Electric-field control of conductance in metal quantum point contacts by electric-double-layer gating

NASA Astrophysics Data System (ADS)

Shibata, K.; Yoshida, K.; Daiguji, K.; Sato, H.; , T., Ii; Hirakawa, K.

2017-10-01

An electric-field control of quantized conductance in metal (gold) quantum point contacts (QPCs) is demonstrated by adopting a liquid-gated electric-double-layer (EDL) transistor geometry. Atomic-scale gold QPCs were fabricated by applying the feedback-controlled electrical break junction method to the gold nanojunction. The electric conductance in gold QPCs shows quantized conductance plateaus and step-wise increase/decrease by the conductance quantum, G0 = 2e2/h, as EDL-gate voltage is swept, demonstrating a modulation of the conductance of gold QPCs by EDL gating. The electric-field control of conductance in metal QPCs may open a way for their application to local charge sensing at room temperature.

Insulator-protected mechanically controlled break junctions for measuring single-molecule conductance in aqueous environments

DOE Office of Scientific and Technical Information (OSTI.GOV)

Muthusubramanian, N.; Zant, H. S. J. van der; Galan, E.

We present a method to fabricate insulated gold mechanically controlled break junctions (MCBJ) by coating the metal with a thin layer of aluminum oxide using plasma enhanced atomic layer deposition. The Al{sub 2}O{sub 3} thickness deposited on the MCBJ devices was varied from 2 to 15 nm to test the suppression of leakage currents in deionized water and phosphate buffered saline. Junctions coated with a 15 nm thick oxide layer yielded atomically sharp electrodes and negligible conductance counts in the range of 1 to 10{sup −4} G{sub 0} (1 G{sub 0} = 77 μS), where single-molecule conductances are commonly observed. The insulated devices were usedmore » to measure the conductance of an amphiphilic oligophenylene ethynylene derivative in deionized water.« less

Thermo-voltage measurements of atomic contacts at low temperature

PubMed Central

Ofarim, Ayelet; Kopp, Bastian; Möller, Thomas; Martin, León; Boneberg, Johannes; Leiderer, Paul

2016-01-01

Summary We report the development of a novel method to determine the thermopower of atomic-sized gold contacts at low temperature. For these measurements a mechanically controllable break junction (MCBJ) system is used and a laser source generates a temperature difference of a few kelvins across the junction to create a thermo-voltage. Since the temperature difference enters directly into the Seebeck coefficient S = −ΔV/ΔT, the determination of the temperature plays an important role. We present a method for the determination of the temperature difference using a combination of a finite element simulation, which reveals the temperature distribution of the sample, and the measurement of the resistance change due to laser heating of sensor leads on both sides next to the junction. Our results for the measured thermopower are in agreement with recent reports in the literature. PMID:27335765

Force and Conductance Spectroscopy of Single Molecule Junctions

NASA Astrophysics Data System (ADS)

Frei, Michael

Investigation of mechanical properties of single molecule junctions is crucial to develop an understanding and enable control of single molecular junctions. This work presents an experimental and analytical approach that enables the statistical evaluation of force and simultaneous conductance data of metallic atomic point contacts and molecular junctions. A conductive atomic force microscope based break junction technique is developed to form single molecular junctions and collect conductance and force data simultaneously. Improvements of the optical components have been achieved through the use of a super-luminescent diode, enabling tremendous increases in force resolution. An experimental procedure to collect data for various molecular junctions has been developed and includes deposition, calibration, and analysis methods. For the statistical analysis of force, novel approaches based on two dimensional histograms and a direct force identification method are presented. The two dimensional method allows for an unbiased evaluation of force events that are identified using corresponding conductance signatures. This is not always possible however, and in these situations, the force based identification of junction rearrangement events is an attractive alternative method. This combined experimental and analytical approach is then applied to three studies: First, the impact of molecular backbones to the mechanical behavior of single molecule junctions is investigated and it is found that junctions formed with identical linkers but different backbone structure result in junctions with varying breaking forces. All molecules used show a clear molecular signature and force data can be evaluated using the 2D method. Second, the effects of the linker group used to attach molecules to gold electrodes are investigated. A study of four alkane molecules with different linkers finds a drastic difference in the evolution of donor-acceptor and covalently bonded molecules respectively. In fact, the covalent bond is found to significantly distort the metal electrode rearrangement such that junction rearrangement events can no longer be identified with a clean and well defined conductance signature. For this case, the force based identification process is used. Third, results for break junction measurements with different metals are presented. It is found that silver and palladium junctions rupture with forces different from those of gold contacts. In the case of silver experiments in ambient conditions, we can also identify oxygen impurities in the silver contact formation process, leading to force and conductance measurements of silver-oxygen structures. For the future, this work provides an experimental and analytical foundation that will enable insights into single molecule systems not previously accessible.

Role of solvent environments in single molecule conductance used insulator-modified mechanically controlled break junctions

NASA Astrophysics Data System (ADS)

Muthusubramanian, Nandini; Maity, Chandan; Galan Garcia, Elena; Eelkema, Rienk; Grozema, Ferdinand; van der Zant, Herre; Kavli Institute of Nanoscience Collaboration; Department of Chemical Engineering Collaboration

We present a method for studying the effects of polar solvents on charge transport through organic/biological single molecules by developing solvent-compatible mechanically controlled break junctions of gold coated with a thin layer of aluminium oxide using plasma enhanced atomic layer deposition (ALD). The optimal oxide thickness was experimentally determined to be 15 nm deposited at ALD operating temperature of 300°C which yielded atomically sharp electrodes and reproducible single-barrier tunnelling behaviour across a wide conductance range between 1 G0 and 10-7 G0. The insulator protected MCBJ devices were found to be effective in various solvents such as deionized water, phosphate buffered saline, methanol, acetonitrile and dichlorobenzene. The yield of molecular junctions using such insulated electrodes was tested by developing a chemical protocol for synthesizing an amphipathic form of oligo-phenylene ethynylene (OPE3-PEO) with thioacetate anchoring groups. This work has further applications in studying effects of solvation, dipole orientation and other thermodynamic interactions on charge transport. Eu Marie Curie Initial Training Network (ITN). MOLECULAR-SCALE ELECTRONICS: ``MOLESCO'' Project Number 606728.

Epitaxial insertion of gold silicide nanodisks during the growth of silicon nanowires.

PubMed

Um, Han-Don; Jee, Sang-Won; Park, Kwang-Tae; Jung, Jin-Young; Guo, Zhongyi; Lee, Jung-Ho

2011-07-01

Nanodisk-shaped, single-crystal gold silicide heterojunctions were inserted into silicon nanowires during vapor-liquid-solid growth using Au as a catalyst within a specific range of chlorine-to-hydrogen atomic ratio. The mechanism of nanodisk formation has been investigated by changing the source gas ratio of SiCl4 to H2. We report that an over-supply of silicon into the Au-Si liquid alloy leads to highly supersaturated solution and enhances the precipitation of Au in the silicon nanowires due to the formation of unstable phases within the liquid alloy. It is shown that the gold precipitates embedded in the silicon nanowires consisted of a metastable gold silicide. Interestingly, faceting of gold silicide was observed at the Au/Si interfaces, and silicon nanowires were epitaxially grown on the top of the nanodisk by vapor-liquid-solid growth. High resolution transmission electron microscopy confirmed that gold silicide nanodisks are epitaxially connected to the silicon nanowires in the direction of growth direction. These gold silicide nanodisks would be useful as nanosized electrical junctions for future applications in nanowire interconnections.

Metal-assisted exfoliation (MAE): green process for transferring graphene to flexible substrates and templating of sub-nanometer plasmonic gaps (Presentation Recording)

NASA Astrophysics Data System (ADS)

Zaretski, Aliaksandr V.; Marin, Brandon C.; Moetazedi, Herad; Dill, Tyler J.; Jibril, Liban; Kong, Casey; Tao, Andrea R.; Lipomi, Darren J.

2015-09-01

This paper describes a new technique, termed "metal-assisted exfoliation," for the scalable transfer of graphene from catalytic copper foils to flexible polymeric supports. The process is amenable to roll-to-roll manufacturing, and the copper substrate can be recycled. We then demonstrate the use of single-layer graphene as a template for the formation of sub-nanometer plasmonic gaps using a scalable fabrication process called "nanoskiving." These gaps are formed between parallel gold nanowires in a process that first produces three-layer thin films with the architecture gold/single-layer graphene/gold, and then sections the composite films with an ultramicrotome. The structures produced can be treated as two gold nanowires separated along their entire lengths by an atomically thin graphene nanoribbon. Oxygen plasma etches the sandwiched graphene to a finite depth; this action produces a sub-nanometer gap near the top surface of the junction between the wires that is capable of supporting highly confined optical fields. The confinement of light is confirmed by surface-enhanced Raman spectroscopy measurements, which indicate that the enhancement of the electric field arises from the junction between the gold nanowires. These experiments demonstrate nanoskiving as a unique and easy-to-implement fabrication technique that is capable of forming sub-nanometer plasmonic gaps between parallel metallic nanostructures over long, macroscopic distances. These structures could be valuable for fundamental investigations as well as applications in plasmonics and molecular electronics.

Peltier cooling in molecular junctions

NASA Astrophysics Data System (ADS)

Cui, Longji; Miao, Ruijiao; Wang, Kun; Thompson, Dakotah; Zotti, Linda Angela; Cuevas, Juan Carlos; Meyhofer, Edgar; Reddy, Pramod

2018-02-01

The study of thermoelectricity in molecular junctions is of fundamental interest for the development of various technologies including cooling (refrigeration) and heat-to-electricity conversion1-4. Recent experimental progress in probing the thermopower (Seebeck effect) of molecular junctions5-9 has enabled studies of the relationship between thermoelectricity and molecular structure10,11. However, observations of Peltier cooling in molecular junctions—a critical step for establishing molecular-based refrigeration—have remained inaccessible. Here, we report direct experimental observations of Peltier cooling in molecular junctions. By integrating conducting-probe atomic force microscopy12,13 with custom-fabricated picowatt-resolution calorimetric microdevices, we created an experimental platform that enables the unified characterization of electrical, thermoelectric and energy dissipation characteristics of molecular junctions. Using this platform, we studied gold junctions with prototypical molecules (Au-biphenyl-4,4'-dithiol-Au, Au-terphenyl-4,4''-dithiol-Au and Au-4,4'-bipyridine-Au) and revealed the relationship between heating or cooling and charge transmission characteristics. Our experimental conclusions are supported by self-energy-corrected density functional theory calculations. We expect these advances to stimulate studies of both thermal and thermoelectric transport in molecular junctions where the possibility of extraordinarily efficient energy conversion has been theoretically predicted2-4,14.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cheng, Jue-Fei; School of Electronics and Information Engineering, Suzhou Vocational University, Suzhou 215104; Zhou, Liping, E-mail: zhoulp@suda.edu.cn, E-mail: leigao@suda.edu.cn

The electronic transport properties of benzene–porphyrin–benzene (BPB) molecules coupled to gold (Au) electrodes were investigated. By successively removing the front-end Au atoms, several BPB junctions with different molecule-electrode contact symmetries were constructed. The calculated current–voltage (I–V) curves depended strongly on the contact configurations between the BPB molecules and the Au electrodes. In particular, a significant low-voltage negative differential resistance effect appeared at −0.3 V in the junctions with pyramidal electrodes on both sides. Along with the breaking of this tip-contact symmetry, the low-bias negative differential resistance effect gradually disappeared. This tip-contact may be ideal for use in the design ofmore » future molecular devices because of its similarity with experimental processes.« less

Surface effects on the mechanical elongation of AuCu nanowires: De-alloying and the formation of mixed suspended atomic chains

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lagos, M. J.; Laboratório Nacional de Nanotecnologia-LNNANO, 13083-970 Campinas-SP; Autreto, P. A. S.

2015-03-07

We report here an atomistic study of the mechanical deformation of Au{sub x}Cu{sub (1−x)} atomic-size wires (nanowires (NWs)) by means of high resolution transmission electron microscopy experiments. Molecular dynamics simulations were also carried out in order to obtain deeper insights on the dynamical properties of stretched NWs. The mechanical properties are significantly dependent on the chemical composition that evolves in time at the junction; some structures exhibit a remarkable de-alloying behavior. Also, our results represent the first experimental realization of mixed linear atomic chains (LACs) among transition and noble metals; in particular, surface energies induce chemical gradients on NW surfacesmore » that can be exploited to control the relative LAC compositions (different number of gold and copper atoms). The implications of these results for nanocatalysis and spin transport of one-atom-thick metal wires are addressed.« less

Pulse-voltammetric glucose detection at gold junction electrodes.

PubMed

Rassaei, Liza; Marken, Frank

2010-09-01

A novel glucose sensing concept based on the localized change or "modulation" in pH within a symmetric gold-gold junction electrode is proposed. A paired gold-gold junction electrode (average gap size ca. 500 nm) is prepared by simultaneous bipotentiostatic electrodeposition of gold onto two closely spaced platinum disk electrodes. For glucose detection in neutral aqueous solution, the potential of the "pH-modulator" electrode is set to -1.5 V vs saturated calomel reference electrode (SCE) to locally increase the pH, and simultaneously, either cyclic voltammetry or square wave voltammetry experiments are conducted at the sensor electrode. A considerable improvement in the sensor electrode response is observed when a normal pulse voltammetry sequence is applied to the modulator electrode (to generate "hydroxide pulses") and the glucose sensor electrode is operated with fixed bias at +0.5 V vs SCE (to eliminate capacitive charging currents). Preliminary data suggest good linearity for the glucose response in the medically relevant 1-10 mM concentration range (corresponding to 0.18-1.8 g L(-1)). Future electroanalytical applications of multidimensional pulse voltammetry in junction electrodes are discussed.

PREFACE: Nanoelectronics, sensors and single molecule biophysics Nanoelectronics, sensors and single molecule biophysics

NASA Astrophysics Data System (ADS)

Tao, Nongjian

2012-04-01

This special section of Journal of Physics: Condensed Matter (JPCM) is dedicated to Professor Stuart M Lindsay on the occasion of his 60th birthday and in recognition of his outstanding contributions to multiple research areas, including light scattering spectroscopy, scanning probe microscopy, biophysics, solid-liquid interfaces and molecular and nanoelectronics. It contains a collection of 14 papers in some of these areas, including a feature article by Lindsay. Each paper was subject to the normal rigorous review process of JPCM. In Lindsay's paper, he discusses the next generations of hybrid chemical-CMOS devices for low cost and personalized medical diagnosis. The discussion leads to several papers on nanotechnology for biomedical applications. Kawaguchi et al report on the detection of single pollen allergen particles using electrode embedded microchannels. Stern et al describe a structural study of three-dimensional DNA-nanoparticle assemblies. Hihath et al measure the conductance of methylated DNA, and discuss the possibility of electrical detection DNA methylation. Portillo et al study the electrostatic effects on the aggregation of prion proteins and peptides with atomic force microscopy. In an effort to understand the interactions between nanostructures and cells, Lamprecht et al report on the mapping of the intracellular distribution of carbon nanotubes with a confocal Raman imaging technique, and Wang et al focus on the intracellular delivery of gold nanoparticles using fluorescence microscopy. Park and Kristic provide theoretical analysis of micro- and nano-traps and their biological applications. This section also features several papers on the fundamentals of electron transport in single atomic wires and molecular junctions. The papers by Xu et al and by Wandlowksi et al describe new methods to measure conductance and forces in single molecule junctions and metallic atomic wires. Scullion et al report on the conductance of molecules with similar lengths but different energy barrier profiles in order to elucidate electron transport in the molecular junctions. Kiguchi and Murakoshi study metallic atomic wires under electrochemical potential control. Asai reports on a theoretical study of rectification in substituted atomic wires. Finally, Weiss et al report on a new method to pattern and functionalize oxide-free germanium surfaces with self-assembled organic monolayers, which provides interfaces between inorganic semiconductors and organic molecules. Nanoelectronics, sensors and single molecule biophysics contents Biochemistry and semiconductor electronics—the next big hit for silicon?Stuart Lindsay Electrical detection of single pollen allergen particles using electrode-embedded microchannelsChihiro Kawaguchi, Tetsuya Noda, Makusu Tsutsui, Masateru Taniguchi, Satoyuki Kawano and Tomoji Kawai Quasi 3D imaging of DNA-gold nanoparticle tetrahedral structuresAvigail Stern, Dvir Rotem, Inna Popov and Danny Porath Effects of cytosine methylation on DNA charge transportJoshua Hihath, Shaoyin Guo, Peiming Zhang and Nongjian Tao Effect of electrostatics on aggregation of prion protein Sup35 peptideAlexander M Portillo, Alexey V Krasnoslobodtsev and Yuri L Lyubchenko Mapping the intracellular distribution of carbon nanotubes after targeted delivery to carcinoma cells using confocal Raman imaging as a label-free techniqueC Lamprecht, N Gierlinger, E Heister, B Unterauer, B Plochberger, M Brameshuber, P Hinterdorfer, S Hild and A Ebner Caveolae-mediated endocytosis of biocompatible gold nanoparticles in living Hela cellsXian Hao, Jiazhen Wu, Yuping Shan, Mingjun Cai, Xin Shang, Junguang Jiang and Hongda Wang Stability of an aqueous quadrupole micro-trapJae Hyun Park and Predrag S Krstić Electron transport properties of single molecular junctions under mechanical modulationsJianfeng Zhou, Cunlan Guo and Bingqian Xu An approach to measure electromechanical properties of atomic and molecular junctionsIlya V Pobelov, Gábor Mészáros, Koji Yoshida, Artem Mishchenko, Murat Gulcur, Martin R Bryce and Thomas Wandlowski Single-molecule conductance determinations on HS(CH2)4O(CH2)4SH and HS(CH2)2O(CH2)2O(CH2)2SH, and comparison with alkanedithiols of the same lengthLisa E Scullion, Edmund Leary, Simon J Higgins and Richard J Nichols Metal atomic contact under electrochemical potential controlManabu Kiguchi and Kei Murakoshi Rectification in substituted atomic wires: a theoretical insightYoshihiro Asai High-fidelity chemical patterning on oxide-free germaniumJ Nathan Hohman, Moonhee Kim, Jeffrey A Lawrence, Patrick D McClanahan and Paul S Weiss

Inelastic transport theory from first principles: Methodology and application to nanoscale devices

NASA Astrophysics Data System (ADS)

Frederiksen, Thomas; Paulsson, Magnus; Brandbyge, Mads; Jauho, Antti-Pekka

2007-05-01

We describe a first-principles method for calculating electronic structure, vibrational modes and frequencies, electron-phonon couplings, and inelastic electron transport properties of an atomic-scale device bridging two metallic contacts under nonequilibrium conditions. The method extends the density-functional codes SIESTA and TRANSIESTA that use atomic basis sets. The inelastic conductance characteristics are calculated using the nonequilibrium Green’s function formalism, and the electron-phonon interaction is addressed with perturbation theory up to the level of the self-consistent Born approximation. While these calculations often are computationally demanding, we show how they can be approximated by a simple and efficient lowest order expansion. Our method also addresses effects of energy dissipation and local heating of the junction via detailed calculations of the power flow. We demonstrate the developed procedures by considering inelastic transport through atomic gold wires of various lengths, thereby extending the results presented in Frederiksen [Phys. Rev. Lett. 93, 256601 (2004)]. To illustrate that the method applies more generally to molecular devices, we also calculate the inelastic current through different hydrocarbon molecules between gold electrodes. Both for the wires and the molecules our theory is in quantitative agreement with experiments, and characterizes the system-specific mode selectivity and local heating.

Tuning a circular p-n junction in graphene from quantum confinement to optical guiding

NASA Astrophysics Data System (ADS)

Jiang, Yuhang; Mao, Jinhai; Moldovan, Dean; Masir, Massoud Ramezani; Li, Guohong; Watanabe, Kenji; Taniguchi, Takashi; Peeters, Francois M.; Andrei, Eva Y.

2017-11-01

The photon-like propagation of the Dirac electrons in graphene, together with its record-high electronic mobility, can lead to applications based on ultrafast electronic response and low dissipation. However, the chiral nature of the charge carriers that is responsible for the high mobility also makes it difficult to control their motion and prevents electronic switching. Here, we show how to manipulate the charge carriers by using a circular p-n junction whose size can be continuously tuned from the nanometre to the micrometre scale. The junction size is controlled with a dual-gate device consisting of a planar back gate and a point-like top gate made by decorating a scanning tunnelling microscope tip with a gold nanowire. The nanometre-scale junction is defined by a deep potential well created by the tip-induced charge. It traps the Dirac electrons in quantum-confined states, which are the graphene equivalent of the atomic collapse states (ACSs) predicted to occur at supercritically charged nuclei. As the junction size increases, the transition to the optical regime is signalled by the emergence of whispering-gallery modes, similar to those observed at the perimeter of acoustic or optical resonators, and by the appearance of a Fabry-Pérot interference pattern for junctions close to a boundary.

A DFT study on surface-enhanced Raman spectroscopy of aromatic dithiol derivatives adsorbed on gold nanojunctions

NASA Astrophysics Data System (ADS)

You, Tingting; Lang, Xiufeng; Huang, Anping; Yin, Penggang

2018-01-01

A computational study on aromatic dithiol derivatives (HS-Ar-X-Ar-SH, X = O, S, Se, NH, CH2, Ndbnd N, CHdbnd CH, Ctbnd C) interacting with gold cluster(s) was presented to investigate the chemical enhancement mechanism related to surface-enhanced Raman spectroscopy (SERS) for molecular junctions. Density functional theory (DFT) were performed on derivatives molecules as well as their single-end-linked (SEL) or double-end-linked (DEL) complexes for geometric, spectra, electronic and excitation properties, leading to discussions on dominant factor during SERS process. The resulted enhancement factors of SEL and DEL complexes exhibited specific dependency on linking atom or functional group between two phenyls, which was in accordance with the variation of polarizabilities and molecule-cluster transition energy.

Single-molecule conductance through multiple π-π-stacked benzene rings determined with direct electrode-to-benzene ring connections.

PubMed

Schneebeli, Severin T; Kamenetska, Maria; Cheng, Zhanling; Skouta, Rachid; Friesner, Richard A; Venkataraman, Latha; Breslow, Ronald

2011-02-23

Understanding electron transport across π-π-stacked systems will help to answer fundamental questions about biochemical redox processes and benefit the design of new materials and molecular devices. Herein we employed the STM break-junction technique to measure the single-molecule conductance of multiple π-π-stacked aromatic rings. We studied electron transport through up to four stacked benzene rings held together in an eclipsed fashion via a paracyclophane scaffold. We found that the strained hydrocarbons studied herein couple directly to gold electrodes during the measurements; hence, we did not require any heteroatom binding groups as electrical contacts. Density functional theory-based calculations suggest that the gold atoms of the electrodes bind to two neighboring carbon atoms of the outermost cyclophane benzene rings in η(2) fashion. Our measurements show an exponential decay of the conductance with an increasing number of stacked benzene rings, indicating a nonresonant tunneling mechanism. Furthermore, STM tip-substrate displacement data provide additional evidence that the electrodes bind to the outermost benzene rings of the π-π-stacked molecular wires.

The enhanced spin-polarized transport behaviors through cobalt benzene-porphyrin-benzene molecular junctions: the effect of functional groups

NASA Astrophysics Data System (ADS)

Cheng, Jue-Fei; Zhou, Liping; Wen, Zhongqian; Yan, Qiang; Han, Qin; Gao, Lei

2017-05-01

The modification effects of the groups amino (NH2) and nitro (NO2) on the spin polarized transport properties of the cobalt benzene-porphyrin-benzene (Co-BPB) molecule coupled to gold (Au) nanowire electrodes are investigated by the nonequilibrium Green’s function method combined with the density functional theory. The calculation results show that functional groups can lead to the significant spin-filter effect, enhanced low-bias negative differential resistance (NDR) behavior and novel reverse rectifying effect in Co-BPB molecular junction. The locations and types of functional groups have distinct influences on spin-polarized transport performances. The configuration with NH2 group substituting H atom in central porphyrin ring has larger spin-down current compared to that with NO2 substitution. And Co-BPB molecule junction with NH2 group substituting H atom in side benzene ring shows reverse rectifying effect. Detailed analyses confirm that NH2 and NO2 group substitution change the spin-polarized transferred charge, which makes the highest occupied molecular orbitals (HOMO) of spin-down channel of Co-BPB closer to the Fermi level. And the shift of HOMO strengthens the spin-polarized coupling between the molecular orbitals and the electrodes, leading to the enhanced spin-polarized behavior. Our findings might be useful in the design of multi-functional molecular devices in the future.

Understanding the Conductance of Single-Molecule Junctions from First Principles

NASA Astrophysics Data System (ADS)

Quek, Su Ying

2008-03-01

Discovering the anatomy of single-molecule junctions, in order to exploit their transport behavior, poses fundamental challenges to nanoscience. First-principles calculations based on density-functional theory (DFT) can, together with experiment, provide detailed atomic-scale insights into the transport properties, and their relation to junction structure and electronic properties. Here, a DFT scattering state approach [1] is used to explore the single-molecule conductance of two prototypical junctions as a function of junction geometry, in the context of recent experiments. First, the computed conductance of 15 distinct benzene-diamine-Au junctions is compared to a large robust experimental data set [2]. The amine-gold bonding is shown to be highly selective, but flexible, resulting in a conductance that is insensitive to other details of the junction structure. The range of computed conductance corresponds well to the narrow distribution in experiment, although the average calculated conductance is approximately 7 times larger. This discrepancy is attributed to the absence of many-electron corrections in the DFT molecular orbital energies; a simple physically-motivated estimate for the self-energy corrections results in a conductance that is much closer to experiment [3]. Second, similar first-principles techniques are applied to a range of bipyridine-Au junctions. The extent to which Au-pyridine link bonding is affected by the constraints of forming bipyridine-Au junctions is investigated. In some contrast to the amine case, the computed conductance shows a strong sensitivity to the tilt of the bipyridine rings relative to the Au surfaces. Experiments probing the conductance of bipyridine-Au junctions are discussed in the context of these findings. [1] H. J. Choi et al, Phys Rev B, 76, 155420 (2007) [2] L. Venkataraman et al, Nano Lett 6, 458 (2006) [3] S. Y. Quek et al, Nano Lett. 7, 3477 (2007)

Interplay of Bias-Driven Charging and the Vibrational Stark Effect in Molecular Junctions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Li, Yajing; Zolotavin, Pavlo; Doak, Peter

We observe large, reversible, bias driven changes in the vibrational energies of PCBM based on simultaneous transport and surface-enhanced Raman spectroscopy (SERS) measurements on PCBM-gold junctions. A combination of linear and quadratic shifts in vibrational energies with voltage is analyzed and compared with similar measurements involving C-60-gold junctions. A theoretical model based on density functional theory (DFT) calculations suggests that both a vibrational Stark effect and bias-induced charging of the junction contribute to the shifts in vibrational energies. In the PCBM case, a linear vibrational Stark effect is observed due to the permanent electric dipole moment of PCBM. The vibrationalmore » Stark shifts shown here for PCBM junctions are comparable to or larger than the charging effects that dominate in C-60 junctions.« less

Interplay of Bias-Driven Charging and the Vibrational Stark Effect in Molecular Junctions

DOE PAGES

Li, Yajing; Zolotavin, Pavlo; Doak, Peter; ...

2016-01-27

We observe large, reversible, bias driven changes in the vibrational energies of PCBM based on simultaneous transport and surface-enhanced Raman spectroscopy (SERS) measurements on PCBM-gold junctions. A combination of linear and quadratic shifts in vibrational energies with voltage is analyzed and compared with similar measurements involving C-60-gold junctions. A theoretical model based on density functional theory (DFT) calculations suggests that both a vibrational Stark effect and bias-induced charging of the junction contribute to the shifts in vibrational energies. In the PCBM case, a linear vibrational Stark effect is observed due to the permanent electric dipole moment of PCBM. The vibrationalmore » Stark shifts shown here for PCBM junctions are comparable to or larger than the charging effects that dominate in C-60 junctions.« less

Determination of gold in geologic materials by solvent extraction and atomic-absorption spectrometry

USGS Publications Warehouse

Huffman, Claude; Mensik, J.D.; Riley, L.B.

1967-01-01

The two methods presented for the determination of traces of gold in geologic materials are the cyanide atomic-absorption method and the fire-assay atomic-absorption method. In the cyanide method gold is leached with a sodium-cyanide solution. The monovalent gold is then oxidized to the trivalent state and concentrated by extracting into methyl isobutyl ketone prior to estimation by atomic absorption. In the fire-assay atomic-absorption method, the gold-silver bead obtained from fire assay is dissolved in nitric and hydrochloric acids. Gold is then concentrated by extracting into methyl isobutyl ketone prior to determination by atomic absorption. By either method concentrations as low as 50 parts per billion of gold can be determined in a 15-gram sample.

Ultralow-Power Electronic Trapping of Nanoparticles with Sub-10 nm Gold Nanogap Electrodes.

PubMed

Barik, Avijit; Chen, Xiaoshu; Oh, Sang-Hyun

2016-10-12

We demonstrate nanogap electrodes for rapid, parallel, and ultralow-power trapping of nanoparticles. Our device pushes the limit of dielectrophoresis by shrinking the separation between gold electrodes to sub-10 nm, thereby creating strong trapping forces at biases as low as the 100 mV ranges. Using high-throughput atomic layer lithography, we manufacture sub-10 nm gaps between 0.8 mm long gold electrodes and pattern them into individually addressable parallel electronic traps. Unlike pointlike junctions made by electron-beam lithography or larger micron-gap electrodes that are used for conventional dielectrophoresis, our sub-10 nm gold nanogap electrodes provide strong trapping forces over a mm-scale trapping zone. Importantly, our technology solves the key challenges associated with traditional dielectrophoresis experiments, such as high voltages that cause heat generation, bubble formation, and unwanted electrochemical reactions. The strongly enhanced fields around the nanogap induce particle-transport speed exceeding 10 μm/s and enable the trapping of 30 nm polystyrene nanoparticles using an ultralow bias of 200 mV. We also demonstrate rapid electronic trapping of quantum dots and nanodiamond particles on arrays of parallel traps. Our sub-10 nm gold nanogap electrodes can be combined with plasmonic sensors or nanophotonic circuitry, and their low-power electronic operation can potentially enable high-density integration on a chip as well as portable biosensing.

Atomically thin p-n junctions with van der Waals heterointerfaces.

PubMed

Lee, Chul-Ho; Lee, Gwan-Hyoung; van der Zande, Arend M; Chen, Wenchao; Li, Yilei; Han, Minyong; Cui, Xu; Arefe, Ghidewon; Nuckolls, Colin; Heinz, Tony F; Guo, Jing; Hone, James; Kim, Philip

2014-09-01

Semiconductor p-n junctions are essential building blocks for electronic and optoelectronic devices. In conventional p-n junctions, regions depleted of free charge carriers form on either side of the junction, generating built-in potentials associated with uncompensated dopant atoms. Carrier transport across the junction occurs by diffusion and drift processes influenced by the spatial extent of this depletion region. With the advent of atomically thin van der Waals materials and their heterostructures, it is now possible to realize a p-n junction at the ultimate thickness limit. Van der Waals junctions composed of p- and n-type semiconductors--each just one unit cell thick--are predicted to exhibit completely different charge transport characteristics than bulk heterojunctions. Here, we report the characterization of the electronic and optoelectronic properties of atomically thin p-n heterojunctions fabricated using van der Waals assembly of transition-metal dichalcogenides. We observe gate-tunable diode-like current rectification and a photovoltaic response across the p-n interface. We find that the tunnelling-assisted interlayer recombination of the majority carriers is responsible for the tunability of the electronic and optoelectronic processes. Sandwiching an atomic p-n junction between graphene layers enhances the collection of the photoexcited carriers. The atomically scaled van der Waals p-n heterostructures presented here constitute the ultimate functional unit for nanoscale electronic and optoelectronic devices.

Thermionic field emission in gold nitride Schottky nanodiodes

NASA Astrophysics Data System (ADS)

Spyropoulos-Antonakakis, N.; Sarantopoulou, E.; Kollia, Z.; Samardžija, Z.; Kobe, S.; Cefalas, A. C.

2012-11-01

We report on the thermionic field emission and charge transport properties of gold nitride nanodomains grown by pulsed laser deposition with a molecular fluorine laser at 157 nm. The nanodomains are sandwiched between the metallic tip of a conductive atomic force microscope and a thin gold layer forming thus a metal-semiconductor-metal junction. Although the limited existing data in the literature indicate that gold nitride was synthesized previously with low efficiency, poor stability, and metallic character; in this work, it is shown that gold nitride nanodomains exhibit semiconducting behavior and the metal-semiconductor-metal contact can be modeled with the back-to-back Schottky barrier model. From the experimental I-V curves, the main charge carrier transport process is found to be thermionic field emission via electron tunneling. The rectifying, near symmetric and asymmetric current response of nanocontacts is related to the effective contact area of the gold nitride nanodomains with the metals. A lower limit for the majority charge carriers concentration at the boundaries of nanodomains is also established using the full depletion approximation, as nanodomains with thickness as low as 6 nm were found to be conductive. Current rectification and charge memory effects are also observed in "quite small" conductive nanodomains (6-10 nm) due to stored charges. Indeed, charges near the surface are identified as inversion domains in the phase shift mapping performed with electrostatic force microscopy and are attributed to charge trapping at the boundaries of the nanodomains.

OVERVIEW OF GOLD HILL MILL, ROAD, AND WARM SPRINGS CAMP ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

OVERVIEW OF GOLD HILL MILL, ROAD, AND WARM SPRINGS CAMP BUILDINGS, LOOKING SOUTH SOUTHEAST. THE FUNCTION OF THE FLAT AREA AT CENTER RIGHT IS UNKNOWN. - Gold Hill Mill, Warm Spring Canyon Road, Death Valley Junction, Inyo County, CA

Induced Superconductivity and Engineered Josephson Tunneling Devices in Epitaxial (111)-Oriented Gold/Vanadium Heterostructures.

PubMed

Wei, Peng; Katmis, Ferhat; Chang, Cui-Zu; Moodera, Jagadeesh S

2016-04-13

We report a unique experimental approach to create topological superconductors by inducing superconductivity into epitaxial metallic thin film with strong spin-orbit coupling. Utilizing molecular beam epitaxy technique under ultrahigh vacuum conditions, we are able to achieve (111) oriented single phase of gold (Au) thin film grown on a well-oriented vanadium (V) s-wave superconductor film with clean interface. We obtained atomically smooth Au thin films with thicknesses even down to below a nanometer showing near-ideal surface quality. The as-grown V/Au bilayer heterostructure exhibits superconducting transition at around 3.9 K. Clear Josephson tunneling and Andreev reflection are observed in S-I-S tunnel junctions fabricated from the epitaxial bilayers. The barrier thickness dependent tunneling and the associated subharmonic gap structures (SGS) confirmed the induced superconductivity in Au (111), paving the way for engineering thin film heterostructures based on p-wave superconductivity and nano devices exploiting Majorana Fermions for quantum computing.

Construction and performance of a dilution-refrigerator based spectroscopic-imaging scanning tunneling microscope.

PubMed

Singh, U R; Enayat, M; White, S C; Wahl, P

2013-01-01

We report on the set-up and performance of a dilution-refrigerator based spectroscopic imaging scanning tunneling microscope. It operates at temperatures below 10 mK and in magnetic fields up to 14T. The system allows for sample transfer and in situ cleavage. We present first-results demonstrating atomic resolution and the multi-gap structure of the superconducting gap of NbSe(2) at base temperature. To determine the energy resolution of our system we have measured a normal metal/vacuum/superconductor tunneling junction consisting of an aluminum tip on a gold sample. Our system allows for continuous measurements at base temperature on time scales of up to ≈170 h.

Charge transport with single molecules--an electrochemical approach.

PubMed

Li, Chen; Mishchenko, Artem; Pobelov, Ilya; Wandlowski, Thomas

2010-01-01

After an introduction and brief review of charge transport in nanoscale molecular systems we report on experimental studies in gold / (single) molecule / gold junctions at solid / liquid interfaces employing a scanning tunneling microscopy (STM)-based 'break junction' technique. We demonstrate attempts in developing basic relationships between molecular structure, conductance properties and nanoscale electrochemical concepts based on four case studies from our own work. In experiments with alpha, omega-alkanedithiol and biphenyldithiol molecular junctions we address the role of sulfur-gold couplings and molecular conformation, such as gauche defects in the alkyl chains and the torsion angle between two phenyl rings. Combination with quantum chemistry calculations enabled a detailed molecular-level understanding of the electronic structure and transport characteristics of both systems. Employing the concept of 'electrolyte gating' with redox-active molecules, such as thiol-terminated derivatives of viologens (HS-6V6-SH or (HS-6V6)) we demonstrate the construction of symmetric and asymmetric active molecular junctions with transistor- or diode-like behavior upon polarization in an electrochemical environment. The experimental data could be represented quantitatively by the Kutznetsov/Ulstrup model assuming a two-step electron transfer with partial vibration relaxation. Finally, we show that surface-immobilized gold nanoparticles with a diameter of (2.4 +/- 0.5) nm exhibit features of locally addressable multi-state electronic switching upon electrolyte gating, which appears to be reminiscent of a sequential charging through several 'oxidation/reduction states'.

Electronic and transport properties of a molecular junction with asymmetric contacts.

PubMed

Tsai, M-H; Lu, T-H

2010-02-10

Asymmetric molecular junctions have been shown experimentally to exhibit a dual-conductance transport property with a pulse-like current-voltage characteristic, by Reed and co-workers. Using a recently developed first-principles integrated piecewise thermal equilibrium current calculation method and a gold-benzene-1-olate-4-thiolate-gold model molecular junction, this unusual transport property has been reproduced. Analysis of the electrostatics and the electronic structure reveals that the high-current state results from subtle bias induced charge transfer at the electrode-molecule contacts that raises molecular orbital energies and enhances the current-contributing molecular density of states and the probabilities of resonance tunneling of conduction electrons from one electrode to another.

From tunneling to contact: Inelastic signals in an atomic gold junction from first principles

NASA Astrophysics Data System (ADS)

Frederiksen, Thomas; Lorente, Nicolás; Paulsson, Magnus; Brandbyge, Mads

2007-06-01

The evolution of electron conductance in the presence of inelastic effects is studied as an atomic gold contact is formed evolving from a low-conductance regime (tunneling) to a high-conductance regime (contact). In order to characterize each regime, we perform density-functional theory (DFT) calculations to study the geometric and electronic structures, together with the strength of the atomic bonds and the associated vibrational frequencies. The conductance is calculated by, first, evaluating the transmission of electrons through the system and, second, by calculating the conductance change due to the excitation of vibrations. As found in previous studies [Paulsson , Phys. Rev. B 72, 201101(R) (2005)], the change in conductance due to inelastic effects permits us to characterize the crossover from tunneling to contact. The most notorious effect is the crossover from an increase in conductance in the tunneling regime to a decrease in conductance in the contact regime when the bias voltage matches a vibrational threshold. Our DFT-based calculations actually show that the effect of vibrational modes in electron conductance is rather complex, in particular, when modes localized in the contact region are permitted to extend into the electrodes. As an example, we find that certain modes can give rise to decreases in conductance when in the tunneling regime, opposite to the above-mentioned result. Whereas details in the inelastic spectrum depend on the size of the vibrational region, we show that the overall change in conductance is quantitatively well approximated by the simplest calculation where only the apex atoms are allowed to vibrate. Our study is completed by the application of a simplified model where the relevant parameters are obtained from the above DFT-based calculations.

Surface and Electrical Characterization of Conjugated Molecular Wires

NASA Astrophysics Data System (ADS)

Demissie, Abel Tesfahun

This thesis describes the surface and electrical characterization of ultrathin organic films and interfaces. These films were synthesized on the surface of gold by utilizing layer by layer synthesis via imine condensation. Film growth by imine click (condensation) chemistry is particularly useful for molecular electronics experiments because it provides a convenient means to obtain and extend ?-conjugation in the growth direction. However, in the context of film growth from a solid substrate, the reaction yield per step has not been characterized previously, though it is critically important. To address these issues, my research focused on a comprehensive characterization of oligophenyleneimine (OPI) wires via Rutherford backscattering spectrometry (RBS), X-ray photoelectron spectroscopy (XPS), spectroscopic ellipsometry (SE), reflection-absorption infrared spectroscopy (RAIRS), and cyclic voltammetry (CV). In addition, we had the unique opportunity of developing the first of its kind implementation of nuclear reaction analysis (NRA) to probe the intensity of carbon atoms after each addition step. Overall the combination of various techniques indicated that film growth proceeds in a quantitative manner. Furthermore, the NRA experiment was optimized to measure the carbon content in self-assembled monolayers of alkyl thiols. The results indicated well-resolved coverage values for ultrathin films with consecutive steps of 2 carbon atoms per molecule. Another fundamental problem in molecular electronics is the vast discrepancy in the values of measured resistance per molecule between small and large area molecular junctions. In collaboration with researchers at the National University of Singapore, we addressed these issues by comparing the electrical properties of OPI wires with the eutectic gallium indium alloy (EGaIn) junction (1000 mum2), and conducting probe atomic force microscopy (CP-AFM) junction (50 nm2). Our results showed that intensive (i.e., area independent) observables such as crossover length, activation energy, and decay constants agreed very well across the two junction platforms. On the other hand, the extensive (area dependent) resistance per molecule values was 100 times higher for EGaIn junction verses CP-AFM after normalizing to contact area. This was most likely due to differences in metal-molecule contact resistances. My contribution to this collaborative work is in synthesis and timely delivery of OPI wires.. The structure-property relationships of OPI wires with 5 terminal F atoms were studied extensively by XPS. The results show similar crossover behavior obtained by molecular junction experiments. Saturated spacers (conjugation disruption units) were introduced into the molecular backbone, and their effects on the intensity of F 1s counts were measured. Overall, there was good correlation between the position and number of saturated units verses F 1s peak area. Even though core hole spectroscopy and time dependent density functional theory (TDDFT) calculations are required to fully understand the charge transport dynamics, the preliminary results point to a new ultrahigh vacuum method of measuring charge transfer rates. Overall, these experiments open significant opportunities to synthesize ultra-thin films and characterize a variety of donor-block-acceptor and metal complex systems in molecular electronics.

Three-dimensional atom probe tomography of oxide, anion, and alkanethiolate coatings on gold.

PubMed

Zhang, Yi; Hillier, Andrew C

2010-07-15

We have used three-dimensional atom probe tomography to analyze several nanometer-thick and monomolecular films on gold surfaces. High-purity gold wire was etched by electropolishing to create a sharp tip suitable for field evaporation with a radius of curvature of <100 nm. The near-surface region of a freshly etched gold tip was examined with the atom probe at subnanometer spatial resolution and with atom-level composition accuracy. A thin contaminant layer, primarily consisting of water and atmospheric gases, was observed on a fresh tip. This sample exhibited crystalline lattice spacings consistent with the interlayer spacing of {200} lattice planes of bulk gold. A thin oxide layer was created on the gold surface via plasma oxidation, and the thickness and composition of this layer was measured. Clear evidence of a nanometer-thick oxide layer was seen coating the gold tip, and the atomic composition of the oxide layer was consistent with the expected stoichiometry for gold oxide. Monomolecular anions layers of Br(-) and I(-) were created via adsorption from aqueous solutions onto the gold. Atom probe data verified the presence of the monomolecular anion layers on the gold surface, with ion density values consistent with literature values. A hexanethiolate monolayer was coated onto the gold tip, and atom probe analysis revealed a thin film whose ion fragments were consistent with the molecular composition of the monolayer and a surface coverage similar to that expected from literature. Details of the various coating compositions and structures are presented, along with discussion of the reconstruction issues associated with properly analyzing these thin-film systems.

Linear response formulism of a carbon nano-onion stringed to gold electrodes

NASA Astrophysics Data System (ADS)

Kaur, Milanpreet; Sawhney, Ravinder Singh; Engles, Derick

2017-04-01

Density functional theory is used to investigate the electronic state of a carbon nano-onion conglobated by endohedral-ing the highly curved C20 fullerene within its parent fullerene C60. The Non-Equilibrium Green's Function is later employed to examine the quantum transport when the carbon nano-onion, C20@C60 is stringed to the pair of gold electrodes of (001) plane. The computed results are evaluated and compared with C20 and C60 junctions. The calculated electronic parameters of these molecular junctions are utilized to extrapolate their two electrical parameters: current and conductance. The carbon nano-onion junction assembled from the C20 and C60 molecules displays the combined effect of their molecular junctions when organized separately. Also, the insertion of C20 molecule in the hollow cavity of C60 fullerene leads to the enhancement of its current and conductance in carbon nano-onion junction formed, when compared to the one constructed otherwise.

Atomically Thin Al2O3 Films for Tunnel Junctions

NASA Astrophysics Data System (ADS)

Wilt, Jamie; Gong, Youpin; Gong, Ming; Su, Feifan; Xu, Huikai; Sakidja, Ridwan; Elliot, Alan; Lu, Rongtao; Zhao, Shiping; Han, Siyuan; Wu, Judy Z.

2017-06-01

Metal-insulator-metal tunnel junctions are common throughout the microelectronics industry. The industry standard AlOx tunnel barrier, formed through oxygen diffusion into an Al wetting layer, is plagued by internal defects and pinholes which prevent the realization of atomically thin barriers demanded for enhanced quantum coherence. In this work, we employ in situ scanning tunneling spectroscopy along with molecular-dynamics simulations to understand and control the growth of atomically thin Al2O3 tunnel barriers using atomic-layer deposition. We find that a carefully tuned initial H2O pulse hydroxylated the Al surface and enabled the creation of an atomically thin Al2O3 tunnel barrier with a high-quality M -I interface and a significantly enhanced barrier height compared to thermal AlOx . These properties, corroborated by fabricated Josephson junctions, show that atomic-layer deposition Al2O3 is a dense, leak-free tunnel barrier with a low defect density which can be a key component for the next generation of metal-insulator-metal tunnel junctions.

Adhesion and Atomic Structures of Gold on Ceria Nanostructures:The Role of Surface Structure and Oxidation State of Ceria Supports

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lin, Yuyuan; Wu, Zili; Wen, Jianguo

2015-01-01

Recent advances in heterogeneous catalysis have demonstrated that oxides supports with the same material but different shapes can result in metal catalysts with distinct catalytic properties. The shape-dependent catalysis was not well-understood owing to the lack of direct visualization of the atomic structures at metal-oxide interface. Herein, we utilized aberration-corrected electron microscopy and revealed the atomic structures of gold particles deposited on ceria nanocubes and nanorods with {100} or {111} facets exposed. For the ceria nanocube support, gold nanoparticles have extended atom layers at the metal-support interface. In contrast, regular gold nanoparticles and rafts are present on the ceria nanorodmore » support. After hours of water gas shift reaction, the extended gold atom layers and rafts vanish, which is associated with the decrease of the catalytic activities. By understanding the atomic structures of the support surfaces, metal-support interfaces, and morphologies of the gold particles, a direct structure-property relationship is established.« less

Generating atomically sharp p -n junctions in graphene and testing quantum electron optics on the nanoscale

NASA Astrophysics Data System (ADS)

Bai, Ke-Ke; Zhou, Jiao-Jiao; Wei, Yi-Cong; Qiao, Jia-Bin; Liu, Yi-Wen; Liu, Hai-Wen; Jiang, Hua; He, Lin

2018-01-01

Creation of high-quality p -n junctions in graphene monolayer is vital in studying many exotic phenomena of massless Dirac fermions. However, even with the fast progress of graphene technology for more than ten years, it remains conspicuously difficult to generate nanoscale and atomically sharp p -n junctions in graphene. Here, we realized nanoscale p -n junctions with atomically sharp boundaries in graphene monolayer by using monolayer vacancy island of Cu surface. The generated sharp p -n junctions with the height as high as 660 meV isolate the graphene above the Cu monolayer vacancy island as nanoscale graphene quantum dots (GQDs) in a continuous graphene sheet. Massless Dirac fermions are confined by the p -n junctions for a finite time to form quasibound states in the GQDs. By using scanning tunneling microscopy, we observe resonances of quasibound states in the GQDs with various sizes and directly visualize effects of geometries of the GQDs on the quantum interference patterns of the quasibound states, which allow us to test the quantum electron optics based on graphene in atomic scale.

In Situ Scanning Tunneling Microscopy Topography Changes of Gold (111) in Aqueous Sulfuric Acid Produced by Electrochemical Surface Oxidation and Reduction and Relaxation Phenomena

NASA Astrophysics Data System (ADS)

Pasquale, M. A.; Nieto, F. J. Rodríguez; Arvia, A. J.

The electrochemical formation and reduction of O-layers on gold (111) films in 1 m sulfuric acid under different potentiodynamic routines are investigated utilizing in situ scanning tunneling microscopy. The surface dynamics is interpreted considering the anodic and cathodic reaction pathways recently proposed complemented with concurrent relaxation phenomena occurring after gold (111) lattice mild disruption (one gold atom deep) and moderate disruption (several atoms deep). The dynamics of both oxidized and reduced gold topographies depends on the potentiodynamic routine utilized to form OH/O surface species. The topography resulting from a mild oxidative disruption is dominated by quasi-2D holes and hillocks of the order of 5 nm, involving about 500-600 gold atoms each, and their coalescence. A cooperative turnover process at the O-layer, in which the anion ad-layer and interfacial water play a key role, determines the oxidized surface topography. The reduction of these O-layers results in gold clusters, their features depending on the applied potential routine. A moderate oxidative disruption produces a surface topography of hillocks and holes several gold atoms high and deep, respectively. The subsequent reduction leads to a spinodal gold pattern. Concurrent coalescence appears to be the result of an Ostwald ripening that involves the surface diffusion of both gold atoms and clusters. These processes produce an increase in surface roughness and an incipient gold faceting. The dynamics of different topographies can be qualitatively explained employing the arguments from colloidal science theory. For 1.1 V ≤ E ≅ Epzc weak electrostatic repulsions favor gold atom/cluster coalescence, whereas for E < Epzc the attenuated electrostatic repulsions among gold surfaces stabilize small clusters over the substrate producing string-like patterns.

OVERVIEW OF GOLD HILL MILL, ROAD, AND WHITE PINE TALC ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

OVERVIEW OF GOLD HILL MILL, ROAD, AND WHITE PINE TALC MINE LOOKING EAST. THE OPENING TO THE TALC MINE IS IN THE DARK AREA AT CENTER LEFT EDGE. WARM SPRINGS CAMP IS OUT OF FRAME TO THE RIGHT. - Gold Hill Mill, Warm Spring Canyon Road, Death Valley Junction, Inyo County, CA

Electron transport in doped fullerene molecular junctions

NASA Astrophysics Data System (ADS)

Kaur, Milanpreet; Sawhney, Ravinder Singh; Engles, Derick

The effect of doping on the electron transport of molecular junctions is analyzed in this paper. The doped fullerene molecules are stringed to two semi-infinite gold electrodes and analyzed at equilibrium and nonequilibrium conditions of these device configurations. The contemplation is done using nonequilibrium Green’s function (NEGF)-density functional theory (DFT) to evaluate its density of states (DOS), transmission coefficient, molecular orbitals, electron density, charge transfer, current, and conductance. We conclude from the elucidated results that Au-C16Li4-Au and Au-C16Ne4-Au devices behave as an ordinary p-n junction diode and a Zener diode, respectively. Moreover, these doped fullerene molecules do not lose their metallic nature when sandwiched between the pair of gold electrodes.

Controlling the thermoelectric effect by mechanical manipulation of the electron's quantum phase in atomic junctions.

PubMed

Aiba, Akira; Demir, Firuz; Kaneko, Satoshi; Fujii, Shintaro; Nishino, Tomoaki; Tsukagoshi, Kazuhito; Saffarzadeh, Alireza; Kirczenow, George; Kiguchi, Manabu

2017-08-11

The thermoelectric voltage developed across an atomic metal junction (i.e., a nanostructure in which one or a few atoms connect two metal electrodes) in response to a temperature difference between the electrodes, results from the quantum interference of electrons that pass through the junction multiple times after being scattered by the surrounding defects. Here we report successfully tuning this quantum interference and thus controlling the magnitude and sign of the thermoelectric voltage by applying a mechanical force that deforms the junction. The observed switching of the thermoelectric voltage is reversible and can be cycled many times. Our ab initio and semi-empirical calculations elucidate the detailed mechanism by which the quantum interference is tuned. We show that the applied strain alters the quantum phases of electrons passing through the narrowest part of the junction and hence modifies the electronic quantum interference in the device. Tuning the quantum interference causes the energies of electronic transport resonances to shift, which affects the thermoelectric voltage. These experimental and theoretical studies reveal that Au atomic junctions can be made to exhibit both positive and negative thermoelectric voltages on demand, and demonstrate the importance and tunability of the quantum interference effect in the atomic-scale metal nanostructures.

Platinum atomic wire encapsulated in gold nanotubes: A first principle study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nigam, Sandeep, E-mail: snigam@barc.gov.in; Majumder, Chiranjib; Sahoo, Suman K.

2014-04-24

The nanotubes of gold incorporated with platinum atomic wire have been investigated by means of firstprinciples density functional theory with plane wave pseudopotential approximation. The structure with zig-zag chain of Pt atoms in side gold is found to be 0.73 eV lower in energy in comparison to straight chain of platinum atoms. The Fermi level of the composite tube was consisting of d-orbitals of Pt atoms. Further interaction of oxygen with these tubes reveals that while tube with zig-zag Pt prefers dissociative adsorption of oxygen molecule, the gold tube with linear Pt wire favors molecular adsorption.

Two-dimensional PdSe2-Pd2Se3 junctions can serve as nanowires

NASA Astrophysics Data System (ADS)

Zuluaga, Sebastian; Lin, Junhao; Suenaga, Kazu; Pantelides, Sokrates T.

2018-07-01

While the exfoliation of almost all layered materials results in a monolayer with the same atomic geometry as its bulk counterpart, the exfoliation of PdSe2 results in a monolayer with a different atomic geometry and a new stoichiometry, Pd2Se3, which is a fusion of two PdSe2 monolayers mediated by Se emission. Here we first report first-principles calculations of lateral junctions between a PdSe2 bilayer and a Pd2Se3 monolayer. We find that, while several distinct junction geometries are possible, they all exhibit empty interface states below the conduction band. As a result, light n-type doping of either or both sides, e.g. by halogen atoms replacing Se atoms, leads to a remotely-doped interface, i.e. a 1D conducting nanowire that runs along the junction, in between the two semiconductors. We have fabricated such junctions inside a scanning transmission electron microscope (STEM), but doping and transport measurements are not currently practical.

Quasiparticle energies and lifetimes in a metallic chain model of a tunnel junction.

PubMed

Szepieniec, Mark; Yeriskin, Irene; Greer, J C

2013-04-14

As electronics devices scale to sub-10 nm lengths, the distinction between "device" and "electrodes" becomes blurred. Here, we study a simple model of a molecular tunnel junction, consisting of an atomic gold chain partitioned into left and right electrodes, and a central "molecule." Using a complex absorbing potential, we are able to reproduce the single-particle energy levels of the device region including a description of the effects of the semi-infinite electrodes. We then use the method of configuration interaction to explore the effect of correlations on the system's quasiparticle peaks. We find that when excitations on the leads are excluded, the device's highest occupied molecular orbital and lowest unoccupied molecular orbital quasiparticle states when including correlation are bracketed by their respective values in the Hartree-Fock (Koopmans) and ΔSCF approximations. In contrast, when excitations on the leads are included, the bracketing property no longer holds, and both the positions and the lifetimes of the quasiparticle levels change considerably, indicating that the combined effect of coupling and correlation is to alter the quasiparticle spectrum significantly relative to an isolated molecule.

Atomically dispersed Au-(OH)x species bound on titania catalyze the low-temperature water-gas shift reaction.

PubMed

Yang, Ming; Allard, Lawrence F; Flytzani-Stephanopoulos, Maria

2013-03-13

We report a new method for stabilizing appreciable loadings (~1 wt %) of isolated gold atoms on titania and show that these catalyze the low-temperature water-gas shift reaction. The method combines a typical gold deposition/precipitation method with UV irradiation of the titania support suspended in ethanol. Dissociation of H2O on the thus-created Au-O-TiO(x) sites is facile. At higher gold loadings, nanoparticles are formed, but they were shown to add no further activity to the atomically bound gold on titania. Removal of this "excess" gold by sodium cyanide leaching leaves the activity intact and the atomically dispersed gold still bound on titania. The new materials may catalyze a number of other reactions that require oxidized active metal sites.

Designing nanoscale constructs from atomic thin sheets of graphene, boron nitride and gold nanoparticles for advanced material applications

NASA Astrophysics Data System (ADS)

Jasuja, Kabeer

2011-12-01

Nanoscale materials invite immense interest from diverse scientific disciplines as these provide access to precisely understand the physical world at their most fundamental atomic level. In concert with this aim of enhancing our understanding of the fundamental behavior at nanoscale, this dissertation presents research on three nanomaterials: Gold nanoparticles (GNPs), Graphene and ultra-thin Boron Nitride sheets (UTBNSs). The three-fold goals which drive this research are: incorporating mobility in nanoparticle based single-electron junction constructs, developing effective strategies to functionalize graphene with nano-forms of metal, and exfoliating ultrathin sheets of Boron Nitride. Gold nanoparticle based electronic constructs can achieve a new degree of operational freedom if nanoscale mobility is incorporated in their design. We achieved such a nano-electromechanical construct by incorporating elastic polymer molecules between GNPs to form 2-dimensional (2-D) molecular junctions which show a nanoscale reversible motion on applying macro scale forces. This GNP-polymer assembly works like a molecular spring opening avenues to maneuver nano components and store energy at nano-scale. Graphene is the first isolated nanomaterial that displays single-atom thickness. It exhibits quantum confinement that enables it to possess a unique combination of fascinating electronic, optical, and mechanical properties. Modifying the surface of graphene is extremely significant to enable its incorporation into applications of interest. We demonstrated the ability of chemically modified graphene sheets to act as GNP stabilizing templates in solution, and utilized this to process GNP composites of graphene. We discovered that GNPs synthesized by chemical or microwave reduction stabilize on graphene-oxide sheets to form snow-flake morphologies and bare-surfaces respectively. These hybrid nano constructs were extensively studied to understand the effect and nature of GNPs' interaction with graphene, and applied to address the challenge of dispersing bare-surfaced GNPs for efficient liquid-phase catalysis. We also revisited the functionalization of graphene and present a non-invasive surface introduction of interfaceable moieties. Isostructural to graphene, ultrathin BN sheet is another atomic-thick nanomaterial possessing a highly diverse set of properties inconceivable from graphene. Exfoliating UTBNSs has been challenging due to their exceptional intersheet-bonding and chemical-inertness. To develop applications of BN monolayers and evolve research, a facile lab-scale approach was desired that can produce processable dispersions of BN monolayers. We demonstrated a novel chlorosulfonic acid based treatment that resulted in protonation assisted layer-by-layer exfoliation of BN monolayers with highest reported yields till date. Further, the BN monolayers exhibited extensively protonated N centers, which are utilized for chemically interfacing GNPs, demonstrating their ability to act as excellent nano-templates. The scientific details obtained from the research shown here will significantly support current research activities and greatly impact their future applications. Our research findings have been published in ACS Nano, Small, Journal of Physical Chemistry Letters, MRS Proceedings and have gathered >45 citations.

Geometric, electronic, and bonding properties of AuNM (N = 1-7, M = Ni, Pd, Pt) clusters.

PubMed

Yuan, D W; Wang, Yang; Zeng, Zhi

2005-03-15

Employing first-principles methods, based on density functional theory, we report the ground state geometric and electronic structures of gold clusters doped with platinum group atoms, Au(N)M (N = 1-7, M = Ni, Pd, Pt). The stability and electronic properties of Ni-doped gold clusters are similar to that of pure gold clusters with an enhancement of bond strength. Due to the strong d-d or s-d interplay between impurities and gold atoms originating in the relativistic effects and unique properties of dopant delocalized s-electrons in Pd- and Pt-doped gold clusters, the dopant atoms markedly change the geometric and electronic properties of gold clusters, and stronger bond energies are found in Pt-doped clusters. The Mulliken populations analysis of impurities and detailed decompositions of bond energies as well as a variety of density of states of the most stable dopant gold clusters are given to understand the different effects of individual dopant atom on bonding and electronic properties of dopant gold clusters. From the electronic properties of dopant gold clusters, the different chemical reactivity toward O(2), CO, or NO molecule is predicted in transition metal-doped gold clusters compared to pure gold clusters.

Structures of 38-atom gold-platinum nanoalloy clusters

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ong, Yee Pin; Yoon, Tiem Leong; Lim, Thong Leng

2015-04-24

Bimetallic nanoclusters, such as gold-platinum nanoclusters, are nanomaterials promising wide range of applications. We perform a numerical study of 38-atom gold-platinum nanoalloy clusters, Au{sub n}Pt{sub 38−n} (0 ≤ n ≤ 38), to elucidate the geometrical structures of these clusters. The lowest-energy structures of these bimetallic nanoclusters at the semi-empirical level are obtained via a global-minimum search algorithm known as parallel tempering multi-canonical basin hopping plus genetic algorithm (PTMBHGA), in which empirical Gupta many-body potential is used to describe the inter-atomic interactions among the constituent atoms. The structures of gold-platinum nanoalloy clusters are predicted to be core-shell segregated nanoclusters. Gold atomsmore » are observed to preferentially occupy the surface of the clusters, while platinum atoms tend to occupy the core due to the slightly smaller atomic radius of platinum as compared to gold’s. The evolution of the geometrical structure of 38-atom Au-Pt clusters displays striking similarity with that of 38-atom Au-Cu nanoalloy clusters as reported in the literature.« less

Tip-Enhanced Raman Nanographs: Mapping Topography and Local Electric Fields

DOE PAGES

El-Khoury, Patrick Z.; Gong, Yu; Abellan, Patricia; ...

2015-03-05

We report tip-enhanced Raman scattering experiments in which topographic and local electric field images are recorded simultaneously. We employ a Raman-active 4,4’-dimercaptostilbene (DMS)-coated gold tip of an atomic force microscope to map the topography and image electric fields localized at nanometric (20 and 5 nm-wide) slits lithographically etched in silver. Bi-modal imaging is feasible by virtue of the recorded scanning probe position-dependent frequency-resolved optical response, which can be sub-divided into two components. The first is a 500-2250 cm-1 Raman-shifted signal, characteristic of DMS. The molecular response reports on topography through intensity contrast in the absence/presence of a plasmonic junction formedmore » between the scanning probe and patterned silver surface. Here, we demonstrate that sub-15 nm spatial resolution is attainable using a 30 nm DMS-coated gold tip. The second response consists of two correlated sub-500 cm-1 signals arising from mirror-like reflections of (i) the incident laser, and (ii) the Raman scattered response of an underlying glass support (at 100-500 cm-1) off the gold tip. We show that both the low-wavenumber signals trace the local electric fields in the vicinity of the nanometric slits.« less

Direct mapping of electrical noise sources in molecular wire-based devices

PubMed Central

Cho, Duckhyung; Lee, Hyungwoo; Shekhar, Shashank; Yang, Myungjae; Park, Jae Yeol; Hong, Seunghun

2017-01-01

We report a noise mapping strategy for the reliable identification and analysis of noise sources in molecular wire junctions. Here, different molecular wires were patterned on a gold substrate, and the current-noise map on the pattern was measured and analyzed, enabling the quantitative study of noise sources in the patterned molecular wires. The frequency spectra of the noise from the molecular wire junctions exhibited characteristic 1/f2 behavior, which was used to identify the electrical signals from molecular wires. This method was applied to analyze the molecular junctions comprising various thiol molecules on a gold substrate, revealing that the noise in the junctions mainly came from the fluctuation of the thiol bonds. Furthermore, we quantitatively compared the frequencies of such bond fluctuations in different molecular wire junctions and identified molecular wires with lower electrical noise, which can provide critical information for designing low-noise molecular electronic devices. Our method provides valuable insights regarding noise phenomena in molecular wires and can be a powerful tool for the development of molecular electronic devices. PMID:28233821

Direct mapping of electrical noise sources in molecular wire-based devices

NASA Astrophysics Data System (ADS)

Cho, Duckhyung; Lee, Hyungwoo; Shekhar, Shashank; Yang, Myungjae; Park, Jae Yeol; Hong, Seunghun

2017-02-01

We report a noise mapping strategy for the reliable identification and analysis of noise sources in molecular wire junctions. Here, different molecular wires were patterned on a gold substrate, and the current-noise map on the pattern was measured and analyzed, enabling the quantitative study of noise sources in the patterned molecular wires. The frequency spectra of the noise from the molecular wire junctions exhibited characteristic 1/f2 behavior, which was used to identify the electrical signals from molecular wires. This method was applied to analyze the molecular junctions comprising various thiol molecules on a gold substrate, revealing that the noise in the junctions mainly came from the fluctuation of the thiol bonds. Furthermore, we quantitatively compared the frequencies of such bond fluctuations in different molecular wire junctions and identified molecular wires with lower electrical noise, which can provide critical information for designing low-noise molecular electronic devices. Our method provides valuable insights regarding noise phenomena in molecular wires and can be a powerful tool for the development of molecular electronic devices.

Statistical evidence of strain induced breaking of metallic point contacts

NASA Astrophysics Data System (ADS)

Alwan, Monzer; Candoni, Nadine; Dumas, Philippe; Klein, Hubert R.

2013-06-01

A scanning tunneling microscopy in break junction regime and a mechanically controllable break junction are used to acquire thousands of conductance-elongation curves by stretching until breaking and re-connecting Au junctions. From a robust statistical analysis performed on large sets of experiments, parameters such as lifetime, elongation and occurrence probabilities are extracted. The analysis of results obtained for different stretching speeds of the electrodes indicates that the breaking mechanism of di- and mono-atomic junction is identical, and that the junctions undergo atomic rearrangement during their stretching and at the moment of breaking.

Single molecule junction conductance and binding geometry

NASA Astrophysics Data System (ADS)

Kamenetska, Maria

This Thesis addresses the fundamental problem of controlling transport through a metal-organic interface by studying electronic and mechanical properties of single organic molecule-metal junctions. Using a Scanning Tunneling Microscope (STM) we image, probe energy-level alignment and perform STM-based break junction (BJ) measurements on molecules bound to a gold surface. Using Scanning Tunneling Microscope-based break-junction (STM-BJ) techniques, we explore the effect of binding geometry on single-molecule conductance by varying the structure of the molecules, metal-molecule binding chemistry and by applying sub-nanometer manipulation control to the junction. These experiments are performed both in ambient conditions and in ultra high vacuum (UHV) at cryogenic temperatures. First, using STM imaging and scanning tunneling spectroscopy (STS) measurements we explore binding configurations and electronic properties of an amine-terminated benzene derivative on gold. We find that details of metal-molecule binding affect energy-level alignment at the interface. Next, using the STM-BJ technique, we form and rupture metal-molecule-metal junctions ˜104 times to obtain conductance-vs-extension curves and extract most likely conductance values for each molecule. With these measurements, we demonstrated that the control of junction conductance is possible through a choice of metal-molecule binding chemistry and sub-nanometer positioning. First, we show that molecules terminated with amines, sulfides and phosphines bind selectively on gold and therefore demonstrate constant conductance levels even as the junction is elongated and the metal-molecule attachment point is modified. Such well-defined conductance is also obtained with paracyclophane molecules which bind to gold directly through the pi system. Next, we are able to create metal-molecule-metal junctions with more than one reproducible conductance signatures that can be accessed by changing junction geometry. In the case of pyridine-linked molecules, conductance can be reliably switched between two distinct conductance states using sub-nanometer mechanical manipulation. Using a methyl sulfide linker attached to an oligoene backbone, we are able to create a 3-nm-long molecular potentiometer, whose resistance can be tuned exponentially with Angstom-scale modulations in metal-molecule configuration. These experiments points to a new paradigm for attaining reproducible electrical characteristics of metal-organic devices which involves controlling linker-metal chemistry rather than fabricating identically structured metal-molecule interfaces. By choosing a linker group which is either insensitive to or responds reproducibly to changes in metal-molecule configuration, one can design single molecule devices with functionality more complex than a simple resistor. These ambient temperature experiments were combined with UHV conductance measurements performed in a commercial STM on amine-terminated benzene derivatives which conduct through a non-resonant tunneling mechanism, at temperatures varying from 5 to 300 Kelvin. Our results indicate that while amine-gold binding remains selective irrespective of environment, conductance is not temperature independent, in contrast to what is expected for a tunneling mechanism. Furthermore, using temperature-dependent measurements in ambient conditions we find that HOMO-conducting amines and LUMO-conducting pyridines show opposite dependence of conductance on temperature. These results indicate that energy-level alignment between the molecule and the electrodes changes as a result of varying electrode structure at different temperatures. We find that temperature can serve as a knob with which to tune transport properties of single molecule-metal junctions.

