In situ monitoring of atomic layer epitaxy via optical ellipsometry

NASA Astrophysics Data System (ADS)

Lyzwa, F.; Marsik, P.; Roddatis, V.; Bernhard, C.; Jungbauer, M.; Moshnyaga, V.

2018-03-01

We report on the use of time-resolved optical ellipsometry to monitor the deposition of single atomic layers with subatomic sensitivity. Ruddlesden-Popper thin films of SrO(SrTiO3) n=4 were grown by means of metalorganic aerosol deposition in the atomic layer epitaxy mode on SrTiO3(1 0 0), LSAT(1 0 0) and DyScO3(1 1 0) substrates. The measured time dependences of ellipsometric angles, Δ(t) and Ψ(t), were described by using a simple optical model, considering the sequence of atomic layers SrO and TiO2 with corresponding bulk refractive indices. As a result, valuable online information on the atomic layer epitaxy process was obtained. Ex situ characterization techniques, i.e. transmission electron microscopy, x-ray diffraction and x-ray reflectometry verify the crystal structure and confirm the predictions of optical ellipsometry.

Interfacial structure of two-dimensional epitaxial Er silicide on Si(111)

NASA Astrophysics Data System (ADS)

Tuilier, M. H.; Wetzel, P.; Pirri, C.; Bolmont, D.; Gewinner, G.

1994-07-01

Auger-electron diffraction (AED) and surface-extended x-ray-absorption fine structure (SEXAFS) have been used to obtain a complete description of the atomic structure of a two-dimensional epitaxial Er silicide layer on Si(111). AED reveals that a monolayer of Er is located underneath a buckled Si double layer. The relevant Er-Si interlayer spacings are determined by means of single scattering cluster simulations and a R-factor analysis to be 1.92+/-0.05 Å to the first and 2.70+/-0.05 Å to the second Si top layer. Er near-neighbor bond lengths and coordination numbers are obtained independently from polarization-dependent SEXAFS. The SEXAFS data, when combined with the Si top-layer geometry inferred from AED, permit the determination of the atomic positions at the silicide/Si(111) interface. The Er is found to reside in relaxed T4 sites of Si(111) with a single Er-Si distance of 3.09+/-0.04 Å to the first- and second-layer Si atoms of the substrate.

A robust molecular probe for Ångstrom-scale analytics in liquids

PubMed Central

Nirmalraj, Peter; Thompson, Damien; Dimitrakopoulos, Christos; Gotsmann, Bernd; Dumcenco, Dumitru; Kis, Andras; Riel, Heike

2016-01-01

Traditionally, nanomaterial profiling using a single-molecule-terminated scanning probe is performed at the vacuum–solid interface often at a few Kelvin, but is not a notion immediately associated with liquid–solid interface at room temperature. Here, using a scanning tunnelling probe functionalized with a single C60 molecule stabilized in a high-density liquid, we resolve low-dimensional surface defects, atomic interfaces and capture Ångstrom-level bond-length variations in single-layer graphene and MoS2. Atom-by-atom controllable imaging contrast is demonstrated at room temperature and the electronic structure of the C60–metal probe complex within the encompassing liquid molecules is clarified using density functional theory. Our findings demonstrates that operating a robust single-molecular probe is not restricted to ultra-high vacuum and cryogenic settings. Hence the scope of high-precision analytics can be extended towards resolving sub-molecular features of organic elements and gauging ambient compatibility of emerging layered materials with atomic-scale sensitivity under experimentally less stringent conditions. PMID:27516157

Soldering to a single atomic layer

NASA Astrophysics Data System (ADS)

Girit, ćaǧlar Ö.; Zettl, A.

2007-11-01

The standard technique to make electrical contact to nanostructures is electron beam lithography. This method has several drawbacks including complexity, cost, and sample contamination. We present a simple technique to cleanly solder submicron sized, Ohmic contacts to nanostructures. To demonstrate, we contact graphene, a single atomic layer of carbon, and investigate low- and high-bias electronic transport. We set lower bounds on the current carrying capacity of graphene. A simple model allows us to obtain device characteristics such as mobility, minimum conductance, and contact resistance.

Soldering to a single atomic layer

NASA Astrophysics Data System (ADS)

Girit, Caglar; Zettl, Alex

2008-03-01

The standard technique to make electrical contact to nanostructures is electron beam lithography. This method has several drawbacks including complexity, cost, and sample contamination. We present a simple technique to cleanly solder submicron sized, Ohmic contacts to nanostructures. To demonstrate, we contact graphene, a single atomic layer of carbon, and investigate low- and high-bias electronic transport. We set lower bounds on the current carrying capacity of graphene. A simple model allows us to obtain device characteristics such as mobility, minimum conductance, and contact resistance.

Atomic layer confined vacancies for atomic-level insights into carbon dioxide electroreduction

NASA Astrophysics Data System (ADS)

Gao, Shan; Sun, Zhongti; Liu, Wei; Jiao, Xingchen; Zu, Xiaolong; Hu, Qitao; Sun, Yongfu; Yao, Tao; Zhang, Wenhua; Wei, Shiqiang; Xie, Yi

2017-02-01

The role of oxygen vacancies in carbon dioxide electroreduction remains somewhat unclear. Here we construct a model of oxygen vacancies confined in atomic layer, taking the synthetic oxygen-deficient cobalt oxide single-unit-cell layers as an example. Density functional theory calculations demonstrate the main defect is the oxygen(II) vacancy, while X-ray absorption fine structure spectroscopy reveals their distinct oxygen vacancy concentrations. Proton transfer is theoretically/experimentally demonstrated to be a rate-limiting step, while energy calculations unveil that the presence of oxygen(II) vacancies lower the rate-limiting activation barrier from 0.51 to 0.40 eV via stabilizing the formate anion radical intermediate, confirmed by the lowered onset potential from 0.81 to 0.78 V and decreased Tafel slope from 48 to 37 mV dec-1. Hence, vacancy-rich cobalt oxide single-unit-cell layers exhibit current densities of 2.7 mA cm-2 with ca. 85% formate selectivity during 40-h tests. This work establishes a clear atomic-level correlation between oxygen vacancies and carbon dioxide electroreduction.

Contrast and Raman spectroscopy study of single- and few-layered charge density wave material: 2H-TaSe2

PubMed Central

Hajiyev, Parviz; Cong, Chunxiao; Qiu, Caiyu; Yu, Ting

2013-01-01

In this article, we report the first successful preparation of single- and few-layers of tantalum diselenide (2H-TaSe2) by mechanical exfoliation technique. Number of layers is confirmed by white light contrast spectroscopy and atomic force microscopy (AFM). Vibrational properties of the atomically thin layers of 2H-TaSe2 are characterized by micro-Raman spectroscopy. Room temperature Raman measurements demonstrate MoS2-like spectral features, which are reliable for thickness determination. E1g mode, usually forbidden in backscattering Raman configuration is observed in the supported TaSe2 layers while disappears in the suspended layers, suggesting that this mode may be enabled because of the symmetry breaking induced by the interaction with the substrate. A systematic in-situ low temperature Raman study, for the first time, reveals the existence of incommensurate charge density wave phase transition in single and double-layered 2H-TaSe2 as reflected by a sudden softening of the second-order broad Raman mode resulted from the strong electron-phonon coupling (Kohn anomaly). PMID:24005335

CVD synthesis of large-area, highly crystalline MoSe2 atomic layers on diverse substrates and application to photodetectors.

PubMed

Xia, Jing; Huang, Xing; Liu, Ling-Zhi; Wang, Meng; Wang, Lei; Huang, Ben; Zhu, Dan-Dan; Li, Jun-Jie; Gu, Chang-Zhi; Meng, Xiang-Min

2014-08-07

Synthesis of large-area, atomically thin transition metal dichalcogenides (TMDs) on diverse substrates is of central importance for the large-scale fabrication of flexible devices and heterojunction-based devices. In this work, we successfully synthesized a large area of highly-crystalline MoSe2 atomic layers on SiO2/Si, mica and Si substrates using a simple chemical vapour deposition (CVD) method at atmospheric pressure. Atomic force microscopy (AFM) and Raman spectroscopy reveal that the as-grown ultrathin MoSe2 layers change from a single layer to a few layers. Photoluminescence (PL) spectroscopy demonstrates that while the multi-layer MoSe2 shows weak emission peaks, the monolayer has a much stronger emission peak at ∼ 1.56 eV, indicating the transition from an indirect to a direct bandgap. Transmission electron microscopy (TEM) analysis confirms the single-crystallinity of MoSe2 layers with a hexagonal structure. In addition, the photoresponse performance of photodetectors based on MoSe2 monolayer was studied for the first time. The devices exhibit a rapid response of ∼ 60 ms and a good photoresponsivity of ∼ 13 mA/W (using a 532 nm laser at an intensity of 1 mW mm(-2) and a bias of 10 V), suggesting that MoSe2 monolayer is a promising material for photodetection applications.

Study on electrical defects level in single layer two-dimensional Ta2O5

NASA Astrophysics Data System (ADS)

Dahai, Li; Xiongfei, Song; Linfeng, Hu; Ziyi, Wang; Rongjun, Zhang; Liangyao, Chen; David, Wei Zhang; Peng, Zhou

2016-04-01

Two-dimensional atomic-layered material is a recent research focus, and single layer Ta2O5 used as gate dielectric in field-effect transistors is obtained via assemblies of Ta2O5 nanosheets. However, the electrical performance is seriously affected by electronic defects existing in Ta2O5. Therefore, spectroscopic ellipsometry is used to calculate the transition energies and corresponding probabilities for two different charged oxygen vacancies, whose existence is revealed by x-ray photoelectron spectroscopy analysis. Spectroscopic ellipsometry fitting also calculates the thickness of single layer Ta2O5, exhibiting good agreement with atomic force microscopy measurement. Nondestructive and noncontact spectroscopic ellipsometry is appropriate for detecting the electrical defects level of single layer Ta2O5. Project supported by the National Natural Science Foundation of China (Grant Nos. 11174058 and 61376093), the Fund from Shanghai Municipal Science and Technology Commission (Grant No. 13QA1400400), the National Science and Technology Major Project, China (Grant No. 2011ZX02707), and the Innovation Program of Shanghai Municipal Education Commission (Grant No. 12ZZ010).

Enhancement of resistive switching properties in Al2O3 bilayer-based atomic switches: multilevel resistive switching

NASA Astrophysics Data System (ADS)

Vishwanath, Sujaya Kumar; Woo, Hyunsuk; Jeon, Sanghun

2018-06-01

Atomic switches are considered to be building blocks for future non-volatile data storage and internet of things. However, obtaining device structures capable of ultrahigh density data storage, high endurance, and long data retention, and more importantly, understanding the switching mechanisms are still a challenge for atomic switches. Here, we achieved improved resistive switching performance in a bilayer structure containing aluminum oxide, with an oxygen-deficient oxide as the top switching layer and stoichiometric oxide as the bottom switching layer, using atomic layer deposition. This bilayer device showed a high on/off ratio (105) with better endurance (∼2000 cycles) and longer data retention (104 s) than single-oxide layers. In addition, depending on the compliance current, the bilayer device could be operated in four different resistance states. Furthermore, the depth profiles of the hourglass-shaped conductive filament of the bilayer device was observed by conductive atomic force microscopy.

Superconducting ferecrystals: turbostratically disordered atomic-scale layered (PbSe)1.14(NbSe2)n thin films.

PubMed

Grosse, Corinna; Alemayehu, Matti B; Falmbigl, Matthias; Mogilatenko, Anna; Chiatti, Olivio; Johnson, David C; Fischer, Saskia F

2016-09-16

Hybrid electronic heterostructure films of semi- and superconducting layers possess very different properties from their bulk counterparts. Here, we demonstrate superconductivity in ferecrystals: turbostratically disordered atomic-scale layered structures of single-, bi- and trilayers of NbSe2 separated by PbSe layers. The turbostratic (orientation) disorder between individual layers does not destroy superconductivity. Our method of fabricating artificial sequences of atomic-scale 2D layers, structurally independent of their neighbours in the growth direction, opens up new possibilities of stacking arbitrary numbers of hybrid layers which are not available otherwise, because epitaxial strain is avoided. The observation of superconductivity and systematic Tc changes with nanostructure make this synthesis approach of particular interest for realizing hybrid systems in the search of 2D superconductivity and the design of novel electronic heterostructures.

Atom-Thin SnS2-xSex with Adjustable Compositions by Direct Liquid Exfoliation from Single Crystals.

PubMed

Yang, Zhanhai; Liang, Hui; Wang, Xusheng; Ma, Xinlei; Zhang, Tao; Yang, Yanlian; Xie, Liming; Chen, Dong; Long, Yujia; Chen, Jitao; Chang, Yunjie; Yan, Chunhua; Zhang, Xinxiang; Zhang, Xueji; Ge, Binghui; Ren, Zhian; Xue, Mianqi; Chen, Genfu

2016-01-26

Two-dimensional (2D) chalcogenide materials are fundamentally and technologically fascinating for their suitable band gap energy and carrier type relevant to their adjustable composition, structure, and dimensionality. Here, we demonstrate the exfoliation of single-crystal SnS2-xSex (SSS) with S/Se vacancies into an atom-thin layer by simple sonication in ethanol without additive. The introduction of vacancies at the S/Se site, the conflicting atomic radius of sulfur in selenium layers, and easy incorporation with an ethanol molecule lead to high ion accessibility; therefore, atom-thin SSS flakes can be effectively prepared by exfoliating the single crystal via sonication. The in situ pyrolysis of such materials can further adjust their compositions, representing tunable activation energy, band gap, and also tunable response to analytes of such materials. As the most basic and crucial step of the 2D material field, the successful synthesis of an uncontaminated and atom-thin sample will further push ahead the large-scale applications of 2D materials, including, but not limited to, electronics, sensing, catalysis, and energy storage fields.

Atomic layer epitaxy of GaN over sapphire using switched metalorganic chemical vapor deposition

NASA Astrophysics Data System (ADS)

Khan, M. A.; Skogman, R. A.; van Hove, J. M.; Olson, D. T.; Kuznia, J. N.

1992-03-01

In this letter the first switched atomic layer epitaxy (SALE) of single crystal GaN over basal plane sapphire substrates is reported. A low pressure metalorganic chemical vapor deposition (LPMOCVD) system was used for the epilayer depositions. In contrast to conventional LPMOCVD requiring temperatures higher than 700 C, the SALE process resulted in single crystal insulating GaN layers at growth temperatures ranging from 900 to 450 C. The band-edge transmission and the photoluminescence of the films from the SALE process were comparable to the best LPMOCVD films. As best as is known this is the first report of insulating GaN films which show excellent band-edge photoluminescence.

Atomic layer epitaxy of GaN over sapphire using switched metalorganic chemical vapor deposition

NASA Astrophysics Data System (ADS)

Asif Khan, M.; Skogman, R. A.; Van Hove, J. M.; Olson, D. T.; Kuznia, J. N.

1992-03-01

In this letter we report the first switched atomic layer epitaxy (SALE) of single crystal GaN over basal plane sapphire substrates. A low pressure metalorganic chemical vapor deposition (LPMOCVD) system was used for the epilayer depositions. In contrast to conventional LPMOCVD requiring temperatures higher than 700 °C, the SALE process resulted in single crystal insulating GaN layers at growth temperatures ranging from 900 to 450 °C. The band-edge transmission and the photoluminescence of the films from the SALE process were comparable to the best LPMOCVD films. To the best of our knowledge this is the first report of insulating GaN films which show excellent band-edge photoluminescence.

Enhanced magnetic anisotropies of single transition-metal adatoms on a defective MoS2 monolayer.

PubMed

Cong, W T; Tang, Z; Zhao, X G; Chu, J H

2015-03-23

Single magnetic atoms absorbed on an atomically thin layer represent the ultimate limit of bit miniaturization for data storage. To approach the limit, a critical step is to find an appropriate material system with high chemical stability and large magnetic anisotropic energy. Here, on the basis of first-principles calculations and the spin-orbit coupling theory, it is elucidated that the transition-metal Mn and Fe atoms absorbed on disulfur vacancies of MoS2 monolayers are very promising candidates. It is analysed that these absorption systems are of not only high chemical stabilities but also much enhanced magnetic anisotropies and particularly the easy magnetization axis is changed from the in-plane one for Mn to the out-of-plane one for Fe by a symmetry-lowering Jahn-Teller distortion. The results point out a promising direction to achieve the ultimate goal of single adatomic magnets with utilizing the defective atomically thin layers.

Investigations into the impact of various substrates and ZnO ultra thin seed layers prepared by atomic layer deposition on growth of ZnO nanowire array

PubMed Central

2012-01-01

The impact of various substrates and zinc oxide (ZnO) ultra thin seed layers prepared by atomic layer deposition on the geometric morphology of subsequent ZnO nanowire arrays (NWs) fabricated by the hydrothermal method was investigated. The investigated substrates included B-doped ZnO films, indium tin oxide films, single crystal silicon (111), and glass sheets. Scanning electron microscopy and X-ray diffraction measurements revealed that the geometry and aligment of the NWs were controlled by surface topography of the substrates and thickness of the ZnO seed layers, respectively. According to atomic force microscopy data, we suggest that the substrate, fluctuate amplitude and fluctuate frequency of roughness on ZnO seed layers have a great impact on the alignment of the resulting NWs, whereas the influence of the seed layers' texture was negligible. PMID:22759838

STM/STS Study of the Sb (111) Surface

NASA Astrophysics Data System (ADS)

Chekmazov, S. V.; Bozhko, S. I.; Smirnov, A. A.; Ionov, A. M.; Kapustin, A. A.

An Sb crystal is a Peierls insulator. Formation of double layers in the Sb structure is due to the shift of atomic planes (111) next but one along the C3 axis. Atomic layers inside the double layer are connected by covalent bonds. The interaction between double layers is determined mainly by Van der Waals forces. The cleave of an Sb single crystal used to be via break of Van der Waals bonds. However, using scanning tunneling microscopy (STM) and spectroscopy (STS) we demonstrated that apart from islands equal in thickness to the double layer, steps of one atomic layer in height also exist on the cleaved Sb (111) surface. Formation of "unpaired" (111) planes on the surface leads to a local break of conditions of Peierls transition. STS experiment reveals higher local density of states (LDOS) measured for "unpaired" (111) planes in comparison with those for the double layer.

Atomic Structures of Silicene Layers Grown on Ag(111): Scanning Tunneling Microscopy and Noncontact Atomic Force Microscopy Observations

PubMed Central

Resta, Andrea; Leoni, Thomas; Barth, Clemens; Ranguis, Alain; Becker, Conrad; Bruhn, Thomas; Vogt, Patrick; Le Lay, Guy

2013-01-01

Silicene, the considered equivalent of graphene for silicon, has been recently synthesized on Ag(111) surfaces. Following the tremendous success of graphene, silicene might further widen the horizon of two-dimensional materials with new allotropes artificially created. Due to stronger spin-orbit coupling, lower group symmetry and different chemistry compared to graphene, silicene presents many new interesting features. Here, we focus on very important aspects of silicene layers on Ag(111): First, we present scanning tunneling microscopy (STM) and non-contact Atomic Force Microscopy (nc-AFM) observations of the major structures of single layer and bi-layer silicene in epitaxy with Ag(111). For the (3 × 3) reconstructed first silicene layer nc-AFM represents the same lateral arrangement of silicene atoms as STM and therefore provides a timely experimental confirmation of the current picture of the atomic silicene structure. Furthermore, both nc-AFM and STM give a unifying interpretation of the second layer (√3 × √3)R ± 30° structure. Finally, we give support to the conjectured possible existence of less stable, ~2% stressed, (√7 × √7)R ± 19.1° rotated silicene domains in the first layer. PMID:23928998

Multilayer Nanoporous Graphene Membranes for Water Desalination.

PubMed

Cohen-Tanugi, David; Lin, Li-Chiang; Grossman, Jeffrey C

2016-02-10

While single-layer nanoporous graphene (NPG) has shown promise as a reverse osmosis (RO) desalination membrane, multilayer graphene membranes can be synthesized more economically than the single-layer material. In this work, we build upon the knowledge gained to date toward single-layer graphene to explore how multilayer NPG might serve as a RO membrane in water desalination using classical molecular dynamic simulations. We show that, while multilayer NPG exhibits similarly promising desalination properties to single-layer membranes, their separation performance can be designed by manipulating various configurational variables in the multilayer case. This work establishes an atomic-level understanding of the effects of additional NPG layers, layer separation, and pore alignment on desalination performance, providing useful guidelines for the design of multilayer NPG membranes.

Theoretical Study of α-V2O5 -Based Double-Wall Nanotubes.

PubMed

Porsev, Vitaly V; Bandura, Andrei V; Evarestov, Robert A

2015-10-05

First-principles calculations of the atomic and electronic structure of double-wall nanotubes (DWNTs) of α-V2 O5 are performed. Relaxation of the DWNT structure leads to the formation of two types of local regions: 1) bulk-type regions and 2) puckering regions. Calculated total density of states (DOS) of DWNTs considerably differ from that of single-wall nanotubes and the single layer, as well as from the DOS of the bulk and double layer. Small shoulders that appear on edges of valence and conduction bands result in a considerable decrease in the band gaps of the DWNTs (up to 1 eV relative to the single-layer gaps). The main reason for this effect is the shift of the inner- and outer-wall DOS in opposite directions on the energetic scale. The electron density corresponding to shoulders at the conduction-band edges is localized on vanadium atoms of the bulk-type regions, whereas the electron density corresponding to shoulders at the valence-band edges belongs to oxygen atoms of both regions. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Single layer of Ge quantum dots in HfO2 for floating gate memory capacitors.

PubMed

Lepadatu, A M; Palade, C; Slav, A; Maraloiu, A V; Lazanu, S; Stoica, T; Logofatu, C; Teodorescu, V S; Ciurea, M L

2017-04-28

High performance trilayer memory capacitors with a floating gate of a single layer of Ge quantum dots (QDs) in HfO 2 were fabricated using magnetron sputtering followed by rapid thermal annealing (RTA). The layer sequence of the capacitors is gate HfO 2 /floating gate of single layer of Ge QDs in HfO 2 /tunnel HfO 2 /p-Si wafers. Both Ge and HfO 2 are nanostructured by RTA at moderate temperatures of 600-700 °C. By nanostructuring at 600 °C, the formation of a single layer of well separated Ge QDs with diameters of 2-3 nm at a density of 4-5 × 10 15 m -2 is achieved in the floating gate (intermediate layer). The Ge QDs inside the intermediate layer are arranged in a single layer and are separated from each other by HfO 2 nanocrystals (NCs) about 8 nm in diameter with a tetragonal/orthorhombic structure. The Ge QDs in the single layer are located at the crossing of the HfO 2 NCs boundaries. In the intermediate layer, besides Ge QDs, a part of the Ge atoms is segregated by RTA at the HfO 2 NCs boundaries, while another part of the Ge atoms is present inside the HfO 2 lattice stabilizing the tetragonal/orthorhombic structure. The fabricated capacitors show a memory window of 3.8 ± 0.5 V and a capacitance-time characteristic with 14% capacitance decay in the first 3000-4000 s followed by a very slow capacitance decrease extrapolated to 50% after 10 years. This high performance is mainly due to the floating gate of a single layer of well separated Ge QDs in HfO 2 , distanced from the Si substrate by the tunnel oxide layer with a precise thickness.

Structure and method for controlling band offset and alignment at a crystalline oxide-on-semiconductor interface

DOEpatents

McKee, Rodney A.; Walker, Frederick J.

2003-11-25

A crystalline oxide-on-semiconductor structure and a process for constructing the structure involves a substrate of silicon, germanium or a silicon-germanium alloy and an epitaxial thin film overlying the surface of the substrate wherein the thin film consists of a first epitaxial stratum of single atomic plane layers of an alkaline earth oxide designated generally as (AO).sub.n and a second stratum of single unit cell layers of an oxide material designated as (A'BO.sub.3).sub.m so that the multilayer film arranged upon the substrate surface is designated (AO).sub.n (A'BO.sub.3).sub.m wherein n is an integer repeat of single atomic plane layers of the alkaline earth oxide AO and m is an integer repeat of single unit cell layers of the A'BO.sub.3 oxide material. Within the multilayer film, the values of n and m have been selected to provide the structure with a desired electrical structure at the substrate/thin film interface that can be optimized to control band offset and alignment.

A new Pb{sup II}(ethylenediaminetetraacetate) coordination polymer with a two-dimensional layer structure

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

Zhao, D., E-mail: iamzd@hpu.edu.cn; Zhang, R. H.; Li, F. F.

2016-12-15

A new Pb{sup II}−edta{sup 4–} coordination polymer, Pb{sub 2}(edta)(H{sub 2}O){sub 0.76} (edta{sup 4–} = ethylenediaminetetraacetate) was synthesized under hydrothermal condition. Single crystal X-ray analysis reveals that it represents a novel two-dimensional (2D) Pb{sup 2+}–edta{sup 4–} layer structure with a (4,8{sup 2})-topology. Each edta{sup 4–} ligand employs its four carboxylate O and two N atoms to chelate one Pb{sup II} atom (hexa-coordinated) and connects five Pb{sup II} atoms (ennea-coordinated) via its four carboxylate groups to form 2D layer framework. Adjacent layers are packed into the overall structure through vander Waals interactions.

Towards ALD thin film stabilized single-atom Pd 1 catalysts

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

Piernavieja-Hermida, Mar; Lu, Zheng; White, Anderson

Supported precious metal single-atom catalysts have shown interesting activity and selectivity in recent studies. However, agglomeration of these highly mobile mononuclear surface species can eliminate their unique catalytic properties. In this paper, we study a strategy for synthesizing thin film stabilized single-atom Pd 1 catalysts using atomic layer deposition (ALD). The thermal stability of the Pd 1 catalysts is significantly enhanced by creating a nanocavity thin film structure. In situ infrared spectroscopy and Pd K-edge X-ray absorption spectroscopy (XAS) revealed that the Pd 1 was anchored on the surface through chlorine sites. The thin film stabilized Pd 1 catalysts weremore » thermally stable under both oxidation and reduction conditions. The catalytic performance in the methanol decomposition reaction is found to depend on the thickness of protecting layers. While Pd 1 catalysts showed promising activity at low temperature in a methanol decomposition reaction, 14 cycle TiO 2 protected Pd 1 was less active at high temperature. Pd L 3 edge XAS indicated that the low reactivity compared with Pd nanoparticles is due to the strong adsorption of carbon monoxide even at 250 °C. Lastly, these results clearly show that the ALD nanocavities provide a basis for future design of single-atom catalysts that are highly efficient and stable.« less

Towards ALD thin film stabilized single-atom Pd 1 catalysts

DOE PAGES

Piernavieja-Hermida, Mar; Lu, Zheng; White, Anderson; ...

2016-07-27

Supported precious metal single-atom catalysts have shown interesting activity and selectivity in recent studies. However, agglomeration of these highly mobile mononuclear surface species can eliminate their unique catalytic properties. In this paper, we study a strategy for synthesizing thin film stabilized single-atom Pd 1 catalysts using atomic layer deposition (ALD). The thermal stability of the Pd 1 catalysts is significantly enhanced by creating a nanocavity thin film structure. In situ infrared spectroscopy and Pd K-edge X-ray absorption spectroscopy (XAS) revealed that the Pd 1 was anchored on the surface through chlorine sites. The thin film stabilized Pd 1 catalysts weremore » thermally stable under both oxidation and reduction conditions. The catalytic performance in the methanol decomposition reaction is found to depend on the thickness of protecting layers. While Pd 1 catalysts showed promising activity at low temperature in a methanol decomposition reaction, 14 cycle TiO 2 protected Pd 1 was less active at high temperature. Pd L 3 edge XAS indicated that the low reactivity compared with Pd nanoparticles is due to the strong adsorption of carbon monoxide even at 250 °C. Lastly, these results clearly show that the ALD nanocavities provide a basis for future design of single-atom catalysts that are highly efficient and stable.« less

Synthesis of millimeter-scale transition metal dichalcogenides single crystals

DOE PAGES

Gong, Yongji; Ye, Gonglan; Lei, Sidong; ...

2016-02-10

The emergence of semiconducting transition metal dichalcogenide (TMD) atomic layers has opened up unprecedented opportunities in atomically thin electronics. Yet the scalable growth of TMD layers with large grain sizes and uniformity has remained very challenging. Here is reported a simple, scalable chemical vapor deposition approach for the growth of MoSe2 layers is reported, in which the nucleation density can be reduced from 105 to 25 nuclei cm -2, leading to millimeter-scale MoSe 2 single crystals as well as continuous macrocrystalline films with millimeter size grains. The selective growth of monolayers and multilayered MoSe2 films with well-defined stacking orientation canmore » also be controlled via tuning the growth temperature. In addition, periodic defects, such as nanoscale triangular holes, can be engineered into these layers by controlling the growth conditions. The low density of grain boundaries in the films results in high average mobilities, around ≈42 cm 2 V -1 s -1, for back-gated MoSe 2 transistors. This generic synthesis approach is also demonstrated for other TMD layers such as millimeter-scale WSe 2 single crystals.« less

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

NASA Astrophysics Data System (ADS)

Muthusubramanian, N.; Galan, E.; Maity, C.; Eelkema, R.; Grozema, F. C.; van der Zant, H. S. J.

2016-07-01

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 Al2O3 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 10-4 G0 (1 G0 = 77 μS), where single-molecule conductances are commonly observed. The insulated devices were used to measure the conductance of an amphiphilic oligophenylene ethynylene derivative in deionized water.

Enhancement of resistive switching properties in Al2O3 bilayer-based atomic switches: multilevel resistive switching.

PubMed

Vishwanath, Sujaya Kumar; Woo, Hyunsuk; Jeon, Sanghun

2018-06-08

Atomic switches are considered to be building blocks for future non-volatile data storage and internet of things. However, obtaining device structures capable of ultrahigh density data storage, high endurance, and long data retention, and more importantly, understanding the switching mechanisms are still a challenge for atomic switches. Here, we achieved improved resistive switching performance in a bilayer structure containing aluminum oxide, with an oxygen-deficient oxide as the top switching layer and stoichiometric oxide as the bottom switching layer, using atomic layer deposition. This bilayer device showed a high on/off ratio (10 5 ) with better endurance (∼2000 cycles) and longer data retention (10 4 s) than single-oxide layers. In addition, depending on the compliance current, the bilayer device could be operated in four different resistance states. Furthermore, the depth profiles of the hourglass-shaped conductive filament of the bilayer device was observed by conductive atomic force microscopy.

Prediction of a new graphenelike Si2BN solid

NASA Astrophysics Data System (ADS)

Andriotis, Antonis N.; Richter, Ernst; Menon, Madhu

2016-02-01

While the possibility to create a single-atom-thick two-dimensional layer from any material remains, only a few such structures have been obtained other than graphene and a monolayer of boron nitride. Here, based upon ab initio theoretical simulations, we propose a new stable graphenelike single-atomic-layer Si2BN structure that has all of its atoms with s p2 bonding with no out-of-plane buckling. The structure is found to be metallic with a finite density of states at the Fermi level. This structure can be rolled into nanotubes in a manner similar to graphene. Combining first- and second-row elements in the Periodic Table to form a one-atom-thick material that is also flat opens up the possibility for studying new physics beyond graphene. The presence of Si will make the surface more reactive and therefore a promising candidate for hydrogen storage.

Evidence of a reduction reaction of oxidized iron/cobalt by boron atoms diffused toward naturally oxidized surface of CoFeB layer during annealing

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

Sato, Soshi, E-mail: sato.soshi@cies.tohoku.ac.jp; Honjo, Hiroaki; Niwa, Masaaki

2015-04-06

We have investigated the redox reaction on the surface of Ta/CoFeB/MgO/CoFeB magnetic tunnel junction stack samples after annealing at 300, 350, and 400 °C for 1 h using angle-resolved X-ray photoelectron spectroscopy for precise analysis of the chemical bonding states. At a capping tantalum layer thickness of 1 nm, both the capping tantalum layer and the surface of the underneath CoFeB layer in the as-deposited stack sample were naturally oxidized. By comparison of the Co 2p and Fe 2p spectra among the as-deposited and annealed samples, reduction of the naturally oxidized cobalt and iron atoms occurred on the surface of the CoFeB layer.more » The reduction reaction was more significant at higher annealing temperature. Oxidized cobalt and iron were reduced by boron atoms that diffused toward the surface of the top CoFeB layer. A single CoFeB layer was prepared on SiO{sub 2}, and a confirmatory evidence of the redox reaction with boron diffusion was obtained by angle-resolved X-ray photoelectron spectroscopy analysis of the naturally oxidized surface of the CoFeB single layer after annealing. The redox reaction is theoretically reasonable based on the Ellingham diagram.« less

A Nanoindentation Study of the Plastic Deformation and Fracture Mechanisms in Single-Crystalline CaFe2As2

NASA Astrophysics Data System (ADS)

Frawley, Keara G.; Bakst, Ian; Sypek, John T.; Vijayan, Sriram; Weinberger, Christopher R.; Canfield, Paul C.; Aindow, Mark; Lee, Seok-Woo

2018-04-01

The plastic deformation and fracture mechanisms in single-crystalline CaFe2As2 has been studied using nanoindentation and density functional theory simulations. CaFe2As2 single crystals were grown in a Sn-flux, resulting in homogeneous and nearly defect-free crystals. Nanoindentation along the [001] direction produces strain bursts, radial cracking, and lateral cracking. Ideal cleavage simulations along the [001] and [100] directions using density functional theory calculations revealed that cleavage along the [001] direction requires a much lower stress than cleavage along the [100] direction. This strong anisotropy of cleavage strength implies that CaFe2As2 has an atomic-scale layered structure, which typically exhibits lateral cracking during nanoindentation. This special layered structure results from weak atomic bonding between the (001) Ca and Fe2As2 layers.

A Nanoindentation Study of the Plastic Deformation and Fracture Mechanisms in Single-Crystalline CaFe 2As 2

DOE PAGES

Frawley, Keara G.; Bakst, Ian; Sypek, John T.; ...

2018-04-10

In this paper, the plastic deformation and fracture mechanisms in single-crystalline CaFe 2As 2 has been studied using nanoindentation and density functional theory simulations. CaFe 2As 2 single crystals were grown in a Sn-flux, resulting in homogeneous and nearly defect-free crystals. Nanoindentation along the [001] direction produces strain bursts, radial cracking, and lateral cracking. Ideal cleavage simulations along the [001] and [100] directions using density functional theory calculations revealed that cleavage along the [001] direction requires a much lower stress than cleavage along the [100] direction. This strong anisotropy of cleavage strength implies that CaFe 2As 2 has an atomic-scalemore » layered structure, which typically exhibits lateral cracking during nanoindentation. This special layered structure results from weak atomic bonding between the (001) Ca and Fe 2As 2 layers.« less

A Nanoindentation Study of the Plastic Deformation and Fracture Mechanisms in Single-Crystalline CaFe 2As 2

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

Frawley, Keara G.; Bakst, Ian; Sypek, John T.

In this paper, the plastic deformation and fracture mechanisms in single-crystalline CaFe 2As 2 has been studied using nanoindentation and density functional theory simulations. CaFe 2As 2 single crystals were grown in a Sn-flux, resulting in homogeneous and nearly defect-free crystals. Nanoindentation along the [001] direction produces strain bursts, radial cracking, and lateral cracking. Ideal cleavage simulations along the [001] and [100] directions using density functional theory calculations revealed that cleavage along the [001] direction requires a much lower stress than cleavage along the [100] direction. This strong anisotropy of cleavage strength implies that CaFe 2As 2 has an atomic-scalemore » layered structure, which typically exhibits lateral cracking during nanoindentation. This special layered structure results from weak atomic bonding between the (001) Ca and Fe 2As 2 layers.« less

Catalytic activity of Pd-doped Cu nanoparticles for hydrogenation as a single-atom-alloy catalyst.

PubMed

Cao, Xinrui; Fu, Qiang; Luo, Yi

2014-05-14

The single atom alloy of extended surfaces is known to provide remarkably enhanced catalytic performance toward heterogeneous hydrogenation. Here we demonstrate from first principles calculations that this approach can be extended to nanostructures, such as bimetallic nanoparticles. The catalytic properties of the single-Pd-doped Cu55 nanoparticles have been systemically examined for H2 dissociation as well as H atom adsorption and diffusion, following the concept of single atom alloy. It is found that doping a single Pd atom at the edge site of the Cu55 shell can considerably reduce the activation energy of H2 dissociation, while the single Pd atom doped at the top site or in the inner layers is much less effective. The H atom adsorption on Cu55 is slightly stronger than that on the Cu(111) surface; however, a larger nanoparticle that contains 147 atoms could effectively recover the weak binding of the H atoms. We have also investigated the H atom diffusion on the 55-atom nanoparticle and found that spillover of the produced H atoms could be a feasible process due to the low diffusion barriers. Our results have demonstrated that facile H2 dissociation and weak H atom adsorption could be combined at the nanoscale. Moreover, the effects of doping one more Pd atom on the H2 dissociation and H atom adsorption have also been investigated. We have found that both the doping Pd atoms in the most stable configuration could independently exhibit their catalytic activity, behaving as two single-atom-alloy catalysts.

Platinum single-atom and cluster catalysis of the hydrogen evolution reaction

NASA Astrophysics Data System (ADS)

Cheng, Niancai; Stambula, Samantha; Wang, Da; Banis, Mohammad Norouzi; Liu, Jian; Riese, Adam; Xiao, Biwei; Li, Ruying; Sham, Tsun-Kong; Liu, Li-Min; Botton, Gianluigi A.; Sun, Xueliang

2016-11-01

Platinum-based catalysts have been considered the most effective electrocatalysts for the hydrogen evolution reaction in water splitting. However, platinum utilization in these electrocatalysts is extremely low, as the active sites are only located on the surface of the catalyst particles. Downsizing catalyst nanoparticles to single atoms is highly desirable to maximize their efficiency by utilizing nearly all platinum atoms. Here we report on a practical synthesis method to produce isolated single platinum atoms and clusters using the atomic layer deposition technique. The single platinum atom catalysts are investigated for the hydrogen evolution reaction, where they exhibit significantly enhanced catalytic activity (up to 37 times) and high stability in comparison with the state-of-the-art commercial platinum/carbon catalysts. The X-ray absorption fine structure and density functional theory analyses indicate that the partially unoccupied density of states of the platinum atoms' 5d orbitals on the nitrogen-doped graphene are responsible for the excellent performance.

Platinum single-atom and cluster catalysis of the hydrogen evolution reaction

PubMed Central

Cheng, Niancai; Stambula, Samantha; Wang, Da; Banis, Mohammad Norouzi; Liu, Jian; Riese, Adam; Xiao, Biwei; Li, Ruying; Sham, Tsun-Kong; Liu, Li-Min; Botton, Gianluigi A.; Sun, Xueliang

2016-01-01

Platinum-based catalysts have been considered the most effective electrocatalysts for the hydrogen evolution reaction in water splitting. However, platinum utilization in these electrocatalysts is extremely low, as the active sites are only located on the surface of the catalyst particles. Downsizing catalyst nanoparticles to single atoms is highly desirable to maximize their efficiency by utilizing nearly all platinum atoms. Here we report on a practical synthesis method to produce isolated single platinum atoms and clusters using the atomic layer deposition technique. The single platinum atom catalysts are investigated for the hydrogen evolution reaction, where they exhibit significantly enhanced catalytic activity (up to 37 times) and high stability in comparison with the state-of-the-art commercial platinum/carbon catalysts. The X-ray absorption fine structure and density functional theory analyses indicate that the partially unoccupied density of states of the platinum atoms' 5d orbitals on the nitrogen-doped graphene are responsible for the excellent performance. PMID:27901129

Atomic layer MoS2-graphene van der Waals heterostructure nanomechanical resonators.

PubMed

Ye, Fan; Lee, Jaesung; Feng, Philip X-L

2017-11-30

Heterostructures play significant roles in modern semiconductor devices and micro/nanosystems in a plethora of applications in electronics, optoelectronics, and transducers. While state-of-the-art heterostructures often involve stacks of crystalline epi-layers each down to a few nanometers thick, the intriguing limit would be hetero-atomic-layer structures. Here we report the first experimental demonstration of freestanding van der Waals heterostructures and their functional nanomechanical devices. By stacking single-layer (1L) MoS 2 on top of suspended single-, bi-, tri- and four-layer (1L to 4L) graphene sheets, we realize an array of MoS 2 -graphene heterostructures with varying thickness and size. These heterostructures all exhibit robust nanomechanical resonances in the very high frequency (VHF) band (up to ∼100 MHz). We observe that fundamental-mode resonance frequencies of the heterostructure devices fall between the values of graphene and MoS 2 devices. Quality (Q) factors of heterostructure resonators are lower than those of graphene but comparable to those of MoS 2 devices, suggesting interface damping related to interlayer interactions in the van der Waals heterostructures. This study validates suspended atomic layer heterostructures as an effective device platform and provides opportunities for exploiting mechanically coupled effects and interlayer interactions in such devices.

TiS2 and ZrS2 single- and double-wall nanotubes: first-principles study.

PubMed

Bandura, Andrei V; Evarestov, Robert A

2014-02-15

Hybrid density functional theory has been applied for investigations of the electronic and atomic structure of bulk phases, nanolayers, and nanotubes based on titanium and zirconium disulfides. Calculations have been performed on the basis of the localized atomic functions by means of the CRYSTAL-2009 computer code. The full optimization of all atomic positions in the regarded systems has been made to study the atomic relaxation and to determine the most favorable structures. The different layered and isotropic bulk phases have been considered as the possible precursors of the nanotubes. Calculations on single-walled TiS2 and ZrS2 nanotubes confirmed that the nanotubes obtained by rolling up the hexagonal crystalline layers with octahedral 1T morphology are the most stable. The strain energy of TiS2 and ZrS2 nanotubes is small, does not depend on the tube chirality, and approximately obeys to D(-2) law (D is nanotube diameter) of the classical elasticity theory. It is greater than the strain energy of the similar TiO2 and ZrO2 nanotubes; however, the formation energy of the disulfide nanotubes is considerably less than the formation energy of the dioxide nanotubes. The distance and interaction energy between the single-wall components of the double-wall nanotubes is proved to be close to the distance and interaction energy between layers in the layered crystals. Analysis of the relaxed nanotube shape using radial coordinate of the metal atoms demonstrates a small but noticeable deviation from completely cylindrical cross-section of the external walls in the armchair-like double-wall nanotubes. Copyright © 2013 Wiley Periodicals, Inc.

Quantitative Subsurface Atomic Structure Fingerprint for 2D Materials and Heterostructures by First-Principles-Calibrated Contact-Resonance Atomic Force Microscopy.

PubMed

Tu, Qing; Lange, Björn; Parlak, Zehra; Lopes, Joao Marcelo J; Blum, Volker; Zauscher, Stefan

2016-07-26

Interfaces and subsurface layers are critical for the performance of devices made of 2D materials and heterostructures. Facile, nondestructive, and quantitative ways to characterize the structure of atomically thin, layered materials are thus essential to ensure control of the resultant properties. Here, we show that contact-resonance atomic force microscopy-which is exquisitely sensitive to stiffness changes that arise from even a single atomic layer of a van der Waals-adhered material-is a powerful experimental tool to address this challenge. A combined density functional theory and continuum modeling approach is introduced that yields sub-surface-sensitive, nanomechanical fingerprints associated with specific, well-defined structure models of individual surface domains. Where such models are known, this information can be correlated with experimentally obtained contact-resonance frequency maps to reveal the (sub)surface structure of different domains on the sample.

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.

Controlling the surface termination of NdGaO3 (110): the role of the gas atmosphere.

PubMed

Cavallaro, Andrea; Harrington, George F; Skinner, Stephen J; Kilner, John A

2014-07-07

In this work the effect of gas atmosphere on the surface termination reconstruction of single crystal NdGaO3 (110) (NGO) during thermal annealing was analyzed. Using Low Energy Ion Scattering (LEIS) it has been possible to study the chemical composition of the first atomic layer of treated NGO single crystal samples. NGO has been analyzed both as-received and after a specific thermal treatment at 1000 °C under different gas fluxes (argon, nitrogen, static air, synthetic air, nitrogen plus 5% hydrogen and wet synthetic air respectively). Thermal annealing of perovskite single crystals, as already reported in the literature, is used to obtain a fully A-cation surface termination. Nevertheless the effect of the gas-atmosphere on this process has not been previously reported. By the use of sequential low energy Ar(+) sputtering combined with the primary ion LEIS analysis, the reconstruction of the outermost atomic layers has allowed the clarification of the mechanism of NGO neodymium surface enrichment. It is proposed that the gallium at the surface is submitted to a reduction/evaporation mechanism caused by low oxygen partial pressure and/or high water pressure in the vector gas. Below the first surface atomic layers of an as-received NGO single-crystal a gallium-rich phase has also been observed.

Atomic Resolution of Calcium and Oxygen Sublattices of Calcite in Ambient Conditions by Atomic Force Microscopy Using qPlus Sensors with Sapphire Tips.

PubMed

Wastl, Daniel S; Judmann, Michael; Weymouth, Alfred J; Giessibl, Franz J

2015-01-01

Characterization and imaging at the atomic scale with atomic force microscopy in biocompatible environments is an ongoing challenge. We demonstrate atomically resolved imaging of the calcite (101̅4) surface plane using stiff quartz cantilevers ("qPlus sensors", stiffness k = 1280 N/m) equipped with sapphire tips in ambient conditions without any surface preparation. With 10 atoms in one surface unit cell, calcite has a highly complex surface structure comprising three different chemical elements (Ca, C, and O). We obtain true atomic resolution of calcite in air at relative humidity ranging from 20% to 40%, imaging atomic steps and single atomic defects. We observe a great durability of sapphire tips with their Mohs hardness of 9, only one step below diamond. Depending on the state of the sapphire tip, we resolve either the calcium or the oxygen sublattice. We determine the tip termination by comparing the experimental images with simulations and discuss the possibility of chemical tip identification in air. The main challenges for imaging arise from the presence of water layers, which form on almost all surfaces and have the potential to dissolve the crystal surface. Frequency shift versus distance spectra show the presence of at least three ordered hydration layers. The measured height of the first hydration layer corresponds well to X-ray diffraction data and molecular dynamic simulations, namely, ∼220 pm. For the following hydration layers we measure ∼380 pm for the second and third layer, ending up in a total hydration layer thickness of at least 1 nm. Understanding the influence of water layers and their structure is important for surface segregation, surface reactions including reconstructions, healing of defects, and corrosion.

Fabrication of low-temperature solid oxide fuel cells with a nanothin protective layer by atomic layer deposition

PubMed Central

2013-01-01

Anode aluminum oxide-supported thin-film fuel cells having a sub-500-nm-thick bilayered electrolyte comprising a gadolinium-doped ceria (GDC) layer and an yttria-stabilized zirconia (YSZ) layer were fabricated and electrochemically characterized in order to investigate the effect of the YSZ protective layer. The highly dense and thin YSZ layer acted as a blockage against electron and oxygen permeation between the anode and GDC electrolyte. Dense GDC and YSZ thin films were fabricated using radio frequency sputtering and atomic layer deposition techniques, respectively. The resulting bilayered thin-film fuel cell generated a significantly higher open circuit voltage of approximately 1.07 V compared with a thin-film fuel cell with a single-layered GDC electrolyte (approximately 0.3 V). PMID:23342963

Piezophototronic Effect in Single-Atomic-Layer MoS2 for Strain-Gated Flexible Optoelectronics.

PubMed

Wu, Wenzhuo; Wang, Lei; Yu, Ruomeng; Liu, Yuanyue; Wei, Su-Huai; Hone, James; Wang, Zhong Lin

2016-10-01

Strain-gated flexible optoelectronics are reported based on monolayer MoS 2 . Utilizing the piezoelectric polarization created at the metal-MoS 2 interface to modulate the separation/transport of photogenerated carriers, the piezophototronic effect is applied to implement atomic-layer-thick phototransistor. Coupling between piezoelectricity and photogenerated carriers may enable the development of novel optoelectronics. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Large Area Atomically Flat Surfaces via Exfoliation of Bulk Bi 2Se 3 Single Crystals

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

Melamed, Celeste L.; Ortiz, Brenden R.; Gorai, Prashun

In this paper, we present an exfoliation method that produces cm 2-area atomically flat surfaces from bulk layered single crystals, with broad applications such as for the formation of lateral heterostructures and for use as substrates for van der Waals epitaxy. Single crystals of Bi 2Se 3 were grown using the Bridgman method and examined with X-ray reciprocal space maps, Auger spectroscopy, low-energy electron diffraction, and X-ray photoelectron spectroscopy. An indium-bonding exfoliation technique was developed that produces multiple ~100 um thick atomically flat, macroscopic (>1 cm 2) slabs from each Bi 2Se 3 source crystal. Two-dimensional X-ray diffraction and reciprocalmore » space maps confirm the high crystalline quality of the exfoliated surfaces. Atomic force microscopy reveals that the exfoliated surfaces have an average root-mean-square (RMS) roughness of ~0.04 nm across 400 μm 2 scans and an average terrace width of 70 um between step edges. First-principles calculations reveal exfoliation energies of Bi 2Se 3 and a number of other layered compounds, which demonstrate relevance of our method across the field of 2D materials. While many potential applications exist, excellent lattice matching with the III-V alloy space suggests immediate potential for the use of these exfoliated layered materials as epitaxial substrates for photovoltaic development.« less

Large Area Atomically Flat Surfaces via Exfoliation of Bulk Bi 2Se 3 Single Crystals

DOE PAGES

Melamed, Celeste L.; Ortiz, Brenden R.; Gorai, Prashun; ...

2017-09-12

In this paper, we present an exfoliation method that produces cm 2-area atomically flat surfaces from bulk layered single crystals, with broad applications such as for the formation of lateral heterostructures and for use as substrates for van der Waals epitaxy. Single crystals of Bi 2Se 3 were grown using the Bridgman method and examined with X-ray reciprocal space maps, Auger spectroscopy, low-energy electron diffraction, and X-ray photoelectron spectroscopy. An indium-bonding exfoliation technique was developed that produces multiple ~100 um thick atomically flat, macroscopic (>1 cm 2) slabs from each Bi 2Se 3 source crystal. Two-dimensional X-ray diffraction and reciprocalmore » space maps confirm the high crystalline quality of the exfoliated surfaces. Atomic force microscopy reveals that the exfoliated surfaces have an average root-mean-square (RMS) roughness of ~0.04 nm across 400 μm 2 scans and an average terrace width of 70 um between step edges. First-principles calculations reveal exfoliation energies of Bi 2Se 3 and a number of other layered compounds, which demonstrate relevance of our method across the field of 2D materials. While many potential applications exist, excellent lattice matching with the III-V alloy space suggests immediate potential for the use of these exfoliated layered materials as epitaxial substrates for photovoltaic development.« less

Adsorption, hydrogenation and dehydrogenation of C2H on a CoCu bimetallic layer

NASA Astrophysics Data System (ADS)

Wu, Donghai; Yuan, Jinyun; Yang, Baocheng; Chen, Houyang

2018-05-01

In this paper, adsorption, hydrogenation and dehydrogenation of C2H on a single atomic layer of bimetallic CoCu were investigated using first-principles calculations. The CoCu bimetallic layer is formed by Cu replacement of partial Co atoms on the top layer of a Co(111) surface. Our adsorption and reaction results showed those sites, which have stronger adsorption energy of C2H, possess higher reactivity. The bimetallic layer possesses higher reactivity than either of the pure monometallic layer. A mechanism of higher reactivity of the bimetallic layer is proposed and identified, i.e. in the bimetallic catalyst, the catalytic performance of one component is promoted by the second component, and in our work, the catalytic performance of Co atoms in the bimetallic layer are improved by introducing Cu atoms, lowing the activation barrier of the reaction of C2H. The bimetallic layer could tune adsorption and reaction of C2H by modulating the ratio of Co and Cu. Results of adsorption energies and adsorption configurations reveal that C2H prefers to be adsorbed in parallel on both the pure Co metallic and CoCu bimetallic layers, and Co atoms in subsurface which support the metallic or bimetallic layer have little effect on C2H adsorption. For hydrogenation reactions, the products greatly depend on the concentration and initial positions of hydrogen atoms, and the C2H hydrogenation forming acetylene is more favorable than forming vinylidene in both thermodynamics and kinetics. This study would provide fundamental guidance for hydrocarbon reactions on Co-based and/or Cu-based bimetallic surface chemistry and for development of new bimetallic catalysts.

