, and for coverages ranging from submonolayer to 11 monolayers. From prior work, three types of clean surface terraces are known to exist. By correlation with a bulk structural model, the major difference between them lies in their transition-metal (TM) content, two being aluminum-rich (0 and 15 at. % TM) and one being TM-rich (40–50 at. % TM). The present article focuses on understanding the difference between Ag film morphologies on these terminations, in terms of their chemical content ...


Formation And Coarsening Of Ag(110) Bilayer Islands On Nial(110): Stm Analysis And Atomistic Lattice-Gas Modeling, Yong Han, Barış Ünal, Dapeng Jing, Feili Qin, Cynthia J. Jenks, Da-Jiang Liu, Patricia A. Thiel, James W. Evans Jan 2010

Formation And Coarsening Of Ag(110) Bilayer Islands On Nial(110): Stm Analysis And Atomistic Lattice-Gas Modeling, Yong Han, Barış Ünal, Dapeng Jing, Feili Qin, Cynthia J. Jenks, Da-Jiang Liu, Patricia A. Thiel, James W. Evans

Chemistry Publications

Scanning tunneling microscopy analysis of the initial stages of film growth during deposition of Ag on NiAl(110) reveals facile formation of bilayer Ag(110) islands at temperatures of 130 K and above. Annealing subsequent to deposition at 130 K induces coarsening of the bilayer island distribution. The thermodynamic driving force for bilayer island formation reflects a lower relative surface energy for films of even layer thicknesses. This feature derives from quantum size effects due to electron confinement in the Ag film. The kinetics of island formation and relaxation is controlled by terrace and edge-diffusion barriers, detachment barriers, interlayer diffusion ...


Lattice Expansion In Islands Stabilized By Electron Confinement: Ag On Si(111)-7×7, Barış Ünal, Alex Belianinov, Patricia A. Thiel, Michael C. Tringides Jan 2010

Lattice Expansion In Islands Stabilized By Electron Confinement: Ag On Si(111)-7×7, Barış Ünal, Alex Belianinov, Patricia A. Thiel, Michael C. Tringides

Chemistry Publications

Ag on Si(111)-7×7 was one of the first systems where height selection of metal islands was attributed to electron confinement, i.e., stabilization of selected heights through a quantum size effect (QSE). However, it has been puzzling how the requisite electron standing waves can form, because the Fermi level EF (along the growth [111] direction) is within the gap for bulk Ag. With detailed experiments over a wide coverage and temperature range, we show that a large increase of 12% is present in the interlayer spacing within the bilayer islands. This can shift EF below ...


Nanoscale “Quantum” Islands On Metal Substrates: Microscopy Studies And Electronic Structure Analyses, Yong Han, Barış Ünal, Dapeng Jing, Patricia A. Thiel, James W. Evans Jan 2010

Nanoscale “Quantum” Islands On Metal Substrates: Microscopy Studies And Electronic Structure Analyses, Yong Han, Barış Ünal, Dapeng Jing, Patricia A. Thiel, James W. Evans

Chemistry Publications

Confinement of electrons can occur in metal islands or in continuous films grown heteroepitaxially upon a substrate of a different metal or on a metallic alloy. Associated quantum size effects (QSE) can produce a significant height-dependence of the surface free energy for nanoscale thicknesses of up to 10–20 layers. This may suffice to induce height selection during film growth. Scanning STM analysis has revealed remarkable flat-topped or mesa-like island and film morphologies in various systems. We discuss in detail observations of QSE and associated film growth behavior for Pb/Cu(111), Ag/Fe(100), and Cu/fcc-Fe/Cu(100 ...


Solvation Dynamics In Ionic Fluids: An Extended Debye–Hückel Dielectric Continuum Model, Xueyu Song Jul 2009

Solvation Dynamics In Ionic Fluids: An Extended Debye–Hückel Dielectric Continuum Model, Xueyu Song

Chemistry Publications

Motivated by our recent proposition on the possibility of using dielectric continuum models to interpret experimental measurements of solvation dynamics in room temperature ionic liquids [J. Phys. Chem. A110, 8623 (2006)], some detailed simulation studies are performed to test the validity of our proposition. From these simulation studies, it seems to be justified that an extended Debye–Hückel continuum model can be used to understand the solvation dynamics of ionic fluids. The theoretical underpinning of such an extended Debye–Hückel model is presented from the general dispersion relation in electrodynamics. The connection with the static extension from the dressed ion ...