Structure and Stability of GeAu{sub n}, n = 1-10 clusters: A Density Functional Study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Priyanka,; Dharamvir, Keya; Sharma, Hitesh

2011-12-12

The structures of Germanium doped gold clusters GeAu{sub n} (n = 1-10) have been investigated using ab initio calculations based on density functional theory (DFT). We have obtained ground state geometries of GeAu{sub n} clusters and have it compared with Silicon doped gold clusters and pure gold clusters. The ground state geometries of the GeAu{sub n} clusters show patterns similar to silicon doped gold clusters except for n = 5, 6 and 9. The introduction of germanium atom increases the binding energy of gold clusters. The binding energy per atom of germanium doped cluster is smaller than the corresponding siliconmore » doped gold cluster. The HUMO-LOMO gap for Au{sub n}Ge clusters have been found to vary between 0.46 eV-2.09 eV. The mullikan charge analysis indicates that charge of order of 0.1e always transfers from germanium atom to gold atom.« less

A history of gap junction structure: hexagonal arrays to atomic resolution.

PubMed

Grosely, Rosslyn; Sorgen, Paul L

2013-02-01

Gap junctions are specialized membrane structures that provide an intercellular pathway for the propagation and/or amplification of signaling cascades responsible for impulse propagation, cell growth, and development. Prior to the identification of the proteins that comprise gap junctions, elucidation of channel structure began with initial observations of a hexagonal nexus connecting apposed cellular membranes. Concomitant with technological advancements spanning over 50 years, atomic resolution structures are now available detailing channel architecture and the cytoplasmic domains that have helped to define mechanisms governing the regulation of gap junctions. Highlighted in this review are the seminal structural studies that have led to our current understanding of gap junction biology.

Charge transport in vertically aligned, self-assembled peptide nanotube junctions.

PubMed

Mizrahi, Mordechay; Zakrassov, Alexander; Lerner-Yardeni, Jenny; Ashkenasy, Nurit

2012-01-21

The self-assembly propensity of peptides has been extensively utilized in recent years for the formation of supramolecular nanostructures. In particular, the self-assembly of peptides into fibrils and nanotubes makes them promising building blocks for electronic and electro-optic applications. However, the mechanisms of charge transfer in these wire-like structures, especially in ambient conditions, are not yet fully understood. We describe here a layer-by-layer deposition methodology of short self-assembled cyclic peptide nanotubes, which results in vertically oriented nanotubes on gold substrates. Using this novel deposition methodology, we have fabricated molecular junctions with a conductive atomic force microscopy tip as a second electrode. Studies of the junctions' current-voltage characteristics as a function of the nanotube length revealed an efficient charge transfer in these supramolecular structures, with a low current attenuation constant of 0.1 Å(-1), which indicate that electron transfer is dominated by hopping. Moreover, the threshold voltage to field-emission dominated transport was found to increase with peptide length in a manner that depends on the nature of the contact with the electrodes. The flexibility in the design of the peptide monomers and the ability to control their sequential order over the nanotube by means of the layer-by-layer assembly process, which is demonstrated in this work, can be used to engineer the electronic properties of self-assembled peptide nanotubes toward device applications.

Precipitation of lamellar gold nanocrystals in molten polymers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Palomba, M.; Carotenuto, G., E-mail: giancaro@unina.it

Non-aggregated lamellar gold crystals with regular shape (triangles, squares, pentagons, etc.) have been produced by thermal decomposition of gold chloride (AuCl) molecules in molten amorphous polymers (polystyrene and poly(methyl methacrylate)). Such covalent inorganic gold salt is high soluble into non-polar polymers and it thermally decomposes at temperatures compatible with the polymer thermal stability, producing gold atoms and chlorine radicals. At the end of the gold precipitation process, the polymer matrix resulted chemically modified because of the partial cross-linking process due to the gold atom formation reaction.

Derivatized gold clusters and antibody-gold cluster conjugates

DOEpatents

Hainfeld, James F.; Furuya, Frederic R.

1994-11-01

Antibody- or antibody fragment-gold cluster conjugates are shown wherein the conjugate size can be as small as 5.0 nm. Methods and reagents are disclosed in which antibodies, Fab' or F(ab').sub.2 fragments thereof are covalently bound to a stable cluster of gold atoms. The gold clusters may contain 6, 8, 9, 11, 13, 55 or 67 gold atoms in their inner core. The clusters may also contain radioactive gold. The antibody-cluster conjugates are useful in electron microscopy applications as well as in clinical applications that include imaging, diagnosis and therapy.

ELECTRON MICROSCOPIC LOCALIZATION OF ACETYLCHOLINESTERASE AND NONSPECIFIC CHOLINESTERASE AT THE NEUROMUSCULAR JUNCTION BY THE GOLD-THIOCHOLINE AND GOLD-THIOLACETIC ACID METHODS

PubMed Central

Davis, Richard; Koelle, George B.

1967-01-01

By means of the gold-thiocholine (AuThCh) and gold-thiolacetic acid (AuThAc) methods, it has been demonstrated electron microscopically that acetylcholinesterase (AChE) is located at the prejunctional axoplasmic membrane and the postjunctional sarcoplasmic membrane, including the full lengths of its invaginations, at the motor end plate of mouse intercostal muscle. Nonspecific cholinesterase (ChE) is present in relatively low concentrations at the same sites, and in greater concentrations in the teloglial Schwann sheath cells. Significant amounts of reaction product appeared in the junctional cleft only after prolonged incubation with both methods. The identification of AChE and ChE was confirmed by the use of appropriate concentrations of several selective inhibitors. In confirmation of previous studies by light microscopy, the AuThCh method is more specific for AChE and ChE, whereas the AuThAc method allows greater accuracy of localization. PMID:6033530

Measure synchronization in a spin-orbit-coupled bosonic Josephson junction

NASA Astrophysics Data System (ADS)

Wang, Wen-Yuan; Liu, Jie; Fu, Li-Bin

2015-11-01

We present measure synchronization (MS) in a bosonic Josephson junction with spin-orbit coupling. The two atomic hyperfine states are coupled by a Raman dressing scheme, and they are regarded as two orientations of a pseudo-spin-1 /2 system. A feature specific to a spin-orbit-coupled (SOC) bosonic Josephson junction is that the transition from non-MS to MS dynamics can be modulated by Raman laser intensity, even in the absence of interspin atomic interaction. A phase diagram of non-MS and MS dynamics as functions of Raman laser intensity and Josephson tunneling amplitude is presented. Taking into account interspin atomic interactions, the system exhibits MS breaking dynamics resulting from the competition between intraspin and interspin atomic interactions. When interspin atomic interactions dominate in the competition, the system always exhibits MS dynamics. For interspin interaction weaker than intraspin interaction, a window for non-MS dynamics is present. Since SOC Bose-Einstein condensates provide a powerful platform for studies on physical problems in various fields, the study of MS dynamics is valuable in researching the collective coherent dynamical behavior in a spin-orbit-coupled bosonic Josephson junction.

Current-voltage characteristics of single-molecule diarylethene junctions measured with adjustable gold electrodes in solution.

PubMed

Briechle, Bernd M; Kim, Youngsang; Ehrenreich, Philipp; Erbe, Artur; Sysoiev, Dmytro; Huhn, Thomas; Groth, Ulrich; Scheer, Elke

2012-01-01

We report on an experimental analysis of the charge transport through sulfur-free photochromic molecular junctions. The conductance of individual molecules contacted with gold electrodes and the current-voltage characteristics of these junctions are measured in a mechanically controlled break-junction system at room temperature and in liquid environment. We compare the transport properties of a series of molecules, labeled TSC, MN, and 4Py, with the same switching core but varying side-arms and end-groups designed for providing the mechanical and electrical contact to the gold electrodes. We perform a detailed analysis of the transport properties of TSC in its open and closed states. We find rather broad distributions of conductance values in both states. The analysis, based on the assumption that the current is carried by a single dominating molecular orbital, reveals distinct differences between both states. We discuss the appearance of diode-like behavior for the particular species 4Py that features end-groups, which preferentially couple to the metal electrode by physisorption. We show that the energetic position of the molecular orbital varies as a function of the transmission. Finally, we show for the species MN that the use of two cyano end-groups on each side considerably enhances the coupling strength compared to the typical behavior of a single cyano group.

Flameless atomic-absorption determination of gold in geological materials

USGS Publications Warehouse

Meier, A.L.

1980-01-01

Gold in geologic material is dissolved using a solution of hydrobromic acid and bromine, extracted with methyl isobutyl ketone, and determined using an atomic-absorption spectrophotometer equipped with a graphite furnace atomizer. A comparison of results obtained by this flameless atomic-absorption method on U.S. Geological Survey reference rocks and geochemical samples with reported values and with results obtained by flame atomic-absorption shows that reasonable accuracy is achieved with improved precision. The sensitivity, accuracy, and precision of the method allows acquisition of data on the distribution of gold at or below its crustal abundance. ?? 1980.

Alloy-assisted deposition of three-dimensional arrays of atomic gold catalyst for crystal growth studies

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fang, Yin; Jiang, Yuanwen; Cherukara, Mathew J.

Large-scale assembly of individual atoms over smooth surfaces is difficult to achieve. A configuration of an atom reservoir, in which individual atoms can be readily extracted, may successfully address this challenge. In this work, we demonstrate that a liquid gold-silicon alloy established in classical vapor-liquid-solid growth can deposit ordered and three-dimensional rings of isolated gold atoms over silicon nanowire sidewalls. Here, we perform ab initio molecular dynamics simulation and unveil a surprising single atomic gold-catalyzed chemical etching of silicon. Experimental verification of this catalytic process in silicon nanowires yields dopant-dependent, massive and ordered 3D grooves with spacing down to similarmore » to 5 nm. Finally, we use these grooves as self-labeled and ex situ markers to resolve several complex silicon growths, including the formation of nodes, kinks, scale-like interfaces, and curved backbones.« less

Alloy-assisted deposition of three-dimensional arrays of atomic gold catalyst for crystal growth studies

DOE PAGES

Fang, Yin; Jiang, Yuanwen; Cherukara, Mathew J.; ...

2017-12-08

Large-scale assembly of individual atoms over smooth surfaces is difficult to achieve. A configuration of an atom reservoir, in which individual atoms can be readily extracted, may successfully address this challenge. In this work, we demonstrate that a liquid gold-silicon alloy established in classical vapor-liquid-solid growth can deposit ordered and three-dimensional rings of isolated gold atoms over silicon nanowire sidewalls. Here, we perform ab initio molecular dynamics simulation and unveil a surprising single atomic gold-catalyzed chemical etching of silicon. Experimental verification of this catalytic process in silicon nanowires yields dopant-dependent, massive and ordered 3D grooves with spacing down to similarmore » to 5 nm. Finally, we use these grooves as self-labeled and ex situ markers to resolve several complex silicon growths, including the formation of nodes, kinks, scale-like interfaces, and curved backbones.« less

Controlling formation of single-molecule junctions by electrochemical reduction of diazonium terminal groups.

PubMed

Hines, Thomas; Díez-Pérez, Ismael; Nakamura, Hisao; Shimazaki, Tomomi; Asai, Yoshihiro; Tao, Nongjian

2013-03-06

We report controlling the formation of single-molecule junctions by means of electrochemically reducing two axialdiazonium terminal groups on a molecule, thereby producing direct Au-C covalent bonds in situ between the molecule and gold electrodes. We report a yield enhancement in molecular junction formation as the electrochemical potential of both junction electrodes approach the reduction potential of the diazonium terminal groups. Step length analysis shows that the molecular junction is significantly more stable, and can be pulled over a longer distance than a comparable junction created with amine anchoring bonds. The stability of the junction is explained by the calculated lower binding energy associated with the direct Au-C bond compared with the Au-N bond.

Inelastic fingerprints of hydrogen contamination in atomic gold wire systems

NASA Astrophysics Data System (ADS)

Frederiksen, Thomas; Paulsson, Magnus; Brandbyge, Mads

2007-03-01

We present series of first-principles calculations for both pure and hydrogen contaminated gold wire systems in order to investigate how such impurities can be detected. We show how a single H atom or a single H2 molecule in an atomic gold wire will affect forces and Au-Au atom distances under elongation. We further determine the corresponding evolution of the low-bias conductance as well as the inelastic contributions from vibrations. Our results indicate that the conductance of gold wires is only slightly reduced from the conductance quantum G0 = 2e2/h by the presence of a single hydrogen impurity, hence making it difficult to use the conductance itself to distinguish between various configurations. On the other hand, our calculations of the inelastic signals predict significant differences between pure and hydrogen contaminated wires, and, importantly, between atomic and molecular forms of the impurity. A detailed characterization of gold wires with a hydrogen impurity should therefore be possible from the strain dependence of the inelastic signals in the conductance.

Multipoint anchoring of the [2.2.2.2]metacyclophane motif to a gold surface via self-assembly: coordination chemistry of a cyclic tetraisocyanide revisited.

PubMed

Toriyama, Masaharu; Maher, Tiffany R; Holovics, Thomas C; Vanka, Kumar; Day, Victor W; Berrie, Cindy L; Thompson, Ward H; Barybin, Mikhail V

2008-04-21

A one-pot transformation of bis(2-isocyano-3-methylphenyl)ethane affords gram quantities of 8,16,24,32-tetraisocyano[2.2.2.2]metacyclophane ( 3). The solid state structure of 3 is remarkably close to the lowest energy conformation found on the potential energy landscape for 3 by DFT. In solution, the structure of metacyclophane 3 is mobile but can be locked in a rectangular gauche- anti- gauche- anti conformation by coordination of the isocyanide substituents to the [W(CO) 5] units to give [M] 4(mu 4-eta (1):eta (1):eta (1):eta (1)- 3) ( 5). The tetranuclear [M] 4(mu 4-eta (1):eta (1):eta (1):eta (1)- 3) motif featured in crystallographically characterized 5 may be present in several insoluble complexes of 3 previously described as mononuclear eta (4) species. A self-assembled monolayer of metacyclophane 3 is formed upon exposing a solution of 3 to the gold(111) surface with no precautions to exclude air or light. The monolayer nature of the film was confirmed by optical ellipsometry. The isocyanide stretching band for 3 shifts from 2119 cm (-1) in solution to 2175 cm (-1) upon chemisorption to metallic gold. The FTIR spectrum of the film indicates interaction of 3 with the gold surface via all four of its isocyanide anchors. No gold-facilitated oxidation of the -NC junctions was detected under ambient conditions. The energy cost associated with accessing the conformations of 3 suitable for mu 4-eta (1):eta (1):eta (1):eta (1) interaction of the molecule with the Au(111) surface is under 8 kcal/mol, a value that can be easily offset by formation of a gold-isocyanide bond. Two different mu 4-eta (1):eta (1):eta (1):eta (1) coordination arrangements of 3 with respect to gold atoms on the (111) face of the fcc Au lattice are suggested.

Effects of the molecule-electrode interface on the low-bias conductance of Cu-H2-Cu single-molecule junctions.

PubMed

Jiang, Zhuoling; Wang, Hao; Shen, Ziyong; Sanvito, Stefano; Hou, Shimin

2016-07-28

The atomic structure and electronic transport properties of a single hydrogen molecule connected to both symmetric and asymmetric Cu electrodes are investigated by using the non-equilibrium Green's function formalism combined with the density functional theory. Our calculations show that in symmetric Cu-H2-Cu junctions, the low-bias conductance drops rapidly upon stretching, while asymmetric ones present a low-bias conductance spanning the 0.2-0.3 G0 interval for a wide range of electrode separations. This is in good agreement with experiments on Cu atomic contacts in a hydrogen environment. Furthermore, the distribution of the calculated vibrational energies of the two hydrogen atoms in the asymmetric Cu-H2-Cu junction is also consistent with experiments. These findings provide clear evidence for the formation of asymmetric Cu-H2-Cu molecular junctions in breaking Cu atomic contacts in the presence of hydrogen and are also helpful for the design of molecular devices with Cu electrodes.

Derivatized gold clusters and antibody-gold cluster conjugates

DOEpatents

Hainfeld, J.F.; Furuya, F.R.

1994-11-01

Antibody- or antibody fragment-gold cluster conjugates are shown wherein the conjugate size can be as small as 5.0 nm. Methods and reagents are disclosed in which antibodies, Fab' or F(ab')[sub 2] fragments are covalently bound to a stable cluster of gold atoms. The gold clusters may contain 6, 8, 9, 11, 13, 55 or 67 gold atoms in their inner core. The clusters may also contain radioactive gold. The antibody-cluster conjugates are useful in electron microscopy applications as well as in clinical applications that include imaging, diagnosis and therapy. 7 figs.

Low resistance contacts for shallow junction semiconductors

NASA Technical Reports Server (NTRS)

Fatemi, Navid S. (Inventor); Weizer, Victor G. (Inventor)

1994-01-01

A method of enhancing the specific contact resistivity in InP semiconductor devices and improved devices produced thereby are disclosed. Low resistivity values are obtained by using gold ohmic contacts that contain small amounts of gallium or indium and by depositing a thin gold phosphide interlayer between the surface of the InP device and the ohmic contact. When both the thin interlayer and the gold-gallium or gold-indium contact metallizations are used, ultra low specific contact resistivities are achieved. Thermal stability with good contact resistivity is achieved by depositing a layer of refractory metal over the gold phosphide interlayer.

Mapping atomic contact between pentacene and a Au surface using scanning tunneling spectroscopy.

PubMed

Song, Young Jae; Lee, Kyuho; Kim, Seong Heon; Choi, Byoung-Young; Yu, Jaejun; Kuk, Young

2010-03-10

We mapped spatially varying intramolecular electronic structures on a pentacene-gold interface using scanning tunneling spectroscopy. Along with ab initio calculations based on density functional theory, we found that the directional nature of the d orbitals of Au atoms plays an important role in the interaction at the pentacene-gold contact. The gold-induced interface states are broadened and shifted by various pentacene-gold distances determined by the various registries of a pentacene molecule on a gold substrate.

MicroED Structure of Au146(p-MBA)57 at Subatomic Resolution Reveals a Twinned FCC Cluster.

PubMed

Vergara, Sandra; Lukes, Dylan A; Martynowycz, Michael W; Santiago, Ulises; Plascencia-Villa, Germán; Weiss, Simon C; de la Cruz, M Jason; Black, David M; Alvarez, Marcos M; López-Lozano, Xochitl; Barnes, Christopher O; Lin, Guowu; Weissker, Hans-Christian; Whetten, Robert L; Gonen, Tamir; Yacaman, Miguel Jose; Calero, Guillermo

2017-11-16

Solving the atomic structure of metallic clusters is fundamental to understanding their optical, electronic, and chemical properties. Herein we present the structure of the largest aqueous gold cluster, Au 146 (p-MBA) 57 (p-MBA: para-mercaptobenzoic acid), solved by electron micro-diffraction (MicroED) to subatomic resolution (0.85 Å) and by X-ray diffraction at atomic resolution (1.3 Å). The 146 gold atoms may be decomposed into two constituent sets consisting of 119 core and 27 peripheral atoms. The core atoms are organized in a twinned FCC structure, whereas the surface gold atoms follow a C 2 rotational symmetry about an axis bisecting the twinning plane. The protective layer of 57 p-MBAs fully encloses the cluster and comprises bridging, monomeric, and dimeric staple motifs. Au 146 (p-MBA) 57 is the largest cluster observed exhibiting a bulk-like FCC structure as well as the smallest gold particle exhibiting a stacking fault.

MicroED structure of Au146(p-MBA)57 at subatomic resolution reveals a twinned FCC cluster

PubMed Central

Vergara, Sandra; Lukes, Dylan A.; Martynowycz, Michael W.; Santiago, Ulises; Plascencia-Villa, German; Weiss, Simon C.; de la Cruz, M. Jason; Black, David M.; Alvarez, Marcos M.; Lopez-Lozano, Xochitl; Barnes, Christopher O.; Lin, Guowu; Weissker, Hans-Christian; Whetten, Robert L.; Gonen, Tamir; Jose-Yacaman, Miguel; Calero, Guillermo

2018-01-01

Solving the atomic structure of metallic clusters is fundamental to understanding their optical, electronic, and chemical properties. Herein we present the structure of the largest aqueous gold cluster, Au146(p-MBA)57 (p-MBA: para-mercaptobenzoic acid), solved by electron diffraction (MicroED) to subatomic resolution (0.85 Å) and by X-ray diffraction at atomic resolution (1.3 Å). The 146 gold atoms may be decomposed into two constituent sets consisting of 119 core and 27 peripheral atoms. The core atoms are organized in a twinned FCC structure whereas the surface gold atoms follow a C2 rotational symmetry about an axis bisecting the twinning plane. The protective layer of 57 p-MBAs fully encloses the cluster and comprises bridging, monomeric, and dimeric staple motifs. Au146(p-MBA)57 is the largest cluster observed exhibiting a bulk-like FCC structure as well as the smallest gold particle exhibiting a stacking fault. PMID:29072840

Fluorescent sensing of cocaine based on a structure switching aptamer, gold nanoparticles and graphene oxide.

PubMed

Shi, Yan; Dai, Haichao; Sun, Yujing; Hu, Jingting; Ni, Pengjuan; Li, Zhuang

2013-12-07

This study demonstrates a cocaine sensing method employing graphene oxide (GO), gold nanoparticles and a structure switching aptamer, which can fold into a three-way junction in the presence of cocaine. On the observation of gold nanoparticles (Au NPs) induced graphene oxide fluorescence quenching, a structure switching aptamer of cocaine was introduced as the linker between the two parts. Firstly, two fragments of a cocaine aptamer were immobilized covalently onto GO and Au NPs, respectively. Then when the three-way junction formed, the Au NPs were drawn near to the GO surface and induced a fluorescence intensity decrease. The limit of detection was 0.1 μM for cocaine in purified water, and well defined results were also obtained in biological fluids and the specificity experiment, which expands the feasibility of the as-prepared sensor for practical applications.

SOUTH ELEVATION OF GOLD HILL MILL, LOOKING NORTH. THE PRIMARY ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

SOUTH ELEVATION OF GOLD HILL MILL, LOOKING NORTH. THE PRIMARY ORE BIN IS A CENTER, WITH A JAW CRUSHER JUST TO THE RIGHT. A CONVEYOR (MISSING) WAS USED TO CARRY CRUSHED ORE UP AND INTO THE SECONDARY ORE BIN. THE STONE RAMP TO THE LEFT OF THE ORE BIN WAS USED TO DRIVE TRUCKS UP TO DUMPING LEVEL. - Gold Hill Mill, Warm Spring Canyon Road, Death Valley Junction, Inyo County, CA

Dynamic Tunneling Junctions at the Atomic Intersection of Two Twisted Graphene Edges.

PubMed

Bellunato, Amedeo; Vrbica, Sasha D; Sabater, Carlos; de Vos, Erik W; Fermin, Remko; Kanneworff, Kirsten N; Galli, Federica; van Ruitenbeek, Jan M; Schneider, Grégory F

2018-04-11

The investigation of the transport properties of single molecules by flowing tunneling currents across extremely narrow gaps is relevant for challenges as diverse as the development of molecular electronics and sequencing of DNA. The achievement of well-defined electrode architectures remains a technical challenge, especially due to the necessity of high precision fabrication processes and the chemical instability of most bulk metals. Here, we illustrate a continuously adjustable tunneling junction between the edges of two twisted graphene sheets. The unique property of the graphene electrodes is that the sheets are rigidly supported all the way to the atomic edge. By analyzing the tunneling current characteristics, we also demonstrate that the spacing across the gap junction can be controllably adjusted. Finally, we demonstrate the transition from the tunneling regime to contact and the formation of an atomic-sized junction between the two edges of graphene.

Dynamic Tunneling Junctions at the Atomic Intersection of Two Twisted Graphene Edges

PubMed Central

2018-01-01

The investigation of the transport properties of single molecules by flowing tunneling currents across extremely narrow gaps is relevant for challenges as diverse as the development of molecular electronics and sequencing of DNA. The achievement of well-defined electrode architectures remains a technical challenge, especially due to the necessity of high precision fabrication processes and the chemical instability of most bulk metals. Here, we illustrate a continuously adjustable tunneling junction between the edges of two twisted graphene sheets. The unique property of the graphene electrodes is that the sheets are rigidly supported all the way to the atomic edge. By analyzing the tunneling current characteristics, we also demonstrate that the spacing across the gap junction can be controllably adjusted. Finally, we demonstrate the transition from the tunneling regime to contact and the formation of an atomic-sized junction between the two edges of graphene. PMID:29513997

Current trends in multimodality treatment of esophageal and gastroesophageal junction cancer - Review article.

PubMed

Klevebro, Fredrik; Ekman, Simon; Nilsson, Magnus

2017-09-01

Multimodality treatment has now been widely introduced in the curatively intended treatment of esophageal and gastroesophageal junction cancer. We aim to give an overview of the scientific evidence for the available treatment strategies and to describe which trends that are currently developing. We conducted a review of the scientific evidence for the different curatively intended treatment strategies that are available today. Relevant articles of randomized controlled trials, cohort studies, and meta analyses were included. After a systematic search of relevant papers we have included 64 articles in the review. The results show that adenocarcinomas and squamous cell carcinomas of the esophagus and gastroesophageal junction are two separate entities and should be analysed and studied as two different diseases. Neoadjuvant treatment followed by surgical resection is the gold standard of the curatively intended treatment today. There is no scientific evidence to support the use of chemoradiotherapy over chemotherapy in the neoadjuvant setting for esophageal or junctional adenocarcinoma. There is reasonable evidence to support definitive chemoradiotherapy as a treatment option for squamous cell carcinoma of the esophagus. The evidence base for curatively intended treatments of esophageal and gastroesophageal junction cancer is not very strong. Several on-going trials have the potential to change the gold standard treatments of today. Copyright © 2017 Elsevier Ltd. All rights reserved.

Electrochemical oxygen reduction behavior of selectively deposited platinum atoms on gold nanoparticles.

PubMed

Sarkar, A; Kerr, J B; Cairns, E J

2013-07-22

Carbon-supported Pt@Au "core-shell" nanoparticles with varying surface concentration of platinum atoms have been synthesized using a novel redox-mediated synthesis approach. The synthesis technique allows for a selective deposition of platinum atoms on the surface of prefabricated gold nanoparticles. Energy dispersive spectroscopic analyses in a scanning electron microscope reveal that the platinum to gold atomic ratios are close to the nominal values, validating the synthesis scheme. X-ray diffraction data indicate an un-alloyed structure. The platinum to gold surface atomic ratio determined from cyclic voltammetry and copper under-potential deposition experiments reveal good agreement with the calculated values at low platinum concentration. However, there is an increase in non-uniformity in the deposition process upon increasing the platinum concentration. Koutecky-Levich analysis of the samples indicates a transition of the total number of electrons transferred (n) in the electrochemical oxygen reduction reaction from two to four electrons upon increasing the surface concentration of platinum atoms. Furthermore, the data indicate that isolated platinum atoms can reduce molecular oxygen but via a two-electron route. Moreover, successful four-electron reduction of molecular oxygen requires clusters of platinum atoms. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Ballistic Anisotropic Magnetoresistance of Single-Atom Contacts.

PubMed

Schöneberg, J; Otte, F; Néel, N; Weismann, A; Mokrousov, Y; Kröger, J; Berndt, R; Heinze, S

2016-02-10

Anisotropic magnetoresistance, that is, the sensitivity of the electrical resistance of magnetic materials on the magnetization direction, is expected to be strongly enhanced in ballistic transport through nanoscale junctions. However, unambiguous experimental evidence of this effect is difficult to achieve. We utilize single-atom junctions to measure this ballistic anisotropic magnetoresistance (AMR). Single Co and Ir atoms are deposited on domains and domain walls of ferromagnetic Fe layers on W(110) to control their magnetization directions. They are contacted with nonmagnetic tips in a low-temperature scanning tunneling microscope to measure the junction conductances. Large changes of the magnetoresistance occur from the tunneling to the ballistic regime due to the competition of localized and delocalized d-orbitals, which are differently affected by spin-orbit coupling. This work shows that engineering the AMR at the single atom level is feasible.

pH-triggered conduction of amine-functionalized single ZnO wire integrated on a customized nanogap electronic platform

PubMed Central

2014-01-01

The electrical conductance response of single ZnO microwire functionalized with amine-groups was tested upon an acid pH variation of a solution environment after integration on a customized gold electrode array chip. ZnO microwires were easily synthesized by hydrothermal route and chemically functionalized with aminopropyl groups. Single wires were deposited from the solution and then oriented through dielectrophoresis across eight nanogap gold electrodes on a platform single chip. Therefore, eight functionalized ZnO microwire-gold junctions were formed at the same time, and being integrated on an ad hoc electronic platform, they were ready for testing without any further treatment. Experimental and simulation studies confirmed the high pH-responsive behavior of the amine-modified ZnO-gold junctions, obtaining in a simple and reproducible way a ready-to-use device for pH detection in the acidic range. We also compared this performance to bare ZnO wires on the same electronic platform, showing the superiority in pH response of the amine-functionalized material. PMID:24484615

Raman Scattering at Plasmonic Junctions Shorted by Conductive Molecular Bridges

DOE Office of Scientific and Technical Information (OSTI.GOV)

El-Khoury, Patrick Z.; Hu, Dehong; Apkarian, V. Ara

2013-04-10

Intensity spikes in Raman scattering, accompanied by switching between line spectra and band spectra, can be assigned to shorting the junction plasmon through molecular conductive bridges. This is demonstrated through Raman trajectories recorded at a plasmonic junction formed by a gold AFM tip in contact with a silver surface coated either with biphenyl-4,4’-dithiol or biphenyl-4-thiol. The fluctuations are absent in the monothiol. In effect, the making and breaking of chemical bonds is tracked.

Transistor-like behavior of single metalloprotein junctions.

PubMed

Artés, Juan M; Díez-Pérez, Ismael; Gorostiza, Pau

2012-06-13

Single protein junctions consisting of azurin bridged between a gold substrate and the probe of an electrochemical tunneling microscope (ECSTM) have been obtained by two independent methods that allowed statistical analysis over a large number of measured junctions. Conductance measurements yield (7.3 ± 1.5) × 10(-6)G(0) in agreement with reported estimates using other techniques. Redox gating of the protein with an on/off ratio of 20 was demonstrated and constitutes a proof-of-principle of a single redox protein field-effect transistor.

Effects of the molecule-electrode interface on the low-bias conductance of Cu–H{sub 2}–Cu single-molecule junctions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jiang, Zhuoling; Centre for Nanoscale Science and Technology, Academy for Advanced Interdisciplinary Studies, Peking University, Beijing 100871; Wang, Hao

The atomic structure and electronic transport properties of a single hydrogen molecule connected to both symmetric and asymmetric Cu electrodes are investigated by using the non-equilibrium Green’s function formalism combined with the density functional theory. Our calculations show that in symmetric Cu–H{sub 2}–Cu junctions, the low-bias conductance drops rapidly upon stretching, while asymmetric ones present a low-bias conductance spanning the 0.2–0.3 G{sub 0} interval for a wide range of electrode separations. This is in good agreement with experiments on Cu atomic contacts in a hydrogen environment. Furthermore, the distribution of the calculated vibrational energies of the two hydrogen atoms inmore » the asymmetric Cu–H{sub 2}–Cu junction is also consistent with experiments. These findings provide clear evidence for the formation of asymmetric Cu–H{sub 2}–Cu molecular junctions in breaking Cu atomic contacts in the presence of hydrogen and are also helpful for the design of molecular devices with Cu electrodes.« less

Dynamic formation of single-atom catalytic active sites on ceria-supported gold nanoparticles

PubMed Central

Wang, Yang-Gang; Mei, Donghai; Glezakou, Vassiliki-Alexandra; Li, Jun; Rousseau, Roger

2015-01-01

Catalysis by gold supported on reducible oxides has been extensively studied, yet issues such as the nature of the catalytic site and the role of the reducible support remain fiercely debated topics. Here we present ab initio molecular dynamics simulations of an unprecedented dynamic single-atom catalytic mechanism for the oxidation of carbon monoxide by ceria-supported gold clusters. The reported dynamic single-atom catalytic mechanism results from the ability of the gold cation to strongly couple with the redox properties of the ceria in a synergistic manner, thereby lowering the energy of redox reactions. The gold cation can break away from the gold nanoparticle to catalyse carbon monoxide oxidation, adjacent to the metal/oxide interface and subsequently reintegrate back into the nanoparticle after the reaction is completed. Our study highlights the importance of the dynamic creation of active sites under reaction conditions and their essential role in catalysis. PMID:25735407

Quantum sized gold nanoclusters with atomic precision.

PubMed

Qian, Huifeng; Zhu, Manzhou; Wu, Zhikun; Jin, Rongchao

2012-09-18

Gold nanoparticles typically have a metallic core, and the electronic conduction band consists of quasicontinuous energy levels (i.e. spacing δ ≪ k(B)T, where k(B)T is the thermal energy at temperature T (typically room temperature) and k(B) is the Boltzmann constant). Electrons in the conduction band roam throughout the metal core, and light can collectively excite these electrons to give rise to plasmonic responses. This plasmon resonance accounts for the beautiful ruby-red color of colloidal gold first observed by Faraday back in 1857. On the other hand, when gold nanoparticles become extremely small (<2 nm in diameter), significant quantization occurs to the conduction band. These quantum-sized nanoparticles constitute a new class of nanomaterial and have received much attention in recent years. To differentiate quantum-sized nanoparticles from conventional plasmonic gold nanoparticles, researchers often refer to the ultrasmall nanoparticles as nanoclusters. In this Account, we chose several typical sizes of gold nanoclusters, including Au(25)(SR)(18), Au(38)(SR)(24), Au(102)(SR)(44), and Au(144)(SR)(60), to illustrate the novel properties of metal nanoclusters imparted by quantum size effects. In the nanocluster size regime, many of the physical and chemical properties of gold nanoparticles are fundamentally altered. Gold nanoclusters have discrete electronic energy levels as opposed to the continuous band in plasmonic nanoparticles. Quantum-sized nanoparticles also show multiple optical absorption peaks in the optical spectrum versus a single surface plasmon resonance (SPR) peak at 520 nm for spherical gold nanocrystals. Although larger nanocrystals show an fcc structure, nanoclusters often have non-fcc atomic packing structures. Nanoclusters also have unique fluorescent, chiral, and magnetic properties. Due to the strong quantum confinement effect, adding or removing one gold atom significantly changes the structure and the electronic and optical properties of the nanocluster. Therefore, precise atomic control of nanoclusters is critically important: the nanometer precision typical of conventional nanoparticles is not sufficient. Atomically precise nanoclusters are represented by molecular formulas (e.g. Au(n)(SR)(m) for thiolate-protected ones, where n and m denote the respective number of gold atoms and ligands). Recently, major advances in the synthesis and structural characterization of molecular purity gold nanoclusters have made in-depth investigations of the size evolution of metal nanoclusters possible. Metal nanoclusters lie in the intermediate regime between localized atomic states and delocalized band structure in terms of electronic properties. We anticipate that future research on quantum-sized nanoclusters will stimulate broad scientific and technological interests in this special type of metal nanomaterial.

Crystallographic analysis of the solid-state dewetting of polycrystalline gold film using automated indexing in a transmission electron microscope

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jang, S. A.; Lee, H. J.; Oh, Y. J., E-mail: yjoh@hanbat.ac.kr

We analyzed the effect of crystallographic anisotropy on the morphological evolution of a 12-nm-thick gold film during solid-state dewetting at high temperatures using automated indexing tool in a transmission electron microscopy. Dewetting initiated at grain-boundary triple junctions adjacent to large grains resulting from abnormal grain growth driven by (111) texture development. Voids at the junctions developed shapes with faceted edges bounded by low-index crystal planes. The kinetic mobility of the edges varied with the crystal orientation normal to the edges, with a predominance of specific edges with the slowest retraction rates as the annealing time was increased.

Holliday Junction Thermodynamics and Structure: Coarse-Grained Simulations and Experiments

NASA Astrophysics Data System (ADS)

Wang, Wujie; Nocka, Laura M.; Wiemann, Brianne Z.; Hinckley, Daniel M.; Mukerji, Ishita; Starr, Francis W.

2016-03-01

Holliday junctions play a central role in genetic recombination, DNA repair and other cellular processes. We combine simulations and experiments to evaluate the ability of the 3SPN.2 model, a coarse-grained representation designed to mimic B-DNA, to predict the properties of DNA Holliday junctions. The model reproduces many experimentally determined aspects of junction structure and stability, including the temperature dependence of melting on salt concentration, the bias between open and stacked conformations, the relative populations of conformers at high salt concentration, and the inter-duplex angle (IDA) between arms. We also obtain a close correspondence between the junction structure evaluated by all-atom and coarse-grained simulations. We predict that, for salt concentrations at physiological and higher levels, the populations of the stacked conformers are independent of salt concentration, and directly observe proposed tetrahedral intermediate sub-states implicated in conformational transitions. Our findings demonstrate that the 3SPN.2 model captures junction properties that are inaccessible to all-atom studies, opening the possibility to simulate complex aspects of junction behavior.

Fabrication and characterization of magnetically tunable metal-semiconductor schottky diode using barium hexaferrite thin film on gold

NASA Astrophysics Data System (ADS)

Kaur, Jotinder; Sharma, Vinay; Sharma, Vipul; Veerakumar, V.; Kuanr, Bijoy K.

2016-05-01

Barium Hexaferrite (BaM) is an extensively studied magnetic material due to its potential device application. In this paper, we study Schottky junction diodes fabricated using gold and BaM and demonstrate the function of a spintronic device. Gold (50 nm)/silicon substrate was used to grow the BaM thin films (100-150 nm) using pulsed laser deposition. I-V characteristics were measured on the Au/BaM structure sweeping the voltage from ±5 volts. The forward and reverse bias current-voltage curves show diode like rectifying characteristics. The threshold voltage decreases while the output current increases with increase in the applied external magnetic field showing that the I-V characteristics of the BaM based Schottky junction diodes can be tuned by external magnetic field. It is also demonstrated that, the fabricated Schottky diode can be used as a half-wave rectifier, which could operate at high frequencies in the range of 1 MHz compared to the regular p-n junction diodes, which rectify below 10 kHz. In addition, it is found that above 1 MHz, Au/BaM diode can work as a rectifier as well as a capacitor filter, making the average (dc) voltage much larger.

Vertical versus Lateral Two-Dimensional Heterostructures: On the Topic of Atomically Abrupt p/n-Junctions.

PubMed

Zhou, Ruiping; Ostwal, Vaibhav; Appenzeller, Joerg

2017-08-09

The key appeal of two-dimensional (2D) materials such as graphene, transition metal dichalcogenides (TMDs), or phosphorene for electronic applications certainly lies in their atomically thin nature that offers opportunities for devices beyond conventional transistors. It is also this property that makes them naturally suited for a type of integration that is not possible with any three-dimensional (3D) material, that is, forming heterostructures by stacking dissimilar 2D materials together. Recently, a number of research groups have reported on the formation of atomically sharp p/n-junctions in various 2D heterostructures that show strong diode-type rectification. In this article, we will show that truly vertical heterostructures do exhibit much smaller rectification ratios and that the reported results on atomically sharp p/n-junctions can be readily understood within the framework of the gate and drain voltage response of Schottky barriers that are involved in the lateral transport.

Living Colloidal Metal Particles from Solvated Metal Atoms. Clustering of Metal Atoms in Organic Media 15.

DTIC Science & Technology

1986-09-23

alchemists , and over the centuries great medicinal powers were ascribed to gold. And as early as 300 A.D. there are references to the 2 consumption of...gold fluid to prolong life. It is doubtful that this was a colloidal solution of gold since aqua regia 3 was unknown to early Chinese alchemists , and

Antenna-coupled photon emission from hexagonal boron nitride tunnel junctions.

PubMed

Parzefall, M; Bharadwaj, P; Jain, A; Taniguchi, T; Watanabe, K; Novotny, L

2015-12-01

The ultrafast conversion of electrical signals to optical signals at the nanoscale is of fundamental interest for data processing, telecommunication and optical interconnects. However, the modulation bandwidths of semiconductor light-emitting diodes are limited by the spontaneous recombination rate of electron-hole pairs, and the footprint of electrically driven ultrafast lasers is too large for practical on-chip integration. A metal-insulator-metal tunnel junction approaches the ultimate size limit of electronic devices and its operating speed is fundamentally limited only by the tunnelling time. Here, we study the conversion of electrons (localized in vertical gold-hexagonal boron nitride-gold tunnel junctions) to free-space photons, mediated by resonant slot antennas. Optical antennas efficiently bridge the size mismatch between nanoscale volumes and far-field radiation and strongly enhance the electron-photon conversion efficiency. We achieve polarized, directional and resonantly enhanced light emission from inelastic electron tunnelling and establish a novel platform for studying the interaction of electrons with strongly localized electromagnetic fields.

Charge-Dependent Atomic-Scale Structures of High-Index and (110) Gold Electrode Surfaces as Revealed by Scanning Tunneling Microscopy

DTIC Science & Technology

1994-02-01

known gold atomic diameter of 2.89 A. Within a given domain, featuring adjacent terrace strings separated by monoatomic steps, the measured unit-cell...to utilize high-index gold faces in exploring the influence of monoatomic steps and related structural features on surface electrochemical phenomena...110) Gold Electrode Surfaces D1 T IC as Revealed by Scanning Tunneling Microscopy FLECTE MAR 10 19941 by E Xiaoping Gao, Gregory J. Edens, Antoinette

Determination of gold in copper-bearing sulphide ores and metallurgical flotation products by atomic-absorption spectrometry.

PubMed

Strong, B; Murray-Smith, R

1974-12-01

A method is described which is specific for the determination of gold in sulphide copper ores and concentrates. Direct decomposition with aqua regia was found to be incomplete. A carefully controlled roasting stage followed by treatment with hydrochloric acid and then aqua regia was effective for dissolving all the gold. The gold is extracted into 4-methylpentan-2-one (methyli-sobutylketone) then aspirated into a very lean air-acetylene flame and the gold determined by atomic-absorption spectrometry. No interferences were observed from large concentrations of copper, iron or nickel.

Shaping the Atomic-Scale Geometries of Electrodes to Control Optical and Electrical Performance of Molecular Devices.

PubMed

Zhao, Zhikai; Liu, Ran; Mayer, Dirk; Coppola, Maristella; Sun, Lu; Kim, Youngsang; Wang, Chuankui; Ni, Lifa; Chen, Xing; Wang, Maoning; Li, Zongliang; Lee, Takhee; Xiang, Dong

2018-04-01

A straightforward method to generate both atomic-scale sharp and atomic-scale planar electrodes is reported. The atomic-scale sharp electrodes are generated by precisely stretching a suspended nanowire, while the atomic-scale planar electrodes are obtained via mechanically controllable interelectrodes compression followed by a thermal-driven atom migration process. Notably, the gap size between the electrodes can be precisely controlled at subangstrom accuracy with this method. These two types of electrodes are subsequently employed to investigate the properties of single molecular junctions. It is found, for the first time, that the conductance of the amine-linked molecular junctions can be enhanced ≈50% as the atomic-scale sharp electrodes are used. However, the atomic-scale planar electrodes show great advantages to enhance the sensitivity of Raman scattering upon the variation of nanogap size. The underlying mechanisms for these two interesting observations are clarified with the help of density functional theory calculation and finite-element method simulation. These findings not only provide a strategy to control the electron transport through the molecule junction, but also pave a way to modulate the optical response as well as to improve the stability of single molecular devices via the rational design of electrodes geometries. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Unimolecular Logic Gate with Classical Input by Single Gold Atoms.

PubMed

Skidin, Dmitry; Faizy, Omid; Krüger, Justus; Eisenhut, Frank; Jancarik, Andrej; Nguyen, Khanh-Hung; Cuniberti, Gianaurelio; Gourdon, Andre; Moresco, Francesca; Joachim, Christian

2018-02-27

By a combination of solution and on-surface chemistry, we synthesized an asymmetric starphene molecule with two long anthracenyl input branches and a short naphthyl output branch on the Au(111) surface. Starting from this molecule, we could demonstrate the working principle of a single molecule NAND logic gate by selectively contacting single gold atoms by atomic manipulation to the longer branches of the molecule. The logical input "1" ("0") is defined by the interaction (noninteraction) of a gold atom with one of the input branches. The output is measured by scanning tunneling spectroscopy following the shift in energy of the electronic tunneling resonances at the end of the short branch of the molecule.

Gold in natural water: A method of determination by solvent extraction and electrothermal atomization

USGS Publications Warehouse

McHugh, J.B.

1984-01-01

A method has been developed using electrothermal atomization to effectively determine the amount of gold in natural water within the nanogram range. The method has four basic steps: (1) evaporating a 1-L sample; (2) putting it in hydrobromic acid-bromine solution; (3) extracting the sample with methyl-isobutyl-ketone; and (4) determining the amount of gold using an atomic absorption spectrophotometer. The limit of detection is 0.001 ??g gold per liter. Results from three studies indicate, respectively, that the method is precise, effective, and free of interference. Specifically, a precision study indicates that the method has a relative standard deviation of 16-18%; a recovery study indicates that the method recovers gold at an average of 93%; and an interference study indicates that the interference effects are eliminated with solvent extraction and background correction techniques. Application of the method to water samples collected from 41 sites throughout the Western United States and Alaska shows a gold concentration range of < 0.001 to 0.036 ??g gold per liter, with an average of 0.005 ??g/L. ?? 1984.

Bottom-up formation of robust gold carbide

PubMed Central

Westenfelder, Benedikt; Biskupek, Johannes; Meyer, Jannik C.; Kurasch, Simon; Lin, Xiaohang; Scholz, Ferdinand; Gross, Axel; Kaiser, Ute

2015-01-01

A new phenomenon of structural reorganization is discovered and characterized for a gold-carbon system by in-situ atomic-resolution imaging at temperatures up to 1300 K. Here, a graphene sheet serves in three ways, as a quasi transparent substrate for aberration-corrected high-resolution transmission electron microscopy, as an in-situ heater, and as carbon supplier. The sheet has been decorated with gold nanoislands beforehand. During electron irradiation at 80 kV and at elevated temperatures, the accumulation of gold atoms has been observed on defective graphene sites or edges as well as at the facets of gold nanocrystals. Both resulted in clustering, forming unusual crystalline structures. Their lattice parameters and surface termination differ significantly from standard gold nanocrystals. The experimental data, supported by electron energy loss spectroscopy and density-functional theory calculations, suggests that isolated gold and carbon atoms form – under conditions of heat and electron irradiation – a novel type of compound crystal, Au-C in zincblende structure. The novel material is metastable, but surprisingly robust, even under annealing condition. PMID:25772348

Thermoelectric generator with hinged assembly for fins

DOEpatents

Purdy, David L.; Shapiro, Zalman M.; Hursen, Thomas F.; Maurer, Gerould W.

1976-11-02

A cylindrical casing has a central shielded capsule of radioisotope fuel. A plurality of thermonuclear modules are axially arranged with their hot junctions resiliently pressed toward the shield and with their cold junctions adjacent a transition member having fins radiating heat to the environment. For each module, the assembly of transition member and fins is hinged to the casing for swinging to permit access to and removal of such module. A ceramic plate having gold layers on opposite faces prevents diffusion bonding of the hot junction to the shield.

Real-Time Plasmonic Monitoring of Single Gold Amalgam Nanoalloy Electrochemical Formation and Stripping.

PubMed

Wang, Jun-Gang; Fossey, John S; Li, Meng; Xie, Tao; Long, Yi-Tao

2016-03-01

Direct electrodeposition of mercury onto gold nanorods on an ITO substrate, without reducing agents, is reported. The growth of single gold amalgam nanoalloy particles and subsequent stripping was monitored in real-time monitoring by plasmonic effects and single-nanoparticle dark-field spectroelectrochemistry techniques. Time-dependent scattering spectral information conferred insight into the growth and stripping mechanism of a single nanoalloy particle. Four critical stages were observed: First, rapid deposition of Hg atoms onto Au nanorods; second, slow diffusion of Hg atoms into Au nanorods; third, prompt stripping of Hg atoms from Au nanorods; fourth, moderate diffusion from the inner core of Au nanorods. Under high Hg(2+) concentrations, homogeneous spherical gold amalgam nanoalloys were obtained. These results demonstrate that the morphology and composition of individual gold amalgam nanoalloys can be precisely regulated electrochemically. Moreover, gold amalgam nanoalloys with intriguing optical properties, such as modulated plasmonic lifetimes and quality factor Q, could be obtained. This may offer opportunities to extend applications in photovoltaic energy conversion and chemical sensing.

Alternative types of molecule-decorated atomic chains in Au–CO–Au single-molecule junctions

PubMed Central

Balogh, Zoltán; Makk, Péter

2015-01-01

Summary We investigate the formation and evolution of Au–CO single-molecule break junctions. The conductance histogram exhibits two distinct molecular configurations, which are further investigated by a combined statistical analysis. According to conditional histogram and correlation analysis these molecular configurations show strong anticorrelations with each other and with pure Au monoatomic junctions and atomic chains. We identify molecular precursor configurations with somewhat higher conductance, which are formed prior to single-molecule junctions. According to detailed length analysis two distinct types of molecule-affected chain-formation processes are observed, and we compare these results to former theoretical calculations considering bridge- and atop-type molecular configurations where the latter has reduced conductance due to destructive Fano interference. PMID:26199840

Alternative types of molecule-decorated atomic chains in Au-CO-Au single-molecule junctions.

PubMed

Balogh, Zoltán; Makk, Péter; Halbritter, András

2015-01-01

We investigate the formation and evolution of Au-CO single-molecule break junctions. The conductance histogram exhibits two distinct molecular configurations, which are further investigated by a combined statistical analysis. According to conditional histogram and correlation analysis these molecular configurations show strong anticorrelations with each other and with pure Au monoatomic junctions and atomic chains. We identify molecular precursor configurations with somewhat higher conductance, which are formed prior to single-molecule junctions. According to detailed length analysis two distinct types of molecule-affected chain-formation processes are observed, and we compare these results to former theoretical calculations considering bridge- and atop-type molecular configurations where the latter has reduced conductance due to destructive Fano interference.

Atom-scale compositional distribution in InAlAsSb-based triple junction solar cells by atom probe tomography.

PubMed

Hernández-Saz, J; Herrera, M; Delgado, F J; Duguay, S; Philippe, T; Gonzalez, M; Abell, J; Walters, R J; Molina, S I

2016-07-29

The analysis by atom probe tomography (APT) of InAlAsSb layers with applications in triple junction solar cells (TJSCs) has shown the existence of In- and Sb-rich regions in the material. The composition variation found is not evident from the direct observation of the 3D atomic distribution and because of this a statistical analysis has been required. From previous analysis of these samples, it is shown that the small compositional fluctuations determined have a strong effect on the optical properties of the material and ultimately on the performance of TJSCs.

Determining gold in water by anion-exchange batch extraction

USGS Publications Warehouse

McHugh, J.B.

1986-01-01

This paper describes a batch procedure for determining gold in natural waters. It is completely adaptable to field operations. The water samples are filtered and acidified before they are equilibrated with an anion-exchange resin by shaking. The gold is then eluted with acetone-nitric acid solution, and the eluate evaporated to dryness. The residue is taken up in hydrobromic acid-bromine solution and the gold is extracted with methyl isobutyl ketone. The extract is electrothermally atomized in an atomic-absorption spectrophotometer. The limit of determination is 1 ng 1. ?? 1986.

Ultrafast, 2 min synthesis of monolayer-protected gold nanoclusters (d < 2 nm)

NASA Astrophysics Data System (ADS)

Martin, Matthew N.; Li, Dawei; Dass, Amala; Eah, Sang-Kee

2012-06-01

An ultrafast synthesis method is presented for hexanethiolate-coated gold nanoclusters (d < 2 nm, <250 atoms per nanocluster), which takes only 2 min and can be easily reproduced. With two immiscible solvents, gold nanoclusters are separated from the reaction byproducts fast and easily without any need for post-synthesis cleaning.An ultrafast synthesis method is presented for hexanethiolate-coated gold nanoclusters (d < 2 nm, <250 atoms per nanocluster), which takes only 2 min and can be easily reproduced. With two immiscible solvents, gold nanoclusters are separated from the reaction byproducts fast and easily without any need for post-synthesis cleaning. Electronic supplementary information (ESI) available: Experimental details of gold nanocluster synthesis and mass-spectrometry. See DOI: 10.1039/c2nr30890h

Thermal depinning of a single superconducting vortex

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sok, Junghyun

1995-06-19

Thermal depinning has been studied for a single vortex trapped in a superconducting thin film in order to determine the value of the superconducting order parameter and the superfluid density when the vortex depins and starts to move around the film. For the Pb film in Pb/Al/Al 2O 3/PbBi junction having a gold line, the vortex depins from the artificial pinning site (Au line) and reproducibly moves through the same sequence of other pinning sites before it leaves the junction area of the Pb film. Values of the normalized order parameter Δ/Δ ° vary from Δ/Δ °=0.20 at the firstmore » motion of the vortex to Δ/Δ °=0.16 where the vortex finally leaves the junction. Equivalently, the value of the normalized superfluid density changes from 4% to 2.5% for this sample in this same temperature interval. For the Nb film in Nb/Al/Al 2O 3/Nb junction, thermal depinning occurs when the value of Δ/Δ ° is approximately 0.22 and the value of ρ s/ρ so is approximately 5%. These values are about 20% larger than those of a Pb sample having a gold line, but the values are really very close. For the Nb sample, grain boundaries are important pinning sites whereas, for the Pb sample with a gold line, pinning may have been dominated by an array Pb 3AU precipitates. Because roughly the same answer was obtained for these rather different kinds of pinning site, there is a reasonable chance that this is a general value within factors of 2 for a wide range of materials.« less

Adsorbed states of chlorophenol on Cu(110) and controlled switching of single-molecule junctions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Okuyama, H., E-mail: hokuyama@kuchem.kyoto-u.ac.jp; Kitaguchi, Y.; Hattori, T.

A molecular junction of substituted benzene (chlorophenol) is fabricated and controlled by using a scanning tunneling microscope (STM). Prior to the junction formation, the bonding geometry of the molecule on the surface is characterized by STM and electron energy loss spectroscopy (EELS). EELS shows that the OH group of chlorophenol is dissociated on Cu(110) and that the molecule is bonded nearly flat to the surface via an O atom, with the Cl group intact. We demonstrate controlled contact of an STM tip to the “available” Cl group and lift-up of the molecule while it is anchored to the surface viamore » an O atom. The asymmetric bonding motifs of the molecule to the electrodes allow for reversible control of the junction.« less

NORTH ELEVATION OF GOLD HILL MILL, LOOKING SOUTH. AT LEFT ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

NORTH ELEVATION OF GOLD HILL MILL, LOOKING SOUTH. AT LEFT EDGE IS THE SINGLE CYLINDER “HOT SHOT” ENGINE THAT PROVIDED POWER FOR THE MILL. JUST IN FRONT OF IT IS AN ARRASTRA. AT CENTER IS THE BALL MILL AND SECONDARY ORE BIN. JUST TO THE RIGHT OF THE BALL MILL IS A RAKE CLASSIFIER, AND TO THE RIGHT ARE THE CONCENTRATION TABLES. WARM SPRINGS CAMP IS IN THE DISTANCE. SEE CA-292-4 FOR IDENTICAL B&W NEGATIVE. - Gold Hill Mill, Warm Spring Canyon Road, Death Valley Junction, Inyo County, CA

NORTH ELEVATION OF GOLD HILL MILL, LOOKING SOUTH. AT LEFT ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

NORTH ELEVATION OF GOLD HILL MILL, LOOKING SOUTH. AT LEFT EDGE IS THE SINGLE CYLINDER “HOT SHOT” ENGINE THAT PROVIDED POWER FOR THE MILL. JUST IN FRONT OF IT IS AN ARRASTRA. AT CENTER IS THE BALL MILL AND SECONDARY ORE BIN. JUST TO THE RIGHT OF THE BALL MILL IS A RAKE CLASSIFIER, AND TO THE RIGHT ARE THE CONCENTRATION TABLES. WARM SPRINGS CAMP IS IN THE DISTANCE. SEE CA-292-17 (CT) FOR IDENTICAL COLOR TRANSPARENCY. - Gold Hill Mill, Warm Spring Canyon Road, Death Valley Junction, Inyo County, CA

Effects of dissolucytotic gold ions on recovering brain lesions.

PubMed

Danscher, Gorm; Larsen, Agnete

2010-04-01

Recent experimental research has shown that metallic gold releases charged gold atoms when placed intracerebrally and that the liberated gold ions affect inflammation in the brain. The observations suggest that metallic gold can be used as a safe suppressor of inflammation in the central nervous system.

Interaction of Chemical Agents with Nanoscale Molecular Junctions

DTIC Science & Technology

2011-08-01

thiS burden to Department of Defense. Washilgton Headqualters Services. Directorate for lnformatie~n Operations and Reports (07()4.()188), 1215...The source of these contaminants were determined to be coming from the glovebox auxiliary vacuum pump, which normally operates continuously for...SAM- NHi NH2-SAM-Gold] molecular junction for analysis. In order to perform electron transport analysis of our nanoscale devices in a "real world

DETERMINATION OF TOTAL MERCURY IN FISH TISSUES USING PYROLYSIS ATOMIC ABSORPTION SPECTROMETRY WITH GOLD AMALGAMATION

EPA Science Inventory

A simple and rapid procedure for measuring total mercury in fish tissues is evaluated and
compared with conventional techniques. Using an automated instrument incorporating combustion, preconcentration by amalgamation with gold, and atomic absorption spectrometry (AAS), mill...

Electron transport in stretched monoatomic gold wires.

PubMed

Grigoriev, A; Skorodumova, N V; Simak, S I; Wendin, G; Johansson, B; Ahuja, R

2006-12-08

The conductance of monoatomic gold wires containing 3-7 gold atoms has been obtained from ab initio calculations. The transmission is found to vary significantly depending on the wire stretching and the number of incorporated atoms. Such oscillations are determined by the electronic structure of the one-dimensional (1D) part of the wire between the contacts. Our results indicate that the conductivity of 1D wires can be suppressed without breaking the contact.

High temperature superconductor step-edge Josephson junctions using Ti-Ca-Ba-Cu-O

DOEpatents

Ginley, David S.; Hietala, Vincent M.; Hohenwarter, Gert K. G.; Martens, Jon S.; Plut, Thomas A.; Tigges, Chris P.; Vawter, Gregory A.; Zipperian, Thomas E.

1994-10-25

A process for formulating non-hysteretic and hysteretic Josephson junctions using HTS materials which results in junctions having the ability to operate at high temperatures while maintaining high uniformity and quality. The non-hysteretic Josephson junction is formed by step-etching a LaAlO.sub.3 crystal substrate and then depositing a thin film of TlCaBaCuO on the substrate, covering the step, and forming a grain boundary at the step and a subsequent Josephson junction. Once the non-hysteretic junction is formed the next step to form the hysteretic Josephson junction is to add capacitance to the system. In the current embodiment, this is accomplished by adding a thin dielectric layer, LaA1O.sub.3, followed by a cap layer of a normal metal where the cap layer is formed by first depositing a thin layer of titanium (Ti) followed by a layer of gold (Au). The dielectric layer and the normal metal cap are patterned to the desired geometry.

An atomic-absorption method for the determination of gold in large samples of geologic materials

USGS Publications Warehouse

VanSickle, Gordon H.; Lakin, Hubert William

1968-01-01

A laboratory method for the determination of gold in large (100-gram) samples has been developed for use in the study of the gold content of placer deposits and of trace amounts of gold in other geologic materials. In this method the sample is digested with bromine and ethyl ether, the gold is extracted into methyl isobutyl ketone, and the determination is made by atomicabsorption spectrophotometry. The lower limit of detection is 0.005 part per million in the sample. The few data obtained so far by this method agree favorably with those obtained by assay and by other atomic-absorption methods. About 25 determinations can be made per man-day.

UV and visible light photocatalytic activity of Au/TiO2 nanoforests with Anatase/Rutile phase junctions and controlled Au locations.

PubMed

Yu, Yang; Wen, Wei; Qian, Xin-Yue; Liu, Jia-Bin; Wu, Jin-Ming

2017-01-24

To magnify anatase/rutile phase junction effects through appropriate Au decorations, a facile solution-based approach was developed to synthesize Au/TiO 2 nanoforests with controlled Au locations. The nanoforests cons®isted of anatase nanowires surrounded by radially grown rutile branches, on which Au nanoparticles were deposited with preferred locations controlled by simply altering the order of the fabrication step. The Au-decoration increased the photocatalytic activity under the illumination of either UV or visible light, because of the beneficial effects of either electron trapping or localized surface plasmon resonance (LSPR). Gold nanoparticles located preferably at the interface of anatase/rutile led to a further enhanced photocatalytic activity. The appropriate distributions of Au nanoparticles magnify the beneficial effects arising from the anatase/rutile phase junctions when illuminated by UV light. Under the visible light illumination, the LSPR effect followed by the consecutive electron transfer explains the enhanced photocatalysis. This study provides a facile route to control locations of gold nanoparticles in one-dimensional nanostructured arrays of multiple-phases semiconductors for achieving a further increased photocatalytic activity.

Superluminescence from an optically pumped molecular tunneling junction by injection of plasmon induced hot electrons

PubMed Central

Braun, Kai; Wang, Xiao; Kern, Andreas M; Adler, Hilmar; Peisert, Heiko; Chassé, Thomas; Zhang, Dai

2015-01-01

Summary Here, we demonstrate a bias-driven superluminescent point light-source based on an optically pumped molecular junction (gold substrate/self-assembled molecular monolayer/gold tip) of a scanning tunneling microscope, operating at ambient conditions and providing almost three orders of magnitude higher electron-to-photon conversion efficiency than electroluminescence induced by inelastic tunneling without optical pumping. A positive, steadily increasing bias voltage induces a step-like rise of the Stokes shifted optical signal emitted from the junction. This emission is strongly attenuated by reversing the applied bias voltage. At high bias voltage, the emission intensity depends non-linearly on the optical pump power. The enhanced emission can be modelled by rate equations taking into account hole injection from the tip (anode) into the highest occupied orbital of the closest substrate-bound molecule (lower level) and radiative recombination with an electron from above the Fermi level (upper level), hence feeding photons back by stimulated emission resonant with the gap mode. The system reflects many essential features of a superluminescent light emitting diode. PMID:26171286

Superfluid-ferromagnet-superfluid junction and the {pi} phase in a superfluid Fermi gas

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kashimura, Takashi; Tsuchiya, Shunji; CREST

2010-09-15

We investigate the possibility of a superfluid-ferromagnet-superfluid (SFS) junction in a superfluid Fermi gas. To examine this possibility in a simple manner, we consider an attractive Hubbard model at T=0 within the mean-field theory. When a potential barrier is embedded in a superfluid Fermi gas with population imbalance (N{sub {up_arrow}}>N{sub {down_arrow}}, where N{sub {sigma}} is the number of atoms with pseudospin {sigma}= {up_arrow}, {down_arrow}), this barrier is shown to be magnetized in the sense that excess {up_arrow}-spin atoms are localized around it. The resulting superfluid Fermi gas is spatially divided into two by this ferromagnet, so that one obtains amore » junction similar to the superconductor-ferromagnet-superconductor junction discussed in superconductivity. Indeed, we show that the so-called {pi} phase, which is a typical phenomenon in the SFS junction, is realized, where the superfluid order parameter changes its sign across the junction. Our results would be useful for the study of magnetic effects on fermion superfluidity using an ultracold Fermi gas.« less

Role of out-of-plane dielectric thickness in the electrostatic simulation of atomically thin lateral junctions

NASA Astrophysics Data System (ADS)

Nipane, Ankur; Zhang, Yefei; Teherani, James T.

2018-06-01

Two-dimensional materials enable novel electronic and optoelectronic devices due to their unique properties. Device modeling plays a fundamental role in developing these novel devices by providing insights into the underlying physics. In this work, we present the dramatic impact of the simulated out-of-plane dielectric thickness on the electrostatics of lateral junctions formed from atomically thin materials. We show that unlike bulk junctions, the boundary conditions on the edges of the simulation region significantly affect the electrostatics of two-dimensional (2D) lateral junctions by modifying the out-of-plane electric field. We also present an intuitive understanding of the Neumann boundary conditions imposed on the boundaries of the simulation region. The Neumann boundary conditions alter the intended simulation by generating reflections of the device across the boundaries. Finally, we derive a minimal dielectric thickness for a symmetrically doped 2D lateral p-n junction, above which the out-of-plane simulation region boundaries minimally affect the simulated electric field, electrostatic potential, and depletion width of the junction.

Self-Assembled Monolayers of Dithiophosphinic Acids on Gold

NASA Astrophysics Data System (ADS)

San Juan, Ronan Roca

This dissertation reports the synthesis of derivatives of dithiophosphinic acids (R1R2DTPAs), and the formation and characterization of DTPA SAMs on gold to build a knowledge base on their nature of binding, organization of the alkyl chains and electrochemical barrier properties. The binding of DTPA molecules on gold depends on the morphology of the gold film: They bind in a mixed monodentate and bidentate modes on standard as-deposited (As-Dep) gold, while they fully chelate on smoother template-stripped (TS) gold. Chapter 2 focuses on van der Waals interactions of various alkyl chain lengths of symmetrical R2DTPA SAMs, which increase with increasing chain lengths similar to those of the analogous n-alkanethiol SAMs, but with alkyl chains that are generally less dense than those of n-alkanethiol SAMs. Chapter 3 addresses why the DTPA compounds do not chelate on the standard As-Dep gold by comparing (C16)2DTPA SAM to (C16 )2DDP SAM. Here, side chain crystallinity stabilizes DTPA SAM structure at the expense of chelation of the DTPA molecules, which leads to a mixture of bidentate and monodentate DTPA molecules, whereas the increased flexibility of the chains in DDP due to the oxygen atoms retains chelation of the DDP molecules. Chapter 4 focuses on the SAMs formed from RlongRshort DTPAs, which shows that the length of the short chain spacer affects SAM packing density and thickness. The SAMs of these molecules also show homogeneous mixing of Rlong and Rshort chains. Chapter 5 investigates PhRDTPA SAMs in preparation for molecular junction studies. The chelation of PhRDTPA molecules on TS gold allows the PhRDTPAs to act as molecular alligator clips. The length of the alkyl chains controls the density of the phenyl group and they fill in the voids between adsorbates to prevent electrical shorting. Finally, Chapter 6 incorporates OH tail group(s) to control the wettability of DTPA SAMs. The presence of OH groups in DTPAs forms hydrophilic SAMs. The symmetrical OH-terminated DTPA forms a SAM with similar packing density to that of an analogous CH3-terminated DTPA SAM, while the OH/CH 3-terminated DTPA forms a thin SAM with low molecular packing, however, the chains of this SAM are homogeneously mixed.