Large scale atomistic simulation of single-layer graphene growth on Ni(111) surface: molecular dynamics simulation based on a new generation of carbon-metal potential

NASA Astrophysics Data System (ADS)

Xu, Ziwei; Yan, Tianying; Liu, Guiwu; Qiao, Guanjun; Ding, Feng

2015-12-01

To explore the mechanism of graphene chemical vapor deposition (CVD) growth on a catalyst surface, a molecular dynamics (MD) simulation of carbon atom self-assembly on a Ni(111) surface based on a well-designed empirical reactive bond order potential was performed. We simulated single layer graphene with recorded size (up to 300 atoms per super-cell) and reasonably good quality by MD trajectories up to 15 ns. Detailed processes of graphene CVD growth, such as carbon atom dissolution and precipitation, formation of carbon chains of various lengths, polygons and small graphene domains were observed during the initial process of the MD simulation. The atomistic processes of typical defect healing, such as the transformation from a pentagon into a hexagon and from a pentagon-heptagon pair (5|7) to two adjacent hexagons (6|6), were revealed as well. The study also showed that higher temperature and longer annealing time are essential to form high quality graphene layers, which is in agreement with experimental reports and previous theoretical results.To explore the mechanism of graphene chemical vapor deposition (CVD) growth on a catalyst surface, a molecular dynamics (MD) simulation of carbon atom self-assembly on a Ni(111) surface based on a well-designed empirical reactive bond order potential was performed. We simulated single layer graphene with recorded size (up to 300 atoms per super-cell) and reasonably good quality by MD trajectories up to 15 ns. Detailed processes of graphene CVD growth, such as carbon atom dissolution and precipitation, formation of carbon chains of various lengths, polygons and small graphene domains were observed during the initial process of the MD simulation. The atomistic processes of typical defect healing, such as the transformation from a pentagon into a hexagon and from a pentagon-heptagon pair (5|7) to two adjacent hexagons (6|6), were revealed as well. The study also showed that higher temperature and longer annealing time are essential to form high quality graphene layers, which is in agreement with experimental reports and previous theoretical results. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr06016h

An assessment of memristor intrinsic fluctuations: a measurement of single atomic motion

NASA Astrophysics Data System (ADS)

Borghetti, Julien; Yang, J. Joshua; Medeiros-Ribeiro, Gilberto; Williams, R. Stanley

2010-03-01

Memristors provides electrically tunable resistance for upcoming non-volatile memory and future neuromorphic computing. One of the key benefits of such a device is its scalability, which can be demonstrated from an architectural perspective as well as from a fundamental physics limit. 4D addressing schemes utilizing cross bar structures that can be stacked several layers high above the chip embodies unlimited addressing space. On the other limit, the basic operating principles of memristive devices allow one to reach storage of information in a single atom. In this report of nanoscale (sub 50nm) devices, we detect single atom fluctuations, which would then represent the ultimate limit for noise sources thus delineating the boundary conditions for circuit design. We show that electrically induced individual atom migrations do not affect the overall device atomic configuration until a critical bias where a single local fluctuation triggers a general atomic reconfiguration. This instability illustrates the robustness of the device non-volatility upon small electrical stress.

Large-Area WS2 Film with Big Single Domains Grown by Chemical Vapor Deposition

NASA Astrophysics Data System (ADS)

Liu, Pengyu; Luo, Tao; Xing, Jie; Xu, Hong; Hao, Huiying; Liu, Hao; Dong, Jingjing

2017-10-01

High-quality WS2 film with the single domain size up to 400 μm was grown on Si/SiO2 wafer by atmospheric pressure chemical vapor deposition. The effects of some important fabrication parameters on the controlled growth of WS2 film have been investigated in detail, including the choice of precursors, tube pressure, growing temperature, holding time, the amount of sulfur powder, and gas flow rate. By optimizing the growth conditions at one atmospheric pressure, we obtained tungsten disulfide single domains with an average size over 100 μm. Raman spectra, atomic force microscopy, and transmission electron microscopy provided direct evidence that the WS2 film had an atomic layer thickness and a single-domain hexagonal structure with a high crystal quality. And the photoluminescence spectra indicated that the tungsten disulfide films showed an evident layer-number-dependent fluorescence efficiency, depending on their energy band structure. Our study provides an important experimental basis for large-area, controllable preparation of atom-thick tungsten disulfide thin film and can also expedite the development of scalable high-performance optoelectronic devices based on WS2 film.

Tuning negative differential resistance in single-atomic layer boron-silicon sheets

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

Zhou, Ming-Yue; Liu, Chun-Sheng, E-mail: csliu@njupt.edu.cn, E-mail: yanxh@njupt.edu.cn; Key Laboratory of Radio Frequency and Micro-Nano Electronics of Jiangsu Province, Nanjing 210023, Jiangsu

2015-03-21

Using density functional theory and nonequilibrium Green's function formalism for quantum transport calculation, we have quantified the ballistic transport properties along different directions in two-dimensional boron-silicon (B-Si) compounds, as well as the current response to bias voltage. The conductance of the most B-Si devices is higher than the conductance of one-atom-thick boron and silicene. Furthermore, the negative differential resistance phenomenon can be found at certain B-Si stoichiometric composition, and it occurs at various bias voltages. Also, the peak-to-valley ratio is sensitive to the B-Si composition and dependent of the direction considered for B-Si monolayers. The present findings could be helpfulmore » for applications of the single-atomic layer B-Si sheets in the field of semiconductor devices or low-dimensional electronic devices.« less

Magnetic spherical cores partly coated with periodic mesoporous organosilica single crystals.

PubMed

Li, Jing; Wei, Yong; Li, Wei; Deng, Yonghui; Zhao, Dongyuan

2012-03-07

Core-shell structured materials are of special significance in various applications. Until now, most reported core-shell structures have polycrystalline or amorphous coatings as their shell layers, with popular morphologies of microspheres or quasi-spheres. However, the single crystals, either mesoscale or atomic ones, are still rarely reported as shell layers. If single crystals can be coated on core materials, it would result in a range of new type core-shell structures with various morphologies, and probably more potential applications. In this work, we demonstrate that periodic mesoporous organosilica (PMO) single crystals can partly grow on magnetic microspheres to form incomplete Fe(3)O(4)@nSiO(2)@PMO core-shell materials in aqueous solution, which indeed is the first illustration that mesoporous single-crystal materials can be used as shell layers for preparation of core-shell materials. The achieved materials have advantages of high specific surface areas, good magnetic responses, embedded functional groups and cubic mesopore channels, which might provide them with various application conveniences. We suppose the partial growth is largely decided by the competition between growing tendency of single crystals and the resistances to this tendency. In principle, other single crystals, including a range of atomic single crystals, such as zeolites, are able to be developed into such core-shell structures.

Protection layers on a superconducting microwave resonator toward a hybrid quantum system

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

Lee, Jongmin, E-mail: jongmin.lee@sandia.gov; Sandia National Laboratories, Albuquerque, New Mexico 87123; Park, Dong Hun, E-mail: leomac@umd.edu

2015-10-07

We propose a protection scheme of a superconducting microwave resonator to realize a hybrid quantum system, where cold neutral atoms are coupled with a single microwave photon through magnetic dipole interaction at an interface inductor. The evanescent field atom trap, such as a waveguide/nanofiber atom trap, brings both surface-scattered photons and absorption-induced broadband blackbody radiation which result in quasiparticles and a low quality factor at the resonator. A proposed multiband protection layer consists of pairs of two dielectric layers and a thin nanogrid conductive dielectric layer above the interface inductor. We show numerical simulations of quality factors and reflection/absorption spectra,more » indicating that the proposed multilayer structure can protect a lumped-element microwave resonator from optical photons and blackbody radiation while maintaining a reasonably high quality factor.« less

Computational discovery of ferromagnetic semiconducting single-layer CrSnTe 3

DOE PAGES

Zhuang, Houlong L.; Xie, Yu; Kent, P. R. C.; ...

2015-07-06

Despite many single-layer materials being reported in the past decade, few of them exhibit magnetism. Here we perform first-principles calculations using accurate hybrid density functional methods (HSE06) to predict that single-layer CrSnTe 3 (CST) is a ferromagnetic semiconductor, with band gaps of 0.9 and 1.2 eV for the majority and minority spin channels, respectively. We determine the Curie temperature as 170 K, significantly higher than that of single-layer CrSiTe 3 (90K) and CrGeTe 3 (130 K). This is due to the enhanced ionicity of the Sn-Te bond, which in turn increases the superexchange coupling between the magnetic Cr atoms. Wemore » further explore the mechanical and dynamical stability and strain response of this single-layer material for possible epitaxial growth. Lastly, our study provides an intuitive approach to understand and design novel single-layer magnetic semiconductors for a wide range of spintronics and energy applications.« less

Multivariate statistical characterization of charged and uncharged domain walls in multiferroic hexagonal YMnO3 single crystal visualized by a spherical aberration-corrected STEM.

PubMed

Matsumoto, Takao; Ishikawa, Ryo; Tohei, Tetsuya; Kimura, Hideo; Yao, Qiwen; Zhao, Hongyang; Wang, Xiaolin; Chen, Dapeng; Cheng, Zhenxiang; Shibata, Naoya; Ikuhara, Yuichi

2013-10-09

A state-of-the-art spherical aberration-corrected STEM was fully utilized to directly visualize the multiferroic domain structure in a hexagonal YMnO3 single crystal at atomic scale. With the aid of multivariate statistical analysis (MSA), we obtained unbiased and quantitative maps of ferroelectric domain structures with atomic resolution. Such a statistical image analysis of the transition region between opposite polarizations has confirmed atomically sharp transitions of ferroelectric polarization both in antiparallel (uncharged) and tail-to-tail 180° (charged) domain boundaries. Through the analysis, a correlated subatomic image shift of Mn-O layers with that of Y layers, exhibiting a double-arc shape of reversed curvatures, have been elucidated. The amount of image shift in Mn-O layers along the c-axis is statistically significant as small as 0.016 nm, roughly one-third of the evident image shift of 0.048 nm in Y layers. Interestingly, a careful analysis has shown that such a subatomic image shift in Mn-O layers vanishes at the tail-to-tail 180° domain boundaries. Furthermore, taking advantage of the annular bright field (ABF) imaging technique combined with MSA, the tilting of MnO5 bipyramids, the very core mechanism of multiferroicity of the material, is evaluated.

Electronic structure studies of a clock-reconstructed Al/Pd(1 0 0) surface alloy

NASA Astrophysics Data System (ADS)

Kirsch, Janet E.; Tainter, Craig J.

We have employed solid-state Fenske-Hall band structure calculations to examine the electronic structure of Al/Pd(1 0 0), a surface alloy that undergoes a reconstruction, or rearrangement, of the atoms in the top few surface layers. Surface alloys are materials that consist primarily of a single elemental metal, but which have a bimetallic surface composition that is only a few atomic layers in thickness. The results of this study indicate that reconstruction into a clock configuration simultaneously optimizes the intralayer bonding within the surface plane and the bonding between the first and second atomic layers. These results also allow us to examine the fundamental relationship between the electronic and physical structures of this reconstructed surface alloy.

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.

Single-crystalline monolayer and multilayer graphene nano switches

NASA Astrophysics Data System (ADS)

Li, Peng; Jing, Gaoshan; Zhang, Bo; Sando, Shota; Cui, Tianhong

2014-03-01

Growth of monolayer, bi-layer, and tri-layer single-crystalline graphene (SCG) using chemical vapor deposition method is reported. SCG's mechanical properties and single-crystalline nature were characterized and verified by atomic force microscope and Raman spectroscopy. Electro-mechanical switches based on mono- and bi-layer SCG were fabricated, and the superb properties of SCG enable the switches to operate at pull-in voltage as low as 1 V, and high switching speed about 100 ns. These devices exhibit lifetime without a breakdown of over 5000 cycles, far more durable than any other graphene nanoelectromechanical system switches reported.

Single-crystalline monolayer and multilayer graphene nano switches

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

Li, Peng; Cui, Tianhong, E-mail: tcui@me.umn.edu; Department of Mechanical Engineering, University of Minnesota, Minneapolis, Minnesota 55455

2014-03-17

Growth of monolayer, bi-layer, and tri-layer single-crystalline graphene (SCG) using chemical vapor deposition method is reported. SCG's mechanical properties and single-crystalline nature were characterized and verified by atomic force microscope and Raman spectroscopy. Electro-mechanical switches based on mono- and bi-layer SCG were fabricated, and the superb properties of SCG enable the switches to operate at pull-in voltage as low as 1 V, and high switching speed about 100 ns. These devices exhibit lifetime without a breakdown of over 5000 cycles, far more durable than any other graphene nanoelectromechanical system switches reported.

Indium droplet formation in InGaN thin films with single and double heterojunctions prepared by MOCVD

PubMed Central

2014-01-01

Indium gallium nitride (InGaN) samples with single heterojunction (SH) and double heterojunction (DH) were prepared using metal-organic chemical vapor deposition. SH has a layer of InGaN thin film (thicknesses, 25, 50, 100, and 200 nm) grown on an uGaN film (thickness, 2 μm). The DH samples are distinguished by DH uGaN film (thickness, 120 nm) grown on the InGaN layer. Reciprocal space mapping measurements reveal that the DH samples are fully strained with different thicknesses, whereas the strain in the SH samples are significantly relaxed with the increasing thickness of the InGaN film. Scanning electron microscopy results show that the surface roughness of the sample increases when the sample is relaxed. High-resolution transmission electron microscopy images of the structure of indium droplets in the DH sample indicate that the thickness of the InGaN layer decreases with the density of indium droplets. The formation of these droplets is attributed to the insufficient kinetic energy of indium atom to react with the elements of group V, resulting to aggregation. The gallium atoms in the GaN thin film will not be uniformly replaced by indium atoms; the InGaN thin film has an uneven distribution of indium atoms and the quality of the epitaxial layer is degraded. PMID:25024692

Aqueous proton transfer across single-layer graphene

DOE PAGES

Achtyl, Jennifer L.; Unocic, Raymond R.; Xu, Lijun; ...

2015-03-17

Proton transfer across single-layer graphene proceeds with large computed energy barriers and is thought to be unfavourable at room temperature unless nanoscale holes or dopants are introduced, or a potential bias is applied. Here we subject single-layer graphene supported on fused ​silica to cycles of high and low pH, and show that protons transfer reversibly from the aqueous phase through the graphene to the other side where they undergo acid–base chemistry with the silica hydroxyl groups. After ruling out diffusion through macroscopic pinholes, the protons are found to transfer through rare, naturally occurring atomic defects. Computer simulations reveal low energymore » barriers of 0.61–0.75 eV for aqueous proton transfer across hydroxyl-terminated atomic defects that participate in a Grotthuss-type relay, while ​pyrylium-like ether terminations shut down proton exchange. In conclusion, unfavourable energy barriers to helium and ​hydrogen transfer indicate the process is selective for aqueous protons.« less

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

Enhanced Stability of Pt-Cu Single-Atom Alloy Catalysts: In Situ Characterization of the Pt/Cu(111) Surface in an Ambient Pressure of CO

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

Simonovis, Juan Pablo; Hunt, Adrian; Palomino, Robert M.

The interaction between a catalyst and reactants often induce changes in the surface structure and composition of the catalyst, which, in turn, affect its reactivity. Therefore, it is important to study such changes using in situ techniques under well-controlled conditions. We have used ambient pressure X-ray photoelectron spectroscopy (AP-XPS) to study the surface stability of a Pt/Cu(111) single atom alloy (SAA) in an ambient pressure of CO. By directly probing the Pt atoms, we found that CO causes a slight surface segregation of Pt atoms at room temperature. In addition, while the Pt/Cu(111) surface demonstrates poor thermal stability in UHV,more » where surface Pt starts to diffuse to the subsurface layer above 400 K, the presence of adsorbed CO enhances the thermal stability of surface Pt atoms. Furthermore, we also found that temperatures above 450 K cause a restructuring of the subsurface layer, which consequently strengthens the CO binding to the surface Pt sites, likely due to the presence of neighboring subsurface Pt atoms.« less

Enhanced Stability of Pt-Cu Single-Atom Alloy Catalysts: In Situ Characterization of the Pt/Cu(111) Surface in an Ambient Pressure of CO

DOE PAGES

Simonovis, Juan Pablo; Hunt, Adrian; Palomino, Robert M.; ...

2018-02-05

The interaction between a catalyst and reactants often induce changes in the surface structure and composition of the catalyst, which, in turn, affect its reactivity. Therefore, it is important to study such changes using in situ techniques under well-controlled conditions. We have used ambient pressure X-ray photoelectron spectroscopy (AP-XPS) to study the surface stability of a Pt/Cu(111) single atom alloy (SAA) in an ambient pressure of CO. By directly probing the Pt atoms, we found that CO causes a slight surface segregation of Pt atoms at room temperature. In addition, while the Pt/Cu(111) surface demonstrates poor thermal stability in UHV,more » where surface Pt starts to diffuse to the subsurface layer above 400 K, the presence of adsorbed CO enhances the thermal stability of surface Pt atoms. Furthermore, we also found that temperatures above 450 K cause a restructuring of the subsurface layer, which consequently strengthens the CO binding to the surface Pt sites, likely due to the presence of neighboring subsurface Pt atoms.« less

Synthesis, crystal structure and electronic structure of the binary phase Rh2Cd5

NASA Astrophysics Data System (ADS)

Koley, Biplab; Chatterjee, S.; Jana, Partha P.

2017-02-01

A new phase in the Rh-Cd binary system - Rh2Cd5 has been identified and characterized by single crystal X-ray diffraction and Energy dispersive X-ray analysis. The stoichiometric compound Rh2Cd5 crystallizes with a unit cell containing 14 atoms, in the orthorhombic space group Pbam (55). The crystal structure of Rh2Cd5 can be described as a defect form of the In3Pd5 structure with ordered vacancies, formed of two 2D atomic layers with the stacking sequence: ABAB. The A type layers consist of (3.6.3.6)-Kagomé nets of Cd atoms while the B type layers consist of (35) (37)- nets of both Cd and Rh atoms. The stability of this line phase is investigated by first principle electronic structure calculations on the model of ordered Rh2Cd5.

Protecting nickel with graphene spin-filtering membranes: A single layer is enough

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

Martin, M.-B.; Dlubak, B.; Piquemal-Banci, M.

2015-07-06

We report on the demonstration of ferromagnetic spin injectors for spintronics which are protected against oxidation through passivation by a single layer of graphene. The graphene monolayer is directly grown by catalytic chemical vapor deposition on pre-patterned nickel electrodes. X-ray photoelectron spectroscopy reveals that even with its monoatomic thickness, monolayer graphene still efficiently protects spin sources against oxidation in ambient air. The resulting single layer passivated electrodes are integrated into spin valves and demonstrated to act as spin polarizers. Strikingly, the atom-thick graphene layer is shown to be sufficient to induce a characteristic spin filtering effect evidenced through the signmore » reversal of the measured magnetoresistance.« less

New twinning route in face-centered cubic nanocrystalline metals.

PubMed

Wang, Lihua; Guan, Pengfei; Teng, Jiao; Liu, Pan; Chen, Dengke; Xie, Weiyu; Kong, Deli; Zhang, Shengbai; Zhu, Ting; Zhang, Ze; Ma, Evan; Chen, Mingwei; Han, Xiaodong

2017-12-15

Twin nucleation in a face-centered cubic crystal is believed to be accomplished through the formation of twinning partial dislocations on consecutive atomic planes. Twinning should thus be highly unfavorable in face-centered cubic metals with high twin-fault energy barriers, such as Al, Ni, and Pt, but instead is often observed. Here, we report an in situ atomic-scale observation of twin nucleation in nanocrystalline Pt. Unlike the classical twinning route, deformation twinning initiated through the formation of two stacking faults separated by a single atomic layer, and proceeded with the emission of a partial dislocation in between these two stacking faults. Through this route, a three-layer twin was nucleated without a mandatory layer-by-layer twinning process. This route is facilitated by grain boundaries, abundant in nanocrystalline metals, that promote the nucleation of separated but closely spaced partial dislocations, thus enabling an effective bypassing of the high twin-fault energy barrier.

Structural and optical properties of GaAs(100) with a thin surface layer doped with chromium

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

Seredin, P. V., E-mail: paul@phys.vsu.ru; Fedyukin, A. V.; Arsentyev, I. N.

The aim of this study is to explore the structural and optical properties of single-crystal GaAs(100) doped with Cr atoms by burning them into the substrate at high temperatures. The diffusion of chromium into single-crystal GaAs(100) substrates brings about the formation of a thin (~20–40 μm) GaAs:Cr transition layer. In this case, chromium atoms are incorporated into the gallium-arsenide crystal lattice and occupy the regular atomic sites of the metal sublattice. As the chromium diffusion time is increased, such behavior of the dopant impurity yields changes in the energy structure of GaAs, a decrease in the absorption at free chargemore » carriers, and a lowering of the surface recombination rate. As a result, the photoluminescence signal from the sample is significantly enhanced.« less

Reducing interface recombination for Cu(In,Ga)Se{sub 2} by atomic layer deposited buffer layers

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

Hultqvist, Adam; Bent, Stacey F.; Li, Jian V.

2015-07-20

Partial CuInGaSe{sub 2} (CIGS) solar cell stacks with different atomic layer deposited buffer layers and pretreatments were analyzed by photoluminescence (PL) and capacitance voltage (CV) measurements to investigate the buffer layer/CIGS interface. Atomic layer deposited ZnS, ZnO, and SnO{sub x} buffer layers were compared with chemical bath deposited CdS buffer layers. Band bending, charge density, and interface state density were extracted from the CV measurement using an analysis technique new to CIGS. The surface recombination velocity calculated from the density of interface traps for a ZnS/CIGS stack shows a remarkably low value of 810 cm/s, approaching the range of single crystallinemore » II–VI systems. Both the PL spectra and its lifetime depend on the buffer layer; thus, these measurements are not only sensitive to the absorber but also to the absorber/buffer layer system. Pretreatment of the CIGS prior to the buffer layer deposition plays a significant role on the electrical properties for the same buffer layer/CIGS stack, further illuminating the importance of good interface formation. Finally, ZnS is found to be the best performing buffer layer in this study, especially if the CIGS surface is pretreated with potassium cyanide.« less

Reducing interface recombination for Cu(In,Ga)Se 2 by atomic layer deposited buffer layers

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

Hultqvist, Adam; Li, Jian V.; Kuciauskas, Darius

2015-07-20

Partial CuInGaSe2 (CIGS) solar cell stacks with different atomic layer deposited buffer layers and pretreatments were analyzed by photoluminescence (PL) and capacitance voltage (CV) measurements to investigate the buffer layer/CIGS interface. Atomic layer deposited ZnS, ZnO, and SnOx buffer layers were compared with chemical bath deposited CdS buffer layers. Band bending, charge density, and interface state density were extracted from the CV measurement using an analysis technique new to CIGS. The surface recombination velocity calculated from the density of interface traps for a ZnS/CIGS stack shows a remarkably low value of 810 cm/s, approaching the range of single crystalline II-VImore » systems. Both the PL spectra and its lifetime depend on the buffer layer; thus, these measurements are not only sensitive to the absorber but also to the absorber/buffer layer system. Pretreatment of the CIGS prior to the buffer layer deposition plays a significant role on the electrical properties for the same buffer layer/CIGS stack, further illuminating the importance of good interface formation. Finally, ZnS is found to be the best performing buffer layer in this study, especially if the CIGS surface is pretreated with potassium cyanide.« less

Reducing interface recombination for Cu(In,Ga)Se 2 by atomic layer deposited buffer layers

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

Hultqvist, Adam; Li, Jian V.; Kuciauskas, Darius

2015-07-20

Partial CuInGaSe2 (CIGS) solar cell stacks with different atomic layer deposited buffer layers and pretreatments were analyzed by photoluminescence (PL) and capacitance voltage (CV) measurements to investigate the buffer layer/CIGS interface. Atomic layer deposited ZnS, ZnO, and SnOx buffer layers were compared with chemical bath deposited CdS buffer layers. Band bending, charge density, and interface state density were extracted from the CV measurement using an analysis technique new to CIGS. The surface recombination velocity calculated from the density of interface traps for a ZnS/CIGS stack shows a remarkably low value of 810 cm/s, approaching the range of single crystalline II–VImore » systems. Both the PL spectra and its lifetime depend on the buffer layer; thus, these measurements are not only sensitive to the absorber but also to the absorber/buffer layer system. Pretreatment of the CIGS prior to the buffer layer deposition plays a significant role on the electrical properties for the same buffer layer/CIGS stack, further illuminating the importance of good interface formation. Finally, ZnS is found to be the best performing buffer layer in this study, especially if the CIGS surface is pretreated with potassium cyanide.« less

Method of manufacture of atomically thin boron nitride

DOEpatents

Zettl, Alexander K

2013-08-06

The present invention provides a method of fabricating at least one single layer hexagonal boron nitride (h-BN). In an exemplary embodiment, the method includes (1) suspending at least one multilayer boron nitride across a gap of a support structure and (2) performing a reactive ion etch upon the multilayer boron nitride to produce the single layer hexagonal boron nitride suspended across the gap of the support structure. The present invention also provides a method of fabricating single layer hexagonal boron nitride. In an exemplary embodiment, the method includes (1) providing multilayer boron nitride suspended across a gap of a support structure and (2) performing a reactive ion etch upon the multilayer boron nitride to produce the single layer hexagonal boron nitride suspended across the gap of the support structure.

Initial evaluation and comparison of plasma damage to atomic layer carbon materials using conventional and low T{sub e} plasma sources

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

Jagtiani, Ashish V.; Miyazoe, Hiroyuki; Chang, Josephine

2016-01-15

The ability to achieve atomic layer precision is the utmost goal in the implementation of atomic layer etch technology. Carbon-based materials such as carbon nanotubes (CNTs) and graphene are single atomic layers of carbon with unique properties and, as such, represent the ultimate candidates to study the ability to process with atomic layer precision and assess impact of plasma damage to atomic layer materials. In this work, the authors use these materials to evaluate the atomic layer processing capabilities of electron beam generated plasmas. First, the authors evaluate damage to semiconducting CNTs when exposed to beam-generated plasmas and compare thesemore » results against the results using typical plasma used in semiconductor processing. The authors find that the beam generated plasma resulted in significantly lower current degradation in comparison to typical plasmas. Next, the authors evaluated the use of electron beam generated plasmas to process graphene-based devices by functionalizing graphene with fluorine, nitrogen, or oxygen to facilitate atomic layer deposition (ALD). The authors found that all adsorbed species resulted in successful ALD with varying impact on the transconductance of the graphene. Furthermore, the authors compare the ability of both beam generated plasma as well as a conventional low ion energy inductively coupled plasma (ICP) to remove silicon nitride (SiN) deposited on top of the graphene films. Our results indicate that, while both systems can remove SiN, an increase in the D/G ratio from 0.08 for unprocessed graphene to 0.22 to 0.26 for the beam generated plasma, while the ICP yielded values from 0.52 to 1.78. Generally, while some plasma-induced damage was seen for both plasma sources, a much wider process window as well as far less damage to CNTs and graphene was observed when using electron beam generated plasmas.« less

Dimensions and Global Twist of Single-Layer DNA Origami Measured by Small-Angle X-ray Scattering.

PubMed

Baker, Matthew A B; Tuckwell, Andrew J; Berengut, Jonathan F; Bath, Jonathan; Benn, Florence; Duff, Anthony P; Whitten, Andrew E; Dunn, Katherine E; Hynson, Robert M; Turberfield, Andrew J; Lee, Lawrence K

2018-06-04

The rational design of complementary DNA sequences can be used to create nanostructures that self-assemble with nanometer precision. DNA nanostructures have been imaged by atomic force microscopy and electron microscopy. Small-angle X-ray scattering (SAXS) provides complementary structural information on the ensemble-averaged state of DNA nanostructures in solution. Here we demonstrate that SAXS can distinguish between different single-layer DNA origami tiles that look identical when immobilized on a mica surface and imaged with atomic force microscopy. We use SAXS to quantify the magnitude of global twist of DNA origami tiles with different crossover periodicities: these measurements highlight the extreme structural sensitivity of single-layer origami to the location of strand crossovers. We also use SAXS to quantify the distance between pairs of gold nanoparticles tethered to specific locations on a DNA origami tile and use this method to measure the overall dimensions and geometry of the DNA nanostructure in solution. Finally, we use indirect Fourier methods, which have long been used for the interpretation of SAXS data from biomolecules, to measure the distance between DNA helix pairs in a DNA origami nanotube. Together, these results provide important methodological advances in the use of SAXS to analyze DNA nanostructures in solution and insights into the structures of single-layer DNA origami.

Observation of High-Harmonic Generation from an Atomically Thin Semiconductor [Observation of High Harmonics from and Atomically Thin Semiconductor

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

Liu, Hanzhe; Li, Yilei; You, Yongsing

We report the observation of nonperturbative high-harmonic generation from monolayer MoS 2. Here, the yield is higher in monolayer compared to a single layer of the bulk, an effect attributed to strong electron-hole interactions in the monolayer.

Observation of High-Harmonic Generation from an Atomically Thin Semiconductor [Observation of High Harmonics from and Atomically Thin Semiconductor

DOE PAGES

Liu, Hanzhe; Li, Yilei; You, Yongsing; ...

2016-01-01

We report the observation of nonperturbative high-harmonic generation from monolayer MoS 2. Here, the yield is higher in monolayer compared to a single layer of the bulk, an effect attributed to strong electron-hole interactions in the monolayer.

Atomic defects in monolayer titanium carbide (Ti 3C 2T x) MXene

DOE PAGES

Sang, Xiahan; Xie, Yu; Lin, Ming -Wei; ...

2016-09-06

Here, the 2D transition metal carbides or nitrides, or MXenes, are emerging as a group of materials showing great promise in lithium ion batteries and supercapacitors. Until now, characterization and properties of single-layer MXenes have been scarcely reported. Here, using scanning transmission electron microscopy, we determined the atomic structure of freestanding monolayer Ti 3C 2T x flakes prepared via the minimally intensive layer delamination method and characterized different point defects that are prevalent in the monolayer flakes. We determine that the Ti vacancy concentration can be controlled by the etchant concentration during preparation. Density function theory-based calculations confirm the defectmore » structures and predict that the defects can influence the surface morphology and termination groups, but do not strongly influence the metallic conductivity. Using devices fabricated from single- and few-layer Ti 3C 2T x MXene flakes, the effect of the number of layers in the flake on conductivity has been demonstrated.« less

Hybrid inorganic–organic superlattice structures with atomic layer deposition/molecular layer deposition

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

Tynell, Tommi; Yamauchi, Hisao; Karppinen, Maarit, E-mail: maarit.karppinen@aalto.fi

2014-01-15

A combination of the atomic layer deposition (ALD) and molecular layer deposition (MLD) techniques is successfully employed to fabricate thin films incorporating superlattice structures that consist of single layers of organic molecules between thicker layers of ZnO. Diethyl zinc and water are used as precursors for the deposition of ZnO by ALD, while three different organic precursors are investigated for the MLD part: hydroquinone, 4-aminophenol and 4,4′-oxydianiline. The successful superlattice formation with all the organic precursors is verified through x-ray reflectivity studies. The effects of the interspersed organic layers/superlattice structure on the electrical and thermoelectric properties of ZnO are investigatedmore » through resistivity and Seebeck coefficient measurements at room temperature. The results suggest an increase in carrier concentration for small concentrations of organic layers, while higher concentrations seem to lead to rather large reductions in carrier concentration.« less

Atomic scale imaging of competing polar states in a Ruddlesden-Popper layered oxide.

PubMed

Stone, Greg; Ophus, Colin; Birol, Turan; Ciston, Jim; Lee, Che-Hui; Wang, Ke; Fennie, Craig J; Schlom, Darrell G; Alem, Nasim; Gopalan, Venkatraman

2016-08-31

Layered complex oxides offer an unusually rich materials platform for emergent phenomena through many built-in design knobs such as varied topologies, chemical ordering schemes and geometric tuning of the structure. A multitude of polar phases are predicted to compete in Ruddlesden-Popper (RP), An+1BnO3n+1, thin films by tuning layer dimension (n) and strain; however, direct atomic-scale evidence for such competing states is currently absent. Using aberration-corrected scanning transmission electron microscopy with sub-Ångstrom resolution in Srn+1TinO3n+1 thin films, we demonstrate the coexistence of antiferroelectric, ferroelectric and new ordered and low-symmetry phases. We also directly image the atomic rumpling of the rock salt layer, a critical feature in RP structures that is responsible for the competing phases; exceptional quantitative agreement between electron microscopy and density functional theory is demonstrated. The study shows that layered topologies can enable multifunctionality through highly competitive phases exhibiting diverse phenomena in a single structure.

Atomic scale imaging of competing polar states in a Ruddlesden–Popper layered oxide

PubMed Central

Stone, Greg; Ophus, Colin; Birol, Turan; Ciston, Jim; Lee, Che-Hui; Wang, Ke; Fennie, Craig J.; Schlom, Darrell G.; Alem, Nasim; Gopalan, Venkatraman

2016-01-01

Layered complex oxides offer an unusually rich materials platform for emergent phenomena through many built-in design knobs such as varied topologies, chemical ordering schemes and geometric tuning of the structure. A multitude of polar phases are predicted to compete in Ruddlesden–Popper (RP), An+1BnO3n+1, thin films by tuning layer dimension (n) and strain; however, direct atomic-scale evidence for such competing states is currently absent. Using aberration-corrected scanning transmission electron microscopy with sub-Ångstrom resolution in Srn+1TinO3n+1 thin films, we demonstrate the coexistence of antiferroelectric, ferroelectric and new ordered and low-symmetry phases. We also directly image the atomic rumpling of the rock salt layer, a critical feature in RP structures that is responsible for the competing phases; exceptional quantitative agreement between electron microscopy and density functional theory is demonstrated. The study shows that layered topologies can enable multifunctionality through highly competitive phases exhibiting diverse phenomena in a single structure. PMID:27578622

Atomic scale imaging of competing polar states in a Ruddlesden-Popper layered oxide

NASA Astrophysics Data System (ADS)

Stone, Greg; Ophus, Colin; Birol, Turan; Ciston, Jim; Lee, Che-Hui; Wang, Ke; Fennie, Craig J.; Schlom, Darrell G.; Alem, Nasim; Gopalan, Venkatraman

2016-08-01

Layered complex oxides offer an unusually rich materials platform for emergent phenomena through many built-in design knobs such as varied topologies, chemical ordering schemes and geometric tuning of the structure. A multitude of polar phases are predicted to compete in Ruddlesden-Popper (RP), An+1BnO3n+1, thin films by tuning layer dimension (n) and strain; however, direct atomic-scale evidence for such competing states is currently absent. Using aberration-corrected scanning transmission electron microscopy with sub-Ångstrom resolution in Srn+1TinO3n+1 thin films, we demonstrate the coexistence of antiferroelectric, ferroelectric and new ordered and low-symmetry phases. We also directly image the atomic rumpling of the rock salt layer, a critical feature in RP structures that is responsible for the competing phases; exceptional quantitative agreement between electron microscopy and density functional theory is demonstrated. The study shows that layered topologies can enable multifunctionality through highly competitive phases exhibiting diverse phenomena in a single structure.

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.

Atomic Scale Study on Growth and Heteroepitaxy of ZnO Monolayer on Graphene.

PubMed

Hong, Hyo-Ki; Jo, Junhyeon; Hwang, Daeyeon; Lee, Jongyeong; Kim, Na Yeon; Son, Seungwoo; Kim, Jung Hwa; Jin, Mi-Jin; Jun, Young Chul; Erni, Rolf; Kwak, Sang Kyu; Yoo, Jung-Woo; Lee, Zonghoon

2017-01-11

Atomically thin semiconducting oxide on graphene carries a unique combination of wide band gap, high charge carrier mobility, and optical transparency, which can be widely applied for optoelectronics. However, study on the epitaxial formation and properties of oxide monolayer on graphene remains unexplored due to hydrophobic graphene surface and limits of conventional bulk deposition technique. Here, we report atomic scale study of heteroepitaxial growth and relationship of a single-atom-thick ZnO layer on graphene using atomic layer deposition. We demonstrate atom-by-atom growth of zinc and oxygen at the preferential zigzag edge of a ZnO monolayer on graphene through in situ observation. We experimentally determine that the thinnest ZnO monolayer has a wide band gap (up to 4.0 eV), due to quantum confinement and graphene-like structure, and high optical transparency. This study can lead to a new class of atomically thin two-dimensional heterostructures of semiconducting oxides formed by highly controlled epitaxial growth.

Effect of Enhanced Thermal Stability of Alumina Support Layer on Growth of Vertically Aligned Single-Walled Carbon Nanotubes and Their Application in Nanofiltration Membranes.

PubMed

In, Jung Bin; Cho, Kang Rae; Tran, Tung Xuan; Kim, Seok-Min; Wang, Yinmin; Grigoropoulos, Costas P; Noy, Aleksandr; Fornasiero, Francesco

2018-06-07

We investigate the thermal stability of alumina supporting layers sputtered at different conditions and its effect on the growth of aligned single-walled carbon nanotube arrays. Radio frequency magnetron sputtering of alumina under oxygen-argon atmosphere produces a Si-rich alumina alloy film on a silicon substrate. Atomic force microscopy on the annealed catalysts reveals that Si-rich alumina films are more stable than alumina layers with low Si content at the elevated temperatures at which the growth of single-walled carbon nanotubes is initiated. The enhanced thermal stability of the Si-rich alumina layer results in a narrower (< 2.2 nm) diameter distribution of the single-walled carbon nanotubes. Thanks to the smaller diameters of their nanotube pores, membranes fabricated with vertically aligned nanotubes grown on the stable layers display improved ion selectivity.

Effect of Enhanced Thermal Stability of Alumina Support Layer on Growth of Vertically Aligned Single-Walled Carbon Nanotubes and Their Application in Nanofiltration Membranes

NASA Astrophysics Data System (ADS)

In, Jung Bin; Cho, Kang Rae; Tran, Tung Xuan; Kim, Seok-Min; Wang, Yinmin; Grigoropoulos, Costas P.; Noy, Aleksandr; Fornasiero, Francesco

2018-06-01

We investigate the thermal stability of alumina supporting layers sputtered at different conditions and its effect on the growth of aligned single-walled carbon nanotube arrays. Radio frequency magnetron sputtering of alumina under oxygen-argon atmosphere produces a Si-rich alumina alloy film on a silicon substrate. Atomic force microscopy on the annealed catalysts reveals that Si-rich alumina films are more stable than alumina layers with low Si content at the elevated temperatures at which the growth of single-walled carbon nanotubes is initiated. The enhanced thermal stability of the Si-rich alumina layer results in a narrower (< 2.2 nm) diameter distribution of the single-walled carbon nanotubes. Thanks to the smaller diameters of their nanotube pores, membranes fabricated with vertically aligned nanotubes grown on the stable layers display improved ion selectivity.

Breakthrough to Non-Vacuum Deposition of Single-Crystal, Ultra-Thin, Homogeneous Nanoparticle Layers: A Better Alternative to Chemical Bath Deposition and Atomic Layer Deposition

PubMed Central

Liao, Yu-Kuang; Liu, Yung-Tsung; Hsieh, Dan-Hua; Shen, Tien-Lin; Hsieh, Ming-Yang; Tzou, An-Jye; Chen, Shih-Chen; Tsai, Yu-Lin; Lin, Wei-Sheng; Chan, Sheng-Wen; Shen, Yen-Ping; Cheng, Shun-Jen; Chen, Chyong-Hua; Wu, Kaung-Hsiung; Chen, Hao-Ming; Kuo, Shou-Yi; Charlton, Martin D. B.; Hsieh, Tung-Po; Kuo, Hao-Chung

2017-01-01

Most thin-film techniques require a multiple vacuum process, and cannot produce high-coverage continuous thin films with the thickness of a few nanometers on rough surfaces. We present a new ”paradigm shift” non-vacuum process to deposit high-quality, ultra-thin, single-crystal layers of coalesced sulfide nanoparticles (NPs) with controllable thickness down to a few nanometers, based on thermal decomposition. This provides high-coverage, homogeneous thickness, and large-area deposition over a rough surface, with little material loss or liquid chemical waste, and deposition rates of 10 nm/min. This technique can potentially replace conventional thin-film deposition methods, such as atomic layer deposition (ALD) and chemical bath deposition (CBD) as used by the Cu(In,Ga)Se2 (CIGS) thin-film solar cell industry for decades. We demonstrate 32% improvement of CIGS thin-film solar cell efficiency in comparison to reference devices prepared by conventional CBD deposition method by depositing the ZnS NPs buffer layer using the new process. The new ZnS NPs layer allows reduction of an intrinsic ZnO layer, which can lead to severe shunt leakage in case of a CBD buffer layer. This leads to a 65% relative efficiency increase. PMID:28383488

Ultrafast atomic layer-by-layer oxygen vacancy-exchange diffusion in double-perovskite LnBaCo2O5.5+δ thin films.

PubMed

Bao, Shanyong; Ma, Chunrui; Chen, Garry; Xu, Xing; Enriquez, Erik; Chen, Chonglin; Zhang, Yamei; Bettis, Jerry L; Whangbo, Myung-Hwan; Dong, Chuang; Zhang, Qingyu

2014-04-22

Surface exchange and oxygen vacancy diffusion dynamics were studied in double-perovskites LnBaCo2O5.5+δ (LnBCO) single-crystalline thin films (Ln = Er, Pr; -0.5 < δ < 0.5) by carefully monitoring the resistance changes under a switching flow of oxidizing gas (O2) and reducing gas (H2) in the temperature range of 250 ~ 800 °C. A giant resistance change ΔR by three to four orders of magnitude in less than 0.1 s was found with a fast oscillation behavior in the resistance change rates in the ΔR vs. t plots, suggesting that the oxygen vacancy exchange diffusion with oxygen/hydrogen atoms in the LnBCO thin films is taking the layer by layer oxygen-vacancy-exchange mechanism. The first principles density functional theory calculations indicate that hydrogen atoms are present in LnBCO as bound to oxygen forming O-H bonds. This unprecedented oscillation phenomenon provides the first direct experimental evidence of the layer by layer oxygen vacancy exchange diffusion mechanism.

A Novel and Functional Single-Layer Sheet of ZnSe

DOE PAGES

Zhou, Jia; Sumpter, Bobby G.; Kent, Paul R. C.; ...

2014-12-23

In this Communication, we report a novel singlelayer sheet of ZnSe, with a three-atomic thickness, which demonstrates a strong quantum confinement effect by exhibiting a large blue shift of 2.0 eV in its absorption edge relative to the zinc blende (ZB) bulk phase. Theoretical optical absorbance shows that the largest absorption of this ultrathin single-layer sheet of ZnSe occurs at a wavelength similar to its four-atom-thick doublelayer counterpart but with higher photoabsorption efficiency, suggesting a superior behavior on incident photon-to-current conversion efficiency for solar water splitting, among other potential applications. The results presented herein for ZnSe may be generalized tomore » other group II-VI analogues.« less

Predicting the structural and electronic properties of two-dimensional single layer boron nitride sheets

NASA Astrophysics Data System (ADS)

Li, Xiao-Dong; Cheng, Xin-Lu

2018-02-01

Three two-dimensional (2D) single layer boron nitride sheets have been predicted based on the first-principles calculations. These 2D boron nitride sheets are comprised of equivalent boron atoms and nitride atoms with sp2 and sp bond hybridization. The geometry optimization reflects that they all possess stable planar crystal structures with the space group P 6 bar 2 m (D3h3) symmetry. The charge density distribution manifests that the B-N bonds in these boron nitride sheets are covalent in nature but with ionic characteristics. The tunable band gaps indicate their potential applications in nanoscale electronic and optoelectronic devices by changing the length of sp-bonded Bsbnd N linkages.

Nanoscale fabrication using single-ion impacts

NASA Astrophysics Data System (ADS)

Millar, Victoria; Pakes, Chris I.; Cimmino, Alberto; Brett, David; Jamieson, David N.; Prawer, Steven D.; Yang, Changyi; Rout, Bidhudutta; McKinnon, Rita P.; Dzurak, Andrew S.; Clark, Robert G.

2001-11-01

We describe a novel technique for the fabrication of nanoscale structures, based on the development of localized chemical modification caused in a PMMA resist by the implantation of single ions. The implantation of 2 MeV He ions through a thin layer of PMMA into an underlying silicon substrate causes latent damage in the resist. On development of the resist we demonstrate the formation within the PMMA layer of clearly defined etched holes, of typical diameter 30 nm, observed using an atomic force microscope employing a carbon nanotube SPM probe in intermittent-contact mode. This technique has significant potential applications. Used purely to register the passage of an ion, it may be a useful verification of the impact sites in an ion-beam modification process operating at the single-ion level. Furthermore, making use of the hole in the PMMA layer to perform subsequent fabrication steps, it may be applied to the fabrication of self-aligned structures in which surface features are fabricated directly above regions of an underlying substrate that are locally doped by the implanted ion. Our primary interest in single-ion resists relates to the development of a solid-state quantum computer based on an array of 31P atoms (which act as qubits) embedded with nanoscale precision in a silicon matrix. One proposal for the fabrication of such an array is by phosphorous-ion implantation. A single-ion resist would permit an accurate verification of 31P implantation sites. Subsequent metalisation of the latent damage may allow the fabrication of self-aligned metal gates above buried phosphorous atoms.

Modeling optical transmissivity of graphene grate in on-chip silicon photonic device

NASA Astrophysics Data System (ADS)

Amiri, Iraj S.; Ariannejad, M. M.; Jalil, M. A.; Ali, J.; Yupapin, P.

2018-06-01

A three-dimensional (3-D) finite-difference-time-domain (FDTD) analysis was used to simulate a silicon photonic waveguide. We have calculated power and transmission of the graphene used as single or multilayers to study the light transmission behavior. A new technique has been developed to define the straight silicon waveguide integrated with grate graphene layer. The waveguide has a variable grate spacing to be filled by the graphene layer. The number of graphene atomic layers varies between 100 and 1000 (or 380 nm and 3800 nm), the transmitted power obtained varies as ∼30% and ∼80%. The ∼99%, blocking of the light was occurred in 10,000 (or 38,000 nm) atomic layers of the graphene grate.

Aggregation, Deposition and Release of Graphene Oxide Nanomaterials in the Aquatic Environment

EPA Science Inventory

Graphene is an atomically thin two dimensional carbon-based nanomaterial that is composed of a single layer of sp2 – hybridized carbon atoms as found in graphite.1, 2 Usage of graphene-based nanomaterials is increasing rapidly and these materials are predicted to be the most abun...

Reaction rates of graphite with ozone measured by etch decoration

NASA Technical Reports Server (NTRS)

Hennig, G. R.; Montet, G. L.

1968-01-01

Etch-decoration technique of detecting vacancies in graphite has been used to determine the reaction rates of graphite with ozone in the directions parallel and perpendicular to the layer planes. It consists essentially of peeling single atom layers off graphite crystals without affecting the remainder of the crystal.

Atomically Defined Templates for Epitaxial Growth of Complex Oxide Thin Films

PubMed Central

Dral, A. Petra; Dubbink, David; Nijland, Maarten; ten Elshof, Johan E.; Rijnders, Guus; Koster, Gertjan

2014-01-01

Atomically defined substrate surfaces are prerequisite for the epitaxial growth of complex oxide thin films. In this protocol, two approaches to obtain such surfaces are described. The first approach is the preparation of single terminated perovskite SrTiO3 (001) and DyScO3 (110) substrates. Wet etching was used to selectively remove one of the two possible surface terminations, while an annealing step was used to increase the smoothness of the surface. The resulting single terminated surfaces allow for the heteroepitaxial growth of perovskite oxide thin films with high crystalline quality and well-defined interfaces between substrate and film. In the second approach, seed layers for epitaxial film growth on arbitrary substrates were created by Langmuir-Blodgett (LB) deposition of nanosheets. As model system Ca2Nb3O10- nanosheets were used, prepared by delamination of their layered parent compound HCa2Nb3O10. A key advantage of creating seed layers with nanosheets is that relatively expensive and size-limited single crystalline substrates can be replaced by virtually any substrate material. PMID:25549000

C 60 -induced Devil's Staircase transformation on a Pb/Si(111) wetting layer

DOE PAGES

Wang, Lin -Lin; Johnson, Duane D.; Tringides, Michael C.

2015-12-03

Density functional theory is used to study structural energetics of Pb vacancy cluster formation on C 60/Pb/Si(111) to explain the unusually fast and error-free transformations between the “Devil's Staircase” (DS) phases on the Pb/Si(111) wetting layer at low temperature (~110K). The formation energies of vacancy clusters are calculated in C 60/Pb/Si(111) as Pb atoms are progressively ejected from the initial dense Pb wetting layer. Vacancy clusters larger than five Pb atoms are found to be stable with seven being the most stable, while vacancy clusters smaller than five are highly unstable, which agrees well with the observed ejection rate ofmore » ~5 Pb atoms per C 60. Furthermore, the high energy cost (~0.8 eV) for the small vacancy clusters to form indicates convincingly that the unusually fast transformation observed experimentally between the DS phases, upon C 60 adsorption at low temperature, cannot be the result of single-atom random walk diffusion but of correlated multi-atom processes.« less

Targeted Single-Site MOF Node Modification: Trivalent Metal Loading via Atomic Layer Deposition

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

Kim, In Soo; Borycz, Joshua; Platero-Prats, Ana E.

Postsynthetic functionalization of metal organic frameworks (MOFs) enables the controlled, high-density incorporation of new atoms on a crystallographically precise framework. Leveraging the broad palette of known atomic layer deposition (ALD) chemistries, ALD in MOFs (AIM) is one such targeted approach to construct diverse, highly functional, few-atom clusters. We here demonstrate the saturating reaction of trimethylindium (InMe3) with the node hydroxyls and ligated water of NU-1000, which takes place without significant loss of MOF crystallinity or internal surface area. We computationally identify the elementary steps by which trimethylated trivalent metal compounds (ALD precursors) react with this Zr-based MOF node to generatemore » a uniform and well characterized new surface layer on the node itself, and we predict a final structure that is fully consistent with experimental X-ray pair distribution function (PDF) analysis. We further demonstrate tunable metal loading through controlled number density of the reactive handles (-OH and -OH2) achieved through node dehydration at elevated temperatures.« less

Noble-metal intercalation process leading to a protected adatom in a graphene hollow site

NASA Astrophysics Data System (ADS)

Narayanan Nair, M.; Cranney, M.; Jiang, T.; Hajjar-Garreau, S.; Aubel, D.; Vonau, F.; Florentin, A.; Denys, E.; Bocquet, M.-L.; Simon, L.

2016-08-01

In previous studies, we have shown that gold deposited on a monolayer (ML) of graphene on SiC(0001) is intercalated below the ML after an annealing procedure and affects the band structure of graphene. Here we prove experimentally and theoretically that some of the gold forms a dispersed phase composed of single adatoms, being intercalated between the ML and the buffer layer and in a hollow position with respect to C atoms of the ML on top. They are freestanding and negatively charged, due to the partial screening of the electron transfer between SiC and the ML, without changing the intrinsic n-type doping of the ML. As these single atoms decouple the ML from the buffer layer, the quasiparticles of graphene are less perturbed, thus increasing their Fermi velocity. Moreover, the hollow position of the intercalated single Au atoms might lead to spin-orbit coupling in the graphene layer covering IC domains. This effect of spin-orbit coupling has been recently observed experimentally in Au-intercalated graphene on SiC(0001) [D. Marchenko, A. Varykhalov, J. Sánchez-Barriga, Th. Seyller, and O. Rader, Appl. Phys. Lett. 108, 172405 (2016), 10.1063/1.4947286] and has been theoretically predicted for heavy atoms, like thallium, in a hollow position on graphene [C. Weeks, J. Hu, J. Alicea, M. Franz, and R. Wu, Phys. Rev. X 1, 021001 (2011), 10.1103/PhysRevX.1.021001; A. Cresti, D. V. Tuan, D. Soriano, A. W. Cummings, and S. Roche, Phys. Rev. Lett. 113, 246603 (2014), 10.1103/PhysRevLett.113.246603].

Atomic-scale analysis of cation ordering in reduced calcium titanate.

PubMed

Li, Luying; Hu, Xiaokang; Jiang, Fan; Jing, Wenkui; Guo, Cong; Jia, Shuangfeng; Gao, Yihua; Wang, Jianbo

2017-11-03

The phenomenon of cation ordering is closely related to certain physical properties of complex oxides, which necessitates the search of underlying structure-property relationship at atomic resolution. Here we study the superlattices within reduced calcium titanate single crystal micro-pillars, which are unexpected from the originally proposed atomic model. Bright and dark contrasts at alternating Ti double layers perpendicular to b axis are clearly observed, but show no signs in corresponding image simulations based on the proposed atomic model. The multi-dimensional chemical analyses at atomic resolution reveal periodic lower Ti concentrations at alternating Ti double layers perpendicular to b axis. The following in-situ heating experiment shows no phase transition at the reported T c and temperature independence of the superlattices. The dimerization of the Ti-Ti bonds at neighboring double rutile-type chains within Ti puckered sheets are directly observed, which is found to be not disturbed by the cation ordering at alternating Ti double layers. The characterization of cation ordering of complex oxides from chemical and structural point of view at atomic resolution, and its reaction to temperature variations are important for further understanding their basic physical properties and exploiting potential applications.

Synthesis of two-dimensional TlxBi1−x compounds and Archimedean encoding of their atomic structure

PubMed Central

Gruznev, Dimitry V.; Bondarenko, Leonid V.; Matetskiy, Andrey V.; Mihalyuk, Alexey N.; Tupchaya, Alexandra Y.; Utas, Oleg A.; Eremeev, Sergey V.; Hsing, Cheng-Rong; Chou, Jyh-Pin; Wei, Ching-Ming; Zotov, Andrey V.; Saranin, Alexander A.