Twofold Surface Of The Decagonal Al-Cu-Co Quasicrystal, T. Duguet, Barış Ünal, M. C. De Weerd, J. Ledieu, R. A. Ribeiro, Paul C. Canfield, S. Deloudi, W. Steurer, Cynthia J. Jenks, J.-M. Dubois, V. Fournée, Patricia A. Thiel Jan 2009

Twofold Surface Of The Decagonal Al-Cu-Co Quasicrystal, T. Duguet, Barış Ünal, M. C. De Weerd, J. Ledieu, R. A. Ribeiro, Paul C. Canfield, S. Deloudi, W. Steurer, Cynthia J. Jenks, J.-M. Dubois, V. Fournée, Patricia A. Thiel

Chemistry Publications

We have investigated the atomic structure of the twofold surface of the decagonal Al-Cu-Co quasicrystal using scanning tunneling microscopy and low-energy electron diffraction. We have found that most of the surface features can be interpreted using the bulk-structure model proposed by Deloudi and Steurer (S. Deloudi, Ph.D. thesis, ETH, Zürich, 2008). The surface consists of terraces separated by steps of various heights. Step heights and steps sequences match with the thickness and the stacking sequence of blocks of layers separated by gaps in the model. These blocks of layers define possible surface terminations consisting of periodic atomic rows which ...


Variation Of The Magnetic Ordering In Gdt2zn20 (T=Fe, Ru, Os, Co, Rh And Ir) And Its Correlation With The Electronic Structure Of Isostructural Yt2zn20, Shuang Jia, Ni Ni, G. D. Samolyuk, A. Safa-Sefat, K. Dennis, Hyunjin Ko, Gordon J. Miller, Sergey L. Bud'ko, Paul C. Canfield Jan 2008

Variation Of The Magnetic Ordering In Gdt2zn20 (T=Fe, Ru, Os, Co, Rh And Ir) And Its Correlation With The Electronic Structure Of Isostructural Yt2zn20, Shuang Jia, Ni Ni, G. D. Samolyuk, A. Safa-Sefat, K. Dennis, Hyunjin Ko, Gordon J. Miller, Sergey L. Bud'ko, Paul C. Canfield

Chemistry Publications

Magnetization, resistivity, and specific heat measurements were performed on solution-grown single crystals of six GdT2Zn20 (T=Fe, Ru, Os, Co, Rh, and Ir) compounds, as well as on their Y analogs. For the Gd compounds, the Fe column members manifest a ferromagnetic (FM) ground state (with an enhanced Curie temperature TC for T=Fe and Ru), whereas the Co column members manifest an antiferromagnetic (AFM) ground state. Thermodynamic measurements on YT2Zn20 revealed that the enhanced TC for GdFe2Zn20 and GdRu2Zn20 can be understood within the framework of Heisenberg moments embedded in a nearly ferromagnetic Fermi liquid. Furthermore, electronic structure calculations ...


Tribological Properties Of Quasicrystals: Effect Of Aperiodic Versus Periodic Surface Order, Jeong Young Park, D. F. Ogletree, M. Salmeron, R. A. Ribeiro, Paul C. Canfield, Cynthia J. Jenks, Patricia A. Thiel Jan 2006

Tribological Properties Of Quasicrystals: Effect Of Aperiodic Versus Periodic Surface Order, Jeong Young Park, D. F. Ogletree, M. Salmeron, R. A. Ribeiro, Paul C. Canfield, Cynthia J. Jenks, Patricia A. Thiel

Chemistry Publications

We investigated the nanoscale tribological properties of a decagonal quasicrystal using a combination of atomic force microscopy and scanning tunneling microscopy in ultrahigh vacuum. This combination permitted a variety of in situ measurements, including atomic-scale structure, friction and adhesion force, tip-sample current, and topography. We found that thiol-passivated tips can be used for reproducible studies of the tip-quasicrystal contact while nonpassivated probes adhere irreversibly to the clean quasicrystalline surface causing permanent modifications. The most remarkable results were obtained on the twofold surface of the Al-Ni-Co decagonal quasicrystal where atoms are arranged periodically along the tenfold axis and aperiodically in the ...