Probing Electrochemical Adsorbate Structure and Reactions with In-Situ Atomic-Resolution Scanning Microscopy: Some Progress and Prospects

DTIC Science & Technology

1992-10-01

organized into hexagonal patterns, but unlike the monoatomic iodine adlayers noted above the close-packed atomic strings tend to lie along the gold ...adsorbate systems. Illustrative results of the former type are presented for the potential-dependent adsorption of iodide at low-index gold electrodes. The...presented for the potential-dependent adsorption of iodide at low-index gold electrodes. The virtues of acquiring "composite-domain" STM images, where

Enhanced Mechanical Stability of Gold Nanotips through Carbon Nanocone Encapsulation

PubMed Central

Cano-Marquez, Abraham G.; Schmidt, Wesller G.; Ribeiro-Soares, Jenaina; Gustavo Cançado, Luiz; Rodrigues, Wagner N.; Santos, Adelina P.; Furtado, Clascidia A.; Autreto, Pedro A.S.; Paupitz, Ricardo; Galvão, Douglas S.; Jorio, Ado

2015-01-01

Gold is a noble metal that, in comparison with silver and copper, has the advantage of corrosion resistance. Despite its high conductivity, chemical stability and biocompatibility, gold exhibits high plasticity, which limits its applications in some nanodevices. Here, we report an experimental and theoretical study on how to attain enhanced mechanical stability of gold nanotips. The gold tips were fabricated by chemical etching and further encapsulated with carbon nanocones via nanomanipulation. Atomic force microscopy experiments were carried out to test their mechanical stability. Molecular dynamics simulations show that the encapsulated nanocone changes the strain release mechanisms at the nanoscale by blocking gold atomic sliding, redistributing the strain along the whole nanostructure. The carbon nanocones are conducting and can induce magnetism, thus opening new avenues on the exploitation of transport, mechanical and magnetic properties of gold covered by sp2 carbon at the nanoscale. PMID:26083864

Asymmetric angular dependence of spin-transfer torques in CoFe/Mg-B-O/CoFe magnetic tunnel junctions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tang, Ling, E-mail: lingtang@zjut.edu.cn; Xu, Zhi-Jun, E-mail: xzj@zjut.edu.cn; Zuo, Xian-Jun

Using a first-principles noncollinear wave-function-matching method, we studied the spin-transfer torques (STTs) in CoFe/Mg-B-O/CoFe(001) magnetic tunnel junctions (MTJs), where three different types of B-doped MgO in the spacer are considered, including B atoms replacing Mg atoms (Mg{sub 3}BO{sub 4}), B atoms replacing O atoms (Mg{sub 4}BO{sub 3}), and B atoms occupying interstitial positions (Mg{sub 4}BO{sub 4}) in MgO. A strong asymmetric angular dependence of STT can be obtained both in ballistic CoFe/Mg{sub 3}BO{sub 4} and CoFe/Mg{sub 4}BO{sub 4} based MTJs, whereas a nearly symmetric STT curve is observed in the junctions based on CoFe/Mg{sub 4}BO{sub 3}. Furthermore, the asymmetry ofmore » the angular dependence of STT can be suppressed significantly by the disorder of B distribution. Such skewness of STTs in the CoFe/Mg-B-O/CoFe MTJs could be attributed to the interfacial resonance states induced by the B diffusion into MgO spacer.« less

Electronic components embedded in a single graphene nanoribbon.

PubMed

Jacobse, P H; Kimouche, A; Gebraad, T; Ervasti, M M; Thijssen, J M; Liljeroth, P; Swart, I

2017-07-25

The use of graphene in electronic devices requires a band gap, which can be achieved by creating nanostructures such as graphene nanoribbons. A wide variety of atomically precise graphene nanoribbons can be prepared through on-surface synthesis, bringing the concept of graphene nanoribbon electronics closer to reality. For future applications it is beneficial to integrate contacts and more functionality directly into single ribbons by using heterostructures. Here, we use the on-surface synthesis approach to fabricate a metal-semiconductor junction and a tunnel barrier in a single graphene nanoribbon consisting of 5- and 7-atom wide segments. We characterize the atomic scale geometry and electronic structure by combined atomic force microscopy, scanning tunneling microscopy, and conductance measurements complemented by density functional theory and transport calculations. These junctions are relevant for developing contacts in all-graphene nanoribbon devices and creating diodes and transistors, and act as a first step toward complete electronic devices built into a single graphene nanoribbon.Adding functional electronic components to graphene nanoribbons requires precise control over their atomic structure. Here, the authors use a bottom-up approach to build a metal-semiconductor junction and a tunnel barrier directly into a single graphene nanoribbon, an exciting development for graphene-based electronic devices.

Atomic-Scale Control of Electron Transport through Single Molecules

NASA Astrophysics Data System (ADS)

Wang, Y. F.; Kröger, J.; Berndt, R.; Vázquez, H.; Brandbyge, M.; Paulsson, M.

2010-04-01

Tin-phthalocyanine molecules adsorbed on Ag(111) were contacted with the tip of a cryogenic scanning tunneling microscope. Orders-of-magnitude variations of the single-molecule junction conductance were achieved by controllably dehydrogenating the molecule and by modifying the atomic structure of the surface electrode. Nonequilibrium Green’s function calculations reproduce the trend of the conductance and visualize the current flow through the junction, which is guided through molecule-electrode chemical bonds.

Chemical control of electrical contact to sp² carbon atoms.

PubMed

Frederiksen, Thomas; Foti, Giuseppe; Scheurer, Fabrice; Speisser, Virginie; Schull, Guillaume

2014-04-16

Carbon-based nanostructures are attracting tremendous interest as components in ultrafast electronics and optoelectronics. The electrical interfaces to these structures play a crucial role for the electron transport, but the lack of control at the atomic scale can hamper device functionality and integration into operating circuitry. Here we study a prototype carbon-based molecular junction consisting of a single C60 molecule and probe how the electric current through the junction depends on the chemical nature of the foremost electrode atom in contact with the molecule. We find that the efficiency of charge injection to a C60 molecule varies substantially for the considered metallic species, and demonstrate that the relative strength of the metal-C bond can be extracted from our transport measurements. Our study further suggests that a single-C60 junction is a basic model to explore the properties of electrical contacts to meso- and macroscopic sp(2) carbon structures.

Chemical control of electrical contact to sp2 carbon atoms

NASA Astrophysics Data System (ADS)

Frederiksen, Thomas; Foti, Giuseppe; Scheurer, Fabrice; Speisser, Virginie; Schull, Guillaume

2014-04-01

Carbon-based nanostructures are attracting tremendous interest as components in ultrafast electronics and optoelectronics. The electrical interfaces to these structures play a crucial role for the electron transport, but the lack of control at the atomic scale can hamper device functionality and integration into operating circuitry. Here we study a prototype carbon-based molecular junction consisting of a single C60 molecule and probe how the electric current through the junction depends on the chemical nature of the foremost electrode atom in contact with the molecule. We find that the efficiency of charge injection to a C60 molecule varies substantially for the considered metallic species, and demonstrate that the relative strength of the metal-C bond can be extracted from our transport measurements. Our study further suggests that a single-C60 junction is a basic model to explore the properties of electrical contacts to meso- and macroscopic sp2 carbon structures.

Semiconductor quantum dot super-emitters: spontaneous emission enhancement combined with suppression of defect environment using metal-oxide plasmonic metafilms

NASA Astrophysics Data System (ADS)

Sadeghi, Seyed M.; Wing, Waylin J.; Gutha, Rithvik R.; Sharp, Christina

2018-01-01

We demonstrate that a metal-oxide plasmonic metafilm consisting of a Si/Al oxide junction in the vicinity of a thin gold layer can quarantine excitons in colloidal semiconductor quantum dots against their defect environments. This process happens while the plasmon fields of the gold layer enhance spontaneous emission decay rates of the quantum dots. We study the emission dynamics of such quantum dots when the distance between the Si/Al oxide junction and the gold thin layer is varied. The results show that for distances less than a critical value the lifetime of the quantum dots can be elongated while they experience intense plasmon fields. This suggests that the metal-oxide metafilm can keep photo-excited electrons in the cores of the quantum dots, suppressing their migration to the surface defect sites. This leads to suppression of Auger recombination, offering quantum dot super-emitters with emission that is enhanced not only by the plasmon fields (Purcell effect), but also by strong suppression of the non-radiative decay caused by the defect sites.

Atomic structure of water/Au, Ag, Cu and Pt atomic junctions.

PubMed

Li, Yu; Kaneko, Satoshi; Fujii, Shintaro; Nishino, Tomoaki; Kiguchi, Manabu

2017-02-08

Much progress has been made in understanding the transport properties of atomic-scale conductors. We prepared atomic-scale metal contacts of Cu, Ag, Au and Pt using a mechanically controllable break junction method at 10 K in a cryogenic vacuum. Water molecules were exposed to the metal atomic contacts and the effect of molecular adsorption was investigated by electronic conductance measurements. Statistical analysis of the electronic conductance showed that the water molecule(s) interacted with the surface of the inert Au contact and the reactive Cu ant Pt contacts, where molecular adsorption decreased the electronic conductance. A clear conductance signature of water adsorption was not apparent at the Ag contact. Detailed analysis of the conductance behaviour during a contact-stretching process indicated that metal atomic wires were formed for the Au and Pt contacts. The formation of an Au atomic wire consisting of low coordination number atoms leads to increased reactivity of the inert Au surface towards the adsorption of water.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Takai, Yoshizo; Kawasaki, Tadahiro; Kimura, Yoshihide

A single-atom-sized gold wire was successfully observed in real time by a newly developed defocus-image modulation processing electron microscope. Because of phase retrieval processing with spherical aberration correction, the single-atom strand wire was observed with high contrast and without contrast blurring. By carefully looking at the atomic distance, the contrast, and the dynamic behavior of the wire, we recognized that there are two stages of the wire. In the first stage the wire maintained the atomic distance in the bulk crystal, but in the second stage the wire showed the atomic distance of the nearest-neighbor atoms with weaker contrast. Themore » gold wire was rather stable for a few seconds under strong electron beam illumination.« less

Effect of gold nanoparticles on structure and dynamics of binary Lennard-Jones liquid: Wave-vector space analysis

NASA Astrophysics Data System (ADS)

Separdar, L.; Davatolhagh, S.

2016-12-01

Molecular dynamics simulations at constant (N , V , T) are used to study the mutual effects of gold nanoparticles on the structure and dynamics of Kob-Andersen binary Lennard-Jones (BLJ) liquid within the framework of mode coupling theory of dynamic glass transition in the reciprocal space. The results show the 'softening' effect of the gold nanoparticles on the liquid dynamics in terms of (i) reducing the mode coupling crossover temperature Tc with respect to that of the bulk BLJ (i.e. BLJ without nanoparticles), (ii) decreasing the time interval of β-relaxation, and (iii) decreasing the exponent γ characterizing the power-law behavior of the α-relaxation time. This softening effect is explained in terms of the van der Waals attraction between the gold atoms comprising the nanoparticle and the BLJ host atoms, such that adsorption of host atoms onto the nanoparticle surface creates more space or free-volume for the other atoms to diffuse. By the same token interactions of purely excluded-volume-type are expected to result in the opposite effect. It is also noted that, much unlike BLJ host particles, the dynamics of gold nanoparticles is much less dependent on the wave-vector and that it exhibits a nearly exponential behavior in the α-relaxation regime.

Excimer laser annealing: A gold process for CZ silicon junction formation

NASA Technical Reports Server (NTRS)

Wong, David C.; Bottenberg, William R.; Byron, Stanley; Alexander, Paul

1987-01-01

A cold process using an excimer laser for junction formation in silicon has been evaluated as a way to avoid problems associated with thermal diffusion. Conventional thermal diffusion can cause bulk precipitation of SiOx and SiC or fail to completely activate the dopant, leaving a degenerate layer at the surface. Experiments were conducted to determine the feasibility of fabricating high quality p-n junctions using a pulsed excimer laser for junction formation at remelt temperature with ion-implanted surfaces. Solar-cell efficiency exceeding 16 percent was obtained using Czochralski single-crystal silicon without benefit of back surface field or surface passivation. Characterization shows that the formation of uniform, shallow junctions (approximately 0.25 micron) by excimer laser scanning preserves the minority carrier lifetime that leads to high current collection. However, the process is sensitive to initial surface conditions and handling parameters that drive the cost up.

Graphene as a Promising Electrode for Low-Current Attenuation in Nonsymmetric Molecular Junctions.

PubMed

Zhang, Qian; Liu, Longlong; Tao, Shuhui; Wang, Congyi; Zhao, Cezhou; González, César; Dappe, Yannick J; Nichols, Richard J; Yang, Li

2016-10-12

We have measured the single-molecule conductance of 1,n-alkanedithiol molecular bridges (n = 4, 6, 8, 10, 12) on a graphene substrate using scanning tunneling microscopy (STM)-formed electrical junctions. The conductance values of this homologous series ranged from 2.3 nS (n = 12) to 53 nS (n = 4), with a decay constant β n of 0.40 per methylene (-CH 2 ) group. This result is explained by a combination of density functional theory (DFT) and Keldysh-Green function calculations. The obtained decay, which is much lower than the one obtained for symmetric gold junctions, is related to the weak coupling at the molecule-graphene interface and the electronic structure of graphene. As a consequence, we show that using graphene nonsymmetric junctions and appropriate anchoring groups may lead to a much-lower decay constant and more-conductive molecular junctions at longer lengths.

Structure and formation of highly luminescent protein-stabilized gold clusters† †Electronic supplementary information (ESI) available. See DOI: 10.1039/c7sc05086k

PubMed Central

Chevrier, D. M.; Thanthirige, V. D.; Luo, Z.; Driscoll, S.; Cho, P.; MacDonald, M. A.; Yao, Q.; Guda, R.; Xie, J.; Johnson, E. R.; Chatt, A.; Zheng, N.

2018-01-01

Highly luminescent gold clusters simultaneously synthesized and stabilized by protein molecules represent a remarkable category of nanoscale materials with promising applications in bionanotechnology as sensors. Nevertheless, the atomic structure and luminescence mechanism of these gold clusters are still unknown after several years of developments. Herein, we report findings on the structure, luminescence and biomolecular self-assembly of gold clusters stabilized by the large globular protein, bovine serum albumin. We highlight the surprising identification of interlocked gold-thiolate rings as the main gold structural unit. Importantly, such gold clusters are in a rigidified state within the protein scaffold, offering an explanation for their highly luminescent character. Combined free-standing cluster synthesis (without protecting protein scaffold) with rigidifying and un-rigidifying experiments, were designed to further verify the luminescence mechanism and gold atomic structure within the protein. Finally, the biomolecular self-assembly process of the protein-stabilized gold clusters was elucidated by time-dependent X-ray absorption spectroscopy measurements and density functional theory calculations. PMID:29732064

Thermo-electric modular structure and method of making same

DOEpatents

Freedman, N.S.; Horsting, C.W.; Lawrence, W.F.; Carrona, J.J.

1974-01-29

A method is presented for making a thermoelectric module wtth the aid of an insulating wafer having opposite metallized surfaces, a pair of similar equalizing sheets of metal, a hot-junction strap of metal, a thermoelectric element having hot- and cold-junction surfaces, and a radiator sheet of metal. The method comprises the following steps: brazing said equalizer sheets to said opposite metallized surfaces, respectively, of said insulating wafer with pure copper in a non-oxidizing ambient; brazing one surface of said hot-junction strap to one of the surfaces of said equalizing sheet with a nickel-gold alloy in a non- oxidizing ambient; and diffusion bonding said hot-junction surface of said thermoelectric element to the other surface of said hot-junction strap and said radiator sheet to said cold-junction surface of said thermoelectric element, said diffusion bonding being carried out in a non-oxidizing ambient, under compressive loading, at a temperature of about 550 deg C., and for about one-half hour. (Official Gazette)

Ion implantation of solar cell junctions without mass analysis

NASA Technical Reports Server (NTRS)

Fitzgerald, D.; Tonn, D. G.

1981-01-01

This paper is a summary of an investigation to determine the feasibility of producing solar cells by means of ion implantation without the use of mass analysis. Ion implants were performed using molecular and atomic phosphorus produced by the vaporization of solid red phosphorus and ionized in an electron bombardment source. Solar cell junctions were ion implanted by mass analysis of individual molecular species and by direct unanalyzed implants from the ion source. The implant dose ranged from 10 to the 14th to 10 to the 16th atoms/sq cm and the energy per implanted atom ranged from 5 KeV to 40 KeV in this study.

The mystery of gold's chemical activity: local bonding, morphology and reactivity of atomic oxygen.

PubMed

Baker, Thomas A; Liu, Xiaoying; Friend, Cynthia M

2011-01-07

Recently, gold has been intensely studied as a catalyst for key synthetic reactions. Gold is an attractive catalyst because, surprisingly, it is highly active and very selective for partial oxidation processes suggesting promise for energy-efficient "green" chemistry. The underlying origin of the high activity of Au is a controversial subject since metallic gold is commonly thought to be inert. Herein, we establish that one origin of the high activity for gold catalysis is the extremely reactive nature of atomic oxygen bound in 3-fold coordination sites on metallic gold. This is the predominant form of O at low concentrations on the surface, which is a strong indication that it is most relevant to catalytic conditions. Atomic oxygen bound to metallic Au in 3-fold sites has high activity for CO oxidation, oxidation of olefins, and oxidative transformations of alcohols and amines. Among the factors identified as important in Au-O interaction are the morphology of the surface, the local binding site of oxygen, and the degree of order of the oxygen overlayer. In this Perspective, we present an overview of both theory and experiments that identify the reactive forms of O and their associated charge density distributions and bond strengths. We also analyze and model the release of Au atoms induced by O binding to the surface. This rough surface also has the potential for O(2) dissociation, which is a critical step if Au is to be activated catalytically. We further show the strong parallels between product distributions and reactivity for O-covered Au at low pressure (ultrahigh vacuum) and for nanoporous Au catalysts operating at atmospheric pressure as evidence that atomic O is the active species under working catalytic conditions when metallic Au is present. We briefly discuss the possible contributions of oxidants that may contain intact O-O bonds and of the Au-metal oxide support interface in Au catalysis. Finally, the challenges and future directions for fully understanding the activity of gold are considered.

3D Band Diagram and Photoexcitation of 2D-3D Semiconductor Heterojunctions.

PubMed

Li, Bo; Shi, Gang; Lei, Sidong; He, Yongmin; Gao, Weilu; Gong, Yongji; Ye, Gonglan; Zhou, Wu; Keyshar, Kunttal; Hao, Ji; Dong, Pei; Ge, Liehui; Lou, Jun; Kono, Junichiro; Vajtai, Robert; Ajayan, Pulickel M

2015-09-09

The emergence of a rich variety of two-dimensional (2D) layered semiconductor materials has enabled the creation of atomically thin heterojunction devices. Junctions between atomically thin 2D layers and 3D bulk semiconductors can lead to junctions that are fundamentally electronically different from the covalently bonded conventional semiconductor junctions. Here we propose a new 3D band diagram for the heterojunction formed between n-type monolayer MoS2 and p-type Si, in which the conduction and valence band-edges of the MoS2 monolayer are drawn for both stacked and in-plane directions. This new band diagram helps visualize the flow of charge carriers inside the device in a 3D manner. Our detailed wavelength-dependent photocurrent measurements fully support the diagrams and unambiguously show that the band alignment is type I for this 2D-3D heterojunction. Photogenerated electron-hole pairs in the atomically thin monolayer are separated and driven by an external bias and control the "on/off" states of the junction photodetector device. Two photoresponse regimes with fast and slow relaxation are also revealed in time-resolved photocurrent measurements, suggesting the important role played by charge trap states.

Inelastic electron tunneling spectroscopy of difurylethene-based photochromic single-molecule junctions

PubMed Central

Sysoiev, Dmytro; Huhn, Thomas; Pauly, Fabian

2017-01-01

Diarylethene-derived molecules alter their electronic structure upon transformation between the open and closed forms of the diarylethene core, when exposed to ultraviolet (UV) or visible light. This transformation results in a significant variation of electrical conductance and vibrational properties of corresponding molecular junctions. We report here a combined experimental and theoretical analysis of charge transport through diarylethene-derived single-molecule devices, which are created using the mechanically controlled break-junction technique. Inelastic electron tunneling (IET) spectroscopy measurements performed at 4.2 K are compared with first-principles calculations in the two distinct forms of diarylethenes connected to gold electrodes. The combined approach clearly demonstrates that the IET spectra of single-molecule junctions show specific vibrational features that can be used to identify different isomeric molecular states by transport experiments. PMID:29259875

Unimolecular rectifiers and proposed unimolecular amplifier.

PubMed

Metzger, Robert M

2003-12-01

The rectification by three molecules that form Langmuir-Blodgett monolayers between gold electrodes is reviewed, along with a proposal for the means to obtain gain in a unimolecular amplifier, the molecular analog of a bipolar junction transistor.

New insights into the extraction of invisible gold in a low-grade high-sulfur Carlin-type gold concentrate by bio-pretreatment

NASA Astrophysics Data System (ADS)

Qiu, Xiao-bin; Wen, Jian-kang; Huang, Song-tao; Yang, Hong-ying; Liu, Mei-lin; Wu, Biao

2017-10-01

To extract gold from a low-grade (13.43 g/t) and high-sulfur (39.94wt% sulfide sulfur) Carlin-type gold concentrate from the Nibao deposit, Guizhou, a bio-pretreatment followed by carbon-in-pulp (CIP) cyanide leaching process was used. Various methods were used to detect the low-grade gold in the concentrate; however, only time-of-flight secondary-ion mass spectrometry (TOF-SIMS) was successful. With bio-pretreatment, the gold recovery rate increased by approximately 70.16% compared with that obtained by direct cyanide leaching of the concentrate. Various attempts were made to increase the final gold recovery rate. However, approximately 20wt% of the gold was non-extractable. To determine the nature of this non-extractable gold, mineralogy liberation analysis (MLA), formation of secondary product during the bio-pretreatment, and the preg-robbing capacity of the carbonaceous matter in the ore were investigated. The results indicated that at least four factors affected the gold recovery rate: gold occurrence, tight junctions of gold-bearing pyrite with gangue minerals, jarosite coating of the ore, and the carbonaceous matter content.

Decoupling of epitaxial graphene via gold intercalation probed by dispersive Raman spectroscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pillai, P. B., E-mail: p.pillai@sheffield.ac.uk, E-mail: m.desouza@sheffield.ac.uk; DeSouza, M., E-mail: p.pillai@sheffield.ac.uk, E-mail: m.desouza@sheffield.ac.uk; Narula, R.

Signatures of a superlattice structure composed of a quasi periodic arrangement of atomic gold clusters below an epitaxied graphene (EG) layer are examined using dispersive Raman spectroscopy. The gold-graphene system exhibits a laser excitation energy dependant red shift of the 2D mode as compared to pristine epitaxial graphene. The phonon dispersions in both the systems are mapped using the experimentally observed Raman signatures and a third-nearest neighbour tight binding electronic band structure model. Our results reveal that the observed excitation dependent Raman red shift in gold EG primarily arise from the modifications of the phonon dispersion in gold-graphene and showsmore » that the extent of decoupling of graphene from the underlying SiC substrate can be monitored from the dispersive nature of the Raman 2D modes. The intercalated gold atoms restore the phonon band structure of epitaxial graphene towards free standing graphene.« less

Single Molecule Junctions: A Laboratory for Chemistry, Mechanics and Bond Rupture

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hybertsen M. S.

Simultaneous measurement [1] of junction conductance and sustained force in single molecule junctions bridging metal electrodes provides a powerful tool in the quantitative study of the character of molecule-metal bonds. In this talk I will discuss three topics. First, I will describe chemical trends in link bond strength based on experiments and Density Functional Theory based calculations. Second, I will focus on the specific case of pyridine-linked junctions. Bond rupture from the high conductance junction structure shows a requires a force that exceeds the rupture force of gold point contacts and clearly indicates the role of additional forces, beyond themore » specific N-Au donor acceptor bond. DFT-D2 calculations with empirical addition of dispersion interactions illustrates the interplay between the donor-acceptor bonding and the non-specific van der Waals interactions between the pyridine rings and Au asperities. Third, I will describe recent efforts to characterize the diversity of junction structures realized in break-junction experiments with suitable models for the potential surfaces that are observed. [1] Venkataraman Group, Columbia University.« less

High temperature superconductor step-edge Josephson junctions using Ti-Ca-Ba-Cu-O

DOEpatents

Ginley, D.S.; Hietala, V.M.; Hohenwarter, G.K.G.; Martens, J.S.; Plut, T.A.; Tigges, C.P.; Vawter, G.A.; Zipperian, T.E.

1994-10-25

A process is disclosed for formulating non-hysteretic and hysteretic Josephson junctions using HTS materials which results in junctions having the ability to operate at high temperatures while maintaining high uniformity and quality. The non-hysteretic Josephson junction is formed by step-etching a LaAlO[sub 3] crystal substrate and then depositing a thin film of TlCaBaCuO on the substrate, covering the step, and forming a grain boundary at the step and a subsequent Josephson junction. Once the non-hysteretic junction is formed the next step to form the hysteretic Josephson junction is to add capacitance to the system. In the current embodiment, this is accomplished by adding a thin dielectric layer, LaA1O[sub 3], followed by a cap layer of a normal metal where the cap layer is formed by first depositing a thin layer of titanium (Ti) followed by a layer of gold (Au). The dielectric layer and the normal metal cap are patterned to the desired geometry. 8 figs.

Gold-promoted structurally ordered intermetallic palladium cobalt nanoparticles for the oxygen reduction reaction.

PubMed

Kuttiyiel, Kurian A; Sasaki, Kotaro; Su, Dong; Wu, Lijun; Zhu, Yimei; Adzic, Radoslav R

2014-11-06

Considerable efforts to make palladium and palladium alloys active catalysts and a possible replacement for platinum have had a marginal success. Here we report on a structurally ordered Au10Pd₄₀Co₅₀ catalyst that exhibits comparable activity to conventional platinum catalysts in both acid and alkaline media. Electron microscopic techniques demonstrate that, at elevated temperatures, palladium cobalt nanoparticles undergo an atomic structural transition from core-shell to a rare intermetallic ordered structure with twin boundaries forming stable {111}, {110} and {100} facets via addition of gold atoms. The superior stability of this catalyst compared with platinum after 10,000 potential cycles in alkaline media is attributed to the atomic structural order of PdCo nanoparticles along with protective effect of clusters of gold atoms on the surface. This strategy of making ordered palladium intermetallic alloy nanoparticles can be used in diverse heterogeneous catalysis where particle size and structural stability matter.

Gold atoms and dimers on amorphous SiO(2): calculation of optical properties and cavity ringdown spectroscopy measurements.

PubMed

Del Vitto, Annalisa; Pacchioni, Gianfranco; Lim, Kok Hwa; Rösch, Notker; Antonietti, Jean-Marie; Michalski, Marcin; Heiz, Ulrich; Jones, Harold

2005-10-27

We report on the optical absorption spectra of gold atoms and dimers deposited on amorphous silica in size-selected fashion. Experimental spectra were obtained by cavity ringdown spectroscopy. Issues on soft-landing, fragmentation, and thermal diffusion are discussed on the basis of the experimental results. In parallel, cluster and periodic supercell density functional theory (DFT) calculations were performed to model atoms and dimers trapped on various defect sites of amorphous silica. Optically allowed electronic transitions were calculated, and comparisons with the experimental spectra show that silicon dangling bonds [[triple bond]Si(.-)], nonbridging oxygen [[triple bond]Si-O(.-)], and the silanolate group [[triple bond]Si-O(-)] act as trapping centers for the gold particles. The results are not only important for understanding the chemical bonding of atoms and clusters on oxide surfaces, but they will also be of fundamental interest for photochemical studies of size-selected clusters on surfaces.

X-ray spectroscopy study of electronic structure of laser-irradiated Au nanoparticles in a silica film

NASA Astrophysics Data System (ADS)

Jonnard, P.; Bercegol, H.; Lamaignère, L.; Morreeuw, J.-P.; Rullier, J.-L.; Cottancin, E.; Pellarin, M.

2005-03-01

The electronic structure of gold nanoparticles embedded in a silica film is studied, both before and after irradiation at 355nm by a laser. The Au 5d occupied valence states are observed by x-ray emission spectroscopy. They show that before irradiation the gold atoms are in metallic states within the nanoparticles. After irradiation with a fluence of 0.5J/cm2, it is found that gold valence states are close to those of a metal-poor gold silicide; thanks to a comparison of the experimental Au 5d states with the calculated ones for gold silicides using the density-functional theory. The formation of such a compound is driven by the diffusion of the gold atoms into the silica film upon the laser irradiation. At higher fluence, 1J/cm2, we find a higher percentage of metallic gold that could be attributed to annealing in the silica matrix.

An investigation into the interactions of gold nanoparticles and anti-arthritic drugs with macrophages, and their reactivity towards thioredoxin reductase

DOE Office of Scientific and Technical Information (OSTI.GOV)

James, Lloyd R.A.; Xu, Zhi-Qiang; Sluyter, Ronald

Gold(I) complexes are an important tool in the arsenal of established approaches for treating rheumatoid arthritis (RA), while some recent studies have suggested that gold nanoparticles (Au NPs) may also be therapeutically efficacious. These observations prompted the current biological studies involving gold(I) anti-RA agents and Au NPs, which are aimed towards improving our knowledge of how they work. The cytotoxicity of auranofin, aurothiomalate, aurothiosulfate and Au NPs towards RAW264.7 macrophages was evaluated using the MTT assay, with the former compound proving to be the most toxic. The extent of cellular uptake of the various gold agents was determined using graphitemore » furnace atomic absorption spectrometry, while their distribution within macrophages was examined using microprobe synchrotron radiation X-ray fluorescence spectroscopy. The latter technique showed accumulation of gold in discrete regions of the cell, and co-localisation with sulfur in the case of cells treated with aurothiomalate or auranofin. Electrospray ionization mass spectrometry was used to characterize thioredoxin reductase (TrxR) in which the penultimate selenocysteine residue was replaced by cysteine. Mass spectra of solutions of TrxR and aurothiomalate, aurothiosulfate or auranofin showed complexes containing bare gold atoms bound to the protein, or protein adducts containing gold atoms retaining some of their initial ligands. These results support TrxR being an important target of gold(I) drugs used to treat RA, while the finding that Au NPs are incorporated into macrophages, but elicit little toxicity, indicates further exploration of their potential for treatment of RA is warranted.« less

How can we make stable linear monoatomic chains? Gold-cesium binary subnanowires as an example of a charge-transfer-driven approach to alloying.

PubMed

Choi, Young Cheol; Lee, Han Myoung; Kim, Woo Youn; Kwon, S K; Nautiyal, Tashi; Cheng, Da-Yong; Vishwanathan, K; Kim, Kwang S

2007-02-16

On the basis of first-principles calculations of clusters and one dimensional infinitely long subnanowires of the binary systems, we find that alkali-noble metal alloy wires show better linearity and stability than either pure alkali metal or noble metal wires. The enhanced alternating charge buildup on atoms by charge transfer helps the atoms line up straight. The cesium doped gold wires showing significant charge transfer from cesium to gold can be stabilized as linear or circular monoatomic chains.

A New-Type of Long-Range Restructuring of Ordered Metal Surfaces Induced by Lateral Adsorbate Interactions: Iodide on AU(110) Electrodes

DTIC Science & Technology

1994-02-01

separated by monoatomic steps. The direction of the (110) gold rows is evident in the atomic- resolution image of a uniform terrace, shown in Fig. 2A...distinguish between the average surface energy of a gold atom within a (110) terrace and at a monoatomic step (edge) site. The difference between these...having (3 x 2) symmetry (coverage - 0.67), is imaged instead of the substrate, with the iodide arranged in parallel close-packed rows in between the gold

Single step synthesis of gold-amino acid composite, with the evidence of the catalytic hydrogen atom transfer (HAT) reaction, for the electrochemical recognition of Serotonin

NASA Astrophysics Data System (ADS)

Choudhary, Meenakshi; Siwal, Samarjeet; Nandi, Debkumar; Mallick, Kaushik

2016-03-01

A composite architecture of amino acid and gold nanoparticles has been synthesized using a generic route of 'in-situ polymerization and composite formation (IPCF)' [1,2]. The formation mechanism of the composite has been supported by a model hydrogen atom (H•≡H++e-) transfer (HAT) type of reaction which belongs to the proton coupled electron transfer (PCET) mechanism. The 'gold-amino acid composite' was used as a catalyst for the electrochemical recognition of Serotonin.

Current at Metal-Organic Interfaces

NASA Astrophysics Data System (ADS)

Kern, Klaus

2012-02-01

Charge transport through atomic and molecular constrictions greatly affects the operation and performance of organic electronic devices. Much of our understanding of the charge injection and extraction processes in these systems relays on our knowledge of the electronic structure at the metal-organic interface. Despite significant experimental and theoretical advances in studying charge transport in nanoscale junctions, a microscopic understanding at the single atom/molecule level is missing. In the present talk I will present our recent results to probe directly the nanocontact between single molecules and a metal electrode using scanning probe microscopy and spectroscopy. The experiments provide unprecedented microscopic details of single molecule and atom junctions and open new avenues to study quantum critical and many body phenomena at the atomic scale. Implications for energy conversion devices and carbon based nanoelectronics will also be discussed.

Antibody-gold cluster conjugates

DOEpatents

Hainfeld, J.F.

1988-06-28

Antibody- or antibody fragment-gold cluster conjugates are shown wherein the conjugate size can be about 5.0 nm. Methods and reagents are disclosed in which antibodies or Fab' fragments thereof are covalently bound to a stable cluster of gold atoms. 2 figs.

Stretching of short monatomic gold chains-some model calculations

NASA Astrophysics Data System (ADS)

Sumali, Priyanka, Verma, Veena; Dharamvir, Keya

2012-06-01

The Mechanical properties of zig-zag monatomic gold chains containing 5 and 7 atoms were studied using the Siesta Code (SC), which works within the framework of DFT formalism and Gupta Potential (GP), which is an effective atom-atom potential. The zig-zag chains were stretched by keeping the end atoms fixed while rest of the atoms were relaxed till minimum energy is obtained. Energy, Force and Young's Modulus found using GP and SC were plotted as functions of total length. It is found that the breaking force in case of GP is of order of 1.6nN while for SIESTA is of the order of 2.9nN for both the chains.

Conductivity and structure of ErAs nanoparticles embedded in GaAs pn junctions analyzed via conductive atomic force microscopy

NASA Astrophysics Data System (ADS)

Park, K. W.; Dasika, V. D.; Nair, H. P.; Crook, A. M.; Bank, S. R.; Yu, E. T.

2012-06-01

We have used conductive atomic force microscopy to investigate the influence of growth temperature on local current flow in GaAs pn junctions with embedded ErAs nanoparticles grown by molecular beam epitaxy. Three sets of samples, one with 1 ML ErAs deposited at different growth temperatures and two grown at 530 °C and 575 °C with varying ErAs depositions, were characterized. Statistical analysis of local current images suggests that the structures grown at 575 °C have about 3 times thicker ErAs nanoparticles than structures grown at 530 °C, resulting in degradation of conductivity due to reduced ErAs coverage. These findings explain previous studies of macroscopic tunnel junctions.

Thin-film semiconductor rectifier has improved properties

NASA Technical Reports Server (NTRS)

1966-01-01

Cadmium selenide-zinc selenide film is used as a thin film semiconductor rectifier. The film is vapor-deposited in a controlled concentration gradient into a glass substrate to form the required junctions between vapor-deposited gold electrodes.

Negative differential resistance observation in complex convoluted fullerene junctions

NASA Astrophysics Data System (ADS)

Kaur, Milanpreet; Sawhney, Ravinder Singh; Engles, Derick

2018-04-01

In this work, we simulated the smallest fullerene molecule, C20 in a two-probe device model with gold electrodes. The gold electrodes comprised of (011) miller planes were carved to construct the novel geometry based four unique shapes, which were strung to fullerene molecules through mechanically controlled break junction techniques. The organized devices were later scrutinized using non-equilibrium Green's function based on the density functional theory to calculate their molecular orbitals, energy levels, charge transfers, and electrical parameters. After intense scrutiny, we concluded that five-edged and six-edged devices have the lowest and highest current-conductance values, which result from their electrode-dominating and electrode-subsidiary effects, respectively. However, an interesting observation was that the three-edged and four-edged electrodes functioned as semi-metallic in nature, allowing the C20 molecule to demonstrate its performance with the complementary effect of these electrodes in the electron conduction process of a two-probe device.

Origin of selenium–gold interaction in F{sub 2}CSe⋯AuY (Y = CN, F, Cl, Br, OH, and CH{sub 3}): Synergistic effects

DOE Office of Scientific and Technical Information (OSTI.GOV)

Guo, Xin; Yang, Yu-Ping; Li, Qing-Zhong, E-mail: liqingzhong1990@sina.com, E-mail: lihaibei@sdu.edu.cn

Selenium–gold interaction plays an important role in crystal materials, molecular self-assembly, and pharmacochemistry involving gold. In this paper, we unveiled the mechanism and nature of selenium–gold interaction by studying complexes F{sub 2}CSe⋯AuY (Y = CN, F, Cl, Br, OH, and CH{sub 3}). The results showed that the formation of selenium–gold interaction is mainly attributed to the charge transfer from the lone pair of Se atom to the Au—Y anti-bonding orbital. Energy decomposition analysis indicated that the polarization energy is nearly equivalent to or exceeds the electrostatic term in the selenium–gold interaction. Interestingly, the chalcogen–gold interaction becomes stronger with the increasemore » of chalcogen atomic mass in F{sub 2}CX⋯AuCN (X = O, S, Se, and Te). The cyclic ternary complexes are formed with the introduction of NH{sub 3} into F{sub 2}CSe⋯AuY, in which selenium–gold interaction is weakened and selenium–nitrogen interaction is strengthened due to the synergistic effects.« less

Molecular oxygen adsorption and dissociation on Au12M clusters with M = Cu, Ag or Ir

NASA Astrophysics Data System (ADS)

Jiménez-Díaz, Laura M.; Pérez, Luis A.

2018-03-01

In this work, we present a density functional theory study of the structural and electronic properties of isolated neutral clusters of the type Au12M, with M = Cu, Ag, or Ir. On the other hand, there is experimental evidence that gold-silver, gold-copper and gold-iridium nanoparticles have an enhanced catalytic activity for the CO oxidation reaction. In order to address these phenomena, we also performed density functional calculations of the adsorption and dissociation of O2 on these nanoparticles. Moreover, to understand the effects of Cu, Ag, and Ir impurity atoms on the dissociation of O2, we also analyze this reaction in the corresponding pure gold cluster. The results indicate that the substitution of one gold atom in a Au13 cluster by Ag, Cu or Ir diminishes the activation energy barrier for the O2 dissociation by nearly 1 eV. This energy barrier is similar for Au12Ag and Au12Cu, whereas for Au12Ir is even lower. These results suggest that the addition of other transition metal atoms to gold nanoclusters can enhance their catalytic activity towards the CO oxidation reaction, independently of the effect that the substrate could have on supported nanoclusters.

Characteristics of pulse gold vapor laser outlined

NASA Astrophysics Data System (ADS)

1981-09-01

Several dozen laser oscillating spectra lines were found within the very broad spectral wavelengths from infrared to ultraviolet. Laser studies of gold vapor were carried out and a pulsed laser of gold atoms of an operating wavelength of 6278 angstroms was obtained.

Magnetic tunnel junctions with monolayer hexagonal boron nitride tunnel barriers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Piquemal-Banci, M.; Galceran, R.; Bouzehouane, K.

We report on the integration of atomically thin 2D insulating hexagonal boron nitride (h-BN) tunnel barriers into Co/h-BN/Fe magnetic tunnel junctions (MTJs). The h-BN monolayer is directly grown by chemical vapor deposition on Fe. The Conductive Tip Atomic Force Microscopy (CT-AFM) measurements reveal the homogeneity of the tunnel behavior of our h-BN layers. As expected for tunneling, the resistance depends exponentially on the number of h-BN layers. The h-BN monolayer properties are also characterized through integration into complete MTJ devices. A Tunnel Magnetoresistance of up to 6% is observed for a MTJ based on a single atomically thin h-BN layer.

The adsorption of helium atoms on small cationic gold clusters.

PubMed

Goulart, Marcelo; Gatchell, Michael; Kranabetter, Lorenz; Kuhn, Martin; Martini, Paul; Gitzl, Norbert; Rainer, Manuel; Postler, Johannes; Scheier, Paul; Ellis, Andrew M

2018-04-04

Adducts formed between small gold cluster cations and helium atoms are reported for the first time. These binary ions, Aun+Hem, were produced by electron ionization of helium nanodroplets doped with neutral gold clusters and were detected using mass spectrometry. For a given value of n, the distribution of ions as a function of the number of added helium atoms, m, has been recorded. Peaks with anomalously high intensities, corresponding to so-called magic number ions, are identified and interpreted in terms of the geometric structures of the underlying Aun+ ions. These features can be accounted for by planar structures for Aun+ ions with n ≤ 7, with the addition of helium having no significant effect on the structures of the underlying gold cluster ions. According to ion mobility studies and some theoretical predictions, a 3-D structure is expected for Au8+. However, the findings for Au8+ in this work are more consistent with a planar structure.

Determination of gold, indium, tellurium and thallium in the same sample digest of geological materials by atomic-absorption spectroscopy and two-step solvent extraction

USGS Publications Warehouse

Hubert, A.E.; Chao, T.T.

1985-01-01

A rock, soil, or stream-sediment sample is decomposed with hydrofluoric acid, aqua regia, and hydrobromic acid-bromine solution. Gold, thallium, indium and tellurium are separated and concentrated from the sample digest by a two-step MIBK extraction at two concentrations of hydrobromic add. Gold and thallium are first extracted from 0.1M hydrobromic acid medium, then indium and tellurium are extracted from 3M hydrobromic acid in the presence of ascorbic acid to eliminate iron interference. The elements are then determined by flame atomic-absorption spectrophotometry. The two-step solvent extraction can also be used in conjunction with electrothermal atomic-absorption methods to lower the detection limits for all four metals in geological materials. ?? 1985.

Simulating the Effect of Contact Atomic Structure on the Spin-Dependent Transport Properties of Gold Nanowires

NASA Astrophysics Data System (ADS)

Ansarino, Masoud; Ravan, Bahram Abedi

Some experimental research works report on the superb magnetoresistance properties of magnetically contacted gold nanowires. With the intention of trying to understand the spin-dependent transport mechanism of these structures, in this work we have used first-principles density functional theory methods to investigate effects of interface structure on the spintronic characteristics of Au nanowires. Monatomic chains of gold are sandwiched between two ferromagnetic electrodes of Fe and by substituting the interfacial Fe atoms with some other transition metal elements (including Cr, Mn, Co and Ni) the occurrence of possible enhancement in the electronic conductance and magnetoresistance characteristics of the device are investigated. It is observed that replacing the interfacial atoms with Ni raises the junction’s magnetoresistance ratio to as high as 2000%.

The Origin of the Elements

ScienceCinema

Murphy, Edward

2018-01-23

The world around us is made of atoms. Did you ever wonder where these atoms came from? How was the gold in our jewelry, the carbon in our bodies, and the iron in our cars made? In this lecture, we will trace the origin of a gold atom from the Big Bang to the present day, and beyond. You will learn how the elements were forged in the nuclear furnaces inside stars, and how, when they die, these massive stars spread the elements into space. You will learn about the origin of the building blocks of matter in the Big Bang, and we will speculate on the future of the atoms around us today.

Investigation of atomic oxygen-surface interactions related to measurements with dual air density explorer satellites

NASA Technical Reports Server (NTRS)

Wood, B. J.; Ablow, C. M.; Wise, H.

1973-01-01

For a number of candidate materials of construction for the dual air density explorer satellites the rate of oxygen atom loss by adsorption, surface reaction, and recombination was determined as a function of surface and temperature. Plain aluminum and anodized aluminum surfaces exhibit a collisional atom loss probability alpha .01 in the temperature range 140 - 360 K, and an initial sticking probability. For SiO coated aluminum in the same temperature range, alpha .001 and So .001. Atom-loss on gold is relatively rapid alpha .01. The So for gold varies between 0.25 and unity in the temperature range 360 - 140 K.

77 FR 33204 - Notice of Intent To Prepare a Supplemental Environmental Impact Statement for the Long-Term...

Federal Register 2010, 2011, 2012, 2013, 2014

2012-06-05

... activities, and generated as a byproduct of the gold mining process. In addition, DOE's National Nuclear... Junction, Colorado; DOE Hanford site near Richland, Washington; Hawthorne Army Depot near Hawthorne, Nevada...

The Design, Synthesis, and Characterization of Open Sites on Metal Clusters

NASA Astrophysics Data System (ADS)

Nigra, Michael Mark

Coordinatively unsaturated corner and edge atoms have been hypothesized to have the highest activity of sites responsible for many catalytic reactions on a metal surface. Recent studies have validated this hypothesis in varied reaction systems. However, quantification of different types of coordinatively unsaturated sites, and elucidation of their individual catalytic rates has remained a largely unresolved challenge when understanding catalysis on metal surfaces. Yet such structure-function knowledge would be invaluable to the design of more active and selective metal-surface catalysts in the future. I investigated the catalytic contributions of undercoordinated sites such as corner and edge atoms are investigated in a model reaction system using organic ligands bound to the gold nanoparticle surface. The catalyst consisted of 4 nm gold nanoparticles on a metal oxide support, using resazurin to resorufin as a model reaction system. My results demonstrate that in this system, corner atom sites are the most undercoordinated sites, and are over an order of magnitude more active when compared to undercoordinated edge atom sites, while terrace sites remain catalytically inactive for the reduction reaction of resazurin to resorufin. Catalytic activity has been also demonstrated for calixarene-bound gold nanoparticles using the reduction of 4-nitrophenol. With the 4-nitrophenol reduction reaction, a comparative study was undertaken to compare calixarene phosphine and calixarene thiol bound 4 nm gold particles. The results of the study suggested that a leached site was responsible for catalysis and not sites on the original gold nanoparticles. Future experiments with calixarene bound gold clusters could investigate ligand effects in reactions where the active site is not a leached or aggregated gold species, possibly in oxidation reactions, where electron-rich gold is hypothesized to be a good catalyst. The results that emphasize the enhanced catalytic activity of undercoordinated sites led me to synthesize small gold clusters consisting of a high fraction of coordinatively unsaturated open sites. This was enabled through an approach that utilized bulky calix[4]arene ligands that are bound to a gold core. Since the size of the calix[4]arene ligand is commensurate with the size of the gold cluster core, the calix[4]arene ligand does not pack closely together on the gold cluster surface. This in turn results in areas of accessible gold atom sites between ligands. Additionally, these calix[4]arene ligands prevent cluster aggregation and electronically tune the gold core in a manner conceptually similar to enzymes affecting reactivity through organic side-chains acting as ligands. I quantified the number of open sites that result from this packing problem on the gold cluster surface, using fluorescence probe chemisorption experiments. The results of these chemisorption measurements support the mechanical model of accessibility whereby accessibility is not dependent on the identity of the functional group, whether it be calixarene phosphines or N-heterocyclic carbenes, bound to the gold surface, but rather to the relative radii of curvature of bound ligands and the gold cluster core. Additional materials characterization was completed with transmission electron microscopy in both bright-field imaging of zeolites, in MCM-22 and delaminated ITQ-2 and UCB-1 materials, and in dark field imaging of glucan coatings on oxide particles. These materials could prove to be interesting materials as to use as supports for the calixarene-bound metal clusters described above or for other metal clusters.

Self-diffusion and microscopic dynamics in a gold-silicon liquid investigated with quasielastic neutron scattering

DOE Office of Scientific and Technical Information (OSTI.GOV)

Evenson, Zach, E-mail: Zachary.Evenson@frm2.tum.de; Institut für Materialphysik im Weltraum, Deutsches Zentrum für Luft- und Raumfahrt; Yang, Fan

2016-03-21

We use incoherent quasielastic neutron scattering to study the atomic dynamics of gold in a eutectic Au{sub 81}Si{sub 19} melt. Despite the glass-forming nature of this system, the gold self-diffusivity displays an Arrhenius behavior with a low activation energy characteristic of simple liquids. At high temperatures, long-range transport of gold atoms is well described by hydrodynamic theory with a simple exponential decay of the self-correlation function. On cooling towards the melting temperature, structural relaxation crosses over to a highly stretched exponential behavior. This suggests the onset of a heterogeneous dynamics, even in the equilibrium melt, and is indicative of amore » very fragile liquid.« less

Conductive atomic force microscopy measurements of nanopillar magnetic tunnel junctions

NASA Astrophysics Data System (ADS)

Evarts, E. R.; Hogg, C.; Bain, J. A.; Majetich, S. A.

2009-03-01

Magnetic tunnel junctions have been studied extensively for their magnetoresistance and potential uses in magnetic logic and data storage devices, but little is known about how their performance will scale with size. Here we examined the electronic behavior of 12 nm diameter magnetic tunnel junctions fabricated by a novel nanomasking process. Scanning electron microscopy images indicated feature diameter of 12 nm, and atomic force microscopy showed a height of 5 nm suggesting that unmasked regions have been milled on average to the oxide barrier layer, and areas should have the remnants of the free layer exposed with no remaining nanoparticle. Electrical contact was made to individual nanopillars using a doped-diamond-coated atomic force microscopy probe with a 40 nm radius of curvature at the tip. Off pillar we observed a resistance of 8.1 x 10^5 φ, while on pillar we found a resistance of 2.85 x 10^6 φ. Based on the RA product for this film, 120 φ-μm^2, a 12 nm diameter cylinder with perfect contact would have a resistance of 1.06 x 10^6 φ. The larger experimental value is consistent with a smaller contact area due to damaging the pillar during the ion milling process. The magnetoresistance characteristics of these magnetic tunnel junctions will be discussed.

3D Band Diagram and Photoexcitation of 2D–3D Semiconductor Heterojunctions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Li, Bo; Shi, Gang; Lei, Sidong

2015-08-17

The emergence of a rich variety of two-dimensional (2D) layered semiconductor materials has enabled the creation of atomically thin heterojunction devices. Junctions between atomically thin 2D layers and 3D bulk semiconductors can lead to junctions that are fundamentally electronically different from the covalently bonded conventional semiconductor junctions. In this paper, we propose a new 3D band diagram for the heterojunction formed between n-type monolayer MoS 2 and p-type Si, in which the conduction and valence band-edges of the MoS 2 monolayer are drawn for both stacked and in-plane directions. This new band diagram helps visualize the flow of charge carriersmore » inside the device in a 3D manner. Our detailed wavelength-dependent photocurrent measurements fully support the diagrams and unambiguously show that the band alignment is type I for this 2D-3D heterojunction. Photogenerated electron–hole pairs in the atomically thin monolayer are separated and driven by an external bias and control the “on/off” states of the junction photodetector device. Finally, two photoresponse regimes with fast and slow relaxation are also revealed in time-resolved photocurrent measurements, suggesting the important role played by charge trap states.« less

Mass spectrometric identification of Au68(SR)34 molecular gold nanoclusters with 34-electron shell closing.

PubMed

Dass, Amala

2009-08-26

The molecular formula Au(68)(SCH(2)CH(2)Ph)(34) has been assigned to the 14 kDa nanocluster using MALDI-TOF mass spectrometry. The 34-electron shell closing in a macroscopically obtained thiolated gold nanocluster is demonstrated. The Au(68) nanocluster is predicted to have a 49 atom Marks decahedral core with 19 inner core atoms and 30 outer atoms chelating with the staple motifs. The nanoclusters' predicted formulation is [Au](19+30) [Au(SR)(2)](11) [Au(2)(SR)(3)](4).

Electrocatalysts having platium monolayers on palladium, palladium alloy, and gold alloy core-shell nanoparticles, and uses thereof

DOEpatents

Adzic, Radoslav; Mo, Yibo; Vukmirovic, Miomir; Zhang, Junliang

2010-12-21

The invention relates to platinum-coated particles useful as fuel cell electrocatalysts. The particles are composed of a noble metal or metal alloy core at least partially encapsulated by an atomically thin surface layer of platinum atoms. The invention particularly relates to such particles having a palladium, palladium alloy, gold alloy, or rhenium alloy core encapsulated by an atomic monolayer of platinum. In other embodiments, the invention relates to fuel cells containing these electrocatalysts and methods for generating electrical energy therefrom.

Enhanced resolution imaging of ultrathin ZnO layers on Ag(111) by multiple hydrogen molecules in a scanning tunneling microscope junction

NASA Astrophysics Data System (ADS)

Liu, Shuyi; Shiotari, Akitoshi; Baugh, Delroy; Wolf, Martin; Kumagai, Takashi

2018-05-01

Molecular hydrogen in a scanning tunneling microscope (STM) junction has been found to enhance the lateral spatial resolution of the STM imaging, referred to as scanning tunneling hydrogen microscopy (STHM). Here we report atomic resolution imaging of 2- and 3-monolayer (ML) thick ZnO layers epitaxially grown on Ag(111) using STHM. The enhanced resolution can be obtained at a relatively large tip to surface distance and resolves a more defective structure exhibiting dislocation defects for 3-ML-thick ZnO than for 2 ML. In order to elucidate the enhanced imaging mechanism, the electric and mechanical properties of the hydrogen molecular junction (HMJ) are investigated by a combination of STM and atomic force microscopy. It is found that the HMJ shows multiple kinklike features in the tip to surface distance dependence of the conductance and frequency shift curves, which are absent in a hydrogen-free junction. Based on a simple modeling, we propose that the junction contains several hydrogen molecules and sequential squeezing of the molecules out of the junction results in the kinklike features in the conductance and frequency shift curves. The model also qualitatively reproduces the enhanced resolution image of the ZnO films.

Atomic-scaled characterization of graphene PN junctions

NASA Astrophysics Data System (ADS)

Zhou, Xiaodong; Wang, Dennis; Dadgar, Ali; Agnihotri, Pratik; Lee, Ji Ung; Reuter, Mark C.; Ross, Frances M.; Pasupathy, Abhay N.

Graphene p-n junctions are essential devices for studying relativistic Klein tunneling and the Veselago lensing effect in graphene. We have successfully fabricated graphene p-n junctions using both lithographically pre-patterned substrates and the stacking of vertical heterostructures. We then use our 4-probe STM system to characterize the junctions. The ability to carry out scanning electron microscopy (SEM) in our STM instrument is essential for us to locate and measure the junction interface. We obtain both the topography and dI/dV spectra at the junction area, from which we track the shift of the graphene chemical potential with position across the junction interface. This allows us to directly measure the spatial width and roughness of the junction and its potential barrier height. We will compare the junction properties of devices fabricated by the aforementioned two methods and discuss their effects on the performance as a Veselago lens.

Nanotube junctions

DOEpatents

Crespi, Vincent Henry; Cohen, Marvin Lou; Louie, Steven Gwon; Zettl, Alexander Karlwalte

2004-12-28

The present invention comprises a new nanoscale metal-semiconductor, semiconductor-semiconductor, or metal-metal junction, designed by introducing topological or chemical defects in the atomic structure of the nanotube. Nanotubes comprising adjacent sections having differing electrical properties are described. These nanotubes can be constructed from combinations of carbon, boron, nitrogen and other elements. The nanotube can be designed having different indices on either side of a junction point in a continuous tube so that the electrical properties on either side of the junction vary in a useful fashion. For example, the inventive nanotube may be electrically conducting on one side of a junction and semiconducting on the other side. An example of a semiconductor-metal junction is a Schottky barrier. Alternatively, the nanotube may exhibit different semiconductor properties on either side of the junction. Nanotubes containing heterojunctions, Schottky barriers, and metal-metal junctions are useful for microcircuitry.

Nanotube junctions

DOEpatents

Crespi, Vincent Henry; Cohen, Marvin Lou; Louie, Steven Gwon Sheng; Zettl, Alexander Karlwalter

2003-01-01

The present invention comprises a new nanoscale metal-semiconductor, semiconductor-semiconductor, or metal-metal junction, designed by introducing topological or chemical defects in the atomic structure of the nanotube. Nanotubes comprising adjacent sections having differing electrical properties are described. These nanotubes can be constructed from combinations of carbon, boron, nitrogen and other elements. The nanotube can be designed having different indices on either side of a junction point in a continuous tube so that the electrical properties on either side of the junction vary in a useful fashion. For example, the inventive nanotube may be electrically conducting on one side of a junction and semiconducting on the other side. An example of a semiconductor-metal junction is a Schottky barrier. Alternatively, the nanotube may exhibit different semiconductor properties on either side of the junction. Nanotubes containing heterojunctions, Schottky barriers, and metal-metal junctions are useful for microcircuitry.

Topological Phases in Graphene Nanoribbons: Junction States, Spin Centers, and Quantum Spin Chains

NASA Astrophysics Data System (ADS)

Cao, Ting; Zhao, Fangzhou; Louie, Steven G.

2017-08-01

We show that semiconducting graphene nanoribbons (GNRs) of different width, edge, and end termination (synthesizable from molecular precursors with atomic precision) belong to different electronic topological classes. The topological phase of GNRs is protected by spatial symmetries and dictated by the terminating unit cell. We have derived explicit formulas for their topological invariants and shown that localized junction states developed between two GNRs of distinct topology may be tuned by lateral junction geometry. The topology of a GNR can be further modified by dopants, such as a periodic array of boron atoms. In a superlattice consisting of segments of doped and pristine GNRs, the junction states are stable spin centers, forming a Heisenberg antiferromagnetic spin 1 /2 chain with tunable exchange interaction. The discoveries here not only are of scientific interest for studies of quasi-one-dimensional systems, but also open a new path for design principles of future GNR-based devices through their topological characters.

Topological Phases in Graphene Nanoribbons: Junction States, Spin Centers, and Quantum Spin Chains.

PubMed

Cao, Ting; Zhao, Fangzhou; Louie, Steven G

2017-08-18

We show that semiconducting graphene nanoribbons (GNRs) of different width, edge, and end termination (synthesizable from molecular precursors with atomic precision) belong to different electronic topological classes. The topological phase of GNRs is protected by spatial symmetries and dictated by the terminating unit cell. We have derived explicit formulas for their topological invariants and shown that localized junction states developed between two GNRs of distinct topology may be tuned by lateral junction geometry. The topology of a GNR can be further modified by dopants, such as a periodic array of boron atoms. In a superlattice consisting of segments of doped and pristine GNRs, the junction states are stable spin centers, forming a Heisenberg antiferromagnetic spin 1/2 chain with tunable exchange interaction. The discoveries here not only are of scientific interest for studies of quasi-one-dimensional systems, but also open a new path for design principles of future GNR-based devices through their topological characters.

DFT Modeling of Cross-Linked Polyethylene: Role of Gold Atoms and Dispersion Interactions.

PubMed

Blaško, Martin; Mach, Pavel; Antušek, Andrej; Urban, Miroslav

2018-02-08

Using DFT modeling, we analyze the concerted action of gold atoms and dispersion interactions in cross-linked polyethylene. Our model consists of two oligomer chains (PEn) with 7, 11, 15, 19, or 23 carbon atoms in each oligomer cross-linked with one to three Au atoms through C-Au-C bonds. In structures with a single gold atom the C-Au-C bond is located in the central position of the oligomer. Binding energies (BEs) with respect to two oligomer radical fragments and Au are as high as 362-489 kJ/mol depending on the length of the oligomer chain. When the dispersion contribution in PEn-Au-PEn oligomers is omitted, BE is almost independent of the number of carbon atoms, lying between 293 and 296 kJ/mol. The dispersion energy contributions to BEs in PEn-Au-PEn rise nearly linearly with the number of carbon atoms in the PEn chain. The carbon-carbon distance in the C-Au-C moiety is around 4.1 Å, similar to the bond distance between saturated closed shell chains in the polyethylene crystal. BEs of pure saturated closed shell PEn-PEn oligomers are 51-187 kJ/mol. Both Au atoms and dispersion interactions contribute considerably to the creation of nearly parallel chains of oligomers with reasonably high binding energies.

Electron microscopy study of gold nanoparticles deposited on transition metal oxides.

PubMed

Akita, Tomoki; Kohyama, Masanori; Haruta, Masatake

2013-08-20

Many researchers have investigated the catalytic performance of gold nanoparticles (GNPs) supported on metal oxides for various catalytic reactions of industrial importance. These studies have consistently shown that the catalytic activity and selectivity depend on the size of GNPs, the kind of metal oxide supports, and the gold/metal oxide interface structure. Although researchers have proposed several structural models for the catalytically active sites and have identified the specific electronic structures of GNPs induced by the quantum effect, recent experimental and theoretical studies indicate that the perimeter around GNPs in contact with the metal oxide supports acts as an active site in many reactions. Thus, it is of immense importance to investigate the detailed structures of the perimeters and the contact interfaces of gold/metal oxide systems by using electron microscopy at an atomic scale. This Account describes our investigation, at the atomic scale using electron microscopy, of GNPs deposited on metal oxides. In particular, high-resolution transmission electron microscopy (HRTEM) and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) are valuable tools to observe local atomic structures, as has been successfully demonstrated for various nanoparticles, surfaces, and material interfaces. TEM can be applied to real powder catalysts as received without making special specimens, in contrast to what is typically necessary to observe bulk materials. For precise structure analyses at an atomic scale, model catalysts prepared by using well-defined single-crystalline substrates are also adopted for TEM observations. Moreover, aberration-corrected TEM, which has high spatial resolution under 0.1 nm, is a promising tool to observe the interface structure between GNPs and metal oxide supports including oxygen atoms at the interfaces. The oxygen atoms in particular play an important role in the behavior of gold/metal oxide interfaces, because they may participate in catalytic reaction steps. Detailed information about the interfacial structures between GNPs and metal oxides provides valuable structure models for theoretical calculations which can elucidate the local electronic structure effective for activating a reactant molecule. Based on our observations with HRTEM and HAADF-STEM, we report the detailed structure of gold/metal oxide interfaces.

Aging behavior of Au-based ohmic contacts to GaAs

NASA Technical Reports Server (NTRS)

Fatemi, Navid S.

1989-01-01

Gold based alloys, commonly used as ohmic contacts for solar cells, are known to react readily with GaAs. It is shown that the contact interaction with the underlying GaAs can continue even at room temperature upon aging, altering both the electrical characteristics of the contacts and the nearby pn junction. Au-Ge-Ni as-deposited (no heat-treatment) contacts made to thin emitter (0.15 microns) GaAs diodes have shown severe shunting of the pn junction upon aging for several months at room temperature. The heat-treated contacts, despite showing degradation in contact resistance, did not affect the underlying pn junction. Au-Zn-Au contacts to p-GaAs emitter (0.2 microns) diodes, however, showed slight improvement in contact resistance upon 200 C isothermal annealing for several months, without degrading the pn junction. The effect of aging on electrical characteristics of the as-deposited and heat-treated contacts and the nearby pn junction, as well as on the surface morphology of the contacts are presented.

Aging behavior of Au-based ohmic contacts to GaAs

NASA Technical Reports Server (NTRS)

Fatemi, Navid S.

1988-01-01

Gold based alloys, commonly used as ohmic contacts for solar cells, are known to react readily with GaAs. It is shown that the contact interaction with the underlying GaAs can continue even at room temperature upon aging, altering both the electrical characteristics of the contacts and the nearby pn junction. Au-Ge-Ni as-deposited (no heat treatment) contacts made to thin emitter (0.15 micrometer) GaAs diodes have shown severe shunting of the pn junction upon aging for several months at room temperature. The heat-treated contacts, despite showing degradation in contact resistance did not affect the underlying pn junction. Au-Zn-Au contacts to p-GaAs emitter (0.2 micrometer) diodes, however, showed slight improvement in contact resistance upon 200 C isothermal annealing for several months, without degrading the pn junction. The effect of aging on electrical characteristics of the as-deposited and heat-treated contacts and the nearby pn junction, as well as on the surface morphology of the contacts are presented.

Gap junctions on hippocampal mossy fiber axons demonstrated by thin-section electron microscopy and freeze–fracture replica immunogold labeling

PubMed Central

Hamzei-Sichani, Farid; Kamasawa, Naomi; Janssen, William G. M.; Yasumura, Thomas; Davidson, Kimberly G. V.; Hof, Patrick R.; Wearne, Susan L.; Stewart, Mark G.; Young, Steven R.; Whittington, Miles A.; Rash, John E.; Traub, Roger D.

2007-01-01

Gap junctions have been postulated to exist between the axons of excitatory cortical neurons based on electrophysiological, modeling, and dye-coupling data. Here, we provide ultrastructural evidence for axoaxonic gap junctions in dentate granule cells. Using combined confocal laser scanning microscopy, thin-section transmission electron microscopy, and grid-mapped freeze–fracture replica immunogold labeling, 10 close appositions revealing axoaxonic gap junctions (≈30–70 nm in diameter) were found between pairs of mossy fiber axons (≈100–200 nm in diameter) in the stratum lucidum of the CA3b field of the rat ventral hippocampus, and one axonal gap junction (≈100 connexons) was found on a mossy fiber axon in the CA3c field of the rat dorsal hippocampus. Immunogold labeling with two sizes of gold beads revealed that connexin36 was present in that axonal gap junction. These ultrastructural data support computer modeling and in vitro electrophysiological data suggesting that axoaxonic gap junctions play an important role in the generation of very fast (>70 Hz) network oscillations and in the hypersynchronous electrical activity of epilepsy. PMID:17640909

Interaction of size-selected gold nanoclusters with dopamine

NASA Astrophysics Data System (ADS)

Montone, Georgia R.; Hermann, Eric; Kandalam, Anil K.

2016-12-01

We present density functional theory based results on the interaction of size-selected gold nanoclusters, Au10 and Au20, with dopamine molecule. The gold clusters interact strongly with the nitrogen site of dopamine, thereby forming stable gold-dopamine complexes. Our calculations further show that there is no site specificity on the planar Au10 cluster with all the edge gold atoms equally preferred. On the other hand, in the pyramidal Au20 cluster, the vertex metal atom is the most active site. As the size increased from Au10 to Au20, the interaction strength has shown a declining trend. The effect of aqueous environment on the interaction strengths were also studied by solvation model. It is found that the presence of solvent water stabilizes the interaction between the metal cluster and dopamine molecule, even though for Au10 cluster the energy ordering of the isomers changed from that of the gas-phase.