2016-01-01

Crystalline atomic layers on solid surfaces are composed of a single building block, unit cell, that is copied and stacked together to form the entire two-dimensional crystal structure. However, it appears that this is not an unique possibility. We report here on synthesis and characterization of the one-atomic-layer-thick TlxBi1−x compounds which display quite a different arrangement. It represents a quasi-periodic tiling structures that are built by a set of tiling elements as building blocks. Though the layer is lacking strict periodicity, it shows up as an ideally-packed tiling of basic elements without any skips or halting. The two-dimensional TlxBi1−x compounds were formed by depositing Bi onto the Tl-covered Si(111) surface where Bi atoms substitute appropriate amount of Tl atoms. Atomic structure of each tiling element as well as arrangement of TlxBi1−x compounds were established in a detail. Electronic properties and spin texture of the selected compounds having periodic structures were characterized. The shown example demonstrates possibility for the formation of the exotic low-dimensional materials via unusual growth mechanisms. PMID:26781340

Atomic layer deposition of Al{sub 2}O{sub 3} for single electron transistors utilizing Pt oxidation and reduction

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

McConnell, Michael S., E-mail: mmcconn5@nd.edu; Schneider, Louisa C.; Karbasian, Golnaz

This work describes the fabrication of single electron transistors using electron beam lithography and atomic layer deposition to form nanoscale tunnel transparent junctions of alumina (Al{sub 2}O{sub 3}) on platinum nanowires using either water or ozone as the oxygen precursor and trimethylaluminum as the aluminum precursor. Using room temperature, low frequency conductance measurements between the source and drain, it was found that devices fabricated using water had higher conductance than devices fabricated with ozone. Subsequent annealing caused both water- and ozone-based devices to increase in conductance by more than 2 orders of magnitude. Furthermore, comparison of devices at low temperaturesmore » (∼4 K) showed that annealed devices displayed much closer to the ideal behavior (i.e., constant differential conductance) outside of the Coulomb blockade region and that untreated devices showed nonlinear behavior outside of the Coulomb blockade region (i.e., an increase in differential conductance with source-drain voltage bias). Transmission electron microscopy cross-sectional images showed that annealing did not significantly change device geometry, but energy dispersive x-ray spectroscopy showed an unusually large amount of oxygen in the bottom platinum layer. This suggests that the atomic layer deposition process results in the formation of a thin platinum surface oxide, which either decomposes or is reduced during the anneal step, resulting in a tunnel barrier without the in-series native oxide contribution. Furthermore, the difference between ozone- and water-based devices suggests that ozone promotes atomic layer deposition nucleation by oxidizing the surface but that water relies on physisorption of the precursors. To test this theory, devices were exposed to forming gas at room temperature, which also reduces platinum oxide, and a decrease in resistance was observed, as expected.« less

Atomic and molecular layer deposition for surface modification

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

Vähä-Nissi, Mika, E-mail: mika.vaha-nissi@vtt.fi; Sievänen, Jenni; Salo, Erkki

2014-06-01

Atomic and molecular layer deposition (ALD and MLD, respectively) techniques are based on repeated cycles of gas–solid surface reactions. A partial monolayer of atoms or molecules is deposited to the surface during a single deposition cycle, enabling tailored film composition in principle down to molecular resolution on ideal surfaces. Typically ALD/MLD has been used for applications where uniform and pinhole free thin film is a necessity even on 3D surfaces. However, thin – even non-uniform – atomic and molecular deposited layers can also be used to tailor the surface characteristics of different non-ideal substrates. For example, print quality of inkjetmore » printing on polymer films and penetration of water into porous nonwovens can be adjusted with low-temperature deposited metal oxide. In addition, adhesion of extrusion coated biopolymer to inorganic oxides can be improved with a hybrid layer based on lactic acid. - Graphical abstract: Print quality of a polylactide film surface modified with atomic layer deposition prior to inkjet printing (360 dpi) with an aqueous ink. Number of printed dots illustrated as a function of 0, 5, 15 and 25 deposition cycles of trimethylaluminum and water. - Highlights: • ALD/MLD can be used to adjust surface characteristics of films and fiber materials. • Hydrophobicity after few deposition cycles of Al{sub 2}O{sub 3} due to e.g. complex formation. • Same effect on cellulosic fabrics observed with low temperature deposited TiO{sub 2}. • Different film growth and oxidation potential with different precursors. • Hybrid layer on inorganic layer can be used to improve adhesion of polymer melt.« less

Simulation of fundamental atomization mechanisms in fuel sprays

NASA Technical Reports Server (NTRS)

Childs, Robert, E.; Mansour, Nagi N.

1988-01-01

Growth of instabilities on the liquid/gas interface in the initial region of fuel sprays is studied by means of numerical simulations. The simulations are based on solutions of the variable-density incompressible Navier-Stokes equations, which are obtained with a new numerical algorithm. The simulations give good agreement with analytical results for the instabilities on a liquid cylinder induced by surface tension and wind-induced instabilities. The effects of boundary layers on the wind-induced instabilities are investigated. It is found that a boundary layer reduces the growth rate for a single interface, and a comparison with inviscid theory suggests that boundary layer effects may be significantly more important than surface tension effects. The results yield a better estimate than inviscid theory for the drop sizes as reported for diesel sprays. Results for the planar jet show that boundary layer effects hasten the growth of Squire's 'symmetric' mode, which is responsible for jet disintegration. This result helps explain the rapid atomization which occurs in swirl and air-blast atomizers.

First-principles study on silicon atom doped monolayer graphene

NASA Astrophysics Data System (ADS)

Rafique, Muhammad; Shuai, Yong; Hussain, Nayyar

2018-01-01

This paper illustrates the structural, electronic and optical properties of individual silicon (Si) atom-doped single layer graphene using density functional theory method. Si atom forms tight bonding with graphene layer. The effect of doping has been investigated by varying the concentration of Si atoms from 3.125% to 9.37% (i.e. From one to three Si atoms in 4 × 4 pure graphene supercell containing 32 carbon atoms), respectively. Electronic structure, partial density of states (PDOS) and optical properties of pure and Si atom-doped graphene sheet were calculated using VASP (Vienna ab-initio Simulation Package). The calculated results for pure graphene sheet were then compared with Si atom doped graphene. It is revealed that upon Si doping in graphene, a finite band gap appears at the high symmetric K-point, thereby making graphene a direct band gap semiconductor. Moreover, the band gap value is directly proportional to the concentration of impurity Si atoms present in graphene lattice. Upon analyzing the optical properties of Si atom-doped graphene structures, it is found that, there is significant change in the refractive index of the graphene after Si atom substitution in graphene. In addition, the overall absorption spectrum of graphene is decreased after Si atom doping. Although a significant red shift in absorption is found to occur towards visible range of radiation when Si atom is substituted in its lattice. The reflectivity of graphene improves in low energy region after Si atom substitution in graphene. These results can be useful for tuning the electronic structure and to manipulate the optical properties of graphene layer in the visible region.

A role for ion implantation in quantum computing

NASA Astrophysics Data System (ADS)

Jamieson, David N.; Prawer, Steven; Andrienko, Igor; Brett, David A.; Millar, Victoria

2001-04-01

We propose to create arrays of phosphorus atoms in silicon for quantum computing using ion implantation. Since the implantation of the ions is essentially random, the yield of usefully spaced atoms is low and therefore some method of registering the passage of a single ion is required. This can be accomplished by implantation of the ions through a thin surface layer consisting of resist. Changes to the chemical and/or electrical properties of the resist will be used to mark the site of the buried ion. For chemical changes, the latent damage will be developed and the atomic force microscope (AFM) used to image the changes in topography. Alternatively, changes in electrical properties (which obviate the need for post-irradiation chemical etching) will be used to register the passage of the ion using scanning tunneling microscopy (STM), the surface current imaging mode of the AFM. We address the central issue of the contrast created by the passage of a single ion through resist layers of PMMA and C 60.

Prediction of another semimetallic silicene allotrope with Dirac fermions

NASA Astrophysics Data System (ADS)

Wu, Haiping; Qian, Yan; Du, Zhengwei; Zhu, Renzhu; Kan, Erjun; Deng, Kaiming

2017-11-01

Materials with Dirac point are so amazing since the charge carriers are massless and have an effective speed of light. However, among the predicted two-dimensional silicon allotropes with Dirac point, no one has been directly proved by experiment. This fact motivates us to search for other two-dimensional silicon allotropes. As a result, another stable single atomic layer thin silicon allotrope is found with the help of CALYPSO code in this work. This silicene allotrope is composed of eight-membered rings linked by Si-Si bonds with buckling formation. The electronic calculation reveals that it behaves as a nodal line semimetal with the linear energy dispersion relation near the Fermi surface. Notably, the ab initio molecular dynamics simulations display that the original atomic configuration can be remained even at an extremely high temperature of 1000 K. Additionally, hydrogenation could induce a semimetal-semiconductor transition in this silicene allotrope. We hope this work can expand the family of single atomic layer thin silicon allotropes with special applications.

Atomic scale imaging of competing polar states in a Ruddlesden–Popper layered oxide

DOE PAGES

Stone, Greg; Ophus, Colin; Birol, Turan; ...

2016-08-31

Layered complex oxides offer an unusually rich materials platform for emergent phenomena through many built-in design knobs such as varied topologies, chemical ordering schemes and geometric tuning of the structure. A multitude of polar phases are predicted to compete in Ruddlesden-Popper (RP), A n+1 B n O 3n+1 , thin films by tuning layer dimension (n) and strain; however, direct atomic-scale evidence for such competing states is currently absent. Using aberration-corrected scanning transmission electron microscopy with sub-Ångstrom resolution in Sr n+1 Ti n O 3n+1 thin films, we demonstrate the coexistence of antiferroelectric, ferroelectric and new ordered and low-symmetry phases.more » We also directly image the atomic rumpling of the rock salt layer, a critical feature in RP structures that is responsible for the competing phases; exceptional quantitative agreement between electron microscopy and density functional theory is demonstrated. The study shows that layered topologies can enable multifunctionality through highly competitive phases exhibiting diverse phenomena in a single structure.« less

DFT studies on the Al, B, and P doping of silicene

NASA Astrophysics Data System (ADS)

Hernández Cocoletzi, H.; Castellanos Águila, J. E.

2018-02-01

The search for efficient adsorbents of atoms and molecules has motivated the study of systems in the presence of defects. For this reason, we have investigated theoretically the creation of mono- and di-vacancies on single layer silicene, as well as the Al, B, and P doping of silicene. Using the first-principles method with the generalized gradient approximation in the parameterization of Perdew-Burke-Ernzerhof, we have found that Al, B, and P interact strongly with Si atoms. Besides, when the vacancies are generated, the dangling bonds are saturated in pairs to form new bonds. Optimal geometries, binding energies, density of states (DOS) and charge density are reported. The results suggest that new chemical modifications can be used to modify the electronic properties of single-layer silicene.

Single-walled carbon nanotubes coated with ZnO by atomic layer deposition

NASA Astrophysics Data System (ADS)

Pal, Partha P.; Gilshteyn, Evgenia; Jiang, Hua; Timmermans, Marina; Kaskela, Antti; Tolochko, Oleg V.; Kurochkin, Alexey V.; Karppinen, Maarit; Nisula, Mikko; Kauppinen, Esko I.; Nasibulin, Albert G.

2016-12-01

The possibility of ZnO deposition on the surface of single-walled carbon nanotubes (SWCNTs) with the help of an atomic layer deposition (ALD) technique was successfully demonstrated. The utilization of pristine SWCNTs as a support resulted in a non-uniform deposition of ZnO in the form of nanoparticles. To achieve uniform ZnO coating, the SWCNTs first needed to be functionalized by treating the samples in a controlled ozone atmosphere. The uniformly ZnO coated SWCNTs were used to fabricate UV sensing devices. An UV irradiation of the ZnO coated samples turned them from hydrophobic to hydrophilic behaviour. Furthermore, thin films of the ZnO coated SWCNTs allowed us switch p-type field effect transistors made of pristine SWCNTs to have ambipolar characteristics.

Single-walled carbon nanotubes coated with ZnO by atomic layer deposition.

PubMed

Pal, Partha P; Gilshteyn, Evgenia; Jiang, Hua; Timmermans, Marina; Kaskela, Antti; Tolochko, Oleg V; Karppinen, Maarit; Nisula, Mikko; Kauppinen, Esko I; Nasibulin, Albert G

2016-12-02

The possibility of ZnO deposition on the surface of single-walled carbon nanotubes (SWCNTs) with the help of an atomic layer deposition (ALD) technique was successfully demonstrated. The utilization of pristine SWCNTs as a support resulted in a non-uniform deposition of ZnO in the form of nanoparticles. To achieve uniform ZnO coating, the SWCNTs first needed to be functionalized by treating the samples in a controlled ozone atmosphere. The uniformly ZnO coated SWCNTs were used to fabricate UV sensing devices. An UV irradiation of the ZnO coated samples turned them from hydrophobic to hydrophilic behaviour. Furthermore, thin films of the ZnO coated SWCNTs allowed us switch p-type field effect transistors made of pristine SWCNTs to have ambipolar characteristics.

Atomic layer deposited oxide films as protective interface layers for integrated graphene transfer

NASA Astrophysics Data System (ADS)

Cabrero-Vilatela, A.; Alexander-Webber, J. A.; Sagade, A. A.; Aria, A. I.; Braeuninger-Weimer, P.; Martin, M.-B.; Weatherup, R. S.; Hofmann, S.

2017-12-01

The transfer of chemical vapour deposited graphene from its parent growth catalyst has become a bottleneck for many of its emerging applications. The sacrificial polymer layers that are typically deposited onto graphene for mechanical support during transfer are challenging to remove completely and hence leave graphene and subsequent device interfaces contaminated. Here, we report on the use of atomic layer deposited (ALD) oxide films as protective interface and support layers during graphene transfer. The method avoids any direct contact of the graphene with polymers and through the use of thicker ALD layers (≥100 nm), polymers can be eliminated from the transfer-process altogether. The ALD film can be kept as a functional device layer, facilitating integrated device manufacturing. We demonstrate back-gated field effect devices based on single-layer graphene transferred with a protective Al2O3 film onto SiO2 that show significantly reduced charge trap and residual carrier densities. We critically discuss the advantages and challenges of processing graphene/ALD bilayer structures.

Metallic atomically-thin layered silicon epitaxially grown on silicene/ZrB 2

DOE PAGES

Gill, Tobias G.; Fleurence, Antoine; Warner, Ben; ...

2017-02-17

We observe a new two-dimensional (2D) silicon crystal, using low energy electron diffraction (LEED) and scanning tunnelling microscopy (STM) and it's formed by depositing additional Si atoms onto spontaneously-formed epitaxial silicene on a ZrB 2 thin film. From scanning tunnelling spectroscopy (STS) studies, we find that this atomically-thin layered silicon has distinctly different electronic properties. Angle resolved photoelectron spectroscopy (ARPES) reveals that, in sharp contrast to epitaxial silicene, the layered silicon exhibits significantly enhanced density of states at the Fermi level resulting from newly formed metallic bands. Furthermore, the 2D growth of this material could allow for direct contacting tomore » the silicene surface and demonstrates the dramatic changes in electronic structure that can occur by the addition of even a single monolayer amount of material in 2D systems.« less

Synthesis of Large-Area 2D Layered Materials and Their Heterostacking Structures

DTIC Science & Technology

2017-10-13

Volume: 6 Pages: 7666 Published: JUL 2015 4. Title: Atomically Thin Heterostructures Based on Single- Layer Tungsten Diselenide and DISTRIBUTION A...AFRL-AFOSR-JP-TR-2017-0070 Synthesis of Large-Area 2D layered Materials and Their Heterostacking Structures Chih-Wei Chu Academia Sinica Final Report...TYPE Final 3. DATES COVERED (From - To) 20 Nov 2014 to 19 Nov 2016 4. TITLE AND SUBTITLE Synthesis of Large-Area 2D layered Materials and Their

Unsupported single-atom-thick copper oxide monolayers

NASA Astrophysics Data System (ADS)

Yin, Kuibo; Zhang, Yu-Yang; Zhou, Yilong; Sun, Litao; Chisholm, Matthew F.; Pantelides, Sokrates T.; Zhou, Wu

2017-03-01

Oxide monolayers may present unique opportunities because of the great diversity of properties of these materials in bulk form. However, reports on oxide monolayers are still limited. Here we report the formation of single-atom-thick copper oxide layers with a square lattice both in graphene pores and on graphene substrates using aberration-corrected scanning transmission electron microscopy. First-principles calculations find that CuO is energetically stable and its calculated lattice spacing matches well with the measured value. Furthermore, free-standing copper oxide monolayers are predicted to be semiconductors with band gaps ˜3 eV. The new wide-bandgap single-atom-thick copper oxide monolayers usher a new frontier to study the highly diverse family of two-dimensional oxides and explore their properties and their potential for new applications.

Using atomistic simulations to model cadmium telluride thin film growth

NASA Astrophysics Data System (ADS)

Yu, Miao; Kenny, Steven D.

2016-03-01

Cadmium telluride (CdTe) is an excellent material for low-cost, high efficiency thin film solar cells. It is important to conduct research on how defects are formed during the growth process, since defects lower the efficiency of solar cells. In this work we use computer simulation to predict the growth of a sputter deposited CdTe thin film. On-the-fly kinetic Monte Carlo technique is used to simulate the CdTe thin film growth on the (1 1 1) surfaces. The results show that on the (1 1 1) surfaces the growth mechanisms on surfaces which are terminated by Cd or Te are quite different, regardless of the deposition energy (0.1∼ 10 eV). On the Te-terminated (1 1 1) surface the deposited clusters first form a single mixed species layer, then the Te atoms in the mixed layer moved up to form a new layer. Whilst on the Cd-terminated (1 1 1) surface the new Cd and Te layers are formed at the same time. Such differences are probably caused by stronger bonding between ad-atoms and surface atoms on the Te layer than on the Cd layer.

Surface texture of single-crystal silicon oxidized under a thin V{sub 2}O{sub 5} layer

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

Nikitin, S. E., E-mail: nikitin@mail.ioffe.ru; Verbitskiy, V. N.; Nashchekin, A. V.

The process of surface texturing of single-crystal silicon oxidized under a V{sub 2}O{sub 5} layer is studied. Intense silicon oxidation at the Si–V{sub 2}O{sub 5} interface begins at a temperature of 903 K which is 200 K below than upon silicon thermal oxidation in an oxygen atmosphere. A silicon dioxide layer 30–50 nm thick with SiO{sub 2} inclusions in silicon depth up to 400 nm is formed at the V{sub 2}O{sub 5}–Si interface. The diffusion coefficient of atomic oxygen through the silicon-dioxide layer at 903 K is determined (D ≥ 2 × 10{sup –15} cm{sup 2} s{sup –1}). A modelmore » of low-temperature silicon oxidation, based on atomic oxygen diffusion from V{sub 2}O{sub 5} through the SiO{sub 2} layer to silicon, and SiO{sub x} precipitate formation in silicon is proposed. After removing the V{sub 2}O{sub 5} and silicon-dioxide layers, texture is formed on the silicon surface, which intensely scatters light in the wavelength range of 300–550 nm and is important in the texturing of the front and rear surfaces of solar cells.« less

Application of atomic force microscopy to microbial surfaces: from reconstituted cell surface layers to living cells.

PubMed

Dufrêne, Y F

2001-02-01

The application of atomic force microscopy (AFM) to probe the ultrastructure and physical properties of microbial cell surfaces is reviewed. The unique capabilities of AFM can be summarized as follows: imaging surface topography with (sub)nanometer lateral resolution; examining biological specimens under physiological conditions; measuring local properties and interaction forces. AFM is being used increasingly for: (i) visualizing the surface ultrastructure of microbial cell surface layers, including bacterial S-layers, purple membranes, porin OmpF crystals and fungal rodlet layers; (ii) monitoring conformational changes of individual membrane proteins; (iii) examining the morphology of bacterial biofilms, (iv) revealing the nanoscale structure of living microbial cells, including fungi, yeasts and bacteria, (v) mapping interaction forces at microbial surfaces, such as van der Waals and electrostatic forces, solvation forces, and steric/bridging forces; and (vi) probing the local mechanical properties of cell surface layers and of single cells.

Method of making coherent multilayer crystals

DOEpatents

Schuller, Ivan K.; Falco, Charles M.

1984-01-01

A new material consisting of a coherent multilayer crystal of two or more elements where each layer is composed of a single element. Each layer may vary in thickness from about 2 .ANG. to 2500 .ANG.. The multilayer crystals are prepared by sputter deposition under conditions which slow the sputtered atoms to near substrate temperatures before they contact the substrate.

Strong anisotropy and magnetostriction in the two-dimensional Stoner ferromagnet Fe 3 GeTe 2

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

Zhuang, Houlong L.; Kent, P. R. C.; Hennig, Richard G.

Comore » mputationally characterizing magnetic properies of novel two-dimensional (2D) materials serves as an important first step of exploring possible applications. Using density-functional theory, we show that single-layer Fe 3 GeTe 2 is a potential 2D material with sufficiently low formation energy to be synthesized by mechanical exfoliation from the bulk phase with a van der Waals layered structure. In addition, we calculated the phonon dispersion demonstrating that single-layer Fe 3 GeTe 2 is dynamically stable. Furthermore, we find that similar to the bulk phase, 2D Fe 3 GeTe 2 exhibits amagnetic moment that originates from a Stoner instability. In contrast to other 2D materials, we find that single-layer Fe 3 GeTe 2 exhibits a significant uniaxial magnetocrystalline anisotropy energy of 920μ eV per Fe atom originating from spin-orbit coupling. In conclusion, we show that applying biaxial tensile strains enhances the anisotropy energy, which reveals strong magnetostriction in single-layer Fe 3 GeTe 2 with a sizable magneostrictive coefficient. Our results indicate that single-layer Fe 3 GeTe 2 is potentially useful for magnetic storage applications.« less

Strong anisotropy and magnetostriction in the two-dimensional Stoner ferromagnet Fe 3 GeTe 2

DOE PAGES

Zhuang, Houlong L.; Kent, P. R. C.; Hennig, Richard G.

2016-04-06

Comore » mputationally characterizing magnetic properies of novel two-dimensional (2D) materials serves as an important first step of exploring possible applications. Using density-functional theory, we show that single-layer Fe 3 GeTe 2 is a potential 2D material with sufficiently low formation energy to be synthesized by mechanical exfoliation from the bulk phase with a van der Waals layered structure. In addition, we calculated the phonon dispersion demonstrating that single-layer Fe 3 GeTe 2 is dynamically stable. Furthermore, we find that similar to the bulk phase, 2D Fe 3 GeTe 2 exhibits amagnetic moment that originates from a Stoner instability. In contrast to other 2D materials, we find that single-layer Fe 3 GeTe 2 exhibits a significant uniaxial magnetocrystalline anisotropy energy of 920μ eV per Fe atom originating from spin-orbit coupling. In conclusion, we show that applying biaxial tensile strains enhances the anisotropy energy, which reveals strong magnetostriction in single-layer Fe 3 GeTe 2 with a sizable magneostrictive coefficient. Our results indicate that single-layer Fe 3 GeTe 2 is potentially useful for magnetic storage applications.« less

Synthesis, crystal structure and electronic structure of the binary phase Rh{sub 2}Cd{sub 5}

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

Koley, Biplab; Chatterjee, S.; Jana, Partha P., E-mail: ppj@chem.iitkgp.ernet.in

2017-02-15

A new phase in the Rh-Cd binary system - Rh{sub 2}Cd{sub 5} has been identified and characterized by single crystal X-ray diffraction and Energy dispersive X-ray analysis. The stoichiometric compound Rh{sub 2}Cd{sub 5} crystallizes with a unit cell containing 14 atoms, in the orthorhombic space group Pbam (55). The crystal structure of Rh{sub 2}Cd{sub 5} can be described as a defect form of the In{sub 3}Pd{sub 5} structure with ordered vacancies, formed of two 2D atomic layers with the stacking sequence: ABAB. The A type layers consist of (3.6.3.6)-Kagomé nets of Cd atoms while the B type layers consist ofmore » (3{sup 5}) (3{sup 7})- nets of both Cd and Rh atoms. The stability of this line phase is investigated by first principle electronic structure calculations on the model of ordered Rh{sub 2}Cd{sub 5}. - Graphical abstract: (3.6.3.6)-Kagomé nets of cadmium atoms (top) and (3{sup 5}) (3{sup 7})- nets of both cadmium and rhodium atoms (bottom) in the structure of Rh{sub 2}Cd{sub 5}.« less

Low-Power Optical Trapping of Nanoparticles and Proteins with Resonant Coaxial Nanoaperture Using 10 nm Gap.

PubMed

Yoo, Daehan; Gurunatha, Kargal L; Choi, Han-Kyu; Mohr, Daniel A; Ertsgaard, Christopher T; Gordon, Reuven; Oh, Sang-Hyun

2018-06-13

We present optical trapping with a 10 nm gap resonant coaxial nanoaperture in a gold film. Large arrays of 600 resonant plasmonic coaxial nanoaperture traps are produced on a single chip via atomic layer lithography with each aperture tuned to match a 785 nm laser source. We show that these single coaxial apertures can act as efficient nanotweezers with a sharp potential well, capable of trapping 30 nm polystyrene nanoparticles and streptavidin molecules with a laser power as low as 4.7 mW. Furthermore, the resonant coaxial nanoaperture enables real-time label-free detection of the trapping events via simple transmission measurements. Our fabrication technique is scalable and reproducible, since the critical nanogap dimension is defined by atomic layer deposition. Thus our platform shows significant potential to push the limit of optical trapping technologies.

Towards precise defect control in layered oxide structures by using oxide molecular beam epitaxy

PubMed Central

Baiutti, Federico; Christiani, Georg

2014-01-01

Summary In this paper we present the atomic-layer-by-layer oxide molecular beam epitaxy (ALL-oxide MBE) which has been recently installed in the Max-Planck Institute for Solid State Research and we report on its present status, providing some examples that demonstrate its successful application in the synthesis of different layered oxides, with particular reference to superconducting La2CuO4 and insulator-to-metal La2− xSrxNiO4. We briefly review the ALL-oxide MBE technique and its unique capabilities in the deposition of atomically smooth single-crystal thin films of various complex oxides, artificial compounds and heterostructures, introducing our goal of pursuing a deep investigation of such systems with particular emphasis on structural defects, with the aim of tailoring their functional properties by precise defects control. PMID:24995148

Targeted Single-Site MOF Node Modification: Trivalent Metal Loading via Atomic Layer Deposition

DOE PAGES

Kim, In Soo; Borycz, Joshua; Platero-Prats, Ana E.; ...

2015-07-02

Postsynthetic functionalization of metal organic frameworks (MOFs) enables the controlled, high-density incorporation of new atoms on a crystallographically precise framework. Leveraging the broad palette of known atomic layer deposition (ALD) chemistries, ALD in MOFs (AIM) is one such targeted approach to construct diverse, highly functional, few-atom clusters. In this paper, we demonstrate the saturating reaction of trimethylindium (InMe 3) with the node hydroxyls and ligated water of NU-1000, which takes place without significant loss of MOF crystallinity or internal surface area. We computationally identify the elementary steps by which trimethylated trivalent metal compounds (ALD precursors) react with this Zr-based MOFmore » node to generate a uniform and well characterized new surface layer on the node itself, and we predict a final structure that is fully consistent with experimental X-ray pair distribution function (PDF) analysis. Finally, we further demonstrate tunable metal loading through controlled number density of the reactive handles (–OH and –OH 2) achieved through node dehydration at elevated temperatures.« less

Targeted Single-Site MOF Node Modification: Trivalent Metal Loading via Atomic Layer Deposition

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

Kim, In Soo; Borycz, Joshua; Platero-Prats, Ana E.

Postsynthetic functionalization of metal organic frameworks (MOFs) enables the controlled, high-density incorporation of new atoms on a crystallographically precise framework. Leveraging the broad palette of known atomic layer deposition (ALD) chemistries, ALD in MOFs (AIM) is one such targeted approach to construct diverse, highly functional, few-atom clusters. In this paper, we demonstrate the saturating reaction of trimethylindium (InMe 3) with the node hydroxyls and ligated water of NU-1000, which takes place without significant loss of MOF crystallinity or internal surface area. We computationally identify the elementary steps by which trimethylated trivalent metal compounds (ALD precursors) react with this Zr-based MOFmore » node to generate a uniform and well characterized new surface layer on the node itself, and we predict a final structure that is fully consistent with experimental X-ray pair distribution function (PDF) analysis. Finally, we further demonstrate tunable metal loading through controlled number density of the reactive handles (–OH and –OH 2) achieved through node dehydration at elevated temperatures.« less

Atomically Phase-Matched Second-Harmonic Generation in a 2D Crystal

DTIC Science & Technology

2016-08-26

thin mate- rials. However, despite the inversion asymmetry of the single layer, the typical crystal stacking restores inversion symmetry for even...typically do not produce SH signals when inversion symmetry is restored in their multilayer counterparts. Group VI transition metal dichalcogenides (TMDCs...group D3h). However, adjacent layers of the 2H are mirrored to restore the inversion symmetry, while the layers in the 3R phase retain the same

Monolayer PtSe₂, a New Semiconducting Transition-Metal-Dichalcogenide, Epitaxially Grown by Direct Selenization of Pt.

PubMed

Wang, Yeliang; Li, Linfei; Yao, Wei; Song, Shiru; Sun, J T; Pan, Jinbo; Ren, Xiao; Li, Chen; Okunishi, Eiji; Wang, Yu-Qi; Wang, Eryin; Shao, Yan; Zhang, Y Y; Yang, Hai-tao; Schwier, Eike F; Iwasawa, Hideaki; Shimada, Kenya; Taniguchi, Masaki; Cheng, Zhaohua; Zhou, Shuyun; Du, Shixuan; Pennycook, Stephen J; Pantelides, Sokrates T; Gao, Hong-Jun

2015-06-10

Single-layer transition-metal dichalcogenides (TMDs) receive significant attention due to their intriguing physical properties for both fundamental research and potential applications in electronics, optoelectronics, spintronics, catalysis, and so on. Here, we demonstrate the epitaxial growth of high-quality single-crystal, monolayer platinum diselenide (PtSe2), a new member of the layered TMDs family, by a single step of direct selenization of a Pt(111) substrate. A combination of atomic-resolution experimental characterizations and first-principle theoretic calculations reveals the atomic structure of the monolayer PtSe2/Pt(111). Angle-resolved photoemission spectroscopy measurements confirm for the first time the semiconducting electronic structure of monolayer PtSe2 (in contrast to its semimetallic bulk counterpart). The photocatalytic activity of monolayer PtSe2 film is evaluated by a methylene-blue photodegradation experiment, demonstrating its practical application as a promising photocatalyst. Moreover, circular polarization calculations predict that monolayer PtSe2 has also potential applications in valleytronics.

Experimental observation of edge transport in graphene nanostructures

NASA Astrophysics Data System (ADS)

Kinikar, Amogh; Sai, T. Phanindra; Bhattacharyya, Semonti; Agarwala, Adhip; Biswas, Tathagata; Sarker, Sanjoy K.; Krishnamurthy, H. R.; Jain, Manish; Shenoy, Vijay B.; Ghosh, Arindam

The zizzag edges of graphene, whether single or few layers, host zero energy gapless states and are perfect 1D ballistic conductors. Conclusive observations of electrical conduction through edge states has been elusive. We report the observation of edge bound transport in atomic-scale constrictions of single and multilayer suspended graphene created stochastically by nanomechanical exfoliation of graphite. We observe that the conductance is quantized in near multiples of e2/h. Non-equilibrium transport shows a split zero bias anomaly and, the magneto-conductance is hysteretic; indicating that the electron transport is through spin polarized edge states in the presence of electron-electron interaction. Atomic force microscope scans on the graphite surface post exfoliation reveal that the final constriction is usually a single layer graphene with a constricting angle of 30o. Tearing along crystallographic angles suggests the tears occur along zigzag and armchair configurations with high fidelity of the edge morphology. We acknowledge the financial support from the DST, Government of India. SS acknowledges support from the NSF (DMR-1508680).

Adsorbate-induced reconstruction in the phase 1 × 2-3H/Rh(110)

NASA Astrophysics Data System (ADS)

Michl, M.; Nichtl-Pecher, W.; Oed, W.; Landskron, H.; Heinz, K.; Müller, K.

1989-10-01

The 1 × 2-3H superstructure of hydrogen on Rh(110) at coverage θ = {3}/{2} is analysed by low energy electron diffraction at 90 K. The spectra of eight beams are recorded with a computer-controlled TV measurement technique which yields low noise data even for weak superstructure spots by multiple averaging. Comparison to full dynamical calculations shows that a kinematic treatment of the hydrogen layer diffraction coupled to the full dynamical diffraction of the substrate is a very good approximation. Spectra computed in this way are compared with experimental data by R-factor evaluation. The three non-equivalent hydrogen atoms are found to adsorb in quasi-three-fold coordinated adsorption sites with slightly different local configurations and with H-Rh bond lengths between 1.87 and 1.93 Å to the first-layer rhodium atoms. Interaction between the adatoms seems to weaken the bonding to the adjacent atom in the second layer, so that H-Rh bond lengths larger than 2.17 Å result. A slight reconstruction of the substrate is necessary to bring superstructure spot intensities near the experimentally observed level. Rhodium atoms bonded to two hydrogen atoms are moved out of the surface by 0.03 ± 0.02 Å relative to Rh atoms bonded to only a single H atom. The relaxation of the first Rh layer spacing is determined to be {d 12}/{d 0} = -3.8 ± 1% and {d 22}/{d 0} = 0 ± 1% . The best fit Pendry R-factor is 0.33.

STM studies of an atomic-scale gate electrode formed by a single charged vacancy in GaAs

NASA Astrophysics Data System (ADS)

Lee, Donghun; Daughton, David; Gupta, Jay

2009-03-01

Electric-field control of spin-spin interactions at the atomic level is desirable for the realization of spintronics and spin-based quantum computation. Here we demonstrate the realization of an atomic-scale gate electrode formed by a single charged vacancy on the GaAs(110) surface[1]. We can position these vacancies with atomic precision using the tip of a home-built, low temperature STM. Tunneling spectroscopy of single Mn acceptors is used to quantify the electrostatic field as a function of distance from the vacancy. Single Mn acceptors are formed by substituting Mn adatoms for Ga atoms in the first layer of the p-GaAs(110) surface[2]. Depending on the distance, the in-gap resonance of single Mn acceptors can shift as much as 200meV. Our data indicate that the electrostatic field decays according to a screened Coulomb potential. The charge state of the vacancy can be switched to neutral, as evidenced by the Mn resonance returning to its unperturbed position. Reversible control of the local electric field as well as charged states of defects in semiconductors can open new insights such as realizing an atomic-scale gate control and studying spin-spin interactions in semiconductors. http://www.physics.ohio-state.edu/sim jgupta [1] D. Lee and J.A. Gupta (in preparation) [2] D. Kitchen et al., Nature 442, 436-439 (2006)

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

Wang, Lin -Lin; Johnson, Duane D.; Tringides, Michael C.

Density functional theory is used to study structural energetics of Pb vacancy cluster formation on C 60/Pb/Si(111) to explain the unusually fast and error-free transformations between the “Devil's Staircase” (DS) phases on the Pb/Si(111) wetting layer at low temperature (~110K). The formation energies of vacancy clusters are calculated in C 60/Pb/Si(111) as Pb atoms are progressively ejected from the initial dense Pb wetting layer. Vacancy clusters larger than five Pb atoms are found to be stable with seven being the most stable, while vacancy clusters smaller than five are highly unstable, which agrees well with the observed ejection rate ofmore » ~5 Pb atoms per C 60. Furthermore, the high energy cost (~0.8 eV) for the small vacancy clusters to form indicates convincingly that the unusually fast transformation observed experimentally between the DS phases, upon C 60 adsorption at low temperature, cannot be the result of single-atom random walk diffusion but of correlated multi-atom processes.« less

Understanding and Controlling the Aggregative Growth of Platinum Nanoparticles in Atomic Layer Deposition: An Avenue to Size Selection

PubMed Central

2017-01-01

We present an atomistic understanding of the evolution of the size distribution with temperature and number of cycles in atomic layer deposition (ALD) of Pt nanoparticles (NPs). Atomistic modeling of our experiments teaches us that the NPs grow mostly via NP diffusion and coalescence rather than through single-atom processes such as precursor chemisorption, atom attachment, and Ostwald ripening. In particular, our analysis shows that the NP aggregation takes place during the oxygen half-reaction and that the NP mobility exhibits a size- and temperature-dependent scaling. Finally, we show that contrary to what has been widely reported, in general, one cannot simply control the NP size by the number of cycles alone. Instead, while the amount of Pt deposited can be precisely controlled over a wide range of temperatures, ALD-like precision over the NP size requires low deposition temperatures (e.g., T < 100 °C) when growth is dominated by atom attachment. PMID:28178779

Selective Nanoscale Mass Transport across Atomically Thin Single Crystalline Graphene Membranes.

PubMed

Kidambi, Piran R; Boutilier, Michael S H; Wang, Luda; Jang, Doojoon; Kim, Jeehwan; Karnik, Rohit

2017-05-01

Atomically thin single crystals, without grain boundaries and associated defect clusters, represent ideal systems to study and understand intrinsic defects in materials, but probing them collectively over large area remains nontrivial. In this study, the authors probe nanoscale mass transport across large-area (≈0.2 cm 2 ) single-crystalline graphene membranes. A novel, polymer-free picture frame assisted technique, coupled with a stress-inducing nickel layer is used to transfer single crystalline graphene grown on silicon carbide substrates to flexible polycarbonate track etched supports with well-defined cylindrical ≈200 nm pores. Diffusion-driven flow shows selective transport of ≈0.66 nm hydrated K + and Cl - ions over ≈1 nm sized small molecules, indicating the presence of selective sub-nanometer to nanometer sized defects. This work presents a framework to test the barrier properties and intrinsic quality of atomically thin materials at the sub-nanometer to nanometer scale over technologically relevant large areas, and suggests the potential use of intrinsic defects in atomically thin materials for molecular separations or desalting. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Interaction between single gold atom and the graphene edge: A study via aberration-corrected transmission electron microscopy

NASA Astrophysics Data System (ADS)

Wang, Hongtao; Li, Kun; Cheng, Yingchun; Wang, Qingxiao; Yao, Yingbang; Schwingenschlögl, Udo; Zhang, Xixiang; Yang, Wei

2012-04-01

Interaction between single noble metal atoms and graphene edges has been investigated via aberration-corrected and monochromated transmission electron microscopy. A collective motion of the Au atom and the nearby carbon atoms is observed in transition between energy-favorable configurations. Most trapping and detrapping processes are assisted by the dangling carbon atoms, which are more susceptible to knock-on displacements by electron irradiation. Thermal energy is lower than the activation barriers in transition among different energy-favorable configurations, which suggests electron-beam irradiation can be an efficient way of engineering the graphene edge with metal atoms.Interaction between single noble metal atoms and graphene edges has been investigated via aberration-corrected and monochromated transmission electron microscopy. A collective motion of the Au atom and the nearby carbon atoms is observed in transition between energy-favorable configurations. Most trapping and detrapping processes are assisted by the dangling carbon atoms, which are more susceptible to knock-on displacements by electron irradiation. Thermal energy is lower than the activation barriers in transition among different energy-favorable configurations, which suggests electron-beam irradiation can be an efficient way of engineering the graphene edge with metal atoms. Electronic supplementary information (ESI) available: Additional Figures for characterization of mono-layer CVD graphene samples with free edges and Pt atoms decorations and analysis of the effect of electron irradiation; supporting movie on edge evolution. See DOI: 10.1039/c2nr00059h

Coherent multilayer crystals and method of making

DOEpatents

Schuller, I.K.; Falco, C.M.

1980-10-30

A new material is described consisting of a coherent multilayer crystal of two or more elements where each layer is composed of a single element. Each layer may vary in thickness from about 2 A to 2500 A. The multilayer crystals are prepared by sputter deposition under conditions which slow the sputtered atoms to near substrate temperatures before they contact the substrate.

Development of W/C soft x-ray multilayer mirror by ion beam sputtering (IBS) system for below 50A wavelength

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

Biswas, A.; Bhattacharyya, D.

A home-made Ion Beam Sputtering (IBS) system has been developed in our laboratory. Using the IBS system single layer W and single layer C film has been deposited at 1000eV Ar ion energy and 10mA ion current. The W-film has been characterized by grazing Incidence X-ray reflectrometry (GIXR) technique and Atomic Force Microscope technique. The single layer C-film has been characterized by Spectroscopic Ellipsometric technique. At the same deposition condition 25-layer W/C multilayer film has been deposited which has been designed for using as mirror at 30 Degree-Sign grazing incidence angle around 50A wavelength. The multilayer sample has been characterizedmore » by measuring reflectivity of CuK{alpha} radiation and soft x-ray radiation around 50A wavelength.« less

Single-unit-cell layer established Bi 2 WO 6 3D hierarchical architectures: Efficient adsorption, photocatalysis and dye-sensitized photoelectrochemical performance

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

Huang, Hongwei; Cao, Ranran; Yu, Shixin

Single-layer catalysis sparks huge interests and gains widespread attention owing to its high activity. Simultaneously, three-dimensional (3D) hierarchical structure can afford large surface area and abundant reactive sites, contributing to high efficiency. Herein, we report an absorbing single-unit-cell layer established Bi2WO6 3D hierarchical architecture fabricated by a sodium dodecyl benzene sulfonate (SDBS)-assisted assembled strategy. The DBS- long chains can adsorb on the (Bi2O2)2+ layers and hence impede stacking of the layers, resulting in the single-unit-cell layer. We also uncovered that SDS with a shorter chain is less effective than SDBS. Due to the sufficient exposure of surface O atoms, single-unit-cellmore » layer 3D Bi2WO6 shows strong selectivity for adsorption on multiform organic dyes with different charges. Remarkably, the single-unit-cell layer 3D Bi2WO6 casts profoundly enhanced photodegradation activity and especially a superior photocatalytic H2 evolution rate, which is 14-fold increase in contrast to the bulk Bi2WO6. Systematic photoelectrochemical characterizations disclose that the substantially elevated carrier density and charge separation efficiency take responsibility for the strengthened photocatalytic performance. Additionally, the possibility of single-unit-cell layer 3D Bi2WO6 as dye-sensitized solar cells (DSSC) has also been attempted and it was manifested to be a promising dye-sensitized photoanode for oxygen evolution reaction (ORR). Our work not only furnish an insight into designing single-layer assembled 3D hierarchical architecture, but also offer a multi-functional material for environmental and energy applications.« less

Diverse and tunable electronic structures of single-layer metal phosphorus trichalcogenides for photocatalytic water splitting

NASA Astrophysics Data System (ADS)

Liu, Jian; Li, Xi-Bo; Wang, Da; Lau, Woon-Ming; Peng, Ping; Liu, Li-Min

2014-02-01

The family of bulk metal phosphorus trichalcogenides (APX3, A = MII, M_{0.5}^IM_{0.5}^{III}; X = S, Se; MI, MII, and MIII represent Group-I, Group-II, and Group-III metals, respectively) has attracted great attentions because such materials not only own magnetic and ferroelectric properties, but also exhibit excellent properties in hydrogen storage and lithium battery because of the layered structures. Many layered materials have been exfoliated into two-dimensional (2D) materials, and they show distinct electronic properties compared with their bulks. Here we present a systematical study of single-layer metal phosphorus trichalcogenides by density functional theory calculations. The results show that the single layer metal phosphorus trichalcogenides have very low formation energies, which indicates that the exfoliation of single layer APX3 should not be difficult. The family of single layer metal phosphorus trichalcogenides exhibits a large range of band gaps from 1.77 to 3.94 eV, and the electronic structures are greatly affected by the metal or the chalcogenide atoms. The calculated band edges of metal phosphorus trichalcogenides further reveal that single-layer ZnPSe3, CdPSe3, Ag0.5Sc0.5PSe3, and Ag0.5In0.5PX3 (X = S and Se) have both suitable band gaps for visible-light driving and sufficient over-potentials for water splitting. More fascinatingly, single-layer Ag0.5Sc0.5PSe3 is a direct band gap semiconductor, and the calculated optical absorption further convinces that such materials own outstanding properties for light absorption. Such results demonstrate that the single layer metal phosphorus trichalcogenides own high stability, versatile electronic properties, and high optical absorption, thus such materials have great chances to be high efficient photocatalysts for water-splitting.

Direct Observation of Charge Transfer at a MgO(111) Surface

NASA Astrophysics Data System (ADS)

Subramanian, A.; Marks, L. D.; Warschkow, O.; Ellis, D. E.

2004-01-01

Transmission electron diffraction (TED) combined with direct methods have been used to study the √(3)×√(3)R30° reconstruction on the polar (111) surface of MgO and refine the valence charge distribution. The surface is nonstoichiometric and is terminated by a single magnesium atom. A charge-compensating electron hole is localized in the next oxygen layer and there is a nominal charge transfer from the oxygen atoms to the top magnesium atom. The partial charges that we obtain for the surface atoms are in reasonable agreement with empirical bond-valence estimations.

Ferromagnetism in CVT grown tungsten diselenide single crystals with nickel doping

NASA Astrophysics Data System (ADS)

Habib, Muhammad; Muhammad, Zahir; Khan, Rashid; Wu, Chuanqiang; Rehman, Zia ur; Zhou, Yu; Liu, Hengjie; Song, Li

2018-03-01

Two dimensional (2D) single crystal layered transition materials have had extensive consideration owing to their interesting magnetic properties, originating from their lattices and strong spin-orbit coupling, which make them of vital importance for spintronic applications. Herein, we present synthesis of a highly crystalline tungsten diselenide layered single crystal grown by chemical vapor transport technique and doped with nickel (Ni) to tailor its magnetic properties. The pristine WSe2 single crystal and Ni-doped crystal were characterized and analyzed for magnetic properties using both experimental and computational aspects. It was found that the magnetic behavior of the 2D layered WSe2 crystal changed from diamagnetic to ferromagnetic after Ni-doping at all tested temperatures. Moreover, first principle density functional theory (DFT) calculations further confirmed the origin of room temperature ferromagnetism of Ni-doped WSe2, where the d-orbitals of the doped Ni atom promoted the spin moment and thus largely contributed to the magnetism change in the 2D layered material.

Water Desalination Using Nanoporous Single-Layer Graphene with Tunable Pore Size

DOE PAGES

Surwade, Sumedh P.; Smirnov, Sergei N.; Vlassiouk, Ivan V.; ...

2015-03-23

Graphene has great potential to serve as a separation membrane due to its unique properties such as chemical and mechanical stability, flexibility and most importantly its one-atom thickness. In this study, we demonstrate first experimental evidence of the use of single-layer porous graphene as a desalination membrane. Nanometer-sized pores are introduced into single layer graphene using a convenient oxygen plasma etching process that permits tuning of the pore size. The resulting porous graphene membrane exhibited high rejection of salt ions and rapid water transport, thus functioning as an efficient water desalination membrane. Salt rejection selectivity of nearly 100% and exceptionallymore » high water fluxes exceeding 105 g m-2 s-1 at 40 C were measured using saturated water vapor as a driving force.« less

Prediction and Measurement of Temperature Fields in Silicon-on-Insulator Electronic Circuits

DTIC Science & Technology

1995-08-01

common dimensions are given in Table 1. Almost all of the device power is dissipated in the channel. The electri- cally insulating implanted layer...data. Region or Component substrate Material SOI implanted insulating layers single-crystal silicon, 3 x 1015 boron atoms cm -3 Thermal... implanted silicon-dioxide layer in SOI wafers. The data for each device for varying powers fall near a line originating at P = 0 and T0 = 303 K

Damage of multilayer optics with varying capping layers induced by focused extreme ultraviolet beam

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

Jody Corso, Alain; Nicolosi, Piergiorgio; Nardello, Marco

2013-05-28

Extreme ultraviolet Mo/Si multilayers protected by capping layers of different materials were exposed to 13.5 nm plasma source radiation generated with a table-top laser to study the irradiation damage mechanism. Morphology of single-shot damaged areas has been analyzed by means of atomic force microscopy. Threshold fluences were evaluated for each type of sample in order to determine the capability of the capping layer to protect the structure underneath.

Infiltrating a thin or single-layer opal with an atomic vapour: Sub-Doppler signals and crystal optics

NASA Astrophysics Data System (ADS)

Moufarej, Elias; Maurin, Isabelle; Zabkov, Ilya; Laliotis, Athanasios; Ballin, Philippe; Klimov, Vasily; Bloch, Daniel

2014-10-01

Artificial thin glass opals can be infiltrated with a resonant alkali-metal vapour, providing novel types of hybrid systems. The reflection at the interface between the substrate and the opal yields a resonant signal, which exhibits sub-Doppler structures in linear spectroscopy for a range of oblique incidences. This result is suspected to originate in an effect of the three-dimensional confinement of the vapour in the opal interstices. It is here extended to a situation where the opal is limited to a few- or even a single-layer opal film, which is a kind of bidimensional grating. We have developed a flexible one-dimensional layered optical model, well suited for a Langmuir-Blodgett opal. Once extended to the case of a resonant infiltration, the model reproduces quick variations of the lineshape with incidence angle or polarization. Alternately, for an opal limited to a single layer of identical spheres, a three-dimensional numerical calculation was developed. It predicts crystalline anisotropy, which is demonstrated through diffraction on an empty opal made of a single layer of polystyrene spheres.

From Single Atoms to Nanoparticles: Autocatalysis and Metal Aggregation in Atomic Layer Deposition of Pt on TiO2 Nanopowder.

PubMed

Grillo, Fabio; Van Bui, Hao; La Zara, Damiano; Aarnink, Antonius A I; Kovalgin, Alexey Y; Kooyman, Patricia; Kreutzer, Michiel T; van Ommen, Jan Rudolf

2018-06-01

A fundamental understanding of the interplay between ligand-removal kinetics and metal aggregation during the formation of platinum nanoparticles (NPs) in atomic layer deposition of Pt on TiO 2 nanopowder using trimethyl(methylcyclo-pentadienyl)platinum(IV) as the precursor and O 2 as the coreactant is presented. The growth follows a pathway from single atoms to NPs as a function of the oxygen exposure (P O2 × time). The growth kinetics is modeled by accounting for the autocatalytic combustion of the precursor ligands via a variant of the Finke-Watzky two-step model. Even at relatively high oxygen exposures (<120 mbar s) little to no Pt is deposited after the first cycle and most of the Pt is atomically dispersed. Increasing the oxygen exposure above 120 mbar s results in a rapid increase in the Pt loading, which saturates at exposures > 120 mbar s. The deposition of more Pt leads to the formation of NPs that can be as large as 6 nm. Crucially, high P O2 (≥5 mbar) hinders metal aggregation, thus leading to narrow particle size distributions. The results show that ALD of Pt NPs is reproducible across small and large surface areas if the precursor ligands are removed at high P O2 . © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Graded Index Silicon Geranium on Lattice Matched Silicon Geranium Semiconductor Alloy

NASA Technical Reports Server (NTRS)

Park, Yeonjoon (Inventor); Choi, Sang H. (Inventor); King, Glen C. (Inventor); Elliott, James R., Jr. (Inventor); Stoakley, Diane M. (Inventor)

2009-01-01

A lattice matched silicon germanium (SiGe) semiconductive alloy is formed when a {111} crystal plane of a cubic diamond structure SiGe is grown on the {0001} C-plane of a single crystalline Al2O3 substrate such that a <110> orientation of the cubic diamond structure SiGe is aligned with a <1,0,-1,0> orientation of the {0001} C-plane. A lattice match between the substrate and the SiGe is achieved by using a SiGe composition that is 0.7223 atomic percent silicon and 0.2777 atomic percent germanium. A layer of Si(1-x), ,Ge(x) is formed on the cubic diamond structure SiGe. The value of X (i) defines an atomic percent of germanium satisfying 0.2277

Diverse forms of bonding in two-dimensional Si allotropes: Nematic orbitals in the MoS2 structure

NASA Astrophysics Data System (ADS)

Gimbert, Florian; Lee, Chi-Cheng; Friedlein, Rainer; Fleurence, Antoine; Yamada-Takamura, Yukiko; Ozaki, Taisuke

2014-10-01

The interplay of sp2- and sp3-type bonding defines silicon allotropes in two- and three-dimensional forms. A two-dimensional phase bearing structural resemblance to a single MoS2 layer is found to possess a lower total energy than low-buckled silicene and to be stable in terms of its phonon dispersion relations. A set of cigar-shaped nematic orbitals originating from the Si sp2 orbitals realizes bonding with a sixfold coordination of the inner Si atoms of the layer. The identification of these nematic orbitals advocates diverse Si bonding configurations different from those of C atoms.

Single ether group in a glycol-based ultra-thin layer prevents surface fouling from undiluted serum.

PubMed

Sheikh, Sonia; Yang, David Yi; Blaszykowski, Christophe; Thompson, Michael

2012-01-30

Through systematic structural modification, it is shown that the internal, single oxygen atom of simple monoethylene glycol-based organic films is essential for radically altering the fouling behaviour of quartz against undiluted serum, as characterized by the electromagnetic piezoelectric acoustic sensor. The synergy is strongest with distal hydroxyls.