Density functional study of structural and electronic properties of bimetallic silver-gold clusters: Comparison with pure gold and silver clusters

NASA Astrophysics Data System (ADS)

Bonacic-Koutecky, Vlasta; Burda, Jaroslav; Mitric, Roland; Ge, Maofa; Zampella, Giuseppe; Fantucci, Piercarlo

2002-08-01

Bimetallic silver-gold clusters offer an excellent opportunity to study changes in metallic versus "ionic" properties involving charge transfer as a function of the size and the composition, particularly when compared to pure silver and gold clusters. We have determined structures, ionization potentials, and vertical detachment energies for neutral and charged bimetallic AgmAun 3[less-than-or-equal](m+n)[less-than-or-equal]5 clusters. Calculated VDE values compare well with available experimental data. In the stable structures of these clusters Au atoms assume positions which favor the charge transfer from Ag atoms. Heteronuclear bonding is usually preferred to homonuclear bonding in clusters with equal numbers of hetero atoms. In fact, stable structures of neutral Ag2Au2, Ag3Au3, and Ag4Au4 clusters are characterized by the maximum number of hetero bonds and peripheral positions of Au atoms. Bimetallic tetramer as well as hexamer are planar and have common structural properties with corresponding one-component systems, while Ag4Au4 and Ag8 have 3D forms in contrast to Au8 which assumes planar structure. At the density functional level of theory we have shown that this is due to participation of d electrons in bonding of pure Aun clusters while s electrons dominate bonding in pure Agm as well as in bimetallic clusters. In fact, Aun clusters remain planar for larger sizes than Agm and AgnAun clusters. Segregation between two components in bimetallic systems is not favorable, as shown in the example of Ag5Au5 cluster. We have found that the structures of bimetallic clusters with 20 atoms Ag10Au10 and Ag12Au8 are characterized by negatively charged Au subunits embedded in Ag environment. In the latter case, the shape of Au8 is related to a pentagonal bipyramid capped by one atom and contains three exposed negatively charged Au atoms. They might be suitable for activating reactions relevant to catalysis. According to our findings the charge transfer in bimetallic clusters is responsible for formation of negatively charged gold subunits which are expected to be reactive, a situation similar to that of gold clusters supported on metal oxides.

Catalytic behavior of ‘Pt-atomic chain encapsulated gold nanotube’: A density functional study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nigam, Sandeep, E-mail: snigam@barc.gov.in; Majumder, Chiranjib

2016-05-23

With an aim to design novel material and explore its catalytic performance towards CO oxidation, Pt atomic chain was introduced inside gold nanotube (Au-NT). Theoretical calculations at the level of first principles formalism was carried out to investigate the atomic and electronic properties of the composite. Geometrically Pt atoms prefer to align in zig-zag fashion. Significant electronic charge transfer from inside Pt atoms to the outer wall Au atoms is observed. Interaction of O{sub 2} with Au-NT wall follows by injection of additional electronic charge in the anti-bonding orbital of oxygen molecule leading to activation of the O-O bond. Furthermore » interaction of CO molecule with the activated oxygen molecule leads to spontaneous oxidation reaction and formation of CO{sub 2}.« less

Anticancer Agents: Does a Phosphonium Behave Like a Gold(I) Phosphine Complex? Let a "Smart" Probe Answer!

PubMed

Ali, Moussa; Dondaine, Lucile; Adolle, Anais; Sampaio, Carla; Chotard, Florian; Richard, Philippe; Denat, Franck; Bettaieb, Ali; Le Gendre, Pierre; Laurens, Véronique; Goze, Christine; Paul, Catherine; Bodio, Ewen

2015-06-11

Gold phosphine complexes, such as auranofin, have been recognized for decades as antirheumatic agents. Clinical trials are now underway to validate their use in anticancer or anti-HIV treatments. However, their mechanisms of action remain unclear. A challenging question is whether the gold phosphine complex is a prodrug that is administered in an inactive precursor form or rather that the gold atom remains attached to the phosphine ligand during treatment. In this study, we present two novel gold complexes, which we compared to auranofin and to their phosphonium analogue. The chosen ligand is a phosphine-based smart probe, whose strong fluorescence depends on the presence of the gold atom. The in vitro biological action of the gold complexes and the phosphonium derivative were investigated, and a preliminary in vivo study in healthy zebrafish larvae allowed us to evaluate gold complex biodistribution and toxicity. The different analyses carried out showed that these gold complexes were stable and behaved differently from phosphonium and auranofin, both in vitro and in vivo. Two-photon microscopy experiments demonstrated that the cellular targets of these gold complexes are not the same as those of the phosphonium analogue. Moreover, despite similar IC50 values in some cancer cell lines, gold complexes displayed a low toxicity in vivo, in contrast to the phosphonium salt. They are therefore suitable for future in vivo investigations.

Theoretical and experimental insights into the origin of the catalytic activity of subnanometric gold clusters: attempts to predict reactivity with clusters and nanoparticles of gold.

PubMed

Boronat, Mercedes; Leyva-Pérez, Antonio; Corma, Avelino

2014-03-18

Particle size is one of the key parameters determining the unexpected catalytic activity of gold, with reactivity improving as the particle gets smaller. While this is valid in the 1-5 nm range, chemists are now investigating the influence of particle size in the subnanometer regime. This is due to recent advances in both characterization techniques and synthetic routes capable of stabilizing these size-controlled gold clusters. Researchers reported in early studies that small clusters or aggregates of a few atoms can be extremely active in some reactions, while 1-2 nm nanoparticles are catalytically more efficient for other reactions. Furthermore, the possibility that small gold clusters generated in situ from gold salts or complexes could be the real active species in homogeneous gold-catalyzed organic reactions should be considered. In this Account, we address two questions. First, what is the origin of the enhanced reactivity of gold clusters on the subnanometer scale? And second, how can we predict the reactions where small clusters should work better than larger nanoparticles? Both geometric factors and electronic or quantum size effects become important in the subnanometer regime. Geometric reasons play a key role in hydrogenation reactions, where only accessible low coordinated neutral Au atoms are needed to dissociate H2. The quantum size effects of gold clusters are important as well, as clusters formed by only a few atoms have discrete molecule-like electronic states and their chemical reactivity is related to interactions between the cluster's frontier molecular orbitals and those of the reactant molecules. From first principles calculations, we predict an enhanced reactivity of small planar clusters for reactions involving activation of CC multiple bonds in alkenes and alkynes through Lewis acid-base interactions, and a better catalytic performance of 3D gold nanoparticles in redox reactions involving bond dissociation by oxidative addition and new bond formation by reductive elimination. In oxidation reactions with molecular O2, initial dissociation of O2 into basic oxygen atoms would be more effectively catalyzed by gold nanoparticles of ∼1 nm diameter. In contrast, small planar clusters should be more active for reactions following a radical pathway involving peroxo or hydroperoxo intermediates. We have experimentally confirmed these predictions for a series of Lewis acid and oxidation reactions catalyzed by gold clusters and nanoparticles either in solution or supported on solid carriers.

Gold nanoparticles with different capping systems: an electronic and structural XAS analysis.

PubMed

López-Cartes, C; Rojas, T C; Litrán, R; Martínez-Martínez, D; de la Fuente, J M; Penadés, S; Fernández, A

2005-05-12

Gold nanoparticles (NPs) have been prepared with three different capping systems: a tetralkylammonium salt, an alkanethiol, and a thiol-derivatized neoglycoconjugate. Also gold NPs supported on a porous TiO(2) substrate have been investigated. X-ray absorption spectroscopy (XAS) has been used to determine the electronic behavior of the different capped/supported systems regarding the electron/hole density of d states. Surface and size effects, as well as the role of the microstructure, have been also studied through an exhaustive analysis of the EXAFS (extended X-ray absorption fine structure) data. Very small gold NPs functionalized with thiol-derivatized molecules show an increase in d-hole density at the gold site due to Au-S charge transfer. This effect is overcoming size effects (which lead to a slightly increase of the d-electron density) for high S:Au atomic ratios and core-shell microstructures where an atomically abrupt Au-S interface likely does not exist. It has been also shown that thiol functionalization of very small gold NPs is introducing a strong distortion as compared to fcc order. To the contrary, electron transfer from reduced support oxides to gold NPs can produce a higher increase in d-electron density at the gold site, as compared to naked gold clusters.

Fungus-mediated biological synthesis of gold nanoparticles: potential in detection of liver cancer

PubMed Central

Chauhan, Arun; Zubair, Swaleha; Tufail, Saba; Sherwani, Asif; Sajid, Mohammad; Raman, Suri C; Azam, Amir; Owais, Mohammad

2011-01-01

Background Nanomaterials are considered to be the pre-eminent component of the rapidly advancing field of nanotechnology. However, developments in the biologically inspired synthesis of nanoparticles are still in their infancy and consequently attracting the attention of material scientists throughout the world. Keeping in mind the fact that microorganism-assisted synthesis of nanoparticles is a safe and economically viable prospect, in the current study we report Candida albicans-mediated biological synthesis of gold nanoparticles. Methods and results Transmission electron microscopy, atomic force microscopy, and various spectrophotometric analyses were performed to characterize the gold nanoparticles. The morphology of the synthesized gold particles depended on the abundance of C. albicans cytosolic extract. Transmission electron microscopy, nanophox particle analysis, and atomic force microscopy revealed the size of spherical gold nanoparticles to be in the range of 20–40 nm and nonspherical gold particles were found to be 60–80 nm. We also evaluated the potential of biogenic gold nanoparticles to probe liver cancer cells by conjugating them with liver cancer cell surface-specific antibodies. The antibody-conjugated gold particles were found to bind specifically to the surface antigens of the cancer cells. Conclusion The antibody-conjugated gold particles synthesized in this study could successfully differentiate normal cell populations from cancerous cells. PMID:22072868

Manganese dioxide causes spurious gold values in flame atomic-absorption readings from HBr-Br2 digestions

USGS Publications Warehouse

Campbell, W.L.

1981-01-01

False readings, apparently caused by the presence of high concentrations of manganese dioxide, have been observed in our current flame atomic-absorption procedure for the determination of gold. After a hydrobromic acid (HBr)-bromine (Br2) leach, simply heating the sample to boiling to remove excess Br2 prior to extraction with methyl-isobutyl-ketone (MIBK) eliminates these false readings. ?? 1981.

Electron transfer dynamics of bistable single-molecule junctions.

PubMed

Danilov, Andrey V; Kubatkin, Sergey E; Kafanov, Sergey G; Flensberg, Karsten; Bjørnholm, Thomas

2006-10-01

We present transport measurements of single-molecule junctions bridged by a molecule with three benzene rings connected by two double bonds and with thiol end-groups that allow chemical binding to gold electrodes. The I-V curves show switching behavior between two distinct states. By statistical analysis of the switching events, we show that a 300 meV mode mediates the transition between the two states. We propose that breaking and reformation of a S-H bond in the contact zone between molecule and electrode explains the observed bistability.

Photoelectrochemical modulation of neuronal activity with free-standing coaxial silicon nanowires

NASA Astrophysics Data System (ADS)

Parameswaran, Ramya; Carvalho-de-Souza, João L.; Jiang, Yuanwen; Burke, Michael J.; Zimmerman, John F.; Koehler, Kelliann; Phillips, Andrew W.; Yi, Jaeseok; Adams, Erin J.; Bezanilla, Francisco; Tian, Bozhi

2018-02-01

Optical methods for modulating cellular behaviour are promising for both fundamental and clinical applications. However, most available methods are either mechanically invasive, require genetic manipulation of target cells or cannot provide subcellular specificity. Here, we address all these issues by showing optical neuromodulation with free-standing coaxial p-type/intrinsic/n-type silicon nanowires. We reveal the presence of atomic gold on the nanowire surfaces, likely due to gold diffusion during the material growth. To evaluate how surface gold impacts the photoelectrochemical properties of single nanowires, we used modified quartz pipettes from a patch clamp and recorded sustained cathodic photocurrents from single nanowires. We show that these currents can elicit action potentials in primary rat dorsal root ganglion neurons through a primarily atomic gold-enhanced photoelectrochemical process.

Atomic oxygen damage characterization by photothermal scanning

NASA Technical Reports Server (NTRS)

Williams, A. W.; Wood, N. J.; Zakaria, A. B.

1993-01-01

In this paper we use a photothermal imaging technique to characterize the damage caused to an imperfectly coated gold-coated Kapton sample exposed to successively increased fluences of atomic oxygen in a laboratory atomic source.

Reinventing solid state electronics: Harnessing quantum confinement in bismuth thin films

NASA Astrophysics Data System (ADS)

Gity, Farzan; Ansari, Lida; Lanius, Martin; Schüffelgen, Peter; Mussler, Gregor; Grützmacher, Detlev; Greer, J. C.

2017-02-01

Solid state electronics relies on the intentional introduction of impurity atoms or dopants into a semiconductor crystal and/or the formation of junctions between different materials (heterojunctions) to create rectifiers, potential barriers, and conducting pathways. With these building blocks, switching and amplification of electrical currents and voltages are achieved. As miniaturisation continues to ultra-scaled transistors with critical dimensions on the order of ten atomic lengths, the concept of doping to form junctions fails and forming heterojunctions becomes extremely difficult. Here, it is shown that it is not needed to introduce dopant atoms nor is a heterojunction required to achieve the fundamental electronic function of current rectification. Ideal diode behavior or rectification is achieved solely by manipulation of quantum confinement using approximately 2 nm thick films consisting of a single atomic element, the semimetal bismuth. Crucially for nanoelectronics, this approach enables room temperature operation.

First principles calculation of current-induced forces in atomic gold contacts

NASA Astrophysics Data System (ADS)

Brandbyge, Mads; Stokbro, Kurt; Taylor, Jeremy; Mozos, Jose-Luis; Ordejon, Pablo

2002-03-01

We have recently developed an first principles method [1] for calculating the electronic structure, electronic transport, and forces acting on the atoms, for atomic scale systems connected to semi-infinite electrodes and with an applied voltage bias. Our method is based on the density functional theory (DFT) as implemented in the well tested SIESTA program [2]. We fully deal with the atomistic structure of the whole system, treating both the contact and the electrodes on the same footing. The effect of the finite bias (including selfconsistency and the solution of the electrostatic problem) is taken into account using nonequilibrium Green's functions. In this talk we show results for the forces acting on the contact atoms due to the nonequilibrium situation in the electronic subsystem, i.e. in the presence of an electronic current. We concentrate on one atom wide gold contacts/wires connected to bulk gold electrodes. References [1] Our implementation is called TranSIESTA and is described in M. Brandbyge, J. Taylor, K. Stokbro, J-L. Mozos, and P. Ordejon, cond-mat/0110650 [2] D. Sanchez-Portal, P. Ordejon, E. Artacho and J. Soler, Int. J. Quantum Chem. 65, 453 (1997).

Room-temperature current blockade in atomically defined single-cluster junctions

NASA Astrophysics Data System (ADS)

Lovat, Giacomo; Choi, Bonnie; Paley, Daniel W.; Steigerwald, Michael L.; Venkataraman, Latha; Roy, Xavier

2017-11-01

Fabricating nanoscopic devices capable of manipulating and processing single units of charge is an essential step towards creating functional devices where quantum effects dominate transport characteristics. The archetypal single-electron transistor comprises a small conducting or semiconducting island separated from two metallic reservoirs by insulating barriers. By enabling the transfer of a well-defined number of charge carriers between the island and the reservoirs, such a device may enable discrete single-electron operations. Here, we describe a single-molecule junction comprising a redox-active, atomically precise cobalt chalcogenide cluster wired between two nanoscopic electrodes. We observe current blockade at room temperature in thousands of single-cluster junctions. Below a threshold voltage, charge transfer across the junction is suppressed. The device is turned on when the temporary occupation of the core states by a transiting carrier is energetically enabled, resulting in a sequential tunnelling process and an increase in current by a factor of ∼600. We perform in situ and ex situ cyclic voltammetry as well as density functional theory calculations to unveil a two-step process mediated by an orbital localized on the core of the cluster in which charge carriers reside before tunnelling to the collector reservoir. As the bias window of the junction is opened wide enough to include one of the cluster frontier orbitals, the current blockade is lifted and charge carriers can tunnel sequentially across the junction.

Morphology dependent near-field response in atomistic plasmonic nanocavities.

PubMed

Chen, Xing; Jensen, Lasse

2018-06-21

In this work we examine how the atomistic morphologies of plasmonic dimers control the near-field response by using an atomistic electrodynamics model. At large separations, the field enhancement in the junction follows a simple inverse power law as a function of the gap separation, which agrees with classical antenna theory. However, when the separations are smaller than 0.8 nm, the so-called quantum size regime, the field enhancement is screened and thus deviates from the simple power law. Our results show that the threshold distance for the deviation depends on the specific morphology of the junction. The near field in the junction can be localized to an area of less than 1 nm2 in the presence of an atomically sharp tip, but the separation distances leading to a large confinement of near field depend strongly on the specific atomistic configuration. More importantly, the highly confined fields lead to large field gradients particularly in a tip-to-surface junction, which indicates that such a plasmonic structure favors observing strong field gradient effects in near-field spectroscopy. We find that for atomically sharp tips the field gradient becomes significant and depends strongly on the local morphology of a tip. We expect our findings to be crucial for understanding the origin of high-resolution near-field spectroscopy and for manipulating optical cavities through atomic structures in the strongly coupled plasmonic systems.

Electrical properties of Al foil/n-4H-SiC Schottky junctions fabricated by surface-activated bonding

NASA Astrophysics Data System (ADS)

Morita, Sho; Liang, Jianbo; Matsubara, Moeko; Dhamrin, Marwan; Nishio, Yoshitaka; Shigekawa, Naoteru

2018-02-01

We fabricate 17-µm-thick Al foil/n-4H-SiC Schottky junctions by surface-activated bonding. Their current-voltage and capacitance-voltage characteristics are compared with those of Schottky junctions fabricated by evaporating Al layers on n-4H-SiC epilayers. We find that the ideality factor of Al foil/SiC junctions is larger than that of conventional junctions, which is due to the irradiation of the fast atom beam (FAB) of Ar. The ideality factor of Al foil/SiC junctions is improved by annealing at 400 °C. We also find that the Schottky barrier height is increased by FAB irradiation, which is likely to be due to the negative charges formed at SiC surfaces.

Preparation of Gelatin Layer Film with Gold Clusters in Using Photographic Film

NASA Astrophysics Data System (ADS)

Kuge, Ken'ichi; Arisawa, Michiko; Aoki, Naokazu; Hasegawa, Akira

2000-12-01

A gelatin layer film with gold clusters is produced by taking advantage of the photosensitivity of silver halide photography. Through exposure silver specks, which are called latent-image specks and are composed of several reduced silver atoms, are formed on the surface of silver halide grains in the photographic film. As the latent-image specks act as a catalyst for redox reaction, reduced gold atoms are deposited on the latent-image specks when the exposed film is immersed in a gold (I) thiocyanate complex solution for 5-20 days. Subsequently, when the silver halide grains are dissolved and removed, the gelatin layer film with gold clusters remains. The film produced by this method is purple and showed an absorption spectrum having a maximum of approximately 560 nm as a result of plasmon absorption. The clusters continued to grow with immersion time, and the growth rate increased as the concentration of the gold complex solution was increased. The cluster diameter changed from 20 nm to 100 nm. By this method, it is possible to produce a gelatin film of a large area with evenly dispersed gold clusters, and since it is produced only on the exposed area, pattern forming is also possible.

Effect of gold subsurface layer on the surface activity and segregation in Pt/Au/Pt3M (where M = 3d transition metals) alloy catalyst from first-principles.

PubMed

Kim, Chang-Eun; Lim, Dong-Hee; Jang, Jong Hyun; Kim, Hyoung Juhn; Yoon, Sung Pil; Han, Jonghee; Nam, Suk Woo; Hong, Seong-Ahn; Soon, Aloysius; Ham, Hyung Chul

2015-01-21

The effect of a subsurface hetero layer (thin gold) on the activity and stability of Pt skin surface in Pt3M system (M = 3d transition metals) is investigated using the spin-polarized density functional theory calculation. First, we find that the heterometallic interaction between the Pt skin surface and the gold subsurface in Pt/Au/Pt3M system can significantly modify the electronic structure of the Pt skin surface. In particular, the local density of states projected onto the d states of Pt skin surface near the Fermi level is drastically decreased compared to the Pt/Pt/Pt3M case, leading to the reduction of the oxygen binding strength of the Pt skin surface. This modification is related to the increase of surface charge polarization of outmost Pt skin atoms by the electron transfer from the gold subsurface atoms. Furthermore, a subsurface gold layer is found to cast the energetic barrier to the segregation loss of metal atoms from the bulk (inside) region, which can enhance the durability of Pt3M based catalytic system in oxygen reduction condition at fuel cell devices. This study highlights that a gold subsurface hetero layer can provide an additional mean to tune the surface activity toward oxygen species and in turn the oxygen reduction reaction, where the utilization of geometric strain already reaches its practical limit.

Enhanced noise at high bias in atomic-scale Au break junctions

PubMed Central

Chen, Ruoyu; Wheeler, Patrick J.; Di Ventra, M.; Natelson, D.

2014-01-01

Heating in nanoscale systems driven out of equilibrium is of fundamental importance, has ramifications for technological applications, and is a challenge to characterize experimentally. Prior experiments using nanoscale junctions have largely focused on heating of ionic degrees of freedom, while heating of the electrons has been mostly neglected. We report measurements in atomic-scale Au break junctions, in which the bias-driven component of the current noise is used as a probe of the electronic distribution. At low biases (<150 mV) the noise is consistent with expectations of shot noise at a fixed electronic temperature. At higher biases, a nonlinear dependence of the noise power is observed. We consider candidate mechanisms for this increase, including flicker noise (due to ionic motion), heating of the bulk electrodes, nonequilibrium electron-phonon effects, and local heating of the electronic distribution impinging on the ballistic junction. We find that flicker noise and bulk heating are quantitatively unlikely to explain the observations. We discuss the implications of these observations for other nanoscale systems, and experimental tests to distinguish vibrational and electron interaction mechanisms for the enhanced noise. PMID:24573177

Efficient and scalable ionization of neutral atoms by an orderly array of gold-doped silicon nanowires

NASA Astrophysics Data System (ADS)

Bucay, Igal; Helal, Ahmed; Dunsky, David; Leviyev, Alex; Mallavarapu, Akhila; Sreenivasan, S. V.; Raizen, Mark

2017-04-01

Ionization of atoms and molecules is an important process in many applications and processes such as mass spectrometry. Ionization is typically accomplished by electron bombardment, and while it is scalable to large volumes, is also very inefficient due to the small cross section of electron-atom collisions. Photoionization methods can be highly efficient, but are not scalable due to the small ionization volume. Electric field ionization is accomplished using ultra-sharp conducting tips biased to a few kilovolts, but suffers from a low ionization volume and tip fabrication limitations. We report on our progress towards an efficient, robust, and scalable method of atomic and molecular ionization using orderly arrays of sharp, gold-doped silicon nanowires. As demonstrated in earlier work, the presence of the gold greatly enhances the ionization probability, which was attributed to an increase in available acceptor surface states. We present here a novel process used to fabricate the nanowire array, results of simulations aimed at optimizing the configuration of the array, and our progress towards demonstrating efficient and scalable ionization.

Aurophilicity in gold(I) catalysis: for better or worse?

PubMed

Weber, Dieter; Gagné, Michel R

2015-01-01

This book chapter discusses the effects of aurophilicity on gold catalysis. First, a brief historic account of aurophilicity in organogold chemistry is given, focusing on the pioneering results which set the stage for its association with catalytic intermediates (gold vinyl and gold aryl complexes); this is followed by an introduction to cationic gold(I) as an electrophilic catalyst, and the first isolation of organogold intermediates from catalysis. In the main section, the growing number of reports observing aurophilic interactions in catalysis or illustrative model systems is reviewed in a non-comprehensive tutorial way. The effects of aurophilicity are discussed in the following structures: (1) the geminal diauration of C(sp²)-atoms; (2) geminal diauration of other atoms; (3) σ-π-diauration of terminal alkynes. It is apparent that in most cases efficient catalysis is hindered by aurophilic effects as less active aggregates tend to be formed from more active species [LAu]⁺, but there are a growing number of reports using aurophilicity as a driving force to access new reactivity and selectivity.

Molecular Simulations of The Formation of Gold-Molecule-Gold Junctions

NASA Astrophysics Data System (ADS)

Wang, Huachuan

2013-03-01

We perform classical molecular simulations by combining grand canonical Monte Carlo (GCMC) sampling with molecular dynamics (MD) simulation to explore the dynamic gold nanojunctions in a Alkenedithiol (ADT) solvent. With the aid of a simple driving-spring model, which can reasonably represent the long-range elasticity of the gold electrode, the spring forces are obtained during the dynamic stretching procedure. A specific multi-time-scale double reversible reference system propagator (double-RESPA) algorithm has been designed for the metal-organic complex in MD simulations to identify the detailed metal-molecule bonding geometry at metal-molecule-metal interface. We investigate the variations of bonding sites of ADT molecules on gold nanojunctions at Au (111) surface at a constant chemical potential. Simulation results show that an Au-ADT-Au interface is formed on Au nanojunctions, bond-breaking intersection is at 1-1 bond of the monatomic chain of the cross-section, instead of at the Au-S bond. Breaking force is around 1.5 nN. These are consistent with the experimental measurements.

High frequency measurements of shot noise suppression in atomic-scale metal contacts

NASA Astrophysics Data System (ADS)

Wheeler, Patrick J.; Evans, Kenneth; Russom, Jeffrey; King, Nicholas; Natelson, Douglas

2009-03-01

Shot noise provides a means of assessing the number and transmission coefficients of transmitting channels in atomic- and molecular-scale junctions. Previous experiments at low temperatures in metal and semiconductor point contacts have demonstrated the expected suppression of shot noise when junction conductance is near an integer multiple of the conductance quantum, G0≡2e^2/h. Using high frequency techniques, we demonstrate the high speed acquisition of such data at room temperature in mechanical break junctions. In clean Au contacts conductance histograms with clear peaks at G0, 2G0, and 3G0 are acquired within hours, and histograms of simultaneous measurements of the shot noise show clear suppression at those conductance values. We describe the dependence of the noise on bias voltage and analyze the noise vs. conductance histograms in terms of a model that averages over transmission coefficients.

Length-dependent transport in molecular junctions based on SAMs of alkanethiols and alkanedithiols: effect of metal work function and applied bias on tunneling efficiency and contact resistance.

PubMed

Engelkes, Vincent B; Beebe, Jeremy M; Frisbie, C Daniel

2004-11-03

Nanoscopic tunnel junctions were formed by contacting Au-, Pt-, or Ag-coated atomic force microscopy (AFM) tips to self-assembled monolayers (SAMs) of alkanethiol or alkanedithiol molecules on polycrystalline Au, Pt, or Ag substrates. Current-voltage traces exhibited sigmoidal behavior and an exponential attenuation with molecular length, characteristic of nonresonant tunneling. The length-dependent decay parameter, beta, was found to be approximately 1.1 per carbon atom (C(-1)) or 0.88 A(-)(1) and was independent of applied bias (over a voltage range of +/-1.5 V) and electrode work function. In contrast, the contact resistance, R(0), extrapolated from resistance versus molecular length plots showed a notable decrease with both applied bias and increasing electrode work function. The doubly bound alkanedithiol junctions were observed to have a contact resistance approximately 1 to 2 orders of magnitude lower than the singly bound alkanethiol junctions. However, both alkanethiol and dithiol junctions exhibited the same length dependence (beta value). The resistance versus length data were also used to calculate transmission values for each type of contact (e.g., Au-S-C, Au/CH(3), etc.) and the transmission per C-C bond (T(C)(-)()(C)).

Electrical transport and structural characterization of epitaxial monolayer MoS2 /n- and p-doped GaN vertical lattice-matched heterojunctions

NASA Astrophysics Data System (ADS)

Ruzmetov, D.; O'Regan, T.; Zhang, K.; Herzing, A.; Mazzoni, A.; Chin, M.; Huang, S.; Zhang, Z.; Burke, R.; Neupane, M.; Birdwell, Ag; Shah, P.; Crowne, F.; Kolmakov, A.; Leroy, B.; Robinson, J.; Davydov, A.; Ivanov, T.

We investigate vertical semiconductor junctions consisting of monolayer MoS2 that is epitaxially grown on n- and p-doped GaN crystals. Such a junction represents a building block for 2D/3D vertical semiconductor heterostructures. Epitaxial, lattice-matched growth of MoS2 on GaN is important to ensure high quality interfaces that are crucial for the efficient vertical transport. The MoS2/GaN junctions were characterized with cross-sectional and planar scanning transmission electron microscopy (STEM), scanning tunneling microscopy, and atomic force microscopy. The MoS2/GaN lattice mismatch is measured to be near 1% using STEM. The electrical transport in the out-of-plane direction across the MoS2/GaN junctions was measured using conductive atomic force microscopy and mechanical nano-probes inside a scanning electron microscope. Nano-disc metal contacts to MoS2 were fabricated by e-beam lithography and evaporation. The current-voltage curves of the vertical MoS2/GaN junctions exhibit rectification with opposite polarities for n-doped and p-doped GaN. The metal contact determines the general features of the current-voltage curves, and the MoS2 monolayer modifies the electrical transport across the contact/GaN interface.

Kinetic Monte Carlo Simulation of the Growth of Various Nanostructures through Atomic and Cluster Deposition: Application to Gold Nanostructure Growth on Graphite

NASA Astrophysics Data System (ADS)

Claassens, C. H.; Hoffman, M. J. H.; Terblans, J. J.; Swart, H. C.

2006-01-01

A Kinetic Monte Carlo (KMC) method is presented to describe the growth of metallic nanostructures through atomic and cluster deposition in the mono -and multilayer regime. The model makes provision for homo- and heteroepitaxial systems with small lattice mismatch. The accuracy of the model is tested with simulations of the growth of gold nanostructures on HOPG and comparisons are made with existing experimental data.

Hydroxyalkyl phosphine gold complexes for use as diagnostic and therapeutic pharmaceuticals and method of making same

DOEpatents

Katti, Kattesh V.; Berning, Douglas E.; Volkert, Wynn A.; Ketring, Alan R.

1998-01-01

A complex and method for making same for use as a diagnostic or therapeutic pharmaceutical includes a ligand comprising at least one hydroxyalkyl phosphine donor group bound to a gold atom to form a gold-ligand complex that is stable in aqueous solutions containing oxygen, serum and other body fluids.

Hydroxyalkyl phosphine gold complexes for use as diagnostic and therapeutic pharmaceuticals and method of making same

DOEpatents

Katti, K.V.; Berning, D.E.; Volkert, W.A.; Ketring, A.R.

1998-12-01

A complex and method for making a diagnostic or therapeutic pharmaceutical includes a ligand comprising at least one hydroxyalkyl phosphine donor group bound to a gold atom to form a gold-ligand complex that is stable in aqueous solutions containing oxygen, serum and other body fluids. 20 figs.

Probing the Structures and Electronic Properties of Dual-Phosphorus-Doped Gold Cluster Anions (AunP-2, n = 1–8): A Density functional Theory Investigation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Xu, Kang-Ming; Huang, Teng; Liu, Yi-Rong

2015-07-29

The geometries of gold clusters doped with two phosphorus atoms, (AunP-2, n = 1–8) were investigated using density functional theory (DFT) methods. Various two-dimensional (2D) and three-dimensional (3D) structures of the doped clusters were studied. The results indicate that the structures of dual-phosphorus-doped gold clusters exhibit large differences from those of pure gold clusters with small cluster sizes. In our study, as for Au6P-2, two cis–trans isomers were found. The global minimum of Au8P-2 presents a similar configuration to that of Au-20, a pyramid-shaped unit, and the potential novel optical and catalytic properties of this structure warrant further attention. Themore » higher stability of AunP-2 clusters relative to Au-n+2 (n = 1–8) clusters was verified based on various energy parameters, and the results indicate that the phosphorus atom can improve the stabilities of the gold clusters. We then explored the evolutionary path of (n = 1–8) clusters. We found that AunP-2 clusters exhibit the 2D–3D structural transition at n = 6, which is much clearer and faster than that of pure gold clusters and single-phosphorus-doped clusters. The electronic properties of AunP-2 (n = 1–8) were then investigated. The photoelectron spectra provide additional fundamental information on the structures and molecular orbitals shed light on the evolution of AunP-2 (n = 1–8). Natural bond orbital (NBO) described the charge distribution in stabilizing structures and revealed the strong relativistic effects of the gold atoms.« less

Cyanide leaching of Au/CeO2: highly active gold clusters for 1,3-butadiene hydrogenation.

PubMed

Guan, Y; Hensen, E J M

2009-11-07

Ceria-supported gold catalysts before and after leaching by NaCN were investigated by X-ray absorption spectroscopy at the Au L(III) edge. After gold leaching, isolated gold cations remain in close interaction with the support. These ions form an ideal precursor to very small clusters of a few gold atoms upon reduction. The resulting gold clusters exhibit a very high intrinsic activity in the hydrogenation of 1,3-butadiene, which is at least one order of magnitude higher than that of the nanometre-sized gold particles in the non-leached parent catalyst. These findings point to a very strong structure sensitivity of the gold-catalyzed hydrogenation of dienes.

Fixed-Gap Tunnel Junction for Reading DNA Nucleotides

PubMed Central

2015-01-01

Previous measurements of the electronic conductance of DNA nucleotides or amino acids have used tunnel junctions in which the gap is mechanically adjusted, such as scanning tunneling microscopes or mechanically controllable break junctions. Fixed-junction devices have, at best, detected the passage of whole DNA molecules without yielding chemical information. Here, we report on a layered tunnel junction in which the tunnel gap is defined by a dielectric layer, deposited by atomic layer deposition. Reactive ion etching is used to drill a hole through the layers so that the tunnel junction can be exposed to molecules in solution. When the metal electrodes are functionalized with recognition molecules that capture DNA nucleotides via hydrogen bonds, the identities of the individual nucleotides are revealed by characteristic features of the fluctuating tunnel current associated with single-molecule binding events. PMID:25380505

Photocatalytic Applications of Electrospun TiO2 Nanofibres Embedded with Bimodal Sized and Prismatic Gold Nanoparticles.

PubMed

Gopika, G; Asha, A M; Sivakumar, N; Balakrishnan, A; Nair, S V; Subramanian, K R V

2015-09-01

In this paper, we have synthesized electrospun TiO2 nanofibers embedded with bimodal sized and prismatic gold nanoparticles. The surface plasmons generated in the gold nanoparticles were used to enhance the performance of photocatalysis. The photocatalytic conversion efficiencies of these bimodal sized/prismatic gold nanoparticles when embedded in electrospun TiO2 fibres showed an enhancement of upto 60% over bare fiber systems and also show higher efficiencies than electrospun fibrous systems embedded with unimodal sized gold nanoparticles. Anisotropic bimodal gold nanoparticles show the highest degree of photocatalytic activity. This may be attributed to greater density/concentration of nanoparticles with higher effective surface area and formation of a junction between the smaller and larger nanoparticles. Such a bimodally distributed range of nanoparticles could also lead to greater trapping of charge carriers at the TiO2 conduction band edge and promoting catalytic reactions on account of these trapped charges. This enhanced photocatalytic activity is explained by invoking different operating mechanisms such as improved surface area, greater trapping, coarse plasmon resonance and band effects. Thus, a useful applicability of the gold nanoparticles is shown in the area of photocatalysis.

Ligand-protected gold clusters: the structure, synthesis and applications

NASA Astrophysics Data System (ADS)

Pichugina, D. A.; Kuz'menko, N. E.; Shestakov, A. F.

2015-11-01

Modern concepts of the structure and properties of atomic gold clusters protected by thiolate, selenolate, phosphine and phenylacetylene ligands are analyzed. Within the framework of the superatom theory, the 'divide and protect' approach and the structure rule, the stability and composition of a cluster are determined by the structure of the cluster core, the type of ligands and the total number of valence electrons. Methods of selective synthesis of gold clusters in solution and on the surface of inorganic composites based, in particular, on the reaction of Aun with RS, RSe, PhC≡C, Hal ligands or functional groups of proteins, on stabilization of clusters in cavities of the α-, β and γ-cyclodextrin molecules (Au15 and Au25) and on anchorage to a support surface (Au25/SiO2, Au20/C, Au10/FeOx) are reviewed. Problems in this field are also discussed. Among the methods for cluster structure prediction, particular attention is given to the theoretical approaches based on the density functional theory (DFT). The structures of a number of synthesized clusters are described using the results obtained by X-ray diffraction analysis and DFT calculations. A possible mechanism of formation of the SR(AuSR)n 'staple' units in the cluster shell is proposed. The structure and properties of bimetallic clusters MxAunLm (M=Pd, Pt, Ag, Cu) are discussed. The Pd or Pt atom is located at the centre of the cluster, whereas Ag and Cu atoms form bimetallic compounds in which the heteroatom is located on the surface of the cluster core or in the 'staple' units. The optical properties, fluorescence and luminescence of ligand-protected gold clusters originate from the quantum effects of the Au atoms in the cluster core and in the oligomeric SR(AuSR)x units in the cluster shell. Homogeneous and heterogeneous reactions catalyzed by atomic gold clusters are discussed in the context of the reaction mechanism and the nature of the active sites. The bibliography includes 345 references.

Fast, clash-free RNA conformational morphing using molecular junctions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Heliou, Amelie; Budday, Dominik; Fonseca, Rasmus

Non-coding ribonucleic acids (ncRNA) are functional RNA molecules that are not translated into protein. They are extremely dynamic, adopting diverse conformational substates, which enables them to modulate their interaction with a large number of other molecules. The flexibility of ncRNA provides a challenge for probing their complex 3D conformational landscape, both experimentally and computationally. As a result, despite their conformational diversity, ncRNAs mostly preserve their secondary structure throughout the dynamic ensemble. Here we present a kinematics-based procedure to morph an RNA molecule between conformational substates, while avoiding inter-atomic clashes. We represent an RNA as a kinematic linkage, with fixed groupsmore » of atoms as rigid bodies and rotatable bonds as degrees of freedom. Our procedure maintains RNA secondary structure by treating hydrogen bonds between base pairs as constraints. The constraints define a lower-dimensional, secondary-structure constraint manifold in conformation space, where motions are largely governed by molecular junctions of unpaired nucleotides. On a large benchmark set, we show that our morphing procedure compares favorably to peer algorithms, and can approach goal conformations to within a low all-atom RMSD by directing fewer than 1% of its atoms. Furthermore, our results suggest that molecular junctions can modulate 3D structural rearrangements, while secondary structure elements guide large parts of the molecule along the transition to the correct final conformation.« less

Fast, clash-free RNA conformational morphing using molecular junctions

DOE PAGES

Heliou, Amelie; Budday, Dominik; Fonseca, Rasmus; ...

2017-03-13

Non-coding ribonucleic acids (ncRNA) are functional RNA molecules that are not translated into protein. They are extremely dynamic, adopting diverse conformational substates, which enables them to modulate their interaction with a large number of other molecules. The flexibility of ncRNA provides a challenge for probing their complex 3D conformational landscape, both experimentally and computationally. As a result, despite their conformational diversity, ncRNAs mostly preserve their secondary structure throughout the dynamic ensemble. Here we present a kinematics-based procedure to morph an RNA molecule between conformational substates, while avoiding inter-atomic clashes. We represent an RNA as a kinematic linkage, with fixed groupsmore » of atoms as rigid bodies and rotatable bonds as degrees of freedom. Our procedure maintains RNA secondary structure by treating hydrogen bonds between base pairs as constraints. The constraints define a lower-dimensional, secondary-structure constraint manifold in conformation space, where motions are largely governed by molecular junctions of unpaired nucleotides. On a large benchmark set, we show that our morphing procedure compares favorably to peer algorithms, and can approach goal conformations to within a low all-atom RMSD by directing fewer than 1% of its atoms. Furthermore, our results suggest that molecular junctions can modulate 3D structural rearrangements, while secondary structure elements guide large parts of the molecule along the transition to the correct final conformation.« less

Contemplating Transport Characteristics by Augmenting the Length of Molecule

NASA Astrophysics Data System (ADS)

Kaur, Milanpreet; Sawhney, Ravinder Singh; Engles, Derick

2013-11-01

In this paper, we contemplated the transport characteristics of a single molecular device junction by augmenting the length of the molecule in the scattering region. The molecules considered here belongs to class of alkanedithiols (CnH2n+2S2). Specifically, we used a tight binding semi-empirical model to compute the transport characteristics of butanedithiol, pentanedithiol, hexanedithiol and heptanedithiol connected to semi-infinite gold electrodes through thiol anchoring elements. The exploration of transport properties of considered alkanes was completed for different bias voltages within the sphere of Keldysh's Non Equilibrium Green's Function (NEGF) and Extended Hückel Theory (EHT), for studying the self-consistent steady-state solution, analyzing the out-of-equilibrium electron distribution, and the behavior of the self-consistent potential. We perceived that the current and conductance retrenches with aggravation with the increase in length of the molecule with exhibition of single electron tunneling. We observed that the coupling regime shifts from strong coupling to weak for higher order alkanedithiols and the transmission is function of evenness or oddness of the carbon atoms forming an alkane.

Direct visualization of quasi-ordered oxygen chain structures on Au(110)-(1 × 2)

NASA Astrophysics Data System (ADS)

Hiebel, F.; Montemore, M. M.; Kaxiras, E.; Friend, C. M.

2016-08-01

The Au(110) surface offers unique advantages for atomically-resolved model studies of catalytic oxidation processes on gold. We investigate the adsorption of oxygen on Au(110) using a combination of scanning tunneling microscopy (STM) and density functional theory (DFT) methods. We identify the typical (empty-states) STM contrast resulting from adsorbed oxygen as atomic-sized dark features of electronic origin. DFT-based image simulations confirm that chemisorbed oxygen is generally detected indirectly, from the binding-induced electronic structure modification of gold. STM images show that adsorption occurs without affecting the general structure of the pristine Au(110) missing-row reconstruction. The tendency to form one-dimensional structures is observed already at low coverage (< 0.05 ML), with oxygen adsorbing on alternate sides of the reconstruction ridges. Consistently, calculations yield preferred adsorption on the (111) facets of the reconstruction, on a 3-fold coordination site, with increased stability when adsorbed in chains. Gold atoms with two oxygen neighbors exhibit enhanced electronic hybridization with the O states. Finally, the species observed are reactive to CO oxidation at 200 K and desorption of CO2 leaves a clean and ordered gold surface.

Study of Nanoscale Friction Behaviors of Graphene on Gold Substrates Using Molecular Dynamics

NASA Astrophysics Data System (ADS)

Zhu, Pengzhe; Li, Rui

2018-02-01

In this paper, we investigate the friction behaviors of graphene flakes sliding on a gold substrate using molecular dynamics simulations. The effects of flake size, flake shape, relative rotation angle between flake and substrate, and crystal orientation of substrate on the friction process are thoroughly studied. It is found that under the same load, the average friction forces per atom are smaller for a bigger graphene flake, which exhibits an obvious size effect. It is also shown that flake shape is critical in determining the friction in the sliding process. The average friction forces per atom for the square flake are much bigger than those for the triangular and round flakes. Moreover, the average friction forces per atom for the triangular flake are the smallest. We also find that the orientation of graphene flake relative to gold substrate plays a vital role in the friction process. The friction forces for the graphene flake sliding along the armchair direction are much bigger than those for the flakes with rotation. In addition, it is also found that single crystalline gold substrate exhibits a significant anisotropic effect of friction, which is attributed to the anisotropic effect of potential energy corrugation. These understandings not only shed light on the underlying mechanisms of graphene flake sliding on the gold substrates but also may guide the design and fabrication of nanoscale graphene-based devices.

{pi} junction and spontaneous current state in a superfluid Fermi gas

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kashimura, Takashi; Tsuchiya, Shunji; CREST

2011-07-15

We discuss an idea to realize a spontaneous current in a superfluid Fermi gas. When a polarized Fermi superfluid (N{sub {up_arrow}}>N{sub {down_arrow}}, where N{sub {sigma}} is the number of atoms in the hyperfine state described by pseudospin {sigma}={up_arrow},{down_arrow}) is loaded onto a ring-shaped trap with a weak potential barrier, some excess atoms ({Delta}N=N{sub {up_arrow}}-N{sub {down_arrow}}) are localized around the barrier. As shown in our previous paper [T. Kashimura, S. Tsuchiya, and Y. Ohashi, Phys. Rev. A 82, 033617 (2010)], this polarized potential barrier works as a {pi} junction in the sense that the superfluid order parameter changes its sign acrossmore » the barrier. Because of this, the phase of the superfluid order parameter outside the junction is shown to be twisted by {pi} along the ring, which naturally leads to a circulating supercurrent. While the ordinary supercurrent state is obtained as a metastable state, this spontaneous current state is shown to be more stable than the case with no current. Our results indicate that localized excess atoms would be useful for the manipulation of the superfluid order parameter in cold Fermi gases.« less

Formation of bimetallic clusters in superfluid helium nanodroplets analysed by atomic resolution electron tomography

PubMed Central

Haberfehlner, Georg; Thaler, Philipp; Knez, Daniel; Volk, Alexander; Hofer, Ferdinand; Ernst, Wolfgang E.; Kothleitner, Gerald

2015-01-01

Structure, shape and composition are the basic parameters responsible for properties of nanoscale materials, distinguishing them from their bulk counterparts. To reveal these in three dimensions at the nanoscale, electron tomography is a powerful tool. Advancing electron tomography to atomic resolution in an aberration-corrected transmission electron microscope remains challenging and has been demonstrated only a few times using strong constraints or extensive filtering. Here we demonstrate atomic resolution electron tomography on silver/gold core/shell nanoclusters grown in superfluid helium nanodroplets. We reveal morphology and composition of a cluster identifying gold- and silver-rich regions in three dimensions and we estimate atomic positions without using any prior information and with minimal filtering. The ability to get full three-dimensional information down to the atomic scale allows understanding the growth and deposition process of the nanoclusters and demonstrates an approach that may be generally applicable to all types of nanoscale materials. PMID:26508471

Low gravity containerless processing of immiscible gold rhodium alloys

NASA Technical Reports Server (NTRS)

Andrews, J. Barry

1986-01-01

Under normal one-g conditions immiscible alloys segregate extensively during solidification due to sedementation of the more dense of the immiscible liquid phases. However, under low-g conditions it should be possible to form a dispersion of the two immiscible liquids and maintain this dispersed structure during solidification. Immiscible (hypermonotectic) gold-rhodium alloys were processed in the Marshall Space Flight Center 105 meter drop tube in order to investigate the influence of low gravity, containerless solidification on their microstructure. Hypermonotectic alloys composed of 65 atomic % rhodium exhibited a tendency for the gold rich liquid to wet the outer surface of the containerless processed samples. This tendency led to extensive segregation in several cases. However, well dispersed microstructures consisting of 2 to 3 micron diameter rhodium-rich spheres in a gold-rich matrix were produced in 23.4 atomic % rhodium alloys. This is one of the best dispersions obtained in research on immiscible alloy-systems to data.

AuNx stabilization with interstitial nitrogen atoms: A Density Functional Theory Study

NASA Astrophysics Data System (ADS)

Quintero, J. H.; Gonzalez-Hernandez, R.; Ospina, R.; Mariño, A.

2017-06-01

Researchers have been studying 4d and 5d Series Transition Metal Nitrides lately as a result of the experimental production of AuN, PtN, CuN. In this paper, we used the Density Functional Theory (DFT) implementing a pseudopotential plane-wave method to study the incorporation of nitrogen atoms in the face-centered cube (fcc) lattice of gold (Au). First, we took the fcc structure of gold, and gradually located the nitrogen atoms in tetrahedral (TH) and octahedral (OH) interstitial sites. AuN stabilized in: 2OH (30%), 4OH and 4TH (50%), 4OH - 2TH (close to the wurtzite structure) and 6TH (60%). This leads us to think that AuN behaves like a Transition Metal Nitride since the nitrogen atoms look for tetrahedral sites.

Gating of Connexin Channels by transjunctional-voltage: Conformations and models of open and closed states.

PubMed

Bargiello, Thaddeus A; Oh, Seunghoon; Tang, Qingxiu; Bargiello, Nicholas K; Dowd, Terry L; Kwon, Taekyung

2018-01-01

Voltage is an important physiologic regulator of channels formed by the connexin gene family. Connexins are unique among ion channels in that both plasma membrane inserted hemichannels (undocked hemichannels) and intercellular channels (aggregates of which form gap junctions) have important physiological roles. The hemichannel is the fundamental unit of gap junction voltage-gating. Each hemichannel displays two distinct voltage-gating mechanisms that are primarily sensitive to a voltage gradient formed along the length of the channel pore (the transjunctional voltage) rather than sensitivity to the absolute membrane potential (V m or V i-o ). These transjunctional voltage dependent processes have been termed V j - or fast-gating and loop- or slow-gating. Understanding the mechanism of voltage-gating, defined as the sequence of voltage-driven transitions that connect open and closed states, first and foremost requires atomic resolution models of the end states. Although ion channels formed by connexins were among the first to be characterized structurally by electron microscopy and x-ray diffraction in the early 1980's, subsequent progress has been slow. Much of the current understanding of the structure-function relations of connexin channels is based on two crystal structures of Cx26 gap junction channels. Refinement of crystal structure by all-atom molecular dynamics and incorporation of charge changing protein modifications has resulted in an atomic model of the open state that arguably corresponds to the physiologic open state. Obtaining validated atomic models of voltage-dependent closed states is more challenging, as there are currently no methods to solve protein structure while a stable voltage gradient is applied across the length of an oriented channel. It is widely believed that the best approach to solve the atomic structure of a voltage-gated closed ion channel is to apply different but complementary experimental and computational methods and to use the resulting information to derive a consensus atomic structure that is then subjected to rigorous validation. In this paper, we summarize our efforts to obtain and validate atomic models of the open and voltage-driven closed states of undocked connexin hemichannels. This article is part of a Special Issue entitled: Gap Junction Proteins edited by Jean Claude Herve. Copyright © 2017 Elsevier B.V. All rights reserved.

Gold Nanoparticles on Functionalized Silicon Substrate under Coulomb Blockade Regime: An Experimental and Theoretical Investigation.

PubMed

Pluchery, Olivier; Caillard, Louis; Dollfus, Philippe; Chabal, Yves J

2018-01-18

Single charge electronics offer a way for disruptive technology in nanoelectronics. Coulomb blockade is a realistic way for controlling the electric current through a device with the accuracy of one electron. In such devices the current exhibits a step-like increase upon bias which reflects the discrete nature of the fundamental charge. We have assembled a double tunnel junction on an oxide-free silicon substrate that exhibits Coulomb staircase characteristics using gold nanoparticles (AuNPs) as Coulomb islands. The first tunnel junction is an insulating layer made of a grafted organic monolayer (GOM) developed for this purpose. The GOM also serves for attaching AuNPs covalently. The second tunnel junction is made by the tip of an STM. We show that this device exhibits reproducible Coulomb blockade I-V curves at 40 K in vacuum. We also show that depending on the doping of the silicon substrate, the whole Coulomb staircase can be adjusted. We have developed a simulation approach based on the orthodox theory that was completed by calculating the bias dependent tunnel barriers and by including an accurate calculation of the band bending. This model accounts for the experimental data and the doping dependence of Coulomb oscillations. This study opens new perspectives toward designing new kind of single electron transistors (SET) based on this dependence of the Coulomb staircase with the charge carrier concentration.

A comprehensive study of catalytic, morphological and electronic properties of ligand-protected gold nanoclusters using XPS, STM, XAFS, and TPD techniques

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wu, Qiyuan; Cen, Jiajie; Zhao, Yue

Ultra-small gold nanoclusters were synthesized via a ligand exchange method and deposited onto different TiO2 supports to study their properties. STM imaging revealed that the as-synthesized gold nanoclusters had 2-D morphology consisting of monolayers of gold atoms. In conclusion, subsequent XPS, XAFS, and CO oxidation TPD results indicated that heat treatments of gold clusters at different temperatures significantly altered their electronic and catalytic properties due to ligand deprotection and cluster agglomeration.

A comprehensive study of catalytic, morphological and electronic properties of ligand-protected gold nanoclusters using XPS, STM, XAFS, and TPD techniques

DOE PAGES

Wu, Qiyuan; Cen, Jiajie; Zhao, Yue; ...

2017-12-08

Ultra-small gold nanoclusters were synthesized via a ligand exchange method and deposited onto different TiO2 supports to study their properties. STM imaging revealed that the as-synthesized gold nanoclusters had 2-D morphology consisting of monolayers of gold atoms. In conclusion, subsequent XPS, XAFS, and CO oxidation TPD results indicated that heat treatments of gold clusters at different temperatures significantly altered their electronic and catalytic properties due to ligand deprotection and cluster agglomeration.

A comprehensive picture in the view of atomic scale on piezoelectricity of ZnO tunnel junctions: The first principles simulation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Genghong; Zhu, Jia; Jiang, Gelei

Piezoelectricity is closely related with the performance and application of piezoelectric devices. It is a crucial issue to understand its detailed fundamental for designing functional devices with more peculiar performances. Basing on the first principles simulations, the ZnO piezoelectric tunnel junction is taken as an example to systematically investigate its piezoelectricity (including the piezopotential energy, piezoelectric field, piezoelectric polarization and piezocharge) and explore their correlation. The comprehensive picture of the piezoelectricity in the ZnO tunnel junction is revealed at atomic scale and it is verified to be the intrinsic characteristic of ZnO barrier, independent of its terminated surface but dependentmore » on its c axis orientation and the applied strain. In the case of the ZnO c axis pointing from right to left, an in-plane compressive strain will induce piezocharges (and a piezopotential energy drop) with positive and negative signs (negative and positive signs) emerging respectively at the left and right terminated surfaces of the ZnO barrier. Meanwhile a piezoelectric polarization (and a piezoelectric field) pointing from right to left (from left to right) are also induced throughout the ZnO barrier. All these piezoelectric physical quantities would reverse when the applied strain switches from compressive to tensile. This study provides an atomic level insight into the fundamental behavior of the piezoelectricity of the piezoelectric tunnel junction and should have very useful information for future designs of piezoelectric devices.« less

Effect of gold nanoparticle on stability of the DNA molecule: A study of molecular dynamics simulation.

PubMed

Izanloo, Cobra

2017-09-02

An understanding of the mechanism of DNA interactions with gold nanoparticles is useful in today medicine applications. We have performed a molecular dynamics simulation on a B-DNA duplex (CCTCAGGCCTCC) in the vicinity of a gold nanoparticle with a truncated octahedron structure composed of 201 gold atoms (diameter ∼1.8 nm) to investigate gold nanoparticle (GNP) effects on the stability of DNA. During simulation, the nanoparticle is closed to DNA and phosphate groups direct the particles into the major grooves of the DNA molecule. Because of peeling and untwisting states that are occur at end of DNA, the nucleotide base lies flat on the surface of GNP. The configuration entropy is estimated using the covariance matrix of atom-positional fluctuations for different bases. The results show that when a gold nanoparticle has interaction with DNA, entropy increases. The results of conformational energy and the hydrogen bond numbers for DNA indicated that DNA becomes unstable in the vicinity of a gold nanoparticle. The radial distribution function was calculated for water hydrogen-phosphate oxygen pairs. Almost for all nucleotide, the presence of a nanoparticle around DNA caused water molecules to be released from the DNA duplex and cations were close to the DNA.

Gold nanoprobes for theranostics

PubMed Central

Panchapakesan, Balaji; Book-Newell, Brittany; Sethu, Palaniappan; Rao, Madhusudhana; Irudayaraj, Joseph

2011-01-01

Gold nanoprobes have become attractive diagnostic and therapeutic agents in medicine and life sciences research owing to their reproducible synthesis with atomic level precision, unique physical and chemical properties, versatility of their morphologies, flexibility in functionalization, ease of targeting, efficiency in drug delivery and opportunities for multimodal therapy. This review highlights some of the recent advances and the potential for gold nanoprobes in theranostics. PMID:22122586

Suppression and enhancement of decoherence in an atomic Josephson junction

NASA Astrophysics Data System (ADS)

Japha, Yonathan; Zhou, Shuyu; Keil, Mark; Folman, Ron; Henkel, Carsten; Vardi, Amichay

2016-05-01

We investigate the role of interatomic interactions when a Bose gas, in a double-well potential with a finite tunneling probability (a ‘Bose-Josephson junction’), is exposed to external noise. We examine the rate of decoherence of a system initially in its ground state with equal probability amplitudes in both sites. The noise may induce two kinds of effects: firstly, random shifts in the relative phase or number difference between the two wells and secondly, loss of atoms from the trap. The effects of induced phase fluctuations are mitigated by atom-atom interactions and tunneling, such that the dephasing rate may be suppressed by half its single-atom value. Random fluctuations may also be induced in the population difference between the wells, in which case atom-atom interactions considerably enhance the decoherence rate. A similar scenario is predicted for the case of atom loss, even if the loss rates from the two sites are equal. We find that if the initial state is number-squeezed due to interactions, then the loss process induces population fluctuations that reduce the coherence across the junction. We examine the parameters relevant for these effects in a typical atom chip device, using a simple model of the trapping potential, experimental data, and the theory of magnetic field fluctuations near metallic conductors. These results provide a framework for mapping the dynamical range of barriers engineered for specific applications and set the stage for more complex atom circuits (‘atomtronics’).

Thermal stability of supported gold nanoparticles

NASA Astrophysics Data System (ADS)

Turba, Timothy Fredrick

Nanoparticle gold is of interest for a wide array of applications including catalysis, gas sensing, and light absorption for color filters and optical switches. Many of these applications are dependent upon the particles having sizes <5nm. In this paper, the thermal stability of nanoparticle gold is evaluated. Unsupported gold nanoparticles can grow (and in some cases double their size) even at room temperature. An important approach to stabilizing gold nanoparticles is through an interaction with a suitable substrate support material. Semiconductor substrates such as GaN are important supports for gold nanoparticles for applications such as sensors, but GaN does not provide a significant stabilizing effect at high temperatures. This paper covers a number of different substrate materials and in particular shows that for some substrates, such as SiO2, gold nanoparticles can be stable at temperatures up to 500°C, which is significantly above the Tammann temperature for bulk gold (395°C). In this dissertation, gold nanoparticles are shown to have complete stability on aluminum-supported silica nanosprings at 550°C in air. This stability window is one of the highest reported for nanoparticle gold and potentially enables a number of applications for this highly active catalyst. X-ray photoelectron spectroscopy measurements were performed before and after heating to 550°C to determine the nature of the interaction between gold and SiO2. A 1.2 eV drop in gold 4f binding energy after heating signified a shift to anionic gold particles (i.e., Au delta-) indicative of strong bonds to oxygen vacancies with neighboring Sidelta+ atoms. Heating in hydrogen at 550°C resulted in a binding energy decrease of 0.4 eV due to an increased fraction of particles with decreased coordination numbers (i.e., more atoms at edges and corners). Lastly, heating gold nanoparticles in an atmosphere of 10% relative humidity at 550°C resulted in apparent encapsulation of the gold.

Effect of surface roughness on substrate-tuned gold nanoparticle gap plasmon resonances.

PubMed

Lumdee, Chatdanai; Yun, Binfeng; Kik, Pieter G

2015-03-07

The effect of nanoscale surface roughness on the gap plasmon resonance of gold nanoparticles on thermally evaporated gold films is investigated experimentally and numerically. Single-particle scattering spectra obtained from 80 nm diameter gold particles on a gold film show significant particle-to-particle variation of the peak scattering wavelength of ±28 nm. The experimental results are compared with numerical simulations of gold nanoparticles positioned on representative rough gold surfaces, modeled based on atomic force microscopy measurements. The predicted spectral variation and average resonance wavelength show good agreement with the measured data. The study shows that nanometer scale surface roughness can significantly affect the performance of gap plasmon-based devices.

Graphene/MoS2 heterostructures as templates for growing two-dimensional metals: Predictions from ab initio calculations

NASA Astrophysics Data System (ADS)

Šljivančanin, Željko; Belić, Milivoj

2017-09-01

Preparation of single-atom-thick layers of ordinary metals has been a challenging task since their closely packed atoms lack layered structure with highly anisotropic bonding. Using computational modeling based on density functional theory we showed that graphene/MoS2 heterostructures can be used as suitable templates to grow stable two-dimensional (2D) clusters, as well as extended monoatomic layers of metals with nonlayered structure in the bulk. Considering gold and lithium as two metals with markedly different properties, we found that Li intercalants strengthen coupling between graphene (G) and MoS2, mainly due to electrostatic attraction of 2D materials with positively charged Li atoms. However, intercalation with large Au atoms gives rise to a significant increase in the distance between G and MoS2 and thus, weakens their interaction. In addition to strong preference for 2D growth, we demonstrated that Au intercalants weakly interact with both G and MoS2, and hence G /MoS2 vertical heterostructures could be a promising framework to prepare gold 2D structures with electronic properties closely resembling those of the hypothetical free-standing hexagonal gold monolayer.

Transport in ultrathin gold films decorated with magnetic Gd atoms

NASA Astrophysics Data System (ADS)

Alemani, Micol; Helgren, Erik; Hugel, Addison; Hellman, Frances

2008-03-01

We have performed four-probe transport measurements of ultrathin Au films decorated with Gd ad-atoms. The samples were prepared by quench condensation, i.e., sequential evaporation on a cryogenically cooled substrate under UHV conditions while monitoring the film thickness and resistance. Electrically continuous Au films at thickness of about 2 mono-layers of material are grown on an amorphous Ge wetting layer. The quench condensation method provides a sensitive control on the sample growth process, allowing us to tune the morphological and electrical configuration of the system. The ultrathin gold films develop from an insulating to a metallic state as a function of film thickness. The temperature dependence of the Au conductivity for different thickness is studied. It evolves from hopping transport for the insulating films, to a ln T dependence for thicker films. For gold films in the insulating regime we found a decreasing resistance by adding Gd. This is in agreement with a decreasing tunneling barrier height between metallic atoms. The Gd magnetic moments are randomly oriented for isolated atoms. This magnetic disorder leads to scattering of the charge carriers and a reduced conductivity compared to nonmagnetic materials.

Experimental demonstration of single electron transistors featuring SiO{sub 2} plasma-enhanced atomic layer deposition in Ni-SiO{sub 2}-Ni tunnel junctions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Karbasian, Golnaz, E-mail: Golnaz.Karbasian.1@nd.edu; McConnell, Michael S.; Orlov, Alexei O.

The authors report the use of plasma-enhanced atomic layer deposition (PEALD) to fabricate single-electron transistors (SETs) featuring ultrathin (≈1 nm) tunnel-transparent SiO{sub 2} in Ni-SiO{sub 2}-Ni tunnel junctions. They show that, as a result of the O{sub 2} plasma steps in PEALD of SiO{sub 2}, the top surface of the underlying Ni electrode is oxidized. Additionally, the bottom surface of the upper Ni layer is also oxidized where it is in contact with the deposited SiO{sub 2}, most likely as a result of oxygen-containing species on the surface of the SiO{sub 2}. Due to the presence of these surface parasitic layersmore » of NiO, which exhibit features typical of thermally activated transport, the resistance of Ni-SiO{sub 2}-Ni tunnel junctions is drastically increased. Moreover, the transport mechanism is changed from quantum tunneling through the dielectric barrier to one consistent with thermally activated resistors in series with tunnel junctions. The reduction of NiO to Ni is therefore required to restore the metal-insulator-metal (MIM) structure of the junctions. Rapid thermal annealing in a forming gas ambient at elevated temperatures is presented as a technique to reduce both parasitic oxide layers. This method is of great interest for devices that rely on MIM tunnel junctions with ultrathin barriers. Using this technique, the authors successfully fabricated MIM SETs with minimal trace of parasitic NiO component. They demonstrate that the properties of the tunnel barrier in nanoscale tunnel junctions (with <10{sup −15} m{sup 2} in area) can be evaluated by electrical characterization of SETs.« less

The structure and binding mode of citrate in the stabilization of gold nanoparticles

NASA Astrophysics Data System (ADS)

Al-Johani, Hind; Abou-Hamad, Edy; Jedidi, Abdesslem; Widdifield, Cory M.; Viger-Gravel, Jasmine; Sangaru, Shiv Shankar; Gajan, David; Anjum, Dalaver H.; Ould-Chikh, Samy; Hedhili, Mohamed Nejib; Gurinov, Andrei; Kelly, Michael J.; El Eter, Mohamad; Cavallo, Luigi; Emsley, Lyndon; Basset, Jean-Marie

2017-09-01

Elucidating the binding mode of carboxylate-containing ligands to gold nanoparticles (AuNPs) is crucial to understand their stabilizing role. A detailed picture of the three-dimensional structure and coordination modes of citrate, acetate, succinate and glutarate to AuNPs is obtained by 13C and 23Na solid-state NMR in combination with computational modelling and electron microscopy. The binding between the carboxylates and the AuNP surface is found to occur in three different modes. These three modes are simultaneously present at low citrate to gold ratios, while a monocarboxylate monodentate (1κO1) mode is favoured at high citrate:gold ratios. The surface AuNP atoms are found to be predominantly in the zero oxidation state after citrate coordination, although trace amounts of Auδ+ are observed. 23Na NMR experiments show that Na+ ions are present near the gold surface, indicating that carboxylate binding occurs as a 2e- L-type interaction for each oxygen atom involved. This approach has broad potential to probe the binding of a variety of ligands to metal nanoparticles.

Experiments with BECs in a Painted Potential: Atom SQUID, Matter Wave Bessel Beams, and Matter Wave Circuits

NASA Astrophysics Data System (ADS)

Boshier, Malcolm; Ryu, Changhyun; Blackburn, Paul; Blinova, Alina; Henderson, Kevin

2014-05-01

The painted potential is a time-averaged optical dipole potential which is able to create arbitrary and dynamic two dimensional potentials for Bose Einstein condensates (BECs). This poster reports three recent experiments using this technique. First, we have realized the dc atom SQUID geometry of a BEC in a toroidal trap with two Josephson junctions. We observe Josephson effects, measure the critical current of the junctions, and find dynamic behavior that is in good agreement with the simple Josephson equations for a tunnel junction with the ideal sinusoidal current-phase relation expected for the parameters of the experiment. Second, we have used free expansion of a rotating toroidal BEC to create matter wave Bessel beams, which are of interest because perfect Bessel beams (plane waves with amplitude profiles described by Bessel functions) propagate without diffraction. Third, we have realized the basic circuit elements necessary to create complex matter wave circuits. We launch BECs at arbitrary velocity along straight waveguides, propagate them around curved waveguides and stadium-shaped waveguide traps, and split them coherently at y-junctions that can also act as switches. Supported by LANL/LDRD.

Formation of neutral and charged gold carbonyls on highly facetted gold nanostructures

NASA Astrophysics Data System (ADS)

Chau, Thoi-Dai; Visart de Bocarmé, Thierry; Kruse, Norbert; Wang, Richard L. C.; Kreuzer, Hans Jürgen

2003-12-01

We show that gold mono- and di-carbonyls are formed on gold field emitter tips during interaction with carbon monoxide gas at room temperature and in the presence of high electrostatic fields. The experiments are done in a time-of-flight atom probe to obtain mass spectra. The yield of monocarbonyl cations is about twice that of di-carbonyl ions. Density functional theory calculations are reported that explain the field stabilization of adsorbed carbonyls and the desorption yield of their cations.

Structure–property relationships in atomic-scale junctions: Histograms and beyond

DOE PAGES

Mark S. Hybertsen; Venkataraman, Latha

2016-03-03

Over the past 10 years, there has been tremendous progress in the measurement, modeling and understanding of structure–function relationships in single molecule junctions. Numerous research groups have addressed significant scientific questions, directed both to conductance phenomena at the single molecule level and to the fundamental chemistry that controls junction functionality. Many different functionalities have been demonstrated, including single-molecule diodes, optically and mechanically activated switches, and, significantly, physical phenomena with no classical analogues, such as those based on quantum interference effects. Experimental techniques for reliable and reproducible single molecule junction formation and characterization have led to this progress. In particular, themore » scanning tunneling microscope based break-junction (STM-BJ) technique has enabled rapid, sequential measurement of large numbers of nanoscale junctions allowing a statistical analysis to readily distinguish reproducible characteristics. Furthermore, harnessing fundamental link chemistry has provided the necessary chemical control over junction formation, enabling measurements that revealed clear relationships between molecular structure and conductance characteristics.« less

Structure–property relationships in atomic-scale junctions: Histograms and beyond

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mark S. Hybertsen; Venkataraman, Latha

Over the past 10 years, there has been tremendous progress in the measurement, modeling and understanding of structure–function relationships in single molecule junctions. Numerous research groups have addressed significant scientific questions, directed both to conductance phenomena at the single molecule level and to the fundamental chemistry that controls junction functionality. Many different functionalities have been demonstrated, including single-molecule diodes, optically and mechanically activated switches, and, significantly, physical phenomena with no classical analogues, such as those based on quantum interference effects. Experimental techniques for reliable and reproducible single molecule junction formation and characterization have led to this progress. In particular, themore » scanning tunneling microscope based break-junction (STM-BJ) technique has enabled rapid, sequential measurement of large numbers of nanoscale junctions allowing a statistical analysis to readily distinguish reproducible characteristics. Furthermore, harnessing fundamental link chemistry has provided the necessary chemical control over junction formation, enabling measurements that revealed clear relationships between molecular structure and conductance characteristics.« less

10 CFR 1002.11 - Description of official seal.

Code of Federal Regulations, 2013 CFR

2013-01-01

... is emblazoned a gold-colored symbolic sun, atom, oil derrick, windmill, and dynamo. It is crested by... increasing demands for energy. The sun, atom, oil derrick, windmill, and dynamo serve as representative...