Diffusion of One-Dimensional Crystals in Channels of Single-Walled Carbon Nanotubes

NASA Astrophysics Data System (ADS)

Zhigalina, V. G.; Kumskov, A. S.; Falaleev, N. S.; Vasiliev, A. L.; Kiselev, N. A.

2018-05-01

The transport of one-dimensional CuI crystals in channels of single-walled carbon nanotubes (SWCNTs) has been studied by high resolution electron microscopy. The diffusion kinetics has been investigated by counting the number of CuI atoms escaping from the nanotube channel. The diffusivity is calculated to be 6.8 × 10-21 m2/s, which corresponds to an activation-barrier height of 1 eV/atom. A comparison with the theoretically estimated height of the energy barrier for molecular transport through a graphene layer is indicative of mass transfer through vacancy defects in graphene.

Mechanical properties of atomically thin boron nitride and the role of interlayer interactions

PubMed Central

Falin, Aleksey; Cai, Qiran; Santos, Elton J. G.; Scullion, Declan; Qian, Dong; Zhang, Rui; Yang, Zhi; Huang, Shaoming; Watanabe, Kenji; Taniguchi, Takashi; Barnett, Matthew R.; Chen, Ying; Ruoff, Rodney S.; Li, Lu Hua

2017-01-01

Atomically thin boron nitride (BN) nanosheets are important two-dimensional nanomaterials with many unique properties distinct from those of graphene, but investigation into their mechanical properties remains incomplete. Here we report that high-quality single-crystalline mono- and few-layer BN nanosheets are one of the strongest electrically insulating materials. More intriguingly, few-layer BN shows mechanical behaviours quite different from those of few-layer graphene under indentation. In striking contrast to graphene, whose strength decreases by more than 30% when the number of layers increases from 1 to 8, the mechanical strength of BN nanosheets is not sensitive to increasing thickness. We attribute this difference to the distinct interlayer interactions and hence sliding tendencies in these two materials under indentation. The significantly better interlayer integrity of BN nanosheets makes them a more attractive candidate than graphene for several applications, for example, as mechanical reinforcements. PMID:28639613

Effects of Stone-Wales and vacancy defects in atomic-scale friction on defective graphite

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

Sun, Xiao-Yu; Key Laboratory of Hubei Province for Water Jet Theory and New Technology, Wuhan University, Wuhan 430072; Wu, RunNi

2014-05-05

Graphite is an excellent solid lubricant for surface coating, but its performance is significantly weakened by the vacancy or Stone-Wales (SW) defect. This study uses molecular dynamics simulations to explore the frictional behavior of a diamond tip sliding over a graphite which contains a single defect or stacked defects. Our results suggest that the friction on defective graphite shows a strong dependence on defect location and type. The 5-7-7-5 structure of SW defect results in an effectively negative slope of friction. For defective graphite containing a defect in the surface, adding a single vacancy in the interior layer will decreasemore » the friction coefficients, while setting a SW defect in the interior layer may increase the friction coefficients. Our obtained results may provide useful information for understanding the atomic-scale friction properties of defective graphite.« less

Nanocrystalline-to-amorphous transition in nanolaminates grown by low temperature atomic layer deposition and related mechanical properties

NASA Astrophysics Data System (ADS)

Raghavan, R.; Bechelany, M.; Parlinska, M.; Frey, D.; Mook, W. M.; Beyer, A.; Michler, J.; Utke, I.

2012-05-01

We report on a comprehensive structural and nanoindentation study of nanolaminates of Al2O3 and ZnO synthesized by atomic layer deposition (ALD). By reducing the bilayer thickness from 50 nm to below 1 nm, the nanocrystal size could be controlled in the nanolaminate structure. The softer and more compliant response of the multilayers as compared to the single layers of Al2O3 and ZnO is attributed to the structural change from nanocrystalline to amorphous at smaller bilayer thicknesses. It is also shown that ALD is a unique technique for studying the inverse Hall-Petch softening mechanism (E. Voce and D. Tabor, J. Inst. Metals 79(12), 465 (1951)) related to grain size effects in nanomaterials.

Dynamical Disentangling and Cooling of Atoms in Bilayer Optical Lattices

NASA Astrophysics Data System (ADS)

Kantian, A.; Langer, S.; Daley, A. J.

2018-02-01

We show how experimentally available bilayer lattice systems can be used to prepare quantum many-body states with exceptionally low entropy in one layer, by dynamically disentangling the two layers. This disentangling operation moves one layer—subsystem A —into a regime where excitations in A develop a single-particle gap. As a result, this operation maps directly to cooling for subsystem A , with entropy being shuttled to the other layer. For both bosonic and fermionic atoms, we study the corresponding dynamics showing that disentangling can be realized cleanly in ongoing experiments. The corresponding entanglement entropies are directly measurable with quantum gas microscopes, and, as a tool for producing lower-entropy states, this technique opens a range of applications beginning with simplifying production of magnetically ordered states of bosons and fermions.

Electronics and optoelectronics of two-dimensional transition metal dichalcogenides.

PubMed

Wang, Qing Hua; Kalantar-Zadeh, Kourosh; Kis, Andras; Coleman, Jonathan N; Strano, Michael S

2012-11-01

The remarkable properties of graphene have renewed interest in inorganic, two-dimensional materials with unique electronic and optical attributes. Transition metal dichalcogenides (TMDCs) are layered materials with strong in-plane bonding and weak out-of-plane interactions enabling exfoliation into two-dimensional layers of single unit cell thickness. Although TMDCs have been studied for decades, recent advances in nanoscale materials characterization and device fabrication have opened up new opportunities for two-dimensional layers of thin TMDCs in nanoelectronics and optoelectronics. TMDCs such as MoS(2), MoSe(2), WS(2) and WSe(2) have sizable bandgaps that change from indirect to direct in single layers, allowing applications such as transistors, photodetectors and electroluminescent devices. We review the historical development of TMDCs, methods for preparing atomically thin layers, their electronic and optical properties, and prospects for future advances in electronics and optoelectronics.

Synthesis of Epitaxial Single-Layer MoS2 on Au(111).

PubMed

Grønborg, Signe S; Ulstrup, Søren; Bianchi, Marco; Dendzik, Maciej; Sanders, Charlotte E; Lauritsen, Jeppe V; Hofmann, Philip; Miwa, Jill A

2015-09-08

We present a method for synthesizing large area epitaxial single-layer MoS2 on the Au(111) surface in ultrahigh vacuum. Using scanning tunneling microscopy and low energy electron diffraction, the evolution of the growth is followed from nanoscale single-layer MoS2 islands to a continuous MoS2 layer. An exceptionally good control over the MoS2 coverage is maintained using an approach based on cycles of Mo evaporation and sulfurization to first nucleate the MoS2 nanoislands and then gradually increase their size. During this growth process the native herringbone reconstruction of Au(111) is lifted as shown by low energy electron diffraction measurements. Within the MoS2 islands, we identify domains rotated by 60° that lead to atomically sharp line defects at domain boundaries. As the MoS2 coverage approaches the limit of a complete single layer, the formation of bilayer MoS2 islands is initiated. Angle-resolved photoemission spectroscopy measurements of both single and bilayer MoS2 samples show a dramatic change in their band structure around the center of the Brillouin zone. Brief exposure to air after removing the MoS2 layer from vacuum is not found to affect its quality.

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.

In-situ crystallization of GeTe\\GaSb phase change memory stacked films

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

Velea, A., E-mail: alin.velea@psi.ch; National Institute of Materials Physics, RO-077125 Magurele, Ilfov; Borca, C. N.

2014-12-21

Single and double layer phase change memory structures based on GeTe and GaSb thin films were deposited by pulsed laser deposition (PLD). Their crystallization behavior was studied using in-situ synchrotron techniques. Electrical resistance vs. temperature investigations, using the four points probe method, showed transition temperatures of 138 °C and 198 °C for GeTe and GaSb single films, respectively. It was found that after GeTe crystallization in the stacked films, Ga atoms from the GaSb layer diffused in the vacancies of the GeTe crystalline structure. Therefore, the crystallization temperature of the Sb-rich GaSb layer is decreased by more than 30 °C. Furthermore, at 210 °C,more » the antimony excess from GaSb films crystallizes as a secondary phase. At higher annealing temperatures, the crystalline Sb phase increased on the expense of GaSb crystalline phase which was reduced. Extended X-ray absorption fine structure (EXAFS) measurements at the Ga and Ge K-edges revealed changes in their local atomic environments as a function of the annealing temperature. Simulations unveil a tetrahedral configuration in the amorphous state and octahedral configuration in the crystalline state for Ge atoms, while Ga is four-fold coordinated in both as-deposited and annealed samples.« less

Sinter-Resistant Platinum Catalyst Supported by Metal-Organic Framework.

PubMed

Kim, In Soo; Li, Zhanyong; Zheng, Jian; Platero-Prats, Ana E; Mavrandonakis, Andreas; Pellizzeri, Steven; Ferrandon, Magali; Vjunov, Aleksei; Gallington, Leighanne C; Webber, Thomas E; Vermeulen, Nicolaas A; Penn, R Lee; Getman, Rachel B; Cramer, Christopher J; Chapman, Karena W; Camaioni, Donald M; Fulton, John L; Lercher, Johannes A; Farha, Omar K; Hupp, Joseph T; Martinson, Alex B F

2018-01-22

Single atoms and few-atom clusters of platinum are uniformly installed on the zirconia nodes of a metal-organic framework (MOF) NU-1000 via targeted vapor-phase synthesis. The catalytic Pt clusters, site-isolated by organic linkers, are shown to exhibit high catalytic activity for ethylene hydrogenation while exhibiting resistance to sintering up to 200 °C. In situ IR spectroscopy reveals the presence of both single atoms and few-atom clusters that depend upon synthesis conditions. Operando X-ray absorption spectroscopy and X-ray pair distribution analyses reveal unique changes in chemical bonding environment and cluster size stability while on stream. Density functional theory calculations elucidate a favorable reaction pathway for ethylene hydrogenation with the novel catalyst. These results provide evidence that atomic layer deposition (ALD) in MOFs is a versatile approach to the rational synthesis of size-selected clusters, including noble metals, on a high surface area support. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Facile fabrication of ultrathin Pt overlayers onto nanoporous metal membranes via repeated Cu UPD and in situ redox replacement reaction.

PubMed

Liu, Pengpeng; Ge, Xingbo; Wang, Rongyue; Ma, Houyi; Ding, Yi

2009-01-06

Ultrathin Pt films from one to several atomic layers are successfully decorated onto nanoporous gold (NPG) membranes by utilizing under potential deposition (UPD) of Cu onto Au or Pt surfaces, followed by in situ redox replacement reaction (RRR) of UPD Cu by Pt. The thickness of Pt layers can be controlled precisely by repeating the Cu-UPD-RRR cycles. TEM observations coupled with electrochemical testing suggest that the morphology of Pt overlayers changes from an ultrathin epitaxial film in the case of one or two atomic layers to well-dispersed nanoislands in the case of four and more atomic layers. Electron diffraction (ED) patterns confirm that the as-prepared NPG-Pt membranes maintain a single-crystalline structure, even though the thickness of Pt films reaches six atomic layers, indicating the decorated Pt films hold the same crystallographic relationship to the NPG substrate during the entire fabrication process. Due to the regular modulation of Pt utilization, the electrocatalytic activity of NPG-Pt exhibits interesting surface structure dependence in methanol, ethanol, and CO electrooxidation reactions. These novel bimetallic nanocatalysts show excellent electrocatalytic activity and much enhanced poison tolerance as compared to the commercial Pt/C catalysts. The success in the fabrication of NPG-Pt-type materials provides a new path to prepare electrocatalysts with ultralow Pt loading and high Pt utilization, which is of great significance in energy-related applications, such as direct alcohol fuel cells (DAFCs).

Control of the π plasmon in a single layer graphene by charge doping

NASA Astrophysics Data System (ADS)

Shin, S. Y.; Kim, N. D.; Kim, J. G.; Kim, K. S.; Noh, D. Y.; Kim, Kwang S.; Chung, J. W.

2011-08-01

We report that the behavior of a low-energy π plasmon excitation in a single layer graphene (SLG) can be modified by doping external potassium (K) atoms, a feature demanded to realize the graphene plasmonics. Using high-resolution electron-energy-loss spectroscopy, we find that upon K-doping the π plasmon energy increases by 1.1 eV due to the K-induced electron density up to n = 7 × 1013 cm-2 in SLG. The four modified dispersions for different K-dopings, however, are found to merge into a single universal curve when plotted in the dimensionless coordinates indicating that the unique plasmonic character of SLG is preserved despite the K-dopings.

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.

Monolayer PtSe 2 , a New Semiconducting Transition-Metal-Dichalcogenide, Epitaxially Grown by Direct Selenization of Pt

DOE PAGES

Wang, Yeliang; Li, Linfei; Yao, Wei; ...

2015-05-21

For single-layer transition-metal dichalcogenides (TMDs) receive significant attention due to their intriguing physical properties for both fundamental research and potential applications in electronics, optoelectronics, spintronics, catalysis, and so on. Here, we demonstrate the epitaxial growth of high-quality single-crystal, monolayer platinum diselenide (PtSe2), a new member of the layered TMDs family, by a single step of direct selenization of a Pt(111) substrate. We found that a combination of atomic-resolution experimental characterizations and first-principle theoretic calculations reveals the atomic structure of the monolayer PtSe2/Pt(111). Angle-resolved photoemission spectroscopy measurements confirm for the first time the semiconducting electronic structure of monolayer PtSe2 (in contrastmore » to its semimetallic bulk counterpart). The photocatalytic activity of monolayer PtSe2 film is evaluated by a methylene-blue photodegradation experiment, demonstrating its practical application as a promising photocatalyst. Moreover, circular polarization calculations predict that monolayer PtSe2 has also potential applications in valleytronics.« less

Two-Dimensional Superconductivity in the Cuprates Revealed by Atomic-Layer-by- Layer Molecular Beam Epitaxy

DOE PAGES

A. T. Bollinger; Bozovic, I.

2016-08-12

Various electronic phases displayed by cuprates that exhibit high temperature superconductivity continue to attract much interest. We provide a short review of several experiments that we have performed aimed at investigating the superconducting state in these compounds. Measurements on single-phase films, bilayers, and superlattices all point to the conclusion that the high-temperature superconductivity in these materials is an essentially quasi-two dimensional phenomenon. With proper control over the film growth, high-temperature superconductivity can exist in a single copper oxide plane with the critical temperatures as high as that achieved in the bulk samples.

Controlled Phase and Tunable Magnetism in Ordered Iron Oxide Nanotube Arrays Prepared by Atomic Layer Deposition

NASA Astrophysics Data System (ADS)

Zhang, Yijun; Liu, Ming; Peng, Bin; Zhou, Ziyao; Chen, Xing; Yang, Shu-Ming; Jiang, Zhuang-De; Zhang, Jie; Ren, Wei; Ye, Zuo-Guang

2016-01-01

Highly-ordered and conformal iron oxide nanotube arrays on an atomic scale are successfully prepared by atomic layer deposition (ALD) with controlled oxidization states and tunable magnetic properties between superparamagnetism and ferrimagnetism. Non-magnetic α-Fe2O3 and superparamagnetic Fe3O4 with a blocking temperature of 120 K are in-situ obtained by finely controlling the oxidation reaction. Both of them exhibit a very small grain size of only several nanometers due to the nature of atom-by-atom growth of the ALD technique. Post-annealing α-Fe2O3 in a reducing atmosphere leads to the formation of the spinel Fe3O4 phase which displays a distinct ferrimagnetic anisotropy and the Verwey metal-insulator transition that usually takes place only in single crystal magnetite or thick epitaxial films at low temperatures. The ALD deposition of iron oxide with well-controlled phase and tunable magnetism demonstrated in this work provides a promising opportunity for the fabrication of 3D nano-devices to be used in catalysis, spintronics, microelectronics, data storages and bio-applications.

Elementary defects in graphane

NASA Astrophysics Data System (ADS)

Podlivaev, A. I.; Openov, L. A.

2017-07-01

The main zero-dimensional defects in graphane, a completely hydrogenated single-layer graphene, having the chair-type conformation have been numerically simulated. The hydrogen and carbon-hydrogen vacancies, Stone-Wales defect, and "transmutation defect" resulting from the simultaneous hoppings of two hydrogen atoms between the neighboring carbon atoms have been considered. The energies of formations of these defects have been calculated and their effect on the electronic structure, phonon spectra, and Young modulus has been studied.

Local carrier distribution imaging on few-layer MoS2 exfoliated on SiO2 by scanning nonlinear dielectric microscopy

NASA Astrophysics Data System (ADS)

Yamasue, Kohei; Cho, Yasuo

2018-06-01

We demonstrate that scanning nonlinear dielectric microscopy (SNDM) can be used for the nanoscale characterization of dominant carrier distribution on atomically thin MoS2 mechanically exfoliated on SiO2. For stable imaging without damaging microscopy tips and samples, SNDM was combined with peak-force tapping mode atomic force microscopy. The identification of dominant carriers and their spatial distribution becomes possible even for single and few-layer MoS2 on SiO2 using the proposed method allowing differential capacitance (dC/dV) imaging. We can expect that SNDM can also be applied to the evaluation of other two-dimensional semiconductors and devices.

Control of thermal deformation in dielectric mirrors using mechanical design and atomic layer deposition.

PubMed

Gabriel, Nicholas T; Kim, Sangho S; Talghader, Joseph J

2009-07-01

A mechanical design technique for optical coatings that simultaneously controls thermal deformation and optical reflectivity is reported. The method requires measurement of the refractive index and thermal stress of single films prior to the design. Atomic layer deposition was used for deposition because of the high repeatability of the film constants. An Al2O3/HfO2 distributed Bragg reflector was deposited with a predicted peak reflectivity of 87.9% at 542.4 nm and predicted edge deformation of -360 nm/K on a 10 cm silicon substrate. The measured peak reflectivity was 85.7% at 541.7 nm with an edge deformation of -346 nm/K.

Detection of subsurface core-level shifts in Si 2p core-level photoemission from Si(111)-(1x1):As

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

Paggel, J.J.; Hasselblatt, M.; Horn, K.

1997-04-01

The (7 x 7) reconstruction of the Si(111) surface arises from a lowering energy through the reduction of the number of dangling bonds. This reconstruction can be removed by the adsorption of atoms such as hydrogen which saturate the dangling bonds, or by the incorporation of atoms, such as arsenic which, because of the additional electron it possesses, can form three bonds and a nonreactive lone pair orbital from the remaining two electrons. Core and valence level photoemission and ion scattering data have shown that the As atoms replace the top silicon atoms. Previous core level spectra were interpreted inmore » terms of a bulk and a single surface doublet. The authors present results demonstrate that the core level spectrum contains two more lines. The authors assign these to subsurface silicon layers which also experience changes in the charge distribution when a silicon atom is replaced by an arsenic atom. Subsurface core level shifts are not unexpected since the modifications of the electronic structure and/or of photohole screening are likely to decay into the bulk and not just to affect the top-most substrate atoms. The detection of subsurface components suggests that the adsorption of arsenic leads to charge flow also in the second double layer of the Si(111) surface. In view of the difference in atomic radius between As and Si, it was suggested that the (1 x 1): As surface is strained. The presence of charge rearrangement up to the second double layer implies that the atomic coordinates also exhibit deviations from their ideal Si(111) counterparts, which might be detected through a LEED I/V or photoelectron diffraction analysis.« less

A Simple Approach for Molecular Controlled Release based on Atomic Layer Deposition Hybridized Organic-Inorganic Layers

PubMed Central

Boehler, Christian; Güder, Firat; Kücükbayrak, Umut M.; Zacharias, Margit; Asplund, Maria

2016-01-01

On-demand release of bioactive substances with high spatial and temporal control offers ground-breaking possibilities in the field of life sciences. However, available strategies for developing such release systems lack the possibility of combining efficient control over release with adequate storage capability in a reasonably compact system. In this study we present a new approach to target this deficiency by the introduction of a hybrid material. This organic-inorganic material was fabricated by atomic layer deposition of ZnO into thin films of polyethylene glycol, forming the carrier matrix for the substance to be released. Sub-surface growth mechanisms during this process converted the liquid polymer into a solid, yet water-soluble, phase. This layer permits extended storage for various substances within a single film of only a few micrometers in thickness, and hence demands minimal space and complexity. Improved control over release of the model substance Fluorescein was achieved by coating the hybrid material with a conducting polymer film. Single dosage and repetitive dispensing from this system was demonstrated. Release was controlled by applying a bias potential of ±0.5 V to the polymer film enabling or respectively suppressing the expulsion of the model drug. In vitro tests showed excellent biocompatibility of the presented system. PMID:26791399

Kelvin-Helmholtz instability in a single-component atomic superfluid

NASA Astrophysics Data System (ADS)

Baggaley, A. W.; Parker, N. G.

2018-05-01

We demonstrate an experimentally feasible method for generating the classical Kelvin-Helmholtz instability in a single-component atomic Bose-Einstein condensate. By progressively reducing a potential barrier between two counterflowing channels, we seed a line of quantized vortices, which precede to form progressively larger clusters, mimicking the classical roll-up behavior of the Kelvin-Helmholtz instability. This cluster formation leads to an effective superfluid shear layer, formed through the collective motion of many quantized vortices. From this we demonstrate a straightforward method to measure the effective viscosity of a turbulent quantum fluid in a system with a moderate number of vortices, within the range of current experimental capabilities.

Nonlinear Ballistic Transport in an Atomically Thin Material.

PubMed

Boland, Mathias J; Sundararajan, Abhishek; Farrokhi, M Javad; Strachan, Douglas R

2016-01-26

Ultrashort devices that incorporate atomically thin components have the potential to be the smallest electronics. Such extremely scaled atomically thin devices are expected to show ballistic nonlinear behavior that could make them tremendously useful for ultrafast applications. While nonlinear diffusive electron transport has been widely reported, clear evidence for intrinsic nonlinear ballistic transport in the growing array of atomically thin conductors has so far been elusive. Here we report nonlinear electron transport of an ultrashort single-layer graphene channel that shows quantitative agreement with intrinsic ballistic transport. This behavior is shown to be distinctly different than that observed in similarly prepared ultrashort devices consisting, instead, of bilayer graphene channels. These results suggest that the addition of only one extra layer of an atomically thin material can make a significant impact on the nonlinear ballistic behavior of ultrashort devices, which is possibly due to the very different chiral tunneling of their charge carriers. The fact that we observe the nonlinear ballistic response at room temperature, with zero applied magnetic field, in non-ultrahigh vacuum conditions and directly on a readily accessible oxide substrate makes the nanogap technology we utilize of great potential for achieving extremely scaled high-speed atomically thin devices.

Raman and electronic transport characterization of few- and single-layer-thick α-RuCl3

NASA Astrophysics Data System (ADS)

Zhou, Boyi; Henriksen, Erik

The layered magnetic semiconductor α-RuCl3, having a honeycomb lattice of spin-1/2 moments, has been identified as a potential candidate material to realize the Kitaev quantum spin liquid. In particular, bulk RuCl3 crystals have been studied and found to be on the cusp of manifesting QSL behavior. As the QSL is primarily a two-dimensional phenomenon, and since the layers of RuCl3 are weakly coupled, we propose to create and study a 2D spin-1/2 honeycomb system by isolating single sheets. Here we report the exfoliation of RuCl3 down to few- and single-layer-thick samples, which we characterize by Raman spectroscopy and atomic force microscopy at room temperature. We will also report our progress on measurements of basic electronic transport properties in the 2D RuCl3 system by controlling the chemical potential via gating in a field-effect configuration.

Spectroellipsometric detection of silicon substrate damage caused by radiofrequency sputtering of niobium oxide

NASA Astrophysics Data System (ADS)

Lohner, Tivadar; Serényi, Miklós; Szilágyi, Edit; Zolnai, Zsolt; Czigány, Zsolt; Khánh, Nguyen Quoc; Petrik, Péter; Fried, Miklós

2017-11-01

Substrate surface damage induced by deposition of metal atoms by radiofrequency (rf) sputtering or ion beam sputtering onto single-crystalline silicon (c-Si) surface has been characterized earlier by electrical measurements. The question arises whether it is possible to characterize surface damage using spectroscopic ellipsometry (SE). In our experiments niobium oxide layers were deposited by rf sputtering on c-Si substrates in gas mixture of oxygen and argon. Multiple angle of incidence spectroscopic ellipsometry measurements were performed, a four-layer optical model (surface roughness layer, niobium oxide layer, native silicon oxide layer and ion implantation-amorphized silicon [i-a-Si] layer on a c-Si substrate) was created in order to evaluate the spectra. The evaluations yielded thicknesses of several nm for the i-a-Si layer. Better agreement could be achieved between the measured and the generated spectra by inserting a mixed layer (with components of c-Si and i-a-Si applying the effective medium approximation) between the silicon oxide layer and the c-Si substrate. High depth resolution Rutherford backscattering (RBS) measurements were performed to investigate the interface disorder between the deposited niobium oxide layer and the c-Si substrate. Atomic resolution cross-sectional transmission electron microscopy investigation was applied to visualize the details of the damaged subsurface region of the substrate.

Diverse and tunable electronic structures of single-layer metal phosphorus trichalcogenides for photocatalytic water splitting

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

Liu, Jian; Beijing Computational Science Research Center, Beijing 100084; College of Electrical and Information Engineering, Hunan Institute of Engineering, Xiangtan 411105, Hunan

2014-02-07

The family of bulk metal phosphorus trichalcogenides (APX{sub 3}, A = M{sup II}, M{sub 0.5}{sup I}M{sub 0.5}{sup III}; X = S, Se; M{sup I}, M{sup II}, and M{sup III} represent Group-I, Group-II, and Group-III metals, respectively) has attracted great attentions because such materials not only own magnetic and ferroelectric properties, but also exhibit excellent properties in hydrogen storage and lithium battery because of the layered structures. Many layered materials have been exfoliated into two-dimensional (2D) materials, and they show distinct electronic properties compared with their bulks. Here we present a systematical study of single-layer metal phosphorus trichalcogenides by density functionalmore » theory calculations. The results show that the single layer metal phosphorus trichalcogenides have very low formation energies, which indicates that the exfoliation of single layer APX{sub 3} should not be difficult. The family of single layer metal phosphorus trichalcogenides exhibits a large range of band gaps from 1.77 to 3.94 eV, and the electronic structures are greatly affected by the metal or the chalcogenide atoms. The calculated band edges of metal phosphorus trichalcogenides further reveal that single-layer ZnPSe{sub 3}, CdPSe{sub 3}, Ag{sub 0.5}Sc{sub 0.5}PSe{sub 3}, and Ag{sub 0.5}In{sub 0.5}PX{sub 3} (X = S and Se) have both suitable band gaps for visible-light driving and sufficient over-potentials for water splitting. More fascinatingly, single-layer Ag{sub 0.5}Sc{sub 0.5}PSe{sub 3} is a direct band gap semiconductor, and the calculated optical absorption further convinces that such materials own outstanding properties for light absorption. Such results demonstrate that the single layer metal phosphorus trichalcogenides own high stability, versatile electronic properties, and high optical absorption, thus such materials have great chances to be high efficient photocatalysts for water-splitting.« less

Surface morphological evolution of epitaxial CrN(001) layers

NASA Astrophysics Data System (ADS)

Frederick, J. R.; Gall, D.

2005-09-01

CrN layers, 57 and 230 nm thick, were grown on MgO(001) at Ts=600-800 °C by ultrahigh-vacuum magnetron sputter deposition in pure N2 discharges from an oblique deposition angle α=80°. Layers grown at 600 °C nucleate as single crystals with a cube-on-cube epitaxial relationship with the substrate. However, rough surfaces with cauliflower-type morphologies cause the nucleation of misoriented CrN grains that develop into cone-shaped grains that protrude out of the epitaxial matrix to form triangular faceted surface mounds. The surface morphology of epitaxial CrN(001) grown at 700 °C is characterized by dendritic ridge patterns extending along the orthogonal <110> directions superposed by square-shaped super mounds with <100> edges. The ridge patterns are attributed to a Bales-Zangwill instability while the supermounds form due to atomic shadowing which leads to the formation of epitaxial inverted pyramids that are separated from the surrounding layer by tilted nanovoids. Growth at 800 °C yields complete single crystals with smooth surfaces. The root-mean-square surface roughness for 230-nm-thick layers decreases from 18.8 to 9.3 to 1.1 nm as Ts is raised from 600 to 700 to 800 °C. This steep decrease is due to a transition in the roughening mechanism from atomic shadowing to kinetic roughening. Atomic shadowing is dominant at 600 and 700 °C, where misoriented grains and supermounds, respectively, capture a larger fraction of the oblique deposition flux in comparison to the surrounding epitaxial matrix, resulting in a high roughening rate that is described by a power law with an exponent β>0.5. In contrast, kinetic roughening controls the surface morphology for Ts=800 °C, as well as the epitaxial fraction of the layers grown at 600 and 700 °C, yielding relatively smooth surfaces and β<=0.27.

Atomic-Level Sculpting of Crystalline Oxides: Toward Bulk Nanofabrication with Single Atomic Plane Precision

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

Jesse, Stephen; He, Qian; Lupini, Andrew R.

2015-10-19

We demonstrate atomic-level sculpting of 3D crystalline oxide nanostructures from metastable amorphous layer in a scanning transmission electron microscope (STEM). Strontium titanate nanostructures grow epitaxially from the crystalline substrate following the beam path. This method can be used for fabricating crystalline structures as small as 1-2 nm and the process can be observed in situ with atomic resolution. We further demonstrate fabrication of arbitrary shape structures via control of the position and scan speed of the electron beam. Combined with broad availability of the atomic resolved electron microscopy platforms, these observations suggest the feasibility of large scale implementation of bulkmore » atomic-level fabrication as a new enabling tool of nanoscience and technology, providing a bottom-up, atomic-level complement to 3D printing.« less

The structure of [MnIII6 CrIII]3+ single-molecule magnets deposited in submono-layers and monolayers on surfaces studied by means of molecular resolved atomic force microscopy (AFM) and Kelvin Probe Force Microscopy in UHV

NASA Astrophysics Data System (ADS)

Heinzmann, U.; Gryzia, A.; Volkmann, T.; Brechling, A.; Hoeke, V.; Glaser, T.

2014-04-01

Single molecule magnets (SMM) deposited in submonolayers and monolayers have been analyzed with respect to their structures by means of non-contact AFM (topographic as well as damping mode) and Kelvin Probe Force Microscopy with molecular resolution.

Synthesis, crystal structure, and magnetic properties of two-dimensional divalent metal glutarate/dipyridylamine coordination polymers, with a single crystal-to-single crystal transformation in the copper derivative

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

Montney, Matthew R.; Supkowski, Ronald M.; Staples, Richard J.

Hydrothermal reaction of divalent metal chlorides with glutaric acid and 4,4'-dipyridylamine (dpa) has afforded an isostructural family of coordination polymers with formulation [M(glu)(dpa)]{sub n} (M=Co (1), Ni (2), Cu (3); glu=glutarate). Square pyramidal coordination is seen in 1-3, with semi-ligation of a sixth donor to produce a '5+1' extended coordination sphere. Neighboring metal atoms are linked into 1D [M(glu)]{sub n} neutral chains through chelating/monodentate bridging glutarate moieties with a syn-anti binding mode, and semi-chelation of the pendant carboxylate oxygen. These chains further connect into 2D layers through dipodal dpa ligands. Neighboring layers stack into the pseudo 3D crystal structure ofmore » 1-3 through supramolecular hydrogen bonding between dpa amine units and the semi-chelated glutarate oxygen atoms. The variable temperature magnetic behavior of 1-3 was explored and modeled as infinite 1D Heisenberg chains. Notably, complex 3 undergoes a thermally induced single crystal-to-single crystal transformation between centric and acentric space groups, with a conformationally disordered unilayer structure at 293 K and an ordered bilayer structure at 173 K. All materials were further characterized via infrared spectroscopy and elemental and thermogravimetric analyses. - Graphical abstract: The coordination polymers [M(glu)(dpa)]{sub n} (M=Co (1), Ni (2), Cu (3); glu=glutarate, dpa=4,4'-dipyridylamine) exhibit 2D layer structures based on 1D [M(glu)]{sub n} chains linked through dpa tethers. Antiferromagnetic coupling is observed for 2 and 3, while ferromagnetism is predominant in 1. Compound 3 undergoes a thermally induced single crystal-to-single crystal transformation from an acentric to a centrosymmetric space group.« less

The edge- and basal-plane-specific electrochemistry of a single-layer graphene sheet

PubMed Central

Yuan, Wenjing; Zhou, Yu; Li, Yingru; Li, Chun; Peng, Hailin; Zhang, Jin; Liu, Zhongfan; Dai, Liming; Shi, Gaoquan

2013-01-01

Graphene has a unique atom-thick two-dimensional structure and excellent properties, making it attractive for a variety of electrochemical applications, including electrosynthesis, electrochemical sensors or electrocatalysis, and energy conversion and storage. However, the electrochemistry of single-layer graphene has not yet been well understood, possibly due to the technical difficulties in handling individual graphene sheet. Here, we report the electrochemical behavior at single-layer graphene-based electrodes, comparing the basal plane of graphene to its edge. The graphene edge showed 4 orders of magnitude higher specific capacitance, much faster electron transfer rate and stronger electrocatalytic activity than those of graphene basal plane. A convergent diffusion effect was observed at the sub-nanometer thick graphene edge-electrode to accelerate the electrochemical reactions. Coupling with the high conductivity of a high-quality graphene basal plane, graphene edge is an ideal electrode for electrocatalysis and for the storage of capacitive charges. PMID:23896697

Environmental sensing with optical fiber sensors processed with focused ion beam and atomic layer deposition

NASA Astrophysics Data System (ADS)

Flores, Raquel; Janeiro, Ricardo; Dahlem, Marcus; Viegas, Jaime

2015-03-01

We report an optical fiber chemical sensor based on a focused ion beam processed optical fiber. The demonstrated sensor is based on a cavity formed onto a standard 1550 nm single-mode fiber by either chemical etching, focused ion beam milling (FIB) or femtosecond laser ablation, on which side channels are drilled by either ion beam milling or femtosecond laser irradiation. The encapsulation of the cavity is achieved by optimized fusion splicing onto a standard single or multimode fiber. The empty cavity can be used as semi-curved Fabry-Pérot resonator for gas or liquid sensing. Increased reflectivity of the formed cavity mirrors can be achieved with atomic layer deposition (ALD) of alternating metal oxides. For chemical selective optical sensors, we demonstrate the same FIB-formed cavity concept, but filled with different materials, such as polydimethylsiloxane (PDMS), poly(methyl methacrylate) (PMMA) which show selective swelling when immersed in different solvents. Finally, a reducing agent sensor based on a FIB formed cavity partially sealed by fusion splicing and coated with a thin ZnO layer by ALD is presented and the results discussed. Sensor interrogation is achieved with spectral or multi-channel intensity measurements.

International Technical Exchange on 2D Atomic Sheets: Optoelectronics, Strain, and Energy Applications

DTIC Science & Technology

2015-01-15

Shi, University of Texas - Austin Thermal and Thermoelectric Properties and Applications of Two-Dimensional Materials beyond Graphene 11:45 – 1:15 pm...M., et al., Large and tunable photo- thermoelectric effect in single-layer MoS2, Nano Letters (2013) [4] Castellanos-Gomez, A., et al., Isolation...phosphorus field- effect transistors. Nano Letters (2014) [6] Buscema M., et al., Photovoltaic effect in few-layer black phosphorus PN junctions

Preparation of Tunable 3D Pillared Carbon Nanotube-Graphene Networks for High-Performance Capacitance

DTIC Science & Technology

2011-01-01

nanotubes ( CNTs ) and two-dimensional (2D) single-atomic layer graphene, have been demonstrated to show superior thermal, electrical, and mechanical...and the much weaker van der Waals interaction in the transverse direction between the layers, how- ever, CNTs and graphene exhibit strong direction...structure are governed by the minimum interpillar distance (MIPD) and the CNT -pillar length (PL) (Figure 1a). Some successes in fabricating randomly

Charge density wave order in 1D mirror twin boundaries of single-layer MoSe 2

DOE PAGES

Barja, Sara; Wickenburg, Sebastian; Liu, Zhen-Fei; ...

2016-04-18

Here, We provide direct evidence for the existence of isolated, one-dimensional charge density waves at mirror twin boundaries (MTBs) of single-layer semiconducting MoSe 2. Such MTBs have been previously observed by transmission electron microscopy and have been predicted to be metallic in MoSe 2 and MoS 2. Our low-temperature scanning tunnelling microscopy/spectroscopy measurements revealed a substantial bandgap of 100 meV opening at the Fermi energy in the otherwise metallic one-dimensional structures. We found a periodic modulation in the density of states along the MTB, with a wavelength of approximately three lattice constants. In addition to mapping the energy-dependent densitymore » of states, we determined the atomic structure and bonding of the MTB through simultaneous high-resolution non-contact atomic force microscopy. Density functional theory calculations based on the observed structure reproduced both the gap opening and the spatially resolved density of states.« less

Mechanical properties and structure evolution of single-crystalline silicon irradiated by 1 MeV Au+ and Cu+ ions

NASA Astrophysics Data System (ADS)

Liang, Wei; Zhu, Fei; Ling, Yunhan; Liu, Kezhao; Hu, Yin; Pan, Qifa; Chen, Limin; Zhang, Zhengjun

2018-05-01

Mechanical and structural evolutions of single-crystalline silicon irradiated by a series of doses 1 MeV Au+ ions and Cu+ ions are characterized by Surface laser-acoustic wave spectroscopy by (LA wave), Rutherford backscattering spectrometry and channeling (RBS/C) and transmission electron microscopy (TEM). The behavior of implanted Au+ and Cu+ ions was also simulated by using Stopping and range of ions in matter (SRIM) software package, respectively. It is demonstrated that LA wave and RBS could be applied for accurate evaluation of the TEM observed amorphous layer's thickness. The modified mechanical properties depend on the species and the dose of implantation. For 1 MeV Au+ ions, the threshold dose of completely amorphous is 5 × 1014 atoms/cm2, while the one for Cu+ ions is 5 × 1015 atoms/cm2. Upon completely amorphous, the young's modulus and layer density decreased significantly while saturated with the dose increasing sequentially.

Direct Growth of Graphene on Silicon by Metal-Free Chemical Vapor Deposition

NASA Astrophysics Data System (ADS)

Tai, Lixuan; Zhu, Daming; Liu, Xing; Yang, Tieying; Wang, Lei; Wang, Rui; Jiang, Sheng; Chen, Zhenhua; Xu, Zhongmin; Li, Xiaolong

2018-06-01

The metal-free synthesis of graphene on single-crystal silicon substrates, the most common commercial semiconductor, is of paramount significance for many technological applications. In this work, we report the growth of graphene directly on an upside-down placed, single-crystal silicon substrate using metal-free, ambient-pressure chemical vapor deposition. By controlling the growth temperature, in-plane propagation, edge-propagation, and core-propagation, the process of graphene growth on silicon can be identified. This process produces atomically flat monolayer or bilayer graphene domains, concave bilayer graphene domains, and bulging few-layer graphene domains. This work would be a significant step toward the synthesis of large-area and layer-controlled, high-quality graphene on single-crystal silicon substrates. [Figure not available: see fulltext.

Atomically thin heterostructures based on single-layer tungsten diselenide and graphene.

PubMed

Lin, Yu-Chuan; Chang, Chih-Yuan S; Ghosh, Ram Krishna; Li, Jie; Zhu, Hui; Addou, Rafik; Diaconescu, Bogdan; Ohta, Taisuke; Peng, Xin; Lu, Ning; Kim, Moon J; Robinson, Jeremy T; Wallace, Robert M; Mayer, Theresa S; Datta, Suman; Li, Lain-Jong; Robinson, Joshua A

2014-12-10

Heterogeneous engineering of two-dimensional layered materials, including metallic graphene and semiconducting transition metal dichalcogenides, presents an exciting opportunity to produce highly tunable electronic and optoelectronic systems. In order to engineer pristine layers and their interfaces, epitaxial growth of such heterostructures is required. We report the direct growth of crystalline, monolayer tungsten diselenide (WSe2) on epitaxial graphene (EG) grown from silicon carbide. Raman spectroscopy, photoluminescence, and scanning tunneling microscopy confirm high-quality WSe2 monolayers, whereas transmission electron microscopy shows an atomically sharp interface, and low energy electron diffraction confirms near perfect orientation between WSe2 and EG. Vertical transport measurements across the WSe2/EG heterostructure provides evidence that an additional barrier to carrier transport beyond the expected WSe2/EG band offset exists due to the interlayer gap, which is supported by theoretical local density of states (LDOS) calculations using self-consistent density functional theory (DFT) and nonequilibrium Green's function (NEGF).

Ruddlesden-Popper interface in correlated manganite heterostructures induces magnetic decoupling and dead layer reduction

NASA Astrophysics Data System (ADS)

Belenchuk, A.; Shapoval, O.; Roddatis, V.; Bruchmann-Bamberg, V.; Samwer, K.; Moshnyaga, V.

2016-12-01

We report on the interface engineering in correlated manganite heterostructures by octahedral decoupling using embedded stacks of atomic layers that form the Ruddlesden-Popper structure. A room temperature magnetic decoupling was achieved through deposition of a (SrO)2-TiO2-(SrO)2 sequence of atomic layers at the interface between La0.7Sr0.3MnO3 and La0.7Sr0.3Mn0.9Ru0.1O3 films. Moreover, the narrowing of the interfacial dead layer in ultrathin La0.7Sr0.3MnO3 films was demonstrated by insertion of a single (SrO)2 rock-salt layer at the interface with the SrTiO3(100) substrate. The obtained results are discussed based on the symmetry breaking and disconnection of the MnO6 octahedra network at the interface that may lead to the improved performance of all-oxide magnetic tunnel junctions. We suggest that octahedral decoupling realized by formation of Ruddlesden-Popper interfaces is an effective structural mechanism to control functionalities of correlated perovskite heterostructures.

Layer-by-layer modification of thin-film metal-semiconductor multilayers with ultrashort laser pulses

NASA Astrophysics Data System (ADS)

Romashevskiy, S. A.; Tsygankov, P. A.; Ashitkov, S. I.; Agranat, M. B.

2018-05-01

The surface modifications in a multilayer thin-film structure (50-nm alternating layers of Si and Al) induced by a single Gaussian-shaped femtosecond laser pulse (350 fs, 1028 nm) in the air are investigated by means of atomic-force microscopy (AFM), scanning electron microscopy (SEM), and optical microscopy (OM). Depending on the laser fluence, various modifications of nanometer-scale metal and semiconductor layers, including localized formation of silicon/aluminum nanofoams and layer-by-layer removal, are found. While the nanofoams with cell sizes in the range of tens to hundreds of nanometers are produced only in the two top layers, layer-by-layer removal is observed for the four top layers under single pulse irradiation. The 50-nm films of the multilayer structure are found to be separated at their interfaces, resulting in a selective removal of several top layers (up to 4) in the form of step-like (concentric) craters. The observed phenomenon is associated with a thermo-mechanical ablation mechanism that results in splitting off at film-film interface, where the adhesion force is less than the bulk strength of the used materials, revealing linear dependence of threshold fluences on the film thickness.

Advances in single-molecule magnet surface patterning through microcontact printing.

PubMed

Mannini, Matteo; Bonacchi, Daniele; Zobbi, Laura; Piras, Federica M; Speets, Emiel A; Caneschi, Andrea; Cornia, Andrea; Magnani, Agnese; Ravoo, Bart Jan; Reinhoudt, David N; Sessoli, Roberta; Gatteschi, Dante

2005-07-01

We present an implementation of strategies to deposit single-molecule magnets (SMMs) using microcontact printing microCP). We describe different approaches of microCP to print stripes of a sulfur-functionalized dodecamanganese (III, IV) cluster on gold surfaces. Comparison by atomic force microscopy profile analysis of the patterned structures confirms the formation of a chemically stable single layer of SMMs. Images based on chemical contrast, obtained by time-of-flight secondary ion mass spectrometry, confirm the patterned structure.

Tunable and high-purity room temperature single-photon emission from atomic defects in hexagonal boron nitride

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

Grosso, Gabriele; Moon, Hyowon; Lienhard, Benjamin

Two-dimensional van der Waals materials have emerged as promising platforms for solid-state quantum information processing devices with unusual potential for heterogeneous assembly. Recently, bright and photostable single photon emitters were reported from atomic defects in layered hexagonal boron nitride (hBN), but controlling inhomogeneous spectral distribution and reducing multi-photon emission presented open challenges. Here, we demonstrate that strain control allows spectral tunability of hBN single photon emitters over 6 meV, and material processing sharply improves the single photon purity. We observe high single photon count rates exceeding 7 × 10 6 counts per second at saturation, after correcting for uncorrelated photonmore » background. Furthermore, these emitters are stable to material transfer to other substrates. High-purity and photostable single photon emission at room temperature, together with spectral tunability and transferability, opens the door to scalable integration of high-quality quantum emitters in photonic quantum technologies.« less

Tunable and high-purity room temperature single-photon emission from atomic defects in hexagonal boron nitride

DOE PAGES

Grosso, Gabriele; Moon, Hyowon; Lienhard, Benjamin; ...

2017-09-26

Two-dimensional van der Waals materials have emerged as promising platforms for solid-state quantum information processing devices with unusual potential for heterogeneous assembly. Recently, bright and photostable single photon emitters were reported from atomic defects in layered hexagonal boron nitride (hBN), but controlling inhomogeneous spectral distribution and reducing multi-photon emission presented open challenges. Here, we demonstrate that strain control allows spectral tunability of hBN single photon emitters over 6 meV, and material processing sharply improves the single photon purity. We observe high single photon count rates exceeding 7 × 10 6 counts per second at saturation, after correcting for uncorrelated photonmore » background. Furthermore, these emitters are stable to material transfer to other substrates. High-purity and photostable single photon emission at room temperature, together with spectral tunability and transferability, opens the door to scalable integration of high-quality quantum emitters in photonic quantum technologies.« less

Density functional theory simulation of titanium migration and reaction with oxygen in the early stages of oxidation of equiatomic NiTi alloy.

PubMed

Nolan, Michael; Tofail, Syed A M

2010-05-01

The biocompatibility of NiTi shape memory alloys (SMA) has made possible applications in self-expandable cardio-vascular stents, stone extraction baskets, catheter guide wires and other invasive and minimally invasive biomedical devices. The NiTi intermetallic alloy spontaneously forms a thin passive layer of TiO(2), which provides its biocompatibility. The oxide layer is thought to form as the Ti in the alloy surface reacts with oxygen, resulting in a depletion of Ti in the subsurface region - experimental evidence indicates formation of a Ni-rich layer below the oxide film. In this paper, we study the initial stages of oxide growth on the (110) surface of the NiTi alloy to understand the formation of alloy/oxide interface. We initially adsorb atomic and molecular oxygen on the (110) surface and then successively add O(2) molecules, up to 2 monolayer of O(2). Oxygen adsorption always results in a large energy gain. With atomic oxygen, Ti is pulled out of the surface layer leaving behind a Ni-rich subsurface region. Molecular O(2), on the other hand adsorbs dissociatively and pulls a Ti atom farther out of the surface layer. The addition of further O(2) up to 1 monolayer is also dissociative and results in complete removal of Ti from the initial surface layer. When further O(2) is added up to 2 monolayer, Ti is pulled even further out of the surface and a single thin layer of composition O-Ti-O is formed. The electronic structure shows that the metallic character of the alloy is unaffected by interaction with oxygen and formation of the oxide layer, consistent with the oxide layer being a passivant. Copyright 2010 Elsevier Ltd. All rights reserved.

Al{sub 2}O{sub 3} multi-density layer structure as a moisture permeation barrier deposited by radio frequency remote plasma atomic layer deposition

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

Jung, Hyunsoo; Samsung Display Co. Ltd., Tangjeong, Chungcheongnam-Do 336-741; Jeon, Heeyoung

2014-02-21

Al{sub 2}O{sub 3} films deposited by remote plasma atomic layer deposition have been used for thin film encapsulation of organic light emitting diode. In this study, a multi-density layer structure consisting of two Al{sub 2}O{sub 3} layers with different densities are deposited with different deposition conditions of O{sub 2} plasma reactant time. This structure improves moisture permeation barrier characteristics, as confirmed by a water vapor transmission rate (WVTR) test. The lowest WVTR of the multi-density layer structure was 4.7 × 10{sup −5} gm{sup −2} day{sup −1}, which is one order of magnitude less than WVTR for the reference single-density Al{submore » 2}O{sub 3} layer. This improvement is attributed to the location mismatch of paths for atmospheric gases, such as O{sub 2} and H{sub 2}O, in the film due to different densities in the layers. This mechanism is analyzed by high resolution transmission electron microscopy, elastic recoil detection, and angle resolved X-ray photoelectron spectroscopy. These results confirmed that the multi-density layer structure exhibits very good characteristics as an encapsulation layer via location mismatch of paths for H{sub 2}O and O{sub 2} between the two layers.« less

Ganoderma-Like MoS2 /NiS2 with Single Platinum Atoms Doping as an Efficient and Stable Hydrogen Evolution Reaction Catalyst.

PubMed

Guan, Yongxin; Feng, Yangyang; Wan, Jing; Yang, Xiaohui; Fang, Ling; Gu, Xiao; Liu, Ruirui; Huang, Zhengyong; Li, Jian; Luo, Jun; Li, Changming; Wang, Yu

2018-05-27

Herein, a unique ganoderma-like MoS 2 /NiS 2 hetero-nanostructure with isolated Pt atoms anchored is reported. This novel ganoderma-like heterostructure can not only efficiently disperse and confine the few-layer MoS 2 nanosheets to fully expose the edge sites of MoS 2 , and provide more opportunity to capture the Pt atoms, but also tune the electronic structure to modify the catalytic activity. Because of the favorable dispersibility and exposed large specific surface area, single Pt atoms can be easily anchored on MoS 2 nanosheets with ultrahigh loading of 1.8 at% (the highest is 1.3 at% to date). Owing to the ganoderma-like structure and platinum atoms doping, this catalyst shows Pt-like catalytic activity for the hydrogen evolution reaction with an ultralow overpotential of 34 mV and excellent durability of only 2% increase in overpotential for 72 h under the constant current density of 10 mA cm -2 . © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Superconductivity in few-layer stanene

DOE PAGES

Liao, Menghan; Zang, Yunyi; Guan, Zhaoyong; ...

2018-01-15

A single atomic slice of α-tin—stanene—has been predicted to host the quantum spin Hall effect at room temperature, offering an ideal platform to study low-dimensional and topological physics. Although recent research has focused on monolayer stanene, the quantum size effect in few-layer stanene could profoundly change material properties, but remains unexplored. By exploring the layer degree of freedom, we discover superconductivity in few-layer stanene down to a bilayer grown on PbTe, while bulk α-tin is not superconductive. Through substrate engineering, we further realize a transition from a single-band to a two-band superconductor with a doubling of the transition temperature. Inmore » situ angle-resolved photoemission spectroscopy (ARPES) together with first-principles calculations elucidate the corresponding band structure. The theory also indicates the existence of a topologically non-trivial band. Thus, our experimental findings open up novel strategies for constructing two-dimensional topological superconductors.« less

Electrochemistry at Edge of Single Graphene Layer in a Nanopore

PubMed Central

Banerjee, Shouvik; Shim, Jiwook; Rivera, Jose; Jin, Xiaozhong; Estrada, David; Solovyeva, Vita; You, Xiuque; Pak, James; Pop, Eric; Aluru, Narayana; Bashir, Rashid

2013-01-01

We study the electrochemistry of single layer graphene edges using a nanopore-based structure consisting of stacked graphene and Al2O3 dielectric layers. Nanopores, with diameters ranging from 5 to 20 nm, are formed by an electron beam sculpting process on the stacked layers. This leads to unique edge structure which, along with the atomically thin nature of the embedded graphene electrode, demonstrates electrochemical current densities as high as 1.2 × 104 A/cm2. The graphene edge embedded structure offers a unique capability to study the electrochemical exchange at an individual graphene edge, isolated from the basal plane electrochemical activity. We also report ionic current modulation in the nanopore by biasing the embedded graphene terminal with respect to the electrodes in the fluid. The high electrochemical specific current density for a graphene nanopore-based device can have many applications in sensitive chemical and biological sensing, and energy storage devices. PMID:23249127

Watering Graphene for Devices and Electricity

NASA Astrophysics Data System (ADS)

Guo, Wanlin; Yin, Jun; Li, Xuemei; Zhang, Zhuhua

2013-03-01

Graphene bring us into a fantastic two-dimensional (2D) age of nanotechnology, which can be fabricated and applied at wafer scale, visible at single layer but showing exceptional properties distinguished from its bulk form graphite, linking the properties of atomic layers with the engineering scale of our mankind. We shown that flow-induced-voltage in graphene can be 20 folds higher than in graphite, not only due to the giant Seebeck coefficient of single layer graphene, but also the exceptional interlayer interaction in few layer graphene. Extremely excitingly, water flow over graphene can generate electricity through unexpected interaction of the ions in the water with the graphene. We also find extraordinary mechanical-electric-magnetic coupling effects in graphene and BN systems. Such extraordinary multifield coupling effects in graphene and functional nanosystems open up new vistas in nanotechnology for efficient energy conversion, self-powering flexible devices and novel functional systems.