10 CFR 1002.11 - Description of official seal.

Code of Federal Regulations, 2010 CFR

2010-01-01

... is emblazoned a gold-colored symbolic sun, atom, oil derrick, windmill, and dynamo. It is crested by... increasing demands for energy. The sun, atom, oil derrick, windmill, and dynamo serve as representative...

10 CFR 1002.11 - Description of official seal.

Code of Federal Regulations, 2011 CFR

2011-01-01

... is emblazoned a gold-colored symbolic sun, atom, oil derrick, windmill, and dynamo. It is crested by... increasing demands for energy. The sun, atom, oil derrick, windmill, and dynamo serve as representative...

10 CFR 1002.11 - Description of official seal.

Code of Federal Regulations, 2014 CFR

2014-01-01

... is emblazoned a gold-colored symbolic sun, atom, oil derrick, windmill, and dynamo. It is crested by... increasing demands for energy. The sun, atom, oil derrick, windmill, and dynamo serve as representative...

10 CFR 1002.11 - Description of official seal.

Code of Federal Regulations, 2012 CFR

2012-01-01

... is emblazoned a gold-colored symbolic sun, atom, oil derrick, windmill, and dynamo. It is crested by... increasing demands for energy. The sun, atom, oil derrick, windmill, and dynamo serve as representative...

Atom chips in the real world: the effects of wire corrugation

NASA Astrophysics Data System (ADS)

Schumm, T.; Estève, J.; Figl, C.; Trebbia, J.-B.; Aussibal, C.; Nguyen, H.; Mailly, D.; Bouchoule, I.; Westbrook, C. I.; Aspect, A.

2005-02-01

We present a detailed model describing the effects of wire corrugation on the trapping potential experienced by a cloud of atoms above a current carrying micro wire. We calculate the distortion of the current distribution due to corrugation and then derive the corresponding roughness in the magnetic field above the wire. Scaling laws are derived for the roughness as a function of height above a ribbon shaped wire. We also present experimental data on micro wire traps using cold atoms which complement some previously published measurements [CITE] and which demonstrate that wire corrugation can satisfactorily explain our observations of atom cloud fragmentation above electroplated gold wires. Finally, we present measurements of the corrugation of new wires fabricated by electron beam lithography and evaporation of gold. These wires appear to be substantially smoother than electroplated wires.

Equivalent Circuit of the Neuro-Electronic Junction for Signal Recordings From Planar and Engulfed Micro-Nano-Electrodes.

PubMed

Massobrio, Giuseppe; Martinoia, Sergio; Massobrio, Paolo

2018-02-01

In the latest years, several attempts to develop extracellular microtransducers to record electrophysiological activity of excitable cells have been done. In particular, many efforts have been oriented to increase the coupling conditions, and, thus, improving the quality of the recorded signal. Gold mushroom-shaped microelectrodes (GMμE) are an example of nano-devices to achieve those requirements. In this study, we developed an equivalent electrical circuit of the neuron-microelectrode system interface to simulate signal recordings from both planar and engulfed micro-nano-electrodes. To this purpose, models of the neuron, planar, gold planar microelectrode, and GMμE, neuro-electronic junction (microelectrode-electrolyte interface, cleft effect, and protein-glycocalyx electric double layer) are presented. Then, neuronal electrical activity is simulated by Hspice software, and analyzed as a function of the most sensitive biophysical models parameters, such as the neuron-microelectrode cleft width, spreading and seal resistances, ion-channel densities, double-layer properties, and microelectrode geometries. Results are referenced to the experimentally recorded electrophysiological neuronal signals reported in the literature.

Monitoring Demineralization and Subsequent Remineralization of Human Teeth at the Dentin-Enamel Junction with Atomic Force Microscopy.

PubMed

Lechner, Bob-Dan; Röper, Stephanie; Messerschmidt, Jens; Blume, Alfred; Magerle, Robert

2015-09-02

Using atomic force microscopy, we monitored the nanoscale surface morphology of human teeth at the dentin-enamel junction after performing successive demineralization steps with an acidic soft drink. Subsequently, we studied the remineralization process with a paste containing calcium and phosphate ions. Repeated atomic force microscopy imaging of the same sample areas on the sample allowed us to draw detailed conclusions regarding the specific mechanism of the demineralization process and the subsequent remineralization process. The about 1-μm-deep grooves that are caused by the demineralization process were preferentially filled with deposited nanoparticles, leading to smoother enamel and dentine surfaces after 90 min exposure to the remineralizing agent. The deposited material is found to homogeneously cover the enamel and dentine surfaces in the same manner. The temporal evolution of the surface roughness indicates that the remineralization caused by the repair paste proceeds in two distinct successive phases.

Modeling single molecule junction mechanics as a probe of interface bonding

NASA Astrophysics Data System (ADS)

Hybertsen, Mark S.

2017-03-01

Using the atomic force microscope based break junction approach, applicable to metal point contacts and single molecule junctions, measurements can be repeated thousands of times resulting in rich data sets characterizing the properties of an ensemble of nanoscale junction structures. This paper focuses on the relationship between the measured force extension characteristics including bond rupture and the properties of the interface bonds in the junction. A set of exemplary model junction structures has been analyzed using density functional theory based calculations to simulate the adiabatic potential surface that governs the junction elongation. The junction structures include representative molecules that bond to the electrodes through amine, methylsulfide, and pyridine links. The force extension characteristics are shown to be most effectively analyzed in a scaled form with maximum sustainable force and the distance between the force zero and force maximum as scale factors. Widely used, two parameter models for chemical bond potential energy versus bond length are found to be nearly identical in scaled form. Furthermore, they fit well to the present calculations of N-Au and S-Au donor-acceptor bonds, provided no other degrees of freedom are allowed to relax. Examination of the reduced problem of a single interface, but including relaxation of atoms proximal to the interface bond, shows that a single-bond potential form renormalized by an effective harmonic potential in series fits well to the calculated results. This allows relatively accurate extraction of the interface bond energy. Analysis of full junction models shows cooperative effects that go beyond the mechanical series inclusion of the second bond in the junction, the spectator bond that does not rupture. Calculations for a series of diaminoalkanes as a function of molecule length indicate that the most important cooperative effect is due to the interactions between the dipoles induced by the donor-acceptor bond formation at the junction interfaces. The force extension characteristic of longer molecules such as diaminooctane, where the dipole interaction effects drop to a negligible level, accurately fit to the renormalized single-bond potential form. The results suggest that measured force extension characteristics for single molecule junctions could be analyzed with a modified potential form that accounts for the energy stored in deformable mechanical components in series.

Modeling single molecule junction mechanics as a probe of interface bonding

DOE PAGES

Hybertsen, Mark S.

2017-03-07

Using the atomic force microscope based break junction approach, applicable to metal point contacts and single molecule junctions, measurements can be repeated thousands of times resulting in rich data sets characterizing the properties of an ensemble of nanoscale junction structures. This paper focuses on the relationship between the measured force extension characteristics including bond rupture and the properties of the interface bonds in the junction. We analyzed a set of exemplary model junction structures using density functional theory based calculations to simulate the adiabatic potential surface that governs the junction elongation. The junction structures include representative molecules that bond tomore » the electrodes through amine, methylsulfide, and pyridine links. The force extension characteristics are shown to be most effectively analyzed in a scaled form with maximum sustainable force and the distance between the force zero and force maximum as scale factors. Widely used, two parameter models for chemical bond potential energy versus bond length are found to be nearly identical in scaled form. Furthermore, they fit well to the present calculations of N–Au and S–Au donor-acceptor bonds, provided no other degrees of freedom are allowed to relax. Examination of the reduced problem of a single interface, but including relaxation of atoms proximal to the interface bond, shows that a single-bond potential form renormalized by an effective harmonic potential in series fits well to the calculated results. This, then, allows relatively accurate extraction of the interface bond energy. Analysis of full junction models shows cooperative effects that go beyond the mechanical series inclusion of the second bond in the junction, the spectator bond that does not rupture. Calculations for a series of diaminoalkanes as a function of molecule length indicate that the most important cooperative effect is due to the interactions between the dipoles induced by the donor-acceptor bond formation at the junction interfaces. The force extension characteristic of longer molecules such as diaminooctane, where the dipole interaction effects drop to a negligible level, accurately fit to the renormalized single-bond potential form. Our results suggest that measured force extension characteristics for single molecule junctions could be analyzed with a modified potential form that accounts for the energy stored in deformable mechanical components in series.« less

Modeling single molecule junction mechanics as a probe of interface bonding

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hybertsen, Mark S.

Using the atomic force microscope based break junction approach, applicable to metal point contacts and single molecule junctions, measurements can be repeated thousands of times resulting in rich data sets characterizing the properties of an ensemble of nanoscale junction structures. This paper focuses on the relationship between the measured force extension characteristics including bond rupture and the properties of the interface bonds in the junction. We analyzed a set of exemplary model junction structures using density functional theory based calculations to simulate the adiabatic potential surface that governs the junction elongation. The junction structures include representative molecules that bond tomore » the electrodes through amine, methylsulfide, and pyridine links. The force extension characteristics are shown to be most effectively analyzed in a scaled form with maximum sustainable force and the distance between the force zero and force maximum as scale factors. Widely used, two parameter models for chemical bond potential energy versus bond length are found to be nearly identical in scaled form. Furthermore, they fit well to the present calculations of N–Au and S–Au donor-acceptor bonds, provided no other degrees of freedom are allowed to relax. Examination of the reduced problem of a single interface, but including relaxation of atoms proximal to the interface bond, shows that a single-bond potential form renormalized by an effective harmonic potential in series fits well to the calculated results. This, then, allows relatively accurate extraction of the interface bond energy. Analysis of full junction models shows cooperative effects that go beyond the mechanical series inclusion of the second bond in the junction, the spectator bond that does not rupture. Calculations for a series of diaminoalkanes as a function of molecule length indicate that the most important cooperative effect is due to the interactions between the dipoles induced by the donor-acceptor bond formation at the junction interfaces. The force extension characteristic of longer molecules such as diaminooctane, where the dipole interaction effects drop to a negligible level, accurately fit to the renormalized single-bond potential form. Our results suggest that measured force extension characteristics for single molecule junctions could be analyzed with a modified potential form that accounts for the energy stored in deformable mechanical components in series.« less

Brittle deformation along the Gulf of Alaska margin in response to Paleocene-Eocene triple junction migration: in Sisson

USGS Publications Warehouse

Haeussler, Peter J.; Bradley, Dwight C.; Goldfarb, Richard J.

2003-01-01

A spreading center was subducted diachronously along a 2200 km segment of what is now the Gulf of Alaska margin between 61 and 50 Ma, and left in its wake near-trench intrusions and high-T, low-P metamorphic rocks. Gold-quartz veins and dikes, linked to ridge subduction by geochronological and relative timing evidence, provide a record of brittle deformation during and after passage of the ridge. The gold-quartz veins are typically hosted by faults, and their regional extent indicates there was widespread deformation of the forearc above the slab window at the time of ridge subduction. Considerable variability in the strain pattern was associated with the slab window and the trailing plate. A diffuse network of dextral, sinistral, and normal faults hosted small lode-gold deposits (<50,000 oz) in south-central Alaska, whereas crustal-scale dextral faults in southeastern Alaska are spatially associated with large gold deposits (up to 800,000 oz).We interpret the gold-quartz veins as having formed above an eastward-migrating slab window, where the forearc crust responded to the diminishing influence of the forward subducting plate, the increasing influence of the trailing plate, and the thermal pulse and decreased basal friction from the slab window. In addition, extensional deformation of the forearc resulted from the diverging motions of the two oceanic plates at the margins of the slab window. Factors that complicate interpretations of fault kinematics and near-trench dike orientations include a change in plate motions at ca. 52 Ma, northward translation of the accretionary complex, oroclinal bending of the south-central Alaska margin, and subduction of transform segments. We find the pattern of syn-ridge subduction faulting in southern Alaska is remarkably similar to brittle faults near the Chile triple junction and to earthquake focal mechanisms in the Woodlark basin - the two modern sites of ridge subduction. Therefore, extensional and strike-slip deformation above slab windows may be a common occurrence.

A Relativity Enhanced, Medium-Strong Au(I)···H-N Hydrogen Bond in a Protonated Phenylpyridine-Gold(I) Thiolate.

PubMed

Berger, Raphael J F; Schoiber, Jürgen; Monkowius, Uwe

2017-01-17

Gold is an electron-rich metal with a high electronegativity comparable to that of sulfur. Hence, hydrogen bonds of the Au(I)···H-E (E = electronegative element) type should be possible, but their existence is still under debate. Experimental results are scarce and often contradictory. As guidance for possible preparative work, we have theoretically investigated (ppyH)Au(SPh) (ppy = 2-phenylpyridine) bearing two monoanionic ligands which are not strongly electronegative at the same time to further increase the charge density on the gold(I) atom. The protonated pyridine nitrogen atom in ppy is geometrically ideally suited to place a proton in close proximity to the gold atom in a favorable geometry for a classical hydrogen bond arrangement. Indeed, the results of the calculations indicate that the hydrogen bonded conformation of (ppyH)Au(SPh) represents a minimum geometry with bond metrics in the expected range for medium-strong hydrogen bonds [r(N-H) = 1.043 Å, r(H···Au) = 2.060 Å, a(N-H···Au) = 141.4°]. The energy difference between the conformer containing the H···Au bond and another conformer without a hydrogen bond amounts to 7.8 kcal mol -1 , which might serve as an estimate of the hydrogen bond strength. Spectroscopic properties were calculated, yielding further characteristics of such hydrogen bonded gold species.

Effect of collector molecular structure on the wettability of gold for froth flotation

NASA Astrophysics Data System (ADS)

Moncayo-Riascos, Ivan; Hoyos, Bibian A.

2017-10-01

Molecular dynamics simulations were conducted to evaluate the alteration of the hydrophilic state of gold surfaces caused by the adsorption of collectors with different molecular structures, using the contact angle of water droplets as an evaluation parameter. Four collectors were evaluated: SDS (with twelve hydrogenated carbon atoms), PAX (with five hydrogenated carbon atoms), DTP (with two branched aliphatic chains) and MBT (with an aromatic ring). The contact angle was evaluated for coatings of a monolayer (ML) and for surface densities of 2.89 μmol/m2 for each collector. For a ML, the hydrophobic effect generated by the aromatic ring of the MBT collector is comparable with the effect of the non-polar short chain of the PAX collector. The increase in hydrophobicity for the gold surfaces achieved by collectors with aliphatic chains is because the water-collector interaction energy is significantly higher (repulsive) than the water-gold interactions (attractive). The lowest increase in hydrophobicity was achieved with the MBT collector, since the carbon-water interaction energy of the aromatic ring is stronger than the interaction with the carbon atoms in the aliphatic chains. The calculated contact angles of the water droplets deviated less than 4% with respect to the experimental values.

Spectrally resolved opacities and Rosseland and Planck mean opacities of lowly ionized gold plasmas: a detailed level-accounting investigation.

PubMed

Zeng, Jiaolong; Yuan, Jianmin

2007-08-01

Calculation details of radiative opacity for lowly ionized gold plasmas by using our developed fully relativistic detailed level-accounting approach are presented to show the importance of accurate atomic data for a quantitative reproduction of the experimental observations. Even though a huge number of transition lines are involved in the radiative absorption of high- Z plasmas so that one believes that statistical models can often give a reasonable description of their opacities, we first show in detail that an adequate treatment of physical effects, in particular the configuration interaction (including the core-valence electron correlation), is essential to produce atomic data of bound-bound and bound-free processes for gold plasmas, which are accurate enough to correctly explain the relative intensity of two strong absorption peaks experimentally observed located near photon energy of 70 and 80 eV. A detailed study is also carried out for gold plasmas of an average ionization degree sequence of 10, for both spectrally resolved opacities and Rosseland and Planck means. For comparison, results obtained by using an average atom model are also given to show that even for a relatively higher density of matter, correlation effects are also important to predict the correct positions of absorption peaks of transition arrays.

Spectroscopic Non-LTE Modeling of Highly Charged Gold Plasma

NASA Astrophysics Data System (ADS)

Dasgupta, A.; Ouart, N. D.; Giuliani, J. L.; Obenschain, S. P.; Clark, R. W.; Aglitskiy, Y.

2013-10-01

An X-ray spectrometer is under development at the Naval Research Laboratory (NRL) to investigate emissions from gold targets irradiated by the NIKE KrF facility. This effort is in support of the indirect drive campaign on the National Ignition Facility (NIF). To analyze and interpret the NIKE experimental spectra, we are theoretically exploring line emissions from a gold plasma in the M-band, i.e., 1.5 to 3.5 keV. We employ a detailed Non-LTE atomic model for ions near Ni-like gold by including an adequate number of configurations to obtain spectroscopic details in this range. The atomic states are coupled both collisionally and radiatively, including all dominant atomic processes that have significant contributions to the ionization and emitted synthetic spectra. In particular, we will investigate the effect of dielectronic recombination, which can have a dominant effect on level populations for highly ionized high Z plasmas. Since the radiation field can affect level populations through photoionization and photoexcitation, our collisional-radiative model will include non-local radiation transport. The line shapes of the strong overlapping lines will be resolved by a multifrequency radiation transport method. Synthetic spectra with radiation transport, including resonant photo-pumping, will be generated for realistic densities and temperatures to compare with the NIKE data. Work supported by DOE/NNSA.

Charge-Induced (1 x 3) Reconstruction of Au(110): Mechanistic Insights from Potentiodynamic Scanning Tunneling Microscopy in Alkali Iodide Electrolytes

DTIC Science & Technology

1994-02-01

In potassium iodide electrolyte, the usual "three-missing-row" (1 x 3) structure is seen to be generated by single gold atomic-row segments shifting...observed, involving the intermediate local formation of "one-missing-row" (I x 3) domains by removal of one-third of the top layer gold rows onto nearby...structure is achieved by aggregation of the displaced monoatomic row segments. The mechanistic value of following atomic-level reconstruction processes by

First-principles Theory of Inelastic Transport and Local Heating in Atomic Gold Wires

NASA Astrophysics Data System (ADS)

Frederiksen, Thomas; Paulsson, Magnus; Brandbyge, Mads; Jauho, Antti-Pekka

2007-04-01

We present theoretical calculations of the inelastic transport properties in atomic gold wires. Our method is based on a combination of density functional theory and non-equilibrium Green's functions. The vibrational spectra for extensive series of wire geometries have been calculated using SIESTA, and the corresponding effects in the conductance are analyzed. In particular, we focus on the heating of the active vibrational modes. By a detailed comparison with experiments we are able to estimate an order of magnitude for the external damping of the active vibrations.

Sub-nanometer Atomic Layer Deposition for Spintronics in Magnetic Tunnel Junctions Based on Graphene Spin-Filtering Membranes

PubMed Central

2014-01-01

We report on the successful integration of low-cost, conformal, and versatile atomic layer deposited (ALD) dielectric in Ni–Al2O3–Co magnetic tunnel junctions (MTJs) where the Ni is coated with a spin-filtering graphene membrane. The ALD tunnel barriers, as thin as 0.6 nm, are grown layer-by-layer in a simple, low-vacuum, ozone-based process, which yields high-quality electron-transport barriers as revealed by tunneling characterization. Even under these relaxed conditions, including air exposure of the interfaces, a significant tunnel magnetoresistance is measured highlighting the robustness of the process. The spin-filtering effect of graphene is enhanced, leading to an almost fully inversed spin polarization for the Ni electrode of −42%. This unlocks the potential of ALD for spintronics with conformal, layer-by-layer control of tunnel barriers in magnetic tunnel junctions toward low-cost fabrication and down-scaling of tunnel resistances. PMID:24988469

Coherent and dissipative transport in a Josephson junction between fermionic superfluids of 6Li atoms

NASA Astrophysics Data System (ADS)

Neri, Elettra; Scazza, Francesco; Roati, Giacomo

2018-04-01

Quantum systems out of equilibrium offer the possibility of understanding intriguing and challenging problems in modern physics. Studying transport properties is not only valuable to unveil fundamental properties of quantum matter but it is also an excellent tool for developing new quantum devices which inherently employ quantum-mechanical effects. In this contribution, we present our experimental studies on quantum transport using ultracold Fermi gases of 6Li atoms. We realize the analogous of a Josephson junction by bisecting fermionic superfluids by a thin optical barrier. We observe coherent dynamics in both the population and in the relative phase between the two reservoirs. For critical parameters, the superfluid dynamics exhibits both coherent and resistive flow due to phase-slippage events manifesting as vortices propagating into the bulk. We uncover also a regime of strong dissipation where the junction operation is irreversibly affected by vortex proliferation. Our studies open new directions for investigating dissipation and superfluid transport in strongly correlated fermionic systems.

A Rutherford Scattering Simulation with Microcomputer Graphics.

ERIC Educational Resources Information Center

Calle, Carlos I.; Wright, Lavonia F.

1989-01-01

Lists a program for a simulation of Rutherford's gold foil experiment in BASIC for both Apple II and IBM compatible computers. Compares Rutherford's model of the atom with Thompson's plum pudding model of the atom. (MVL)

Properties of the gold-sulphur interface: from self-assembled monolayers to clusters

NASA Astrophysics Data System (ADS)

Bürgi, Thomas

2015-09-01

The gold-sulphur interface of self-assembled monolayers (SAMs) was extensively studied some time ago. More recently tremendous progress has been made in the preparation and characterization of thiolate-protected gold clusters. In this feature article we address different properties of the two systems such as their structure, the mobility of the thiolates on the surface and other dynamical aspects, the chirality of the structures and characteristics related to it and their vibrational properties. SAMs and clusters are in the focus of different communities that typically use different experimental approaches to study the respective systems. However, it seems that the nature of the Au-S interfaces in the two cases is quite similar. Recent single crystal X-ray structures of thiolate-protected gold clusters reveal staple motifs characterized by gold ad-atoms sandwiched between two sulphur atoms. This finding contradicts older work on SAMs. However, newer studies on SAMs also reveal ad-atoms. Whether this finding can be generalized remains to be shown. In any case, more and more studies highlight the dynamic nature of the Au-S interface, both on flat surfaces and in clusters. At temperatures slightly above ambient thiolates migrate on the gold surface and on clusters. Evidence for desorption of thiolates at room temperature, at least under certain conditions, has been demonstrated for both systems. The adsorbed thiolate can lead to chirality at different lengths scales, which has been shown both on surfaces and for clusters. Chirality emerges from the organization of the thiolates as well as locally at the molecular level. Chirality can also be transferred from a chiral surface to an adsorbate, as evidenced by vibrational spectroscopy.

Properties of the gold-sulphur interface: from self-assembled monolayers to clusters.

PubMed

Bürgi, Thomas

2015-10-14

The gold-sulphur interface of self-assembled monolayers (SAMs) was extensively studied some time ago. More recently tremendous progress has been made in the preparation and characterization of thiolate-protected gold clusters. In this feature article we address different properties of the two systems such as their structure, the mobility of the thiolates on the surface and other dynamical aspects, the chirality of the structures and characteristics related to it and their vibrational properties. SAMs and clusters are in the focus of different communities that typically use different experimental approaches to study the respective systems. However, it seems that the nature of the Au-S interfaces in the two cases is quite similar. Recent single crystal X-ray structures of thiolate-protected gold clusters reveal staple motifs characterized by gold ad-atoms sandwiched between two sulphur atoms. This finding contradicts older work on SAMs. However, newer studies on SAMs also reveal ad-atoms. Whether this finding can be generalized remains to be shown. In any case, more and more studies highlight the dynamic nature of the Au-S interface, both on flat surfaces and in clusters. At temperatures slightly above ambient thiolates migrate on the gold surface and on clusters. Evidence for desorption of thiolates at room temperature, at least under certain conditions, has been demonstrated for both systems. The adsorbed thiolate can lead to chirality at different lengths scales, which has been shown both on surfaces and for clusters. Chirality emerges from the organization of the thiolates as well as locally at the molecular level. Chirality can also be transferred from a chiral surface to an adsorbate, as evidenced by vibrational spectroscopy.

Atomically precise metal nanoclusters: stable sizes and optical properties

NASA Astrophysics Data System (ADS)

Jin, Rongchao

2015-01-01

Controlling nanoparticles with atomic precision has long been a major dream of nanochemists. Breakthroughs have been made in the case of gold nanoparticles, at least for nanoparticles smaller than ~3 nm in diameter. Such ultrasmall gold nanoparticles indeed exhibit fundamentally different properties from those of the plasmonic counterparts owing to the quantum size effects as well as the extremely high surface-to-volume ratio. These unique nanoparticles are often called nanoclusters to distinguish them from conventional plasmonic nanoparticles. Intense work carried out in the last few years has generated a library of stable sizes (or stable stoichiometries) of atomically precise gold nanoclusters, which are opening up new exciting opportunities for both fundamental research and technological applications. In this review, we have summarized the recent progress in the research of thiolate (SR)-protected gold nanoclusters with a focus on the reported stable sizes and their optical absorption spectra. The crystallization of nanoclusters still remains challenging; nevertheless, a few more structures have been achieved since the earlier successes in Au102(SR)44, Au25(SR)18 and Au38(SR)24 nanoclusters, and the newly reported structures include Au20(SR)16, Au24(SR)20, Au28(SR)20, Au30S(SR)18, and Au36(SR)24. Phosphine-protected gold and thiolate-protected silver nanoclusters are also briefly discussed in this review. The reported gold nanocluster sizes serve as the basis for investigating their size dependent properties as well as the development of applications in catalysis, sensing, biological labelling, optics, etc. Future efforts will continue to address what stable sizes are existent, and more importantly, what factors determine their stability. Structural determination and theoretical simulations will help to gain deep insight into the structure-property relationships.

Mechanical break junctions: enormous information in a nanoscale package.

PubMed

Natelson, Douglas

2012-04-24

Mechanical break junctions, particularly those in which a metal tip is repeatedly moved in and out of contact with a metal film, have provided many insights into electronic conduction at the atomic and molecular scale, most often by averaging over many possible junction configurations. This averaging throws away a great deal of information, and Makk et al. in this issue of ACS Nano demonstrate that, with both simulated and real experimental data, more sophisticated two-dimensional analysis methods can reveal information otherwise obscured in simple histograms. As additional measured quantities come into play in break junction experiments, including thermopower, noise, and optical response, these more sophisticated analytic approaches are likely to become even more powerful. While break junctions are not directly practical for useful electronic devices, they are incredibly valuable tools for unraveling the electronic transport physics relevant for ultrascaled nanoelectronics.

Spatial inhomogeneity in Schottky barrier height at graphene/MoS2 Schottky junctions

NASA Astrophysics Data System (ADS)

Tomer, D.; Rajput, S.; Li, L.

2017-04-01

Transport properties of graphene semiconductor Schottky junctions strongly depend on interfacial inhomogeneities due to the inherent formation of ripples and ridges. Here, chemical vapor deposited graphene is transferred onto multilayer MoS2 to fabricate Schottky junctions. These junctions exhibit rectifying current-voltage behavior with the zero bias Schottky barrier height increases and ideality factor decreases with increasing temperature between 210 and 300 K. Such behavior is attributed to the inhomogeneous interface that arises from graphene ripples and ridges, as revealed by atomic force and scanning tunneling microscopy imaging. Assuming a Gaussian distribution of the barrier height, a mean value of 0.96  ±  0.14 eV is obtained. These findings indicate a direct correlation between temperature dependent Schottky barrier height and spatial inhomogeneity in graphene/2D semiconductor Schottky junctions.

Electronic transport in gadolinium atomic-size contacts

NASA Astrophysics Data System (ADS)

Olivera, B.; Salgado, C.; Lado, J. L.; Karimi, A.; Henkel, V.; Scheer, E.; Fernández-Rossier, J.; Palacios, J. J.; Untiedt, C.

2017-02-01

We report on the fabrication, transport measurements, and density functional theory (DFT) calculations of atomic-size contacts made of gadolinium (Gd). Gd is known to have local moments mainly associated with f electrons. These coexist with itinerant s and d bands that account for its metallic character. Here we explore whether and how the local moments influence electronic transport properties at the atomic scale. Using both scanning tunneling microscope and lithographic mechanically controllable break junction techniques under cryogenic conditions, we study the conductance of Gd when only few atoms form the junction between bulk electrodes made of the very same material. Thousands of measurements show that Gd has an average lowest conductance, attributed to single-atom contact, below 2/e2 h . Our DFT calculations for monostrand chains anticipate that the f bands are fully spin polarized and insulating and that the conduction may be dominated by s , p , and d bands. We also analyze the electronic transport for model nanocontacts using the nonequilibrium Green's function formalism in combination with DFT. We obtain an overall good agreement with the experimental results for zero bias and show that the contribution to the electronic transport from the f channels is negligible and that from the d channels is marginal.

Preparation and characterization of carbon-supported sub-monolayer palladium decorated gold nanoparticles for the electro-oxidation of ethanol in alkaline media

NASA Astrophysics Data System (ADS)

Zhu, L. D.; Zhao, T. S.; Xu, J. B.; Liang, Z. X.

Carbon-supported gold nanoparticles (Au/C) are successfully decorated with mono- or sub-monolayer palladium atoms with different Pd/Au atomic ratios by a chemically epitaxial seeded growth method. TEM, UV-vis spectrometry and XRD techniques are used to characterize the particle size, dispersion, palladium coverage on gold seeds and crystal structures of the prepared catalysts. Cyclic voltammetric tests show that the Pd-decorated Au/C (denoted by Pd@Au/C) have higher specific activities than that of Pd/C for the oxidation of ethanol in alkaline media. This suggests that the Pd utilization is improved with such a surface-alloyed nanostructure. In addition, stable chronoamperometric responses are achieved with the so-prepared electrocatalysts during ethanol oxidation.

Chemical Phenomena of Atomic Force Microscopy Scanning

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ievlev, Anton V.; Brown, Chance; Burch, Matthew J.

Atomic force microscopy is widely used for nanoscale characterization of materials by scientists worldwide. The long-held belief of ambient AFM is that the tip is generally chemically inert but can be functionalized with respect to the studied sample. This implies that basic imaging and scanning procedures do not affect surface and bulk chemistry of the studied sample. However, an in-depth study of the confined chemical processes taking place at the tip–surface junction and the associated chemical changes to the material surface have been missing as of now. Here, we used a hybrid system that combines time-of-flight secondary ion mass spectrometrymore » with an atomic force microscopy to investigate the chemical interactions that take place at the tip–surface junction. Investigations showed that even basic contact mode AFM scanning is able to modify the surface of the studied sample. In particular, we found that the silicone oils deposited from the AFM tip into the scanned regions and spread to distances exceeding 15 μm from the tip. These oils were determined to come from standard gel boxes used for the storage of the tips. In conclusion, the explored phenomena are important for interpreting and understanding results of AFM mechanical and electrical studies relying on the state of the tip–surface junction.« less

Chemical Phenomena of Atomic Force Microscopy Scanning

DOE PAGES

Ievlev, Anton V.; Brown, Chance; Burch, Matthew J.; ...

2018-01-30

Atomic force microscopy is widely used for nanoscale characterization of materials by scientists worldwide. The long-held belief of ambient AFM is that the tip is generally chemically inert but can be functionalized with respect to the studied sample. This implies that basic imaging and scanning procedures do not affect surface and bulk chemistry of the studied sample. However, an in-depth study of the confined chemical processes taking place at the tip–surface junction and the associated chemical changes to the material surface have been missing as of now. Here, we used a hybrid system that combines time-of-flight secondary ion mass spectrometrymore » with an atomic force microscopy to investigate the chemical interactions that take place at the tip–surface junction. Investigations showed that even basic contact mode AFM scanning is able to modify the surface of the studied sample. In particular, we found that the silicone oils deposited from the AFM tip into the scanned regions and spread to distances exceeding 15 μm from the tip. These oils were determined to come from standard gel boxes used for the storage of the tips. In conclusion, the explored phenomena are important for interpreting and understanding results of AFM mechanical and electrical studies relying on the state of the tip–surface junction.« less

Adsorption of Pyridine at the Au(100)-Solution Interface.

DTIC Science & Technology

1987-09-25

quatiatively characterize the energetics of pyridine adsorption onto a gold ( 100) single crystal electrode surface. Over the potential region investigated...0.8 to +0.6 A., three orientationis of the pyridine molecules on the gold surface have been observed. The pyridine orientation Is strongly 1nflue ied by...the electrode potential. At a positively charged surface, the pyridine assumes a verticle orientation with .fie nitrogen atom facing the gold surface

Nano-scaling law: geometric foundation of thiolated gold nanomolecules.

PubMed

Dass, Amala

2012-04-07

Thiolated gold nanomolecules show a power correlation between the number of gold atoms and the thiolate ligands with a 2/3 scaling similar to Platonic and Archimedean solids. Nanomolecule stability is influenced by a universal geometric factor that is foundational to its stability through the Euclidean surface rule, in addition to the electronic shell closing factor and staple motif requirements. This journal is © The Royal Society of Chemistry 2012

Myochrysine Solution Structure and Reactivity

PubMed Central

Jones, William B.; Zhao, Zheng; Dorsey, John G.; Tepperman, Katherine

1994-01-01

We have determined the framework structure of Myochrysine (disodium gold(I)thiomalate) in the solid state and extremely concentrated aqueous solution, previously. It consists of an open chain polymer with linear gold coordination to two thiolates from the thiomalic acid moieties which bridge between pairs of gold atoms providing an Au-S-Au angle of 95°. The question remained: was this structure relevant to the dilute solutions of drugs administered and the still lower concentrations of gold found in the bodies of patients (typically 1 ppm Au in blood and urine or 5 μM in Au). We have provided an answer to that question using extended X-ray absorption spectroscopy (EXAFS) and capillary zone electrophoresis (CZE). EXAFS studies confirm that the polymeric structure with two sulfur atoms per gold atom persists from molar concentrations down to millimolar concentrations. CZE is able to separate and detect Myochrysine at millimolar levels. More importantly, at micromolar levels Myochrysine solutions exhibit identical CZE behavior to that measured at millimolar levels. Thus, aqueous solutions of the drug remain oligomeric at concentrations commensurate with those found in patient blood and urine. The reactivity of Myochrysine with cyanide, a species especially prevalent in smoking patients, was explored using CZE. Cyanide freely replaces thiomalic acid to form [Au(CN)2]- and thiomalic acid via a mixed ligand intermediate. The overall apparent equilibrium constant (Kapp) for the reaction is 6×10-4M-1. Further reaction of [Au(CN)2]- with a large excess of L, where L is cysteine, N-acetylcysteine, or glutathione, shows that these amino acids readily replace cyanide to form [AuL2]-. These species are thus potential metabolites and could possibly be active forms of gold in vivo. That all of these species are readily separated and quantified using CZE demonstrates that capillary electrophoresis is an accessible and powerful tool to add to those used for the study of gold-based antiarthritis drugs. PMID:18476256

Electrical characterization of gold-DNA-gold structures in presence of an external magnetic field by means of I-V curve analysis.

PubMed

Khatir, Nadia Mahmoudi; Banihashemian, Seyedeh Maryam; Periasamy, Vengadesh; Ritikos, Richard; Abd Majid, Wan Haliza; Abdul Rahman, Saadah

2012-01-01

This work presents an experimental study of gold-DNA-gold structures in the presence and absence of external magnetic fields with strengths less than 1,200.00 mT. The DNA strands, extracted by standard method were used to fabricate a Metal-DNA-Metal (MDM) structure. Its electric behavior when subjected to a magnetic field was studied through its current-voltage (I-V) curve. Acquisition of the I-V curve demonstrated that DNA as a semiconductor exhibits diode behavior in the MDM structure. The current versus magnetic field strength followed a decreasing trend because of a diminished mobility in the presence of a low magnetic field. This made clear that an externally imposed magnetic field would boost resistance of the MDM structure up to 1,000.00 mT and for higher magnetic field strengths we can observe an increase in potential barrier in MDM junction. The magnetic sensitivity indicates the promise of using MDM structures as potential magnetic sensors.

Electrical Characterization of Gold-DNA-Gold Structures in Presence of an External Magnetic Field by Means of I–V Curve Analysis

PubMed Central

Khatir, Nadia Mahmoudi; Banihashemian, Seyedeh Maryam; Periasamy, Vengadesh; Ritikos, Richard; Majid, Wan Haliza Abd; Rahman, Saadah Abdul

2012-01-01

This work presents an experimental study of gold-DNA-gold structures in the presence and absence of external magnetic fields with strengths less than 1,200.00 mT. The DNA strands, extracted by standard method were used to fabricate a Metal-DNA-Metal (MDM) structure. Its electric behavior when subjected to a magnetic field was studied through its current-voltage (I–V) curve. Acquisition of the I–V curve demonstrated that DNA as a semiconductor exhibits diode behavior in the MDM structure. The current versus magnetic field strength followed a decreasing trend because of a diminished mobility in the presence of a low magnetic field. This made clear that an externally imposed magnetic field would boost resistance of the MDM structure up to 1,000.00 mT and for higher magnetic field strengths we can observe an increase in potential barrier in MDM junction. The magnetic sensitivity indicates the promise of using MDM structures as potential magnetic sensors. PMID:22737025

Atomic Josephson Vortex

NASA Astrophysics Data System (ADS)

Kaurov, Vitaliy; Kuklov, Anatoly

2006-03-01

We show that atomic Josephson vortices [1] in a quasi-1D atomic junction can be controllably manipulated by imposing a tunneling bias current created by a difference of chemical potentials on the atomic BEC waveguides forming the junction. This effect, which has its origin in the Berry phase structure of a vortex, turns out to be very robust in the whole range of the parameters where such vortices can exist [2]. Acceleration of the vortex up to a certain threshold speed, determined by the strength of the Josephson coupling, results in the phase slip causing switching of the vorticity. This effect is directly related to the interconversion [1], when slow variation of the coupling can cause transformation of the vortex into the dark soliton and vice verse. We also propose that a Josephson vortex can be created by the phase imprinting technique and can be identified by a specific tangential feature in the interference picture produced by expanding clouds released from the waveguides [2]. [1] V. M. Kaurov , A. B. Kuklov, Phys. Rev. A 71, 11601(R) (2005). [2] V. M. Kaurov , A. B. Kuklov cond-mat/0508342

Solar-energy conversion and light emission in an atomic monolayer p-n diode.

PubMed

Pospischil, Andreas; Furchi, Marco M; Mueller, Thomas

2014-04-01

The limitations of the bulk semiconductors currently used in electronic devices-rigidity, heavy weight and high costs--have recently shifted the research efforts to two-dimensional atomic crystals such as graphene and atomically thin transition-metal dichalcogenides. These materials have the potential to be produced at low cost and in large areas, while maintaining high material quality. These properties, as well as their flexibility, make two-dimensional atomic crystals attractive for applications such as solar cells or display panels. The basic building blocks of optoelectronic devices are p-n junction diodes, but they have not yet been demonstrated in a two-dimensional material. Here, we report a p-n junction diode based on an electrostatically doped tungsten diselenide (WSe2) monolayer. We present applications as a photovoltaic solar cell, a photodiode and a light-emitting diode, and obtain light-power conversion and electroluminescence efficiencies of ∼ 0.5% and ∼ 0.1%, respectively. Given recent advances in the large-scale production of two-dimensional crystals, we expect them to profoundly impact future developments in solar, lighting and display technologies.

Polymer supported gold nanoparticles: Synthesis and characterization of functionalized polystyrene-supported gold nanoparticles and their application in catalytic oxidation of alcohols in water

NASA Astrophysics Data System (ADS)

Kaboudin, Babak; Khanmohammadi, Hamid; Kazemi, Foad

2017-12-01

Sulfonated polystyrene microsphere were functionalized using ethylene diamine to introduce amine groups to the polymer chains. The amine functionalized polymers were used as a support for gold nanoparticles. A thorough structural characterization has been carried out by means of transmission electron microscopy (TEM), scanning electron microscopy (SEM) images, EDS, CHN and atomic absorption spectroscopy. The polymer supported gold nanoparticles was found to be an efficient catalyst for the oxidation of alcohols in water.

Plastic Schottky barrier solar cells

DOEpatents

Waldrop, James R.; Cohen, Marshall J.

1984-01-24

A photovoltaic cell structure is fabricated from an active medium including an undoped, intrinsically p-type organic semiconductor comprising polyacetylene. When a film of such material is in rectifying contact with a magnesium electrode, a Schottky-barrier junction is obtained within the body of the cell structure. Also, a gold overlayer passivates the magnesium layer on the undoped polyacetylene film.

Controlling the rectification properties of molecular junctions through molecule–electrode coupling

DOE PAGES

Koepf, Matthieu; Koenigsmann, Christopher; Ding, Wendu; ...

2016-08-17

The development of molecular components functioning as switches, rectifiers or amplifiers is a great challenge in molecular electronics. A desirable property of such components is functional robustness, meaning that the intrinsic functionality of components must be preserved regardless of the strategy used to integrate them into the final assemblies. Here, this issue is investigated for molecular diodes based on N-phenylbenzamide (NPBA) backbones. The transport properties of molecular junctions derived from NPBA are characterized while varying the nature of the functional groups interfacing the backbone and the gold electrodes required for break-junction measurements. Furthermore, combining experimental and theoretical methods, it ismore » shown that at low bias (<0.85 V) transport is determined by the same frontier molecular orbital originating from the NPBA core, regardless of the anchoring group employed. The magnitude of rectification, however, is strongly dependent on the strength of the electronic coupling at the gold–NPBA interface and on the spatial distribution of the local density of states of the dominant transport channel of the molecular junction.« less

Controlling the rectification properties of molecular junctions through molecule–electrode coupling

DOE Office of Scientific and Technical Information (OSTI.GOV)

Koepf, Matthieu; Koenigsmann, Christopher; Ding, Wendu

The development of molecular components functioning as switches, rectifiers or amplifiers is a great challenge in molecular electronics. A desirable property of such components is functional robustness, meaning that the intrinsic functionality of components must be preserved regardless of the strategy used to integrate them into the final assemblies. Here, this issue is investigated for molecular diodes based on N-phenylbenzamide (NPBA) backbones. The transport properties of molecular junctions derived from NPBA are characterized while varying the nature of the functional groups interfacing the backbone and the gold electrodes required for break-junction measurements. Furthermore, combining experimental and theoretical methods, it ismore » shown that at low bias (<0.85 V) transport is determined by the same frontier molecular orbital originating from the NPBA core, regardless of the anchoring group employed. The magnitude of rectification, however, is strongly dependent on the strength of the electronic coupling at the gold–NPBA interface and on the spatial distribution of the local density of states of the dominant transport channel of the molecular junction.« less

Chemisorbed monolayers of corannulene penta-thioethers on gold.

PubMed

Angelova, Polina; Solel, Ephrath; Parvari, Galit; Turchanin, Andrey; Botoshansky, Mark; Gölzhäuser, Armin; Keinan, Ehud

2013-02-19

Penta(tert-butylthio)corannulene and penta(4-dimethylaminophenylthio)corannulene form highly stable monolayers on gold surfaces, as indicated by X-ray photoelectron spectroscopy (XPS). Formation of these homogeneous monolayers involves multivalent coordination of the five sulfur atoms to gold with the peripheral alkyl or aryl substituents pointing away from the surface. No dissociation of C-S bonds upon binding could be observed at room temperature. Yet, the XPS experiments reveal strong chemical bonding between the thioether groups and gold. Temperature-dependent XPS study shows that the thermal stability of the monolayers is higher than the typical stability of self-assembled monolayers (SAMs) of thiolates on gold.

Two-dimensional gold nanostructures with high activity for selective oxidation of carbon-hydrogen bonds.

PubMed

Wang, Liang; Zhu, Yihan; Wang, Jian-Qiang; Liu, Fudong; Huang, Jianfeng; Meng, Xiangju; Basset, Jean-Marie; Han, Yu; Xiao, Feng-Shou

2015-04-22

Efficient synthesis of stable two-dimensional (2D) noble metal catalysts is a challenging topic. Here we report the facile synthesis of 2D gold nanosheets via a wet chemistry method, by using layered double hydroxide as the template. Detailed characterization with electron microscopy and X-ray photoelectron spectroscopy demonstrates that the nanosheets are negatively charged and [001] oriented with thicknesses varying from single to a few atomic layers. X-ray absorption spectroscopy reveals unusually low gold-gold coordination numbers. These gold nanosheets exhibit high catalytic activity and stability in the solvent-free selective oxidation of carbon-hydrogen bonds with molecular oxygen.

Two-dimensional gold nanostructures with high activity for selective oxidation of carbon-hydrogen bonds

NASA Astrophysics Data System (ADS)

Wang, Liang; Zhu, Yihan; Wang, Jian-Qiang; Liu, Fudong; Huang, Jianfeng; Meng, Xiangju; Basset, Jean-Marie; Han, Yu; Xiao, Feng-Shou

2015-04-01

Efficient synthesis of stable two-dimensional (2D) noble metal catalysts is a challenging topic. Here we report the facile synthesis of 2D gold nanosheets via a wet chemistry method, by using layered double hydroxide as the template. Detailed characterization with electron microscopy and X-ray photoelectron spectroscopy demonstrates that the nanosheets are negatively charged and [001] oriented with thicknesses varying from single to a few atomic layers. X-ray absorption spectroscopy reveals unusually low gold-gold coordination numbers. These gold nanosheets exhibit high catalytic activity and stability in the solvent-free selective oxidation of carbon-hydrogen bonds with molecular oxygen.

In-situ suspended aggregate microextraction of gold nanoparticles from water samples and determination by electrothermal atomic absorption spectrometry.

PubMed

Choleva, Tatiana G; Kappi, Foteini A; Tsogas, George Z; Vlessidis, Athanasios G; Giokas, Dimosthenis L

2016-05-01

This work describes a new method for the extraction and determination of gold nanoparticles in environmental samples by means of in-situ suspended aggregate microextraction and electrothermal atomic absorption spectrometry. The method relies on the in-situ formation of a supramolecular aggregate phase through ion-association between a cationic surfactant and a benzene sulfonic acid derivative. Gold nanoparticles are physically entrapped into the aggregate phase which is separated from the bulk aqueous solution by vacuum filtration on the surface of a cellulose filter in the form of a thin film. The film is removed from the filter surface and is dissociated into an acidified methanolic solution which is used for analysis. Under the optimized experimental conditions, gold nanoparticles can be efficiently extracted from water samples with recovery rates between 81.0-93.3%, precision 5.4-12.0% and detection limits as low as 75femtomolL(-1) using only 20mL of sample volume. The satisfactory analytical features of the method along with the simplicity indicate the efficiency of this new approach to adequately collect and extract gold nanoparticle species from water samples. Copyright © 2016 Elsevier B.V. All rights reserved.

Direct writing of gold nanostructures with an electron beam: On the way to pure nanostructures by combining optimized deposition with oxygen-plasma treatment

PubMed Central

Belić, Domagoj; Shawrav, Mostafa M; Bertagnolli, Emmerich

2017-01-01

This work presents a highly effective approach for the chemical purification of directly written 2D and 3D gold nanostructures suitable for plasmonics, biomolecule immobilisation, and nanoelectronics. Gold nano- and microstructures can be fabricated by one-step direct-write lithography process using focused electron beam induced deposition (FEBID). Typically, as-deposited gold nanostructures suffer from a low Au content and unacceptably high carbon contamination. We show that the undesirable carbon contamination can be diminished using a two-step process – a combination of optimized deposition followed by appropriate postdeposition cleaning. Starting from the common metal-organic precursor Me2-Au-tfac, it is demonstrated that the Au content in pristine FEBID nanostructures can be increased from 30 atom % to as much as 72 atom %, depending on the sustained electron beam dose. As a second step, oxygen-plasma treatment is established to further enhance the Au content in the structures, while preserving their morphology to a high degree. This two-step process represents a simple, feasible and high-throughput method for direct writing of purer gold nanostructures that can enable their future use for demanding applications. PMID:29259868

Tuning Chemical Potential Difference across Alternately Doped Graphene p-n Junctions for High-Efficiency Photodetection.

PubMed

Lin, Li; Xu, Xiang; Yin, Jianbo; Sun, Jingyu; Tan, Zhenjun; Koh, Ai Leen; Wang, Huan; Peng, Hailin; Chen, Yulin; Liu, Zhongfan

2016-07-13

Being atomically thin, graphene-based p-n junctions hold great promise for applications in ultrasmall high-efficiency photodetectors. It is well-known that the efficiency of such photodetectors can be improved by optimizing the chemical potential difference of the graphene p-n junction. However, to date, such tuning has been limited to a few hundred millielectronvolts. To improve this critical parameter, here we report that using a temperature-controlled chemical vapor deposition process, we successfully achieved modulation-doped growth of an alternately nitrogen- and boron-doped graphene p-n junction with a tunable chemical potential difference up to 1 eV. Furthermore, such p-n junction structure can be prepared on a large scale with stable, uniform, and substitutional doping and exhibits a single-crystalline nature. This work provides a feasible method for synthesizing low-cost, large-scale, high efficiency graphene p-n junctions, thus facilitating their applications in optoelectronic and energy conversion devices.

Investigations on rectifying behavior of Y{sub 0.95}Ca{sub 0.05}MnO{sub 3}/Si junction

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dhruv, Davit; V.V.P. Engineering College, Gujarat Technological University, Rajkot – 360 005; Joshi, Zalak

2016-05-06

In this communication, we report the rectifying properties observed across the junction, consists of Ca{sup +2} doped hexagonal YMnO{sub 3} manganite film, grown on n-type (100) Si single crystalline substrate. The junction was grown using cost effective chemical solution deposition (CSD) technique by employing spin coating method. Surface morphology of Y{sub 0.9}5Ca{sub 0.05}MnO{sub 3}/Si (YCMO/Si) film was carried out by atomic force microscopy and magnetic response of film was studied by magnetic force microscopy. Current – voltage characteristics of the junction was carried out by using Keithley source meter in current perpendicular to plane (CPP) mode at different temperatures. Rectificationmore » in I – V behavior has been observed for the junction at all the temperatures studied. With increase in temperature, rectification ratio, in the range of 10{sup 4}, increases across the junction. Results have been discussed in the context of thermal effects.« less

Spatially inhomogeneous barrier height in graphene/MoS2 Schottky junctions

NASA Astrophysics Data System (ADS)

Tomer, Dushyant; Rajput, Shivani; Li, Lian

Graphene interfaced with a semiconductor forms a Schottky junction with rectifying properties. In this study, graphene Schottky junctions are fabricated by transferring CVD monolayer graphene on mechanically exfoliated MoS2 multilayers. The forward bias current-voltage characteristics are measured in the temperature range of 210-300 K. An increase in the zero bias barrier height and decrease in the ideality factor are observed with increasing temperature. Such behavior is attributed to Schottky barrier inhomogeneities possibly due to graphene ripples and ridges at the junction interface as suggested by atomic force microscopy. Assuming a Gaussian distribution of the barrier height, mean barrier of 0.97+/-0.10 eV is found for the graphene MoS2 junction. Our findings provide significant insight on the barrier height inhomogeneities in graphene/two dimensional semiconductor Schottky junctions. U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering Award No. DEFG02-07ER46228.

Density matrix renormalization group study of Y-junction spin systems

NASA Astrophysics Data System (ADS)

Guo, Haihui

Junction systems are important to understand both from the fundamental and the practical point of view, as they are essential components in existing and future electronic and spintronic devices. With the continuous advance of technology, device size will eventual reach the atomic scale. Some of the most interesting and useful junction systems will be strongly correlated. We chose the Density Matrix Renormalization Group method to study two types of Y-junction systems, the Y and YDelta junctions, on strongly correlated spin chains. With new ideas coming from the quantum information field, we have made a very efficient. Y-junction DMRG algorithm, which improves the overall CUB cost from O(m6) to O(m4), where m is the number of states kept per block. We studied the ground state properties, the correlation length, and investigated the degeneracy problem on the Y and YDelta junctions. For the excited states, we researched the existence of magnon bound states for various conditions, and have shown that the bound state exists when the central coupling constant is small.

Nanoscale Structural Changes Upon Electrooxidation of Au(111) as Probed by Potentiodynamic Scanning Tunneling Microscopy

DTIC Science & Technology

1994-02-01

electrochemical formation and removal of oxide films is of broadbased practical as well as fundamental importance. Studies of noble metals, such as gold and...atomic level. At the current state of development of STM, monocrystalline gold electrodes provide efficacious choices of systems, partly in view of...several in-situ STM studies have focussed on the surface morphological changes attending oxidation and rereduction of single-crystal gold electrodes

High thermopower of mechanically stretched single-molecule junctions

PubMed Central

Tsutsui, Makusu; Morikawa, Takanori; He, Yuhui; Arima, Akihide

2015-01-01

Metal-molecule-metal junction is a promising candidate for thermoelectric applications that utilizes quantum confinement effects in the chemically defined zero-dimensional atomic structure to achieve enhanced dimensionless figure of merit ZT. A key issue in this new class of thermoelectric nanomaterials is to clarify the sensitivity of thermoelectricity on the molecular junction configurations. Here we report simultaneous measurements of the thermoelectric voltage and conductance on Au-1,4-benzenedithiol (BDT)-Au junctions mechanically-stretched in-situ at sub-nanoscale. We obtained the average single-molecule conductance and thermopower of 0.01 G0 and 15 μV/K, respectively, suggesting charge transport through the highest occupied molecular orbital. Meanwhile, we found the single-molecule thermoelectric transport properties extremely-sensitive to the BDT bridge configurations, whereby manifesting the importance to design the electrode-molecule contact motifs for optimizing the thermoelectric performance of molecular junctions. PMID:26112999

Oxygen isotope exchange with quartz during pyrolysis of silver sulfate and silver nitrate.

PubMed

Schauer, Andrew J; Kunasek, Shelley A; Sofen, Eric D; Erbland, Joseph; Savarino, Joel; Johnson, Ben W; Amos, Helen M; Shaheen, Robina; Abaunza, Mariana; Jackson, Terri L; Thiemens, Mark H; Alexander, Becky

2012-09-30

Triple oxygen isotopes of sulfate and nitrate are useful metrics for the chemistry of their formation. Existing measurement methods, however, do not account for oxygen atom exchange with quartz during the thermal decomposition of sulfate. We present evidence for oxygen atom exchange, a simple modification to prevent exchange, and a correction for previous measurements. Silver sulfates and silver nitrates with excess (17)O were thermally decomposed in quartz and gold (for sulfate) and quartz and silver (for nitrate) sample containers to O(2) and byproducts in a modified Temperature Conversion/Elemental Analyzer (TC/EA). Helium carries O(2) through purification for isotope-ratio analysis of the three isotopes of oxygen in a Finnigan MAT253 isotope ratio mass spectrometer. The Δ(17)O results show clear oxygen atom exchange from non-zero (17)O-excess reference materials to zero (17)O-excess quartz cup sample containers. Quartz sample containers lower the Δ(17)O values of designer sulfate reference materials and USGS35 nitrate by 15% relative to gold or silver sample containers for quantities of 2-10 µmol O(2). Previous Δ(17)O measurements of sulfate that rely on pyrolysis in a quartz cup have been affected by oxygen exchange. These previous results can be corrected using a simple linear equation (Δ(17)O(gold) = Δ(17)O(quartz) * 1.14 + 0.06). Future pyrolysis of silver sulfate should be conducted in gold capsules or corrected to data obtained from gold capsules to avoid obtaining oxygen isotope exchange-affected data. Copyright © 2012 John Wiley & Sons, Ltd.

Gold and gold-iron oxide magnetic glyconanoparticles: synthesis, characterization and magnetic properties.

PubMed

de la Fuente, Jesús M; Alcántara, David; Eaton, Peter; Crespo, Patricia; Rojas, Teresa C; Fernandez, Asunción; Hernando, Antonio; Penadés, Soledad

2006-07-06

The preparation, characterization and the magnetic properties of gold and gold-iron oxide glyconanoparticles (GNPs) are described. Glyconanoparticles were prepared in a single step procedure in the presence of aqueous solution of thiol functionalized neoglycoconjugates and either gold salts or both gold and iron salts. Neoglycoconjugates of lactose and maltose disaccharides with different linkers were used. Iron-free gold or gold-iron oxide GNPs with controlled gold-iron ratios were obtained. The average core-size diameters are in the range of 1.5-2.5 nm. The GNPs are fully characterized by (1)H NMR spectrometry, transmission electron microscopy (TEM), and UV-vis and X-ray absorption (XAS) spectroscopies. Inductive plasma-atomic emission spectrometry (ICP) and elemental analysis gave the average number of neoglycoconjugates per cluster. The magnetic properties were measured in a SQUID magnetometer. The most remarkable results was the observation of a permanent magnetism up to room temperature in the iron-free gold GNPs, that was not present in the corresponding gold-iron oxide GNPs.

Structure and reactivity of a mononuclear gold(II) complex

NASA Astrophysics Data System (ADS)

Preiß, Sebastian; Förster, Christoph; Otto, Sven; Bauer, Matthias; Müller, Patrick; Hinderberger, Dariush; Hashemi Haeri, Haleh; Carella, Luca; Heinze, Katja

2017-12-01

Mononuclear gold(II) complexes are very rare labile species. Transient gold(II) species have been suggested in homogeneous catalysis and in medical applications, but their geometric and electronic structures have remained essentially unexplored: even fundamental data, such as the ionic radius of gold(II), are unknown. Now, an unprecedentedly stable neutral gold(II) complex of a porphyrin derivative has been isolated, and its structural and spectroscopic features determined. The gold atom adopts a 2+2 coordination mode in between those of gold(III) (four-coordinate square planar) and gold(I) (two-coordinate linear), owing to a second-order Jahn-Teller distortion enabled by the relativistically lowered 6s orbital of gold. The reactivity of this gold(II) complex towards dioxygen, nitrosobenzene and acids is discussed. This study provides insight on the ionic radius of gold(II), and allows it to be placed within the homologous series of nd9 Cu/Ag/Au divalent ions and the 5d8/9/10 Pt/Au/Hg 'relativistic' triad in the periodic table.

RBS, TEM and SEM Characterization of Gold Nanoclusters in TiO2(110)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shutthanandan, V; Zhang, Yanwen; Wang, Chong M.

2004-05-01

Nucleation of gold nanoclusters in TiO2(110) single crystal using ion implantation and subsequent annealing were studied by Rutherford backscattering spectrometry /channeling (RBS/C), scanning electron microscopy (SEM) and transmission electron microscopy (TEM). Approximately 1000 Au2+/nm2 was implanted at room temperature in TiO2(110) substrates. TEM and SEM measurements revel that rounded nanoclusters were formed during the implantation. In contrast subsequent annealing in air for 10 hours at 1275 K promoted the formation of faceted (rectangular shaped) Au nano structures in TiO2. RBS channeling measurements further reveled that Au atoms randomly occupied in the host TiO2 lattice during the implantation. However, some ofmore » the gold atoms were moved into the Ti lattice position after annealing.« less

Comparison of Adsorbed Mercury Screening Method With Cold-Vapor Atomic Absorption Spectrophotometry for Determination of Mercury in Soil

NASA Technical Reports Server (NTRS)

Easterling, Donald F.; Hovanitz, Edward S.; Street, Kenneth W.

2000-01-01

A field screening method for the determination of elemental mercury in environmental soil samples involves the thermal desorption of the mercury from the sample onto gold and then the thermal desorption from the gold to a gold-film mercury vapor analyzer. This field screening method contains a large number of conditions that could be optimized for the various types of soils encountered. In this study, the conditions were optimized for the determination of mercury in silty clay materials, and the results were comparable to the cold-vapor atomic absorption spectrophotometric method of determination. This paper discusses the benefits and disadvantages of employing the field screening method and provides the sequence of conditions that must be optimized to employ this method of determination on other soil types.

Molecular ion yield enhancement induced by gold deposition in static secondary ion mass spectrometry

NASA Astrophysics Data System (ADS)

Wehbe, Nimer; Delcorte, Arnaud; Heile, Andreas; Arlinghaus, Heinrich F.; Bertrand, Patrick

2008-12-01

Static ToF-SIMS was used to evaluate the effect of gold condensation as a sample treatment prior to analysis. The experiments were carried out with a model molecular layer (Triacontane M = 422.4 Da), upon atomic (In +) and polyatomic (Bi 3+) projectile bombardment. The results indicate that the effect of molecular ion yield improvement using gold metallization exists only under atomic projectile impact. While the quasi-molecular ion (M+Au) + signal can become two orders of magnitude larger than that of the deprotonated molecular ion from the pristine sample under In + bombardment, it barely reaches the initial intensity of (M-H) + when Bi 3+ projectiles are used. The differences observed for mono- and polyatomic primary ion bombardment might be explained by differences in near-surface energy deposition, which influences the sputtering and ionization processes.

Tuning optical properties of magic number cluster (SiO2)4O2H4 by substitutional bonding with gold atoms.

PubMed

Cai, Xiulong; Zhang, Peng; Ma, Liuxue; Zhang, Wenxian; Ning, Xijing; Zhao, Li; Zhuang, Jun

2009-04-30

By bonding gold atoms to the magic number cluster (SiO(2))(4)O(2)H(4), two groups of Au-adsorbed shell-like clusters Au(n)(SiO(2))(4)O(2)H(4-n) (n = 1-4) and Au(n)(SiO(2))(4)O(2) (n = 5-8) were obtained, and their spectral properties were studied. The ground-state structures of these clusters were optimized by density functional theory, and the results show that in despite of the different numbers and types of the adsorbed Au atoms, the cluster core (SiO(2))(4)O(2) of T(d) point-group symmetry keeps almost unchanged. The absorption spectra were obtained by time-dependent density functional theory. From one group to the other, an extension of absorption wavelength from the UV-visible to the NIR region was observed, and in each group the absorption strengths vary linearly with the number of Au atoms. These features indicate their advantages for exploring novel materials with easily controlled tunable optical properties. Furthermore, due to the weak electronic charge transfer between the Au atoms, the clusters containing Au(2) dimers, especially Au(8)(SiO(2))(4)O(2), absorb strongly NIR light at 900 approximately 1200 nm. Such strong absorption suggests potential applications of these shell-like clusters in tumor cells thermal therapy, like the gold-coated silica nanoshells with larger sizes.

Understanding the evolution of luminescent gold quantum clusters in protein templates.

PubMed

Chaudhari, Kamalesh; Xavier, Paulrajpillai Lourdu; Pradeep, Thalappil

2011-11-22

We show that the time-dependent biomineralization of Au(3+) by native lactoferrin (NLf) and bovine serum albumin (BSA) resulting in near-infrared (NIR) luminescent gold quantum clusters (QCs) occurs through a protein-bound Au(1+) intermediate and subsequent emergence of free protein. The evolution was probed by diverse tools, principally, using matrix-assisted laser desorption ionization mass spectrometry (MALDI MS), X-ray photoelectron spectroscopy (XPS), and photoluminescence spectroscopy (PL). The importance of alkaline pH in the formation of clusters was probed. At neutral pH, a Au(1+)-protein complex was formed (starting from Au(3+)) with the binding of 13-14 gold atoms per protein. When the pH was increased above 12, these bound gold ions were further reduced to Au(0) and nucleation and growth of cluster commenced, which was corroborated by the beginning of emission; at this point, the number of gold atoms per protein was ~25, suggesting the formation of Au(25). During the cluster evolution, at certain time intervals, for specific molar ratios of gold and protein, occurrence of free protein was noticed in the mass spectra, suggesting a mixture of products and gold ion redistribution. By providing gold ions at specific time of the reaction, monodispersed clusters with enhanced luminescence could be obtained, and the available quantity of free protein could be utilized efficiently. Monodispersed clusters would be useful in obtaining single crystals of protein-protected noble metal quantum clusters where homogeneity of the system is of primary concern. © 2011 American Chemical Society

Green synthesis of stabilized spherical shaped gold nanoparticles using novel aqueous Elaeis guineensis (oil palm) leaves extract

NASA Astrophysics Data System (ADS)

Ahmad, Tausif; Bustam, Mohamad Azmi; Irfan, Muhammad; Moniruzzaman, Muhammad; Anwaar Asghar, Hafiz Muhammad; Bhattacharjee, Sekhar

2018-05-01

In the last decade, development of bioinspired protocols to synthesize gold nanoparticles (AuNPs) using plants and their extracts have been dealt by researchers due to their low cost, renewability and non-toxic features. A simple, cheap and ecofriendly method is reported to synthesize stabilized AuNPs of size 35-75 nm at room temperature using aqueous Elaeis guineensis (oil palm) leaves extract without addition of any external agent. Oil palm leaves mediated AuNPs were characterized using FTIR, UV-vis spectrophotometer, EDAX, XPS, FESEM, TEM, DLS and TGA. FTIR spectra results revealed contribution of phenolic, carboxylic, amines and amides in reduction of trivalent gold ions and stabilization of formed gold atoms. Reaction solution color change and UV-vis spectra confirmed reduction of gold ions to generate gold atoms. Reaction mechanism explained the role of phenolic compounds in reduction reaction using FTIR and UV-vis spectra results. EDAX and XPS results further validated the formation of metallic gold particles through bioreduction of gold ions. Crystal structure of metallic gold particles was confirmed through XRD peaks indexing to (111), (200), (220) and (311) planes. TEM and FESEM particles size measurements exhibited the formation of nanostructured AuNPs. Synthesis of well scattered and spherical shaped AuNPs was revealed through FESEM and TEM images. The excellent stability of AuNPs was shown through high negative zeta potential value (-14.7 ± 4.68 mV) and uniform dispersion in aqueous media. Our results disclosed the excellent potential of Elaeis guineensis (oil palm) leaves as reducing and stabilizing agents in green synthesis of well scattered spherical shaped AuNPs, which can be employed as strong candidates in medical drug delivery and industrial applications.

Synthesis of camptothecin-loaded gold nanomaterials

NASA Astrophysics Data System (ADS)

Xing, Zhimin; Liu, Zhiguo; Zu, Yuangang; Fu, Yujie; Zhao, Chunjian; Zhao, Xiuhua; Meng, Ronghua; Tan, Shengnan

2010-04-01

Camptothecin-loaded gold nanomaterials have been synthesized by the sodium borohydride reduction method under a strong basic condition. The obtained gold nanomaterials have been characterized by transmission electron microscopy (TEM), atomic force microscopy (AFM) and UV-vis absorption spectroscopy. The camptothecin-loaded gold colloidal solution was very stable and can be stored for more than two months at room temperature without obvious changes. The color of the colloidal solution can change from wine red to purple and blue during the acidifying process. It was revealed that the release of camptothecin and the aggregation of gold nanoparticles can be controlled by tuning the solution pH. The present study implied that the gold nanomaterials can be used as the potential carrier for CPT delivery.