Superconductivity in few-layer stanene

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

Liao, Menghan; Zang, Yunyi; Guan, Zhaoyong

A single atomic slice of α-tin—stanene—has been predicted to host the quantum spin Hall effect at room temperature, offering an ideal platform to study low-dimensional and topological physics. Although recent research has focused on monolayer stanene, the quantum size effect in few-layer stanene could profoundly change material properties, but remains unexplored. By exploring the layer degree of freedom, we discover superconductivity in few-layer stanene down to a bilayer grown on PbTe, while bulk α-tin is not superconductive. Through substrate engineering, we further realize a transition from a single-band to a two-band superconductor with a doubling of the transition temperature. Inmore » situ angle-resolved photoemission spectroscopy (ARPES) together with first-principles calculations elucidate the corresponding band structure. The theory also indicates the existence of a topologically non-trivial band. Thus, our experimental findings open up novel strategies for constructing two-dimensional topological superconductors.« less

Efficiency Improvement Using Molybdenum Disulphide Interlayers in Single-Wall Carbon Nanotube/Silicon Solar Cells.

PubMed

Alzahly, Shaykha; Yu, LePing; Shearer, Cameron J; Gibson, Christopher T; Shapter, Joseph G

2018-04-21

Molybdenum disulphide (MoS₂) is one of the most studied and widely applied nanomaterials from the layered transition-metal dichalcogenides (TMDs) semiconductor family. MoS₂ has a large carrier diffusion length and a high carrier mobility. Combining a layered structure of single-wall carbon nanotube (SWCNT) and MoS₂ with n-type silicon (n-Si) provided novel SWCNT/n-Si photovoltaic devices. The solar cell has a layered structure with Si covered first by a thin layer of MoS₂ flakes and then a SWCNT film. The films were examined using scanning electron microscopy, atomic force microscopy and Raman spectroscopy. The MoS₂ flake thickness ranged from 5 to 90 nm while the nanosheet’s lateral dimensions size ranged up to 1 μm². This insertion of MoS₂ improved the photoconversion efficiency (PCE) of the SWCNT/n-Si solar cells by approximately a factor of 2.

Superconductivity in few-layer stanene

NASA Astrophysics Data System (ADS)

Liao, Menghan; Zang, Yunyi; Guan, Zhaoyong; Li, Haiwei; Gong, Yan; Zhu, Kejing; Hu, Xiao-Peng; Zhang, Ding; Xu, Yong; Wang, Ya-Yu; He, Ke; Ma, Xu-Cun; Zhang, Shou-Cheng; Xue, Qi-Kun

2018-04-01

A single atomic slice of α-tin—stanene—has been predicted to host the quantum spin Hall effect at room temperature, offering an ideal platform to study low-dimensional and topological physics. Although recent research has focused on monolayer stanene, the quantum size effect in few-layer stanene could profoundly change material properties, but remains unexplored. By exploring the layer degree of freedom, we discover superconductivity in few-layer stanene down to a bilayer grown on PbTe, while bulk α-tin is not superconductive. Through substrate engineering, we further realize a transition from a single-band to a two-band superconductor with a doubling of the transition temperature. In situ angle-resolved photoemission spectroscopy (ARPES) together with first-principles calculations elucidate the corresponding band structure. The theory also indicates the existence of a topologically non-trivial band. Our experimental findings open up novel strategies for constructing two-dimensional topological superconductors.

Aluminum surface modification by a non-mass-analyzed nitrogen ion beam

NASA Astrophysics Data System (ADS)

Ohira, Shigeo; Iwaki, Masaya

Non-mass-analyzed nitrogen ion implantation into polycrystal and single crystal aluminum sheets has been carried out at an accelerating voltage of 90 kV and a dose of 1 × 10 18 N ions/cm 2 using a Zymet implanter model Z-100. The pressure during implantation rose to 10 -3 Pa due to the influence of N gas feeding into the ion source. The characteristics of the surface layers were investigated by means of Auger electron spectroscopy (AES), X-ray diffraction (XRD), transmission electron diffraction (TED), and microscopy (TEM). The AES depth profiling shows a rectangular-like distribution of N atoms and little migration of O atoms near the surface. The high dose N-implantation forms c-axis oriented aluminum nitride (AIN) crystallines, and especially irradiation of Al single crystals with N ions leads to the formation of a hcp AlN single crystal. It is concluded that the high dose N-implantation in Al can result in the formation of AlN at room temperature without any thermal annealing. Furthermore, non-mass-analyzed N-implantation at a pressure of 10 -3 Pa of the nitrogen atmosphere causes the formation of pure AlN single crystals in the Al surface layer and consequently it can be practically used for AlN production.

Matrix Synthesis of Graphene on a Diamond Surface and Its Simulation

NASA Astrophysics Data System (ADS)

Alekseev, N. I.

2018-07-01

A quantum-chemical simulation is performed for the transformation of the upper sublayer of carbon atoms in the lattice of single-crystal diamond into a flat graphene lattice under the influence of the atoms of a molten copper film on the diamond surface. It is established that the stable system configuration corresponds to the thermally activated motion of carbon atoms in the lower sublayer of the interface diamond layer to the position of graphene, i.e., at the same level as the atoms of the upper sublayer. The energy gain in comparison to the noninteracting subsystems of the copper and diamond atoms is approximately 0.7 eV per atom of the lower sublayer. The maximum size of the resulting graphene film is estimated and a possible mechanism for its rupture is considered.

Atomic Migration Induced Crystal Structure Transformation and Core-Centered Phase Transition in Single Crystal Ge2Sb2Te5 Nanowires.

PubMed

Lee, Jun-Young; Kim, Jeong-Hyeon; Jeon, Deok-Jin; Han, Jaehyun; Yeo, Jong-Souk

2016-10-12

A phase change nanowire holds a promise for nonvolatile memory applications, but its transition mechanism has remained unclear due to the analytical difficulties at atomic resolution. Here we obtain a deeper understanding on the phase transition of a single crystalline Ge 2 Sb 2 Te 5 nanowire (GST NW) using atomic scale imaging, diffraction, and chemical analysis. Our cross-sectional analysis has shown that the as-grown hexagonal close-packed structure of the single crystal GST NW transforms to a metastable face-centered cubic structure due to the atomic migration to the pre-existing vacancy layers in the hcp structure going through iterative electrical switching. We call this crystal structure transformation "metastabilization", which is also confirmed by the increase of set-resistance during the switching operation. For the set to reset transition between crystalline and amorphous phases, high-resolution imaging indicates that the longitudinal center of the nanowire mainly undergoes phase transition. According to the atomic scale analysis of the GST NW after repeated electrical switching, partial crystallites are distributed around the core-centered amorphous region of the nanowire where atomic migration is mainly induced, thus potentially leading to low power electrical switching. These results provide a novel understanding of phase change nanowires, and can be applied to enhance the design of nanowire phase change memory devices for improved electrical performance.

Controlled Phase and Tunable Magnetism in Ordered Iron Oxide Nanotube Arrays Prepared by Atomic Layer Deposition

DOE PAGES

Zhang, Yijun; Liu, Ming; Peng, Bin; ...

2016-01-27

Highly-ordered and conformal iron oxide nanotube arrays on an atomic scale are successfully prepared by atomic layer deposition (ALD) with controlled oxidization states and tunable magnetic properties between superparamagnetism and ferrimagnetism. Non-magnetic α-Fe 2O 3 and superparamagnetic Fe 2O 3with a blocking temperature of 120 K are in-situ obtained by finely controlling the oxidation reaction. Both of them exhibit a very small grain size of only several nanometers due to the nature of atom-by-atom growth of the ALD technique. Post-annealing α-Fe 2O 3 in a reducing atmosphere leads to the formation of the spinel Fe 3O 4 phase which displaysmore » a distinct ferrimagnetic anisotropy and the Verwey metal-insulator transition that usually takes place only in single crystal magnetite or thick epitaxial films at low temperatures. Finally, the ALD deposition of iron oxide with well-controlled phase and tunable magnetism demonstrated in this work provides a promising opportunity for the fabrication of 3D nano-devices to be used in catalysis, spintronics, microelectronics, data storages and bio-applications.« less

Vibrational and optical properties of MoS2: From monolayer to bulk

NASA Astrophysics Data System (ADS)

Molina-Sánchez, Alejandro; Hummer, Kerstin; Wirtz, Ludger

2015-12-01

Molybdenum disulfide, MoS2, has recently gained considerable attention as a layered material where neighboring layers are only weakly interacting and can easily slide against each other. Therefore, mechanical exfoliation allows the fabrication of single and multi-layers and opens the possibility to generate atomically thin crystals with outstanding properties. In contrast to graphene, it has an optical gap of ~1.9 eV. This makes it a prominent candidate for transistor and opto-electronic applications. Single-layer MoS2 exhibits remarkably different physical properties compared to bulk MoS2 due to the absence of interlayer hybridization. For instance, while the band gap of bulk and multi-layer MoS2 is indirect, it becomes direct with decreasing number of layers. In this review, we analyze from a theoretical point of view the electronic, optical, and vibrational properties of single-layer, few-layer and bulk MoS2. In particular, we focus on the effects of spin-orbit interaction, number of layers, and applied tensile strain on the vibrational and optical properties. We examine the results obtained by different methodologies, mainly ab initio approaches. We also discuss which approximations are suitable for MoS2 and layered materials. The effect of external strain on the band gap of single-layer MoS2 and the crossover from indirect to direct band gap is investigated. We analyze the excitonic effects on the absorption spectra. The main features, such as the double peak at the absorption threshold and the high-energy exciton are presented. Furthermore, we report on the the phonon dispersion relations of single-layer, few-layer and bulk MoS2. Based on the latter, we explain the behavior of the Raman-active A1g and E2g1 modes as a function of the number of layers. Finally, we compare theoretical and experimental results of Raman, photoluminescence, and optical-absorption spectroscopy.

Influence of cutting parameters on the depth of subsurface deformed layer in nano-cutting process of single crystal copper.

PubMed

Wang, Quanlong; Bai, Qingshun; Chen, Jiaxuan; Su, Hao; Wang, Zhiguo; Xie, Wenkun

2015-12-01

Large-scale molecular dynamics simulation is performed to study the nano-cutting process of single crystal copper realized by single-point diamond cutting tool in this paper. The centro-symmetry parameter is adopted to characterize the subsurface deformed layers and the distribution and evolution of the subsurface defect structures. Three-dimensional visualization and measurement technology are used to measure the depth of the subsurface deformed layers. The influence of cutting speed, cutting depth, cutting direction, and crystallographic orientation on the depth of subsurface deformed layers is systematically investigated. The results show that a lot of defect structures are formed in the subsurface of workpiece during nano-cutting process, for instance, stair-rod dislocations, stacking fault tetrahedron, atomic clusters, vacancy defects, point defects. In the process of nano-cutting, the depth of subsurface deformed layers increases with the cutting distance at the beginning, then decreases at stable cutting process, and basically remains unchanged when the cutting distance reaches up to 24 nm. The depth of subsurface deformed layers decreases with the increase in cutting speed between 50 and 300 m/s. The depth of subsurface deformed layer increases with cutting depth, proportionally, and basically remains unchanged when the cutting depth reaches over 6 nm.

Theoretical study of magnetic layers of nickel on copper; dead or alive?

NASA Astrophysics Data System (ADS)

Ernst, A.; Lueders, M.; Temmerman, W. M.; Szotek, Z.; van der Laan, G.

2000-07-01

We studied the persistence of magnetism in ultrathin nickel films on copper. Layer-dependent magnetic moments in Ni films on the (001), (110) and (111) surfaces of Cu have been calculated using the Korringa-Kohn-Rostoker Green's function method. The results show that, at temperature T = 0, a single nickel monolayer is ferromagnetic on Cu(001) and Cu(110) but magnetically `dead' on the more closely packed Cu(111) surface. Films of two and more layers of Ni are always ferromagnetic, with the magnetic moment enhanced in the surface layer but strongly reduced in the interface layer. Due to the short screening length, both the effect of the interface and that of the surface are confined to only a few atomic layers.

Single-layer ZnS supported on Au(111): A combined XPS, LEED, STM and DFT study

DOE PAGES

Deng, Xingyi; Sorescu, Dan C.; Lee, Junseok

2016-12-31

Single-layer of ZnS, consisting of one atomic layer of ZnS(111) plane, has been grown on Au(111) and characterized using X-ray photoelectron spectroscopy (XPS), low energy electron diffraction (LEED) and scanning tunneling microscopy (STM). While the LEED measurement indicates a coincidence structure of ZnS-(3×3)/Au(111)-(4×4), high resolution STM images reveal hexagonal unit cells of 6.7×6.7 Å 2 and 11.6×11.6 Å 2, corresponding to √3 and 3 times the unit cell of the ideal zincblende ZnS-(1×1), respectively, depending on the tunneling conditions. Calculations based on density functional theory (DFT) indicate a significantly reconstructed non-planar structure of ZnS single-layer on Au(111) with 2/3 ofmore » the S anions being located nearly in the plane of the Zn cations and the rest 1/3 of the S anions protruding above the Zn plane. In conclusion, the calculated STM image shows similar characteristics to those of the experimental STM image. Additionally, the DFT calculations reveal the different bonding nature of the S anions in ZnS single-layer supported on Au(111).« less

Synthesis of Freestanding Single-crystal Perovskite Films and Heterostructures by Etching of Sacrificial Water-soluble Layers

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

Lu, Di; Baek, David J.; Hong, Seung Sae

2016-08-22

The ability to create and manipulate materials in two-dimensional (2D) form has repeatedly had transformative impact on science and technology. In parallel with the exfoliation and stacking of intrinsically layered crystals, atomic-scale thin film growth of complex materials has enabled the creation of artificial 2D heterostructures with novel functionality and emergent phenomena, as seen in perovskite heterostructures. However, separation of these layers from the growth substrate has proven challenging, limiting the manipulation capabilities of these heterostructures with respect to exfoliated materials. Here we present a general method to create freestanding perovskite membranes. The key is the epitaxial growth of water-solublemore » Sr 3Al 2O 6 on perovskite substrates, followed by in situ growth of films and heterostructures. Millimetre-size single-crystalline membranes are produced by etching the Sr 3Al 2O 6 layer in water, providing the opportunity to transfer them to arbitrary substrates and integrate them with heterostructures of semiconductors and layered compounds.« less

Parametric Investigation of the Isothermal Kinetics of Growth of Graphene on a Nickel Catalyst in the Process of Chemical Vapor Deposition of Hydrocarbons

NASA Astrophysics Data System (ADS)

Futko, S. I.; Shulitskii, B. G.; Labunov, V. A.; Ermolaeva, E. M.

2016-11-01

A kinetic model of isothermal synthesis of multilayer graphene on the surface of a nickel foil in the process of chemical vapor deposition, on it, of hydrocarbons supplied in the pulsed regime is considered. The dependences of the number of graphene layers formed and the time of their growth on the temperature of the process, the concentration of acetylene, and the thickness of the nickel foil were calculated. The regime parameters of the process of chemical vapor deposition, at which single-layer graphene and bi-layer graphene are formed, were determined. The dynamics of growth of graphene domains at chemical-vapor-deposition parameters changing in wide ranges was investigated. It is shown that the time dependences of the rates of growth of single-layer graphene and bi-layer graphene are nonlinear in character and that they are determined by the kinetics of nucleation and growth of graphene and the diffusion flow of carbon atoms in the nickel foil.

Atomic and electronic structures of single-layer FeSe on SrTiO 3(001): The role of oxygen deficiency

DOE PAGES

Bang, Junhyeok; Li, Zhi; Sun, Y. Y.; ...

2013-06-06

Using first-principles calculation, we propose an interface structure for single triple-layer FeSe on the SrTiO 3(001) surface, a high-T c superconductor found recently. The key component of this structure is the oxygen deficiency on the top layer of the SrTiO 3 substrate, as a result of Se etching used in preparing the high-T c samples. The O vacancies strongly bind the FeSe triple layer to the substrate giving rise to a (2×1) reconstruction, as observed by scanning tunneling microscopy. The enhanced binding correlates to the significant increase of T c observed in experiment. The O vacancies also serve as themore » source of electron doping, which modifies the Fermi surface of the first FeSe layer by filling the hole pocket near the center of the surface Brillouin zone, as suggested from angle-resolved photoemission spectroscopy measurement.« less

High transport and excellent optical property of a two-dimensional single-layered hybrid perovskite (C4H9NH3)2PbBr4: a theoretical study.

PubMed

Lei, Jun-Hui; Zhao, Yu-Qing; Tang, Qiong; Lin, Jian-Guo; Cai, Meng-Qiu

2018-05-16

Organic-inorganic hybrid perovskites are developed to pursue high charge carrier mobility and light absorption coefficient. In this study, we present a detailed comparative research of the atomic and electronic structures of single-layered perovskites (C4H9NH3)2PbBr4 with two-dimensional/three-dimensional (2D/3D) spatial arrangement to predict the in plane charge carrier mobility along with the charge effective mass, elastic constant, and deformation potential. The calculated results reveal that the intrinsic in plane carrier mobilities of 2D single-layered hybrid perovskite (C4H9NH3)2PbBr4 along the 100 and 010 directions are superior to those of the 3D structure. Furthermore, the optical properties are calculated from the electronic structure; it is found that the light absorption spectrum of 2D single-layered perovskite (C4H9NH3)2PbBr4 with a high absorption coefficient is wider than that of the 3D phase. We speculate that the superior mobility and wider absorption spectrum of the 2D mono-layered perovskite are due to high charge density and ferroelectricity originating from structure distortion upon 3D-to-2D structure transformation. These results indicate that the 2D single-layered hybrid perovskite (C4H9NH3)2PbBr4 is a potential candidate for application in the optoelectronic and photovoltaic fields.

ZnO Functionalization of Multi-walled Carbon Nanotubes for Methane Sensing at Single Parts Per Million Concentration Levels

EPA Science Inventory

This paper presents a novel atomic layer deposition (ALD) based ZnO functionalization of surface pre-treated multi-walled carbon nanotubes (MWCNTs) for highly sensitive methane chemoresistive sensors. The temperature optimization of the ALD process leads to enhanced ZnO nanopart...

Cavity enhanced atomic magnetometry

PubMed Central

Crepaz, Herbert; Ley, Li Yuan; Dumke, Rainer

2015-01-01

Atom sensing based on Faraday rotation is an indispensable method for precision measurements, universally suitable for both hot and cold atomic systems. Here we demonstrate an all-optical magnetometer where the optical cell for Faraday rotation spectroscopy is augmented with a low finesse cavity. Unlike in previous experiments, where specifically designed multipass cells had been employed, our scheme allows to use conventional, spherical vapour cells. Spherical shaped cells have the advantage that they can be effectively coated inside with a spin relaxation suppressing layer providing long spin coherence times without addition of a buffer gas. Cavity enhancement shows in an increase in optical polarization rotation and sensitivity compared to single-pass configurations. PMID:26481853

Interaction of overlayers of Al and Rb with single-crystalline surfaces of Bi2Sr2CaCu2O8

NASA Astrophysics Data System (ADS)

Lindberg, P. A. P.; Wells, B. O.; Shen, Z.-X.; Dessau, D. S.; Lindau, I.; Spicer, W. E.; Mitzi, D. B.; Kapitulnik, A.

1990-03-01

Photoemission results from Al and Rb interfaces with single crystals of Bi2Sr2CaCu2O8 high-temperature superconductors are reported. The Al and Rb adsorbates are found to react quite differently with the Bi2Sr2CaCu2O8 substrate. While adatoms of Rb significantly affect only the Bi and O atoms in the top atomic layer, the Al adsorbate profoundly disrupts the bonding character of the whole Bi2Sr2CaCu2O8 material. For Al, the Bi and Cu states are strongly reduced, and the Sr and O states show evidence of oxidized components. In addition, Al causes a strong out-diffusion of oxygen from the bulk. The differences in the reactivity of Al and Rb are discussed in terms of the different mobility of the two atoms.

2-Acetyl-1,1,3,3-tetra­methyl­guanidine

PubMed Central

Tiritiris, Ioannis

2012-01-01

In the mol­ecule of the title compound, C7H15N3O, the central C atom is surrounded in a nearly ideal trigonal–planar geometry by three N atoms. The C—N bond lengths in the CN3 unit are 1.3353 (13), 1.3463 (12) and 1.3541 (13) Å, indicating an inter­mediate character between a single and a double bond for each C—N bond. The bonds between the N atoms and the terminal C-methyl groups all have values close to that of a typical single bond [1.4526 (13)–1.4614 (14) Å]. In the crystal, the guanidine mol­ecules are connected by weak C—H⋯O and C—H⋯N hydrogen bonds, generating layers parallel to the ab plane. PMID:23125768

Fabrication of a trimer/single atom tip for gas field ion sources by means of field evaporation without tip heating.

PubMed

Kim, Kwang-Il; Kim, Young Heon; Ogawa, Takashi; Choi, Suji; Cho, Boklae; Ahn, Sang Jung; Park, In-Yong

2018-05-11

A gas field ion source (GFIS) has many advantages that are suitable for ion microscope sources, such as high brightness and a small virtual source size, among others. In order to apply a tip-based GFIS to an ion microscope, it is better to create a trimer/single atom tip (TSAT), where the ion beam must be generated in several atoms of the tip apex. Here, unlike the conventional method which uses tip heating or a reactive gas, we show that the tip surface can be cleaned using only the field evaporation phenomenon and that the TSAT can also be fabricated using an insulating layer containing tungsten oxide, which remains after electrochemical etching. Using this method, we could get TSAT over 90% of yield. Copyright © 2018. Published by Elsevier B.V.

‘Pd20Sn13’ revisited: crystal structure of Pd6.69Sn4.31

PubMed Central

Klein, Wilhelm; Jin, Hanpeng; Hlukhyy, Viktor; Fässler, Thomas F.

2015-01-01

The crystal structure of the title compound was previously reported with composition ‘Pd20Sn13’ [Sarah et al. (1981 ▸). Z. Metallkd, 72, 517–520]. For the original structure model, as determined from powder X-ray data, atomic coordinates from the isostructural compound Ni13Ga3Ge6 were transferred. The present structure determination, resulting in a composition Pd6.69Sn4.31, is based on single crystal X-ray data and includes anisotropic displacement parameters for all atoms as well as standard uncertainties for the atomic coordinates, leading to higher precision and accuracy for the structure model. Single crystals of the title compound were obtained via a solid-state reaction route, starting from the elements. The crystal structure can be derived from the AlB2 type of structure after removing one eighth of the atoms at the boron positions and shifting adjacent atoms in the same layer in the direction of the voids. One atomic site is partially occupied by both elements with a Pd:Sn ratio of 0.38 (3):0.62 (3). One Sn and three Pd atoms are located on special positions with site symmetry 2. (Wyckoff letter 3a and 3b). PMID:26279872

Investigating the Catalytic Growth of Carbon Nanotubes with In Situ Raman Monitoring

DTIC Science & Technology

2015-06-01

single-walled carbon nanotube growth using cobalt deposited on Si/SiO2 as a model system. In situ Raman studies revealed that thin catalyst layers... cobalt thickness were studied. Surface analyses showed that during the catalyst preparation, catalyst atoms at the interface with silica form small...nanostructures. However, highly-reducing conditions are required to reduce the small silicate domains into small cobalt particles able to grow single-walled

Synergistic approach to high-performance oxide thin film transistors using a bilayer channel architecture.

PubMed

Yu, Xinge; Zhou, Nanjia; Smith, Jeremy; Lin, Hui; Stallings, Katie; Yu, Junsheng; Marks, Tobin J; Facchetti, Antonio

2013-08-28

We report here a bilayer metal oxide thin film transistor concept (bMO TFT) where the channel has the structure: dielectric/semiconducting indium oxide (In2O3) layer/semiconducting indium gallium oxide (IGO) layer. Both semiconducting layers are grown from solution via a low-temperature combustion process. The TFT mobilities of bottom-gate/top-contact bMO TFTs processed at T = 250 °C are ~5tmex larger (~2.6 cm(2)/(V s)) than those of single-layer IGO TFTs (~0.5 cm(2)/(V s)), reaching values comparable to single-layer combustion-processed In2O3 TFTs (~3.2 cm(2)/(V s)). More importantly, and unlike single-layer In2O3 TFTs, the threshold voltage of the bMO TFTs is ~0.0 V, and the current on/off ratio is significantly enhanced to ~1 × 10(8) (vs ~1 × 10(4) for In2O3). The microstructure and morphology of the In2O3/IGO bilayers are analyzed by X-ray diffraction, atomic force microscopy, X-ray photoelectron spectroscopy, and transmission electron microscopy, revealing the polycrystalline nature of the In2O3 layer and the amorphous nature of the IGO layer. This work demonstrates that solution-processed metal oxides can be implemented in bilayer TFT architectures with significantly enhanced performance.

Efficiency Enhancement of Nanotextured Black Silicon Solar Cells Using Al2O3/TiO2 Dual-Layer Passivation Stack Prepared by Atomic Layer Deposition.

PubMed

Wang, Wei-Cheng; Tsai, Meng-Chen; Yang, Jason; Hsu, Chuck; Chen, Miin-Jang

2015-05-20

In this study, efficient nanotextured black silicon (NBSi) solar cells composed of silicon nanowire arrays and an Al2O3/TiO2 dual-layer passivation stack on the n(+) emitter were fabricated. The highly conformal Al2O3 and TiO2 surface passivation layers were deposited on the high-aspect-ratio surface of the NBSi wafers using atomic layer deposition. Instead of the single Al2O3 passivation layer with a negative oxide charge density, the Al2O3/TiO2 dual-layer passivation stack treated with forming gas annealing provides a high positive oxide charge density and a low interfacial state density, which are essential for the effective field-effect and chemical passivation of the n(+) emitter. In addition, the Al2O3/TiO2 dual-layer passivation stack suppresses the total reflectance over a broad range of wavelengths (400-1000 nm). Therefore, with the Al2O3/TiO2 dual-layer passivation stack, the short-circuit current density and efficiency of the NBSi solar cell were increased by 11% and 20%, respectively. In conclusion, a high efficiency of 18.5% was achieved with the NBSi solar cells by using the n(+)-emitter/p-base structure passivated with the Al2O3/TiO2 stack.

Optimization Methods on Synthesis of Atomically Thin Layered Materials and Heterostructures

NASA Astrophysics Data System (ADS)

Temiz, Selcuk

Two dimensional (2D) materials have emerged as a new class of materials that only a few atoms thick. Owing to their low dimensionality, 2D materials bear rather unusual properties that do not exist in traditional three dimensional (3D) materials. Graphene, a single layer of carbon atoms arrange in a 2D hexagonal lattice, has started the revolutionary progress in materials science and condensed matter physics, and motivated intense research in other 2D materials such as h-BN, and layered metal dichalcogenides. Chemical vapor deposition (CVD) is the most studied bottom-up graphene production method for building the prototypes of next-generation electronic devices due to its scalability; however, there is still not an ultimate consensus of growth mechanisms on control the size and morphology of synthesized-crystals. In order to have better understanding the growth mechanisms, the role of oxygen exposure in the graphene growth has been comprehensively studied. The oxygen gas is introduced into the CVD reactor before and during the growth, and its effects on the morphology, crystallinity, and nucleation density of graphene are systematically studied. It is found that introducing oxygen during growth significantly improves the graphene crystallinity while pre-dosing oxygen before growth reduces the graphene nucleation density. The stacking of graphene and other layered materials in the lateral or vertical geometries can offer extended functionality by exploiting interfacial phenomena, quantum confinement and tunneling, which requires the interface between the layered materials be free of contaminates. The vertical heterostructures of CVD-grown graphene and h-BN single crystals are deeply investigated by analytical scanning transmission electron microscopy (STEM) and electron energy loss spectroscopy (EELS). It is shown that graphene contamination, undetectable using optical microscopy, is prevalent at the nanoscale, and the interfacial contamination between the layers reduces the interlayer coupling and ultimately undermines the graphene/h-BN heterostructures. Raman spectroscopy is a versatile and non-destructive technique for the identification of structural properties and phonon features of atomically thin layered materials. Especially, the second order resonant Raman spectroscopy, which can be applied to the resonance conditions in energy of the incoming photon and interband transitions of an electron in a crystal lattice, reveals additional phonon modes to typical Raman active modes in a spectra. Various 2D materials, including SnSe2, WSe2, SnS2, and MoTe2, and their heterostructures are fabricated by dry transfer method as a top-down approach. The vibrational characteristics of these 2D materials systems are unambiguously established by using second order Resonant Raman spectroscopy.

Disentangling atomic-layer-specific x-ray absorption spectra by Auger electron diffraction spectroscopy

NASA Astrophysics Data System (ADS)

Matsui, Fumihiko; Matsushita, Tomohiro; Kato, Yukako; Hashimoto, Mie; Daimon, Hiroshi

2009-11-01

In order to investigate the electronic and magnetic structures of each atomic layer at subsurface, we have proposed a new method, Auger electron diffraction spectroscopy, which is the combination of x-ray absorption spectroscopy (XAS) and Auger electron diffraction (AED) techniques. We have measured a series of Ni LMM AED patterns of the Ni film grown on Cu(001) surface for various thicknesses. Then we deduced a set of atomic-layer-specific AED patterns in a numerical way. Furthermore, we developed an algorithm to disentangle XANES spectra from different atomic layers using these atomic-layer-specific AED patterns. Surface and subsurface core level shift were determined for each atomic layer.

Atomically Thin Heterostructures Based on Single-Layer Tungsten Diselenide and Graphene [Plus Supplemental Information

DOE PAGES

Lin, Yu-Chuan; Chang, Chih-Yuan S.; Ghosh, Ram Krishna; ...

2014-11-10

Heterogeneous engineering of two-dimensional layered materials, including metallic graphene and semiconducting transition metal dichalcogenides, presents an exciting opportunity to produce highly tunable electronic and optoelectronic systems. We report the direct growth of highly crystalline, monolayer tungsten diselenide (WSe 2) on epitaxial graphene (EG). Raman spectroscopy and photoluminescence confirms high-quality WSe 2 monolayers; while transmission electron microscopy shows an atomically sharp interface and low energy electron diffraction confirms near perfect orientation between WSe 2 and EG. Vertical transport measurements across the WSe 2/EG heterostructure provides evidence that a tunnel barrier exists due to the van der Waals gap, and is supportedmore » by density functional theory that predicts a 1.6 eV barrier for transport from WSe 2 to graphene.« less

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

Gill, Tobias G.; Fleurence, Antoine; Warner, Ben

We observe a new two-dimensional (2D) silicon crystal, using low energy electron diffraction (LEED) and scanning tunnelling microscopy (STM) and it's formed by depositing additional Si atoms onto spontaneously-formed epitaxial silicene on a ZrB 2 thin film. From scanning tunnelling spectroscopy (STS) studies, we find that this atomically-thin layered silicon has distinctly different electronic properties. Angle resolved photoelectron spectroscopy (ARPES) reveals that, in sharp contrast to epitaxial silicene, the layered silicon exhibits significantly enhanced density of states at the Fermi level resulting from newly formed metallic bands. Furthermore, the 2D growth of this material could allow for direct contacting tomore » the silicene surface and demonstrates the dramatic changes in electronic structure that can occur by the addition of even a single monolayer amount of material in 2D systems.« less

Surface characterization of Nb samples electropolished together with real superconducting rf accelerator cavities

DOE PAGES

Xin Zhao; Geng, Rong -Li; Tyagi, P. V.; ...

2010-12-30

Here, we report the results of surface characterizations of niobium (Nb) samples electropolished together with a single cell superconducting radio-frequency accelerator cavity. These witness samples were located in three regions of the cavity, namely at the equator, the iris and the beam-pipe. Auger electron spectroscopy (AES) was utilized to probe the chemical composition of the topmost four atomic layers. Scanning electron microscopy with energy dispersive X-ray for elemental analysis (SEM/EDX) was used to observe the surface topography and chemical composition at the micrometer scale. A few atomic layers of sulfur (S) were found covering the samples non-uniformly. Niobium oxide granulesmore » with a sharp geometry were observed on every sample. Some Nb-O granules appeared to also contain sulfur.« less

Enhanced ZnO Thin-Film Transistor Performance Using Bilayer Gate Dielectrics.

PubMed

Alshammari, Fwzah H; Nayak, Pradipta K; Wang, Zhenwei; Alshareef, Husam N

2016-09-07

We report ZnO TFTs using Al2O3/Ta2O5 bilayer gate dielectrics grown by atomic layer deposition. The saturation mobility of single layer Ta2O5 dielectric TFT was 0.1 cm(2) V(-1) s(-1), but increased to 13.3 cm(2) V(-1) s(-1) using Al2O3/Ta2O5 bilayer dielectric with significantly lower leakage current and hysteresis. We show that point defects present in ZnO film, particularly VZn, are the main reason for the poor TFT performance with single layer dielectric, although interfacial roughness scattering effects cannot be ruled out. Our approach combines the high dielectric constant of Ta2O5 and the excellent Al2O3/ZnO interface quality, resulting in improved device performance.

Atom-scale covalent electrochemical modification of single-layer graphene on SiC substrates by diaryliodonium salts

DOE PAGES

Gearba, Raluca I.; Mueller, Kory M.; Veneman, Peter A.; ...

2015-05-09

Owing to its high conductivity, graphene holds promise as an electrode for energy devices such as batteries and photovoltaics. However, to this end, the work function and doping levels in graphene need to be precisely tuned. One promising route for modifying graphene’s electronic properties is via controlled covalent electrochemical grafting of molecules. We show that by employing diaryliodonium salts instead of the commonly used diazonium salts, spontaneous functionalization is avoided. This then allows for precise tuning of the grafting density. Moreover, by employing bis(4-nitrophenyl)iodonium(III) tetrafluoroborate (DNP) salt calibration curves, the surface functionalization density (coverage) of glassy carbon was controlled usingmore » cyclic voltammetry in varying salt concentrations. These electro-grafting conditions and calibration curves translated directly over to modifying single layer epitaxial graphene substrates (grown on insulating 6H-SiC (0 0 0 1)). In addition to quantifying the functionalization densities using electrochemical methods, samples with low grafting densities were characterized by low-temperature scanning tunneling microscopy (LT-STM). We show that the use of buffer-layer free graphene substrates is required for clear observation of the nitrophenyl modifications. Furthermore, atomically-resolved STM images of single site modifications were obtained, showing no preferential grafting at defect sites or SiC step edges as supposed previously in the literature. Most of the grafts exhibit threefold symmetry, but occasional extended modifications (larger than 4 nm) were observed as well.« less

Direct observation of interfacial Au atoms on TiO₂ in three dimensions.

PubMed

Gao, Wenpei; Sivaramakrishnan, Shankar; Wen, Jianguo; Zuo, Jian-Min

2015-04-08

Interfacial atoms, which result from interactions between the metal nanoparticles and support, have a large impact on the physical and chemical properties of nanoparticles. However, they are difficult to observe; the lack of knowledge has been a major obstacle toward unraveling their role in chemical transformations. Here we report conclusive evidence of interfacial Au atoms formed on the rutile (TiO2) (110) surfaces by activation using high-temperature (∼500 °C) annealing in air. Three-dimensional imaging was performed using depth-sectioning enabled by aberration-corrected scanning transmission electron microscopy. Results show that the interface between Au nanocrystals and TiO2 (110) surfaces consists of a single atomic layer with Au atoms embedded inside Ti-O. The number of interfacial Au atoms is estimated from ∼1-8 in an interfacial atomic column. Direct impact of interfacial Au atoms is observed on an enhanced Au-TiO2 interaction and the reduction of surface TiO2; both are critical to Au catalysis.

Ejection-ionization of molecules from free standing graphene

NASA Astrophysics Data System (ADS)

Verkhoturov, Stanislav V.; Czerwinski, Bartlomiej; Verkhoturov, Dmitriy S.; Geng, Sheng; Delcorte, Arnaud; Schweikert, Emile A.

2017-02-01

We present the first data on emission of -C60 stimulated by single impacts of 50 keV C60+2 on the self-assembled molecular layer of C60 deposited on free standing 2 layer graphene. The yield, Y, of -C60 emitted in the transmission direction is 1.7%. To characterize the ejection and ionization of molecules, we have measured the emission of -C60 from the surface of bulk C60 (Y = 3.7%) and from a single layer of C60 deposited on bulk pyrolytic graphite (Y = 3.3%). To gain insight into the mechanism(s) of ejection, molecular dynamic simulations were performed. The scenario of the energy deposition and ejection of molecules is different for the case of graphene due to the confined volume of projectile-analyte interaction. In the case of 50 keV C60+2 impacts on graphene plus C60, the C atoms of the projectile collide with those of the target. The knocked-on atoms take on a part of the kinetic energy of the projectile atoms. Another part of the kinetic energy is deposited into the rim around the impact site. The ejection of molecules from the rim is a result of collective movement of the molecules and graphene membrane, where the membrane movement provides the impulse for ejection. The efficient emission of the intact molecular ions implies an effective ionization probability of intact C60. The proposed mechanism of ionization involves the tunneling of electrons from the vibrationally exited area around the hole to the ejecta.

Point defects in the 1 T' and 2 H phases of single-layer MoS2: A comparative first-principles study

NASA Astrophysics Data System (ADS)

Pizzochero, Michele; Yazyev, Oleg V.

2017-12-01

The metastable 1 T' phase of layered transition metal dichalcogenides has recently attracted considerable interest due to electronic properties, possible topological phases, and catalytic activity. We report a comprehensive theoretical investigation of intrinsic point defects in the 1 T' crystalline phase of single-layer molybdenum disulfide (1 T'-MoS2 ) and provide comparison to the well-studied semiconducting 2 H phase. Based on density functional theory calculations, we explore a large number of configurations of vacancy, adatom, and antisite defects and analyze their atomic structure, thermodynamic stability, and electronic and magnetic properties. The emerging picture suggests that, under thermodynamic equilibrium, 1 T'-MoS2 is more prone to hosting lattice imperfections than the 2 H phase. More specifically, our findings reveal that the S atoms that are closer to the Mo atomic plane are the most reactive sites. Similarly to the 2 H phase, S vacancies and adatoms in 1 T'-MoS2 are very likely to occur while Mo adatoms and antisites induce local magnetic moments. Contrary to the 2 H phase, Mo vacancies in 1 T'-MoS2 are expected to be an abundant defect due to the structural relaxation that plays a major role in lowering the defect formation energy. Overall, our study predicts that the realization of high-quality flakes of 1 T'-MoS2 should be carried out under very careful laboratory conditions but at the same time the facile defects introduction can be exploited to tailor physical and chemical properties of this polymorph.

Formation of Multilayer Cu Islands Embedded beneath the Surface of Graphite: Characterization and Fundamental Insights

DOE PAGES

Lii-Rosales, Ann; Han, Yong; Evans, James W.; ...

2018-02-06

Here in this paper, we present an extensive experimental study of the conditions under which Cu forms encapsulated islands under the top surface layers of graphite, as a result of physical vapor deposition of Cu on argon-ion-bombarded graphite. When the substrate is held at 800 K during deposition, conditions are optimal for formation of encapsulated multilayer Cu islands. Deposition temperatures below 600 K favor adsorbed Cu clusters, while deposition temperatures above 800 K favor a different type of feature that is probably a single-layer intercalated Cu island. The multilayer Cu islands are characterized with respect to size and shape, thicknessmore » and continuity of the graphitic overlayer, relationship to graphite steps, and stability in air. The experimental techniques are scanning tunneling microscopy and X-ray photoelectron spectroscopy. We also present an extensive study using density functional theory to compare stabilities of a wide variety of configurations of Cu atoms, Cu clusters, and Cu layers on/under the graphite surface. The only configuration that is significantly more stable under the graphite surface than on top of it, is a single Cu atom. This analysis leads us to conclude that formation of encapsulated Cu islands is kinetically driven, rather than thermodynamically driven.« less

Formation of Multilayer Cu Islands Embedded beneath the Surface of Graphite: Characterization and Fundamental Insights

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

Lii-Rosales, Ann; Han, Yong; Evans, James W.

Here in this paper, we present an extensive experimental study of the conditions under which Cu forms encapsulated islands under the top surface layers of graphite, as a result of physical vapor deposition of Cu on argon-ion-bombarded graphite. When the substrate is held at 800 K during deposition, conditions are optimal for formation of encapsulated multilayer Cu islands. Deposition temperatures below 600 K favor adsorbed Cu clusters, while deposition temperatures above 800 K favor a different type of feature that is probably a single-layer intercalated Cu island. The multilayer Cu islands are characterized with respect to size and shape, thicknessmore » and continuity of the graphitic overlayer, relationship to graphite steps, and stability in air. The experimental techniques are scanning tunneling microscopy and X-ray photoelectron spectroscopy. We also present an extensive study using density functional theory to compare stabilities of a wide variety of configurations of Cu atoms, Cu clusters, and Cu layers on/under the graphite surface. The only configuration that is significantly more stable under the graphite surface than on top of it, is a single Cu atom. This analysis leads us to conclude that formation of encapsulated Cu islands is kinetically driven, rather than thermodynamically driven.« less

Large-area, freestanding, single-layer graphene-gold: a hybrid plasmonic nanostructure.

PubMed

Iyer, Ganjigunte R Swathi; Wang, Jian; Wells, Garth; Guruvenket, Srinivasan; Payne, Scott; Bradley, Michael; Borondics, Ferenc

2014-06-24

Graphene-based plasmonic devices have recently drawn great attention. However, practical limitations in fabrication and device architectures prevent studies from being carried out on the intrinsic properties of graphene and their change by plasmonic structures. The influence of a quasi-infinite object (i.e., the substrate) on graphene, being a single sheet of carbon atoms, and the plasmonic device is overwhelming. To address this and put the intrinsic properties of the graphene-plasmonic nanostructures in focus, we fabricate large-area, freestanding, single-layer graphene-gold (LFG-Au) sandwich structures and Au nanoparticle decorated graphene (formed via thermal treatment) hybrid plasmonic nanostructures. We observed two distinct plasmonic enhancement routes of graphene unique to each structure via surface-enhanced Raman spectroscopy. The localized electronic structure variation in the LFG due to graphene-Au interaction at the nanoscale is mapped using scanning transmission X-ray microscopy. The measurements show an optical density of ∼0.007, which is the smallest experimentally determined for single-layer graphene thus far. Our results on freestanding graphene-Au plasmonic structures provide great insight for the rational design and future fabrication of graphene plasmonic hybrid nanostructures.

Influence of low energy argon plasma treatment on the moisture barrier performance of hot wire-CVD grown SiNx multilayers

NASA Astrophysics Data System (ADS)

Majee, Subimal; Fátima Cerqueira, Maria; Tondelier, Denis; Geffroy, Bernard; Bonnassieux, Yvan; Alpuim, Pedro; Bourée, Jean Eric

2014-01-01

The reliability and stability are key issues for the commercial utilization of organic photovoltaic devices based on flexible polymer substrates. To increase the shelf-lifetime of these devices, transparent moisture barriers of silicon nitride (SiNx) films are deposited at low temperature by hot wire CVD (HW-CVD) process. Instead of the conventional route based on organic/inorganic hybrid structures, this work defines a new route consisting in depositing multilayer stacks of SiNx thin films, each single layer being treated by argon plasma. The plasma treatment allows creating smoother surface and surface atom rearrangement. We define a critical thickness of the single layer film and focus our attention on the effect of increasing the number of SiNx single-layers on the barrier properties. A water vapor transmission rate (WVTR) of 2 × 10-4 g/(m2·day) is reported for SiNx multilayer stack and a physical interpretation of the plasma treatment effect is given.

Mechanical behavior enhancement of defective graphene sheet employing boron nitride coating via atomistic study

NASA Astrophysics Data System (ADS)

Setoodeh, A. R.; Badjian, H.

2017-12-01

The most stable form of boron nitride polymorph naming hexagonal boron nitride sheet has recently been widely concerned like graphite due to its interesting features such as electrical insulation and high thermal conductivity. In this study, the molecular dynamic simulations are implemented to investigate the mechanical properties of single-layer graphene sheets under tensile and compressive loadings in the absence and presence of boron-nitride coating layers. In this introduced hybrid nanostructure, the benefit of combining both individual interesting features of graphene and boron-nitride sheets such as exceptional mechanical and electrical properties can be simultaneously achieved for future potential application in nano devices. The influences of chiral indices, boundary conditions and presence of mono-atomic vacancy defects as well as coating dimension on the mechanical behavior of the resulted hybrid structure are reported. The interatomic forces between the atoms are modeled by employing the AIREBO and Tersoff-Brenner potentials for carbon-carbon and boron-nitrogen atoms in each layer, respectively. Furthermore, the van der Waal interlayer forces of carbon-boron and carbon-nitrogen are estimated by the Lennard-Jones potential field. Besides the potential improvement in electrical and physical properties of the nanostructure, it is demonstrated that the buckling load capacity of the fully coated graphene sheet with 3% concentration of mono-atomic vacancy defects noticeably enhances by amounts of 24.1%.

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

Han, Yong; Lii-Rosales, A.; Zhou, Y.

Theory and stochastic lattice-gas modeling is developed for the formation of intercalated metal islands in the gallery between the top layer and the underlying layer at the surface of layered materials. Our model for this process involves deposition of atoms, some fraction of which then enter the gallery through well-separated pointlike defects in the top layer. Subsequently, these atoms diffuse within the subsurface gallery leading to nucleation and growth of intercalated islands nearby the defect point source. For the case of a single point defect, continuum diffusion equation analysis provides insight into the nucleation kinetics. However, complementary tailored lattice-gas modelingmore » produces a more comprehensive and quantitative characterization. We analyze the large spread in nucleation times and positions relative to the defect for the first nucleated island. We also consider the formation of subsequent islands and the evolution of island growth shapes. The shapes reflect in part our natural adoption of a hexagonal close-packed island structure. As a result, motivation and support for the model is provided by scanning tunneling microscopy observations of the formation of intercalated metal islands in highly-ordered pyrolytic graphite at higher temperatures.« less

Heat-transport mechanisms in molecular building blocks of inorganic/organic hybrid superlattices

NASA Astrophysics Data System (ADS)

Giri, Ashutosh; Niemelä, Janne-Petteri; Tynell, Tommi; Gaskins, John T.; Donovan, Brian F.; Karppinen, Maarit; Hopkins, Patrick E.

2016-03-01

Nanomaterial interfaces and concomitant thermal resistances are generally considered as atomic-scale planes that scatter the fundamental energy carriers. Given that the nanoscale structural and chemical properties of solid interfaces can strongly influence this thermal boundary conductance, the ballistic and diffusive nature of phonon transport along with the corresponding phonon wavelengths can affect how energy is scattered and transmitted across an interfacial region between two materials. In hybrid composites composed of atomic layer building blocks of inorganic and organic constituents, the varying interaction between the phononic spectrum in the inorganic crystals and vibronic modes in the molecular films can provide a new avenue to manipulate the energy exchange between the fundamental vibrational energy carriers across interfaces. Here, we systematically study the heat transfer mechanisms in hybrid superlattices of atomic- and molecular-layer-grown zinc oxide and hydroquinone with varying thicknesses of the inorganic and organic layers in the superlattices. We demonstrate ballistic energy transfer of phonons in the zinc oxide that is limited by scattering at the zinc oxide/hydroquinone interface for superlattices with a single monolayer of hydroquinone separating the thicker inorganic layers. The concomitant thermal boundary conductance across the zinc oxide interfacial region approaches the maximal thermal boundary conductance of a zinc oxide phonon flux, indicative of the contribution of long wavelength vibrations across the aromatic molecular monolayers in transmitting energy across the interface. This transmission of energy across the molecular interface decreases considerably as the thickness of the organic layers are increased.

Nucleation and growth kinetics for intercalated islands during deposition on layered materials with isolated pointlike surface defects

DOE PAGES

Han, Yong; Lii-Rosales, A.; Zhou, Y.; ...

2017-10-13

Theory and stochastic lattice-gas modeling is developed for the formation of intercalated metal islands in the gallery between the top layer and the underlying layer at the surface of layered materials. Our model for this process involves deposition of atoms, some fraction of which then enter the gallery through well-separated pointlike defects in the top layer. Subsequently, these atoms diffuse within the subsurface gallery leading to nucleation and growth of intercalated islands nearby the defect point source. For the case of a single point defect, continuum diffusion equation analysis provides insight into the nucleation kinetics. However, complementary tailored lattice-gas modelingmore » produces a more comprehensive and quantitative characterization. We analyze the large spread in nucleation times and positions relative to the defect for the first nucleated island. We also consider the formation of subsequent islands and the evolution of island growth shapes. The shapes reflect in part our natural adoption of a hexagonal close-packed island structure. As a result, motivation and support for the model is provided by scanning tunneling microscopy observations of the formation of intercalated metal islands in highly-ordered pyrolytic graphite at higher temperatures.« less

Interpenetration of a 3D Icosahedral M@Ni12 (M=Al, Ga) Framework with Porphyrin-Reminiscent Boron Layers in MNi9 B8.

PubMed

Zheng, Qiang; Wagner, Frank R; Ormeci, Alim; Prots, Yurii; Burkhardt, Ulrich; Schmidt, Marcus; Schnelle, Walter; Grin, Yuri; Leithe-Jasper, Andreas

2015-11-09

Two ternary borides MNi9 B8 (M=Al, Ga) were synthesized by thermal treatment of mixtures of the elements. Single-crystal X-ray diffraction data reveal AlNi9 B8 and GaNi9 B8 crystallizing in a new type of structure within the space group Cmcm and the lattice parameters a=7.0896(3) Å, b=8.1181(3) Å, c=10.6497(4) Å and a=7.0897(5) Å, b=8.1579(4) Å, c=10.6648(7) Å, respectively. The boron atoms build up two-dimensional layers, which consist of puckered [B16 ] rings with two tailing B atoms, whereas the M atoms reside in distorted vertices-condensed [Ni12 ] icosahedra, which form a three-dimensional framework interpenetrated by boron porphyrin-reminiscent layers. An unusual local arrangement resembling a giant metallo-porphyrin entity is formed by the [B16 ] rings, which, due to their large annular size of approximately 8 Å, chelate four of the twelve icosahedral Ni atoms. An analysis of the chemical bonding by means of the electron localizability approach reveals strong covalent B-B interactions and weak Ni-Ni interactions. Multi-center dative B-Ni interaction occurs between the Al-Ni framework and the boron layers. In agreement with the chemical bonding analysis and band structure calculations, AlNi9 B8 is a Pauli-paramagnetic metal. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Effect of Ti seed layers on structure of self-organized epitaxial face-centered-cubic-Ag(001) oriented nanodots

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

Kamiko, M.; Nose, K.; Suenaga, R.

2013-12-28

The influence of Ti seed layers on the structure of self-organized Ag nanodots, obtained with a Ti seed-layer-assisted thermal agglomeration method, has been investigated. The samples were grown on MgO(001) single crystal substrates by RF magnetron sputter deposition. The samples were deposited at room temperature and post-annealed at 350 °C for 4 h while maintaining the chamber vacuum conditions. The results of atomic force microscopy (AFM) observations indicated that the insertion of the Ti seed layer (0.6–5.0 nm) between the MgO substrate and Ag layer promotes the agglomeration process, forming the nanodot array. Comparisons between the AFM images revealed thatmore » the size of the Ag nanodots was increased with an increase in the Ti seed layer thickness. The atomic concentration of the film surface was confirmed by X-ray photoelectron spectroscopy (XPS). The XPS result suggested that the nanodot surface mainly consisted of Ag. Moreover, X-ray diffraction results proved that the initial deposition of the Ti seed layer (0.6–5.0 nm) onto MgO(001) prior to the Ag deposition yielded high-quality fcc-Ag(001) oriented epitaxial nanodots. The optical absorbance spectra of the fabricated Ag nanodots with various Ti seed layer thicknesses were obtained in the visible light range.« less

Tuning the properties of metal–organic framework nodes as supports of single-site iridium catalysts: node modification by atomic layer deposition of aluminium

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

Yang, Dong; Momeni, Mohammad R.; Demir, Hakan

The metal–organic framework NU-1000, with Zr 6-oxo, hydroxo, and aqua nodes, was modified by incorporation of hydroxylated Al(iii) ions by ALD-like chemistry with [Al(CH 3) 2(iso-propoxide)] 2followed by steam (ALD = atomic layer deposition). Al ions were installed to the extent of approximately 7 per node. Single-site iridium diethylene complexes were anchored to the nodes of the modified and unmodified MOFs by reaction with Ir(C 2H 4) 2(acac) (acac = acetylacetonate) and converted to Ir(CO) 2complexes by treatment with CO. Infrared spectra of these supported complexes show that incorporation of Al weakened the electron donor tendency of the MOF. Correspondingly,more » the catalytic activity of the initial supported iridium complexes for ethylene hydrogenation increased, as did the selectivity for ethylene dimerization. The results of density functional theory calculations with a simplified model of the nodes incorporating Al(iii) ions are in qualitative agreement with some catalyst performance data.« less

Strength and stability analysis of a single-walled black phosphorus tube under axial compression

NASA Astrophysics Data System (ADS)

Cai, Kun; Wan, Jing; Wei, Ning; Qin, Qing H.