Theoretical and Experimental Investigation of Heterojunction Interfaces

DTIC Science & Technology

1983-11-01

every two surface atoms at the junction. In terms of our theoretical alchemy one proton must be added for every two surface atoms. Note that this...Chye. I. Lindau. P PianetU, C. M. Gamer , and W E Spicer, Phys Rev. B 17, 2682 11978|. "J. R. Waldrop and R W. Grant. Appl. Phys. Lett. 34. 630

Photoinduced electron transfer through peptide-based self-assembled monolayers chemisorbed on gold electrodes: directing the flow-in and flow-out of electrons through peptide helices.

PubMed

Venanzi, Mariano; Gatto, Emanuela; Caruso, Mario; Porchetta, Alessandro; Formaggio, Fernando; Toniolo, Claudio

2014-08-21

Photoinduced electron transfer (PET) experiments have been carried out on peptide self-assembled monolayers (SAM) chemisorbed on a gold substrate. The oligopeptide building block was exclusively formed by C(α)-tetrasubstituted α-aminoisobutyric residues to attain a helical conformation despite the shortness of the peptide chain. Furthermore, it was functionalized at the C-terminus by a pyrene choromophore to enhance the UV photon capture cross-section of the compound and by a lipoic group at the N-terminus for linking to gold substrates. Electron transfer across the peptide SAM has been studied by photocurrent generation experiments in an electrochemical cell employing a gold substrate modified by chemisorption of a peptide SAM as a working electrode and by steady-state and time-resolved fluorescence experiments in solution and on a gold-coated glass. The results show that the electronic flow through the peptide bridge is strongly asymmetric; i.e., PET from the C-terminus to gold is highly favored with respect to PET in the opposite direction. This effect arises from the polarity of the Au-S linkage (Au(δ+)-S(δ-), junction effect) and from the electrostatic field generated by the peptide helix.

Tuning of optical and electrical properties of wide band gap Fe:SnO2/Li:NiO p- n junctions using 80 MeV oxygen ion beam

NASA Astrophysics Data System (ADS)

Mistry, Bhaumik V.; Avasthi, D. K.; Joshi, U. S.

2016-12-01

Electrical and optical properties of pristine and swift heavy ion (SHI) irradiated p- n junction diode have been investigated for advanced electronics application. Fe:SnO2/Li:NiO p- n junction was fabricated by using pulsed laser deposition on c-sapphire substrate. The optical band gaps of Fe:SnO2 and Li:NiO films were obtained to be 3.88 and 3.37 eV, respectively. The current-voltage characteristics of the oxide-based p- n junction showed a rectifying behaviour with turn-on voltage of 0.95 V. The oxide-based p- n junction diode was irradiated to 80 MeV O+6 ions with 1 × 1012 ions/cm2 fluence. Decrease in grain size due to SHI irradiation is confirmed by the grazing angle X-ray diffraction and atomic force microscopy. In comparison with the pristine p- n junction diode, O+6 ion irradiated p-n junction diode shows the increase of surface roughness and decrease of percentage transmittance in visible region. For irradiated p- n junction diode, current-voltage curve has still rectifying behaviour but exhibits lower turn-on voltage than that of virgin p- n junction diode.

Real-space microscopic electrical imaging of n+-p junction beneath front-side Ag contact of multicrystalline Si solar cells

NASA Astrophysics Data System (ADS)

Jiang, C.-S.; Li, Z. G.; Moutinho, H. R.; Liang, L.; Ionkin, A.; Al-Jassim, M. M.

2012-04-01

We investigated the quality of the n+-p diffused junction beneath the front-side Ag contact of multicrystalline Si solar cells by characterizing the uniformities of electrostatic potential and doping concentration across the junction using the atomic force microscopy-based electrical imaging techniques of scanning Kelvin probe force microscopy and scanning capacitance microscopy. We found that Ag screen-printing metallization fired at the over-fire temperature significantly degrades the junction uniformity beneath the Ag contact grid, whereas metallization at the optimal- and under-fire temperatures does not cause degradation. Ag crystallites with widely distributed sizes were found at the Ag-grid/emitter-Si interface of the over-fired cell, which is associated with the junction damage beneath the Ag grid. Large crystallites protrude into Si deeper than the junction depth. However, the junction was not broken down; instead, it was reformed on the entire front of the crystallite/Si interface. We propose a mechanism of junction-quality degradation, based on emitter Si melting at the temperature around the Ag-Si eutectic point during firing, and subsequent re-crystallization with incorporation of Ag and other impurities and with formation of crystallographic defects during quenching. The effect of this junction damage on solar cell performance is discussed.

Real-Space Microscopic Electrical Imaging of n+-p Junction Beneath Front-Side Ag Contact of Multicrystalline Si Solar Cells

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jiang, C. S.; Li, Z. G.; Moutinho, H. R.

2012-04-15

We investigated the quality of the n+-p diffused junction beneath the front-side Ag contact of multicrystalline Si solar cells by characterizing the uniformities of electrostatic potential and doping concentration across the junction using the atomic force microscopy-based electrical imaging techniques of scanning Kelvin probe force microscopy and scanning capacitance microscopy. We found that Ag screen-printing metallization fired at the over-fire temperature significantly degrades the junction uniformity beneath the Ag contact grid, whereas metallization at the optimal- and under-fire temperatures does not cause degradation. Ag crystallites with widely distributed sizes were found at the Ag-grid/emitter-Si interface of the over-fired cell, whichmore » is associated with the junction damage beneath the Ag grid. Large crystallites protrude into Si deeper than the junction depth. However, the junction was not broken down; instead, it was reformed on the entire front of the crystallite/Si interface. We propose a mechanism of junction-quality degradation, based on emitter Si melting at the temperature around the Ag-Si eutectic point during firing, and subsequent re-crystallization with incorporation of Ag and other impurities and with formation of crystallographic defects during quenching. The effect of this junction damage on solar cell performance is discussed.« less

Controlling the electric charge of gold nanoplatelets on an insulator by field emission nc-AFM

NASA Astrophysics Data System (ADS)

Baris, Bulent; Alchaar, Mohanad; Prasad, Janak; Gauthier, Sébastien; Dujardin, Erik; Martrou, David

2018-03-01

Charging of 2D Au nanoplatelets deposited on an insulating SiO2 substrate to or from the tip of a non-contact atomic force microscope (nc-AFM) is demonstrated. Charge transfer is controlled by monitoring the resonance frequency shift Δf(V) during the bias voltage ramp V applied to the tip-back electrode junction. The onset of charge transfer is revealed by a transition from a capacitive parabolic behavior to a constant Δf(V) region for both polarities. An analytical model, based on charging by electron field emission, shows that the field-emitted current saturates shortly after the onset of the charging, due to the limiting effect of the charge-induced rise of the Au platelet potential. The value of this current plateau depends only on the rate of the bias voltage ramp and on the value of the platelet/SiO2/back electrode capacitance. This analysis is confirmed by numerical simulations based on a virtual nc-AFM model that faithfully matches the experimental data. Our charging protocol could be used to tune the potential of the platelets at the single charge level.

Length-Dependent Nanotransport and Charge Hopping Bottlenecks in Long Thiophene-Containing π-Conjugated Molecular Wires.

PubMed

Smith, Christopher E; Odoh, Samuel O; Ghosh, Soumen; Gagliardi, Laura; Cramer, Christopher J; Frisbie, C Daniel

2015-12-23

Self-assembled conjugated molecular wires containing thiophene up to 6 nm in length were grown layer-by-layer using click chemistry. Reflection-absorption infrared spectroscopy, ellipsometry and X-ray photoelectron spectroscopy were used to follow the stepwise growth. The electronic structure of the conjugated wires was studied with cyclic voltammetry and UV-vis spectroscopy as well as computationally with density functional theory (DFT). The current-voltage curves (±1 V) of the conjugated molecular wires were measured with conducting probe atomic force microscopy (CP-AFM) in which the molecular wire film bound to a gold substrate was contacted with a conductive AFM probe. By systematically measuring the low bias junction resistance as a function of length for molecules 1-4 nm long, we extracted the structure dependent tunneling attenuation factor (β) of 3.4 nm(-1) and a contact resistance of 220 kΩ. The crossover from tunneling to hopping transport was observed at a molecular length of 4-5 nm with an activation energy of 0.35 eV extracted from Arrhenius plots of resistance versus temperature. DFT calculations revealed localizations of spin densities (polarons) on molecular wire radical cations. The calculations were employed to gauge transition state energies for hopping of polarons along wire segments. Individual estimated transition state energies were 0.2-0.4 eV, in good agreement with the experimental activation energy. The transition states correspond to flattening of dihedral angles about specific imine bonds. These results open up possibilities to further explore the influence of molecular architecture on hopping transport in molecular junctions, and highlight the utility of DFT to understand charge localization and associated hopping-based transport.

A single-molecule diode

NASA Astrophysics Data System (ADS)

Elbing, Mark; Ochs, Rolf; Koentopp, Max; Fischer, Matthias; von Hänisch, Carsten; Weigend, Florian; Evers, Ferdinand; Weber, Heiko B.; Mayor, Marcel

2005-06-01

We have designed and synthesized a molecular rod that consists of two weakly coupled electronic π -systems with mutually shifted energy levels. The asymmetry thus implied manifests itself in a current-voltage characteristic with pronounced dependence on the sign of the bias voltage, which makes the molecule a prototype for a molecular diode. The individual molecules were immobilized by sulfur-gold bonds between both electrodes of a mechanically controlled break junction, and their electronic transport properties have been investigated. The results indeed show diode-like current-voltage characteristics. In contrast to that, control experiments with symmetric molecular rods consisting of two identical π -systems did not show significant asymmetries in the transport properties. To investigate the underlying transport mechanism, phenomenological arguments are combined with calculations based on density functional theory. The theoretical analysis suggests that the bias dependence of the polarizability of the molecule feeds back into the current leading to an asymmetric shape of the current-voltage characteristics, similar to the phenomena in a semiconductor diode. Author contributions: F.E., H.B.W., and M.M. designed research; M.E., R.O., M.K., M.F., F.E., H.B.W., and M.M. performed research; M.E., R.O., M.K., M.F., C.v.H., F.W., F.E., H.B.W., and M.M. contributed new reagents/analytic tools; M.E., R.O., M.K., C.v.H., F.E., H.B.W., and M.M. analyzed data; and F.E., H.B.W., and M.M. wrote the paper.This paper was submitted directly (Track II) to the PNAS office.Abbreviations: A, acceptor; D, donor; MCB, mechanically controlled break junction.Data deposition: The atomic coordinates have been deposited in the Cambridge Structural Database, Cambridge Crystallographic Data Centre, Cambridge CB2 1EZ, United Kingdom (CSD reference no. 241632).

Molecularly resolved protein electromechanical properties.

PubMed

Axford, Daniel; Davis, Jason J; Wang, Nan; Wang, Dongxu; Zhang, Tiantian; Zhao, Jianwei; Peters, Ben

2007-08-02

Previous work has shown that protein molecules can be trapped between the conductive surfaces presented by a metal-coated AFM probe and an underlying planar substrate where their molecule-specific conductance characteristics can be assayed. Herein, we demonstrate that transport across such a derived metal-protein-electrode junction falls within three, pressure-dependent, regimes and, further, that pressure-dependent conductance can be utilized in analyzing temporal variations of protein fold. Specifically, the electronic and mechanical properties of the metalloprotein azurin have been characterized under conditions of anisotropic vertical compression through the use of a conducting atomic force microscope (CP-AFM). By utilizing the ability of azurin to chemically self-assemble on the gold surface presented either by the apex of a suitably coated AFM probe or a planar metallic surface, molecular-level transport characteristics are assayable. Under conditions of low force, typically less than 2 nN, the weak physical and electronic coupling between the protein and the conducting contacts impedes tunneling and leads to charge buildup followed by dielectric breakdown. At slightly increased force, 3-5 nN, the copper protein exhibits temporal electron occupation with observable negative differential resistance, while the redox-inactive zinc mutant does not. At imposed loads greater than 5 nN, appreciable electron tunneling can be detected even at low bias for both the redox-active and -inactive species. Dynamic current-voltage characteristics have been recorded and are well-described by a modified Simmons tunneling model. Subsequent analyses enable the electron tunneling barrier height and barrier length to be determined under conditions of quantified vertical stress. The variance observed describes, in essence, the protein's mechanical properties within the confines of the tunnel junction.

Mechanistic Investigations of Branched Macromolecules and Metal Nanocomposites for Nonlinear Optical Applications

DTIC Science & Technology

2009-09-26

gold which show a band gap opening. them with alkyl or aryl thiolates and they are often referred as monolayer protected gold clusters (MPC...workers16-18, as well as Tsukuda and co-workers19 with several thiolate capped MPCs. The PI’s laboratory has observed luminescence mainly in the near...properties for sizes between ~50 and ~1000 atoms is not well understood. Careful analysis of absorption spectra for thiolate stabilized gold MPC

Au102(p-MBA)44 nanocluster, a superatom suitable for bio-applications

NASA Astrophysics Data System (ADS)

Häkkinen, Hannu

2016-12-01

Inorganic nanoparticles, including metals, semiconductors and metal oxides, comprise a common set of structures exhibiting an inorganic core `passivated' by an organic shell. Ligated inorganic nanoparticles currently provoke widespread fundamental interest in their structural, optical and magnetic properties, which differ fundamentally from bulk counterparts. These nanomaterials are already finding applications in biology, medicine, solar energy, and display panels. 1-6 Conjugating inorganic nanoparticles with organic (biological) material for applications in nanobiology and nanomedicine creates significant challenges for controlling the effects on the environment, particularly regarding toxicity. Chemical reactions of almost identical substances can lead to drastically different outcomes in a biological environment. As a simplistic example one can consider the case of ethanol vs. methanol. Ethanol (CH3CH2OH) can be consumed by humans while even a small dose of methanol (CH3OH) can be fatal, yet the difference between the molecular formulas of these substances is just the smallest meaningful hydrocarbon unit CH2. This illuminates the fact that minute differences in the size and structure of molecular compounds can have drastically different end effects in a biological environment due to the way the compounds start to react with the environment. In recent years, gold nanoparticles covered by ligands that make them water-soluble have become a popular target for research in nanobiology and nanomedicine. 1,2 In most cases up to now, colloidal nanoparticles (5 nm and larger) have been used for sensing and photothermal applications. However, this class of gold-based nanomaterials still has large uncertainties regarding the atomic composition of the nanoparticle surface and particularly the metal-ligand interface. A simple example illuminates the facts. The density of atoms in the fcc lattice of macrosocopic gold metal is about 59 atoms/nm3. This means that a spherical colloidal gold nanoparticle with radius of 5 nm has about 3850 atoms. Even in a sample of extremely narrow range of diameters ranging from 5.25 nm to 4.75 nm (+/- 5% of the mean) the particles will have anywhere between 3300 and 4750 atoms, and their surface area can differ up to 20%. It is clear that such particles are not suitable for applications that would need molecularly precise size, structure and shape of the metal nanoparticle and precise knowledge of the composition of its organic surface. In 1994, Brust, Schiffrin and coworkers published a landmark synthesis recipe on how to prepare thiol(ate)-stabilized small gold nanoparticles of about 2 nm in size. 7 This paper started a completely new field which has now matured to studies of several "atom-precise" or "molecularly precise" gold-thiolate compounds for which molecular formulas Aux(SR)y can be written and the substances in most cases have a good ambient stability allowing for storage and later use.8 Atomic structures of the gold core and the thiolate layer have been resolved for many of these compounds, opening doors for detailed density functional theory (DFT) simulations of their properties. This Perspective discusses developments in understanding the structure and properties of one of such compounds, which can be used for site-specific (or "molecularly precise") targeting of capsid proteins on a viral surface.

[ZHENG's gold hook fishing acupuncture for lumbar disc herniation: a clinical observation].

PubMed

Zhu, Bowen; Zhang, Xinghua; Sun, Runjie; Qin, Xiaoguang

2016-04-01

To compare the clinical efficacy differences between Zheng's gold hook, fishing acupuncture and electroacupuncture (EA) for lumbar disc herniation (LDH). Sixty patients of LDH were randomly allocated to a gold hook fishing acupuncture group and an EA group, 30 cases in each one. Lumbar Jiaji (EX-1 B 2), Yaoyangguan (GV 3), Shenshu (BL 23), Dachangshu (BL 25), Guanyuanshu (BL 26) and ashi points were selected in the gold hook fishing acupuncture group; after the needles were inserted, the manipulation of gold hook fishing acupuncture was applied at tendon junction points and ashi points. The identical acupoints were selected in the EA group and patients were treated with EA. The treatment was both given once a day; ten days of treatment were taken as one session, and totally 3 sessions were given. The clinical effective rate, visual analogue scale (VAS), low back pain score and Oswestry disability index (ODI) were used for efficacy evaluation. The effective rate was 93.3% (28/30) in the gold hook fishing acupuncture group, which was superior to 86.7% (26/30) in the EA group (P < 0.05). The VAS, low back pain score and ODI were both significantly improved after treatment (all P < 0.05), which were more significant in the gold hook fishing acupuncture group (all P < 0.05). ZHENG's gold hook fishing acupuncture could effectively improve the symptoms and sings of LDH, reduce the disability index and improve the quality of life, which is superior to EA.

A porphyrin complex of Gold(I): (Phosphine)gold(I) azides as cation precursors

PubMed Central

Partyka, David V.; Robilotto, Thomas J.; Zeller, Matthias; Hunter, Allen D.; Gray, Thomas G.

2008-01-01

A silver- and Brönsted acid-free protocol for generating the (tricyclohexylphosphine)gold(I) cation from the corresponding azide complexes is disclosed. The gold(I) cations so liberated are trapped by complexation with octaethylporphyrin. The first structurally authenticated gold(I) porphyrin complex crystallizes with formula C72H112Au2F12N4P2Sb2, space group C2/c, a = 21.388 (4), b = 19.679 (4), c = 19.231 (3) Å; β = 111.030 (3)°. Solution spectroscopic studies indicate that the di-gold complex fragments on dissolution in organic solvents. Approximate density-functional theory calculations find an electrostatic origin for the binding of two gold(I) centers to the unprotonated nitrogen atoms, despite greater orbital density on the porphyrin meso carbons. PMID:18780788

Spectrometric characteristics and tumor-affinity of a novel photosensitizer: mono-l-aspartyl aurochlorin e6 (Au-NPe6).

PubMed

Ishizumi, Taichiro; Aizawa, Katsuo; Tsuchida, Takaaki; Okunaka, Tetsuya; Kato, Harubumi

2004-12-01

Photodiagnosis and photodynamic therapy with photosensitizers can be indicated only for tumors of the superficial type, because these approaches utilizing visible light are limited by said light penetrability. To overcome this disadvantage, we innovated a novel photosensitizer, mono-l-aspartyl aurochlorin e6 (Au-NPe6), by incorporating a gold atom in the center of tetrapyrrole ring of NPe6 with a coordination bond. The gold atom in Au-NPe6 plays a role as an X-ray interceptor to detect deeply sited tumors. In this study, the absorption spectrum of novel Au-NPe6 in the diagnosis of deeply sited tumors was investigated, and the results were compared with the parent photosensitizer NPe6. Furthermore, the tumor-affinity of Au-NPe6 was evaluated using atomic absorption spectrometry. Despite the fact that both photosensitizers display a difference in the absorption spectrum, waveform changes of either photosensitizer with human serum albumin established a saturation point at a molar ratio of 1:1. The results indicate that it is highly possible that Au-NPe6 bound with albumin at a molar ratio (1:1) similar to NPe6. The accumulation rate of gold in tumor tissues was always significantly (p<0.05) higher than that in normal muscle tissues during the observation terms. Moreover, absorption spectra of tumor-tissue homogenates obtained from tumor-bearing mice after Au-NPe6 administration revealed a common peak with a wavelength equivalent to that of albumin-bond Au-NPe. This result suggests that the gold atom and NPe6 probably remained bonded even when Au-NPe6 was incorporated in tumor tissues.

Spin-Valve Effect in NiFe/MoS2/NiFe Junctions.

PubMed

Wang, Weiyi; Narayan, Awadhesh; Tang, Lei; Dolui, Kapildeb; Liu, Yanwen; Yuan, Xiang; Jin, Yibo; Wu, Yizheng; Rungger, Ivan; Sanvito, Stefano; Xiu, Faxian

2015-08-12

Two-dimensional (2D) layered transition metal dichalcogenides (TMDs) have been recently proposed as appealing candidate materials for spintronic applications owing to their distinctive atomic crystal structure and exotic physical properties arising from the large bonding anisotropy. Here we introduce the first MoS2-based spin-valves that employ monolayer MoS2 as the nonmagnetic spacer. In contrast with what is expected from the semiconducting band-structure of MoS2, the vertically sandwiched-MoS2 layers exhibit metallic behavior. This originates from their strong hybridization with the Ni and Fe atoms of the Permalloy (Py) electrode. The spin-valve effect is observed up to 240 K, with the highest magnetoresistance (MR) up to 0.73% at low temperatures. The experimental work is accompanied by the first principle electron transport calculations, which reveal an MR of ∼9% for an ideal Py/MoS2/Py junction. Our results clearly identify TMDs as a promising spacer compound in magnetic tunnel junctions and may open a new avenue for the TMDs-based spintronic applications.

Anomalous Photovoltaic Response of Graphene-on-GaN Schottky Photodiodes.

PubMed

Lee, Jae Hyung; Lee, Won Woo; Yang, Dong Won; Chang, Won Jun; Kwon, Sun Sang; Park, Won Il

2018-04-25

Graphene has attracted great attention as an alternative to conventional metallic or transparent conducting electrodes. Despite its similarities with conventional electrodes, recent studies have shown that a single-atom layer of graphene possesses unique characteristics, such as a tunable work function and transparencies for electric potential, reactivity, and wetting. Nevertheless, a systematic analysis of graphene and semiconductor junction characteristics has not yet been carried out. Here, we report the photoresponse characteristics of graphene-on-GaN Schottky junction photodiodes (Gr-GaN SJPDs), showing a typical rectifying behavior and distinct photovoltaic and photoelectric responses. Following the initial abrupt response to UV illumination, the Gr-GaN SJPDs exhibited a distinct difference in photocarrier dynamics depending on the applied bias voltage, which is characterized by either a negative or positive change in photocurrent with time. We propose underlying mechanisms for the anomalous photocarrier dynamics based on the interplay between electrostatic molecular interactions over the one-atom-thick graphene and GaN junction and trapped photocarriers at the defect states in the GaN thin film.

Comparative Study of the Binding of Concanavalin A to Self-Assembled Monolayers Containing a Thiolated α-Mannoside on Flat Gold and on Nanoporous Gold

PubMed Central

Pandey, Binod; Tan, Yih Horng; Fujikawa, Kohki; Demchenko, Alexei V.

2013-01-01

We have prepared SAMs containing 8-mercaptooctyl α-D-mannopyranoside, either as a single component or in mixed SAMs with n-octanethiol on flat gold surfaces and on nanoporous gold. Electrochemical impedance spectroscopy showed that the mixed SAMs on flat gold surfaces showed the highest Con A binding near 1:9 solution molar ratio of thiolatedα-mannoside to n-octanethiol whereas those on NPG showed the highest response at 1:19 solution molar ratio of thiolated α-mannoside to n-octanethiol. Atomic force microscopy was employed to image the monolayers, and also to image the bound Con A protein. PMID:23519474

Gold atoms and clusters on MgO(100) films; an EPR and IRAS study

NASA Astrophysics Data System (ADS)

Yulikov, M.; Sterrer, M.; Risse, T.; Freund, H.-J.

2009-06-01

Single gold atoms deposited on single crystalline MgO(1 0 0) films grown on Mo(1 0 0) are characterized by electron paramagnetic resonance spectroscopy as well as IR spectroscopy using CO as probe molecules. In this article we describe the first angular dependent measurements to determine the principal hyperfine components of a secondary hyperfine interaction, namely, with 17O of the MgO. The values determined here are in perfect agreement with theoretical expectations and corroborate the previously reported binding mechanism of Au atoms on the oxygen anions of the MgO terrace. The temperature dependent EPR data reveal an onset of Au atom mobility at about 80 K while the formation of Au particles occurs only above 125 K. By an analysis of the EPR line width in combination with STM measurements it is possible to deduce an increase of the interatomic distance above 80 K. The Au/CO complexes show a somewhat smaller temperature stability as compared to the Au atoms. The observed thermal stability is in perfect agreement with theoretical predictions for CO desorption.

Origin of the selectivity in the gold-mediated oxidation of benzyl alcohol

NASA Astrophysics Data System (ADS)

Rodríguez-Reyes, Juan Carlos F.; Friend, Cynthia M.; Madix, Robert J.

2012-08-01

Benzyl alcohol has received substantial attention as a probe molecule to test the selectivity and efficiency of novel metallic gold catalysts. Herein, the mechanisms of benzyl alcohol oxidation on a gold surface covered with atomic oxygen are elucidated; the results show direct correspondence to the reaction on gold-based catalysts. The selective, partial oxidation of benzyl alcohol to benzaldehyde is achieved with low oxygen surface concentrations and takes place through dehydrogenation of the alcohol to form benzaldehyde via a benzyloxy (C6H5-CH2O) intermediate. While in this case atomic oxygen plays solely a dehydrogenating role, at higher concentrations it leads to the formation of intermediates from benzaldehyde, producing benzoic acid and CO2. Facile ester (benzyl benzoate) formation also occurs at low oxygen concentrations, which indicates that benzoic acid is not a precursor of further oxidation of the ester; instead, the ester is produced by the coupling of adsorbed benzyloxy and benzaldehyde. Key to the high selectivity seen at low oxygen concentrations is the fact that the production of the aldehyde (and esters) is kinetically favored over the production of benzoic acid.

Chronic hemodynamic overload of the atria is an important factor for gap junction remodeling in human and rat hearts.

PubMed

Rucker-Martin, Catherine; Milliez, Paul; Tan, Sisareuth; Decrouy, Xavier; Recouvreur, Michel; Vranckx, Roger; Delcayre, Claude; Renaud, Jean-François; Dunia, Irene; Segretain, Dominique; Hatem, Stéphane N

2006-10-01

The expression and distribution of connexins is abnormal in a number of cardiac diseases, including atrial fibrillation, and is believed to favor conduction slowing and arrhythmia. Here, we studied the role of atrial structural remodeling in the disorganization of gap junctions and whether redistributed connexins can form new functional junction channels. Expression of connexin-43 (Cx43) was characterized by immunoblotting and immunohistochemistry in human right atrial specimens and in rat atria after myocardial infarction (MI). Gap junctions were studied by electron and 3-D microscopy, and myocyte-myocyte coupling was determined by Lucifer yellow dye transfer. In both chronically hemodynamically overloaded human atria in sinus rhythm and in dilated atria from MI-rats, Cx43 were dephosphorylated and redistributed from the intercalated disc to the lateral cell membranes as observed during atrial fibrillation. In MI-rats, the gap junctions at the intercalated disc were smaller (20% decrease) and contained very little Cx43 (0 or 1 gold particle vs. 42 to 98 in sham-operated rats). In the lateral membranes of myocytes, numerous connexon aggregates comprising non-phosphorylated Cx43 were observed. These connexon aggregates were in no case assembled into gap junction plaque-like structures. However, N-cadherin was well organized in the intercalated disc. There was very little myocyte-myocyte coupling in MI-rat atria and no myocyte-fibroblast coupling. Regression of the atrial remodeling was associated with the normalization of Cx43 localization. Structural alteration of the atrial myocardium is an important factor in the disorganization of connexins and gap junction. Moreover, redistributed Cx43 do not form junction channels.

Raman mapping and in situ SERS spectroelectrochemical studies of 6-mercaptopurine SAMs on the gold electrode.

PubMed

Yang, Haifeng; Liu, Yanli; Liu, Zhimin; Yang, Yu; Jiang, Jianhui; Zhang, Zongrang; Shen, Guoli; Yu, Ruqin

2005-02-24

The self-assembled monolayers (SAMs) of 6-mercaptopurine (6MP) were formed at the roughened polycrystalline gold surfaces in acid and alkaline media. The time-dependent Raman mapping spectral analysis in conjunction with the quantum calculations for the vibrational modes using ab initio BLYP/6-31G method suggested that both of the resulted 6MP SAMs adopted the same adsorption mode through the S atom of pyrimidine moiety and the N7 atom of the imidazole moiety anchoring the gold surface in a vertical way. The in situ surface-enhanced Raman scattering spectroelectrochemical experiment was conducted to examine the stability of the SAMs at various bias potentials. It was found that the detaching process of the 6MP SAMs from the surface involved one electron reduction as the voltage was applied at ca. 0.7 V vs a standard calomel electrode.

Single-atom gold catalysis in the context of developments in parahydrogen-induced polarization.

PubMed

Corma, Avelino; Salnikov, Oleg G; Barskiy, Danila A; Kovtunov, Kirill V; Koptyug, Igor V

2015-05-04

A highly isolated monoatomic gold catalyst, with single gold atoms dispersed on multiwalled carbon nanotubes (MWCNTs), has been synthesized, characterized, and tested in heterogeneous hydrogenation of 1,3-butadiene and 1-butyne with parahydrogen to maximize the polarization level and the contribution of the pairwise hydrogen addition route. The Au/MWCNTs catalyst was found to be active and efficient in pairwise hydrogen addition and the estimated contributions from the pairwise hydrogen addition route are at least an order of magnitude higher than those for supported metal nanoparticle catalysts. Therefore, the use of the highly isolated monoatomic catalysts is very promising for production of hyperpolarized fluids that can be used for the significant enhancement of NMR signals. A mechanism of 1,3-butadiene hydrogenation with parahydrogen over the highly isolated monoatomic Au/MWCNTs catalyst is also proposed. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Hydrogen in Mono-Atomic Gold Wires

NASA Astrophysics Data System (ADS)

Barnett, Robert N.; Sherbakov, Andrew G.; Landman, Uzi; Hakkinen, Hannu

2004-03-01

Results of ab-initio scalar relativistic density functional calculations of the interaction between a mono-atomic gold wire (suspended between two gold tips) and a hydrogen molecule, at various stages of wire stretching, are presented. The hydrogen molecule does not bind to the wire until the wire is sufficiently stretched, i.e. starting to break, at which time the molecule inserts itself into the wire restoring a fraction of the conductance quantum g. With subsequent compression of the wire the axis of the molecule gradually tips away from the wire axis until it becomes "quasi-dissociated" with the H-H axis perpendicular to the wire. At this point the conductance almost vanishes, while for the bare wire the conductance at this tip-to-tip separation is close to 1g. These results, and the frequency of various vibrational modes of the hydrogen molecule, are compared with recent experimental and theoretical work involving platinum wires.

Silicon-based visible and near-infrared optoelectric devices

DOEpatents

Mazur, Eric; Carey, James Edward

2017-10-17

In one aspect, the present invention provides a silicon photodetector having a surface layer that is doped with sulfur inclusions with an average concentration in a range of about 0.5 atom percent to about 1.5 atom percent. The surface layer forms a diode junction with an underlying portion of the substrate. A plurality of electrical contacts allow application of a reverse bias voltage to the junction in order to facilitate generation of an electrical signal, e.g., a photocurrent, in response to irradiation of the surface layer. The photodetector exhibits a responsivity greater than about 1 A/W for incident wavelengths in a range of about 250 nm to about 1050 nm, and a responsivity greater than about 0.1 A/W for longer wavelengths, e.g., up to about 3.5 microns.

Silicon-based visible and near-infrared optoelectric devices

DOEpatents

Mazur, Eric [Concord, MA; Carey, III, James E.

2011-02-08

In one aspect, the present invention provides a silicon photodetector having a surface layer that is doped with sulfur inclusions with an average concentration in a range of about 0.5 atom percent to about 1.5 atom percent. The surface layer forms a diode junction with an underlying portion of the substrate. A plurality of electrical contacts allow application of a reverse bias voltage to the junction in order to facilitate generation of an electrical signal, e.g., a photocurrent, in response to irradiation of the surface layer. The photodetector exhibits a responsivity greater than about 1 A/W for incident wavelengths in a range of about 250 nm to about 1050 nm, and a responsivity greater than about 0.1 A/W for longer wavelengths, e.g., up to about 3.5 microns.

Silicon-based visible and near-infrared optoelectric devices

DOEpatents

Mazur, Eric; Carey, III, James E.

2010-08-24

In one aspect, the present invention provides a silicon photodetector having a surface layer that is doped with sulfur inclusions with an average concentration in a range of about 0.5 atom percent to about 1.5 atom percent. The surface layer forms a diode junction with an underlying portion of the substrate. A plurality of electrical contacts allow application of a reverse bias voltage to the junction in order to facilitate generation of an electrical signal, e.g., a photocurrent, in response to irradiation of the surface layer. The photodetector exhibits a responsivity greater than about 1 A/W for incident wavelengths in a range of about 250 nm to about 1050 nm, and a responsivity greater than about 0.1 A/W for longer wavelengths, e.g., up to about 3.5 microns.

Silicon-based visible and near-infrared optoelectric devices

DOEpatents

Mazur, Eric [Concord, MA; Carey, III, James Edward

2009-03-17

In one aspect, the present invention provides a silicon photodetector having a surface layer that is doped with sulfur inclusions with an average concentration in a range of about 0.5 atom percent to about 1.5 atom percent. The surface layer forms a diode junction with an underlying portion of the substrate. A plurality of electrical contacts allow application of a reverse bias voltage to the junction in order to facilitate generation of an electrical signal, e.g., a photocurrent, in response to irradiation of the surface layer. The photodetector exhibits a responsivity greater than about 1 A/W for incident wavelengths in a range of about 250 nm to about 1050 nm, and a responsivity greater than about 0.1 A/W for longer wavelengths, e.g., up to about 3.5 microns.

Silicon-based visible and near-infrared optoelectric devices

DOEpatents

Carey, III, James Edward; Mazur, Eric [Concord, MA

2011-12-20

In one aspect, the present invention provides a silicon photodetector having a surface layer that is doped with sulfur inclusions with an average concentration in a range of about 0.5 atom percent to about 1.5 atom percent. The surface layer forms a diode junction with an underlying portion of the substrate. A plurality of electrical contacts allow application of a reverse bias voltage to the junction in order to facilitate generation of an electrical signal, e.g., a photocurrent, in response to irradiation of the surface layer. The photodetector exhibits a responsivity greater than about 1 A/W for incident wavelengths in a range of about 250 nm to about 1050 nm, and a responsivity greater than about 0.1 A/W for longer wavelengths, e.g., up to about 3.5 microns.

Silicon-based visible and near-infrared optoelectric devices

DOEpatents

Carey, III, James Edward; Mazur, Eric

2006-06-06

In one aspect, the present invention provides a silicon photodetector having a surface layer that is doped with sulfur inclusions with an average concentration in a range of about 0.5 atom percent to about 1.5 atom percent. The surface layer forms a diode junction with an underlying portion of the substrate. A plurality of electrical contacts allow application of a reverse bias voltage to the junction in order to facilitate generation of an electrical signal, e.g., a photocurrent, in response to irradiation of the surface layer. The photodetector exhibits a responsivity greater than about 1 A/W for incident wavelengths in a range of about 250 nm to about 1050 nm, and a responsivity greater than about 0.1 A/W for longer wavelengths, e.g., up to about 3.5 microns.

Silicon-based visible and near-infrared optoelectric devices

DOEpatents

Mazur, Eric; Carey, James Edward

2016-03-01

In one aspect, the present invention provides a silicon photodetector having a surface layer that is doped with sulfur inclusions with an average concentration in a range of about 0.5 atom percent to about 1.5 atom percent. The surface layer forms a diode junction with an underlying portion of the substrate. A plurality of electrical contacts allow application of a reverse bias voltage to the junction in order to facilitate generation of an electrical signal, e.g., a photocurrent, in response to irradiation of the surface layer. The photodetector exhibits a responsivity greater than about 1 A/W for incident wavelengths in a range of about 250 nm to about 1050 nm, and a responsivity greater than about 0.1 A/W for longer wavelengths, e.g., up to about 3.5 microns.

Silicon-based visible and near-infrared optoelectric devices

DOEpatents

Mazur, Eric; Carey, James Edward

2013-12-10

In one aspect, the present invention provides a silicon photodetector having a surface layer that is doped with sulfur inclusions with an average concentration in a range of about 0.5 atom percent to about 1.5 atom percent. The surface layer forms a diode junction with an underlying portion of the substrate. A plurality of electrical contacts allow application of a reverse bias voltage to the junction in order to facilitate generation of an electrical signal, e.g., a photocurrent, in response to irradiation of the surface layer. The photodetector exhibits a responsivity great than about 1 A/W for incident wavelengths in a range of about 250 nm to about 1050 nm, and a responsivity greater than about 0.1 A/W for longer wavelenths, e.g., up to about 3.5 microns.

The interaction of a gold atom with carbon nanohorn and carbon nanotube tips and their complexes with a CO molecule: A first principle calculation

NASA Astrophysics Data System (ADS)

Khongpracha, P.; Probst, M.; Limtrakul, J.

2008-07-01

The interactions of a gold atom with: (a) a single-wall carbon nanohorn (SWNH) conic tip; (b) with a single-wall carbon nanotube (SWNT) tip; and (c) their complexes with a CO molecule were studied using first-principle calculations based on density functional theory. The analysis of the pyramidalization angle (θp) as well as the π-orbital misalignment angles indicate that there should be many reactive carbon sites on the tips of SWNH and SWNT. It was found that SWNH provides reactive sites that can more selectively interact with the target atom. We identified five sites on both the SWNT tip and the nanohorn where attachment of a gold atom leads to a stable complex. This metal is found to be bi-coordinated with the tip of SWNH, while it is mono-coordinated with the SWNT tip. The largest interaction energies are -10.75 kcal/mol and -16.17 kcal/mol, respectively. The CO probe molecule binds to Au on the Au/SWNH or Au/SWNT tips with interaction energies of -22.34 and -18.29 kcal/mol, respectively. The main contributions of the interaction with both carbon nanostructures stems from σ-donation and π-backbonding. The results suggest that SWNHs could be one of the promising candidates for the development of high-specifity nanosensors.

Imaging and manipulation of adatoms on an alumina surface by noncontact atomic force microscopy

NASA Astrophysics Data System (ADS)

Simon, G. H.; Heyde, M.; Freund, H.-J.

2012-02-01

Noncontact atomic force microscopy (NC-AFM) has been performed on an aluminum oxide film grown on NiAl(110) in ultrahigh vacuum (UHV) at low temperature (5 K). Results reproduce the topography of the structural model, unlike scanning tunnelling microscopy (STM) images. Equipped with this extraordinary contrast the network of extended defects, which stems from domain boundaries intersecting the film surface, can be analysed in atomic detail. The knowledge of occurring surface structures opens up the opportunity to determine adsorption sites of individual adsorbates on the alumina film. The level of difficulty for such imaging depends on the imaging characteristics of the substrate and the interaction which can be maintained above the adsorbate. Positions of single adsorbed gold atoms within the unit cell have been determined despite their easy removal at slightly higher interaction strength. Preliminary manipulation experiments indicate a pick-up process for the vanishing of the gold adatoms from the film surface.

Gold–promoted structurally ordered intermetallic palladium cobalt nanoparticles for the oxygen reduction reaction

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kuttiyiel, Kurian A.; Sasaki, Kotaro; Su, Dong

2014-11-06

Considerable efforts to make palladium and palladium alloys active catalysts and a possible replacement for platinum have had a marginal success. Here, we report on a structurally ordered Au₁₀Pd₄₀Co₅₀ catalyst that exhibits comparable activity to conventional platinum catalysts in both acid and alkaline media. Electron microscopic techniques demonstrate that via addition of gold atoms PdCo nanoparticles undergo at elevated temperatures an atomic structural transition from core-shell to a rare intermetallic ordered structure with twin boundaries forming stable {111}, {110} and {100} facets. The superior stability of this catalyst compared to platinum after 10,000 potential cycles in alkaline media is attributedmore » to the atomic structural order of PdCo nanoparticles along with protective effect of clusters of gold atoms on the surface. This strategy of making ordered palladium intermetallic alloy nanoparticles can be used in diverse heterogeneous catalysis where particle size and structural stability matters.« less

Mono-Mercury Doping of Au25 and the HOMO/LUMO Energies Evaluation Employing Differential Pulse Voltammetry.

PubMed

Liao, Lingwen; Zhou, Shiming; Dai, Yafei; Liu, Liren; Yao, Chuanhao; Fu, Cenfeng; Yang, Jinlong; Wu, Zhikun

2015-08-05

Controlling the bimetal nanoparticle with atomic monodispersity is still challenging. Herein, a monodisperse bimetal nanoparticle is synthesized in 25% yield (on gold atom basis) by an unusual replacement method. The formula of the nanoparticle is determined to be Au24Hg1(PET)18 (PET: phenylethanethiolate) by high-resolution ESI-MS spectrometry in conjunction with multiple analyses including X-ray photoelectron spectroscopy (XPS) and thermogravimetric analysis (TGA). X-ray single-crystal diffraction reveals that the structure of Au24Hg1(PET)18 remains the structural framework of Au25(PET)18 with one of the outer-shell gold atoms replaced by one Hg atom, which is further supported by theoretical calculations and experimental results as well. Importantly, differential pulse voltammetry (DPV) is first employed to estimate the highest occupied molecular orbit (HOMO) and the lowest unoccupied molecular orbit (LUMO) energies of Au24Hg1(PET)18 based on previous calculations.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Paulauskas, Tadas; Buurma, Christopher; Colegrove, Eric

Dislocation cores have long dominated the electronic and optical behaviors of semiconductor devices and detailed atomic characterization is required to further explore their effects. Miniaturization of semiconductor devices to nanometre scale also puts emphasis on a material's mechanical properties to withstand failure due to processing or operational stresses. Sessile junctions of dislocations provide barriers to propagation of mobile dislocations and may lead to work-hardening. The sessile Lomer–Cottrell and Hirth lock dislocations, two stable lowest elastic energy stair-rods, are studied in this paper. More specifically, using atomic resolution high-angle annular dark-field imaging and atomic-column-resolved X-ray spectrum imaging in an aberration-corrected scanningmore » transmission electron microscope, dislocation core structures are examined in zinc-blende CdTe. A procedure is outlined for atomic scale analysis of dislocation junctions which allows determination of their identity with specially tailored Burgers circuits and also formation mechanisms of the polar core structures based on Thompson's tetrahedron adapted to reactions of polar dislocations as they appear in CdTe and other zinc-blende solids. Strain fields associated with the dislocations calculatedviageometric phase analysis are found to be diffuse and free of `hot spots' that reflect compact structures and low elastic energy of the pure-edge stair-rods.« less

Tunable synthesis and acetylation of dendrimer-entrapped or dendrimer-stabilized gold-silver alloy nanoparticles.

PubMed

Liu, Hui; Shen, Mingwu; Zhao, Jinglong; Guo, Rui; Cao, Xueyan; Zhang, Guixiang; Shi, Xiangyang

2012-06-01

In this study, amine-terminated generation 5 poly(amidoamine) dendrimers were used as templates or stabilizers to synthesize dendrimer-entrapped or dendrimer-stabilized Au-Ag alloy nanoparticles (NPs) with different gold atom/silver atom/dendrimer molar ratios with the assistance of sodium borohydride reduction chemistry. Following a one-step acetylation reaction to transform the dendrimer terminal amines to acetyl groups, a series of dendrimer-entrapped or dendrimer-stabilized Au-Ag alloy NPs with terminal acetyl groups were formed. The formed Au-Ag alloy NPs before and after acetylation reaction were characterized using different techniques. We showed that the optical property and the size of the bimetallic NPs were greatly affected by the metal composition. At the constant total metal atom/dendrimer molar ratio, the size of the alloy NPs decreased with the gold content. The formed Au-Ag alloy NPs were stable at different pH (pH 5-8) and temperature (4-50°C) conditions. X-ray absorption coefficient measurements showed that the attenuation of the binary NPs was dependent on both the gold content and the surface modification. With the increase of gold content in the binary NPs, their X-ray attenuation intensity was significantly enhanced. At a given metal composition, the X-ray attenuation intensity of the binary NPs was enhanced after acetylation. Cytotoxicity assays showed that after acetylation, the cytocompatibility of Au-Ag alloy NPs was significantly improved. With the controllable particle size and optical property, metal composition-dependent X-ray attenuation characteristics, and improved cytocompatibility after acetylation, these dendrimer-entrapped or dendrimer-stabilized Au-Ag alloy NPs should have a promising potential for CT imaging and other biomedical applications. Copyright © 2012 Elsevier B.V. All rights reserved.

Influence of the pH value of a colloidal gold solution on the absorption spectra of an LSPR-assisted sensor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhu, Jin; Li, Wenbin; Zhu, Mao

2014-03-15

The localized surface plasmon resonances (LSPRs) of gold particles assembled on a crystal plate are a powerful tool for biological sensors. Here, we prepare gold colloids in different pH solutions. We monitor the effects of the particle radius and particle coverage on the absorption spectra of AT-cut (r-face dihedral angle of about 3°) crystal plates supporting gold nanoparticles. The surface morphologies were monitored on silicon dioxide substrates using ultraviolet and visible (UV-vis) spectroscopy, and atomic force microscopy (AFM). The results showed that the gold particle coverage decreases with increasing pH value of the gold colloid solution. This phenomenon demonstrates thatmore » self-assembled gold surfaces were formed via the electrostatic adsorption of gold particles on the positively charged, ionized amino groups on the crystal plates in the acidic solution. The spectrum of gold nanoparticles with different coverage degree on the crystal plates showed that the LSPR properties are highly dependent on pH.« less

In Situ Gold Nanoparticle Gradient Formation in a 3D Meso- and Macroporous Polymer Matrix.

PubMed

Penders, Jelle; Rajasekharan, Anand K; Hulander, Mats; Andersson, Martin

2017-08-01

Herein, the development and characterization of a 3D gradient structure of gold nanoparticles is described. The gradient of gold nanoparticles is made in situ in a macroporous nonionic block copolymer hydrogel matrix, through gold ion diffusion control. The polymer provides a matrix for diffusion of gold ions, acts as a template for controlling nanoparticle growth, and facilitates the in situ reduction of gold ions to gold nanoparticles. A clear gradient in gold nanoparticles is observed across the 3D space of the polymer matrix using scanning electron microscopy, fluorescence microscopy, atomic force microscopy, and thermogravimetric analysis. The particle gradient is further functionalized with both hydrophobic and hydrophilic groups via thiol-gold linkage to demonstrate the ability to form gradients with different chemical functionalities. Using additive manufacturing, the polymer can also be printed as a porous network with possible applications for 3D cell culturing in, e.g., biomaterials research. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Optimal energy for cell radiosensitivity enhancement by gold nanoparticles using synchrotron-based monoenergetic photon beams

PubMed Central

Rahman, Wan Nordiana; Corde, Stéphanie; Yagi, Naoto; Abdul Aziz, Siti Aishah; Annabell, Nathan; Geso, Moshi

2014-01-01

Gold nanoparticles have been shown to enhance radiation doses delivered to biological targets due to the high absorption coefficient of gold atoms, stemming from their high atomic number (Z) and physical density. These properties significantly increase the likelihood of photoelectric effects and Compton scattering interactions. Gold nanoparticles are a novel radiosensitizing agent that can potentially be used to increase the effectiveness of current radiation therapy techniques and improve the diagnosis and treatment of cancer. However, the optimum radiosensitization effect of gold nanoparticles is strongly dependent on photon energy, which theoretically is predicted to occur in the kilovoltage range of energy. In this research, synchrotron-generated monoenergetic X-rays in the 30–100 keV range were used to investigate the energy dependence of radiosensitization by gold nanoparticles and also to determine the photon energy that produces optimum effects. This investigation was conducted using cells in culture to measure dose enhancement. Bovine aortic endothelial cells with and without gold nanoparticles were irradiated with X-rays at energies of 30, 40, 50, 60, 70, 81, and 100 keV. Trypan blue exclusion assays were performed after irradiation to determine cell viability. Cell radiosensitivity enhancement was indicated by the dose enhancement factor which was found to be maximum at 40 keV with a value of 3.47. The dose enhancement factor obtained at other energy levels followed the same direction as the theoretical calculations based on the ratio of the mass energy absorption coefficients of gold and water. This experimental evidence shows that the radiosensitization effect of gold nanoparticles varies with photon energy as predicted from theoretical calculations. However, prediction based on theoretical assumptions is sometimes difficult due to the complexity of biological systems, so further study at the cellular level is required to fully characterize the effects of gold nanoparticles with ionizing radiation. PMID:24899803

Optimal energy for cell radiosensitivity enhancement by gold nanoparticles using synchrotron-based monoenergetic photon beams.

PubMed

Rahman, Wan Nordiana; Corde, Stéphanie; Yagi, Naoto; Abdul Aziz, Siti Aishah; Annabell, Nathan; Geso, Moshi

2014-01-01

Gold nanoparticles have been shown to enhance radiation doses delivered to biological targets due to the high absorption coefficient of gold atoms, stemming from their high atomic number (Z) and physical density. These properties significantly increase the likelihood of photoelectric effects and Compton scattering interactions. Gold nanoparticles are a novel radiosensitizing agent that can potentially be used to increase the effectiveness of current radiation therapy techniques and improve the diagnosis and treatment of cancer. However, the optimum radiosensitization effect of gold nanoparticles is strongly dependent on photon energy, which theoretically is predicted to occur in the kilovoltage range of energy. In this research, synchrotron-generated monoenergetic X-rays in the 30-100 keV range were used to investigate the energy dependence of radiosensitization by gold nanoparticles and also to determine the photon energy that produces optimum effects. This investigation was conducted using cells in culture to measure dose enhancement. Bovine aortic endothelial cells with and without gold nanoparticles were irradiated with X-rays at energies of 30, 40, 50, 60, 70, 81, and 100 keV. Trypan blue exclusion assays were performed after irradiation to determine cell viability. Cell radiosensitivity enhancement was indicated by the dose enhancement factor which was found to be maximum at 40 keV with a value of 3.47. The dose enhancement factor obtained at other energy levels followed the same direction as the theoretical calculations based on the ratio of the mass energy absorption coefficients of gold and water. This experimental evidence shows that the radiosensitization effect of gold nanoparticles varies with photon energy as predicted from theoretical calculations. However, prediction based on theoretical assumptions is sometimes difficult due to the complexity of biological systems, so further study at the cellular level is required to fully characterize the effects of gold nanoparticles with ionizing radiation.

Gd@Au15: A magic magnetic gold cluster for cancer therapy and bioimaging

NASA Astrophysics Data System (ADS)

Yadav, Brahm Deo; Kumar, Vijay

2010-09-01

We report from ab initio calculations a magic magnetic cage cluster of gold, Gd@Au15, obtained by doping of a Gd atom in gold clusters. It has a highest occupied molecular orbital-lowest unoccupied molecular orbital gap of 1.31 eV within the generalized gradient approximation that makes it a potential candidate for cancer therapy with an additional attractive feature that its large magnetic moment of 7 μB could be beneficial for magnetic resonance imaging.

Elucidating Complex Surface Reconstructions with Atomic-Resolution Scanning Tunneling Microscopy: Au(100)-Aqueous Electrochemical Interface

DTIC Science & Technology

1992-05-01

that unusually high-quality STM data of this type 5-7can be obtained at ordered gold -aqueous interfaces. Reconstruction is seen 2 to be triggered on...all three low-index gold surfaces by altering the potential to values corresponding to small (10-15 pC cm-2 ) negative surface electronic 5-7 charges...connections. The former was platinum and the latter was a freshly electrooxidized gold wire. All electrode potentials quoted here, however, are

Functionalization of surfactant wrapped graphenenanosheets with alkylazides for enhanced dispersibility

NASA Astrophysics Data System (ADS)

Vadukumpully, Sajini; Gupta, Jhinuk; Zhang, Yongping; Xu, Guo Qin; Valiyaveettil, Suresh

2011-01-01

A facile and simple approach for the covalent functionalization of surfactant wrapped graphene sheets is described. The approach involves functionalization of dispersible graphene sheets with various alkylazides and 11-azidoundecanoic acid proved the best azide for enhanced dispersibility. The functionalization was confirmed by infrared spectroscopy and scanning tunneling microscopy. The free carboxylic acidgroups can bind to gold nanoparticles, which were introduced as markers for the reactive sites. The interaction between gold nanoparticles and the graphene sheets was followed by UV-vis spectroscopy. The gold nanoparticle-graphene composite was characterized by transmission electron microscopy and atomic force microscopy, demonstrating the uniform distribution of gold nanoparticles all over the surface. Our results open the possibility to control the functionalization on graphene in the construction of composite nanomaterials.A facile and simple approach for the covalent functionalization of surfactant wrapped graphene sheets is described. The approach involves functionalization of dispersible graphene sheets with various alkylazides and 11-azidoundecanoic acid proved the best azide for enhanced dispersibility. The functionalization was confirmed by infrared spectroscopy and scanning tunneling microscopy. The free carboxylic acidgroups can bind to gold nanoparticles, which were introduced as markers for the reactive sites. The interaction between gold nanoparticles and the graphene sheets was followed by UV-vis spectroscopy. The gold nanoparticle-graphene composite was characterized by transmission electron microscopy and atomic force microscopy, demonstrating the uniform distribution of gold nanoparticles all over the surface. Our results open the possibility to control the functionalization on graphene in the construction of composite nanomaterials. Electronic Supplementary Information (ESI) available: Synthesis and characterization details of dodecylazide, hexylazide, 11-azidoundecanol (AUO), micrographs (SEM and TEM images) of the various azide functionalized samples and the statistical analysis of the graphene thickness. See 10.1039/c0nr00547a.

Structural and dynamical characterization of water on the Au (100) and graphene surfaces: A molecular dynamics simulation approach

NASA Astrophysics Data System (ADS)

Foroutan, Masumeh; Darvishi, Mehdi; Fatemi, S. Mahmood

2017-09-01

The positioning, adsorption, and movement of water on substrates is dependent upon the chemical nature and arrangement of the atoms of the surface. Therefore the behavior of water molecules on a substrate is a reflection of properties of the surface. Based on this premise, graphene and gold substrates were chosen to study this subject from a molecular perspective. In this work, the structural and dynamical behaviors of a water nanodroplet on Au (100) and the graphene interfaces have been studied by molecular dynamics simulation. The results have shown how the structural and dynamical behaviors of water molecules at the interface reflect the characteristics of these surfaces. The results have demonstrated that residence time and hydrogen bonds' lifetime at the water-Au (100) interface are bigger than at the water-graphene interface. Energy contour map analysis indicates a more uniform surface energy on graphene than on the gold surface. The obtained results illustrate that water clusters on gold and graphene form tetramer and hexamer structures, respectively. Furthermore, the water molecules are more ordered on the gold surface than on graphene. The study of hydrogen bonds showed that the order, stability, and the number of hydrogen bonds is higher on the gold surface. The positioning pattern of water molecules is also similar to the arrangement of gold atoms while no regularity was observed on graphene. The study of dynamical behavior of water molecules revealed that the movement of water on gold is much less than on graphene which is in agreement with the strong water-gold interaction in comparison to the water-graphene interaction.

Separation and Enrichment of Gold in Water, Geological and Environmental Samples by Solid Phase Extraction on Multiwalled Carbon Nanotubes Prior to its Determination by Flame Atomic Absorption Spectrometry.

PubMed

Duran, Ali; Tuzen, Mustafa; Soylak, Mustafa

2015-01-01

This study proposes the application of multi-walled carbon nanotubes as a solid sorbent for the preconcentration of gold prior to its flame atomic absorption spectrometry determination. Extraction was achieved by using a glass column (15.0 cm in length and 1.0 cm in diameter). Quantitative recoveries were obtained in the pH range of 2.5-4.0; the elution step was carried out with 5.0 ml of 1.0 mol/L HNO3 in acetone. In the ligand-free study, variables such as pH, eluent type, sample volume, flow rates, and matrix effect were examined for the optimum recovery of gold ions. The gold ions were able to be pre-concentrated by a factor of 150 and their LOD was determined to be 1.71 μg/L. In order to evaluate the accuracy of the developed method, addition-recovery tests were applied for the tap water, mineral water, and sea water samples. Gold recovery studies were implemented using a wet digestion technique for mine and soil samples taken from various media, and this method was also applied for anodic slime samples taken from the factories located in the Kayseri Industrial Zone of Turkey.

Optimum Particle Size for Gold-Catalyzed CO Oxidation

PubMed Central

2018-01-01

The structure sensitivity of gold-catalyzed CO oxidation is presented by analyzing in detail the dependence of CO oxidation rate on particle size. Clusters with less than 14 gold atoms adopt a planar structure, whereas larger ones adopt a three-dimensional structure. The CO and O2 adsorption properties depend strongly on particle structure and size. All of the reaction barriers relevant to CO oxidation display linear scaling relationships with CO and O2 binding strengths as main reactivity descriptors. Planar and three-dimensional gold clusters exhibit different linear scaling relationship due to different surface topologies and different coordination numbers of the surface atoms. On the basis of these linear scaling relationships, first-principles microkinetics simulations were conducted to determine CO oxidation rates and possible rate-determining step of Au particles. Planar Au9 and three-dimensional Au79 clusters present the highest CO oxidation rates for planar and three-dimensional clusters, respectively. The planar Au9 cluster is much more active than the optimum Au79 cluster. A common feature of optimum CO oxidation performance is the intermediate binding strengths of CO and O2, resulting in intermediate coverages of CO, O2, and O. Both these optimum particles present lower performance than maximum Sabatier performance, indicating that there is sufficient room for improvement of gold catalysts for CO oxidation. PMID:29707098

Coprecipitation of gold(III) complex ions with manganese(II) hydroxide and their stoichiometric reduction to atomic gold (Au(0)): analysis by Mössbauer spectroscopy and XPS.

PubMed

Yamashita, Mamiko; Ohashi, Hironori; Kobayashi, Yasuhiro; Okaue, Yoshihiro; Kurisaki, Tsutomu; Wakita, Hisanobu; Yokoyama, Takushi

2008-03-01

To elucidate the formation process of precursor of gold-supported manganese dioxide (MnO2), the coprecipitation behavior of [AuCl4-n(OH)n](-) (n=0-4) (Au(III)) complex ions with manganese(II) hydroxide (Mn(OH)2 and the change in their chemical state were examined. The Au(III) complex ions were rapidly and effectively coprecipitated with Mn(OH)(2) at pH 9. According to the Mössbauer spectra for gold (Au) coprecipitated with Mn(OH)2, below an Au content of 60 wt% in the coprecipitates, all of the coprecipitated Au existed in the atomic state (Au(0)), while, above an Au content of 65 wt%, part of the gold existed in the Au(III) state, and the proportion increased with increasing coprecipitated Au content. Based on the results of X-ray photoelectron spectroscopy, Mn(II) in Mn(OH)2 converted to Mn(IV) in conjunction with coprecipitation of Au(III) complex ions. These results indicate that the rapid stoichiometric reduction of Au(III) to Au(0) is caused by electron transfer from Mn(II) in Mn(OH)2 to the Au(III) complex ion through an Mn-O-Au bond.

Solid sampling high-resolution continuum source graphite furnace atomic absorption spectrometry for gold determination in geological samples after preconcentration onto carbon nanotubes

NASA Astrophysics Data System (ADS)

Dobrowolski, Ryszard; Mróz, Agnieszka; Dąbrowska, Marzena; Olszański, Piotr

2017-06-01

A novelty method for the determination of gold in geological samples by solid sampling high-resolution continuum source graphite furnace atomic absorption spectrometry (SS HR CS GF AAS) after solid-phase extraction onto modified carbon nanotubes (CNT) was described. The methodology developed is based on solid phase extraction of Au(III) ions from digested samples to eliminate strong interference caused by iron compounds and problems related to inhomogeneities of the samples. The use of aqueous or solid standard for calibration was studied and the slope of calibration curve was the same for both of these modes. This statement indicates the possibility to perform the calibration of the method using aqueous standard solutions. Under optimum conditions the absolute detection limit for gold was equal to 2.24 · 10- 6 μg g- 1 while the adsorption capacity of modified carbon nanotubes was 264 mg g- 1. The proposed procedure was validated by the application of certified reference materials (CRMs) with different content of gold and different matrix, the results were in good agreement with certified values. The method was successfully applied for separation and determination of gold ions in complex geological samples, with precision generally better than 8%.

Structures of ˜100 nm Size Produced by Atom Lithography with Metastable He

NASA Astrophysics Data System (ADS)

Reeves, Jason; Corder, Christopher; Lu, Xiaoxu; Allred, Claire; Metcalf, Harold

2010-03-01

We have used neutral atom lithography with metastable 2^3S He (He*) to produce structures of size ˜100 nm. A beam of He* from our source is collimated by the bichromatic forceootnotetextM. Partlow et al., Phys. Rev. Lett. 93, 213004 (2004) and then by optical molasses. Atoms cross a standing wave of λ= 389 nm light tuned ˜80 MHz below the 2^3S1->3^3P2 transition and are focussed into lines striking a self assembled monolayer (SAM) of nonanethiol coated over a gold film on a single crystal Si wafer. The 20 eV internal energy of He* destroys the SAM molecules ultimately leaving a pattern of SAM on the gold. Subsequent etching of the unprotected region of the gold results in these featuresootnotetextC. Allred et al., submitted to J. Appl. Phys.^,ootnotetextC. Allred, Ph.D. Thesis, Stony Brook, NY (2009) - unpublished.. The lines are separated by 194.5 nm and they occupy about 60% of their spacing. AFM measurements of our first samples show their width to be ˜120 nm and their depth to be ˜10 nm.

Structures of ˜100 nm Size Produced by Atom Lithography with Metastable He

NASA Astrophysics Data System (ADS)

Reeves, Jason; Corder, Christopher; Lu, Xiaoxu; Allred, Claire; Metcalf, Harold

2010-03-01

We have used neutral atom lithography with metastable 2^3S He (He*) to produce structures of size ˜100 nm. A beam of He* from our source is collimated by the bichromatic forcefootnotetextM. Partlow et al., Phys. Rev. Lett. 93, 213004 (2004) and then by optical molasses. Atoms cross a standing wave of λ= 389 nm light tuned ˜80 MHz below the 2^3S1->3^3P2 transition and are focussed into lines striking a self assembled monolayer (SAM) of nonanethiol coated over a gold film on a single crystal Si wafer. The 20 eV internal energy of He* destroys the SAM molecules ultimately leaving a pattern of SAM on the gold. Subsequent etching of the unprotected region of the gold results in these featuresfootnotetextC. Allred et al., submitted to J. Appl. Phys.^,footnotetextC. Allred, Ph.D. Thesis, Stony Brook, NY (2009) - unpublished.. The lines are separated by 194.5 nm and they occupy about 60% of their spacing. AFM measurements of our first samples show their width to be ˜120 nm and their depth to be ˜10 nm.

Toward Scalable Ion Traps for Quantum Information Processing

DTIC Science & Technology

2010-01-01

3/033031 Abstract. In this paper, we report the design, fabrication and preliminary testing of a 150 zone ion trap array built in a ‘ surface ...gates [4–6]. We report here on the design, fabrication and preliminary testing of a large array built in a ‘ surface -electrode’ geometry [7, 8] and...report the first transport of atomic ions through a surface -electrode trap junction. Transport of ions through a junction has been demonstrated previously

Nanoscale insight into the p-n junction of alkali-incorporated Cu(In,Ga)Se 2 solar cells

DOE PAGES

Stokes, Adam; Al-Jassim, Mowafak; Norman, Andrew; ...

2017-04-05

The effects of alkali diffusion and post-deposition treatment in three-stage processed Cu(In,Ga)Se 2 solar cells are examined by using atom probe tomography and electrical property measurements. Cells, for which the substrate was treated at 650 °C to induce alkali diffusion from the substrate prior to absorber deposition, exhibited high open-circuit voltage (758 mV) and efficiency (18.2%) and also exhibited a 50 to 100-nm-thick ordered vacancy compound layer at the metallurgical junction. Surprisingly, these high-temperature samples exhibited higher concentrations of K at the junction (1.8 at.%) than post-deposition treatment samples (0.4 at.%). A model that uses Ga/(Ga + In) and Cu/(Gamore » + In) profiles to predict bandgaps (+/-17.9 meV) of 22 Cu(In,Ga)Se2 solar cells reported in literature was discussed and ultimately used to predict band properties at the nanoscale by using atom probe tomography data. The high-temperature samples exhibited a greater drop in the valence band maximum (200 meV) due to a lower Cu/(Ga + In) ratio than the post-deposition treatment samples. There was an anticorrelation of K concentrations and Cu/(Ga + In) ratios for all samples, regardless of processing conditions. In conclusion, changes in elemental profiles at the active junctions correlate well with the electrical behaviour of these devices.« less

Normal metal - insulator - superconductor thermometers and coolers with titanium-gold bilayer as the normal metal

NASA Astrophysics Data System (ADS)

Räisänen, I. M. W.; Geng, Z.; Kinnunen, K. M.; Maasilta, I. J.

2018-03-01

We have fabricated superconductor - insulator - normal metal - insulator - superconductor (SINIS) tunnel junctions in which Al acts as the superconductor, AlOx is the insulator, and the normal metal consists of a thin Ti layer (5 nm) covered with a thicker Au layer (40 nm). We have characterized the junctions by measuring their current-voltage curves between 60 mK and 750 mK. For comparison, the same measurements have been performed for a SINIS junction pair whose normal metal is Cu. The Ti-Au bilayer decreases the SINIS tunneling resistance by an order of magnitude compared to junctions where Cu is used as normal metal, made with the same oxidation parameters. The Ti-Au devices are much more robust against chemical attacks, and their lower tunneling resistance makes them more robust against static charge. More significantly, they exhibit significantly stronger electron cooling than Cu devices with identical fabrication steps, when biased close to the energy gap of the superconducting Al. By using a self-consistent thermal model, we can fit the current-voltage characteristics well, and show an electron cooling from 200 mK to 110 mK, with a non-optimized device.

Secret in the Margins: Rutherford's Gold Foil Experiment

ERIC Educational Resources Information Center

Aydin, Sevgi; Hanuscin, Deborah L.

2011-01-01

In this article, the authors describe a lesson that uses the 5E Learning Cycle to help students not only understand the atomic model but also how Ernest Rutherford helped develop it. The lesson uses Rutherford's gold foil experiment to focus on three aspects of the nature of science: the empirical nature of science, the tentativeness of scientific…

Recovery of gold from electronic waste using chemical assisted microbial biosorption (hybrid) technique.

PubMed

Sheel, Anvita; Pant, Deepak

2018-01-01

The aim of present study was to develop a modified method of gold recovery from e-waste. Selective biosorption of gold from contact point of printed circuit board was achieved by using the combination of ammonium thiosulfate (AT) and Lactobacillus acidophilus (LA).Improvement in biosorption was due to the π-π interaction and resultant change in amide absorption bond between AT and LA, as evidenced by infrared spectroscopy. Selection was justified by some basic postulates of ionic radii and confirmed by inductively coupled plasma atomic emission spectroscopy. This methodology provides a unique leaching-sorption method for gold recovery and 85% of gold was recovered (from AT leachant) by the proposed combination. Copyright © 2017 Elsevier Ltd. All rights reserved.

New processes and materials for ultraviolet detection with solid state devices

NASA Technical Reports Server (NTRS)

Chopra, D.

1977-01-01

The three major effects that degrade external responsivity of silicon from the 1/lambda theoretical curve for a quantum detector are: surface reflectance, surface recombination, and junction depth. Since the p-n junction must be very shallow, problems relating to surface are further enhanced. MOS type of processing is necessary. HCl oxides and numerous acid clean-ups are utilized in order to obtain a contamination free surface with low Qss levels. Stringent process controls such as CV shifts, spreading resistance measurements, thickness monitoring etc., are used to analyze the surface contaminations, surface mobile charges, surface concentrations, junction depth, oxide thickness etc. Low surface concentrations of 10 to the 18th atoms/cu cm are achieved by low temperature boron nitride depositions. Shallow junction depths of the order of a few tenths of a micron are achieved by low temperature controlled diffusions. In order to improve breakdown characteristics of these shallow junction devices, field plate and deep diffused p(+) ring geometries are used.

Synthesis of gold nanoparticles with graphene oxide.

PubMed

Wang, Wenshuo; He, Dawei; Zhang, Xiqing; Duan, Jiahua; Wu, Hongpeng; Xu, Haiteng; Wang, Yongsheng

2014-05-01

Single sheets of functionalized graphene oxide are derived through chemical exfoliation of natural flake graphite. We present an effective synthetic method of graphene-gold nanoparticles hybrid nanocomposites. AFM (Atomic Force Microscope) was used to measure the thickness of the individual GO nanosheet. FTIR (Fourier transform infrared) spectroscopy was used to verify the attachment of oxygen functionalities on the surface of graphene oxide. TEM (Transmission Electron Microscope) data revealed the average diameters of the gold colloids and characterized the composite particles situation. Absorption spectroscopy showed that before and after synthesis the gold particle size did not change. Our studies indicate that the hybrid is potential substrates for catalysts and biosensors.

Two-dimensional gold nanostructures with high activity for selective oxidation of carbon–hydrogen bonds

PubMed Central

Wang, Liang; Zhu, Yihan; Wang, Jian-Qiang; Liu, Fudong; Huang, Jianfeng; Meng, Xiangju; Basset, Jean-Marie; Han, Yu; Xiao, Feng-Shou

2015-01-01

Efficient synthesis of stable two-dimensional (2D) noble metal catalysts is a challenging topic. Here we report the facile synthesis of 2D gold nanosheets via a wet chemistry method, by using layered double hydroxide as the template. Detailed characterization with electron microscopy and X-ray photoelectron spectroscopy demonstrates that the nanosheets are negatively charged and [001] oriented with thicknesses varying from single to a few atomic layers. X-ray absorption spectroscopy reveals unusually low gold–gold coordination numbers. These gold nanosheets exhibit high catalytic activity and stability in the solvent-free selective oxidation of carbon–hydrogen bonds with molecular oxygen. PMID:25902034

Comparison of amino acids interaction with gold nanoparticle.

PubMed

Ramezani, Fatemeh; Amanlou, Massoud; Rafii-Tabar, Hashem

2014-04-01

The study of nanomaterial/biomolecule interface is an important emerging field in bionanoscience, and additionally in many biological processes such as hard-tissue growth and cell-surface adhesion. To have a deeper understanding of the amino acids/gold nanoparticle assemblies, the adsorption of these amino acids on the gold nanoparticles (GNPs) has been investigated via molecular dynamics simulation. In these simulations, all the constituent atoms of the nanoparticles were considered to be dynamic. The geometries of amino acids, when adsorbed on the nanoparticle, were studied and their flexibilities were compared with one another. The interaction of each of 20 amino acids was considered with 3 and 8 nm gold GNPs.

Environmental impact of the gold mining industry in Ghana.

PubMed

Bamford, S A; Osae, E; Aboh, I; Biney, C A; Antwi, L A

1990-01-01

X-ray Fluorescence (XRF) Analysis and Atomic Absorption Spectrophotometry (AAS) have been used in assessing heavy metal pollution from some gold mines in Ghana. The presence and levels of heavy metals in gold ore, gold tailings, inland waters, and river sediments have been determined. Using these techniques, the heavy metals: Cr, Mn, Fe, Cu, Zn, As, Pb, Rb, Sr, Y, Zr, and Nb were identified in some of the solid samples within a concentration range of 0.08 ppm--4.9%. However, the inland waters showed the presence of only Fe and Zn at levels of 0.08-2.4 micrograms/mL.

Evidence for Defect-Mediated Tunneling in Hexagonal Boron Nitride-Based Junctions.

PubMed

Chandni, U; Watanabe, K; Taniguchi, T; Eisenstein, J P

2015-11-11

We investigate electron tunneling through atomically thin layers of hexagonal boron nitride (hBN). Metal (Cr/Au) and semimetal (graphite) counter-electrodes are employed. While the direct tunneling resistance increases nearly exponentially with barrier thickness as expected, the thicker junctions also exhibit clear signatures of Coulomb blockade, including strong suppression of the tunnel current around zero bias and step-like features in the current at larger biases. The voltage separation of these steps suggests that single-electron charging of nanometer-scale defects in the hBN barrier layer are responsible for these signatures. We find that annealing the metal-hBN-metal junctions removes these defects and the Coulomb blockade signatures in the tunneling current.

Simple and rapid mercury ion selective electrode based on 1-undecanethiol assembled Au substrate and its recognition mechanism.

PubMed

Li, Xian-Qing; Liang, Hai-Qing; Cao, Zhong; Xiao, Qing; Xiao, Zhong-Liang; Song, Liu-Bin; Chen, Dan; Wang, Fu-Liang

2017-03-01

A simple and rapid mercury ion selective electrode based on 1-undecanethiol (1-UDT) assembled Au substrate (Au/1-UDT) has been well constructed. 1-UDT was for the purpose of generating self-assembled monolayer on gold surface to recognize Hg 2+ in aqueous solution, which had a working concentration range of 1.0×10 -8 -1.0×10 -4 molL -1 , with a Nernst response slope of 28.83±0.4mV/-pC, a detection limit of 4.5×10 -9 molL -1 , and a good selectivity over the other tested cations. Also, the Au/1-UDT possessed good reproducibility, stability, and short response time. The recovery obtained for the determination of mercury ion in practical tremella samples was in the range of 99.8-103.4%. Combined electrochemical analysis and X-ray photoelectron spectroscopy (XPS) with quantum chemical computation, the probable recognition mechanism of the electrode for selective recognition of Hg 2+ has been investigated. The covalent bond formed between mercury and sulfur is stronger than the one between gold and sulfur and thus prevents the adsorption of 1-UDT molecules on the gold surface. The quantum chemical computation with density functional theory further demonstrates that the strong interaction between the mercury atom and the sulfur atom on the gold surface leads to the gold sulfur bond ruptured and the gold mercury metallophilic interaction. Copyright © 2016 Elsevier B.V. All rights reserved.

Size-focusing synthesis of gold nanoclusters with p-mercaptobenzoic acid.

PubMed

Tvedte, Laura M; Ackerson, Christopher J

2014-09-18

Etching or size-focusing methods are now widespread for preparation of atomically monodisperse thiolate-protected gold nanoparticles. Size-focusing methods are not widespread, however, in the production of water-soluble gold nanoparticles. Reported here is a new method for size-focusing of large gold nanoparticles utilizing p-mercaptobenzoic acid. We observe preferential formation of three large gold nanoparticles with approximate masses of 23, 51, and 88 kDa. On the basis of the stability of these masses against further etching or growth, they appear to be especially stable sizes. These sizes are not prominent after etching challenges with organosoluble ligands, and the 51 and 88 kDa sizes appear to be novel stable thiolate-protected gold cluster sizes. The overall trend in particle size distribution over time is also unusual, with larger sizes dominating at longer time points.

Low energy implantation of boron with decaborane ions

NASA Astrophysics Data System (ADS)

Albano, Maria Angela

The goal of this dissertation was to determine the feasibility of a novel approach to forming ultra shallow p-type junctions (tens of nm) needed for future generations of Si MOS devices. In the new approach, B dopant atoms are implanted by cluster ions obtained by ionization of decaborane (B 10H14) vapor. An experimental ion implanter with an electron impact ion source and magnetic mass separation was built at the Ion Beam and Thin Film Research Laboratory at NJIT. Beams of B10Hx+ ions with currents of a few microamperes and energies of 1 to 12 keV were obtained and used for implantation experiments. Profiles of B and H atoms implanted in Si were measured by Secondary Ion Mass Spectroscopy (SIMS) before and after rapid thermal annealing (RTA). From the profiles, the junction depth of 57 nm (at 1018 cm-3 B concentration) was obtained with 12 keV decaborane ions followed by RTA. The dose of B atoms that can be implanted at low energy into Si is limited by sputtering as the ion beam sputters both the matrix and the implanted atoms. As the number of sputtered B atoms increases with the implanted dose and approaches the number of the implanted atoms, equilibrium of B in Si is established. This effect was investigated by comparison of the B dose calculated from the ion beam integration with B content in the sample measured by Nuclear Reaction Analysis (NRA). Maximum (equilibrium) doses of 1.35 x 1016 B cm -2 and 2.67 x 1016 B cm-2 were obtained at the beam energies of 5 and 12 keV, respectively. The problem of forming shallow p-type junctions in Si is related not only to implantation depth, but also to transient enhanced diffusion (TED). TED in Si implanted with B10Hx+ was measured on boron doping superlattice (B-DSL) marker layers. It was found that TED, following decaborane implantation, is the same as with monomer B+ ion implantation of equivalent energy and that it decreases with the decreasing ion energy. (Abstract shortened by UMI.)

An ab initio study on the effect of iron atom junction on transport characteristics of carbon-silicon mixed chain

NASA Astrophysics Data System (ADS)

Hu, Wei; Zhou, Qinghua; Liu, Wenhua; Liang, Yan; Wang, Tao; Wan, Haiqing

2018-04-01

The effect of iron atom junction on transport characteristics of carbon-silicon mixed chain has been studied from an ab initio study. At zero bias, the Fe(CSi)n system appears to be the decrease of the conductance as the number of the Si-C pairs in the chain increases (n changes). When n > 5, the conductance tends to zero. These changes are independent of the transferring charge of the system, depending on the coupling of the electrodes and the central region. Under bias, the higher the bias voltage, the bigger the transmission coefficient of the system, and the transmission peak moves closer to the Fermi level. The I-V curves of Fe(CSi)2 and Fe (CSi)3 are linear, showing the behavior of metal resistance.

Photo-Sensitivity of Large Area Physical Vapor Deposited Mono and Bilayer MoS2 (Postprint)

DTIC Science & Technology

2014-07-01

layer MoS2 without any apparent rectifying junctions , making device fabrication straightforward. For bi-layers, no such effect was present, suggesting...layer MoS2 without any apparent rectifying junctions , making device fabrication straightforward. For bi-layers, no such effect was present, suggesting...pressure below 5×10−9 Torr for atomically sharp and clean interfaces. The mono and bi-layer specimens were grown on 100 nm thick thermal oxide coated silicon

Structural analysis of jewelry from the Moche tomb of the `lady of Cao' by X-ray digital radiography

NASA Astrophysics Data System (ADS)

Azeredo, S. R.; Cesareo, R.; Franco, R.; Fernandez, A.; Bustamante, A.; Lopes, R. T.

2018-04-01

Nose ornaments from the tomb of the `Lady of Cao', a mummified woman representative of the Moche culture and dated to the third-or-fourth century AD, were analyzed by X-ray digital radiography. These spectacular gold and silver jewels are some of the most sophisticated metalworking ever produced in ancient America. The Mochecivilization flourished along the north coast of present-day Peru, between the Andes and the Pacific Ocean, approximately between 100 and 600 AD. The Moche were very sophisticated artisans and metal smiths, being considered the finest producers of jewels and artifacts of the region. A portable X-ray digital radiography (XDR) system consisting of a flat panel detector with high resolution image and a mini X-ray tube was used for the structural analysis of the Moche jewels aiming at inferring different joining methods of the silver-gold sheets. The radiographic analysis showed some differences in the joint of the silver-and-gold sheets. Presence of filler material and adhesive for joining the silver-and-gold sheets was visible as well as silver-gold junctions without filler material (or with a material invisible in radiography). Furthermore, the technique demonstrated the advantage of using a portable XDR micro system when the sample cannot be brought to the laboratory.

MCNP6.1 simulations for low-energy atomic relaxation: Code-to-code comparison with GATEv7.2, PENELOPE2014, and EGSnrc

NASA Astrophysics Data System (ADS)

Jung, Seongmoon; Sung, Wonmo; Lee, Jaegi; Ye, Sung-Joon

2018-01-01

Emerging radiological applications of gold nanoparticles demand low-energy electron/photon transport calculations including details of an atomic relaxation process. Recently, MCNP® version 6.1 (MCNP6.1) has been released with extended cross-sections for low-energy electron/photon, subshell photoelectric cross-sections, and more detailed atomic relaxation data than the previous versions. With this new feature, the atomic relaxation process of MCNP6.1 has not been fully tested yet with its new physics library (eprdata12) that is based on the Evaluated Atomic Data Library (EADL). In this study, MCNP6.1 was compared with GATEv7.2, PENELOPE2014, and EGSnrc that have been often used to simulate low-energy atomic relaxation processes. The simulations were performed to acquire both photon and electron spectra produced by interactions of 15 keV electrons or photons with a 10-nm-thick gold nano-slab. The photon-induced fluorescence X-rays from MCNP6.1 fairly agreed with those from GATEv7.2 and PENELOPE2014, while the electron-induced fluorescence X-rays of the four codes showed more or less discrepancies. A coincidence was observed in the photon-induced Auger electrons simulated by MCNP6.1 and GATEv7.2. A recent release of MCNP6.1 with eprdata12 can be used to simulate the photon-induced atomic relaxation.

The anchoring effect on the spin transport properties and I-V characteristics of pentacene molecular devices suspended between nickel electrodes.

PubMed

Caliskan, S; Laref, A

2014-07-14

Spin-polarized transport properties are determined for pentacene sandwiched between Ni surface electrodes with various anchoring ligands. These calculations are carried out using spin density functional theory in tandem with a non-equilibrium Green's function technique. The presence of a Se atom at the edge of the pentacene molecule significantly modifies the transport properties of the device because Se has a different electronegativity than S. Our theoretical results clearly show a larger current for spin-up electrons than for spin-down electrons in the molecular junction that is attached asymmetrically across the Se linker at one side of the Ni electrodes (in an APL magnetic orientation). Moreover, this molecular junction exhibits pronounced NDR as the bias voltage is increased from 0.8 to 1.0 V. However, this novel NDR behavior is only detected in this promising pentacene molecular device. The NDR in the current-voltage (I-V) curve results from the narrowness of the density of states for the molecular states. The feasibility of controlling the TMR is also predicted in these molecular device nanostructures. Spin-dependent transmission calculations show that the sign and strength of the current-bias voltage characteristics and the TMR could be tailored for the organic molecule devices. These molecular junctions are joined symmetrically and asymmetrically between Ni metallic probes across the S and Se atoms (at the ends of the edges of the pentacene molecule). Our theoretical findings show that spin-valve phenomena can occur in these prototypical molecular junctions. The TMR and NDR results show that nanoscale junctions with spin valves could play a vital role in the production of novel functional molecular devices.

Effect of mechanical and electrical stimuli in conductive atomic force microscopy with noble metal-coated tips

NASA Astrophysics Data System (ADS)

Zade, Vishal; Kang, Hung-Sen; Lee, Min Hwan

2018-01-01

Conductive atomic force microscopy has been widely employed to study the localized electrical properties of a wide range of substrates in non-vacuum conditions by the use of noble metal-coated tips. However, quantitative characterization of the electrical properties was often precluded by unpredictable changes in the tip apex morphology, and/or electronic transport characteristics of undesired oxide overcoats on the tip. In this paper, the impact of mechanical and electrical stimuli on the apex geometry of gold coated tips and electrical conduction properties at the tip-substrate contact is discussed by choosing gold and highly ordered pyrolytic graphite as the representative tip and substrate materials, respectively.

Two-dimensional dopant profiling of gallium nitride p-n junctions by scanning capacitance microscopy

NASA Astrophysics Data System (ADS)

Lamhamdi, M.; Cayrel, F.; Frayssinet, E.; Bazin, A. E.; Yvon, A.; Collard, E.; Cordier, Y.; Alquier, D.

2016-04-01

Two-dimensional imaging of dopant profiles for n and p-type regions are relevant for the development of new power semiconductors, especially for gallium nitride (GaN) for which classical profiling techniques are not adapted. This is a challenging task since it needs a technique with simultaneously good sensitivity, high spatial resolution and high dopant gradient resolution. To face these challenges, scanning capacitance microscopy combined with Atomic Force Microscopy is a good candidate, presenting reproducible results, as demonstrated in literature. In this work, we attempt to distinguish reliably and qualitatively the various doping concentrations and type at p-n and unipolar junctions. For both p-n and unipolar junctions three kinds of samples were prepared and measured separately. The space-charge region of the p-n metallurgical junction, giving rise to different contrasts under SCM imaging, is clearly observed, enlightening the interest of the SCM technique.

New Nanomedicine Approaches Using Gold-thioguanine Nanoconjugates as Metallo-ligands

PubMed Central

Sleightholm, Lee; Zambre, Ajit; Chanda, Nripen; Afrasiabi, Zahra; Katti, Kattesh; Kannan, Raghuraman

2011-01-01

Gold-thioguanine nanoconjugates (AuNP-TG) of size 3–4 nm were synthesized and the ratio between gold and 6-Thioguanine (TG) was estimated as ~1:1.5 using a cyanide digestion method and confirmed by flame atomic absorption spectroscopic analysis. AuNP-TG constructs showed high in vitro stability under different pH conditions and biologically relevant solutions for a period of 24 hours. Reaction of AuNP-TG with europium or platinum salts resulted in the formation of organized self-assembled metallo-networks. PMID:21709763

Compilation of Atomic and Molecular Data Relevant to Gas Lasers. Volume VII.

DTIC Science & Technology

1980-12-01

Schaefer and A. E. Orel, "Potential Energy Curves for Diatomic Zinc and Codmium", J. Chem. Phys. 71, 1122 (1979). 19. M. F. Golde and A. Kuaran...34Chemiluminescence of Argon Bromide. I. The Emission Spectrum of ArBr", J. Chem. Phys. 72, 434 (1980). 20. M. F. Golde and K. Kuaran, "Chemiluminescence of...72, 2469 (1980). (A-4.6 - A-4.17). 3. M. F. Golde and A. Kvaran, "Chemiluminescence of Argon Bromide. I. The Emission Spectrum of Ar Br", J. Chem

Gate-dependent asymmetric transport characteristics in pentacene barristors with graphene electrodes.

PubMed

Hwang, Wang-Taek; Min, Misook; Jeong, Hyunhak; Kim, Dongku; Jang, Jingon; Yoo, Daekyung; Jang, Yeonsik; Kim, Jun-Woo; Yoon, Jiyoung; Chung, Seungjun; Yi, Gyu-Chul; Lee, Hyoyoung; Wang, Gunuk; Lee, Takhee

2016-11-25

We investigated the electrical characteristics and the charge transport mechanism of pentacene vertical hetero-structures with graphene electrodes. The devices are composed of vertical stacks of silicon, silicon dioxide, graphene, pentacene, and gold. These vertical heterojunctions exhibited distinct transport characteristics depending on the applied bias direction, which originates from different electrode contacts (graphene and gold contacts) to the pentacene layer. These asymmetric contacts cause a current rectification and current modulation induced by the gate field-dependent bias direction. We observed a change in the charge injection barrier during variable-temperature current-voltage characterization, and we also observed that two distinct charge transport channels (thermionic emission and Poole-Frenkel effect) worked in the junctions, which was dependent on the bias magnitude.

Photon calorimeter

DOEpatents

Chow, Tze-Show

1988-04-22

A photon calorimeter is provided that comprises a laminar substrate that is uniform in density and homogeneous in atomic composition. A plasma-sprayed coating, that is generally uniform in density and homogeneous in atomic composition within the proximity of planes that are parallel to the surfaces of the substrate, is applied to either one or both sides of the laminar substrate. The plasma-sprayed coatings may be very efficiently spectrally tailored in atomic number. Thermocouple measuring junctions, are positioned within the plasma-sprayed coatings. The calorimeter is rugged, inexpensive, and equilibrates in temperature very rapidly. 4 figs.

X-ray absorption spectroscopic studies on gold nanoparticles in mesoporous and microporous materials.

PubMed

Akolekar, Deepak B; Foran, Garry; Bhargava, Suresh K

2004-05-01

Au L(3)-edge X-ray absorption spectroscopic measurements were carried out over a series of mesoporous and microporous materials containing gold nanoparticles to investigate the effects of the host matrix and preparation methods on the properties of gold nanoparticles. The materials of structure type MCM-41, ZSM-5, SAPO-18 and LSX with varying framework composition containing low concentrations of gold nanoparticles were prepared and characterized. In these materials the size of the gold nanoparticles varied in the range approximately 1 to 4 nm. A series of gold nanoparticles within different mesoporous and microporous materials have been investigated using X-ray absorption fine structure (XANES, EXAFS) and other techniques. Information such as atomic distances, bonding and neighbouring environment obtained from XAFS measurements was useful in elucidating the nature and structure of gold nanoparticles on these catalytic materials. The influence of the high-temperature (823, 1113, 1273 K) treatment on gold nanoparticles inside the mesoporous matrix was investigated using the XAFS technique. The XAFS and XANES results confirm various characteristics of gold nanoparticles in these materials suitable for catalysis, fabrication of nanodevices and other applications.

Atomistic simulations of highly conductive molecular transport junctions under realistic conditions

NASA Astrophysics Data System (ADS)

French, William R.; Iacovella, Christopher R.; Rungger, Ivan; Souza, Amaury Melo; Sanvito, Stefano; Cummings, Peter T.

2013-04-01

We report state-of-the-art atomistic simulations combined with high-fidelity conductance calculations to probe structure-conductance relationships in Au-benzenedithiolate (BDT)-Au junctions under elongation. Our results demonstrate that large increases in conductance are associated with the formation of monatomic chains (MACs) of Au atoms directly connected to BDT. An analysis of the electronic structure of the simulated junctions reveals that enhancement in the s-like states in Au MACs causes the increases in conductance. Other structures also result in increased conductance but are too short-lived to be detected in experiment, while MACs remain stable for long simulation times. Examinations of thermally evolved junctions with and without MACs show negligible overlap between conductance histograms, indicating that the increase in conductance is related to this unique structural change and not thermal fluctuation. These results, which provide an excellent explanation for a recently observed anomalous experimental result [Bruot et al., Nat. Nanotechnol., 2012, 7, 35-40], should aid in the development of mechanically responsive molecular electronic devices.We report state-of-the-art atomistic simulations combined with high-fidelity conductance calculations to probe structure-conductance relationships in Au-benzenedithiolate (BDT)-Au junctions under elongation. Our results demonstrate that large increases in conductance are associated with the formation of monatomic chains (MACs) of Au atoms directly connected to BDT. An analysis of the electronic structure of the simulated junctions reveals that enhancement in the s-like states in Au MACs causes the increases in conductance. Other structures also result in increased conductance but are too short-lived to be detected in experiment, while MACs remain stable for long simulation times. Examinations of thermally evolved junctions with and without MACs show negligible overlap between conductance histograms, indicating that the increase in conductance is related to this unique structural change and not thermal fluctuation. These results, which provide an excellent explanation for a recently observed anomalous experimental result [Bruot et al., Nat. Nanotechnol., 2012, 7, 35-40], should aid in the development of mechanically responsive molecular electronic devices. Electronic supplementary information (ESI) available. See DOI: 10.1039/c3nr00459g

Metastability of the atomic structures of size-selected gold nanoparticles

NASA Astrophysics Data System (ADS)

Wells, Dawn M.; Rossi, Giulia; Ferrando, Riccardo; Palmer, Richard E.

2015-04-01

All nanostructures are metastable - but some are more metastable than others. Here we employ aberration-corrected electron microscopy and atomistic computer simulations to demonstrate the hierarchy of metastability in deposited, size-selected gold nanoparticles (clusters), an archetypal class of nanomaterials well known for the catalytic activity which only appears on the nanometer-scale. We show that the atomic structures presented by ``magic number'' Au561, Au742 and Au923 clusters are ``locked''. They are in fact determined by the solidification which occurs from the liquid state early in their growth (by assembly from atoms in the gas phase) followed by template growth. It is quite likely that transitions from a locked, metastable configuration to a more stable (but still metastable) structure, as observed here under the electron beam, will occur during catalytic reactions, for example.All nanostructures are metastable - but some are more metastable than others. Here we employ aberration-corrected electron microscopy and atomistic computer simulations to demonstrate the hierarchy of metastability in deposited, size-selected gold nanoparticles (clusters), an archetypal class of nanomaterials well known for the catalytic activity which only appears on the nanometer-scale. We show that the atomic structures presented by ``magic number'' Au561, Au742 and Au923 clusters are ``locked''. They are in fact determined by the solidification which occurs from the liquid state early in their growth (by assembly from atoms in the gas phase) followed by template growth. It is quite likely that transitions from a locked, metastable configuration to a more stable (but still metastable) structure, as observed here under the electron beam, will occur during catalytic reactions, for example. Electronic supplementary information (ESI) available. See DOI: 10.1039/c4nr05811a

Orthogonal chemical functionalization of patterned gold on silica surfaces

PubMed Central

Léonard, Didier; Le Mogne, Thierry; Zuttion, Francesca; Chevalier, Céline; Phaner-Goutorbe, Magali; Souteyrand, Éliane

2015-01-01

Summary Single-step orthogonal chemical functionalization procedures have been developed with patterned gold on silica surfaces. Different combinations of a silane and a thiol were simultaneously deposited on a gold/silica heterogeneous substrate. The orthogonality of the functionalization (i.e., selective grafting of the thiol on the gold areas and the silane on the silica) was demonstrated by X-ray photoelectron spectroscopy (XPS) as well as time-of-flight secondary ion mass spectrometry (ToF–SIMS) mapping. The orthogonal functionalization was used to immobilize proteins onto gold nanostructures on a silica substrate, as demonstrated by atomic force microscopy (AFM). These results are especially promising in the development of future biosensors where the selective anchoring of target molecules onto nanostructured transducers (e.g., nanoplasmonic biosensors) is a major challenge. PMID:26734519

Why can a gold salt react as a base?

PubMed

Anania, Mariarosa; Jašíková, Lucie; Jašík, Juraj; Roithová, Jana

2017-09-26

This study shows that gold salts [(L)AuX] (L = PMe 3 , PPh 3 , JohnPhos, IPr; X = SbF 6 , PF 6 , BF 4 , TfO, Tf 2 N) act as bases in aqueous solutions and can transform acetone to digold acetonyl complexes [(L) 2 Au 2 (CH 2 COCH 3 )] + without any additional base present in solution. The key step is the formation of digold hydroxide complexes [(L) 2 Au 2 (OH)] + . The kinetics of the formation of the digold complexes and their mutual transformation is studied by electrospray ionization mass spectrometry and the delayed reactant labelling method. We show that the formation of digold hydroxide is the essential first step towards the formation of the digold acetonyl complex, the reaction is favoured by more polar solvents, and the effect of counter ions is negligible. DFT calculations suggest that digold hydroxide and digold acetonyl complexes can exist in solution only due to the stabilization by the interaction with two gold atoms. The reaction between the digold hydroxide and acetone proceeds towards the dimer {[(L)Au(OH)]·[(L)Au(CH 3 COCH 3 )] + }. The monomeric units interact at the gold atoms in the perpendicular arrangement typical of the gold clusters bound by the aurophilic interaction. The hydrogen is transferred within the dimer and the reaction continues towards the digold acetonyl complex and water.

Energetic stabilities of thiolated pyrimidines on gold nanoparticles investigated by Raman spectroscopy and density functional theory calculations.

PubMed

Ganbold, Erdene-Ochir; Yoon, Jinha; Cho, Kwang-Hwi; Joo, Sang-Woo

2015-01-01

The adsorption structures of 2-thiocytosine (2TC) on gold surfaces were examined by means of vibrational Raman spectroscopy and quantum mechanical density functional theory calculations. The 1H-thione-amino form was calculated to be most stable among the six examined tautomers. The three plausible binding geometries of sulfur, pyrimidine nitrogen, and amino group binding modes were calculated to estimate the binding energies of the 1H-thione-amino form with six gold cluster atoms. Thiouracils including 2-thiouracil (2TU), 4-thiouracil (4TU), and 6-methyl-2-thiouracil (6M2TU) were also studied to compare their relative binding energies on gold atoms. The intracellular localization of a DNA base analog of 2TC on gold nanoparticles (AuNPs) in HeLa cells was identified by means of surface-enhanced Raman scattering. AuNPs were modified with 2TC by self-assembly. Our dark-field microscopy and z-depth-dependent confocal Raman spectroscopy indicated that 2TC-assembled AuNPs could be found inside cancer cells. On the other hand, we did not observe noticeably strong Raman peaks in the cases of thiouracils including 2TU, 4TU, and 6M2TU. This may be due to the additional amino group of 2TC, which can lead to a stronger binding of adsorbates on AuNPs. Copyright © 2015. Published by Elsevier B.V.

Plastic Schottky-barrier solar cells

DOEpatents

Waldrop, J.R.; Cohen, M.J.

1981-12-30

A photovoltaic cell structure is fabricated from an active medium including an undoped polyacetylene, organic semiconductor. When a film of such material is in rectifying contact with a metallic area electrode, a Schottky-barrier junction is obtained within the body of the cell structure. Also, a gold overlayer passivates a magnesium layer on the undoped polyacetylene film. With the proper selection and location of elements a photovoltaic cell structure and solar cell are obtained.

Nano-fabrication of molecular electronic junctions by targeted modification of metal-molecule bonds

NASA Astrophysics Data System (ADS)

Jafri, S. Hassan M.; Löfås, Henrik; Blom, Tobias; Wallner, Andreas; Grigoriev, Anton; Ahuja, Rajeev; Ottosson, Henrik; Leifer, Klaus

2015-09-01

Reproducibility, stability and the coupling between electrical and molecular properties are central challenges in the field of molecular electronics. The field not only needs devices that fulfill these criteria but they also need to be up-scalable to application size. In this work, few-molecule based electronics devices with reproducible electrical characteristics are demonstrated. Our previously reported 5 nm gold nanoparticles (AuNP) coated with ω-triphenylmethyl (trityl) protected 1,8-octanedithiol molecules are trapped in between sub-20 nm gap spacing gold nanoelectrodes forming AuNP-molecule network. When the trityl groups are removed, reproducible devices and stable Au-thiol junctions are established on both ends of the alkane segment. The resistance of more than 50 devices is reduced by orders of magnitude as well as a reduction of the spread in the resistance histogram is observed. By density functional theory calculations the orders of magnitude decrease in resistance can be explained and supported by TEM observations thus indicating that the resistance changes and strongly improved resistance spread are related to the establishment of reproducible and stable metal-molecule bonds. The same experimental sequence is carried out using 1,6-hexanedithiol functionalized AuNPs. The average resistances as a function of molecular length, demonstrated herein, are comparable to the one found in single molecule devices.

A novel colorimetric aptasensor for ultrasensitive detection of cocaine based on the formation of three-way junction pockets on the surfaces of gold nanoparticles.

PubMed

Abnous, Khalil; Danesh, Noor Mohammad; Ramezani, Mohammad; Taghdisi, Seyed Mohammad; Emrani, Ahmad Sarreshtehdar

2018-08-22

Herein, a novel colorimetric aptasensor was introduced for detection of cocaine based on the formation of three-way junction pockets on the surfaces of gold nanoparticles (AuNPs) and the catalytic activity of the surfaces of AuNPs. Simplicity and detection of cocaine in a short time (only 35 min) are some of the unique features of the proposed sensing strategy. In the presence of cocaine, triple-fragment aptamer (TFA) forms on the surfaces of AuNPs, leading to a significant decrease of the catalytic activity of AuNPs and the color of samples remains yellow. In the absence of target, TFA does not form on the surfaces of AuNPs and 4-Nitrophenol, as a colorimetric agent, has more access to the surfaces of AuNPs, resulting in the reduction of 4-Nitrophenol and the color of sample changes from yellow to colorless. The sensing strategy showed good specificity, a limit of detection (LOD) of 440 pM and a dynamic range over 2-100 nM. The sensing method was also successfully applied to detect cocaine in spiked human serum samples with recovery of 94.71-98.63%. Copyright © 2018 Elsevier B.V. All rights reserved.

Increased cellular uptake of peptide-modified PEGylated gold nanoparticles.

PubMed

He, Bo; Yang, Dan; Qin, Mengmeng; Zhang, Yuan; He, Bing; Dai, Wenbing; Wang, Xueqing; Zhang, Qiang; Zhang, Hua; Yin, Changcheng

2017-12-09

Gold nanoparticles are promising drug delivery vehicles for nucleic acids, small molecules, and proteins, allowing various modifications on the particle surface. However, the instability and low bioavailability of gold nanoparticles compromise their clinical application. Here, we functionalized gold nanoparticles with CPP fragments (CALNNPFVYLI, CALRRRRRRRR) through sulfhydryl PEG to increase their stability and bioavailability. The resulting gold nanoparticles were characterized with transmission electron microscopy (TEM), dynamic light scattering (DLS), UV-visible spectrometry and X-ray photoelectron spectroscopy (XPS), and the stability in biological solutions was evaluated. Comparing to PEGylated gold nanoparticles, CPP (CALNNPFVYLI, CALRRRRRRRR)-modified gold nanoparticles showed 46 folds increase in cellular uptake in A549 and B16 cell lines, as evidenced by the inductively coupled plasma atomic emission spectroscopy (ICP-AES). The interactions between gold nanoparticles and liposomes indicated CPP-modified gold nanoparticles bind to cell membrane more effectively than PEGylated gold nanoparticles. Surface plasmon resonance (SPR) was used to measure interactions between nanoparticles and the membrane. TEM and uptake inhibitor experiments indicated that the cellular entry of gold nanoparticles was mediated by clathrin and macropinocytosis. Other energy independent endocytosis pathways were also identified. Our work revealed a new strategy to modify gold nanoparticles with CPP and illustrated the cellular uptake pathway of CPP-modified gold nanoparticles. Copyright © 2017 Elsevier Inc. All rights reserved.

Catalytically active Au-O(OH) x- species stabilized by alkali ions on zeolites and mesoporous oxides

DOE PAGES

Yang, Ming; Li, Sha; Wang, Yuan; ...

2014-11-27

Here we report that the addition of alkali ions (sodium or potassium) to gold on KLTL-zeolite and mesoporous MCM-41 silica stabilizes mononuclear gold in Au-O(OH) x-(Na or K) ensembles. This single-site gold species is active for the low-temperature (<200°C) water-gas shift (WGS) reaction. Unexpectedly, gold is thus similar to platinum in creating –O linkages with more than eight alkali ions and establishing an active site on various supports. The intrinsic activity of the single-site gold species is the same on irreducible supports as on reducible ceria, iron oxide, and titania supports, apparently all sharing a common, similarly structured gold activemore » site. This finding paves the way for using earth-abundant supports to disperse and stabilize precious metal atoms with alkali additives for the WGS and potentially other fuel-processing reactions.« less

Platinum Electrodeposition for Supported ALD Templated Foam Hohlraum Liners

DOE PAGES

Horwood, Corie; Stadermann, Michael; Biener, Monika; ...

2017-12-20

Two commercially available platinum plating solutions (Platanex III and Platanex Luna) were evaluated for the electrodeposition of platinum layers on gold hohlraums and cylindrically shaped silver-gold ingots. The successful deposition of thin Pt layers on gold hohlraums as well as thick Pt layers on silver-gold alloys will allow for the integration of atomic layer deposition templated foam inside a hohlraum. We found that when the manufacturer’s recommendations for the Pt plating solutions were used, the coatings obtained were unacceptable because of cracking, poor adhesion, or thin and powdery Pt deposits. Therefore, alternative plating parameters were investigated, and the conditions resultingmore » in acceptable coatings are reported here.« less

Platinum Electrodeposition for Supported ALD Templated Foam Hohlraum Liners

DOE Office of Scientific and Technical Information (OSTI.GOV)

Horwood, Corie; Stadermann, Michael; Biener, Monika

Two commercially available platinum plating solutions (Platanex III and Platanex Luna) were evaluated for the electrodeposition of platinum layers on gold hohlraums and cylindrically shaped silver-gold ingots. The successful deposition of thin Pt layers on gold hohlraums as well as thick Pt layers on silver-gold alloys will allow for the integration of atomic layer deposition templated foam inside a hohlraum. We found that when the manufacturer’s recommendations for the Pt plating solutions were used, the coatings obtained were unacceptable because of cracking, poor adhesion, or thin and powdery Pt deposits. Therefore, alternative plating parameters were investigated, and the conditions resultingmore » in acceptable coatings are reported here.« less

Ligand-free gold atom clusters adsorbed on graphene nano sheets generated by oxidative laser fragmentation in water

NASA Astrophysics Data System (ADS)

Lau, Marcus; Haxhiaj, Ina; Wagener, Philipp; Intartaglia, Romuald; Brandi, Fernando; Nakamura, Junji; Barcikowski, Stephan

2014-08-01

Over three decades after the first synthesis of stabilized Au55-clusters many scientific questions about gold cluster properties are still unsolved and ligand-free colloidal clusters are difficult to fabricate. Here we present a novel route to produce ultra-small gold particles by using a green technique, the laser ablation and fragmentation in water, without using reductive or stabilizing agents at any step of the synthesis. For fabrication only a pulsed laser, a gold-target, pure water, sodium hydroxide and hydrogen peroxide are deployed. The particles are exemplarily hybridized to graphene supports showing that these carbon-free colloidal clusters might serve as versatile building blocks.

Gold Nanoparticles Doped with (199) Au Atoms and Their Use for Targeted Cancer Imaging by SPECT.

PubMed

Zhao, Yongfeng; Pang, Bo; Luehmann, Hannah; Detering, Lisa; Yang, Xuan; Sultan, Deborah; Harpstrite, Scott; Sharma, Vijay; Cutler, Cathy S; Xia, Younan; Liu, Yongjian

2016-04-20

Gold nanoparticles have been labeled with various radionuclides and extensively explored for single photon emission computed tomography (SPECT) in the context of cancer diagnosis. The stability of most radiolabels, however, still needs to be improved for accurate detection of cancer biomarkers and thereby monitoring of tumor progression and metastasis. Here, the first synthesis of Au nanoparticles doped with (199)Au atoms for targeted SPECT tumor imaging in a mouse triple negative breast cancer (TNBC) model is reported. By directly incorporating (199)Au atoms into the crystal lattice of each Au nanoparticle, the stability of the radiolabel can be ensured. The synthetic procedure also allows for a precise control over both the radiochemistry and particle size. When conjugated with D-Ala1-peptide T-amide, the Au nanoparticles doped with (199)Au atoms can serve as a C-C chemokine receptor 5 (CCR5)-targeted nanoprobe for the sensitive and specific detection of both TNBC and its metastasis in a mouse tumor model. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Atomic Scattering Factor of the ASTRO-H (Hitomi) SXT Reflector Around the Gold's L Edges

NASA Technical Reports Server (NTRS)

Kikuchi, Naomichi; Kurashima, Sho; Ishida, Manabu; Iizuka, Ryo; Maeda, Yoshitomo; Hayashi, Takayuki; Okajima, Takashi; Matsumoto, Hironori; Mitsubishi, Ikuyuki; Saji, Shigetaka

2016-01-01

The atomic scattering factor in the energy range of 11.2 - 15.4 keV for the ASTRO-H Soft X-ray Telescope (SXT) is reported. The large effective area of the SXT makes use of photon spectra above 10 keV viable, unlike most other X-ray satellites with total-reflection mirror optics. Presence of gold's L-edges in the energy band is a major issue, as it complicates the function of the effective area. In order to model the area, the reflectivity measurements in the 11.2 - 15.4 keV band with the energy pitch of 0.4 - 0.7 eV were made in the synchrotron beam-line Spring-8 BL01B1. We obtained atomic scattering factors f1 and f2 by the curve fitting to the reflectivities of our witness sample. The edges associated with the L-I, II, and III transitions are identified, of which the depths are found to be roughly 60 shallower than those expected from the Henkes atomic scattering factor.

Atomistic theory for the damping of vibrational modes in monoatomic gold chains

NASA Astrophysics Data System (ADS)

Engelund, M.; Brandbyge, M.; Jauho, A. P.

2009-07-01

We develop a computational method for evaluating the damping of vibrational modes in monatomic metallic chains suspended between bulk crystals under external strain. The damping is due to the coupling between the chain and contact modes and the phonons in the bulk substrates. The geometry of the atoms forming the contact is taken into account. The dynamical matrix is computed with density-functional theory in the atomic chain and the contacts using finite atomic displacements while an empirical method is employed for the bulk substrate. As a specific example, we present results for the experimentally realized case of gold chains in two different crystallographic directions. The range of the computed damping rates confirms the estimates obtained by fits to experimental data [T. Frederiksen , Phys. Rev. B 75, 205413 (2007)]. Our method indicates that an order-of-magnitude variation in the harmonic damping is possible even for relatively small changes in the strain. Such detailed insight is necessary for a quantitative analysis of damping in metallic atomic chains and in explaining the rich phenomenology seen in the experiments.

Synthesis and characterization of core-shell gold nanoparticles with poly(vinyl pyrrolidone) from a new precursor salt

NASA Astrophysics Data System (ADS)

Behera, M.; Ram, S.

2013-02-01

In this article, we report a facile one-step chemical synthesis of gold (Au) nanoparticles (GNPs) from a new precursor salt i.e., gold hydroxide in the presence of poly(vinyl pyrrolidone) (PVP) polymer. The non-aqueous dispersion of GNPs was comprehensively characterized by UV-Visible, FTIR, zeta potential, and transmission electron microscope (TEM). A strong surface plasmon resonance band at 529 nm in the UV-Visible spectrum confirms the formation of GNPs in the Au colloid. The FTIR spectroscopic results showed that PVP molecules get chemisorbed onto the surface of GNP via O-atom of carbonyl group. A negative zeta potential of (-)16 mV reveals accumulation of nonbonding electrons of O-atom of carbonyl group of PVP molecules on the nanosurface of GNP. TEM images demonstrate a core-shell nanostructure with an Au-crystalline core covered by a thin amorphous PVP-shell. PVP-capped GNPs could be a potential candidate for bio-sensing, catalysis, and other applications.

Terasonic Excitations in 2D Gold Nanoparticle Arrays in a Water Matrix as Revealed by Atomistic Simulations

DOE PAGES

Bolmatov, Dima; Zhernenkov, Mikhail; Zav’yalov, Dmitry; ...

2016-08-19

Here in this work we report on terahertz phononic excitations in 2D gold nanoparticle arrays in a water matrix through a series of large-scale molecular dynamics simulations. For the first time, we observe acoustic Dirac-like crossings in H (H 2O) atomic (molecular) networks which emerge due to an intraband phononic scattering. These crossings are the phononic fingerprints of ice-like arrangements of H (H 2O) atomic (molecular) networks at nanometer scale. We reveal how phononic excitations in metallic nanoparticles and the water matrix reciprocally impact on one another providing the mechanism for the THz phononics manipulation via structural engineering. In addition,more » we show that by tuning the arrangement of 2D gold nanoparticle assemblies the Au phononic polarizations experience sub-terahertz hybridization (Kohn anomaly) due to surface electron-phonon relaxation processes. This opens the way for the sound control and manipulation in soft matter metamaterials at nanoscale.« less

Formation of self-assembled monolayer of curcuminoid molecules on gold surfaces

NASA Astrophysics Data System (ADS)

Berlanga, Isadora; Etcheverry-Berríos, Álvaro; Mella, Andy; Jullian, Domingo; Gómez, Victoria Alejandra; Aliaga-Alcalde, Núria; Fuenzalida, Victor; Flores, Marcos; Soler, Monica

2017-01-01

We investigated the formation of self-assembled monolayers of two thiophene curcuminoid molecules, 2-thphCCM (1) and 3-thphCCM (2), on polycrystalline gold substrates prepared by immersion of the surfaces in a solution of the molecules during 24 h. The functionalized surfaces were studied by scanning tunneling microscopy (STM) and X-ray photoelectron spectroscopy (XPS). Despite the fact that both molecules have the same composition and almost the same structure, these molecules exhibit different behavior on the gold surface, which can be explained by the different positions of the sulfur atoms in the terminal aromatic rings. In the case of molecule 1, the complete formation of a SAM can be observed after 24 h of immersion. In the case of molecule 2, the transition from flat-lying to upright configuration on the surface is still in process after 24 h of immersion. This is attributed to the fact that molecule 2 have the sulfur atoms more exposed than molecule 1.

Computational Study of Quasi-2D Liquid State in Free Standing Platinum, Silver, Gold, and Copper Monolayers.

PubMed

Yang, Li-Ming; Ganz, Ariel B; Dornfeld, Matthew; Ganz, Eric

2016-12-01

Recently, freestanding atomically thick Fe metal patches up to 10 atoms wide have been fabricated experimentally in tiny pores in graphene. This concept can be extended conceptually to extended freestanding monolayers. We have therefore performed ab initio molecular dynamics simulations to evaluate the early melting stages of platinum, silver, gold, and copper freestanding metal monolayers. Our calculations show that all four freestanding monolayers will form quasi-2D liquid layers with significant out-of-plane motion and diffusion in the plane. Remarkably, we observe a 4% reduction in the Pt most likely bond length as the system enters the liquid state at 2400 K (and a lower effective spring constant), compared to the system at 1200 and 1800 K. We attribute this to the reduced average number of bonds per atom in the Pt liquid state. We used the highly accurate and reliable Density Functional Theory (DFT-D) method that includes dispersion corrections. These liquid states are found at temperatures of 2400 K, 1050 K, 1600 K, and 1400 K for platinum, silver, gold, and copper respectively. The pair correlation function drops in the liquid state, while the bond orientation order parameter is reduced to a lesser degree. Movies of the simulations can be viewed online (see Supplementary Material).

Synthesis, crystal structures, and characterization of double complex salts [Au(en)2][Rh(NO2)6]·2H2O and [Au(en)2][Rh(NO2)6

NASA Astrophysics Data System (ADS)

Plyusnin, Pavel E.; Makotchenko, Evgenia V.; Shubin, Yury V.; Baidina, Iraida A.; Korolkov, Ilya V.; Sheludyakova, Liliya A.; Korenev, Sergey V.

2015-11-01

Double complex salts of rhodium(III) and gold(III) of the composition [Au(en)2][Rh(NO2)6]·2H2O (1) and [Au(en)2][Rh(NO2)6] (2) have been prepared. Crystal structures of the compounds have been determined by single crystal X-ray diffraction. The compounds have been characterized by PXRD, IR, far-IR, CHN and DTA. The complexes have a layered structures. The presence of water in 1 makes the structure of the hydrated DCS less dense as compared to the anhydrous one. The environment of the cation and the anion in the two structures is the same, oxygen atoms of the nitro groups are involved in hydrogen bonds N-H⋯O, N⋯O distances being approximately the same. The structures of 1 and 2 are notable in having shortened contacts between the gold atoms and the oxygen atoms of the nitro groups of the neighboring complex anions. The thermal behavior of the complexes in a hydrogen atmosphere was investigated. The final product of thermolysis prepared at the temperature 600°C is a two-phase mixture of pure metallic gold and the solid solution Rh0.93Au0.07.

Evaluation of the memory effect on gold-coated silica adsorption tubes used for the analysis of gaseous mercury by cold vapor atomic absorption spectrometry.

PubMed

Rahman, Mohammad Mahmudur; Brown, Richard J C; Kim, Ki-Hyun; Yoon, Hye-On; Phan, Nhu-Thuc

2013-01-01

In an effort to reduce the experimental bias involved in the analysis of gaseous elemental mercury (Hg(o)), the blank response from gold-coated adsorption tubes has been investigated using cold vapor atomic absorption spectrometry (CVAAS). Our study has been compared with our recent investigation on memory effect in a cold vapour atomic fluorescence spectrometry (CVAFS). The pattern of blank responses was quantified after loading different amounts of mercury and after different time intervals of 1, 14, and 45 days. In case of the one day interval, the result of five to six instant blank heating cycles confirmed successful liberation of mercury following the second and third blank heating cycles. The results of 14 or 45 days generally suggest that liberation of excess mercury is affected by both the initial loading amount and the length of storage time prior to analysis. We have demonstrated a possibly effective way to reduce memory effects. Some similarities of these results with those from CVAFS experiment suggests that the blank response is caused by a combination of mercury absorbed within the bulk gold and micro- and nanoparticles liberated during heating and not from coabsorbing interfering gaseous species.

Evaluation of the Memory Effect on Gold-Coated Silica Adsorption Tubes Used for the Analysis of Gaseous Mercury by Cold Vapor Atomic Absorption Spectrometry

PubMed Central

Rahman, Mohammad Mahmudur; Brown, Richard J. C.; Yoon, Hye-On; Phan, Nhu-Thuc

2013-01-01

In an effort to reduce the experimental bias involved in the analysis of gaseous elemental mercury (Hgo), the blank response from gold-coated adsorption tubes has been investigated using cold vapor atomic absorption spectrometry (CVAAS). Our study has been compared with our recent investigation on memory effect in a cold vapour atomic fluorescence spectrometry (CVAFS). The pattern of blank responses was quantified after loading different amounts of mercury and after different time intervals of 1, 14, and 45 days. In case of the one day interval, the result of five to six instant blank heating cycles confirmed successful liberation of mercury following the second and third blank heating cycles. The results of 14 or 45 days generally suggest that liberation of excess mercury is affected by both the initial loading amount and the length of storage time prior to analysis. We have demonstrated a possibly effective way to reduce memory effects. Some similarities of these results with those from CVAFS experiment suggests that the blank response is caused by a combination of mercury absorbed within the bulk gold and micro- and nanoparticles liberated during heating and not from coabsorbing interfering gaseous species. PMID:23589708

Structural superlubricity of platinum on graphite under ambient conditions: The effects of chemistry and geometry

NASA Astrophysics Data System (ADS)

Özoǧul, Alper; Ipek, Semran; Durgun, Engin; Baykara, Mehmet Z.

2017-11-01

An investigation of the frictional behavior of platinum nanoparticles laterally manipulated on graphite has been conducted to answer the question of whether the recent observation of structural superlubricity under ambient conditions [E. Cihan, S. İpek, E. Durgun, and M. Z. Baykara, Nat. Commun. 7, 12055 (2016)] is exclusively limited to the gold-graphite interface. Platinum nanoparticles have been prepared by e-beam evaporation of a thin film of platinum on graphite, followed by post-deposition annealing. Morphological and structural characterization of the nanoparticles has been performed via scanning electron microscopy and transmission electron microscopy, revealing a crystalline structure with no evidence of oxidation under ambient conditions. Lateral manipulation experiments have been performed via atomic force microscopy under ambient conditions, whereby results indicate the occurrence of structural superlubricity at mesoscopic interfaces of 4000-75 000 nm2, with a noticeably higher magnitude of friction forces when compared with gold nanoparticles of similar contact areas situated on graphite. Ab initio simulations of sliding involving platinum and gold slabs on graphite confirm the experimental observations, whereby the higher magnitude of friction forces is attributed to stronger energy barriers encountered by platinum atoms sliding on graphite, when compared with gold. On the other hand, as predicted by theory, the scaling power between friction force and contact size is found to be independent of the chemical identity of the sliding atoms, but to be determined by the geometric qualities of the interface, as characterized by an average "sharpness score" assigned to the nanoparticles.

Submicron nickel-oxide-gold tunnel diode detectors for rectennas

NASA Technical Reports Server (NTRS)

Hoofring, A. B.; Kapoor, V. J.; Krawczonek, W.

1989-01-01

The characteristics of a metal-oxide-metal (MOM) tunnel diode made of nickel, nickel-oxide, and gold, designed and fabricated by standard integrated circuit technology for use in FIR rectennas, are presented. The MOM tunnel diode was formed by overlapping a 0.8-micron-wide layer of 1000-A of nickel, which was oxidized to form a thin layer of nickel oxide, with a 1500 A-thick layer of gold. The dc current-voltage characteristics of the MOM diode showed that the current dependence on voltage was linear about zero bias up to a bias of about 70 mV. The maximum detection of a low-level signal (10-mV ac) was determined to be at a dc voltage of 70 mV across the MOM diode. The rectified output signal due to a chopped 10.6-micron CO2 laser incident upon the rectenna device was found to increase with dc bias, with a maximum value of 1000 nV for a junction bias of 100 mV at room temperature.

Energy dependence of the trapping of uranium atoms by aluminum oxide surfaces

NASA Technical Reports Server (NTRS)

Librecht, K. G.

1979-01-01

The energy dependence of the trapping probability for sputtered U-235 atoms striking an oxidized aluminum collector surface at energies between 1 eV and 184 eV was measured. At the lowest energies, approximately 10% of the uranium atoms are not trapped, while above 10 eV essentially all of them stick. Trapping probabilities averaged over the sputtered energy distribution for uranium incident on gold and mica are also presented.

Thin Metallic Films From Solvated Metal Atoms

NASA Astrophysics Data System (ADS)

Trivino, Galo C.; Klabunde, Kenneth J.; Dale, Brock

1988-02-01

Metals were evaporated under vacuum and the metal atoms solvated by excess organic solvents at low temperature. Upon warming stable colloidal metal particles were formed by controlled metal atom clustering. The particles were stabilized toward flocculation by solvation and electrostatic effects. Upon solvent removal the colloidal particles grew to form thin films that were metallic in appearance, but showed higher resistivities than pure metallic films. Gold, palladium, platinium, and especially indium are discussed.

Tunneling rates in electron transport through double-barrier molecular junctions in a scanning tunneling microscope

PubMed Central

Nazin, G. V.; Wu, S. W.; Ho, W.

2005-01-01

The scanning tunneling microscope enables atomic-scale measurements of electron transport through individual molecules. Copper phthalocyanine and magnesium porphine molecules adsorbed on a thin oxide film grown on the NiAl(110) surface were probed. The single-molecule junctions contained two tunneling barriers, vacuum gap, and oxide film. Differential conductance spectroscopy shows that electron transport occurs via vibronic states of the molecules. The intensity of spectral peaks corresponding to the individual vibronic states depends on the relative electron tunneling rates through the two barriers of the junction, as found by varying the vacuum gap tunneling rate by changing the height of the scanning tunneling microscope tip above the molecule. A simple, sequential tunneling model explains the observed trends. PMID:15956189

Tunneling rates in electron transport through double-barrier molecular junctions in a scanning tunneling microscope.

PubMed

Nazin, G V; Wu, S W; Ho, W

2005-06-21

The scanning tunneling microscope enables atomic-scale measurements of electron transport through individual molecules. Copper phthalocyanine and magnesium porphine molecules adsorbed on a thin oxide film grown on the NiAl(110) surface were probed. The single-molecule junctions contained two tunneling barriers, vacuum gap, and oxide film. Differential conductance spectroscopy shows that electron transport occurs via vibronic states of the molecules. The intensity of spectral peaks corresponding to the individual vibronic states depends on the relative electron tunneling rates through the two barriers of the junction, as found by varying the vacuum gap tunneling rate by changing the height of the scanning tunneling microscope tip above the molecule. A simple, sequential tunneling model explains the observed trends.

Structure–function relationships in single molecule rectification by N-phenylbenzamide derivatives

DOE PAGES

Koenigsmann, Christopher; Ding, Wendu; Koepf, Matthieu; ...

2016-06-30

Here, we examine structure–function relationships in a series of N-phenylbenzamide (NPBA) derivatives by using computational modeling to identify molecular structures that exhibit both rectification and good conductance together with experimental studies of bias-dependent single molecule conductance and rectification behavior using the scanning tunneling microscopy break-junction technique. From a large number of computationally screened molecular diode structures, we have identified NPBA as a promising candidate, relative to the other structures that were screened. We demonstrate experimentally that conductance and rectification are both enhanced by functionalization of the NPBA 4-carboxamido-aniline moiety with electron donating methoxy groups, and are strongly correlated with themore » energy of the conducting frontier orbital relative to the Fermi level of the gold leads used in break-junction experiments.« less

Structure–function relationships in single molecule rectification by N-phenylbenzamide derivatives

DOE Office of Scientific and Technical Information (OSTI.GOV)

Koenigsmann, Christopher; Ding, Wendu; Koepf, Matthieu

Here, we examine structure–function relationships in a series of N-phenylbenzamide (NPBA) derivatives by using computational modeling to identify molecular structures that exhibit both rectification and good conductance together with experimental studies of bias-dependent single molecule conductance and rectification behavior using the scanning tunneling microscopy break-junction technique. From a large number of computationally screened molecular diode structures, we have identified NPBA as a promising candidate, relative to the other structures that were screened. We demonstrate experimentally that conductance and rectification are both enhanced by functionalization of the NPBA 4-carboxamido-aniline moiety with electron donating methoxy groups, and are strongly correlated with themore » energy of the conducting frontier orbital relative to the Fermi level of the gold leads used in break-junction experiments.« less

A grand unified model for liganded gold clusters

NASA Astrophysics Data System (ADS)

Xu, Wen Wu; Zhu, Beien; Zeng, Xiao Cheng; Gao, Yi

2016-12-01

A grand unified model (GUM) is developed to achieve fundamental understanding of rich structures of all 71 liganded gold clusters reported to date. Inspired by the quark model by which composite particles (for example, protons and neutrons) are formed by combining three quarks (or flavours), here gold atoms are assigned three `flavours' (namely, bottom, middle and top) to represent three possible valence states. The `composite particles' in GUM are categorized into two groups: variants of triangular elementary block Au3(2e) and tetrahedral elementary block Au4(2e), all satisfying the duet rule (2e) of the valence shell, akin to the octet rule in general chemistry. The elementary blocks, when packed together, form the cores of liganded gold clusters. With the GUM, structures of 71 liganded gold clusters and their growth mechanism can be deciphered altogether. Although GUM is a predictive heuristic and may not be necessarily reflective of the actual electronic structure, several highly stable liganded gold clusters are predicted, thereby offering GUM-guided synthesis of liganded gold clusters by design.

On the Enhanced Antibacterial Activity of Antibiotics Mixed with Gold Nanoparticles

NASA Astrophysics Data System (ADS)

Burygin, G. L.; Khlebtsov, B. N.; Shantrokha, A. N.; Dykman, L. A.; Bogatyrev, V. A.; Khlebtsov, N. G.

2009-08-01

The bacterial action of gentamicin and that of a mixture of gentamicin and 15-nm colloidal-gold particles on Escherichia coli K12 was examined by the agar-well-diffusion method, enumeration of colony-forming units, and turbidimetry. Addition of gentamicin to colloidal gold changed the gold color and extinction spectrum. Within the experimental errors, there were no significant differences in antibacterial activity between pure gentamicin and its mixture with gold nanoparticles (NPs). Atomic absorption spectroscopy showed that upon application of the gentamicin-particle mixture, there were no gold NPs in the zone of bacterial-growth suppression in agar. Yet, free NPs diffused into the agar. These facts are in conflict with the earlier findings indicating an enhancement of the bacterial activity of similar gentamicin-gold nanoparticle mixtures. The possible causes for these discrepancies are discussed, and the suggestion is made that a necessary condition for enhancement of antibacterial activity is the preparation of stable conjugates of NPs coated with the antibiotic molecules.

Silk fibroin/gold nanocrystals: a new example of biopolymer-based nanocomposites

NASA Astrophysics Data System (ADS)

Noinville, S.; Garnier, A.; Courty, A.

2017-05-01

The dispersion of nanoparticles in ordered polymer nanostructures can provide control over particle location and orientation, and pave the way for tailored nanomaterials that have enhanced mechanical, electrical, or optical properties. Here we used silk fibroin, a natural biopolymer, to embed gold nanocrystals (NCs), so as to obtain well-ordered structures such as nanowires and self-assembled triangular nanocomposites. Monodisperse gold NCs synthesized in organic media are mixed to silk fibroin and the obtained nanocomposites are characterized by UV-visible spectroscopy, transmission electron microscopy (TEM), scanning electron microscopy (FE-SEM), atomic force microscopy (AFM) and Infrared spectroscopy. The optical properties study of gold NCs and silk-gold nanocomposites shows that the Surface Plasmon band is blue shifted compared to gold NCs. The size and shape of NCs gold superlattices can be well controlled by the presence of silk fibroin giving nanowires and also self-assembled triangular nanocomposites as characterized by TEM, FE-SEM and AFM. The strong interaction between gold NCs and silk fibroin is also revealed by the conformation change of silk protein in presence of gold NCs, as shown by FTIR analysis. The formation of such ordered nanocomposites (gold NCs/silk fibroin) will provide new nanoplasmonic devices.

Gold nanoparticles deposited on glass: physicochemical characterization and cytocompatibility

PubMed Central

2013-01-01

Properties of gold films sputtered under different conditions onto borosilicate glass substrate were studied. Mean thickness of sputtered gold film was measured by gravimetry, and film contact angle was determined by goniometry. Surface morphology was examined by atomic force microscopy, and electrical sheet resistance was determined by two-point technique. The samples were seeded with rat vascular smooth muscle cells, and their adhesion and proliferation were studied. Gold depositions lead to dramatical changes in the surface morphology and roughness in comparison to pristine substrate. For sputtered gold structures, the rapid decline of the sheet resistance appears on structures deposited for the times above 100 s. The thickness of deposited gold nanoparticles/layer is an increasing function of sputtering time and current. AFM images prove the creation of separated gold islands in the initial deposition phase and a continuous gold coverage for longer deposition times. Gold deposition has a positive effect on the proliferation of vascular smooth muscle cells. Largest number of cells was observed on sample sputtered with gold for 20 s and at the discharge current of 40 mA. This sample exhibits lowest contact angle, low relative roughness, and only mild increase of electrical conductivity. PMID:23705782

Silver enhancement of nanogold and undecagold

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hainfield, J.F.; Furuya, F.R.

1995-07-01

A recent advance in immunogold technology has been the use of molecular gold instead of colloidal gold. A number of advantages are realized by this approach, such as stable covalent, site-specific attachment, small probe size and absence of aggregates for improved penetration. Silver enhancement has led to improved and unique results for electron and light microscopy, as well as their use with blots and gels. Most previous work with immunogold silver staining has been done with colloidal gold particles. More recently, large gold compounds (``clusters``) having a definite number of gold atoms and defined organic shell, have been used, frequentlymore » with improved results. These gold dusters, large compared to simple compounds, are, however, at the small end of the colloidal gold scale in size; undecagold is 0.8 nm and Nanogold is 1.4 nm. They may be used in practically all applications where colloidal gold is used (Light and electron microscopy, dot blots, etc.) and in some unique applications, where at least the larger colloidal golds don`t work, such as running gold labeled proteins on gels (which are later detected by silver enhancement). The main differences between gold clusters and colloidal golds are the small size of the dusters and their covalent attachment to antibodies or other molecules.« less

One-pot synthesis of keto thioethers by palladium/gold-catalyzed click and pinacol reactions.

PubMed

Cadu, Alban; Watile, Rahul A; Biswas, Srijit; Orthaber, Andreas; Sjöberg, Per J R; Samec, Joseph S M

2014-11-07

An atom-efficient synthesis of keto thioethers was devised via tandem gold/palladium catalysis. The reaction proceeds through a regioselective thiol attack at the β-position of the alcohol, followed by an alkyl, aryl, or benzyl 1,2-shift. Both acyclic and cyclic systems were studied, in the latter case leading to the ring expansion of cyclic substrates.

FY2014 Parameters for Helions and Gold Ions in Booster, AGS, and RHIC

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gardner, C. J.

The nominal parameters for helions (helion is the bound state of two protons and one neutron, the nucleus of a helium-3 atom) and gold ions in Booster, AGS, and RHIC are given for the FY2014 running period. The parameters are found using various formulas to derive mass, helion anomalous g-factor, kinetic parameters, RF parameters, ring parameters, etc..

The Emergence of Atomic-Level Structural Information for Ordered Metal-Solution Interfaces: Some Recent Contributions from In-Situ Infrared Spectroscopy and Scanning Tunneling Microscopy

DTIC Science & Technology

1992-02-28

Distribution/ Availabilit Codes jAval’ an~d/or Dist Speoial (19. cont.) reconstruction at gold-aqueous interfaces. All three low-index gold surfaces are...uncharged (vide supra). This difference may well be due to the influence of the interfacial water , or conceivably to adsorbed perchlorate anions. Both Au

Nanoscale functionalization and characterization of surfaces with hydrogel patterns and biomolecules

NASA Astrophysics Data System (ADS)

Dinakar, Hariharasudhan Chirra

The advent of numerous tools, ease of techniques, and concepts related to nanotechnology, in combination with functionalization via simple chemistry has made gold important for various biomedical applications. In this dissertation, the development and characterization of planar gold surfaces with responsive hydrogel patterns for rapid point of care sensing and the functionalization of gold nanoparticles for drug delivery are highlighted. Biomedical micro- and nanoscale devices that are spatially functionalized with intelligent hydrogels are typically fabricated using conventional UV-lithography. Herein, precise 3-D hydrogel patterns made up of temperature responsive crosslinked poly(N-isopropylacrylamide) over gold were synthesized. The XY control of the hydrogel was achieved using microcontact printing, while thickness control was achieved using atom transfer radical polymerization (ATRP). Atomic force microscopy analysis showed that to the ATRP reaction time governed the pattern growth. The temperature dependent swelling ratio was tailored by tuning the mesh size of the hydrogel. While nanopatterns exhibited a broad lower critical solution temperature (LCST) transition, surface roughness showed a sharp LCST transition. Quartz crystal microbalance with dissipation showed rapid response behavior of the thin films, which makes them applicable as functional components in biomedical devices. The easy synthesis, relative biocompatibility, inertness, and easy functionalization of gold nanoparticles (GNPs) have made them useful for various biomedical applications. Although ATRP can be successfully carried out over GNPs, the yield of stable solution based GNPs for biomedical applications prove to be low. As an alternative approach, a novel method of ISOlating, FUnctionalizing, and REleasing nanoparticles (ISOFURE) was proposed. Biodegradable poly(beta-amino ester) hydrogels were used to synthesize ISOFURE-GNP composites. ATRP was performed inside the composite, and the final hydrogel coated GNPs were released via matrix degradation. Response analysis confirmed that the ISOFURE method led to the increased stability and yield of the hydrogel coated ISOFURE-GNPs. The ISOFURE protocol was also utilized in functionalizing GNPs with enzyme catalase in the absence of a stabilizing reagent. Biotin-streptavidin affinity was used as the bioconjugation method. Activity analysis of the conjugated enzyme showed that the ISOFURE-GNPs showed enhanced biomolecular loading relative to solution based stabilizing reagent passivated GNPs. KEYWORDS: Hydrogel, Gold nanoparticle, ISOFURE, Atom transfer radical polymerization, Microcontact printing

NREL/Boeing Spectrolab Team Wins Research and Development Award | News |

Science.gov Websites

approach represents a powerful new technology for designing super-efficient multi-junction solar cells. The results in superior electrical performance. But, with the HEMM approach, the atoms are unevenly spaced

Quantum Conductance in Metal Nanowires

NASA Astrophysics Data System (ADS)

Ugarte, Daniel

2004-03-01

Quantum Conductance in Metal Nanowires D. Ugarte Brazilian National Synchrotron Light Laboratory C.P. 6192, 13084-971 Campinas SP, Brazil. Electrical transport properties of metallic nanowires (NWs) have received great attention due to their quantum conductance behavior. Atomic scale wires can be generated by stretching metal contacts; during the elongation and just before rupture, the NW conductance shows flat plateaus and abrupt jumps of approximately a conductance quantum. In this experiments, both the NW atomic arrangement and conductance change simultaneously, making difficult to discriminate electronic and structural effects. In this work, the atomic structure of NWs was studied by time-resolved in situ experiments in a high resolution transmission electron microscope, while their electrical properties using an UHV mechanically controllable break junction (MCBJ). From the analysis of numerous HRTEM images and videos, we have deduced that metal (Au, Ag, Pt, etc.) junctions generated by tensile deformation are crystalline and free of defects. The neck structure is strongly dependent on the surface properties of the analyzed metal, this was verified by comparing different metal NWs (Au, Ag, Cu), which have similar atomic structure (FCC), but show very different faceting patterns. The correlation between the observed structural and transport properties of NW points out that the quantum conductance behavior is defined by preferred atomic arrangement at the narrowest constriction. In the case of magnetic (ex. Fe,Co,Ni) or quasi-magnetic (ex. Pd) wires, we have observed that one-atom-thick structures show a conductance of half the quantum as expected for a fully spin polarized current. This phenomenon seems to occur spontaneously for magnetic suspended atom-chains in zero magnetic field and at room temperature. These results open new opportunities for spin control in nanostructures. Funded by FAPESP, LNLS and CNPq.