2016-07-01

Few-layered black phosphorus materials currently attract much attention due to their special electronic properties. As a consequence, a single-layer black phosphorus (SLBP) nanotube has been theoretically built. The corresponding electronic properties of such a black phosphorus nanotube (BPNT) were also evaluated numerically. However, unlike graphene formed with 2sp2 covalent carbon atoms, SLBP is formed with 3sp3 bonded atoms. It means that the structure from SLBP will possess lower Young’s modulus and mechanical strength than those of carbon nanotubes. In this study, molecular dynamics simulation is performed to investigate the strength and stability of BPNTs affected by the factors of diameter, length, loading speed and temperature. Results are fundamental for investigating the other physical properties of a BPNT acting as a component in a nanodevice. For example, buckling of the BPNT happens earlier than fracture, before which the nanostructure has very small axial strain. For the same BPNT, a higher load speed results in lower critical axial strain and a nanotube with lower axial strain can still be stable at a higher temperature.

Microcutting characteristics on the single crystal diamond tool with edge radius using molecular dynamics

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

Kim, Jeong-Du; Moon, Chan-Hong

1995-12-31

Ultraprecision metal cutting (UPMC) technology which makes possible submicrometer form accuracy and manometer roughness is developed to reach the 1nm nominal (undeformed) thickness of cut. At this thickness level, a few of atom`s layers should be considered. In this paper using the Molecuar Dynamics simulation, the phenomena of microcutting with a subnanometer chip thickness, the cutting mechanism for tool edge configuration to consider the sharp edge and round edge tool, the cut material and cutting speed are evaluated. Cutting mechanism of subnanometer depth of cut is evaluated.

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

Toward the growth of an aligned single-layer MoS2 film.

PubMed

Kim, Daeho; Sun, Dezheng; Lu, Wenhao; Cheng, Zhihai; Zhu, Yeming; Le, Duy; Rahman, Talat S; Bartels, Ludwig

2011-09-20

Molybdenum disulfide (molybdenite) monolayer islands and flakes have been grown on a copper surface at comparatively low temperature and mild conditions through sulfur loading of the substrate using thiophenol (benzenethiol) followed by the evaporation of Mo atoms and annealing. The MoS(2) islands show a regular Moiré pattern in scanning tunneling microscopy, attesting to their atomic ordering and high quality. They are all aligned with the substrate high-symmetry directions providing for rotational-domain-free monolayer growth. © 2011 American Chemical Society

MCP performance improvement using alumina thin film

NASA Astrophysics Data System (ADS)

Yang, Yuzhen; Yan, Baojun; Liu, Shulin; Zhao, Tianchi; Yu, Yang; Wen, Kaile; Li, Yumei; Qi, Ming

2017-10-01

The performance improvement using alumina thin film on a dual microchannel plate (MCP) detector for single electron counting was investigated. The alumina thin film was coated on all surfaces of the MCPs by atomic layer deposition method. It was found that the gain, the single electron resolution and the peak-to-valley ratio of the dual MCP detector were significantly enhanced by coating the alumina thin film. The optimum operating conditions of the new dual MCP detector have been studied.

Auger electron diffraction study of the initial stage of Ge heteroepitaxy on Si(001)

NASA Astrophysics Data System (ADS)

Sasaki, M.; Abukawa, T.; Yeom, H. W.; Yamada, M.; Suzuki, S.; Sato, S.; Kono, S.

1994-12-01

The initial stage of pure and surfactant (Sb)-assisted Ge growth on a Si(001) surface has been studied by Auger electron diffraction (AED) and X-ray photoelectron diffraction (XPD). A single-domain Si(001)2 × 1 substrate was used to avoid the ambiguity arising from the usual double-domain substrate. For the pure Ge growth, 1 monolayer of Ge was deposited onto the room temperature substrate followed by annealing at 350°C-600°C, which appeared to have (1 × 2) periodicity by LEED. Ge LMM AED patterns were measured to find that a substantial amount of Ge atoms diffuse to the bulk Si positions up to the fourth layer at least. For the Sb-assisted Ge growth, a Sb(1 × 2)/Si(001) surface was first prepared and Sb 3d XPD patterns were measured to find that Sb forms dimers on the substrate. 1 ML of Ge was deposited onto the Sb(1 × 2)/Si(001) surface and then the surface was annealed at 600°C. Ge LMM AED and Sb 3d XPD patterns measured for this surface showed that surfactant Sb atoms are indeed present on the first layer forming dimers and that Ge atoms are present mainly on the second layer with a substantial amount of Ge diffused into the third and fourth layers.

Resolving the Chemically Discrete Structure of Synthetic Borophene Polymorphs.

PubMed

Campbell, Gavin P; Mannix, Andrew J; Emery, Jonathan D; Lee, Tien-Lin; Guisinger, Nathan P; Hersam, Mark C; Bedzyk, Michael J

2018-05-09

Atomically thin two-dimensional (2D) materials exhibit superlative properties dictated by their intralayer atomic structure, which is typically derived from a limited number of thermodynamically stable bulk layered crystals (e.g., graphene from graphite). The growth of entirely synthetic 2D crystals, those with no corresponding bulk allotrope, would circumvent this dependence upon bulk thermodynamics and substantially expand the phase space available for structure-property engineering of 2D materials. However, it remains unclear if synthetic 2D materials can exist as structurally and chemically distinct layers anchored by van der Waals (vdW) forces, as opposed to strongly bound adlayers. Here, we show that atomically thin sheets of boron (i.e., borophene) grown on the Ag(111) surface exhibit a vdW-like structure without a corresponding bulk allotrope. Using X-ray standing wave-excited X-ray photoelectron spectroscopy, the positions of boron in multiple chemical states are resolved with sub-angström spatial resolution, revealing that the borophene forms a single planar layer that is 2.4 Å above the unreconstructed Ag surface. Moreover, our results reveal that multiple borophene phases exhibit these characteristics, denoting a unique form of polymorphism consistent with recent predictions. This observation of synthetic borophene as chemically discrete from the growth substrate suggests that it is possible to engineer a much wider variety of 2D materials than those accessible through bulk layered crystal structures.

Surface passivation of n-type doped black silicon by atomic-layer-deposited SiO2/Al2O3 stacks

NASA Astrophysics Data System (ADS)

van de Loo, B. W. H.; Ingenito, A.; Verheijen, M. A.; Isabella, O.; Zeman, M.; Kessels, W. M. M.

2017-06-01

Black silicon (b-Si) nanotextures can significantly enhance the light absorption of crystalline silicon solar cells. Nevertheless, for a successful application of b-Si textures in industrially relevant solar cell architectures, it is imperative that charge-carrier recombination at particularly highly n-type doped black Si surfaces is further suppressed. In this work, this issue is addressed through systematically studying lowly and highly doped b-Si surfaces, which are passivated by atomic-layer-deposited Al2O3 films or SiO2/Al2O3 stacks. In lowly doped b-Si textures, a very low surface recombination prefactor of 16 fA/cm2 was found after surface passivation by Al2O3. The excellent passivation was achieved after a dedicated wet-chemical treatment prior to surface passivation, which removed structural defects which resided below the b-Si surface. On highly n-type doped b-Si, the SiO2/Al2O3 stacks result in a considerable improvement in surface passivation compared to the Al2O3 single layers. The atomic-layer-deposited SiO2/Al2O3 stacks therefore provide a low-temperature, industrially viable passivation method, enabling the application of highly n- type doped b-Si nanotextures in industrial silicon solar cells.

Charge transfer in single and multiple scattering events at metal surfaces: a wavepacket study of the Na(+)/Cu(100) system.

PubMed

Sindona, A; Pisarra, M; Maletta, S; Riccardi, P; Falcone, G

2010-12-01

Resonant neutralization of hyperthermal energy Na(+) ions impinging on Cu(100) surfaces is studied, focusing on two specific collision events: one in which the projectile is reflected off the surface, the other in which the incident atom penetrates the outer surface layers initiating a series of scattering processes, within the target, and coming out together with a single surface atom. A semi-empirical model potential is adopted that embeds: (i) the electronic structure of the sample, (ii) the central field of the projectile, and (iii) the contribution of the Cu atom ejected in multiple scattering events. The evolution of the ionization orbital of the scattered atom is simulated, backwards in time, using a wavepacket propagation algorithm. The output of the approach is the neutralization probability, obtained by projecting the time-reversed valence wavefunction of the projectile onto the initially filled conduction band states. The results are in agreement with available data from the literature (Keller et al 1995 Phys. Rev. Lett. 75 1654) indicating that the motion of surface atoms, exiting the targets with kinetic energies of the order of a few electronvolts, plays a significant role in the final charge state of projectiles.

Vertically Oriented Growth of GaN Nanorods on Si Using Graphene as an Atomically Thin Buffer Layer.

PubMed

Heilmann, Martin; Munshi, A Mazid; Sarau, George; Göbelt, Manuela; Tessarek, Christian; Fauske, Vidar T; van Helvoort, Antonius T J; Yang, Jianfeng; Latzel, Michael; Hoffmann, Björn; Conibeer, Gavin; Weman, Helge; Christiansen, Silke

2016-06-08

The monolithic integration of wurtzite GaN on Si via metal-organic vapor phase epitaxy is strongly hampered by lattice and thermal mismatch as well as meltback etching. This study presents single-layer graphene as an atomically thin buffer layer for c-axis-oriented growth of vertically aligned GaN nanorods mediated by nanometer-sized AlGaN nucleation islands. Nanostructures of similar morphology are demonstrated on graphene-covered Si(111) as well as Si(100). High crystal and optical quality of the nanorods are evidenced through scanning transmission electron microscopy, micro-Raman, and cathodoluminescence measurements supported by finite-difference time-domain simulations. Current-voltage characteristics revealed high vertical conduction of the as-grown GaN nanorods through the Si substrates. These findings are substantial to advance the integration of GaN-based devices on any substrates of choice that sustains the GaN growth temperatures, thereby permitting novel designs of GaN-based heterojunction device concepts.

Molecular dynamics study of the melting of a supported 887-atom Pd decahedron.

PubMed

Schebarchov, D; Hendy, S C; Polak, W

2009-04-08

We employ classical molecular dynamics simulations to investigate the melting behaviour of a decahedral Pd(887) cluster on a single layer of graphite (graphene). The interaction between Pd atoms is modelled with an embedded-atom potential, while the adhesion of Pd atoms to the substrate is approximated with a Lennard-Jones potential. We find that the decahedral structure persists at temperatures close to the melting point, but that just below the melting transition, the cluster accommodates to the substrate by means of complete melting and then recrystallization into an fcc structure. These structural changes are in qualitative agreement with recently proposed models, and they verify the existence of an energy barrier preventing softly deposited clusters from 'wetting' the substrate at temperatures below the melting point.

Crystallinity of tellurium capping and epitaxy of ferromagnetic topological insulator films on SrTiO 3

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

Park, Jihwey; Soh, Yeong-Ah; Aeppli, Gabriel

2015-06-30

Thin films of topological insulators are often capped with an insulating layer since topological insulators are known to be fragile to degradation. However, capping can hinder the observation of novel transport properties of the surface states. To understand the influence of capping on the surface states, it is crucial to understand the crystal structure and the atomic arrangement at the interfaces. Here, we use x-ray diffraction to establish the crystal structure of magnetic topological insulator Cr-doped (Bi,Sb) 2Te 3 (CBST) films grown on SrTiO 3 (1 1 1) substrates with and without a Te capping layer. We find that bothmore » the film and capping layer are single crystal and that the crystal quality of the film is independent of the presence of the capping layer, but that x-rays cause sublimation of the CBST film, which is prevented by the capping layer. Our findings show that the different transport properties of capped films cannot be attributed to a lower crystal quality but to a more subtle effect such as a different electronic structure at the interface with the capping layer. Our results on the crystal structure and atomic arrangements of the topological heterostructure will enable modelling the electronic structure and design of topological heterostructures.« less

Formation of nanooctahedra in molybdenum disulfide and molybdenum diselenide using pulsed laser vaporization.

PubMed

Parilla, Philip A; Dillon, Anne C; Parkinson, Bruce A; Jones, Kim M; Alleman, Jeff; Riker, Gerald; Ginley, David S; Heben, Michael J

2004-05-20

Pulsed laser vaporization has been used to produce nanooctahedra of MoS2 and MoSe2. The nanooctahedra primarily form in two- or three-layer nested octahedra, although nesting up to five layers has been observed. Tilting the TEM sample stage and mapping how the images of single particles transformed provided the evidence to verify their octahedral geometry. Analysis of 30 two- and three-layered octahedra showed that their outer edge lengths clustered at approximately 3.8 nm and approximately 5.1 nm, respectively. This discreet sizing and the high symmetry of these closed nanooctahedra represent the closest inorganic analogy yet to the carbon fullerenes. The geometrical implications for forming octahedra from these layered compounds are investigated by considering different atomic arrangements assuming either trigonal prismatic or octahedral coordination around the Mo atom and yields two possible configurations for the actual structure of the nanooctahedra. A preliminary survey of pulsed laser vaporization of other layered metal chalcogenides shows that these dichalcogenides differ in their tendency to form small closed layered fullerene-like structures. These materials can be ranked from highest tendency to lowest as follows: NbSe2, WS2, WSe2, SnS2, TaS2, GaS, ReS2, and MoTe2.

Theoretical modeling and experimental observations of the atomic layer deposition of SrO using a cyclopentadienyl Sr precursor

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

Fredrickson, Kurt D.; Slepko, Alex; Demkov, Alexander A., E-mail: demkov@physics.utexas.edu

2016-08-14

First-principle calculations are used to model the adsorption and hydration of strontium bis(cyclopentadienyl) [Sr(Cp){sub 2}] on TiO{sub 2}-terminated strontium titanate, SrTiO{sub 3} (STO), for the deposition of strontium oxide, SrO, by atomic layer deposition (ALD). The Sr(Cp){sub 2} precursor is shown to adsorb on the TiO{sub 2}-terminated surface, with the Sr atom assuming essentially the bulk position in STO. The C–Sr bonds are weaker than in the free molecule, with a Ti atom at the surface bonding to one of the C atoms in the cyclopentadienyl rings. The surface does not need to be hydrogenated for precursor adsorption. The calculationsmore » are compared with experimental observations for a related Sr cyclopentadienyl precursor, strontium bis(triisopropylcyclopentadienyl) [Sr({sup i}Pr{sub 3}Cp){sub 2}], adsorbed on TiO{sub 2}-terminated STO. High-resolution x-ray photoelectron spectroscopy and low-energy ion scattering spectroscopy show adsorption of the Sr precursor on the TiO{sub 2}-terminated STO after a single precursor dose. This study suggests that ALD growth from the strontium precursors featuring cyclopentadienyl ligands, such as Sr(Cp){sub 2}, may initiate film growth on non-hydroxylated surfaces.« less

The deflection of carbon composite carbon nanotube / graphene using molecular dynamics simulation

NASA Astrophysics Data System (ADS)

Kolesnikova, A. S.; Kirillova, I. V.; Kossovich, L. U.

2018-02-01

For the first time, the dependence of the bending force on the transverse displacement of atoms in the center of the composite material consisting of graphene and parallel oriented zigzag nanotubes was studied. Mathematical modeling of the action of the needle of the atomic force microscope was carried out using the single-layer armchair carbon nanotube. Armchair nanotubes are convenient for using them as a needle of an atomic force microscope, because their edges are not sharpened (unlike zigzag tubes). Consequently, armchair nanotubes will cause minimal damage upon contact with the investigation object. The geometric parameters of the composite was revealed under the action of the bending force of 6μN.

New-class of Semiconducting 2D materials: Tin Dichalcogenides (SnX2)

NASA Astrophysics Data System (ADS)

Ataca, Can; Wu, Kedi; Saritas, Kayahan; Tongay, Sefaattin; Grossman, Jeffrey C.

2015-03-01

Recent studies have focused on a new generation of atomically thin films of semiconducting materials. A broad family of two-dimensional (2D) semiconducting transition metal dichalcogenides (MX2) have been fabricated and investigated in monolayer, bilayer and few layer form. In this work, we investigated the electronic, optical and elastic properties of single and few layer and bulk SnX2 (X = S, Se) both theoretically and experimentally. Using density functional theory (DFT) we carried out stability analysis through phonon and electronic, optical and elastic structure calculations. Single-few layer SnX2s are mechanically exfoliated and Raman and photoluminescence (PL) measurements are taken. UV-Vis absorption spectrum together with PL measurements and DFT calculations yield an indirect gap of ~ 2.5 eV for SnS2 structures (bulk). Tunability of the energy band gap and indirect-direct gap transitions are investigated by controlling the number of layers and applied stress. Lowering the number of layers decreases the indirect gap (0.1-0.3 eV), but indirect-direct gap transition occurs when layer-layer distance is reduced. Due to flexibility in engineering the electronic and optical properties, SnX2 compounds are promising materials for future optoelectronic nanoscale applications.

Transition from moving to stationary double layers in a single-ended Q machine

NASA Technical Reports Server (NTRS)

Song, Bin; Merlino, R. L.; D'Angelo, N.

1990-01-01

Large-amplitude (less than about 100 percent) relaxation oscillations in the plasma potential are known to be generated when the cold endplate of a single-ended Q machine is biased positively. These oscillations are associated with double layers that form near the hot plate (plasma source) and travel toward the endplate at about the ion-acoustic velocity. At the endplate they dissolve and then form again near the hot plate, the entire process repeating itself in a regular manner. By admitting a sufficient amount of neutral gas into the system, the moving double layers were slowed down and eventually stopped. The production of stationary double layers requires an ion source on the high-potential side of the double layers. These ions are provided by ionization of the neutral gas by electrons that are accelerated through the double layer. The dependence of the critical neutral gas pressure required for stationary double-layer formation on endplate voltage, magnetic field strength, and neutral atom mass has been examined. These results are discussed in terms of a simple model of ion production and loss, including ion losses across the magnetic field.

Atom-Dependent Edge-Enhanced Second-Harmonic Generation on MoS2 Monolayers.

PubMed

Lin, Kuang-I; Ho, Yen-Hung; Liu, Shu-Bai; Ciou, Jian-Jhih; Huang, Bo-Ting; Chen, Christopher; Chang, Han-Ching; Tu, Chien-Liang; Chen, Chang-Hsiao

2018-02-14

Edge morphology and lattice orientation of single-crystal molybdenum disulfide (MoS 2 ) monolayers, a transition metal dichalcogenide (TMD), possessing a triangular shape with different edges grown by chemical vapor deposition are characterized by atomic force microscopy and transmission electron microscopy. Multiphoton laser scanning microscopy is utilized to study one-dimensional atomic edges of MoS 2 monolayers with localized midgap electronic states, which result in greatly enhanced optical second-harmonic generation (SHG). Microscopic S-zigzag edge and S-Mo Klein edge (bare Mo atoms protruding from a S-zigzag edge) terminations and the edge-atom dependent resonance energies can therefore be deduced based on SHG images. Theoretical calculations based on density functional theory clearly explain the lower energy of the S-zigzag edge states compared to the corresponding S-Mo Klein edge states. Characterization of the atomic-scale variation of edge-enhanced SHG is a step forward in this full-optical and high-yield technique of atomic-layer TMDs.

Efficiency Improvement Using Molybdenum Disulphide Interlayers in Single-Wall Carbon Nanotube/Silicon Solar Cells

PubMed Central

Alzahly, Shaykha; Yu, LePing; Gibson, Christopher T.

2018-01-01

Molybdenum disulphide (MoS2) is one of the most studied and widely applied nanomaterials from the layered transition-metal dichalcogenides (TMDs) semiconductor family. MoS2 has a large carrier diffusion length and a high carrier mobility. Combining a layered structure of single-wall carbon nanotube (SWCNT) and MoS2 with n-type silicon (n-Si) provided novel SWCNT/n-Si photovoltaic devices. The solar cell has a layered structure with Si covered first by a thin layer of MoS2 flakes and then a SWCNT film. The films were examined using scanning electron microscopy, atomic force microscopy and Raman spectroscopy. The MoS2 flake thickness ranged from 5 to 90 nm while the nanosheet’s lateral dimensions size ranged up to 1 μm2. This insertion of MoS2 improved the photoconversion efficiency (PCE) of the SWCNT/n-Si solar cells by approximately a factor of 2. PMID:29690503

Optical and Excitonic Properties of Atomically Thin Transition-Metal Dichalcogenides

NASA Astrophysics Data System (ADS)

Berkelbach, Timothy C.; Reichman, David R.

2018-03-01

Starting with the isolation of a single sheet of graphene, the study of layered materials has been one of the most active areas of condensed matter physics, chemistry, and materials science. Single-layer transition-metal dichalcogenides are direct-gap semiconducting analogs of graphene that exhibit novel electronic and optical properties. These features provide exciting opportunities for the discovery of both new fundamental physical phenomena as well as innovative device platforms. Here, we review the progress associated with the creation and use of a simple microscopic framework for describing the optical and excitonic behavior of few-layer transition-metal dichalcogenides, which is based on symmetry, band structure, and the effective interactions between charge carriers in these materials. This approach provides an often quantitative account of experiments that probe the physics associated with strong electron–hole interactions in these quasi two-dimensional systems and has been successfully employed by many groups to both describe and predict emergent excitonic behavior in these layered semiconducting systems.

Boron Nitride Nanoporous Membranes with High Surface Charge by Atomic Layer Deposition.

PubMed

Weber, Matthieu; Koonkaew, Boonprakrong; Balme, Sebastien; Utke, Ivo; Picaud, Fabien; Iatsunskyi, Igor; Coy, Emerson; Miele, Philippe; Bechelany, Mikhael

2017-05-17

In this work, we report the design and the fine-tuning of boron nitride single nanopore and nanoporous membranes by atomic layer deposition (ALD). First, we developed an ALD process based on the use of BBr 3 and NH 3 as precursors in order to synthesize BN thin films. The deposited films were characterized in terms of thickness, composition, and microstructure. Next, we used the newly developed process to grow BN films on anodic aluminum oxide nanoporous templates, demonstrating the conformality benefit of BN prepared by ALD, and its scalability for the manufacturing of membranes. For the first time, the ALD process was then used to tune the diameter of fabricated single transmembrane nanopores by adjusting the BN thickness and to enable studies of the fundamental aspects of ionic transport on a single nanopore. At pH = 7, we estimated a surface charge density of 0.16 C·m -2 without slip and 0.07 C·m -2 considering a reasonable slip length of 3 nm. Molecular dynamics simulations performed with experimental conditions confirmed the conductivities and the sign of surface charges measured. The high ion transport results obtained and the ability to fine-tune nanoporous membranes by such a scalable method pave the way toward applications such as ionic separation, energy harvesting, and ultrafiltration devices.

Microstructural and mechanical properties of Al2O3/ZrO2 nanomultilayer thin films prepared by pulsed laser deposition

NASA Astrophysics Data System (ADS)

Balakrishnan, G.; Sastikumar, D.; Kuppusami, P.; Babu, R. Venkatesh; Song, Jung Il

2018-02-01

Single layer aluminium oxide (Al2O3), zirconium oxide (ZrO2) and Al2O3/ZrO2 nano multilayer films were deposited on Si (100) substrates at room temperature by pulsed laser deposition. The development of Al2O3/ZrO2 nanolayered structure is an important method used to stabilize the high temperature phase (tetragonal and cubic) of ZrO2 at room temperature. In the Al2O3/ZrO2 multilayer structure, the Al2O3 layer was kept constant at 5 nm, while the ZrO2 layer thickness varied from 5 to 20 nm (5/5, 5/10, 5/15 and 5/20 nm) with a total of 40 bilayers. The X-ray diffraction studies of single layer Al2O3 indicated the γ-Al2O3 of cubic structure, while the single layer ZrO2 indicated both monoclinic and tetragonal phases. The 5/5 and 5/10 nm multilayer films showed the nanocrystalline nature of ZrO2 with tetragonal phase. The high resolution transmission electron microscopy studies indicated the formation of well-defined Al2O3 and ZrO2 layers and that they are of uniform thickness. The atomic force microscopy studies revealed the uniform and dense distribution of nanocrystallites. The nanoindentation studies indicated the hardness of 20.8 ± 1.10 and 10 ± 0.60 GPa, for single layer Al2O3 and ZrO2, respectively, and the hardness of multilayer films varied with bilayer thickness.

Self-limited growth of Si on B atomic-layer formed Ge(1 0 0) by ultraclean low-pressure CVD system

NASA Astrophysics Data System (ADS)

Yokogawa, Takashi; Ishibashi, Kiyohisa; Sakuraba, Masao; Murota, Junichi; Inokuchi, Yasuhiro; Kunii, Yasuo; Kurokawa, Harushige

2008-07-01

Utilizing BCl 3 reaction on Ge(1 0 0) and subsequent Si epitaxial growth by SiH 4 reaction at 300 °C, B atomic-layer doping in Si/Ge(1 0 0) heterostructure was investigated. Cl atoms on the B atomic-layer formed Ge(1 0 0) scarcely affect upon the SiH 4 reaction. It is also found that Si atom amount deposited by SiH 4 reaction on Ge(1 0 0) is effectively enhanced by the existence of B atomic layer and the deposition rate tends to decrease at around 2-3 atomic layers which is three times larger than that in the case without B. The results of angle-resolved X-ray photoelectron spectroscopy show that most B atoms are incorporated at the heterointerface between the Si and Ge.

Epitaxial Growth of Rhenium with Sputtering

DTIC Science & Technology

2016-05-06

corresponds to two atomic Re layers , considering that the c-axis lattice constant of the tri- atomic layered hcp Re unit cell is ~4.5 Å. Frequently, two...Å) corresponds to two Re atomic layers since the c-axis lattice constant of hcp Re, which is composed of three Re atomic layers , is ~4.5 Å...The growth starts in a three dimensional mode but transforms into two dimensional mode as the film gets thicker. With a thin (~2 nm) seed layer

Direct growth of graphene on in situ epitaxial hexagonal boron nitride flakes by plasma-assisted molecular beam epitaxy

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

Xu, Zhongguang; Zheng, Renjing; Khanaki, Alireza

2015-11-23

Hexagonal boron nitride (h-BN) single-crystal domains were grown on cobalt (Co) substrates at a substrate temperature of 850–900 °C using plasma-assisted molecular beam epitaxy. Three-point star shape h-BN domains were observed by scanning electron microscopy, and confirmed by Raman and X-ray photoelectron spectroscopy. The h-BN on Co template was used for in situ growth of multilayer graphene, leading to an h-BN/graphene heterostructure. Carbon atoms preferentially nucleate on Co substrate and edges of h-BN and then grow laterally to form continuous graphene. Further introduction of carbon atoms results in layer-by-layer growth of graphene on graphene and lateral growth of graphene on h-BNmore » until it may cover entire h-BN flakes.« less

Synthesis of freestanding single-crystal perovskite films and heterostructures by etching of sacrificial water-soluble layers

DOE PAGES

Lu, Di; Baek, David J.; Hong, Seung Sae; ...

2016-09-12

Here, the ability to create and manipulate materials in two-dimensional (2D) form has repeatedly had transformative impact on science and technology. In parallel with the exfoliation and stacking of intrinsically layered crystals 1, 2, 3, 4, 5, atomic-scale thin film growth of complex materials has enabled the creation of artificial 2D heterostructures with novel functionality 6, 7, 8, 9 and emergent phenomena, as seen in perovskite heterostructures 10, 11, 12. However, separation of these layers from the growth substrate has proved challenging, limiting the manipulation capabilities of these heterostructures with respect to exfoliated materials. Here we present a general methodmore » to create freestanding perovskite membranes. The key is the epitaxial growth of water-soluble Sr 3Al 2O 6 on perovskite substrates, followed by in situ growth of films and heterostructures. Millimetre-size single-crystalline membranes are produced by etching the Sr 3Al 2O 6 layer in water, providing the opportunity to transfer them to arbitrary substrates and integrate them with heterostructures of semiconductors and layered compounds 13, 14.« less

Postgrowth tuning of the bandgap of single-layer molybdenum disulfide films by sulfur/selenium exchange.

PubMed

Ma, Quan; Isarraraz, Miguel; Wang, Chen S; Preciado, Edwin; Klee, Velveth; Bobek, Sarah; Yamaguchi, Koichi; Li, Emily; Odenthal, Patrick Michael; Nguyen, Ariana; Barroso, David; Sun, Dezheng; von Son Palacio, Gretel; Gomez, Michael; Nguyen, Andrew; Le, Duy; Pawin, Greg; Mann, John; Heinz, Tony F; Rahman, Talat Shahnaz; Bartels, Ludwig

2014-05-27

We demonstrate bandgap tuning of a single-layer MoS2 film on SiO2/Si via substitution of its sulfur atoms by selenium through a process of gentle sputtering, exposure to a selenium precursor, and annealing. We characterize the substitution process both for S/S and S/Se replacement. Photoluminescence and, in the latter case, X-ray photoelectron spectroscopy provide direct evidence of optical band gap shift and selenium incorporation, respectively. We discuss our experimental observations, including the limit of the achievable bandgap shift, in terms of the role of stress in the film as elucidated by computational studies, based on density functional theory. The resultant films are stable in vacuum, but deteriorate under optical excitation in air.

Slater-Koster Tight-Binding parametrization of single and few-layer Black-Phosphorus from first-principles calculations

NASA Astrophysics Data System (ADS)

Menezes, Marcos; Capaz, Rodrigo

Black Phosphorus (BP) is a promising material for applications in electronics, especially due to the tuning of its band gap by increasing the number of layers. In single-layer BP, also called Phosphorene, the P atoms form two staggered chains bonded by sp3 hybridization, while neighboring layers are bonded by Van-der-Waals interactions. In this work, we present a Tight-Binding (TB) parametrization of the electronic structure of single and few-layer BP, based on the Slater-Koster model within the two-center approximation. Our model includes all 3s and 3p orbitals, which makes this problem more complex than that of graphene, where only 2pz orbitals are needed for most purposes. The TB parameters are obtained from a least-squares fit of DFT calculations carried on the SIESTA code. We compare the results for different basis-sets used to expand the ab-initio wavefunctions and discuss their applicability. Our model can fit a larger number of bands than previously reported calculations based on Wannier functions. Moreover, our parameters have a clear physical interpretation based on chemical bonding. As such, we expect our results to be useful in a further understanding of multilayer BP and other 2D-materials characterized by strong sp3 hybridization. CNPq, FAPERJ, INCT-Nanomateriais de Carbono.

Flame Synthesis Used to Create Metal-Catalyzed Carbon Nanotubes

NASA Technical Reports Server (NTRS)

VanderWal, Randy L.

2001-01-01

Metal-catalyzed carbon nanotubes are highly ordered carbon structures of nanoscale dimensions. They may be thought of as hollow cylinders whose walls are formed by single atomic layers of graphite. Such cylinders may be composed of many nested, concentric atomic layers of carbon or only a single layer, the latter forming a single-walled carbon nanotube. This article reports unique results using a flame for their synthesis. Only recently were carbon nanotubes discovered within an arc discharge and recognized as fullerene derivatives. Today metal-catalyzed carbon nanotubes are of great interest for many reasons. They can be used as supports for the metal catalysts like those found in catalytic converters. Open-ended nanotubes are highly desirable because they can be filled by other elements, metals or gases, for battery and fuel cell applications. Because of their highly crystalline structure, they are significantly stronger than the commercial carbon fibers that are currently available (10 times as strong as steel but possessing one-sixth of the weight). This property makes them highly desirable for strengthening polymer and ceramic composite materials. Current methods of synthesizing carbon nanotubes include thermal pyrolysis of organometallics, laser ablation of metal targets within hydrocarbon atmospheres at high temperatures, and arc discharges. Each of these methods is costly, and it is unclear if they can be scaled for the commercial synthesis of carbon nanotubes. In contrast, flame synthesis is an economical means of bulk synthesis of a variety of aerosol materials such as carbon black. Flame synthesis of carbon nanotubes could potentially realize an economy of scale that would enable their use in common structural materials such as car-body panels. The top figure is a transmission electron micrograph of a multiwalled carbon nanotube. The image shows a cross section of the atomic structure of the nanotube. The dark lines are individual atomic layer planes of carbon, seen here in cross section. They form a nested series of concentric cylinders, much like the growth rings on a tree. This sample was obtained by the supported catalyst method, whereby the nanoscale catalysts are dispersed on a substrate providing their support. The substrate with catalyst particles was immersed within an acetylene diffusion flame to which nitrogen had been added to eliminate soot formation. Upon removal from the flame, the nanotubes were dispersed on a holder suitable for electron microscopy. Although not seen in the figure, the tube diameter reflects that of the catalyst particle.

Nano-fabricated superconducting radio-frequency composites, method for producing nano-fabricated superconducting rf composites

DOEpatents

Norem, James H.; Pellin, Michael J.

2013-06-11

Superconducting rf is limited by a wide range of failure mechanisms inherent in the typical manufacture methods. This invention provides a method for fabricating superconducting rf structures comprising coating the structures with single atomic-layer thick films of alternating chemical composition. Also provided is a cavity defining the invented laminate structure.

Molecular beam epitaxy growth of SrO buffer layers on graphite and graphene for the integration of complex oxides

DOE PAGES

Ahmed, Adam S.; Wen, Hua; Ohta, Taisuke; ...

2016-04-27

Here, we report the successful growth of high-quality SrO films on highly-ordered pyrolytic graphite (HOPG) and single-layer graphene by molecular beam epitaxy. The SrO layers have (001) orientation as confirmed by X-ray diffraction (XRD) while atomic force microscopy measurements show continuous pinhole-free films having rms surface roughness of <1.5 Å. Moreover, transport measurements of exfoliated graphene, after SrO deposition, show a strong dependence between the Dirac point and Sr oxidation. As a result, the SrO is leveraged as a buffer layer for more complex oxide integration via the demonstration of (001) oriented SrTiO3 grown atop a SrO/HOPG stack.

Molecular beam epitaxy growth of SrO buffer layers on graphite and graphene for the integration of complex oxides

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

Ahmed, Adam S.; Wen, Hua; Ohta, Taisuke

Here, we report the successful growth of high-quality SrO films on highly-ordered pyrolytic graphite (HOPG) and single-layer graphene by molecular beam epitaxy. The SrO layers have (001) orientation as confirmed by X-ray diffraction (XRD) while atomic force microscopy measurements show continuous pinhole-free films having rms surface roughness of <1.5 Å. Moreover, transport measurements of exfoliated graphene, after SrO deposition, show a strong dependence between the Dirac point and Sr oxidation. As a result, the SrO is leveraged as a buffer layer for more complex oxide integration via the demonstration of (001) oriented SrTiO3 grown atop a SrO/HOPG stack.

The low coherence Fabry-Pérot interferometer with diamond and ZnO layers

NASA Astrophysics Data System (ADS)

Majchrowicz, D.; Den, W.; Hirsch, M.

2016-09-01

The authors present a fiber-optic Fabry-Pérot interferometer built with the application of diamond and zinc oxide (ZnO) thin layers. Thin ZnO films were deposited on the tip of a standard telecommunication single-mode optical fiber (SMF- 28) while the diamond layer was grown on the plate of silicon substrate. Investigated ZnO layers were fabricated by atomic layer deposition (ALD) and the diamond films were deposited using Microwave Plasma Enhanced Chemical Vapor Deposition (μPE CVD) system. Different thickness of layers was examined. The measurements were performed for the fiber-optic Fabry-Pérot interferometer working in the reflective mode. Spectra were registered for various thicknesses of ZnO layer and various length of the air cavity. As a light source, two superluminescent diodes (SLD) with central wavelength of 1300 nm and 1550 nm were used in measurement set-up.

Crested Tunnel Barriers for Fast, Scalable, Nonvolatile Semiconductor Memories (Theme 3)

DTIC Science & Technology

2006-12-01

single layer Si0 2 with similar EOT [19]. In Fig. 2, the solid symbols represent the typical I-V characteristics of an AI/(HfON-Si3N4)/Si structure. The...black curve (with open symbols ) is a simulated I-V curve for theoretical Si0 2 with the same EOT. It can be seen clearly that it takes only 3 volts for...R. Wasser , B. Reichenberg, and S. Tiedke, "Resistive switching mechanism of TiO 2 thin films grown by atomic-layer deposition", J. App/. Phys., vol

Automatic software correction of residual aberrations in reconstructed HRTEM exit waves of crystalline samples

DOE PAGES

Ophus, Colin; Rasool, Haider I.; Linck, Martin; ...

2016-11-30

We develop an automatic and objective method to measure and correct residual aberrations in atomic-resolution HRTEM complex exit waves for crystalline samples aligned along a low-index zone axis. Our method uses the approximate rotational point symmetry of a column of atoms or single atom to iteratively calculate a best-fit numerical phase plate for this symmetry condition, and does not require information about the sample thickness or precise structure. We apply our method to two experimental focal series reconstructions, imaging a β-Si 3N 4 wedge with O and N doping, and a single-layer graphene grain boundary. We use peak and latticemore » fitting to evaluate the precision of the corrected exit waves. We also apply our method to the exit wave of a Si wedge retrieved by off-axis electron holography. In all cases, the software correction of the residual aberration function improves the accuracy of the measured exit waves.« less

Automatic software correction of residual aberrations in reconstructed HRTEM exit waves of crystalline samples

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

Ophus, Colin; Rasool, Haider I.; Linck, Martin

We develop an automatic and objective method to measure and correct residual aberrations in atomic-resolution HRTEM complex exit waves for crystalline samples aligned along a low-index zone axis. Our method uses the approximate rotational point symmetry of a column of atoms or single atom to iteratively calculate a best-fit numerical phase plate for this symmetry condition, and does not require information about the sample thickness or precise structure. We apply our method to two experimental focal series reconstructions, imaging a β-Si 3N 4 wedge with O and N doping, and a single-layer graphene grain boundary. We use peak and latticemore » fitting to evaluate the precision of the corrected exit waves. We also apply our method to the exit wave of a Si wedge retrieved by off-axis electron holography. In all cases, the software correction of the residual aberration function improves the accuracy of the measured exit waves.« less

X-ray reflectometry and simulation of the parameters of SiC epitaxial films on Si(111), grown by the atomic substitution method

NASA Astrophysics Data System (ADS)

Kukushkin, S. A.; Nussupov, K. Kh.; Osipov, A. V.; Beisenkhanov, N. B.; Bakranova, D. I.

2017-05-01

The structure and composition of SiC nanolayers are comprehensively studied by X-ray reflectometry, IR-spectroscopy, and atomic-force microscopy (AFM) methods for the first time. SiC films were synthesized by the new method of topochemical substitution of substrate atoms at various temperatures and pressure of CO active gas on the surface of high-resistivity low-dislocation single-crystal n-type silicon (111). Based on an analysis and generalization of experimental data obtained using X-ray reflectometry, IR spectroscopy, and AFM methods, a structural model of SiC films on Si was proposed. According to this model, silicon carbide film consists of a number of layers parallel to the substrate, reminiscent of a layer cake. The composition and thickness of each layer entering the film structure is experimentally determined. It was found that all samples contain superstoichiometric carbon; however, its structure is significantly different for the samples synthesized at temperatures of 1250 and 1330°C, respectively. In the former case, the film surface is saturated with silicon vacancies and carbon in the structurally loose form reminiscent of HOPG carbon. In the films grown at 1330°C, carbon is in a dense structure with a close-to-diamond density.

Highly effective synthesis of NiO/CNT nanohybrids by atomic layer deposition for high-rate and long-life supercapacitors.

PubMed

Yu, Lei; Wang, Guilong; Wan, Gengping; Wang, Guizhen; Lin, Shiwei; Li, Xinyue; Wang, Kan; Bai, Zhiming; Xiang, Yang

2016-09-21

In this work, we report an atomic layer deposition (ALD) method for the fabrication of NiO/CNT hybrid structures in order to improve electronic conductivity, enhance cycling stability and increase rate capability of NiO used as supercapacitor electrodes. A uniform NiO coating can be well deposited on carbon nanotubes (CNTs) through simultaneously employing O3 and H2O as oxidizing agents in a single ALD cycle of NiO for the first time, with a high growth rate of nearly 0.3 Å per cycle. The electrochemical properties of the as-prepared NiO/CNT were then investigated. The results show that the electrochemical capacitive properties are strongly associated with the thickness of the NiO coating. The NiO/CNT composite materials with 200 cycles of NiO deposition exhibit the best electrochemical properties, involving high specific capacitance (622 F g(-1) at 2 A g(-1), 2013 F g(-1) for NiO), excellent rate capability (74% retained at 50 A g(-1)) and outstanding cycling stability. The impressive results presented here suggest a great potential for the fabrication of composite electrode materials by atomic layer deposition applied in high energy density storage systems.

Uniform large-area growth of nanotemplated high-quality monolayer MoS2

NASA Astrophysics Data System (ADS)

Young, Justin R.; Chilcote, Michael; Barone, Matthew; Xu, Jinsong; Katoch, Jyoti; Luo, Yunqiu Kelly; Mueller, Sara; Asel, Thaddeus J.; Fullerton-Shirey, Susan K.; Kawakami, Roland; Gupta, Jay A.; Brillson, Leonard J.; Johnston-Halperin, Ezekiel

2017-06-01

Over the past decade, it has become apparent that the extreme sensitivity of 2D crystals to surface interactions presents a unique opportunity to tune material properties through surface functionalization and the mechanical assembly of 2D heterostructures. However, this opportunity carries with it a concurrent challenge: an enhanced sensitivity to surface contamination introduced by standard patterning techniques that is exacerbated by the difficulty in cleaning these atomically thin materials. Here, we report a templated MoS2 growth technique wherein Mo is deposited onto atomically stepped sapphire substrates through a SiN stencil with feature sizes down to 100 nm and subsequently sulfurized at high temperature. These films have a quality comparable to the best MoS2 prepared by other methodologies, and the thickness of the resulting MoS2 patterns can be tuned layer-by-layer by controlling the initial Mo deposition. The quality and thickness of the films are confirmed by scanning electron, scanning tunneling, and atomic force microscopies; Raman, photoluminescence, and x-ray photoelectron spectroscopies; and electron transport measurements. This approach critically enables the creation of patterned, single-layer MoS2 films with pristine surfaces suitable for subsequent modification via functionalization and mechanical stacking. Further, we anticipate that this growth technique should be broadly applicable within the family of transition metal dichalcogenides.

Oxygen Displacement in Cuprates under Ionic Liquid Field-Effect Gating

PubMed Central

Dubuis, Guy; Yacoby, Yizhak; Zhou, Hua; He, Xi; Bollinger, Anthony T.; Pavuna, Davor; Pindak, Ron; Božović, Ivan

2016-01-01

We studied structural changes in a 5 unit cell thick La1.96Sr0.04CuO4 film, epitaxially grown on a LaSrAlO4 substrate with a single unit cell buffer layer, when ultra-high electric fields were induced in the film by applying a gate voltage between the film (ground) and an ionic liquid in contact with it. Measuring the diffraction intensity along the substrate-defined Bragg rods and analyzing the results using a phase retrieval method we obtained the three-dimensional electron density in the film, buffer layer, and topmost atomic layers of the substrate under different applied gate voltages. The main structural observations were: (i) there were no structural changes when the voltage was negative, holes were injected into the film making it more metallic and screening the electric field; (ii) when the voltage was positive, the film was depleted of holes becoming more insulating, the electric field extended throughout the film, the partial surface monolayer became disordered, and equatorial oxygen atoms were displaced towards the surface; (iii) the changes in surface disorder and the oxygen displacements were both reversed when a negative voltage was applied; and (iv) the c-axis lattice constant of the film did not change in spite of the displacement of equatorial oxygen atoms. PMID:27578237

Bi-layer channel structure-based oxide thin-film transistors consisting of ZnO and Al-doped ZnO with different Al compositions and stacking sequences

NASA Astrophysics Data System (ADS)

Cho, Sung Woon; Yun, Myeong Gu; Ahn, Cheol Hyoun; Kim, So Hee; Cho, Hyung Koun

2015-03-01

Zinc oxide (ZnO)-based bi-layers, consisting of ZnO and Al-doped ZnO (AZO) layers grown by atomic layer deposition, were utilized as the channels of oxide thin-film transistors (TFTs). Thin AZO layers (5 nm) with different Al compositions (5 and 14 at. %) were deposited on top of and beneath the ZnO layers in a bi-layer channel structure. All of the bi-layer channel TFTs that included the AZO layers showed enhanced stability (Δ V Th ≤ 3.2 V) under a positive bias stress compared to the ZnO single-layer channel TFT (Δ V Th = 4.0 V). However, the AZO/ZnO bi-layer channel TFTs with an AZO interlayer between the gate dielectric and the ZnO showed a degraded field effect mobility (0.3 cm2/V·s for 5 at. % and 1.8 cm2/V·s for 14 at. %) compared to the ZnO single-layer channel TFT (5.5 cm2/V·s) due to increased scattering caused by Al-related impurities near the gate dielectric/channel interface. In contrast, the ZnO/AZO bi-layer channel TFTs with an AZO layer on top of the ZnO layer exhibited an improved field effect mobility (7.8 cm2/V·s for 14 at. %) and better stability. [Figure not available: see fulltext.

Direct observation of nanowire growth and decomposition.

PubMed

Rackauskas, Simas; Shandakov, Sergey D; Jiang, Hua; Wagner, Jakob B; Nasibulin, Albert G

2017-09-26

Fundamental concepts of the crystal formation suggest that the growth and decomposition are determined by simultaneous embedding and removal of the atoms. Apparently, by changing the crystal formation conditions one can switch the regimes from the growth to decomposition. To the best of our knowledge, so far this has been only postulated, but never observed at the atomic level. By means of in situ environmental transmission electron microscopy we monitored and examined the atomic layer transformation at the conditions of the crystal growth and its decomposition using CuO nanowires selected as a model object. The atomic layer growth/decomposition was studied by varying an O 2 partial pressure. Three distinct regimes of the atomic layer evolution were experimentally observed: growth, transition and decomposition. The transition regime, at which atomic layer growth/decomposition switch takes place, is characterised by random nucleation of the atomic layers on the growing {111} surface. The decomposition starts on the side of the nanowire by removing the atomic layers without altering the overall crystal structure, which besides the fundamental importance offers new possibilities for the nanowire manipulation. Understanding of the crystal growth kinetics and nucleation at the atomic level is essential for the precise control of 1D crystal formation.

Silicon carbide transparent chips for compact atomic sensors

NASA Astrophysics Data System (ADS)

Huet, L.; Ammar, M.; Morvan, E.; Sarazin, N.; Pocholle, J.-P.; Reichel, J.; Guerlin, C.; Schwartz, S.

2017-11-01

Atom chips [1] are an efficient tool for trapping, cooling and manipulating cold atoms, which could open the way to a new generation of compact atomic sensors addressing space applications. This is in particular due to the fact that they can achieve strong magnetic field gradients near the chip surface, hence strong atomic confinement at moderate electrical power. However, this advantage usually comes at the price of reducing the optical access to the atoms, which are confined very close to the chip surface. We will report at the conference experimental investigations showing how these limits could be pushed farther by using an atom chip made of a gold microcircuit deposited on a single-crystal Silicon Carbide (SiC) substrate [2]. With a band gap energy value of about 3.2 eV at room temperature, the latter material is transparent at 780nm, potentially restoring quasi full optical access to the atoms. Moreover, it combines a very high electrical resistivity with a very high thermal conductivity, making it a good candidate for supporting wires with large currents without the need of any additional electrical insulation layer [3].

From carbon nanotubes to carbon atomic chains

NASA Astrophysics Data System (ADS)

Casillas García, Gilberto; Zhang, Weijia; José-Yacamán, Miguel

2010-10-01

Carbyne is a linear allotrope of carbon. It is formed by a linear arrangement of carbon atoms with sp-hybridization. We present a reliable and reproducible experiment to obtain these carbon atomic chains using few-layer-graphene (FLG) sheets and a HRTEM. First the FLG sheets were synthesized from worm-like exfoliated graphite and then drop-casted on a lacey-carbon copper grid. Once in the TEM, two holes are opened near each other in a FLG sheet by focusing the electron beam into a small spot. Due to the radiation, the carbon atoms rearrange themselves between the two holes and form carbon fibers. The beam is concentrated on the carbon fibers in order excite the atoms and induce a tension until multi wall carbon nanotube (MWCNT) is formed. As the radiation continues the MWCNT breaks down until there is only a single wall carbon nanotube (SWCNT). Then, when the SWCNT breaks, an atomic carbon chain is formed, lasts for several seconds under the radiation and finally breaks. This demonstrates the stability of this carbon structure.

Effect of Elastic Strain Fluctuation on Atomic Layer Growth of Epitaxial Silicide in Si Nanowires by Point Contact Reactions.

PubMed

Chou, Yi-Chia; Tang, Wei; Chiou, Chien-Jyun; Chen, Kai; Minor, Andrew M; Tu, K N

2015-06-10

Effects of strain impact a range of applications involving mobility change in field-effect-transistors. We report the effect of strain fluctuation on epitaxial growth of NiSi2 in a Si nanowire via point contact and atomic layer reactions, and we discuss the thermodynamic, kinetic, and mechanical implications. The generation and relaxation of strain shown by in situ TEM is periodic and in synchronization with the atomic layer reaction. The Si lattice at the epitaxial interface is under tensile strain, which enables a high solubility of supersaturated interstitial Ni atoms for homogeneous nucleation of an epitaxial atomic layer of the disilicide phase. The tensile strain is reduced locally during the incubation period of nucleation by the dissolution of supersaturated Ni atoms in the Si lattice but the strained-Si state returns once the atomic layer epitaxial growth of NiSi2 occurs by consuming the supersaturated Ni.

Atomic-Layer-Deposited Transparent Electrodes for Silicon Heterojunction Solar Cells

DOE PAGES

Demaurex, Benedicte; Seif, Johannes P.; Smit, Sjoerd; ...

2014-11-01

We examine damage-free transparent-electrode deposition to fabricate high-efficiency amorphous silicon/crystalline silicon heterojunction solar cells. Such solar cells usually feature sputtered transparent electrodes, the deposition of which may damage the layers underneath. Using atomic layer deposition, we insert thin protective films between the amorphous silicon layers and sputtered contacts and investigate their effect on device operation. We find that a 20-nm-thick protective layer suffices to preserve, unchanged, the amorphous silicon layers beneath. Insertion of such protective atomic-layer-deposited layers yields slightly higher internal voltages at low carrier injection levels. However, we identify the presence of a silicon oxide layer, formed during processing,more » between the amorphous silicon and the atomic-layer-deposited transparent electrode that acts as a barrier, impeding hole and electron collection.« less

Structure and growth of Bi(110) islands on Si(111)√{3 }×√{3 }-B substrates

NASA Astrophysics Data System (ADS)

Nagase, Kentaro; Kokubo, Ikuya; Yamazaki, Shiro; Nakatsuji, Kan; Hirayama, Hiroyuki

2018-05-01

The structure and growth of ultrathin Bi(110) islands were investigated on a Si(111)√{3 }×√{3 }-B substrate by scanning tunneling microscopy and scanning tunneling spectroscopy (STS). Both even- and odd-layer-height islands nucleated on a one-monolayer-thick wetting layer. The islands preferred the even layer heights over the odd layer heights with an area ratio of 3:1. A weak, long-range corrugation was observed to overlap on the atomic arrangement at the top of the islands. The average distance between the peaks of the corrugation oscillated in accordance with the alternation of even and odd layer heights. Nucleation of single- and double-layer terraces occurred on the islands with even layer heights but not on those with odd layer heights. The unit cell of the single-layer terrace was aligned with that of the underlying even-layer-height island. The inequality in the height preference and the height-dependent oscillation of the corrugation suggested that the even- and odd-layer-height islands possessed different structures. The dominance and stability against terrace nucleation of the even-layer-height islands were consistent with the theoretically predicted stability of the paired layer-stacked black-phosphorus (BP)-like structure for ultrathin Bi(110) films. The alignment of the unit cell at the terrace on the island and STS spectra suggested a BP-like/bulklike/BP-like sandwich structure for the odd-layer-height Bi(110) islands.

Structural disorder and elementary magnetic properties of triangular lattice ErMgGaO 4 single crystals

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

Cevallos, F. Alex; Stolze, Karoline; Cava, Robert J.

The single crystal growth, structure, and basic magnetic properties of ErMgGaO 4 are reported. The structure consists of triangular layers of magnetic ErO 6 octahedra separated by a double layer of randomly occupied non-magnetic (Ga,Mg)O 5 bipyramids. The Er atoms are positionally disordered. Magnetic measurements parallel and perpendicular to the c axis of a single crystal reveal dominantly antiferromagnetic interactions, with a small degree of magnetic anisotropy. A weighted average of the directional data suggests an antiferromagnetic Curie Weiss temperature of approximately -30 K. Below 10 K the temperature dependences of the inverse susceptibilities in the in-plane and perpendicular-to planemore » directions are parallel, indicative of an isotropic magnetic moment at low temperatures. In conclusion, no sign of magnetic ordering is observed above 1.8 K, suggesting that ErMgGaO 4 is a geometrically frustrated magnet.« less

Deterministic strain-induced arrays of quantum emitters in a two-dimensional semiconductor

PubMed Central

Branny, Artur; Kumar, Santosh; Proux, Raphaël; Gerardot, Brian D

2017-01-01

An outstanding challenge in quantum photonics is scalability, which requires positioning of single quantum emitters in a deterministic fashion. Site positioning progress has been made in established platforms including defects in diamond and self-assembled quantum dots, albeit often with compromised coherence and optical quality. The emergence of single quantum emitters in layered transition metal dichalcogenide semiconductors offers new opportunities to construct a scalable quantum architecture. Here, using nanoscale strain engineering, we deterministically achieve a two-dimensional lattice of quantum emitters in an atomically thin semiconductor. We create point-like strain perturbations in mono- and bi-layer WSe2 which locally modify the band-gap, leading to efficient funnelling of excitons towards isolated strain-tuned quantum emitters that exhibit high-purity single photon emission. We achieve near unity emitter creation probability and a mean positioning accuracy of 120±32 nm, which may be improved with further optimization of the nanopillar dimensions. PMID:28530219

Structural disorder and elementary magnetic properties of triangular lattice ErMgGaO 4 single crystals

DOE PAGES

Cevallos, F. Alex; Stolze, Karoline; Cava, Robert J.

2018-03-23

The single crystal growth, structure, and basic magnetic properties of ErMgGaO 4 are reported. The structure consists of triangular layers of magnetic ErO 6 octahedra separated by a double layer of randomly occupied non-magnetic (Ga,Mg)O 5 bipyramids. The Er atoms are positionally disordered. Magnetic measurements parallel and perpendicular to the c axis of a single crystal reveal dominantly antiferromagnetic interactions, with a small degree of magnetic anisotropy. A weighted average of the directional data suggests an antiferromagnetic Curie Weiss temperature of approximately -30 K. Below 10 K the temperature dependences of the inverse susceptibilities in the in-plane and perpendicular-to planemore » directions are parallel, indicative of an isotropic magnetic moment at low temperatures. In conclusion, no sign of magnetic ordering is observed above 1.8 K, suggesting that ErMgGaO 4 is a geometrically frustrated magnet.« less

Growing Cutting-edge X-ray Optics

ScienceCinema

Conley, Ray

2018-03-02

Ever imagined that an Xbox controller could help open a window into a world spanning just one billionth of a meter? Brookhaven Lab's Ray Conley grows cutting-edge optics called multilayer Laue lenses (MLL) one atomic layer at a time to focus high-energy x-rays to within a single nanometer. To achieve this focusing feat, Ray uses a massive, custom-built atomic deposition device, an array of computers, and a trusty Xbox controller. These lenses will be deployed at the Lab's National Synchrotron Light Source II, due to begin shining super-bright light on pressing scientific puzzles in 2015.

Strong polarization enhancement in asymmetric three-component ferroelectric superlattices

NASA Astrophysics Data System (ADS)

Lee, Ho Nyung; Christen, Hans M.; Chisholm, Matthew F.; Rouleau, Christopher M.; Lowndes, Douglas H.

2005-01-01

Theoretical predictions-motivated by recent advances in epitaxial engineering-indicate a wealth of complex behaviour arising in superlattices of perovskite-type metal oxides. These include the enhancement of polarization by strain and the possibility of asymmetric properties in three-component superlattices. Here we fabricate superlattices consisting of barium titanate (BaTiO3), strontium titanate (SrTiO3) and calcium titanate (CaTiO3) with atomic-scale control by high-pressure pulsed laser deposition on conducting, atomically flat strontium ruthenate (SrRuO3) layers. The strain in BaTiO3 layers is fully maintained as long as the BaTiO3 thickness does not exceed the combined thicknesses of the CaTiO3 and SrTiO3 layers. By preserving full strain and combining heterointerfacial couplings, we find an overall 50% enhancement of the superlattice global polarization with respect to similarly grown pure BaTiO3, despite the fact that half the layers in the superlattice are nominally non-ferroelectric. We further show that even superlattices containing only single-unit-cell layers of BaTiO3 in a paraelectric matrix remain ferroelectric. Our data reveal that the specific interface structure and local asymmetries play an unexpected role in the polarization enhancement.

Mitigating leaks in membranes

DOEpatents

Karnik, Rohit N.; Bose, Suman; Boutilier, Michael S.H.; Hadjiconstantinou, Nicolas G.; Jain, Tarun Kumar; O'Hern, Sean C.; Laoui, Tahar; Atieh, Muataz A.; Jang, Doojoon

2018-02-27

Two-dimensional material based filters, their method of manufacture, and their use are disclosed. In one embodiment, a membrane may include an active layer including a plurality of defects and a deposited material associated with the plurality of defects may reduce flow therethrough. Additionally, a majority of the active layer may be free from the material. In another embodiment, a membrane may include a porous substrate and an atomic layer deposited material disposed on a surface of the porous substrate. The atomic layer deposited material may be less hydrophilic than the porous substrate and an atomically thin active layer may be disposed on the atomic layer deposited material.

Localized surface plasmon resonance nanosensor: a high-resolution distance-dependence study using atomic layer deposition.

PubMed

Whitney, Alyson V; Elam, Jeffrey W; Zou, Shengli; Zinovev, Alex V; Stair, Peter C; Schatz, George C; Van Duyne, Richard P

2005-11-03

Atomic layer deposition (ALD) is used to deposit 1-600 monolayers of Al(2)O(3) on Ag nanotriangles fabricated by nanosphere lithography (NSL). Each monolayer of Al(2)O(3) has a thickness of 1.1 A. It is demonstrated that the localized surface plasmon resonance (LSPR) nanosensor can detect Al(2)O(3) film growth with atomic spatial resolution normal to the nanoparticle surface. This is approximately 10 times greater spatial resolution than that in our previous long-range distance-dependence study using multilayer self-assembled monolayer shells. The use of ALD enables the study of both the long- and short-range distance dependence of the LSPR nanosensor in a single unified experiment. Ag nanoparticles with fixed in-plane widths and decreasing heights yield larger sensing distances. X-ray photoelectron spectroscopy, variable angle spectroscopic ellipsometry, and quartz crystal microbalance measurements are used to study the growth mechanism. It is proposed that the growth of Al(2)O(3) is initiated by the decomposition of trimethylaluminum on Ag. Semiquantitative theoretical calculations were compared with the experimental results and yield excellent agreement.

Molecular dynamic simulation study of plasma etching L10 FePt media in embedded mask patterning (EMP) process

NASA Astrophysics Data System (ADS)

Zhu, Jianxin; Quarterman, P.; Wang, Jian-Ping

2017-05-01

Plasma etching process of single-crystal L10-FePt media [H. Wang et al., Appl. Phys. Lett. 102(5) (2013)] is studied using molecular dynamic simulation. Embedded-Atom Method [M. S. Daw and M. I. Baskes, Phy. Rev. B 29, 6443 (1984); X. W. Zhou, R. A. Johnson and H. N. G. Wadley, Phy. Rev. B 69, 144113 (2004)] is used to calculate the interatomic potential within atoms in FePt alloy, and ZBL potential [J.F. Ziegler, J. P. Biersack and U. Littmark, "The Stopping and Range of Ions in Matter," Volume 1, Pergamon,1985] in comparison with conventional Lennard-Jones "12-6" potential is applied to interactions between etching gas ions and metal atoms. It is shown the post-etch structure defects can include amorphized surface layer and lattice interstitial point defects that caused by etchant ions passed through the surface layer. We show that the amorphized or damaged FePt lattice surface layer (or "magnetic dead-layer") thickness after etching increases with ion energy for Ar ion impacts, but significantly small for He ions at up to 250eV ion energy. However, we showed that He sputtering creates more interstitial defects at lower energy levels and defects are deeper below the surface compared to Ar sputtering. We also calculate the interstitial defect level and depth as dependence on ion energy for both Ar and He ions. Media magnetic property loss due to these defects is also discussed.

Thermally induced alkylation of diamond.

PubMed

Hoeb, Marco; Auernhammer, Marianne; Schoell, Sebastian J; Brandt, Martin S; Garrido, Jose A; Stutzmann, Martin; Sharp, Ian D

2010-12-21

We present an approach for the thermally activated formation of alkene-derived self-assembled monolayers on oxygen-terminated single and polycrystalline diamond surfaces. Chemical modification of the oxygen and hydrogen plasma-treated samples was achieved by heating in 1-octadecene. The resulting layers were characterized using X-ray photoelectron spectroscopy, thermal desorption spectroscopy, atomic force microscopy, Fourier transform infrared spectroscopy, and water contact angle measurements. This investigation reveals that alkenes selectively attach to the oxygen-terminated sites via covalent C-O-C bonds. The hydrophilic oxygen-terminated diamond is rendered strongly hydrophobic following this reaction. The nature of the process limits the organic layer growth to a single monolayer, and FTIR measurements reveal that such monolayers are dense and well ordered. In contrast, hydrogen-terminated diamond sites remain unaffected by this process. This method is thus complementary to the UV-initiated reaction of alkenes with diamond, which exhibits the opposite reactivity contrast. Thermal alkylation increases the range of available diamond functionalization strategies and provides a means of straightforwardly forming single organic layers in order to engineer the surface properties of diamond.

Fabrication of Subnanometer-Precision Nanopores in Hexagonal Boron Nitride

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

Gilbert, S. Matt; Dunn, Gabriel; Azizi, Amin

Here, we demonstrate the fabrication of individual nanopores in hexagonal boron nitride (h-BN) with atomically precise control of the pore shape and size. Previous methods of pore production in other 2D materials typically create pores with irregular geometry and imprecise diameters. In contrast, other studies have shown that with careful control of electron irradiation, defects in h-BN grow with pristine zig-zag edges at quantized triangular sizes, but they have failed to demonstrate production and control of isolated defects. In this work, we combine these techniques to yield a method in which we can create individual size-quantized triangular nanopores through anmore » h-BN sheet. The pores are created using the electron beam of a conventional transmission electron microscope; which can strip away multiple layers of h-BN exposing single-layer regions, introduce single vacancies, and preferentially grow vacancies only in the single-layer region. We further demonstrate how the geometry of these pores can be altered beyond triangular by changing beam conditions. Precisely size- and geometry-tuned nanopores could find application in molecular sensing, DNA sequencing, water desalination, and molecular separation.« less

Fabrication of Subnanometer-Precision Nanopores in Hexagonal Boron Nitride

DOE PAGES

Gilbert, S. Matt; Dunn, Gabriel; Azizi, Amin; ...

2017-11-08

Here, we demonstrate the fabrication of individual nanopores in hexagonal boron nitride (h-BN) with atomically precise control of the pore shape and size. Previous methods of pore production in other 2D materials typically create pores with irregular geometry and imprecise diameters. In contrast, other studies have shown that with careful control of electron irradiation, defects in h-BN grow with pristine zig-zag edges at quantized triangular sizes, but they have failed to demonstrate production and control of isolated defects. In this work, we combine these techniques to yield a method in which we can create individual size-quantized triangular nanopores through anmore » h-BN sheet. The pores are created using the electron beam of a conventional transmission electron microscope; which can strip away multiple layers of h-BN exposing single-layer regions, introduce single vacancies, and preferentially grow vacancies only in the single-layer region. We further demonstrate how the geometry of these pores can be altered beyond triangular by changing beam conditions. Precisely size- and geometry-tuned nanopores could find application in molecular sensing, DNA sequencing, water desalination, and molecular separation.« less

Chemical shielding properties for BN, BP, AlN, and AlP nanocones: DFT studies

NASA Astrophysics Data System (ADS)

Mirzaei, Mahmoud; Yousefi, Mohammad; Meskinfam, Masoumeh

2012-06-01

The properties of boron nitride (BN), boron phosphide (BP), aluminum nitride (AlN), and aluminum phosphide (AlP) nanocones were investigated by density functional theory (DFT) calculations. The investigated structures were optimized and chemical shielding (CS) properties including isotropic and anisotropic CS parameters were calculated for the atoms of the optimized structures. The magnitudes of CS parameters were observed to be mainly dependent on the bond lengths of considered atoms. The results indicated that the atoms could be divided into atomic layers due to the similarities of their CS properties for the atoms of each layer. The trend means that the atoms of each layer detect almost similar electronic environments. Moreover, the atoms at the apex and mouth of nanocones exhibit different properties with respect to the other atomic layers.

Photocatalytic C60-amorphous TiO2 composites prepared by atomic layer deposition

NASA Astrophysics Data System (ADS)

Justh, Nóra; Firkala, Tamás; László, Krisztina; Lábár, János; Szilágyi, Imre Miklós

2017-10-01

Nanocomposites of TiO2 and single fullerene (C60) molecule are prepared by atomic layer deposition (ALD). To create nucleation sites for the ALD reaction, the bare fullerene is functionalized by H2SO4/HNO3 treatment, which results in C60-SO3H. After a NaOH washing step the intermediate hydrolyzes into C60sbnd OH. This process and the consecutive ALD growth of TiO2 are monitored with FTIR, TG/DTA-MS, EDX, Raman, FTIR, XRD, and TEM measurements. Although the TiO2 grown by ALD at 80 and 160 °C onto fullerol is amorphous it enhances the decomposition of methyl orange under UV exposure. This study proves that amorphous TiO2 grown by low temperature ALD has photocatalytic activity, and it can be used e.g. as self-cleaning coatings also on heat sensitive substrates.

A buetschliite-type rare-earth borate, KBaY(BO 3) 2

NASA Astrophysics Data System (ADS)

Gao, Jianhua; Song, Limei; Hu, Xiaoyun; Zhang, Dekai

2011-01-01

The title compound was firstly synthesized by solid state reaction and its single crystals were successfully obtained using a selected flux. It is isotypic with the mineral buetschliite, K 2Ca(CO 3) 2, and crystallizes in the trigonal space group R-3m with a = 5.4526(12) Å, c = 17.781(8) Å, Z = 3. In the structure, Ba and K atoms are disordered on a same site in the proportion of 0.492(4):0.508(4). The fundamental building units are YO 6 octahedra and BO 3 triangles. The structure consists of [YB 2O 6] ∞ double layers constructed by corner-sharing YO 6 and BO 3 groups. Ba/K atoms occupy the spaces between these two layers and play the role of bridges. In addition, the luminescence properties of Eu 3+ doped KBaY(BO 3) 2 were also studied.

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

Femtosecond laser patterning, synthesis, defect formation, and structural modification of atomic layered materials

DOE PAGES

Yoo, Jae-Hyuck; Kim, Eunpa; Hwang, David J.

2016-12-06

This article summarizes recent research on laser-based processing of twodimensional (2D) atomic layered materials, including graphene and transition metal dichalcogenides (TMDCs). Ultrafast lasers offer unique processing routes that take advantage of distinct interaction mechanisms with 2D materials to enable extremely localized energy deposition. Experiments have shown that ablative direct patterning of graphene by ultrafast lasers can achieve resolutions of tens of nanometers, as well as single-step pattern transfer. Ultrafast lasers also induce non-thermal excitation mechanisms that are useful for the thinning of TMDCs to tune the 2D material bandgap. Laser-assisted site-specific doping was recently demonstrated where ultrafast laser radiation undermore » ambient air environment could be used for the direct writing of high-quality graphene patterns on insulating substrates. This article concludes with an outlook towards developing further advanced laser processing with scalability, in situ monitoring strategies and potential applications.« less

Atomic layer deposition modified track-etched conical nanochannels for protein sensing.

PubMed

Wang, Ceming; Fu, Qibin; Wang, Xinwei; Kong, Delin; Sheng, Qian; Wang, Yugang; Chen, Qiang; Xue, Jianming

2015-08-18

Nanopore-based devices have recently become popular tools to detect biomolecules at the single-molecule level. Unlike the long-chain nucleic acids, protein molecules are still quite challenging to detect, since the protein molecules are much smaller in size and usually travel too fast through the nanopore with poor signal-to-noise ratio of the induced transport signals. In this work, we demonstrate a new type of nanopore device based on atomic layer deposition (ALD) Al2O3 modified track-etched conical nanochannels for protein sensing. These devices show very promising properties of high protein (bovine serum albumin) capture rate with well time-resolved transport signals and excellent signal-to-noise ratio for the transport events. Also, a special mechanism involving transient process of ion redistribution inside the nanochannel is proposed to explain the unusual biphasic waveshapes of the current change induced by the protein transport.

Science and Emerging Technology of 2D Atomic Layered Materials and Devices

DTIC Science & Technology

2017-09-09

AFRL-AFOSR-JP-TR-2017-0067 Science & Emerging Technology of 2D Atomic Layered Materials and Devices Angel Rubio UNIVERSIDAD DEL PAIS VASCO - EUSKAL...Emerging Technology of 2D Atomic Layered Materials and Devices 5a.  CONTRACT NUMBER 5b.  GRANT NUMBER FA2386-15-1-0006 5c.  PROGRAM ELEMENT NUMBER...reporting documents for AOARD project 144088, “2D Materials and Devices Beyond Graphene Science & Emerging Technology of 2D Atomic Layered Materials and

Partially Oxidized SnS2 Atomic Layers Achieving Efficient Visible-Light-Driven CO2 Reduction.

PubMed

Jiao, Xingchen; Li, Xiaodong; Jin, Xiuyu; Sun, Yongfu; Xu, Jiaqi; Liang, Liang; Ju, Huanxin; Zhu, Junfa; Pan, Yang; Yan, Wensheng; Lin, Yue; Xie, Yi

2017-12-13

Unraveling the role of surface oxide on affecting its native metal disulfide's CO 2 photoreduction remains a grand challenge. Herein, we initially construct metal disulfide atomic layers and hence deliberately create oxidized domains on their surfaces. As an example, SnS 2 atomic layers with different oxidation degrees are successfully synthesized. In situ Fourier transform infrared spectroscopy spectra disclose the COOH* radical is the main intermediate, whereas density-functional-theory calculations reveal the COOH* formation is the rate-limiting step. The locally oxidized domains could serve as the highly catalytically active sites, which not only benefit for charge-carrier separation kinetics, verified by surface photovoltage spectra, but also result in electron localization on Sn atoms near the O atoms, thus lowering the activation energy barrier through stabilizing the COOH* intermediates. As a result, the mildly oxidized SnS 2 atomic layers exhibit the carbon monoxide formation rate of 12.28 μmol g -1 h -1 , roughly 2.3 and 2.6 times higher than those of the poorly oxidized SnS 2 atomic layers and the SnS 2 atomic layers under visible-light illumination. This work uncovers atomic-level insights into the correlation between oxidized sulfides and CO 2 reduction property, paving a new way for obtaining high-efficiency CO 2 photoreduction performances.

Probabilistic distributions of pinhole defects in atomic layer deposited films on polymeric substrates

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

Yersak, Alexander S., E-mail: alexander.yersak@colorado.edu; Lee, Yung-Cheng

Pinhole defects in atomic layer deposition (ALD) coatings were measured in an area of 30 cm{sup 2} in an ALD reactor, and these defects were represented by a probabilistic cluster model instead of a single defect density value with number of defects over area. With the probabilistic cluster model, the pinhole defects were simulated over a manufacturing scale surface area of ∼1 m{sup 2}. Large-area pinhole defect simulations were used to develop an improved and enhanced design method for ALD-based devices. A flexible thermal ground plane (FTGP) device requiring ALD hermetic coatings was used as an example. Using a single defectmore » density value, it was determined that for an application with operation temperatures higher than 60 °C, the FTGP device would not be possible. The new probabilistic cluster model shows that up to 40.3% of the FTGP would be acceptable. With this new approach the manufacturing yield of ALD-enabled or other thin film based devices with different design configurations can be determined. It is important to guide process optimization and control and design for manufacturability.« less

Data Mining for New Two- and One-Dimensional Weakly Bonded Solids and Lattice-Commensurate Heterostructures.

PubMed

Cheon, Gowoon; Duerloo, Karel-Alexander N; Sendek, Austin D; Porter, Chase; Chen, Yuan; Reed, Evan J

2017-03-08

Layered materials held together by weak interactions including van der Waals forces, such as graphite, have attracted interest for both technological applications and fundamental physics in their layered form and as an isolated single-layer. Only a few dozen single-layer van der Waals solids have been subject to considerable research focus, although there are likely to be many more that could have superior properties. To identify a broad spectrum of layered materials, we present a novel data mining algorithm that determines the dimensionality of weakly bonded subcomponents based on the atomic positions of bulk, three-dimensional crystal structures. By applying this algorithm to the Materials Project database of over 50,000 inorganic crystals, we identify 1173 two-dimensional layered materials and 487 materials that consist of weakly bonded one-dimensional molecular chains. This is an order of magnitude increase in the number of identified materials with most materials not known as two- or one-dimensional materials. Moreover, we discover 98 weakly bonded heterostructures of two-dimensional and one-dimensional subcomponents that are found within bulk materials, opening new possibilities for much-studied assembly of van der Waals heterostructures. Chemical families of materials, band gaps, and point groups for the materials identified in this work are presented. Point group and piezoelectricity in layered materials are also evaluated in single-layer forms. Three hundred and twenty-five of these materials are expected to have piezoelectric monolayers with a variety of forms of the piezoelectric tensor. This work significantly extends the scope of potential low-dimensional weakly bonded solids to be investigated.

Theoretical study for heterojunction surface of NEA GaN photocathode dispensed with Cs activation

NASA Astrophysics Data System (ADS)

Xia, Sihao; Liu, Lei; Wang, Honggang; Wang, Meishan; Kong, Yike

2016-09-01

For the disadvantages of conventional negative electron affinity (NEA) GaN photocathodes activated by Cs or Cs/O, new-type NEA GaN photocathodes with heterojunction surface dispensed with Cs activation are investigated based on first-principle study with density functional theory. Through the growth of an ultrathin n-type GaN cap layer on p-type GaN emission layer, a p-n heterojunction is formed on the surface. According to the calculation results, it is found that Si atoms tend to replace Ga atoms to result in an n-type doped cap layer which contributes to the decreasing of work function. After the growth of n-type GaN cap layer, the atom structure near the p-type emission layer is changed while that away from the surface has no obvious variations. By analyzing the E-Mulliken charge distribution of emission surface with and without cap layer, it is found that the positive charge of Ga and Mg atoms in the emission layer decrease caused by the cap layer, while the negative charge of N atom increases. The conduction band moves downwards after the growth of cap layer. Si atom produces donor levels around the valence band maximum. The absorption coefficient of GaN emission layer decreases and the reflectivity increases caused by n-type GaN cap layer.

Compositional modulated atomic layer stacking and uniaxial magnetocrystalline anisotropy of CoPt alloy sputtered films with close-packed plane orientation

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

Saito, Shin, E-mail: ssaito@ecei.tohoku.ac.jp; Nozawa, Naoki; Hinata, Shintaro

An atomic layer stacking structure in hexagonal close packed (hcp) Co{sub 100−x}Pt{sub x} alloy films with c-plane sheet texture was directly observed by a high-angle annular dark-field imaging scanning transmission electron microscopy. The analysis of sequential and/or compositional atomic layer stacking structure and uniaxial magnetocrystalline anisotropy (K{sub u} = K{sub u1} + K{sub u2}) revealed that (1) integrated intensity of the superlattice diffraction takes the maximum at x = 20 at. % and shows broadening feature against x for the film fabricated under the substrate temperature (T{sub sub}) of 400 °C. (2) Compositional separation structure in atomic layers is formed for the films fabricated under T{sub sub} = 400 °C.more » A sequential alternative stacking of atomic layers with different compositions is hardly formed in the film with x = 50 at. %, whereas easily formed in the film with x = 20 at. %. This peculiar atomic layer stacking structure consists of in-plane-disordered Pt-rich and Pt-poor layers, which is completely different from the so-called atomic site ordered structure. (3) A face centered cubic atomic layer stacking as faults appeared in the host hcp atomic layer stacking exists in accompanies with irregularities for the periodicity of the compositional modulation atomic layers. (4) K{sub u1} takes the maximum of 1.4 × 10{sup 7 }erg/cm{sup 3} at around x = 20 at. %, whereas K{sub u2} takes the maximum of 0.7 × 10{sup 7 }erg/cm{sup 3} at around x = 40 at. %, which results in the maximum of 1.8 × 10{sup 7 }erg/cm{sup 3} of K{sub u} at x = 30 at. % and a shoulder in compositional dependence of K{sub u} in the range of x = 30–60 at. %. Not only compositional separation of atomic layers but also sequential alternative stacking of different compositional layers is quite important to improve essential uniaxial magnetocrystalline anisotropy.« less

Surface reconstruction switching induced by tensile stress of DB steps: From Ba/Si(0 0 1)- 2 × 3 to Ba/Si(0 0 1)-4° off- 3 × 2

NASA Astrophysics Data System (ADS)

Kim, Hidong; Lkhagvasuren, Altaibaatar; Zhang, Rui; Seo, Jae M.

2018-05-01

The alkaline-earth metal adsorption on Si(0 0 1) has attracted much interest for finding a proper template in the growth of high- κ and crystalline films. Up to now on the flat Si(0 0 1) surface with double domains and single-layer steps, the adsorbed Ba atoms are known to induce the 2 × 3 structure through removing two Si dimers and adding a Ba atom per unit cell in each domain. In the present investigation, the Si(0 0 1)-4° off surface with DB steps and single domains has been employed as a substrate and the reconstruction at the initial stage of Ba adsorption has been investigated by scanning tunneling microscopy and synchrotron photoemission spectroscopy. On this vicinal and single domain terrace, a novel 3 × 2 structure rotated by 90° from the 2 × 3 structure has been found. Such a 3 × 2 structure turns out to be formed by adding a Ba atom and a Si dimer per unit cell. This results from the fact that the adsorbed Ba2+ ions with a larger ionic radius relieve tensile stress on the original Si dimers exerted by the rebonded atoms at the DB step.

Electronic Bandgap and Edge Reconstruction in Phosphorene Materials

DOE PAGES

Liang, Liangbo; Wang, Jun; Lin, Wenzhi; ...

2014-11-12

Single-layer black phosphorous (BP), or phosphorene, is a highly-anisotropic two-dimensional elemental material possessing promising semiconductor properties for flexible electronics. However, the direct bandgap of single-layer black phosphorus predicted theoretically has not been directly measured, and the properties of its edges have not been considered in detail. Here we report atomic scale electronic variation related to strain-induced anisotropic deformation of the puckered honeycomb structure of freshly cleaved black phosphorus using a highresolved scanning tunneling spectroscopy (STS) survey along the light (x) and heavy (y) effective mass directions. Through a combination of STS measurements and first-principles calculations, a model for edge reconstructionmore » is also determined. The reconstruction is shown to self-passivate any dangling bond by switching the oxidation state of phosphorous from +3 to +5.« less

Isolated Pt Atoms Stabilized by Amorphous Tungstenic Acid for Metal-Support Synergistic Oxygen Activation.

PubMed

Zhang, Qian; Qin, Xixi; Duanmu, Fanpeng; Ji, Huiming; Shen, Zhurui; Han, Xiaopeng; Hu, Wenbin

2018-06-05

Oxygen activation plays a crucial role in many important chemical reactions such as organics oxidation and oxygen reduction. For developing highly active materials for oxygen activation, herein, we report an atomically dispersed Pt on WO3 nanoplates stabilized by in-situ formed amorphous H2WO4 out-layer and the mechanism for activating molecular oxygen. Experimental and theoretical studies demonstrate that the isolated Pt atoms coordinated with oxygen atoms from [WO6] and water of H2WO4, consequently leading to optimized surface electronic configuration and strong metal support interaction (SMSI). In exemplified reactions of butanone oxidation sensing and oxygen reduction, the atomic Pt/WO3 hybrid exhibits superior activity than those of Pt nanoclusters/WO3 and bare WO3 as well as enhanced long-term durability. This work will provide insight on the origin of activity and stability for atomically dispersed materials, thus promoting the development of highly efficient and durable single atom-based catalysts. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Atomically layer-by-layer diffusion of oxygen/hydrogen in highly epitaxial PrBaCo2O5.5+δ thin films

NASA Astrophysics Data System (ADS)

Bao, Shanyong; Xu, Xing; Enriquez, Erik; Mace, Brennan E.; Chen, Garry; Kelliher, Sean P.; Chen, Chonglin; Zhang, Yamei; Whangbo, Myung-Hwan; Dong, Chuang; Zhang, Qinyu

2015-12-01

Single-crystalline epitaxial thin films of PrBaCo2O5.5+δ (PrBCO) were prepared, and their resistance R(t) under a switching flow of oxidizing and reducing gases were measured as a function of the gas flow time t in the temperature range of 200-800 °C. During the oxidation cycle under O2, the PrBCO films exhibit fast oscillations in their dR(t)/dt vs. t plots, which reflect the oxidation processes, Co2+/Co3+ → Co3+ and Co3+ → Co3+/Co4+, that the Co atoms of PrBCO undergo. Each oscillation consists of two peaks, with larger and smaller peaks representing the oxygen/hydrogen diffusion through the (BaO)(CoO2)(PrO)(CoO2) layers of PrBCO via the oxygen-vacancy-exchange mechanism. This finding paves a significant avenue for cathode materials operating in low-temperature solid-oxide-fuel-cell devices and for chemical sensors with wide range of operating temperature.

Room-temperature superparamagnetism due to giant magnetic anisotropy in Mo S defected single-layer MoS2.

PubMed

Khan, M A; Leuenberger, Michael N

2018-04-18

Room-temperature superparamagnetism due to a large magnetic anisotropy energy (MAE) of a single atom magnet has always been a prerequisite for nanoscale magnetic devices. Realization of two dimensional (2D) materials such as single-layer (SL) MoS 2 , has provided new platforms for exploring magnetic effects, which is important for both fundamental research and for industrial applications. Here, we use density functional theory (DFT) to show that the antisite defect (Mo S ) in SL MoS 2 is magnetic in nature with a magnetic moment μ of  ∼2 [Formula: see text] and, remarkably, exhibits an exceptionally large atomic scale MAE [Formula: see text] of  ∼500 meV. Our calculations reveal that this giant anisotropy is the joint effect of strong crystal field and significant spin-orbit coupling (SOC). In addition, the magnetic moment μ can be tuned between 1 [Formula: see text] and 3 [Formula: see text] by varying the Fermi energy [Formula: see text], which can be achieved either by changing the gate voltage or by chemical doping. We also show that MAE can be raised to  ∼1 eV with n-type doping of the MoS 2 :Mo S sample. Our systematic investigations deepen our understanding of spin-related phenomena in SL MoS 2 and could provide a route to nanoscale spintronic devices.

Room-temperature superparamagnetism due to giant magnetic anisotropy in Mo S defected single-layer MoS2

NASA Astrophysics Data System (ADS)

Khan, M. A.; Leuenberger, Michael N.

2018-04-01

Room-temperature superparamagnetism due to a large magnetic anisotropy energy (MAE) of a single atom magnet has always been a prerequisite for nanoscale magnetic devices. Realization of two dimensional (2D) materials such as single-layer (SL) MoS2, has provided new platforms for exploring magnetic effects, which is important for both fundamental research and for industrial applications. Here, we use density functional theory (DFT) to show that the antisite defect (Mo S ) in SL MoS2 is magnetic in nature with a magnetic moment μ of  ∼2 μB and, remarkably, exhibits an exceptionally large atomic scale MAE =\\varepsilon\\parallel-\\varepsilon\\perp of  ∼500 meV. Our calculations reveal that this giant anisotropy is the joint effect of strong crystal field and significant spin–orbit coupling (SOC). In addition, the magnetic moment μ can be tuned between 1 μB and 3 μB by varying the Fermi energy \\varepsilonF , which can be achieved either by changing the gate voltage or by chemical doping. We also show that MAE can be raised to  ∼1 eV with n-type doping of the MoS2:Mo S sample. Our systematic investigations deepen our understanding of spin-related phenomena in SL MoS2 and could provide a route to nanoscale spintronic devices.

Adsorption of dysprosium on the graphite (0001) surface: Nucleation and growth at 300 K

DOE PAGES

Kwolek, Emma J.; Lei, Huaping; Lii-Rosales, Ann; ...

2016-06-13

We have studied nucleation and growth of Dy islands on the basal plane of graphite at 300 K using scanning tunneling microscopy, density functional theory (DFT) in a form that includes van der Waals interactions, and analytic theory. The interaction of atomic Dy with graphite is strong, while the diffusion barrier is small. Experiment shows that at 300 K, the density of nucleated islands is close to the value predicted for homogeneous nucleation, using critical nucleus size of 1 and the DFT-derived diffusion barrier. Homogeneous nucleation is also supported by the monomodal shape of the island size distributions. Comparison withmore » the published island density of Dy on graphene shows that the value is about two orders of magnitude smaller on graphite, which can be attributed to more effective charge screening in graphite. The base of each island is 3 atomic layers high and atomically ordered, forming a coincidence lattice with the graphite. Islands resist coalescence, probably due to multiple rotational orientations associated with the coincidence lattice. Upper levels grow as discernible single-atom layers. Analysis of the level populations reveals significant downward interlayer transport, which facilitates growth of the base. As a result, this island shape is metastable, since more compact three-dimensional islands form at elevated growth temperature.« less

Adsorption of dysprosium on the graphite (0001) surface: Nucleation and growth at 300 K

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

Kwolek, Emma J.; Lii-Rosales, Ann; Department of Chemistry, Iowa State University, Ames, Iowa 50011

2016-12-07

We have studied nucleation and growth of Dy islands on the basal plane of graphite at 300 K using scanning tunneling microscopy, density functional theory (DFT) in a form that includes van der Waals interactions, and analytic theory. The interaction of atomic Dy with graphite is strong, while the diffusion barrier is small. Experiment shows that at 300 K, the density of nucleated islands is close to the value predicted for homogeneous nucleation, using critical nucleus size of 1 and the DFT-derived diffusion barrier. Homogeneous nucleation is also supported by the monomodal shape of the island size distributions. Comparison withmore » the published island density of Dy on graphene shows that the value is about two orders of magnitude smaller on graphite, which can be attributed to more effective charge screening in graphite. The base of each island is 3 atomic layers high and atomically ordered, forming a coincidence lattice with the graphite. Islands resist coalescence, probably due to multiple rotational orientations associated with the coincidence lattice. Upper levels grow as discernible single-atom layers. Analysis of the level populations reveals significant downward interlayer transport, which facilitates growth of the base. This island shape is metastable, since more compact three-dimensional islands form at elevated growth temperature.« less

Engineering New Layered Solids from Exfoliated Inorganics: a Periodically Alternating Hydrotalcite – Montmorillonite Layered Hybrid

PubMed Central

Chalasani, Rajesh; Gupta, Amit; Vasudevan, Sukumaran

2013-01-01

Two-dimensional (2D) nanosheets obtained by exfoliating inorganic layered crystals have emerged as a new class of materials with unique attributes. One of the critical challenges is to develop robust and versatile methods for creating new nanostructures from these 2D-nanosheets. Here we report the delamination of layered materials that belonging to two different classes - the cationic clay, montmorillonite, and the anionic clay, hydrotalcite - by intercalation of appropriate ionic surfactants followed by dispersion in a non-polar solvent. The solids are delaminated to single layers of atomic thickness with the ionic surfactants remaining tethered to the inorganic and consequently the nanosheets are electrically neutral. We then show that when dispersions of the two solids are mixed the exfoliated sheets self-assemble as a new layered solid with periodically alternating hydrotalcite and montmorillonite layers. The procedure outlined here is easily extended to other layered solids for creating new superstructures from 2D-nanosheets by self-assembly. PMID:24336682

Use of Single-Layer g-C3N4/Ag Hybrids for Surface-Enhanced Raman Scattering (SERS)

PubMed Central

Jiang, Jizhou; Zou, Jing; Wee, Andrew Thye Shen; Zhang, Wenjing

2016-01-01

Surface-enhanced Raman scattering (SERS) substrates with high activity and stability are desirable for SERS sensing. Here, we report a new single atomic layer graphitic-C3N4 (S-g-C3N4) and Ag nanoparticles (NPs) hybrid as high-performance SERS substrates. The SERS mechanism of the highly stable S-g-C3N4/Ag substrates was systematically investigated by a combination of experiments and theoretical calculations. From the results of XPS and Raman spectroscopies, it was found that there was a strong interaction between S-g-C3N4 and Ag NPs, which facilitates the uniform distribution of Ag NPs over the edges and surfaces of S-g-C3N4 nanosheets, and induces a charge transfer from S-g-C3N4 to the oxidizing agent through the silver surface, ultimately protecting Ag NPs from oxidation. Based on the theoretical calculations, we found that the net surface charge of the Ag atoms on the S-g-C3N4/Ag substrates was positive and the Ag NPs presented high dispersibility, suggesting that the Ag atoms on the S-g-C3N4/Ag substrates were not likely to be oxidized, thereby ensuring the high stability of the S-g-C3N4/Ag substrate. An understanding of the stability mechanism in this system can be helpful for developing other effective SERS substrates with long-term stability. PMID:27687573

Site selectivity on chalcogen atoms in superconducting La(O,F)BiSSe

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

Tanaka, Masashi, E-mail: Tanaka.Masashi@nims.go.jp; Matsushita, Yoshitaka; Fujioka, Masaya

2015-03-16

Single crystals of La(O,F)BiSSe were grown by using a CsCl flux method. Single crystal X-ray structural analysis reveals that the crystal structure is isostructural to the BiS{sub 2}- or BiSe{sub 2}-based compounds crystallizing with space group P4/nmm (lattice parameters a = 4.1110(2) Å, c = 13.6010(7) Å). However, the S atoms are selectively occupied at the apical site of the Bi-SSe pyramids in the superconducting layer. The single crystals show a superconducting transition at around 4.2 K in the magnetic susceptibility and resistivity measurements. The superconducting anisotropic parameter is determined to be 34–35 from its upper critical magnetic field. The anisotropy is in the same range withmore » that of other members of the La(O,F)BiCh{sub 2} (Ch = S, Se) family under ambient pressure.« less

Synthesis and structure of cesium complexes of nitrilotris(methylenephosphonic) acid [Cs-μ6-NH(CH2PO3)3H4] and [Cs2-μ10-NH(CH2PO3H)3] · H2O

NASA Astrophysics Data System (ADS)

Somov, N. V.; Chausov, F. F.; Zakirov, R. M.

2017-07-01

3D coordination polymers cesium nitrilotris(methylenephosphonate) and dicesium nitrilotris( methylenephosphonate) are synthesized and their crystal structure is determined. In the crystal of [Cs-μ6-NH(CH2PO3)3H4] (space group P, Z = 2), cesium atoms occupy two crystallographically inequivalent positions with c.n. = 10 and c.n. = 14. The phosphonate ligand plays the bridging function; its denticity is nine. The crystal packing consists of alternating layers of Cs atoms in different environments with layers of ligand molecules between them. A ligand is bound to three Cs atoms of one layer and three Cs atoms of another layer. In the crystal of [Cs2-μ10-NH(CH2PO3H)3] · H2O (space group P, Z = 2), the complex has a dimeric structure: the bridging phosphonate ligand coordinates Cs to form a three-dimensional Cs4O6 cluster. The denticity of the ligand is equal to nine; the coordination numbers of cesium atoms are seven and nine. Two-dimensional corrugated layers of Cs4O6 clusters lie in the (002) plane, and layers of ligand molecules are located between them. Each ligand molecule coordinates eight Cs atoms of one layer and two Cs atoms of the neighboring layer.

Consequences of atomic layer etching on wafer scale uniformity in inductively coupled plasmas

NASA Astrophysics Data System (ADS)

Huard, Chad M.; Lanham, Steven J.; Kushner, Mark J.

2018-04-01

Atomic layer etching (ALE) typically divides the etching process into two self-limited reactions. One reaction passivates a single layer of material while the second preferentially removes the passivated layer. As such, under ideal conditions the wafer scale uniformity of ALE should be independent of the uniformity of the reactant fluxes onto the wafers, provided all surface reactions are saturated. The passivation and etch steps should individually asymptotically saturate after a characteristic fluence of reactants has been delivered to each site. In this paper, results from a computational investigation are discussed regarding the uniformity of ALE of Si in Cl2 containing inductively coupled plasmas when the reactant fluxes are both non-uniform and non-ideal. In the parameter space investigated for inductively coupled plasmas, the local etch rate for continuous processing was proportional to the ion flux. When operated with saturated conditions (that is, both ALE steps are allowed to self-terminate), the ALE process is less sensitive to non-uniformities in the incoming ion flux than continuous etching. Operating ALE in a sub-saturation regime resulted in less uniform etching. It was also found that ALE processing with saturated steps requires a larger total ion fluence than continuous etching to achieve the same etch depth. This condition may result in increased resist erosion and/or damage to stopping layers using ALE. While these results demonstrate that ALE provides increased etch depth uniformity, they do not show an improved critical dimension uniformity in all cases. These possible limitations to ALE processing, as well as increased processing time, will be part of the process optimization that includes the benefits of atomic resolution and improved uniformity.

Surface topography and electrical properties in Sr2FeMoO6 films studied at cryogenic temperatures

NASA Astrophysics Data System (ADS)

Angervo, I.; Saloaro, M.; Mäkelä, J.; Lehtiö, J.-P.; Huhtinen, H.; Paturi, P.

2018-03-01

Pulsed laser deposited Sr2FeMoO6 thin films were investigated for the first time with scanning tunneling microscopy and spectroscopy. The results confirm atomic scale layer growth, with step-terrace structure corresponding to a single lattice cell scale. The spectroscopy research reveals a distribution of local electrical properties linked to structural deformation in the initial thin film layers at the film substrate interface. Significant hole structure giving rise to electrically distinctive regions in thinner film also seems to set a thickness limit for the thinnest films to be used in applications.

Diffusion of Supercritical Fluids through Single-Layer Nanoporous Solids: Theory and Molecular Simulations.

PubMed

Oulebsir, Fouad; Vermorel, Romain; Galliero, Guillaume

2018-01-16

With the advent of graphene material, membranes based on single-layer nanoporous solids appear as promising devices for fluid separation, be it liquid or gaseous mixtures. The design of such architectured porous materials would greatly benefit from accurate models that can predict their transport and separation properties. More specifically, there is no universal understanding of how parameters such as temperature, fluid loading conditions, or the ratio of the pore size to the fluid molecular diameter influence the permeation process. In this study, we address the problem of pure supercritical fluids diffusing through simplified models of single-layer porous materials. Basically, we investigate a toy model that consists of a single-layer lattice of Lennard-Jones interaction sites with a slit gap of controllable width. We performed extensive equilibrium and biased molecular dynamics simulations to document the physical mechanisms involved at the molecular scale. We propose a general constitutive equation for the diffusional transport coefficient derived from classical statistical mechanics and kinetic theory, which can be further simplified in the ideal gas limit. This transport coefficient relates the molecular flux to the fluid density jump across the single-layer membrane. It is found to be proportional to the accessible surface porosity of the single-layer porous solid and to a thermodynamic factor accounting for the inhomogeneity of the fluid close to the pore entrance. Both quantities directly depend on the potential of mean force that results from molecular interactions between solid and fluid atoms. Comparisons with the simulations data show that the kinetic model captures how narrowing the pore size below the fluid molecular diameter lowers dramatically the value of the transport coefficient. Furthermore, we demonstrate that our general constitutive equation allows for a consistent interpretation of the intricate effects of temperature and fluid loading conditions on the permeation process.

Fine tuning of nanopipettes using atomic layer deposition for single molecule sensing.

PubMed

Sze, Jasmine Y Y; Kumar, Shailabh; Ivanov, Aleksandar P; Oh, Sang-Hyun; Edel, Joshua B

2015-07-21

Nanopipettes are an attractive single-molecule tool for identification and characterisation of nucleic acids and proteins in solutions. They enable label-free analysis and reveal individual molecular properties, which are generally masked by ensemble averaging. Having control over the pore dimensions is vital to ensure that the dimensions of the molecules being probed match those of the pore for optimization of the signal to noise. Although nanopipettes are simple and easy to fabricate, challenges exist, especially when compared to more conventional solid-state analogues. For example, a sub-20 nm pore diameter can be difficult to fabricate and the batch-to-batch reproducibility is often poor. To improve on this limitation, atomic layer deposition (ALD) is used to deposit ultrathin layers of alumina (Al2O3) on the surface of the quartz nanopipettes enabling sub-nm tuning of the pore dimensions. Here, Al2O3 with a thickness of 8, 14 and 17 nm was deposited onto pipettes with a starting pore diameter of 75 ± 5 nm whilst a second batch had 5 and 8 nm Al2O3 deposited with a starting pore diameter of 25 ± 3 nm respectively. This highly conformal process coats both the inner and outer surfaces of pipettes and resulted in the fabrication of pore diameters as low as 7.5 nm. We show that Al2O3 modified pores do not interfere with the sensing ability of the nanopipettes and can be used for high signal-to-noise DNA detection. ALD provides a quick and efficient (batch processing) for fine-tuning nanopipettes for a broad range of applications including the detection of small biomolecules like RNA, aptamers and DNA-protein interactions at the single molecule level.

Oxygen Displacement in Cuprates under IonicLiquid Field-Effect Gating

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

Dubuis, Guy; Yacoby, Yizhak; Zhou, Hua

We studied structural changes in a 5 unit cell thick La 1.96Sr 0.04CuO 4 film, epitaxially grown on a LaSrAlO 4 substrate with a single unit cell buffer layer, when ultra-high electric fields were induced in the film by applying a gate voltage between the film and an ionic liquid in contact with it. Measuring the diffraction intensity along the substrate-defined Bragg rods and analyzing the results using a phase retrieval method we obtained the three-dimensional electron density in the film, buffer layer, and topmost atomic layers of the substrate under different applied gate voltages. The main structural observations were:more » (i) there were no structural changes when the voltage was negative, holes were injected into the film making it more metallic and screening the electric field; (ii) when the voltage was positive, the film was depleted of holes becoming more insulating, the electric field extended throughout the film, the partial surface monolayer became disordered, and planar oxygen atoms were displaced towards the sample surface; (iii) the changes in surface disorder and the oxygen displacements were both reversed when a negative voltage was applied; and (iv) the c-axis lattice constant of the film did not change in spite of the displacement of planar oxygen atoms.« less

Oxygen Displacement in Cuprates under IonicLiquid Field-Effect Gating

DOE PAGES

Dubuis, Guy; Yacoby, Yizhak; Zhou, Hua; ...

2016-08-15

We studied structural changes in a 5 unit cell thick La 1.96Sr 0.04CuO 4 film, epitaxially grown on a LaSrAlO 4 substrate with a single unit cell buffer layer, when ultra-high electric fields were induced in the film by applying a gate voltage between the film and an ionic liquid in contact with it. Measuring the diffraction intensity along the substrate-defined Bragg rods and analyzing the results using a phase retrieval method we obtained the three-dimensional electron density in the film, buffer layer, and topmost atomic layers of the substrate under different applied gate voltages. The main structural observations were:more » (i) there were no structural changes when the voltage was negative, holes were injected into the film making it more metallic and screening the electric field; (ii) when the voltage was positive, the film was depleted of holes becoming more insulating, the electric field extended throughout the film, the partial surface monolayer became disordered, and planar oxygen atoms were displaced towards the sample surface; (iii) the changes in surface disorder and the oxygen displacements were both reversed when a negative voltage was applied; and (iv) the c-axis lattice constant of the film did not change in spite of the displacement of planar oxygen atoms.« less

Cross-Sectional Imaging of Boundary Lubrication Layer Formed by Fatty Acid by Means of Frequency-Modulation Atomic Force Microscopy.

PubMed

Hirayama, Tomoko; Kawamura, Ryota; Fujino, Keita; Matsuoka, Takashi; Komiya, Hiroshi; Onishi, Hiroshi

2017-10-10

To observe in situ the adsorption of fatty acid onto metal surfaces, cross-sectional images of the adsorption layer were acquired by frequency-modulation atomic force microscopy (FM-AFM). Hexadecane and palmitic acid were used as the base oil and typical fatty acid, respectively. A Cu-coated silicon wafer was prepared as the target substrate. The solvation structure formed by hexadecane molecules at the interface between the Cu substrate and the hexadecane was observed, and the layer pitch was found to be about 0.6 nm, which corresponds to the height of hexadecane molecules. This demonstrates that hexadecane molecules physically adsorbed onto the surface due to van der Waals forces with lying orientation because hexadecane is a nonpolar hydrocarbon. When hexadecane with palmitic acid was put on the Cu substrate instead of pure hexadecane, an adsorption layer of palmitic acid was observed at the interface. The layer pitch was about 2.5-2.8 nm, which matches the chain length of palmitic acid molecules well. This indicates that the original adsorption layer was monolayer or single bilayer in the local area. In addition, a cross-sectional image captured 1 h after observation started to reveal that the adsorbed additive layer gradually grew up to be thicker than about 20 nm due to an external stimulus, such as cantilever oscillation. This is the first report of in situ observation of an adsorbed layer by FM-AFM in the tribology field and demonstrates that FM-AFM is useful for clarifying the actual boundary lubrication mechanism.

Nanoforging Single Layer MoSe 2 Through Defect Engineering with Focused Helium Ion Beams

DOE PAGES

Iberi, Vighter; Liang, Liangbo; Ievlev, Anton V.; ...

2016-08-02

Development of devices and structures based on the layered 2D materials critically hinges on the capability to induce, control, and tailor the electronic, transport, and optoelectronic properties via defect engineering, much like doping strategies have enabled semiconductor electronics and forging enabled introduction of iron age. Here, we demonstrate the use of a scanning helium ion microscope (HIM) for tailoring the functionality of single layer MoSe 2 locally, and decipher associated mechanisms at atomic level. We demonstrate He + beam bombardment that locally creates vacancies, shifts the Fermi energy landscape and thereby increases the Young s modulus of elasticity. Furthermore, wemore » observe for the first time, an increase in the B-exciton photoluminescence signal from the nanoforged regions at room temperature. In conclusion, the approach for precise defect engineering demonstrated here opens opportunities for creating functional 2D optoelectronic devices with a wide range of customizable properties that include operating in the visible region.« less

Nanoforging Single Layer MoSe 2 Through Defect Engineering with Focused Helium Ion Beams

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

Iberi, Vighter; Liang, Liangbo; Ievlev, Anton V.

Development of devices and structures based on the layered 2D materials critically hinges on the capability to induce, control, and tailor the electronic, transport, and optoelectronic properties via defect engineering, much like doping strategies have enabled semiconductor electronics and forging enabled introduction of iron age. Here, we demonstrate the use of a scanning helium ion microscope (HIM) for tailoring the functionality of single layer MoSe 2 locally, and decipher associated mechanisms at atomic level. We demonstrate He + beam bombardment that locally creates vacancies, shifts the Fermi energy landscape and thereby increases the Young s modulus of elasticity. Furthermore, wemore » observe for the first time, an increase in the B-exciton photoluminescence signal from the nanoforged regions at room temperature. In conclusion, the approach for precise defect engineering demonstrated here opens opportunities for creating functional 2D optoelectronic devices with a wide range of customizable properties that include operating in the visible region.« less

Nanoforging Single Layer MoSe2 Through Defect Engineering with Focused Helium Ion Beams

NASA Astrophysics Data System (ADS)

Iberi, Vighter; Liang, Liangbo; Ievlev, Anton V.; Stanford, Michael G.; Lin, Ming-Wei; Li, Xufan; Mahjouri-Samani, Masoud; Jesse, Stephen; Sumpter, Bobby G.; Kalinin, Sergei V.; Joy, David C.; Xiao, Kai; Belianinov, Alex; Ovchinnikova, Olga S.

2016-08-01

Development of devices and structures based on the layered 2D materials critically hinges on the capability to induce, control, and tailor the electronic, transport, and optoelectronic properties via defect engineering, much like doping strategies have enabled semiconductor electronics and forging enabled introduction the of iron age. Here, we demonstrate the use of a scanning helium ion microscope (HIM) for tailoring the functionality of single layer MoSe2 locally, and decipher associated mechanisms at the atomic level. We demonstrate He+ beam bombardment that locally creates vacancies, shifts the Fermi energy landscape and increases the Young’s modulus of elasticity. Furthermore, we observe for the first time, an increase in the B-exciton photoluminescence signal from the nanoforged regions at the room temperature. The approach for precise defect engineering demonstrated here opens opportunities for creating functional 2D optoelectronic devices with a wide range of customizable properties that include operating in the visible region.

The Effect of Buffer Types on the In0.82Ga0.18As Epitaxial Layer Grown on an InP (100) Substrate.

PubMed

Zhang, Min; Guo, Zuoxing; Zhao, Liang; Yang, Shen; Zhao, Lei

2018-06-08

In 0.82 Ga 0.18 As epitaxial layers were grown on InP (100) substrates at 530 °C by a low-pressure metalorganic chemical vapor deposition (LP-MOCVD) technique. The effects of different buffer structures, such as a single buffer layer, compositionally graded buffer layers, and superlattice buffer layers, on the crystalline quality and property were investigated. Double-crystal X-ray diffraction (DC-XRD) measurement, Raman scattering spectrum, and Hall measurements were used to evaluate the crystalline quality and electrical property. Scanning electron microscope (SEM), atomic force microscope (AFM), and transmission electron microscope (TEM) were used to characterize the surface morphology and microstructure, respectively. Compared with the In 0.82 Ga 0.18 As epitaxial layer directly grown on an InP substrate, the quality of the sample is not obviously improved by using a single In 0.82 Ga 0.18 As buffer layer. By introducing the graded In x Ga 1−x As buffer layers, it was found that the dislocation density in the epitaxial layer significantly decreased and the surface quality improved remarkably. In addition, the number of dislocations in the epitaxial layer greatly decreased under the combined action of multi-potential wells and potential barriers by the introduction of a In 0.82 Ga 0.18 As/In 0.82 Al 0.18 As superlattice buffer. However, the surface subsequently roughened, which may be explained by surface undulation.