Ultimately short ballistic vertical graphene Josephson junctions

PubMed Central

Lee, Gil-Ho; Kim, Sol; Jhi, Seung-Hoon; Lee, Hu-Jong

2015-01-01

Much efforts have been made for the realization of hybrid Josephson junctions incorporating various materials for the fundamental studies of exotic physical phenomena as well as the applications to superconducting quantum devices. Nonetheless, the efforts have been hindered by the diffusive nature of the conducting channels and interfaces. To overcome the obstacles, we vertically sandwiched a cleaved graphene monoatomic layer as the normal-conducting spacer between superconducting electrodes. The atomically thin single-crystalline graphene layer serves as an ultimately short conducting channel, with highly transparent interfaces with superconductors. In particular, we show the strong Josephson coupling reaching the theoretical limit, the convex-shaped temperature dependence of the Josephson critical current and the exceptionally skewed phase dependence of the Josephson current; all demonstrate the bona fide short and ballistic Josephson nature. This vertical stacking scheme for extremely thin transparent spacers would open a new pathway for exploring the exotic coherence phenomena occurring on an atomic scale. PMID:25635386

Fabrication of Mg-X-O (X = Fe, Co, Ni, Cr, Mn, Ti, V, and Zn) barriers for magnetic tunnel junctions

NASA Astrophysics Data System (ADS)

Yakushiji, K.; Kitagawa, E.; Ochiai, T.; Kubota, H.; Shimomura, N.; Ito, J.; Yoda, H.; Yuasa, S.

2018-05-01

We fabricated magnetic tunnel junctions with a 3d-transition material(X)-doped MgO (Mg-X-O) barrier, and evaluated the effect of the doping on magnetoresistance (MR) and microstructure. Among the variations of X (X = Fe, Co, Ni, Cr, Mn, Ti, V, and Zn), X = Fe and Mn showed a high MR ratio of more than 100%, even at a low resistance-area product of 3 Ωμm2. The microstructure analysis revealed that (001) textured orientation formed for X = Fe and Mn despite substantial doping (about 10 at%). The elemental mappings indicated that Fe atoms in the Mg-Fe-O barrier were segregated at the interfaces, while Mn atoms were evenly involved in the Mg-Mn-O barrier. This suggests that MgO has high adaptability for Fe and Mn dopants in terms of high MR ratio.

NANOELECTRONICS. Epitaxial growth of a monolayer WSe2-MoS2 lateral p-n junction with an atomically sharp interface.

PubMed

Li, Ming-Yang; Shi, Yumeng; Cheng, Chia-Chin; Lu, Li-Syuan; Lin, Yung-Chang; Tang, Hao-Lin; Tsai, Meng-Lin; Chu, Chih-Wei; Wei, Kung-Hwa; He, Jr-Hau; Chang, Wen-Hao; Suenaga, Kazu; Li, Lain-Jong

2015-07-31

Two-dimensional transition metal dichalcogenides (TMDCs) such as molybdenum sulfide MoS2 and tungsten sulfide WSe2 have potential applications in electronics because they exhibit high on-off current ratios and distinctive electro-optical properties. Spatially connected TMDC lateral heterojunctions are key components for constructing monolayer p-n rectifying diodes, light-emitting diodes, photovoltaic devices, and bipolar junction transistors. However, such structures are not readily prepared via the layer-stacking techniques, and direct growth favors the thermodynamically preferred TMDC alloys. We report the two-step epitaxial growth of lateral WSe2-MoS2 heterojunction, where the edge of WSe2 induces the epitaxial MoS2 growth despite a large lattice mismatch. The epitaxial growth process offers a controllable method to obtain lateral heterojunction with an atomically sharp interface. Copyright © 2015, American Association for the Advancement of Science.

Electron Transport through Porphyrin Molecular Junctions

NASA Astrophysics Data System (ADS)

Zhou, Qi

The goal of this work is to study the properties that would affect the electron transport through a porphyrin molecular junction. This work contributes to the field of electron transport in molecular junctions in the following 3 aspects. First of all, by carrying out experiments comparing the conductance of the iron (III) porphyrin (protected) and the free base porphyrin (protected), it is confirmed that the molecular energy level broadening and shifting occurs for porphyrin molecules when coupled with the metal electrodes, and this level broadening and shifting plays an important role in the electron transport through molecular junctions. Secondly, by carrying out an in-situ deprotection of the acetyl-protected free base porphyrin molecules, it is found out that the presence of acetyl groups reduces the conductance. Thirdly, by incorporating the Matrix-assisted laser desorption/ionization (MALDI) spectrum and the in-situ deprotection prior to formation of molecular junctions, it allows a more precise understanding of the molecules involved in the formation of molecular junctions, and therefore allows an accurate analysis of the conductance histogram. The molecules are prepared by self-assembly and the junctions are formed using a Scanning Tunneling Microscopy (STM) molecular break junction technique. The porphyrin molecules are characterized by MALDI in solution before self-assembly to a gold/mica substrate. The self-assembled monolayers (SAMs) of porphyrins on gold are characterized by Ultraviolet-visible (UV-Vis) reflection spectroscopy to confirm that the molecules are attached to the substrate. The SAMs are then characterized by Angle-Resolved X-ray photoelectron spectroscopy (ARXPS) to determine the thickness and the average molecular orientation of the molecular layer. The electron transport is measured by conductance-displacement (G-S) experiments under a given bias (-0.4V). The conductance value of a single molecule is identified by a statistical analysis over a large set of measurements. In this thesis, I focus on two factors that would affect the electron transport through the porphyrin molecules, namely, the metal ion center, and the deprotection of the end groups. The effect of metal ion center is studied by comparing the conductance of an iron (III) porphyrin (protected) to that of a free base porphyrin (protected). The in-situ deprotection of the molecules before forming the junctions is completed to study the effect of the molecular-electrode interaction. The first factor studied, that is, the metal ion center in the porphyrin molecule, show that the conductance for iron (III) porphyrin (protected) is 3.74 x10-5 G0, and the conductance for the free base porphyrin (protected) is 4.73x10-5 G0 , where G0 = e2 / pih = (25.8kO)-1 is the quantized unit of electrical conductance. Through our collaborative efforts, first principles calculations carried out by our collaborators for the molecular levels of an isolated molecule (without electrodes) show that the energy levels of an iron (III) porphyrin molecule are slightly shifted compared to that of the free base porphyrin. For the free base porphyrin, the highest occupied molecular orbital (HOMO) level (-4.952 eV) lies between the chemical potentials of the substrate (-4.7 eV) and the STM tip (-5.1 eV). This level serves as a channel for electron transport. For the iron (III) porphyrin, the HOMO is at -5.306 eV, which is not in between the chemical potentials of the substrate. Therefore, a significantly smaller conductance is expected for the iron (III) porphyrin compared to the conductance of a free base porphyrin, because of the lack of the electron transport channel. However, the conductance measured from G-S experiments is comparable, i.e. 3.74 x10-5 G0 for iron (III) porphyrin and 4.73x10-5 G0 for free base porphyrin. This suggests that the molecular energy level broadening and shifting occurs for porphyrin molecules when coupled with the metal electrodes, and this level broadening and shifting may significantly affect the electron transport through molecular junctions. The second factor studied, that is, the deprotection of the porphyrin end groups (acetylthio, -SCOCH3), was completed in-situ for the free base porphyrin through the reaction of the acetylthio with sulfuric acid at 35° Celsius for 3 hours. MALDI spectroscopy confirms that two additional deprotected porphyrin species are formed by deprotection, with protonated (MH+) molecular masses of 721 and 679, corresponding to a partially deprotected porphyrin (i.e. only one of the two end groups deprotected), and a fully deprotected porphyrin molecule. Along with the un-reacted acetyl protected porphyrin, a total of 3 porphyrin species are in the solution. This solution is used for self-assembly on a gold/mica surface. The thickness of the in-situ deprotected SAM is determined to be ˜1.7 nm, confirming a relatively upright molecular orientation (54.0°-63.5° between the substrate surface and the molecule), compared to a thickness of ˜1.5 nm for the protected SAM that has a more flat-lying molecular orientation (˜45.6° between the substrate surface and the molecule). From G-S measurements on SAMs prepared by in-situ deprotection, junctions with lower conductance steps at mid 10-5 G0 and junctions with higher conductance steps around 10-4 G 0 are observed. Supported by computational modeling from our collaborating research group, we associate the lower conductance steps to junctions based on the protected form of thiols at the tip-molecule interface, and the higher conductance steps to the deprotected form of the thiol contacts. We suggest that the reduced conductance in the protected porphyrin originates from the presence of the acetyl end groups (-COCH3), rather than from the elongation of the sulfur-gold (S-Au) bonds at the tip-molecule interface. By studying these two factors, I expect this work to provide insights into electron transport through molecules or metal-molecule-metal junctions, and in applications related to integrating molecules as functional units in electronic devices. Future work related to this thesis may include the molecular conductance based on reduction-oxidation (redox) properties of iron ligated porphyrins for the application of molecular switches and molecular memory elements.

Focal Activation of Cells by Plasmon Resonance Assisted Optical Injection of Signaling Molecules

PubMed Central

2015-01-01

Experimental methods for single cell intracellular delivery are essential for probing cell signaling dynamics within complex cellular networks, such as those making up the tumor microenvironment. Here, we show a quantitative and general method of interrogation of signaling pathways. We applied highly focused near-infrared laser light to optically inject gold-coated liposomes encapsulating bioactive molecules into single cells for focal activation of cell signaling. For this demonstration, we encapsulated either inositol trisphosphate (IP3), an endogenous cell signaling second messenger, or adenophostin A (AdA), a potent analogue of IP, within 100 nm gold-coated liposomes, and injected these gold-coated liposomes and their contents into the cytosol of single ovarian carcinoma cells to initiate calcium (Ca2+) release from intracellular stores. Upon optical injection of IP3 or AdA at doses above the activation threshold, we observed increases in cytosolic Ca2+ concentration within the injected cell initiating the propagation of a Ca2+ wave throughout nearby cells. As confirmed by octanol-induced inhibition, the intercellular Ca2+ wave traveled via gap junctions. Optical injection of gold-coated liposomes represents a quantitative method of focal activation of signaling cascades of broad interest in biomedical research. PMID:24877558

Sonochemical Synthesis of a Zinc Oxide Core-Shell Nanorod Radial p-n Homojunction Ultraviolet Photodetector.

PubMed

Vabbina, Phani Kiran; Sinha, Raju; Ahmadivand, Arash; Karabiyik, Mustafa; Gerislioglu, Burak; Awadallah, Osama; Pala, Nezih

2017-06-14

We report for the first time on the growth of a homogeneous radial p-n junction in the ZnO core-shell configuration with a p-doped ZnO nanoshell structure grown around a high-quality unintentionally n-doped ZnO nanorod using sonochemistry. The simultaneous decomposition of phosphorous (P), zinc (Zn), and oxygen (O) from their respective precursors during sonication allows for the successful incorporation of P atoms into the ZnO lattice. The as-formed p-n junction shows a rectifying current-voltage characteristic that is consistent with a p-n junction with a threshold voltage of 1.3 V and an ideality factor of 33. The concentration of doping was estimated to be N A = 6.7 × 10 17 cm -3 on the p side from the capacitance-voltage measurements. The fabricated radial p-n junction demonstrated a record optical responsivity of 9.64 A/W and a noise equivalent power of 0.573 pW/√Hz under ultraviolet illumination, which is the highest for ZnO p-n junction devices.

Aluminum-catalyzed silicon nanowires: Growth methods, properties, and applications

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hainey, Mel F.; Redwing, Joan M.

Metal-mediated vapor-liquid-solid (VLS) growth is a promising approach for the fabrication of silicon nanowires, although residual metal incorporation into the nanowires during growth can adversely impact electronic properties particularly when metals such as gold and copper are utilized. Aluminum, which acts as a shallow acceptor in silicon, is therefore of significant interest for the growth of p-type silicon nanowires but has presented challenges due to its propensity for oxidation. This paper summarizes the key aspects of aluminum-catalyzed nanowire growth along with wire properties and device results. In the first section, aluminum-catalyzed nanowire growth is discussed with a specific emphasis onmore » methods to mitigate aluminum oxide formation. Next, the influence of growth parameters such as growth temperature, precursor partial pressure, and hydrogen partial pressure on nanowire morphology is discussed, followed by a brief review of the growth of templated and patterned arrays of nanowires. Aluminum incorporation into the nanowires is then discussed in detail, including measurements of the aluminum concentration within wires using atom probe tomography and assessment of electrical properties by four point resistance measurements. Finally, the use of aluminum-catalyzed VLS growth for device fabrication is reviewed including results on single-wire radial p-n junction solar cells and planar solar cells fabricated with nanowire/nanopyramid texturing.« less

Negative differential resistance observed from vertical p+-n+ junction device with two-dimensional black phosphorous

NASA Astrophysics Data System (ADS)

Lee, Daeyeong; Jang, Young Dae; Kweon, Jaehwan; Ryu, Jungjin; Hwang, Euyheon; Yoo, Won Jong; Samsung-SKKU Graphene/2D Center (SSGC) Collaboration

A vertical p+-n+ homojunction was fabricated by using black phosphorus (BP) as a van der Waals two-dimensional (2D) material. The top and bottom layers of the materials were doped by chemical dopants of gold chloride (AuCl3) for p-type doping and benzyl viologen (BV) for n-type doping. The negative differential resistance (NDR) effect was clearly observed from the output curves of the fabricated BP vertical devices. The thickness range of the 2D material showing NDR and the peak to valley current ratio of NDR are found to be strongly dependent on doping condition, gate voltage, and BP's degradation level. Furthermore, the carrier transport of the p+-n+ junction was simulated by using density functional theory (DFT) and non-equilibrium Green's function (NEGF). Both the experimental and simulation results confirmed that the NDR is attributed to the band-to-band tunneling (BTBT) across the 2D BP p+-n+ junction, and further quantitative details on the carrier transport in the vertical p+-n+ junction devices were explored, according to the analyses of the measured transfer curves and the DFT simulation results. This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MEST) (2013R1A2A2A01015516).

Multi-technique characterization of gold electroplating on silver substrates for cultural heritage applications

NASA Astrophysics Data System (ADS)

Ortega-Feliu, I.; Ager, F. J.; Roldán, C.; Ferretti, M.; Juanes, D.; Scrivano, S.; Respaldiza, M. A.; Ferrazza, L.; Traver, I.; Grilli, M. L.

2017-09-01

This work presents a detailed study of a series of silver plates gilded via electroplating techniques in which the characteristics of the coating gold layers are investigated as a function of the electroplating variables (voltage, time, anode surface and temperature). Some reference samples were coated by radio frequency sputtering in order to compare gold layer homogeneity and effective density. Surface analysis was performed by means of atomic and nuclear techniques (SEM-EDX, EDXRF, PIXE and RBS) to obtain information about thickness, homogeneity, effective density, profile concentration of the gold layers and Au-Ag diffusion profiles. The gold layer thickness obtained by PIXE and EDXRF is consistent with the thickness obtained by means of RBS depth profiling. Electroplated gold mass thickness increases with electroplating time, anode area and voltage. However, electrodeposited samples present rough interfaces and gold layer effective densities lower than the nominal density of Au (19.3 g/cm3), whereas sputtering produces uniform layers with nominal density. These analyses provide valuable information to historians and curators and can help the restoration process of gold-plated silver objects.

Gold Nanoparticles: An Efficient Antimicrobial Agent against Enteric Bacterial Human Pathogen

PubMed Central

Shamaila, Shahzadi; Zafar, Noshin; Riaz, Saira; Sharif, Rehana; Nazir, Jawad; Naseem, Shahzad

2016-01-01

Enteric bacterial human pathogens, i.e., Escherichia coli, Staphylococcus aureus, Bacillus subtilis and Klebsiella pneumoniae, are the major cause of diarrheal infections in children and adults. Their structure badly affects the human immune system. It is important to explore new antibacterial agents instead of antibiotics for treatment. This project is an attempt to explain how gold nanoparticles affect these bacteria. We investigated the important role of the mean particle size, and the inhibition of a bacterium is dose-dependent. Ultra Violet (UV)-visible spectroscopy revealed the size of chemically synthesized gold nanoparticle as 6–40 nm. Atomic force microscopy (AFM) analysis confirmed the size and X-ray diffractometry (XRD) analysis determined the polycrystalline nature of gold nanoparticles. The present findings explained how gold nanoparticles lyse Gram-negative and Gram-positive bacteria. PMID:28335198

Structural details of Al/Al 2O3 junctions and their role in the formation of electron tunnel barriers

NASA Astrophysics Data System (ADS)

Koberidze, M.; Puska, M. J.; Nieminen, R. M.

2018-05-01

We present a computational study of the adhesive and structural properties of the Al/Al 2O3 interfaces as building blocks of the metal-insulator-metal (MIM) tunnel devices, where electron transport is accomplished via tunneling mechanism through the sandwiched insulating barrier. The main goal of this paper is to understand, on the atomic scale, the role of the geometrical details in the formation of the tunnel barrier profiles. Initially, we concentrate on the adhesive properties of the interfaces. To provide reliable results, we carefully assess the accuracy of the traditional methods used to examine Al/Al 2O3 systems. These are the most widely employed exchange-correlation functionals—local-density approximation and two different generalized gradient approximations; the universal binding-energy relation for predicting equilibrium interfacial distances and adhesion energies; and the ideal work of separation as a measure of junction stability. In addition, we show that the established interpretation of the computed ideal work of separation might be misleading in predicting the optimal interface structures. Finally, we perform a detailed analysis of the atomic and interplanar relaxations in each junction, and identify their contributions to the tunnel barrier parameters. Our results imply that the structural irregularities on the surface of the Al film have a significant contribution to lowering the tunnel barrier height, while atomic relaxations at the interface and interplanar relaxations in Al2O3 may considerably change the width of the barrier and, thus, distort its uniformity. Both the effects may critically influence the performance of the MIM tunnel devices.

Use of electrothermal atomic absorption spectrometry for size profiling of gold and silver nanoparticles.

PubMed

Panyabut, Teerawat; Sirirat, Natnicha; Siripinyanond, Atitaya

2018-02-13

Electrothermal atomic absorption spectrometry (ETAAS) was applied to investigate the atomization behaviors of gold nanoparticles (AuNPs) and silver nanoparticles (AgNPs) in order to relate with particle size information. At various atomization temperatures from 1400 °C to 2200 °C, the time-dependent atomic absorption peak profiles of AuNPs and AgNPs with varying sizes from 5 nm to 100 nm were examined. With increasing particle size, the maximum absorbance was observed at the longer time. The time at maximum absorbance was found to linearly increase with increasing particle size, suggesting that ETAAS can be applied to provide the size information of nanoparticles. With the atomization temperature of 1600 °C, the mixtures of nanoparticles containing two particle sizes, i.e., 5 nm tannic stabilized AuNPs with 60, 80, 100 nm citrate stabilized AuNPs, were investigated and bimodal peaks were observed. The particle size dependent atomization behaviors of nanoparticles show potential application of ETAAS for providing size information of nanoparticles. The calibration plot between the time at maximum absorbance and the particle size was applied to estimate the particle size of in-house synthesized AuNPs and AgNPs and the results obtained were in good agreement with those from flow field-flow fractionation (FlFFF) and transmission electron microscopy (TEM) techniques. Furthermore, the linear relationship between the activation energy and the particle size was observed. Copyright © 2017 Elsevier B.V. All rights reserved.

Anisotropy induced Kondo splitting in a mechanically stretched molecular junction: A first-principles based study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Xiaoli; Hou, Dong, E-mail: houdong@ustc.edu.cn; Zheng, Xiao, E-mail: xz58@ustc.edu.cn

2016-01-21

The magnetic anisotropy and Kondo phenomena in a mechanically stretched magnetic molecular junction are investigated by combining the density functional theory (DFT) and hierarchical equations of motion (HEOM) approach. The system is comprised of a magnetic complex Co(tpy–SH){sub 2} sandwiched between adjacent gold electrodes, which is mechanically stretched in experiments done by Parks et al. [Science 328, 1370 (2010)]. The electronic structure and mechanical property of the stretched system are investigated via the DFT calculations. The HEOM approach is then employed to characterize the Kondo resonance features, based on the Anderson impurity model parameterized from the DFT results. It ismore » confirmed that the ground state prefers the S = 1 local spin state. The structural properties, the magnetic anisotropy, and corresponding Kondo peak splitting in the axial stretching process are systematically evaluated. The results reveal that the strong electron correlations and the local magnetic properties of the molecule magnet are very sensitive to structural distortion. This work demonstrates that the combined DFT+HEOM approach could be useful in understanding and designing mechanically controlled molecular junctions.« less

Anomalous length dependence of conductance of aromatic nanoribbons with amine anchoring groups

NASA Astrophysics Data System (ADS)

Bilić, Ante; Sanvito, Stefano

2012-09-01

Two sets of aromatic nanoribbons, based around a common hexagonal scaffolding, with single and dual terminal amine groups have been considered as potential molecular wires in a junction formed by gold leads. Charge transport through the two-terminal device has been modeled using density functional theory (with and without self-interaction correction) and the nonequilibrium Green's function method. The effects of wire length, multiple terminal contacts, and pathways across the junction have been investigated. For nanoribbons with the oligopyrene motif and conventional single amine terminal groups, an increase in the wire length causes an exponential drop in the conductance. In contrast, for the nanoribbons with the oligoperylene motif and dual amine anchoring groups the predicted conductance rises with the wire length over the whole range of investigated lengths. Only when the effects of self-interaction correction are taken into account, the conductance of the oligoperylene ribbons exhibits saturation for longer members of the series. The oligoperylene nanoribbons, with dual amine groups at both terminals, show the potential to fully harness the highly conjugated system of π molecular orbitals across the junction.

Interaction between benzenedithiolate and gold: Classical force field for chemical bonding

NASA Astrophysics Data System (ADS)

Leng, Yongsheng; Krstić, Predrag S.; Wells, Jack C.; Cummings, Peter T.; Dean, David J.

2005-06-01

We have constructed a group of classical potentials based on ab initio density-functional theory (DFT) calculations to describe the chemical bonding between benzenedithiolate (BDT) molecule and gold atoms, including bond stretching, bond angle bending, and dihedral angle torsion involved at the interface between the molecule and gold clusters. Three DFT functionals, local-density approximation (LDA), PBE0, and X3LYP, have been implemented to calculate single point energies (SPE) for a large number of molecular configurations of BDT-1, 2 Au complexes. The three DFT methods yield similar bonding curves. The variations of atomic charges from Mulliken population analysis within the molecule/metal complex versus different molecular configurations have been investigated in detail. We found that, except for bonded atoms in BDT-1, 2 Au complexes, the Mulliken partial charges of other atoms in BDT are quite stable, which significantly reduces the uncertainty in partial charge selections in classical molecular simulations. Molecular-dynamics (MD) simulations are performed to investigate the structure of BDT self-assembled monolayer (SAM) and the adsorption geometry of S adatoms on Au (111) surface. We found that the bond-stretching potential is the most dominant part in chemical bonding. Whereas the local bonding geometry of BDT molecular configuration may depend on the DFT functional used, the global packing structure of BDT SAM is quite independent of DFT functional, even though the uncertainty of some force-field parameters for chemical bonding can be as large as ˜100%. This indicates that the intermolecular interactions play a dominant role in determining the BDT SAMs global packing structure.

Interaction between benzenedithiolate and gold: classical force field for chemical bonding.

PubMed

Leng, Yongsheng; Krstić, Predrag S; Wells, Jack C; Cummings, Peter T; Dean, David J

2005-06-22

We have constructed a group of classical potentials based on ab initio density-functional theory (DFT) calculations to describe the chemical bonding between benzenedithiolate (BDT) molecule and gold atoms, including bond stretching, bond angle bending, and dihedral angle torsion involved at the interface between the molecule and gold clusters. Three DFT functionals, local-density approximation (LDA), PBE0, and X3LYP, have been implemented to calculate single point energies (SPE) for a large number of molecular configurations of BDT-1, 2 Au complexes. The three DFT methods yield similar bonding curves. The variations of atomic charges from Mulliken population analysis within the molecule/metal complex versus different molecular configurations have been investigated in detail. We found that, except for bonded atoms in BDT-1, 2 Au complexes, the Mulliken partial charges of other atoms in BDT are quite stable, which significantly reduces the uncertainty in partial charge selections in classical molecular simulations. Molecular-dynamics (MD) simulations are performed to investigate the structure of BDT self-assembled monolayer (SAM) and the adsorption geometry of S adatoms on Au (111) surface. We found that the bond-stretching potential is the most dominant part in chemical bonding. Whereas the local bonding geometry of BDT molecular configuration may depend on the DFT functional used, the global packing structure of BDT SAM is quite independent of DFT functional, even though the uncertainty of some force-field parameters for chemical bonding can be as large as approximately 100%. This indicates that the intermolecular interactions play a dominant role in determining the BDT SAMs global packing structure.

Tunable optical metamaterial based on liquid crystal-gold nanosphere composite.

PubMed

Pratibha, R; Park, K; Smalyukh, I I; Park, W

2009-10-26

Effect of the surrounding anisotropic liquid crystal medium on the surface plasmon resonance (SPR) exhibited by concentrated suspensions of gold nanospheres has been investigated experimentally and compared with the Mie scattering theory. The observed polarization-sensitive SPR and the red-shift in the SPR wavelength with increasing concentration of the gold nanospheres in the liquid crystal matrix have been explained using calculations based on the Maxwell Garnet effective medium theory. Agglomeration of the gold nanospheres that could also lead to such a red-shift has been ruled out using Atomic force microscopy study of thin nanoparticle-doped smectic films obtained on solid substrates. Our study demonstrates feasibility of obtaining tunable optical bulk metamaterials based on smectic liquid crystal - nanoparticle composites.

Chiral Gold Nanoclusters: Atomic Level Origins of Chirality.

PubMed

Zeng, Chenjie; Jin, Rongchao

2017-08-04

Chiral nanomaterials have received wide interest in many areas, but the exact origin of chirality at the atomic level remains elusive in many cases. With recent significant progress in atomically precise gold nanoclusters (e.g., thiolate-protected Au n (SR) m ), several origins of chirality have been unveiled based upon atomic structures determined by using single-crystal X-ray crystallography. The reported chiral Au n (SR) m structures explicitly reveal a predominant origin of chirality that arises from the Au-S chiral patterns at the metal-ligand interface, as opposed to the chiral arrangement of metal atoms in the inner core (i.e. kernel). In addition, chirality can also be introduced by a chiral ligand, manifested in the circular dichroism response from metal-based electronic transitions other than the ligand's own transition(s). Lastly, the chiral arrangement of carbon tails of the ligands has also been discovered in a very recent work on chiral Au 133 (SR) 52 and Au 246 (SR) 80 nanoclusters. Overall, the origins of chirality discovered in Au n (SR) m nanoclusters may provide models for the understanding of chirality origins in other types of nanomaterials and also constitute the basis for the development of various applications of chiral nanoparticles. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Quantitative Evaluation of Ion-implanted Arsenic in Silicon by Instrumental Neutron Activation Analysis

NASA Astrophysics Data System (ADS)

Takatsuka, Toshiko; Hirata, Kouichi; Kobayashi, Yoshinori; Kuroiwa, Takayoshi; Miura, Tsutomu; Matsue, Hideaki

2008-11-01

Certified reference materials (CRMs) of shallow arsenic implants in silicon are now under development at the National Metrology Institute of Japan (NMIJ). The amount of ion-implanted arsenic atoms is quantified by Instrumental Neutron Activation Analysis (INAA) using research reactor JRR-3 in Japan Atomic Energy Agency (JAEA). It is found that this method can evaluate arsenic amounts of 1015 atoms/cm2 with small uncertainties, and is adaptable to shallower dopants. The estimated uncertainties can satisfy the industrial demands for reference materials to calibrate the implanted dose of arsenic at shallow junctions.

Atomically thin resonant tunnel diodes built from synthetic van der Waals heterostructures.

PubMed

Lin, Yu-Chuan; Ghosh, Ram Krishna; Addou, Rafik; Lu, Ning; Eichfeld, Sarah M; Zhu, Hui; Li, Ming-Yang; Peng, Xin; Kim, Moon J; Li, Lain-Jong; Wallace, Robert M; Datta, Suman; Robinson, Joshua A

2015-06-19

Vertical integration of two-dimensional van der Waals materials is predicted to lead to novel electronic and optical properties not found in the constituent layers. Here, we present the direct synthesis of two unique, atomically thin, multi-junction heterostructures by combining graphene with the monolayer transition-metal dichalcogenides: molybdenum disulfide (MoS2), molybdenum diselenide (MoSe2) and tungsten diselenide (WSe2). The realization of MoS2-WSe2-graphene and WSe2-MoS2-graphene heterostructures leads to resonant tunnelling in an atomically thin stack with spectrally narrow, room temperature negative differential resistance characteristics.

Stretching single atom contacts at multiple subatomic step-length.

PubMed

Wei, Yi-Min; Liang, Jing-Hong; Chen, Zhao-Bin; Zhou, Xiao-Shun; Mao, Bing-Wei; Oviedo, Oscar A; Leiva, Ezequiel P M

2013-08-14

This work describes jump-to-contact STM-break junction experiments leading to novel statistical distribution of last-step length associated with conductance of a single atom contact. Last-step length histograms are observed with up to five for Fe and three for Cu peaks at integral multiples close to 0.075 nm, a subatomic distance. A model is proposed in terms of gliding from a fcc hollow-site to a hcp hollow-site of adjacent atomic planes at 1/3 regular layer spacing along with tip stretching to account for the multiple subatomic step-length behavior.

Photon Calorimeter

DOEpatents

Chow, Tze-Show

1989-01-01

A photon calorimeter (20, 40) is provided that comprises a laminar substrate (10, 22, 42) that is uniform in density and homogeneous in atomic composition. A plasma-sprayed coating (28, 48, 52), that is generally uniform in density and homogeneous in atomic composition within the proximity of planes that are parallel to the surfaces of the substrate, is applied to either one or both sides of the laminar substrate. The plasma-sprayed coatings may be very efficiently spectrally tailored in atomic number. Thermocouple measuring junctions (30, 50, 54) are positioned within the plasma-sprayed coatings. The calorimeter is rugged, inexpensive, and equilibrates in temperature very rapidly.

Ultra-cold 4He atom beams

NASA Astrophysics Data System (ADS)

Mulders, N.; Wyatt, A. F. G.

1994-02-01

It has been shown that it is possible to create ultra-cold 4He atom beams, using a metal film heater covered with a superfluid helium film. The transient behaviour of the atom pulse can be improved significantly by shaping of the heater pulse. The leading edge of more energetic atoms can be suppressed nearly completely, leaving a core of mono-energetic atoms. The maximum number of atoms in the pulse is determined by the amount of helium in the superfluid film on the heater. This seriously limits the ranges of pulse width and energy over which this beam source can be operated. However, these can be increased significantly by using porous gold smoke heaters.

Electronic Devices with Diffusion Barrier and Process for Making Same

DTIC Science & Technology

2001-05-09

conductivity metallization materials such as gold , silver, and platinum. As can be appreciated from the foregoing, a barrier film is needed which... gold ), as well as platinum. These metals are highly attractive 10 for interconnect strategies on account of there intrinsic low resistivity and...the monolayer portion of the barrier -7- material. The monolayer ( monoatomic ) layer of metal atoms and the homoepitaxial film of metal halide

A Sodium-Containing Quasicrystal: Using Gold To Enhance Sodium's Covalency in Intermetallic Compounds

DOE Office of Scientific and Technical Information (OSTI.GOV)

Smetana, Volodymyr; Lin, Qisheng; Pratt, Daniel K.

2013-09-26

Gold macht stabil: Na 13Au 12Ga 15, ein natriumhaltiges thermodynamisch stabiles quasikristallines Material, wurde bei einer systematischen Studie des polaren Na-Au-Ga-Intermetallsystems entdeckt. Sein Elektron/Atom-Verhältnis von 1.75 ist für Bergman-Ikosaederphasen extrem klein, doch der substanzielle Au-Anteil sorgt für eine Hume-Rothery-Stabilisierung und neuartige polar-kovalente Na-Au-Wechselwirkungen.

Rational Design in Catalysis: A Mechanistic Study of β-Hydride Eliminations in Gold(I) and Gold(III) Complexes Based on Features of the Reaction Valley.

PubMed

Castiñeira Reis, Marta; López, Carlos Silva; Kraka, Elfi; Cremer, Dieter; Faza, Olalla Nieto

2016-09-06

β-Hydride eliminations for ethylgold(III) dichloride complexes are identified as reactions with an unusually long prechemical stage corresponding to the conformational preparation of the reaction complex and spanning six phases. The prechemical process is characterized by a geared rotation of the L-Au-L group (L = Cl) driving methyl group rotation and causing a repositioning of the ligands. This requires more than 28 kcal/mol of the total barrier of 34.0 kcal/mol, according to the unified reaction valley approach, which also determines that the energy requirements of the actual chemical process leading to the β-elimination product are only about 5.5 kcal/mol. A detailed mechanistic analysis was used as a basis for a rational design of substrates (via substituents on the ethyl group) and/or ligands, which can significantly reduce the reaction barrier. This strategy takes advantage of either a higher trans activity of the ligands or a tuned electronic demand of the ethyl group. The β-hydride elimination of gold(I) was found to suffer from strong Coulomb and exchange repulsion when a positively charged hydrogen atom enforces a coordination position in a d(10)-configured gold atom, thus triggering an unassisted σ-π Au(I)-C conversion.

Routine and timely sub-picoNewton force stability and precision for biological applications of atomic force microscopy.

PubMed

Churnside, Allison B; Sullan, Ruby May A; Nguyen, Duc M; Case, Sara O; Bull, Matthew S; King, Gavin M; Perkins, Thomas T

2012-07-11

Force drift is a significant, yet unresolved, problem in atomic force microscopy (AFM). We show that the primary source of force drift for a popular class of cantilevers is their gold coating, even though they are coated on both sides to minimize drift. Drift of the zero-force position of the cantilever was reduced from 900 nm for gold-coated cantilevers to 70 nm (N = 10; rms) for uncoated cantilevers over the first 2 h after wetting the tip; a majority of these uncoated cantilevers (60%) showed significantly less drift (12 nm, rms). Removing the gold also led to ∼10-fold reduction in reflected light, yet short-term (0.1-10 s) force precision improved. Moreover, improved force precision did not require extended settling; most of the cantilevers tested (9 out of 15) achieved sub-pN force precision (0.54 ± 0.02 pN) over a broad bandwidth (0.01-10 Hz) just 30 min after loading. Finally, this precision was maintained while stretching DNA. Hence, removing gold enables both routine and timely access to sub-pN force precision in liquid over extended periods (100 s). We expect that many current and future applications of AFM can immediately benefit from these improvements in force stability and precision.

Mechanically Assisted Self-Healing of Ultrathin Gold Nanowires.

PubMed

Wang, Binjun; Han, Ying; Xu, Shang; Qiu, Lu; Ding, Feng; Lou, Jun; Lu, Yang

2018-04-17

As the critical feature sizes of integrated circuits approaching sub-10 nm, ultrathin gold nanowires (diameter <10 nm) have emerged as one of the most promising candidates for next-generation interconnects in nanoelectronics. Also due to their ultrasmall dimensions, however, the structures and morphologies of ultrathin gold nanowires are more prone to be damaged during practical services, for example, Rayleigh instability can significantly alter their morphologies upon Joule heating, hindering their applications as interconnects. Here, it is shown that upon mechanical perturbations, predamaged, nonuniform ultrathin gold nanowires can quickly recover into uniform diameters and restore their smooth surfaces, via a simple mechanically assisted self-healing process. By examining the local self-healing process through in situ high-resolution transmission electron microscopy, the underlying mechanism is believed to be associated with surface atomic diffusion as evidenced by molecular dynamics simulations. In addition, mechanical manipulation can assist the atoms to overcome the diffusion barriers, as suggested by ab initio calculations, to activate more surface adatoms to diffuse and consequently speed up the self-healing process. This result can provide a facile method to repair ultrathin metallic nanowires directly in functional devices, and quickly restore their microstructures and morphologies by simple global mechanical perturbations. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Reflectivity around the gold L-edges of x-ray reflector of the soft x-ray telescope onboard ASTRO-H

NASA Astrophysics Data System (ADS)

Maeda, Yoshitomo; Kikuchi, Naomichi; Kurashima, Sho; Ishida, Manabu; Iizuka, Ryo; Hayashi, Takayuki; Okajima, Takashi; Matsumoto, Hironori; Mitsuishi, Ikuyuki; Saji, Shigetaka; Sato, Toshiki; Tachibana, Sasagu; Mori, Hideyuki; Christensen, Finn; Brejnholt, Nicolai; Nitta, Kiyofumi; Uruga, Tomoya

2016-07-01

We report the atomic scattering factor in the 11.2{15.4 keV for the ASTRO-H Soft X-ray Telescope (SXT)9 obtained in the ground based measurements. The large effective area of the SXT covers above 10 keV. In fact, the flight data show the spectra of the celestical objects in the hard X-ray band. In order to model the area, the reflectivity measurements in the 11.2{15.4 keV band with the energy pitch of 0.4 { 0.7 eV were made in the synchrotron beamline Spring-8 BL01B1. We obtained atomic scattering factors f1 and f2 by the curve fitting to the reflectivities of our witness sample. The edges associated with the gold's L-I, II, and III transitions are identified, of which the depths are found to be roughly 60% shallower than those expected from the Henke's atomic scattering factor.

Reflectivity Around the Gold L-Edges of X-Ray Reflector of the Soft X-Ray Telescope Onboard ASTRO-H

NASA Technical Reports Server (NTRS)

Maeda, Yoshitomo; Kikuchi, Naomichi; Kurashima, Sho; Ishida, Manabu; Iizuka, Ryo; Hayashi, Takayuki; Okajima, Takashi; Matsumoto, Hironori; Mitsuishi, Ikuyuki; Saji, Shigetaka;

Interaction of benzene thiol and thiolate with small gold clusters.

PubMed

Letardi, Sara; Cleri, Fabrizio

2004-06-01

We studied the interaction between benzene thiol and thiolate molecules, and gold clusters made of 1 to 3 atoms, by means of ab initio density functional theory in the local density approximation. We find that the thiolate is energetically more stable than the thiol, however the process of detachment of H from the thiol appears to be possibly mediated by the intermediate step of H chemisorption on Au. Cleavage of the S-H bond is accompanied by a 90 degrees rotation of the molecule around the S-Au bond, showing a strong steric specificity. Such a rotation is induced by the relative energy shift of the S atom p orbitals with respect to the benzene pi ring and the Au d orbitals. By analyzing the correlation of the bond energy, bond lengths, and HOMO-LUMO gap with the number of S-Au bonds, we find that the thiolate S atom appears to prefer a low-coordination condition on Au clusters. (c) 2004 American Institute of Physics.

First-principles investigation of quantum transport in GeP3 nanoribbon-based tunneling junctions

NASA Astrophysics Data System (ADS)

Wang, Qiang; Li, Jian-Wei; Wang, Bin; Nie, Yi-Hang

2018-06-01

Two-dimensional (2D) GeP3 has recently been theoretically proposed as a new low-dimensional material [ Nano Lett. 17(3), 1833 (2017)]. In this manuscript, we propose a first-principles calculation to investigate the quantum transport properties of several GeP3 nanoribbon-based atomic tunneling junctions. Numerical results indicate that monolayer GeP3 nanoribbons show semiconducting behavior, whereas trilayer GeP3 nanoribbons express metallic behavior owing to the strong interaction between each of the layers. This behavior is in accordance with that proposed in two-dimensional GeP3 layers. The transmission coefficient T( E) of tunneling junctions is sensitive to the connecting formation between the central monolayer GeP3 nanoribbon and the trilayer GeP3 nanoribbon at both ends. The T( E) value of the bottom-connecting tunneling junction is considerably larger than those of the middle-connecting and top-connecting ones. With increases in gate voltage, the conductances increase for the bottom-connecting and middle-connecting tunneling junctions, but decrease for the top-connecting tunneling junctions. In addition, the conductance decreases exponentially with respect to the length of the central monolayer GeP3 nanoribbon for all the tunneling junctions. I-V curves show approximately linear behavior for the bottom-connecting and middle-connecting structures, but exhibit negative differential resistance for the top-connecting structures. The physics of each phenomenon is analyzed in detail.

Quantum conductance oscillation in linear monatomic silicon chains

NASA Astrophysics Data System (ADS)

Liu, Fu-Ti; Cheng, Yan; Yang, Fu-Bin; Chen, Xiang-Rong

2014-02-01

The conductance of linear silicon atomic chains with n=1-8 atoms sandwiched between Au electrodes is investigated by using the density functional theory combined with non-equilibrium Green's function. The results show that the conductance oscillates with a period of two atoms as the number of atoms in the chain is varied. We optimize the geometric structure of nanoscale junctions in different distances, and obtain that the average bond-length of silicon atoms in each chain at equilibrium positions is 2.15±0.03 Å. The oscillation of average Si-Si bond-length can explain the conductance oscillation from the geometric structure of atomic chains. We calculate the transmission spectrum of the chains in the equilibrium positions, and explain the conductance oscillation from the electronic structure. The transport channel is mainly contributed by px and py orbital electrons of silicon atoms. The even-odd oscillation is robust under external voltage up to 1.2 V.

Atomtronics: Realizing the behavior of electronic components in ultracold atomic systems

NASA Astrophysics Data System (ADS)

Pepino, Ron

2007-06-01

Atomtronics focuses on creating an analogy of electronic devices and circuits with ultracold atoms. Such an analogy can come from the highly tunable band structure of ultracold neutral atoms trapped in optical lattices. Solely by tuning the parameters of the optical lattice, we demonstrate that conditions can be created that cause atoms in lattices to exhibit the same behavior as electrons moving through solid state media. We present our model and show how the atomtronic diode, field effect transistor, and bipolar junction transistor can all be realized. Our analogs of these fundamental components exhibit precisely-controlled atomic signal amplification, trimming, and switching (on/off) characteristics. In addition, the evolution of dynamics of the superfluid atomic currents within these systems is completely reversible. This implies a possible use of atomtronic systems in the development of quantum computational devices.

An important rule for realizing metal → half-metal → semiconductor transition in single-molecule junctions

NASA Astrophysics Data System (ADS)

Zeng, Jing; Chen, Ke-Qiu; Long, Mengqiu

2017-06-01

Recently, Zhong et al (2015 Nano Lett. 15 8091) found that two additional hydrogen atoms can be adsorbed to the opposite aza-bridging nitrogen atoms of the manganese phthalocyanine (MnPc) macrocycle when exposed to H2. Thus the symmetry of the MnPc molecule is changed from 4-fold to 2-fold. Motivated by this recent experiment, we theoretically investigate a MnPc-based single-molecule junction in this work and propose a simple and reliable way to realize the transition of its electronic properties. On the basis of spin-polarized density-functional theory calculations combined with the Keldysh nonequilibrium Green’s technique, we find that the gradual hydrogenation in MnPc molecules gives rise to the changes of the hardness of the electron density and spin-selective orbital decoupling, which eventually leads to the realization of the first ever metal  →  half-metal  →  semiconductor transition behavior in single-molecule junctions. Analysis of molecular projected self-consistent Hamiltonian, Mulliken population, and local density of states also reveals an important rule for realizing this transition behavior. Our research confirms that the hydrogenation of MnPc molecules can realize various molecular functionalities in unitary material background.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stokes, Adam; Al-Jassim, Mowafak; Norman, Andrew

The effects of alkali diffusion and post-deposition treatment in three-stage processed Cu(In,Ga)Se 2 solar cells are examined by using atom probe tomography and electrical property measurements. Cells, for which the substrate was treated at 650 °C to induce alkali diffusion from the substrate prior to absorber deposition, exhibited high open-circuit voltage (758 mV) and efficiency (18.2%) and also exhibited a 50 to 100-nm-thick ordered vacancy compound layer at the metallurgical junction. Surprisingly, these high-temperature samples exhibited higher concentrations of K at the junction (1.8 at.%) than post-deposition treatment samples (0.4 at.%). A model that uses Ga/(Ga + In) and Cu/(Gamore » + In) profiles to predict bandgaps (+/-17.9 meV) of 22 Cu(In,Ga)Se2 solar cells reported in literature was discussed and ultimately used to predict band properties at the nanoscale by using atom probe tomography data. The high-temperature samples exhibited a greater drop in the valence band maximum (200 meV) due to a lower Cu/(Ga + In) ratio than the post-deposition treatment samples. There was an anticorrelation of K concentrations and Cu/(Ga + In) ratios for all samples, regardless of processing conditions. In conclusion, changes in elemental profiles at the active junctions correlate well with the electrical behaviour of these devices.« less

A thermal microprobe fabricated with wafer-stage processing

NASA Astrophysics Data System (ADS)

Zhang, Yongxia; Zhang, Yanwei; Blaser, Juliana; Sriram, T. S.; Enver, Ahsan; Marcus, R. B.

1998-05-01

A thermal microprobe has been designed and built for high resolution temperature sensing. The thermal sensor is a thin-film thermocouple junction at the tip of an atomic force microprobe (AFM) silicon probe needle. Only wafer-stage processing steps are used for the fabrication. For high resolution temperature sensing it is essential that the junction be confined to a short distance at the AFM tip. This confinement is achieved by a controlled photoresist coating process. Experiment prototypes have been made with an Au/Pd junction confined to within 0.5 μm of the tip, with the two metals separated elsewhere by a thin insulating oxide layer. Processing begins with double-polished, n-type, 4 in. diameter, 300-μm-thick silicon wafers. Atomically sharp probe tips are formed by a combination of dry and wet chemical etching, and oxidation sharpening. The metal layers are sputtering deposited and the cantilevers are released by a combination of KOH and dry etching. A resistively heated calibration device was made for temperature calibration of the thermal microprobe over the temperature range 25-110 °C. Over this range the thermal outputs of two microprobes are 4.5 and 5.6 μV/K and is linear. Thermal and topographical images are also obtained from a heated tungsten thin film fuse.

Superior visible light hydrogen evolution of Janus bilayer junctions via atomic-level charge flow steering

NASA Astrophysics Data System (ADS)

Li, Jie; Zhan, Guangming; Yu, Ying; Zhang, Lizhi

2016-05-01

Although photocatalytic hydrogen evolution (PHE) is ideal for solar-to-fuel conversion, it remains challenging to construct a highly efficient PHE system by steering the charge flow in a precise manner. Here we tackle this challenge by assembling 1T MoS2 monolayers selectively and chemically onto (Bi12O17) end-faces of Bi12O17Cl2 monolayers to craft two-dimensional (2D) Janus (Cl2)-(Bi12O17)-(MoS2) bilayer junctions, a new 2D motif different from van der Waals heterostructure. Electrons and holes from visible light-irradiated Bi12O17Cl2 are directionally separated by the internal electric field to (Bi12O17) and (Cl2) end-faces, respectively. The separated electrons can further migrate to MoS2 via Bi-S bonds formed between (Bi12O17) and MoS2 monolayers. This atomic-level directional charge separation endows the Janus bilayers with ultralong carrier lifetime of 3,446 ns and hence a superior visible-light PHE rate of 33 mmol h-1 g-1. Our delineated Janus bilayer junctions on the basis of the oriented assembly of monolayers presents a new design concept to effectively steer the charge flow for PHE.

Contact and Length Dependent Effects in Single-Molecule Electronics

NASA Astrophysics Data System (ADS)

Hines, Thomas

Understanding charge transport in single molecules covalently bonded to electrodes is a fundamental goal in the field of molecular electronics. In the past decade, it has become possible to measure charge transport on the single-molecule level using the STM break junction method. Measurements on the single-molecule level shed light on charge transport phenomena which would otherwise be obfuscated by ensemble measurements of groups of molecules. This thesis will discuss three projects carried out using STM break junction. In the first project, the transition between two different charge transport mechanisms is reported in a set of molecular wires. The shortest wires show highly length dependent and temperature invariant conductance behavior, whereas the longer wires show weakly length dependent and temperature dependent behavior. This trend is consistent with a model whereby conduction occurs by coherent tunneling in the shortest wires and by incoherent hopping in the longer wires. Measurements are supported with calculations and the evolution of the molecular junction during the pulling process is investigated. The second project reports controlling the formation of single-molecule junctions by means of electrochemically reducing two axial-diazonium terminal groups on a molecule, thereby producing direct Au-C covalent bonds in-situ between the molecule and gold electrodes. Step length analysis shows that the molecular junction is significantly more stable, and can be pulled over a longer distance than a comparable junction created with amine anchoring bonds. The stability of the junction is explained by the calculated lower binding energy associated with the direct Au-C bond compared with the Au-N bond. Finally, the third project investigates the role that molecular conformation plays in the conductance of oligothiophene single-molecule junctions. Ethyl substituted oligothiophenes were measured and found to exhibit temperature dependent conductance and transition voltage for molecules with between two and six repeat units. While the molecule with only one repeat unit shows temperature invariant behavior. Density functional theory calculations show that at higher temperatures the oligomers with multiple repeat units assume a more planar conformation, which increases the conjugation length and decreases the effective energy barrier of the junction.

Coherent coupling of a superconducting flux qubit to an electron spin ensemble in diamond.

PubMed

Zhu, Xiaobo; Saito, Shiro; Kemp, Alexander; Kakuyanagi, Kosuke; Karimoto, Shin-ichi; Nakano, Hayato; Munro, William J; Tokura, Yasuhiro; Everitt, Mark S; Nemoto, Kae; Kasu, Makoto; Mizuochi, Norikazu; Semba, Kouichi

2011-10-12

During the past decade, research into superconducting quantum bits (qubits) based on Josephson junctions has made rapid progress. Many foundational experiments have been performed, and superconducting qubits are now considered one of the most promising systems for quantum information processing. However, the experimentally reported coherence times are likely to be insufficient for future large-scale quantum computation. A natural solution to this problem is a dedicated engineered quantum memory based on atomic and molecular systems. The question of whether coherent quantum coupling is possible between such natural systems and a single macroscopic artificial atom has attracted considerable attention since the first demonstration of macroscopic quantum coherence in Josephson junction circuits. Here we report evidence of coherent strong coupling between a single macroscopic superconducting artificial atom (a flux qubit) and an ensemble of electron spins in the form of nitrogen-vacancy colour centres in diamond. Furthermore, we have observed coherent exchange of a single quantum of energy between a flux qubit and a macroscopic ensemble consisting of about 3 × 10(7) such colour centres. This provides a foundation for future quantum memories and hybrid devices coupling microwave and optical systems.

First-principles density functional theory (DFT) study of gold nanorod and its interaction with alkanethiol ligands.

PubMed

Hu, Hang; Reven, Linda; Rey, Alejandro

2013-10-17

The structure and mechanical properties of gold nanorods and their interactions with alkenthiolate self-assembled monolayers have been determined using a novel first-principle density functional theory simulation approach. The multifaceted, 1-dimensional, octagonal nanorod has alternate Au100 and Au110 surfaces. The structural optimization of the gold nanorods was performed with a mixed basis: the outermost layer of gold atoms used double-ζ plus polarization (DZP), the layer below used double-ζ (DZ), and the inner layers used single-ζ (SZ). The final structure compares favorably with simulations using DZP for all atoms. Phonon dispersion calculations and ab initio molecular dynamics (AIMD) were used to establish the dynamic and thermal stability of the system. From the AIMD simulations it was found that the nanorod system will undergo significant surface reconstruction at 300 K. In addition, when subjected to mechanical stress in the axial direction, the nanorod responds as an orthotropic material, with uniform expansion along the radial direction. The Young's moduli are 207 kbar in the axial direction and 631 kbar in the radial direction. The binding of alkanethiolates, ranging from methanethiol to pentanethiol, caused formation of surface point defects on the Au110 surfaces. On the Au100 surfaces, the defects occurred in the inner layer, creating a small surface island. These defects make positive and negative concavities on the gold nanorod surface, which helps the ligand to achieve a more stable state. The simulation results narrowed significant knowledge gaps on the alkanethiolate adsorption process and on their mutual interactions on gold nanorods. The mechanical characterization offers a new dimension to understand the physical chemistry of these complex nanoparticles.

An electrically actuated molecular toggle switch

NASA Astrophysics Data System (ADS)

Gerhard, Lukas; Edelmann, Kevin; Homberg, Jan; Valášek, Michal; Bahoosh, Safa G.; Lukas, Maya; Pauly, Fabian; Mayor, Marcel; Wulfhekel, Wulf

2017-03-01

Molecular electronics is considered a promising approach for future nanoelectronic devices. In order that molecular junctions can be used as electrical switches or even memory devices, they need to be actuated between two distinct conductance states in a controlled and reproducible manner by external stimuli. Here we present a tripodal platform with a cantilever arm and a nitrile group at its end that is lifted from the surface. The formation of a coordinative bond between the nitrile nitrogen and the gold tip of a scanning tunnelling microscope can be controlled by both electrical and mechanical means, and leads to a hysteretic switching of the conductance of the junction by more than two orders of magnitude. This toggle switch can be actuated with high reproducibility so that the forces involved in the mechanical deformation of the molecular cantilever can be determined precisely with scanning tunnelling microscopy.

Electron scattering effects at physisorbed hydrogen molecules on break-junction electrodes and nanowires formation in hydrogen environment

NASA Astrophysics Data System (ADS)

van der Maas, M.; Vasnyov, S.; Hendriksen, B. L. M.; Shklyarevskii, O. I.; Speller, S.

2012-06-01

Physisorption of hydrogen molecules on the surface of gold and other coinage metals has been studied using distance tunneling spectroscopy. We have observed that the distance dependence of the tunnel current (resistance) displays a strong N-shaped deviation from exponential behavior. Such deviations are difficult to explain within the Tersoff-Hamann approximation. We suggest the scattering of tunneling electrons by H2 molecules as an origin for the observed effect. We have found that this phenomenon is also common for strongly adsorbed organic molecules with a single anchoring group. Pulling Au, Cu and Pt nanowires at 22 K in hydrogen environment shows that the break-junction electrodes are still connected through hydrogen-metal monoatomic chains down to very low conductance values of 10-4-10-6 G0.

Junction-to-Case Thermal Resistance of a Silicon Carbide Bipolar Junction Transistor Measured

NASA Technical Reports Server (NTRS)

Niedra, Janis M.

2006-01-01

Junction temperature of a prototype SiC-based bipolar junction transistor (BJT) was estimated by using the base-emitter voltage (V(sub BE)) characteristic for thermometry. The V(sub BE) was measured as a function of the base current (I(sub B)) at selected temperatures (T), all at a fixed collector current (I(sub C)) and under very low duty cycle pulse conditions. Under such conditions, the average temperature of the chip was taken to be the same as that of the temperature-controlled case. At increased duty cycle such as to substantially heat the chip, but same I(sub C) pulse height, the chip temperature was identified by matching the V(sub BE) to the thermometry curves. From the measured average power, the chip-to-case thermal resistance could be estimated, giving a reasonable value. A tentative explanation for an observed bunching with increasing temperature of the calibration curves may relate to an increasing dopant atom ionization. A first-cut analysis, however, does not support this.

Spatial fluctuations in barrier height at the graphene-silicon carbide Schottky junction.

PubMed

Rajput, S; Chen, M X; Liu, Y; Li, Y Y; Weinert, M; Li, L

2013-01-01

When graphene is interfaced with a semiconductor, a Schottky contact forms with rectifying properties. Graphene, however, is also susceptible to the formation of ripples upon making contact with another material. Here we report intrinsic ripple- and electric field-induced effects at the graphene semiconductor Schottky junction, by comparing chemical vapour-deposited graphene transferred on semiconductor surfaces of opposite polarization-the hydrogen-terminated silicon and carbon faces of hexagonal silicon carbide. Using scanning tunnelling microscopy/spectroscopy and first-principles calculations, we show the formation of a narrow Schottky dipole barrier approximately 10 Å wide, which facilitates the observed effective electric field control of the Schottky barrier height. We further find atomic-scale spatial fluctuations in the Schottky barrier that directly follow the undulation of ripples on both graphene-silicon carbide junctions. These findings reveal fundamental properties of the graphene/semiconductor Schottky junction-a key component of vertical graphene devices that offer functionalities unattainable in planar device architecture.

Scanning Tunneling Microscopy, Atomic Force Microscopy, and Related Techniques.

DTIC Science & Technology

1992-06-15

images of the heaoal ekdprotein monolayer pressed powder samples of pismO claim and sea urchin shells found ~ ~ sx inteotrcelwl fDincoccu radioduran...can be in- Semiconductor Substrates. The atomic structure of sem - vastigated using AFM but has not been as extensively re- iconductor-detal interfaces...from SEM mage (D99). Komaica and p-type Si(00) and p-n junctions formed by implantation of ANALYTICAL CHEMISTRY. VOL 84, NO. 12. JILNE 18. 1992 121R

Performance enhancement of Ge-on-Insulator tunneling FETs with source junctions formed by low-energy BF2 ion implantation

NASA Astrophysics Data System (ADS)

Katoh, Takumi; Matsumura, Ryo; Takaguchi, Ryotaro; Takenaka, Mitsuru; Takagi, Shinichi

2018-04-01

To clarify the process of formation of source regions of high-performance Ge n-channel tunneling field-effect transistors (TFETs), p+-n junctions formed by low-energy ion implantation (I/I) of BF2 atoms are characterized. Here, the formation of p+-n junctions with steep B profiles and low junction leakage is a key issue. The steepness of 5.7 nm/dec in profiles of B implanted into Ge is obtained for BF2 I/I at 3 keV with a dose of 4 × 1014 cm-2. Ge-on-insulator (GOI) n-TFETs with the source tunnel junctions formed by low-energy B and BF2 I/I are fabricated on GOI substrates and the device operation is confirmed. Although the performance at room temperature is significantly degraded by the source junction leakage current, an I on/I off ratio of 105 and the minimum sub-threshold swing (S.S.) of 130 mV/dec are obtained at 10 K. It is found that GOI n-TFETs with steeper B profiles formed by BF2 I/I have led to higher on current and a lower sub-threshold slope, demonstrating the effectiveness of steep B profiles in enhancing the GOI TFET performance.

Realization of radial p-n junction silicon nanowire solar cell based on low-temperature and shallow phosphorus doping

NASA Astrophysics Data System (ADS)

Dong, Gangqiang; Liu, Fengzhen; Liu, Jing; Zhang, Hailong; Zhu, Meifang

2013-12-01

A radial p-n junction solar cell based on vertically free-standing silicon nanowire (SiNW) array is realized using a novel low-temperature and shallow phosphorus doping technique. The SiNW arrays with excellent light trapping property were fabricated by metal-assisted chemical etching technique. The shallow phosphorus doping process was carried out in a hot wire chemical vapor disposition chamber with a low substrate temperature of 250°C and H2-diluted PH3 as the doping gas. Auger electron spectroscopy and Hall effect measurements prove the formation of a shallow p-n junction with P atom surface concentration of above 1020 cm-3 and a junction depth of less than 10 nm. A short circuit current density of 37.13 mA/cm2 is achieved for the radial p-n junction SiNW solar cell, which is enhanced by 7.75% compared with the axial p-n junction SiNW solar cell. The quantum efficiency spectra show that radial transport based on the shallow phosphorus doping of SiNW array improves the carrier collection property and then enhances the blue wavelength region response. The novel shallow doping technique provides great potential in the fabrication of high-efficiency SiNW solar cells.

A biocompatible synthesis of gold nanoparticles by Tris(hydroxymethyl)aminomethane

NASA Astrophysics Data System (ADS)

Chen, Feng; Wang, Yanwei; Ma, Jun; Yang, Guangcan

2014-05-01

Gold nanoparticles' novel properties are widely realized in catalysis, plasmonics, electronics, and biomedical applications. For biomedical application, one challenge is to find a non-toxic chemical and/or physical method of functionalizing gold nanoparticles with biomolecular compounds that can promote efficient binding, clearance, and biocompatibility and to assess their safety to other biological systems and their long-term effects on human health and reproduction. In the present study, we describe a new method by using Tris(hydroxymethyl)aminomethane (Tris), a widely used buffer solvent of nucleic acid and proteins, as the reducing agent for synthesizing gold nanoparticles by one step. It is found that Tris carries out the reduction reactions in relatively mild conditions for biomacromolecules. Particularly, it can be used to modify the DNA during the process of preparation of gold nanoparticles. The morphology and size distribution of gold nanoparticles are consistent and were confirmed by many different approaches including dynamic light scattering (DLS), UV-visible (UV-vis) spectrophotometry, atomic force microscopy (AFM), and transmission electron microscopy (TEM).

Matter, energy, and heat transfer in a classical ballistic atom pump.

PubMed

Byrd, Tommy A; Das, Kunal K; Mitchell, Kevin A; Aubin, Seth; Delos, John B

2014-11-01

A ballistic atom pump is a system containing two reservoirs of neutral atoms or molecules and a junction connecting them containing a localized time-varying potential. Atoms move through the pump as independent particles. Under certain conditions, these pumps can create net transport of atoms from one reservoir to the other. While such systems are sometimes called "quantum pumps," they are also models of classical chaotic transport, and their quantum behavior cannot be understood without study of the corresponding classical behavior. Here we examine classically such a pump's effect on energy and temperature in the reservoirs, in addition to net particle transport. We show that the changes in particle number, of energy in each reservoir, and of temperature in each reservoir vary in unexpected ways as the incident particle energy is varied.

Twinning in fcc lattice creates low-coordinated catalytically active sites in porous gold

DOE Office of Scientific and Technical Information (OSTI.GOV)

Krajčí, Marian; Kameoka, Satoshi; Tsai, An-Pang

We describe a new mechanism for creation of catalytically active sites in porous gold. Samples of porous gold prepared by de-alloying Al{sub 2}Au exhibit a clear correlation between the catalytic reactivity towards CO oxidation and structural defects in the fcc lattice of Au. We have found that on the stepped (211) surfaces quite common twin boundary defects in the bulk structure of porous gold can form long close-packed rows of atoms with the coordination number CN = 6. DFT calculations confirm that on these low-coordinated Au sites dioxygen chemisorbs and CO oxidation can proceed via the Langmuir–Hinshelwood mechanism with themore » activation energy of 37 kJ/mol or via the CO–OO intermediate with the energy barrier of 19 kJ/mol. The existence of the twins in porous gold is stabilized by the surface energy.« less

Nanoporous Gold for Enzyme Immobilization.

PubMed

Stine, Keith J; Jefferson, Kenise; Shulga, Olga V

2017-01-01

Nanoporous gold (NPG) is a material of emerging interest for immobilization of biomolecules, especially enzymes. The material provides a high surface area form of gold that is suitable for physisorption or for covalent modification by self-assembled monolayers. The material can be used as a high surface area electrode and with immobilized enzymes can be used for amperometric detection schemes. NPG can be prepared in a variety of formats from alloys containing between 20 and 50 % atomic composition of gold and less noble element(s) by dealloying procedures. Materials resembling NPG can be prepared by hydrothermal and electrodeposition methods. Related high surface area gold structures have been prepared using templating approaches. Covalent enzyme immobilization can be achieved by first forming a self-assembled monolayer on NPG bearing a terminal reactive functional group followed by conjugation to the enzyme through amide linkages to lysine residues. Enzymes can also be entrapped by physisorption or immobilized by electrostatic interactions.

Novel Catalysis by Gold: A Modern Alchemy

NASA Astrophysics Data System (ADS)

Haruta, Masatake

Gold has long been neglected as a catalyst because of its chemical inertness. However, when gold is deposited as nanoparticles on carbon and polymer materials as well as on base metal oxides and hydroxides, it exhibits unique catalytic properties for many reactions such as CO oxidation at a temperature as low as 200 K, gas phase direct epoxidation of propylene, and aerobic oxidation of glucose to gluconic acid. The structure-catalytic activity correlations are discussed with emphasis on the contact structure, support selection, and the size control of gold particles. Gold clusters with diameters smaller than 2 nm are expected to exhibit novel properties in catalysis, optics, and electronics depending on the size (number of atoms), shape, and the electronic and chemical interaction with the support materials. The above achievements and attempts can be regarded as a modern alchemy that creates valuables by means of the noblest element with little practical use.

Formation of mono-layered gold nanoparticles in shallow depth of SiO 2 thin film by low-energy negative-ion implantation

NASA Astrophysics Data System (ADS)

Tsuji, H.; Arai, N.; Ueno, K.; Matsumoto, T.; Gotoh, N.; Adachi, K.; Kotaki, H.; Gotoh, Y.; Ishikawa, J.

2006-01-01

Mono-layered gold nanoparticles just below the surface of silicon oxide film have been formed by a gold negative-ion implantation at a very low-energy, where the deviation of implanted atoms was sufficiently narrow comparing to the size of nanoparticles. Gold negative ions were implanted into SiO2 thin films on Si substrate at energies of 35, 15 and 1 keV. The samples were annealed in Ar flow for 1 h at 900 or 1000 °C. Cross-sectional TEM observation for the implantation at 1 keV showed existence of Au nanoparticles aligned in the same depth of 5 nm from the surface. The nanoparticles had almost same diameter of 7 nm. The nanoparticles were found to be gold single crystal from a high-resolution TEM image.

Atomically resolved calcium phosphate coating on a gold substrate.

PubMed

Metoki, Noah; Baik, Sung-Il; Isheim, Dieter; Mandler, Daniel; Seidman, David N; Eliaz, Noam

2018-05-10

Some articles have revealed that the electrodeposition of calcium phosphate (CaP) coatings entails a precursor phase, similarly to biomineralization in vivo. The chemical composition of the initial layer and its thickness are, however, still arguable, to the best of our knowledge. Moreover, while CaP and electrodeposition of metal coatings have been studied utilizing atom-probe tomography (APT), the electrodeposition of CaP ceramics has not been heretofore studied. Herein, we present an investigation of the CaP deposition on a gold substrate. Using APT and transmission electron microscopy (TEM) it is found that a mixture of phases, which could serve as transient precursor phases to hydroxyapatite (HAp), can be detected. The thickness of these phases is tens of nanometers, and they consist of amorphous CaP (ACP), dibasic calcium phosphate dihydrate (DCPD), and octacalcium phosphate (OCP). This demonstrates the value of using atomic-resolved characterization techniques for identifying the precursor phases. It also indicates that the kinetics of their transformation into the more stable HAp is not too fast to enable their observation. The coating gradually displays higher Ca/P atomic ratios, a porous nature, and concomitantly a change in its density.

Determination of iridium in mafic rocks by atomic absorption

USGS Publications Warehouse

Grimaldi, F.S.; Schnepfe, M.M.

1970-01-01

Iridium is determined in mineralized mafic rocks by atomic absorption after fire-assay concentration into a gold bead. Interelement interferences in the atomic-absorption determination are removed and Ir sensitivity is increased by buffering the solutions with a mixture of copper and sodium sulphates. Substantial amounts of Ag, Al, Au, Bi, Ca, Cd, Co, Cr, Fe, Ho, Hg, K, La, Mg, Mn, Mo, Ni, Pb, Te, Ti, V, Y, Zn and platinum metals can be tolerated in the atomic-absorption determination. The sensitivity and detection limits are 3.2 and 0.25 ppm of Ir, respectively. ?? 1970.