Zn or O? An Atomic Level Comparison on Antibacterial Activities of Zinc Oxides.

PubMed

Yu, Fen; Fang, Xuan; Jia, Huimin; Liu, Miaoxing; Shi, Xiaotong; Xue, Chaowen; Chen, Tingtao; Wei, Zhipeng; Fang, Fang; Zhu, Hui; Xin, Hongbo; Feng, Jing; Wang, Xiaolei

2016-06-06

For the first time, the influence of different types of atoms (Zn and O) on the antibacterial activities of nanosized ZnO was quantitatively evaluated with the aid of a 3D-printing-manufactured evaluation system. Two different outermost atomic layers were manufactured separately by using an ALD (atomic layer deposition) method. Interestingly, we found that each outermost atomic layer exhibited certain differences against gram-positive or gram-negative bacterial species. Zinc atoms as outermost layer (ZnO-Zn) showed a more pronounced antibacterial effect towards gram-negative E. coli (Escherichia coli), whereas oxygen atoms (ZnO-O) showed a stronger antibacterial activity against gram-positive S. aureus (Staphylococcus aureus). A possible antibacterial mechanism has been comprehensively discussed from different perspectives, including Zn(2+) concentrations, oxygen vacancies, photocatalytic activities and the DNA structural characteristics of different bacterial species. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Dynamics of radiocesium exchange and interstratification in anhydrous clay interlayers: Bridging the atom and single crystal scales

NASA Astrophysics Data System (ADS)

Lammers, L. N.; Pestana, L. R.; Schaettle, K. B.; Head-Gordon, T.

2016-12-01

High structural charge clay minerals govern the transport and retention of radiocesium in soils and clay-rich geologic repositories. Cation exchange capacities in these phases are typically assumed to be limited to fast-exchanging basal and high-affinity edge sites, while ions in anhydrous interlayers, usually K+, are considered non-exchangeable. However, recent high resolution imaging and spectroscopic studies have demonstrated that Cs ions can in fact exchange with interlayer K without the formation of a hydrated intermediate.1,2 These exchange reactions result in sharp exchange fronts wherein K+ ions are completely replaced by Cs+ at the exchange interface, and the rate of exchange varies from layer to layer, resulting in the formation of interstratified structures (i.e., randomly alternating layers of exchanged and pristine interlayers). Currently, this process cannot be explained by any known exchange mechanism, and consequently, no kinetic expressions are available to account for this phenomenon in models of subsurface radiocesium fate and transport. We present a mesoscale model for direct exchange in anhydrous clay interlayers that is based on the kinetics of single ion migration events. Single atom migration kinetics derived from density functional theory (DFT) calculations are used as inputs to kinetic Monte Carlo (kMC) simulations, which capture the collective dynamics of the exchange process over length- and timescales relevant for implementation in reactive transport models. Potential energy surfaces derived from DFT demonstrate that exchange of Cs+ for K+ in anhydrous interlayers lowers the energy barrier to K ion migration by 145 kJ/mol, leading to a positive feedback mechanism that generates atomically sharp exchange fronts. Our work demonstrates the application of "coarse-graining" techniques to develop models for processes with characteristic length- and timescales not accessible by direct atomistic simulation. 1 Okumura T. et al. (2014) Direct observation of cesium at the interlayer region in phlogopite mica. Microscopy 63(1), 65-72. 2 Fuller A. J. et al. (2015) Caesium incorporation and retention in illite interlayers. Appl. Clay Sci. 108, 128-134.

Interface reconstruction with emerging charge ordering in hexagonal manganite

PubMed Central

Xu, Changsong; Han, Myung-Geun; Bao, Shanyong; Nan, Cewen; Bellaiche, Laurent

2018-01-01

Multiferroic materials, which simultaneously have multiple orderings, hold promise for use in the next generation of memory devices. We report a novel self-assembled MnO double layer forming at the interface between a multiferroic YMnO3 film and a c-Al2O3 substrate. The crystal structures and the valence states of this MnO double layer were studied by atomically resolved scanning transmission electron microscopy and spectroscopy, as well as density functional theory (DFT) calculations. A new type of charge ordering has been identified within this MnO layer, which also contributes to a polarization along the [001] direction. DFT calculations further establish the occurrence of multiple couplings between charge and lattice in this novel double layer, in addition to the polarization in nearby YMnO3 single layer. The interface reconstruction reported here creates a new playground for emergent physics, such as giant ferroelectricity and strong magnetoelectric coupling, in manganite systems. PMID:29795782

Choosing a therapy electron accelerator target.

PubMed

Hutcheon, R M; Schriber, S O; Funk, L W; Sherman, N K

1979-01-01

Angular distributions of photon depth dose produced by 25-MeV electrons incident on several fully stopping single-element targets (C, Al, Cu, Mo, Ta, Pb) and two composite layered targets (Ni-Al, W-Al) were studied. Depth-dose curves measured using TLD-700 (thermoluminescent dosimeter) chips embedded in lucite phantoms. Several useful therapy electron accelerator design curves were determined, including relative flattener thickness as a function of target atomic number, "effective" bremsstrahlung endpoint energy or beam "hardness" as a function of target atomic number and photon emission angle, and estimates of shielding thickness as a function of angle required to reduce the radiation outside the treatment cone to required levels.

Ultrahard carbon film from epitaxial two-layer graphene

NASA Astrophysics Data System (ADS)

Gao, Yang; Cao, Tengfei; Cellini, Filippo; Berger, Claire; de Heer, Walter A.; Tosatti, Erio; Riedo, Elisa; Bongiorno, Angelo

2018-02-01

Atomically thin graphene exhibits fascinating mechanical properties, although its hardness and transverse stiffness are inferior to those of diamond. So far, there has been no practical demonstration of the transformation of multilayer graphene into diamond-like ultrahard structures. Here we show that at room temperature and after nano-indentation, two-layer graphene on SiC(0001) exhibits a transverse stiffness and hardness comparable to diamond, is resistant to perforation with a diamond indenter and shows a reversible drop in electrical conductivity upon indentation. Density functional theory calculations suggest that, upon compression, the two-layer graphene film transforms into a diamond-like film, producing both elastic deformations and sp2 to sp3 chemical changes. Experiments and calculations show that this reversible phase change is not observed for a single buffer layer on SiC or graphene films thicker than three to five layers. Indeed, calculations show that whereas in two-layer graphene layer-stacking configuration controls the conformation of the diamond-like film, in a multilayer film it hinders the phase transformation.

Electron Doping of Ultrathin Black Phosphorus with Cu Adatoms.

PubMed

Koenig, Steven P; Doganov, Rostislav A; Seixas, Leandro; Carvalho, Alexandra; Tan, Jun You; Watanabe, Kenji; Taniguchi, Takashi; Yakovlev, Nikolai; Castro Neto, Antonio H; Özyilmaz, Barbaros

2016-04-13

Few-layer black phosphorus is a monatomic two-dimensional crystal with a direct band gap that has high carrier mobility for both holes and electrons. Similarly to other layered atomic crystals, like graphene or layered transition metal dichalcogenides, the transport behavior of few-layer black phosphorus is sensitive to surface impurities, adsorbates, and adatoms. Here we study the effect of Cu adatoms onto few-layer black phosphorus by characterizing few-layer black phosphorus field effect devices and by performing first-principles calculations. We find that the addition of Cu adatoms can be used to controllably n-dope few layer black phosphorus, thereby lowering the threshold voltage for n-type conduction without degrading the transport properties. We demonstrate a scalable 2D material-based complementary inverter which utilizes a boron nitride gate dielectric, a graphite gate, and a single bP crystal for both the p- and n-channels. The inverter operates at matched input and output voltages, exhibits a gain of 46, and does not require different contact metals or local electrostatic gating.

Oriented Y-type hexagonal ferrite thin films prepared by chemical solution deposition

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

Buršík, J., E-mail: bursik@iic.cas.cz; Kužel, R.; Knížek, K.

2013-07-15

Thin films of Ba{sub 2}Zn{sub 2}Fe{sub 12}O{sub 22} (Y) hexaferrite were prepared through the chemical solution deposition method on SrTiO{sub 3}(1 1 1) (ST) single crystal substrates using epitaxial SrFe{sub 12}O{sub 19} (M) hexaferrite thin layer as a seed template layer. The process of crystallization was mainly investigated by means of X-ray diffraction and atomic force microscopy. A detailed inspection revealed that growth of seed layer starts through the break-up of initially continuous film into isolated grains with expressive shape anisotropy and hexagonal habit. The vital parameters of the seed layer, i.e. thickness, substrate coverage, crystallization conditions and temperature rampmore » were optimized with the aim to obtain epitaxially crystallized Y phase. X-ray diffraction Pole figure measurements and Φ scans reveal perfect parallel in-plane alignment of SrTiO{sub 3} substrate and both hexaferrite phases. - Graphical abstract: XRD pole figure and AFM patterns of Ba{sub 2}Zn{sub 2}Fe{sub 12}O{sub 22} thin film epitaxially grown on SrTiO{sub 3}(1 1 1) single crystal using seeding layer templating. - Highlights: • Single phase Y-type hexagonal ferrite thin films were prepared by CSD method. • Seed M layer breaks into isolated single crystal islands and serves as a template. • Large seed grains grow by consuming the grains within the bulk of recoated film. • We explained the observed orientation relation of epitaxial domains. • Epitaxial growth on SrTiO{sub 3}(1 1 1) with relation (0 0 1){sub M,Y}//(1 1 1){sub ST}+[1 0 0]{sub M,Y}//[2 −1 −1]{sub ST}.« less

Ionothermal synthesis, characterization of a new layered gallium phosphate with an unusual heptamer SBU

NASA Astrophysics Data System (ADS)

Gao, Fan; Huang, Liangliang; Ma, Yike; Jiao, Shufei; Jiang, Yansong; Bi, Yanfeng

2017-10-01

A new layered gallium phosphate Ga3(PO4)4(C2N2H8)·(H2C2N2H8)2·Cl (compound 1), has been ionothermally synthesized in the presence of deep eutectic solvent (DES) comprising mixtures of choline chloride and 2-imidazolidone (IMI). Single-crystal X-ray diffraction analysis reveals that compound 1 shows 2D layered framework with 10-ring windows, which is constructed from unusual heptamer second building units (SBUs). The ethylenediamine (en) units deriving from the decomposition of IMI, play a dual role as bidentate ligands coordinated with 6-fold coordinate gallium atoms and the templates. Additionally, compound 1 shows photoluminescence property in solid state at room temperature.

FAST TRACK COMMUNICATION: Graphene based quantum dots

NASA Astrophysics Data System (ADS)

Zhang, H. G.; Hu, H.; Pan, Y.; Mao, J. H.; Gao, M.; Guo, H. M.; Du, S. X.; Greber, T.; Gao, H.-J.

2010-08-01

Laterally localized electronic states are identified on a single layer of graphene on ruthenium by low temperature scanning tunneling spectroscopy (STS). The individual states are separated by 3 nm and comprise regions of about 90 carbon atoms. This constitutes a highly regular quantum dot-array with molecular precision. It is evidenced by quantum well resonances (QWRs) with energies that relate to the corrugation of the graphene layer. The dI/dV conductance spectra are modeled by a layer height dependent potential-well with a delta-function potential that describes the barrier for electron penetration into graphene. The resulting QWRs are strongest and lowest in energy on the isolated 'hill' regions with a diameter of 2 nm, where the graphene is decoupled from the surface.

Graphene based quantum dots.

PubMed

Zhang, H G; Hu, H; Pan, Y; Mao, J H; Gao, M; Guo, H M; Du, S X; Greber, T; Gao, H-J

2010-08-04

Laterally localized electronic states are identified on a single layer of graphene on ruthenium by low temperature scanning tunneling spectroscopy (STS). The individual states are separated by 3 nm and comprise regions of about 90 carbon atoms. This constitutes a highly regular quantum dot-array with molecular precision. It is evidenced by quantum well resonances (QWRs) with energies that relate to the corrugation of the graphene layer. The dI/dV conductance spectra are modeled by a layer height dependent potential-well with a delta-function potential that describes the barrier for electron penetration into graphene. The resulting QWRs are strongest and lowest in energy on the isolated 'hill' regions with a diameter of 2 nm, where the graphene is decoupled from the surface.

High-pressure synthesis and crystal structures of the strontium oxogallates Sr2Ga2O5 and Sr5Ga6O14

NASA Astrophysics Data System (ADS)

Kahlenberg, Volker; Goettgens, Valerie; Mair, Philipp; Schmidmair, Daniela

2015-08-01

High-pressure synthesis experiments in a piston-cylinder apparatus at 1.5 GPa/3.0 GPa and 1000 °C resulted in the formation of single-crystals of Sr2Ga2O5 and Sr5Ga6O14, respectively. The structures of both compounds have been solved from single-crystal diffraction data sets using direct methods. The first compound is orthorhombic with space group type Pbca (a=10.0021(4) Å, b=9.601(4) Å, c=10.6700(4) Å, V=1024.6(4) Å3, Mr=394.68 u, Z=8, Dx=5.12 g/cm3) and belongs to the group of single layer gallates. Individual sheets are parallel to (0 0 1) and can be built from the condensation of unbranched vierer single chains running along [0 1 0]. The layers are characterized by the presence of four- and strongly elliptical eight-membered rings of corner connected tetrahedra in UUDD and UUUUDDDD conformation. Strontium atoms are sandwiched between the tetrahedral layers for charge compensation and are coordinated by six and seven oxygen ligands, respectively. Sr2Ga2O5 is isotypic with several other double sulfides and selenides. To the best of our knowledge, it is the first example of an oxide with this structure type. From a structural point of view, Sr5Ga6O14 is a phyllogallate as well. The crystal structure adopts the monoclinic space group P21/c (a=8.1426(3) Å, b=8.1803(3) Å, c=10.8755(4) Å, β=91.970(4)° V=723.98(5) Å3, Mr=1080.42 u, Z=2, Dx=4.96 g/cm3). Individual sheets extend along (0 0 1). Basic building units are unbranched dreier single chains parallel to [1 0 0]. The layers contain tertiary (Q3) und quaternary (Q4) connected [GaO4]-tetrahedra in the ratio 2:1 resulting in a Ga:O ratio of 3:7 and the formation of exclusively five-membered rings. Linkage between adjacent tetrahedral sheets is provided by three symmetrically independent strontium ions which are surrounded by six to eight oxygen atoms. The layers in Sr5Ga6O14 are similar to those observed in the melilite structure-type. Crystallochemical relationships between the present phases and other known compounds are discussed in detail.

Patterned growth of p-type MoS 2 atomic layers using sol-gel as precursor

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

Zheng, Wei; Lin, Junhao; Feng, Wei

2D layered MoS 2 has drawn intense attention for its applications in flexible electronic, optoelectronic, and spintronic devices. Most of the MoS 2 atomic layers grown by conventional chemical vapor deposition techniques are n-type due to the abundant sulfur vacancies. Facile production of MoS 2 atomic layers with p-type behavior, however, remains challenging. Here, a novel one-step growth has been developed to attain p-type MoS 2 layers in large scale by using Mo-containing sol–gel, including 1% tungsten (W). Atomic-resolution electron microscopy characterization reveals that small tungsten oxide clusters are commonly present on the as-grown MoS 2 film due to themore » incomplete reduction of W precursor at the reaction temperature. These omnipresent small tungsten oxide clusters contribute to the p-type behavior, as verified by density functional theory calculations, while preserving the crystallinity of the MoS 2 atomic layers. The Mo containing sol–gel precursor is compatible with the soft-lithography techniques, which enables patterned growth of p-type MoS 2 atomic layers into regular arrays with different shapes, holding great promise for highly integrated device applications. Lastly, an atomically thin p–n junction is fabricated by the as-prepared MoS 2, which shows strong rectifying behavior.« less

Patterned growth of p-type MoS 2 atomic layers using sol-gel as precursor

DOE PAGES

Zheng, Wei; Lin, Junhao; Feng, Wei; ...

2016-07-19

2D layered MoS 2 has drawn intense attention for its applications in flexible electronic, optoelectronic, and spintronic devices. Most of the MoS 2 atomic layers grown by conventional chemical vapor deposition techniques are n-type due to the abundant sulfur vacancies. Facile production of MoS 2 atomic layers with p-type behavior, however, remains challenging. Here, a novel one-step growth has been developed to attain p-type MoS 2 layers in large scale by using Mo-containing sol–gel, including 1% tungsten (W). Atomic-resolution electron microscopy characterization reveals that small tungsten oxide clusters are commonly present on the as-grown MoS 2 film due to themore » incomplete reduction of W precursor at the reaction temperature. These omnipresent small tungsten oxide clusters contribute to the p-type behavior, as verified by density functional theory calculations, while preserving the crystallinity of the MoS 2 atomic layers. The Mo containing sol–gel precursor is compatible with the soft-lithography techniques, which enables patterned growth of p-type MoS 2 atomic layers into regular arrays with different shapes, holding great promise for highly integrated device applications. Lastly, an atomically thin p–n junction is fabricated by the as-prepared MoS 2, which shows strong rectifying behavior.« less

Effect of the intra-layer potential distributions and spatial currents on the performance of graphene SymFETs

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

Hasan, Mehdi; Sensale-Rodriguez, Berardi, E-mail: berardi.sensale@utah.edu

2015-09-15

In this paper, a two-dimensional (2-D) model for a graphene symmetric field effect transistor (SymFET), which considers (a) the intra-graphene layer potential distributions and (b) the internal current flows through the device, is presented and discussed. The local voltages along the graphene electrodes as well as the current-voltage characteristics of the device are numerically calculated based on a single-particle tunneling model. Our numerical results show that: (i) when the tunneling current is small, due to either a large tunneling thickness (≥ 2 atomic layers of BN) or a small coherence length, the voltage distributions along the graphene electrodes have almostmore » zero variations upon including these distributed effects, (ii) when the tunnel current is large, due to either a small tunneling thickness (∼ 1 atomic layer of BN) or due to a large coherence length, the local voltage distributions along the graphene electrodes become appreciable and the device behavior deviates from that predicted by a 1-D approximation. These effects, which are not captured in one-dimensional SymFET models, can provide a better understanding about the electron dynamics in the device and might indicate potential novel applications for this proposed device.« less

Structure and cation ordering in La 2UO 6, Ce 2UO 6, LaUO 4, and CeUO 4 by first principles calculations

DOE PAGES

Casillas-Trujillo, Luis; Xu, H.; McMurray, Jake W.; ...

2016-07-06

In the present work, we have used density functional theory (DFT) and DFT+U to investigate the crystal structure and phase stability of four model compounds in the Ln 2O 3-UO 2-UO 3 ternary oxide system: La2UO 6, Ce 2UO 6, LaUO 4, CeUO 4, due to the highly-correlated nature of the f-electrons in uranium. We have considered both hypothetical ordered compounds and compounds in which the cations randomly occupy atomic sites in a fluorite-like lattice. We determined that ordered compounds are stable and are energetically favored compared to disordered configurations, though the ordering tendencies are weak. To model and analyzemore » the structures of these complex oxides, we have used supercells based on a layered atomic model. In the layer model, the supercell is composed of alternating planes of anions and cations. We have considered two different ordering motifs for the cations, namely single species (isoatomic) cation layers versus mixed species cation layers. Energy differences between various ordered cationic arrangements were found to be small. This may have implications regarding radiation stability, since cationic arrangements should be able to change under irradiation with little cost in energy.« less

A benchmark of co-flow and cyclic deposition/etch approaches for the selective epitaxial growth of tensile-strained Si:P

NASA Astrophysics Data System (ADS)

Hartmann, J. M.; Veillerot, M.; Prévitali, B.

2017-10-01

We have compared co-flow and cyclic deposition/etch processes for the selective epitaxial growth of Si:P layers. High growth rates, relatively low resistivities and significant amounts of tensile strain (up to 10 nm min-1, 0.55 mOhm cm and a strain equivalent to 1.06% of substitutional C in Si:C layers) were obtained at 700 °C, 760 Torr with a co-flow approach and a SiH2Cl2 + PH3 + HCl chemistry. This approach was successfully used to thicken the sources and drains regions of n-type fin-shaped Field Effect Transistors. Meanwhile, the (Si2H6 + PH3/HCl + GeH4) CDE process evaluated yielded at 600 °C, 80 Torr even lower resistivities (0.4 mOhm cm, typically), at the cost however of the tensile strain which was lost due to (i) the incorporation of Ge atoms (1.5%, typically) into the lattice during the selective etch steps and (ii) a reduction by a factor of two of the P atomic concentration in CDE layers compared to that in layers grown in a single step (5 × 1020 cm-3 compared to 1021 cm-3).

Buckling reversal of the Si(111) bilayer termination of 2-dimensional ErSi2 upon H dosing

NASA Astrophysics Data System (ADS)

Wetzel, P.; Pirri, C.; Gewinner, G.

1997-05-01

Hydrogen-induced reconstruction of 2-dimensional (2D) ErSi2 epitaxially grown on Si(111) is studied by Auger-electron diffraction (AED) and low-energy electron diffraction (LEED). The intensity of the Er MNN Auger line is measured vs. polar angle along the [1 - 2 1] and [- 1 2 - 1] azimuths for clean and H-saturated (1 × 1) ErSi2 silicides. The atomic structure of clean 2D silicide, previously established by AED as well as other techniques, consists of a hexagonal monolayer of Er located underneath a buckled Si layer comparable to the Si(111) substrate double layers. Moreover, for clean 2D ErSi2 only the B-type orientation is observed, i.e. the buckled Si top layer is always rotated by 180° around the surface normal relative to the relevant double layers of the substrate. After atomic H saturation, AED reveals drastic changes in the silicide structure involving a major most remarkable reconstruction of the Si bilayer termination. The latter is found to switch from B-type to A-type orientation upon H dosing, i.e. H-saturated 2D ErSi2 exhibits a buckled Si top layer oriented in the same way as the substrate double layers. A comparison with single scattering cluster simulations demonstrates that the latter phenomenon is accompanied by a large expansion of the Er-Si interlayer spacing close to 0.3 Å.

Exciton Dynamics, Transport, and Annihilation in Atomically Thin Two-Dimensional Semiconductors.

PubMed

Yuan, Long; Wang, Ti; Zhu, Tong; Zhou, Mingwei; Huang, Libai

2017-07-20

Large binding energy and unique exciton fine structure make the transition metal dichalcogenides (TMDCs) an ideal platform to study exciton behaviors in two-dimensional (2D) systems. While excitons in these systems have been extensively researched, there currently lacks a consensus on mechanisms that control dynamics. In this Perspective, we discuss extrinsic and intrinsic factors in exciton dynamics, transport, and annihilation in 2D TMDCs. Intrinsically, dark and bright exciton energy splitting is likely to play a key role in modulating the dynamics. Extrinsically, defect scattering is prevalent in single-layer TMDCs, which leads to rapid picosecond decay and limits exciton transport. The exciton-exciton annihilation process in single-layer TMDCs is highly efficient, playing an important role in the nonradiative recombination rate in the high exciton density regime. Future challenges and opportunities to control exciton dynamics are discussed.

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

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

Cooling without contact in bilayer dipolar Fermi gases

NASA Astrophysics Data System (ADS)

Tanatar, Bilal; Renklioglu, Basak; Oktel, M. Ozgur

2016-05-01

We consider two parallel layers of dipolar ultracold Fermi gases at different temperatures and calculate the heat transfer between them. The effective interactions describing screening and correlation effects between the dipoles in a single layer are modelled within the Euler-Lagrange Fermi-hypernetted chain approximation. The random-phase approximation is employed for the interactions across the layers. We investigate the amount of transferred power between the layers as a function of the temperature difference. Energy transfer proceeds via the long-range dipole-dipole interactions. A simple thermal model is developed to investigate the feasibility of using the contactless sympathetic cooling of the ultracold polar atoms/molecules. Our calculations indicate that dipolar heat transfer is effective for typical polar molecule experiments and may be utilized as a cooling process. Supported by TUBA and TUBITAK (112T974).

Extracting elastic properties of an atomically thin interfacial layer by time-domain analysis of femtosecond acoustics

NASA Astrophysics Data System (ADS)

Chen, H.-Y.; Huang, Y.-R.; Shih, H.-Y.; Chen, M.-J.; Sheu, J.-K.; Sun, C.-K.

2017-11-01

Modern devices adopting denser designs and complex 3D structures have created much more interfaces than before, where atomically thin interfacial layers could form. However, fundamental information such as the elastic property of the interfacial layers is hard to measure. The elastic property of the interfacial layer is of great importance in both thermal management and nano-engineering of modern devices. Appropriate techniques to probe the elastic properties of interfacial layers as thin as only several atoms are thus critically needed. In this work, we demonstrated the feasibility of utilizing the time-resolved femtosecond acoustics technique to extract the elastic properties and mass density of a 1.85-nm-thick interfacial layer, with the aid of transmission electron microscopy. We believe that this femtosecond acoustics approach will provide a strategy to measure the absolute elastic properties of atomically thin interfacial layers.

Triangular lattice atomic layer of Sn(1 × 1) at graphene/SiC(0001) interface

NASA Astrophysics Data System (ADS)

Hayashi, Shingo; Visikovskiy, Anton; Kajiwara, Takashi; Iimori, Takushi; Shirasawa, Tetsuroh; Nakastuji, Kan; Miyamachi, Toshio; Nakashima, Shuhei; Yaji, Koichiro; Mase, Kazuhiko; Komori, Fumio; Tanaka, Satoru

2018-01-01

Sn atomic layers attract considerable interest owing to their spin-related physical properties caused by their strong spin-orbit interactions. We performed Sn intercalation into the graphene/SiC(0001) interface and found a new type of Sn atomic layer. Sn atoms occupy on-top sites of Si-terminated SiC(0001) with in-plane Sn-Sn bondings, resulting in a triangular lattice. Angle-resolved photoemission spectroscopy revealed characteristic dispersions at \\bar{\\text{K}} and \\bar{\\text{M}} points, which agreed well with density functional theory calculations. The Sn triangular lattice atomic layer at the interface showed no oxidation upon exposure to air, which is useful for characterization and device fabrication ex situ.

Single-layer 1T‧-MoS2 under electron irradiation from ab initio molecular dynamics

NASA Astrophysics Data System (ADS)

Pizzochero, Michele; Yazyev, Oleg V.

2018-04-01

Irradiation with high-energy particles has recently emerged as an effective tool for tailoring the properties of two-dimensional transition metal dichalcogenides. In order to carry out an atomically-precise manipulation of the lattice, a detailed understanding of the beam-induced events occurring at the atomic scale is necessary. Here, we investigate the response of 1T' -MoS2 to the electron irradiation by ab initio molecular dynamics means. Our simulations suggest that an electron beam with energy smaller than 75 keV does not result in any knock-on damage. The displacement threshold energies are different for the two nonequivalent sulfur atoms in 1T' -MoS2 and strongly depend on whether the top or bottom chalcogen layer is considered. As a result, a careful tuning of the beam energy can promote the formation of ordered defects in the sample. We further discuss the effect of the electron irradiation in the neighborhood of a defective site, the mobility of the sulfur vacancies created and their tendency to aggregate. Overall, our work provides useful guidelines for the imaging and the defect engineering of 1T' -MoS2 using electron microscopy.

Hydrogen-induced structural transition in single layer ReS2

NASA Astrophysics Data System (ADS)

Yagmurcukardes, M.; Bacaksiz, C.; Senger, R. T.; Sahin, H.

2017-09-01

By performing density functional theory-based calculations, we investigate how structural, electronic and mechanical properties of single layer ReS2 can be tuned upon hydrogenation of its surfaces. It is found that a stable, fully hydrogenated structure can be obtained by formation of strong S-H bonds. The optimized atomic structure of ReS2H2 is considerably different than that of the monolayer ReS2 which has a distorted-1T phase. By performing phonon dispersion calculations, we also predict that the Re2-dimerized 1T structure (called 1T {{}\\text{R{{\\text{e}}2}}} ) of the ReS2H2 is dynamically stable. Unlike the bare ReS2 the 1T {{}\\text{R{{\\text{e}}2}}} -ReS2H2 structure which is formed by breaking the Re4 clusters into separated Re2 dimers, is an indirect-gap semiconductor. Furthermore, mechanical properties of the 1T {{}\\text{R{{\\text{e}}2}}} phase in terms of elastic constants, in-plane stiffness (C) and Poisson ratio (ν) are investigated. It is found that full hydrogenation not only enhances the flexibility of the single layer ReS2 crystal but also increases anisotropy of the elastic constants.

Coated armor system and process for making the same

DOEpatents

Chu, Henry S.; Lillo, Thomas M.; McHugh, Kevin M.

2010-11-23

An armor system and method involves providing a core material and a stream of atomized coating material that comprises a liquid fraction and a solid fraction. An initial layer is deposited on the core material by positioning the core material in the stream of atomized coating material wherein the solid fraction of the stream of atomized coating material is less than the liquid fraction of the stream of atomized coating material on a weight basis. An outer layer is then deposited on the initial layer by positioning the core material in the stream of atomized coating material wherein the solid fraction of the stream of atomized coating material is greater than the liquid fraction of the stream of atomized coating material on a weight basis.

Armor systems including coated core materials

DOEpatents

Chu, Henry S [Idaho Falls, ID; Lillo, Thomas M [Idaho Falls, ID; McHugh, Kevin M [Idaho Falls, ID

2012-07-31

An armor system and method involves providing a core material and a stream of atomized coating material that comprises a liquid fraction and a solid fraction. An initial layer is deposited on the core material by positioning the core material in the stream of atomized coating material wherein the solid fraction of the stream of atomized coating material is less than the liquid fraction of the stream of atomized coating material on a weight basis. An outer layer is then deposited on the initial layer by positioning the core material in the stream of atomized coating material wherein the solid fraction of the stream of atomized coating material is greater than the liquid fraction of the stream of atomized coating material on a weight basis.

Armor systems including coated core materials

DOEpatents

Chu, Henry S; Lillo, Thomas M; McHugh, Kevin M

2013-10-08

An armor system and method involves providing a core material and a stream of atomized coating material that comprises a liquid fraction and a solid fraction. An initial layer is deposited on the core material by positioning the core material in the stream of atomized coating material wherein the solid fraction of the stream of atomized coating material is less than the liquid fraction of the stream of atomized coating material on a weight basis. An outer layer is then deposited on the initial layer by positioning the core material in the stream of atomized coating material wherein the solid fraction of the stream of atomized coating material is greater than the liquid fraction of the stream of atomized coating material on a weight basis.

Atom Probe Tomography Analysis of Ag Doping in 2D Layered Material (PbSe) 5(Bi 2Se 3) 3

DOE PAGES

Ren, Xiaochen; Singh, Arunima K.; Fang, Lei; ...

2016-09-07

Impurity doping in two-dimensional (2D) materials can provide a route to tuning electronic properties, so it is important to be able to determine the distribution of dopant atoms within and between layers. Here we report the totnographic mapping of dopants in layered 2D materials with atomic sensitivity and subnanometer spatial resolution using atom, probe tomography (APT). Also, APT analysis shows that Ag dopes both Bi 2Se 3 and PbSe layers in (PbSe) 5(Bi 2Se 3) 3, and correlations :in the position of Ag atoms suggest a pairing across neighboring Bi 2Se 3 and PbSe layers. Finally, density functional theory (DFT)more » calculations confirm the favorability of substitutional-doping for both Pb and Bi and provide insights into the,observed spatial correlations in dopant locations.« less

Atomic Oxygen Durability of Second Surface Silver Microsheet Glass Concentrators

NASA Technical Reports Server (NTRS)

deGroh, Kim K.; Jaworske, Donald A.; Smith, Daniela C.; Mroz, Thaddeus S.

1996-01-01

Second surface silver microsheet glass concentrators are being developed for potential use in future solar dynamic space power systems. Traditional concentrators are aluminum honeycomb sandwich composites with either aluminum or graphite epoxy face sheets, where a reflective aluminum layer is deposited onto an organic leveling layer on the face sheet. To protect the underlying layers, a SiO2 layer is applied on top of the aluminum reflective layer. These concentrators may be vulnerable to atomic oxygen degradation due to possible atomic oxygen attack of the organic layers at defect sites in the protective and reflective coatings. A second surface microsheet glass concentrator would be inherently more atomic oxygen durable than these first surface concentrators. In addition, a second surface microsheet glass concentrator design provides a smooth optical surface and allows for silver to be used as a reflective layer, which would improve the reflectivity of the concentrator and the performance of the system. A potential threat to the performance of second surface microsheet glass concentrators is atomic oxygen attack of the underlying silver at seams and edges or at micrometeoroid and debris (MMD) impacts sites. Second surface silver microsheet glass concentrator samples were fabricated and tested for atomic oxygen durability. The samples were iteratively exposed to an atomic oxygen environment in a plasma asher. Samples were evaluated for potential degradation at fabrication seams, simulated MMD impact sites, and edges. Optical microscopy was used to evaluate atomic oxygen degradation. Reflectance was obtained for an impacted sample prior to and after atomic oxygen exposure. After an initial atomic oxygen exposure to an effective fluence of approx. 1 x 10(exp 21) atoms/cm(exp 2), oxidation of the silver at defect sites and edges was observed. Exposure to an additional approx. 1 x 10(exp 21) atoms/cm(exp 2) caused no observed increase in oxidation. Oxidation at an impact site caused negligible changes in reflectance. In all cases oxidation was found to be confined to the vicinity of the seams, impact sites, edges or defect sites. Asher to in-space atomic oxygen correlation issues will be addressed.

Effects of nitrogen incorporation in HfO(2) grown on InP by atomic layer deposition: an evolution in structural, chemical, and electrical characteristics.

PubMed

Kang, Yu-Seon; Kim, Dae-Kyoung; Kang, Hang-Kyu; Jeong, Kwang-Sik; Cho, Mann-Ho; Ko, Dae-Hong; Kim, Hyoungsub; Seo, Jung-Hye; Kim, Dong-Chan

2014-03-26

We investigated the effects of postnitridation on the structural characteristics and interfacial reactions of HfO2 thin films grown on InP by atomic layer deposition (ALD) as a function of film thickness. By postdeposition annealing under NH3 vapor (PDN) at 600 °C, an InN layer formed at the HfO2/InP interface, and ionized NHx was incorporated in the HfO2 film. We demonstrate that structural changes resulting from nitridation of HfO2/InP depend on the film thickness (i.e., a single-crystal interfacial layer of h-InN formed at thin (2 nm) HfO2/InP interfaces, whereas an amorphous InN layer formed at thick (>6 nm) HfO2/InP interfaces). Consequently, the tetragonal structure of HfO2 transformed into a mixture structure of tetragonal and monoclinic because the interfacial InN layer relieved interfacial strain between HfO2 and InP. During postdeposition annealing (PDA) in HfO2/InP at 600 °C, large numbers of oxidation states were generated as a result of interfacial reactions between interdiffused oxygen impurities and out-diffused InP substrate elements. However, in the case of the PDN of HfO2/InP structures at 600 °C, nitrogen incorporation in the HfO2 film effectively blocked the out-diffusion of atomic In and P, thus suppressing the formation of oxidation states. Accordingly, the number of interfacial defect states (Dit) within the band gap of InP was significantly reduced, which was also supported by DFT calculations. Interfacial InN in HfO2/InP increased the electron-barrier height to ∼0.6 eV, which led to low-leakage-current density in the gate voltage region over 2 V.

Surface passivation investigation on ultra-thin atomic layer deposited aluminum oxide layers for their potential application to form tunnel layer passivated contacts

NASA Astrophysics Data System (ADS)

Xin, Zheng; Ling, Zhi Peng; Nandakumar, Naomi; Kaur, Gurleen; Ke, Cangming; Liao, Baochen; Aberle, Armin G.; Stangl, Rolf

2017-08-01

The surface passivation performance of atomic layer deposited ultra-thin aluminium oxide layers with different thickness in the tunnel layer regime, i.e., ranging from one atomic cycle (∼0.13 nm) to 11 atomic cycles (∼1.5 nm) on n-type silicon wafers is studied. The effect of thickness and thermal activation on passivation performance is investigated with corona-voltage metrology to measure the interface defect density D it(E) and the total interface charge Q tot. Furthermore, the bonding configuration variation of the AlO x films under various post-deposition thermal activation conditions is analyzed by Fourier transform infrared spectroscopy. Additionally, poly(3,4-ethylenedioxythiophene) poly(styrene sulfonate) is used as capping layer on ultra-thin AlO x tunneling layers to further reduce the surface recombination current density to values as low as 42 fA/cm2. This work is a useful reference for using ultra-thin ALD AlO x layers as tunnel layers in order to form hole selective passivated contacts for silicon solar cells.

Microstructure and properties of single crystal BaTiO3 thin films synthesized by ion implantation-induced layer transfer

NASA Astrophysics Data System (ADS)

Park, Young-Bae; Ruglovsky, Jennifer L.; Atwater, Harry A.

2004-07-01

Single crystal BaTiO3 thin films have been transferred onto Pt-coated and Si3N4-coated substrates by the ion implantation-induced layer transfer method using H + and He+ ion coimplantation and subsequent annealing. The transferred BaTiO3 films are single crystalline with root mean square roughness of 17nm. Polarized optical and piezoresponse force microscopy (PFM) indicate that the BaTiO3 film domain structure closely resembles that of bulk tetragonal BaTiO3 and atomic force microscopy shows a 90° a -c domain structure with a tetragonal angle of 0.5°-0.6°. Micro-Raman spectroscopy indicates that the local mode intensity is degraded in implanted BaTiO3 but recovers during anneals above the Curie temperature. The piezoelectric coefficient, d33, is estimated from PFM to be 80-100pm/V and the coercive electric field (Ec) is 12-20kV/cm, comparable to those in single crystal BaTiO3.

Electrochemical, Structural and Magnetic Analysis of Electrodeposited CoCu/Cu Multilayers: Influence of Cu Layer Deposition Potential

NASA Astrophysics Data System (ADS)

Tekgül, Atakan; Kockar, Hakan; Kuru, Hilal; Alper, Mürsel; ÜnlÜ, C. Gökhan

2018-03-01

The electrochemical, structural and magnetic properties of CoCu/Cu multilayers electrodeposited at different cathode potentials were investigated from a single bath. The Cu layer deposition potentials were selected as - 0.3, V - 0.4 V, and - 0.5 V with respect to saturated calomel electrode (SCE) while the Co layer deposition potential was constant at - 1.5 V versus SCE. For the electrochemical analysis, the current-time transients were obtained. The amount of noble non-magnetic (Cu) metal materials decreased with the increase of deposition potentials due to anomalous codeposition. Further, current-time transient curves for the Co layer deposition and capacitance were calculated. In the structural analysis, the multilayers were found to be polycrystalline with both Co and Cu layers adopting the face-centered cubic structure. The (111) peak shifts towards higher angle with the increase of the deposition potentials. Also, the lattice parameters of the multilayers decrease from 0.3669 nm to 0.3610 nm with the increase of the deposition potentials from - 0.3 V to - 0.5 V, which corresponds to the bulk values of Cu and Co, respectively. The electrochemical and structural results demonstrate that the amount of Co atoms increased and the Cu atoms decreased in the layers with the increase of deposition potentials due to anomalous codeposition. For magnetic measurements, the saturation magnetizations, M_s obtained from the magnetic curves of the multilayers were obtained as 212 kA/m, 276 kA/m, and 366 kA/m with - 0.3 V, - 0.4 V, and - 0.5 V versus SCE, respectively. It is seen that the M_s values increased with the increase of the deposition potentials confirming the increase of the Co atoms and decrease of the Cu amount. The results of electrochemical and structural analysis show that the deposition potentials of non-magnetic layers plays important role on the amount of magnetic and non-magnetic materials in the layers and thus on the magnetic properties of the multilayers.

Atomic hydrogen storage method and apparatus

NASA Technical Reports Server (NTRS)

Woollam, J. A. (Inventor)

1978-01-01

Atomic hydrogen, for use as a fuel or as an explosive, is stored in the presence of a strong magnetic field in exfoliated layered compounds such as molybdenum disulfide or an elemental layer material such as graphite. The compound is maintained at liquid helium temperatures and the atomic hydrogen is collected on the surfaces of the layered compound which are exposed during delamination (exfoliation). The strong magnetic field and the low temperature combine to prevent the atoms of hydrogen from recombining to form molecules.

Atomic hydrogen storage method and apparatus

NASA Technical Reports Server (NTRS)

Woollam, J. A. (Inventor)

1980-01-01

Atomic hydrogen, for use as a fuel or as an explosive, is stored in the presence of a strong magnetic field in exfoliated layered compounds such as molybdenum disulfide or an elemental layer material such as graphite. The compounds maintained at liquid helium temperatures and the atomic hydrogen is collected on the surfaces of the layered compound which are exposed during delamination (exfoliation). The strong magnetic field and the low temperature combine to prevent the atoms of hydrogen from recombining to form molecules.

Atomic hydrogen storage. [cryotrapping and magnetic field strength

NASA Technical Reports Server (NTRS)

Woollam, J. A. (Inventor)

1980-01-01

Atomic hydrogen, for use as a fuel or as an explosive, is stored in the presence of a strong magnetic field in exfoliated layered compounds such as molybdenum disulfide or an elemental layer material such as graphite. The compound is maintained at liquid temperatures and the atomic hydrogen is collected on the surfaces of the layered compound which are exposed during delamination (exfoliation). The strong magnetic field and the low temperature combine to prevent the atoms of hydrogen from recombining to form molecules.

Superconducting and Magnetic Properties of Vanadium/iron Superlattices.

NASA Astrophysics Data System (ADS)

Wong, Hong-Kuen

A novel ultrahigh vacuum evaporator was constructed for the preparation of superlattice samples. The thickness control was much better than an atomic plane. With this evaporator we prepared V/Fe superlattice samples on (0001) sapphire substrates with different thicknesses. All samples showed a good bcc(110) structure. Mossbauer experiments showed that the interface mixing extended a distance of about one atomic plane indicating an almost rectangular composition profile. Because of this we were able to prepare samples with layer thickness approaching one atomic plane. Even with ultrathin Fe layers, the samples are ferromagnetic, at least at lower temperatures. Superparamagnetism and spin glass states were not seen. In the absence of an external field, the magnetic moments lie close to the film plane. In addition to this shape anisotropy, there is some uniaxial anisotropy. No magnetic dead layers have been observed. The magnetic moments within the Fe layers vary little with the distance from the interfaces. At the interfaces the Fe moment is reduced and an antiparallel moment is induced on the vanadium atoms. It is observed that ultrathin Fe layers behave in a 2D fashion when isolated by sufficiently thick vanadium layers; however, on thinning the vanadium layers, a magnetic coupling between the Fe layers has been observed. We also studied the superconducting properties of V/Fe sandwiches and superlattices. In both cases, the Fe layer, a strong pair-breaker, suppresses the superconducting transition temperature consistent with the current knowledge of the magnetic proximity effect. For the sandwiches with thin (thick) vanadium layers, the temperature dependence of the upper critical fields is consistent with the simple theory for a 2D (3D) superconductor. For the superlattices, when the vanadium layer is on the order of the BCS coherence length and the Fe layer is only a few atomic planes thick, a 2D-3D crossover has been observed in the temperature dependence of the parallel upper critical field. This implies the coexistence of superconductivity and ferromagnetism. We observe three dimensional behavior for thinner Fe layers ((TURN)1 atomic plane) and two dimensional behavior for thicker Fe layers (greater than 10 atomic planes).

Crystalline boron nitride aerogels

DOEpatents

Zettl, Alexander K.; Rousseas, Michael; Goldstein, Anna P.; Mickelson, William; Worsley, Marcus A.; Woo, Leta

2017-04-04

This disclosure provides methods and materials related to boron nitride aerogels. In one aspect, a material comprises an aerogel comprising boron nitride. The boron nitride has an ordered crystalline structure. The ordered crystalline structure may include atomic layers of hexagonal boron nitride lying on top of one another, with atoms contained in a first layer being superimposed on atoms contained in a second layer.

Radical Beam Gettering Epitaxy of Zno and Gan

NASA Astrophysics Data System (ADS)

Georgobiani, A. N.; Demin, V. I.; Vorobiev, M. O.; Gruzintsev, A. N.; Hodos, I. I.; Kotljarevsky, M. B.; Kidalov, V. V.; Rogozin, I. V.

2002-11-01

P-type ZnO layers with a hole mobility about 23 cm2/(V s), and a hole concentration about 1015 cm-3 were grown by means of radical-beam gettering epitaxy (the annealing of n-ZnO single crystals in atomic oxygen flux). The effect of native defects on the photoluminescence spectra of the layers was studied. The dominant bands in the spectra peaked at 370.2 and 400 nm. These bands were attributed to the annihilation of exciton localised on neutral Vzn and to electron transitions from the conduction band to singly positively charged Vzn correspondingly. The effect of annealing in atomic nitrogen flux of p-CaN:Mg films on their photoluminescence spectra and on the value of their conductivity were studied. Such annealing leads to appearance of a number of emission bands that peaked at 404.9, 390.8 and 378.9 nm and increases hole concentration from 5 × 1015 to 5 × 1016 cm-3, and the hole mobility from 120 to 150 cm2/(V s). The n-ZnO - p-GaN:Mg electroluminescence heterostructures were obtained. Their spectrum contains bands in the excitonic region of GaN at the wavelength 360.2 nm and in the edge region at wavelengths 378.9 and 390.8 nm.

Ortho and para hydrogen dimers on G/SiC(0001): combined STM and DFT study.

PubMed

Merino, P; Švec, M; Martínez, J I; Mutombo, P; Gonzalez, C; Martín-Gago, J A; de Andres, P L; Jelinek, P

2015-01-01

The hydrogen (H) dimer structures formed upon room-temperature H adsorption on single layer graphene (SLG) grown on SiC(0001) are addressed using a combined theoretical-experimental approach. Our study includes density functional theory (DFT) calculations for the full (6√3 × 6√3)R30° unit cell of the SLG/SiC(0001) substrate and atomically resolved scanning tunneling microscopy images determining simultaneously the graphene lattice and the internal structure of the H adsorbates. We show that H atoms normally group in chemisorbed coupled structures of different sizes and orientations. We make an atomic scale determination of the most stable experimental geometries, the small dimers and ellipsoid-shaped features, and we assign them to hydrogen adsorbed in para dimers and ortho dimers configuration, respectively, through comparison with the theory.

Atomic-Layer-Confined Doping for Atomic-Level Insights into Visible-Light Water Splitting.

PubMed

Lei, Fengcai; Zhang, Lei; Sun, Yongfu; Liang, Liang; Liu, Katong; Xu, Jiaqi; Zhang, Qun; Pan, Bicai; Luo, Yi; Xie, Yi

2015-08-03

A model of doping confined in atomic layers is proposed for atomic-level insights into the effect of doping on photocatalysis. Co doping confined in three atomic layers of In2S3 was implemented with a lamellar hybrid intermediate strategy. Density functional calculations reveal that the introduction of Co ions brings about several new energy levels and increased density of states at the conduction band minimum, leading to sharply increased visible-light absorption and three times higher carrier concentration. Ultrafast transient absorption spectroscopy reveals that the electron transfer time of about 1.6 ps from the valence band to newly formed localized states is due to Co doping. The 25-fold increase in average recovery lifetime is believed to be responsible for the increased of electron-hole separation. The synthesized Co-doped In2S3 (three atomic layers) yield a photocurrent of 1.17 mA cm(-2) at 1.5 V vs. RHE, nearly 10 and 17 times higher than that of the perfect In2S3 (three atomic layers) and the bulk counterpart, respectively. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Ultrafast Optical Microscopy of Single Monolayer Molybdenum Disulfide Flakes

DOE PAGES

Seo, Minah; Yamaguchi, Hisato; Mohite, Aditya D.; ...

2016-02-15

We performed ultrafast optical microscopy on single flakes of atomically thin CVD-grown molybdenum disulfide, using non-degenerate femtosecond pump-probe spectroscopy to excite and probe carriers above and below the indirect and direct band gaps. These measurements reveal the influence of layer thickness on carrier dynamics when probing near the band gap. Furthermore, fluence-dependent measurements indicate that carrier relaxation is primarily influenced by surface-related defect and trap states after above-bandgap photoexcitation. Furthermore, the ability to probe femtosecond carrier dynamics in individual flakes can thus give much insight into light-matter interactions in these two-dimensional nanosystems.

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

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.

First-principles study of Ti intercalation between graphene and Au surface

NASA Astrophysics Data System (ADS)

Kaneko, T.; Imamura, H.

2011-06-01

We investigate the effects of Ti intercalation between graphene and Au surface on binding energy and charge doping by using the first-principles calculations. We show that the largest binding energy is realized by the intercalation of single mono-layer of Ti. We also show that electronic structure is very sensitive to the arrangement of metal atoms at the interface. If the composition of the interface layer is Ti0.33Au0.67 and the Ti is located at the top site, the Fermi level lies closely at the Dirac point, i.e., the Dirac cone of the ideal free-standing graphene is recovered.

Numerical study of electronic impact and radiation in sonoluminescence

NASA Astrophysics Data System (ADS)

Xu, Ning; Wang, Long; Hu, Xiwei

1998-02-01

A hydrodynamic simulation of pure argon single-bubble sonoluminescence including electron collisional ionization, recombination, and radiative energy loss has been performed. We find that near the moment that the bubble reaches its minimum radius the atoms inside a very thin layer around the origin of the bubble are strongly ionized, and the light emission occurs nearly simultaneously. Therefore we conclude that multiple ionization and recombination, which mainly occur in the thin layer of plasma, play a dramatically important role in the noble gas sonoluminescence. We also find that the temperature and the intensity of luminescence are not so high as those predicted by previous models, which consider only neutral gases.

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

Hong, Seung Sae; Yu, Jung Ho; Lu, Di

Long-range order and phase transitions in two-dimensional (2D) systems—such as magnetism, superconductivity, and crystallinity—have been important research topics for decades. The issue of 2D crystalline order has reemerged recently, with the development of exfoliated atomic crystals. Understanding the dimensional limit of crystalline phases, with different types of bonding and synthetic techniques, is at the foundation of low-dimensional materials design. We study ultrathin membranes of SrTiO 3, an archetypal perovskite oxide with isotropic (3D) bonding. Atomically controlled membranes are released after synthesis by dissolving an underlying epitaxial layer. Although all unreleased films are initially single-crystalline, the SrTiO 3 membrane lattice collapsesmore » below a critical thickness (5 unit cells). This crossover from algebraic to exponential decay of the crystalline coherence length is analogous to the 2D topological Berezinskii-Kosterlitz-Thouless (BKT) transition. Finally, the transition is likely driven by chemical bond breaking at the 2D layer-3D bulk interface, defining an effective dimensional phase boundary for coherent crystalline lattices.« less

Theoretical aspects of studies of oxide and semiconductor surfaces using low energy positrons

NASA Astrophysics Data System (ADS)

Fazleev, N. G.; Maddox, W. B.; Weiss, A. H.

2011-01-01

This paper presents the results of a theoretical study of positron surface and bulk states and annihilation characteristics of surface trapped positrons at the oxidized Cu(100) single crystal and at both As- and Ga-rich reconstructed GaAs(100) surfaces. The variations in atomic structure and chemical composition of the topmost layers of the surfaces associated with oxidation and reconstructions and the charge redistribution at the surfaces are found to affect localization and spatial extent of the positron surface-state wave functions. The computed positron binding energy, work function, and annihilation characteristics reveal their sensitivity to charge transfer effects, atomic structure and chemical composition of the topmost layers of the surfaces. Theoretical positron annihilation probabilities with relevant core electrons computed for the oxidized Cu(100) surface and the As- and Ga-rich reconstructed GaAs(100) surfaces are compared with experimental ones estimated from the positron annihilation induced Auger peak intensities measured from these surfaces.

Soft chemical synthesis of silicon nanosheets and their applications

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

Nakano, Hideyuki; Ikuno, Takashi

2016-12-15

Two-dimensional silicon nanomaterials are expected to show different properties from those of bulk silicon materials by virtue of surface functionalization and quantum size effects. Since facile fabrication processes of large area silicon nanosheets (SiNSs) are required for practical applications, a development of soft chemical synthesis route without using conventional vacuum processes is a challenging issue. We have recently succeeded to prepare SiNSs with sub-nanometer thicknesses by exfoliating layered silicon compounds, and they are found to be composed of crystalline single-atom-thick silicon layers. In this review, we present the synthesis and modification methods of SiNSs. These SiNSs have atomically flat andmore » smooth surfaces due to dense coverage of organic moieties, and they are easily self-assembled in a concentrated state to form a regularly stacked structure. We have also characterized the electron transport properties and the electronic structures of SiNSs. Finally, the potential applications of these SiNSs and organic modified SiNSs are also reviewed.« less

Thermal conductivity of Er{sup +3}:Y{sub 2}O{sub 3} films grown by atomic layer deposition

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

Raeisi Fard, Hafez; Hess, Andrew; Pashayi, Kamyar

2013-11-04

Cross-plane thermal conductivity of 800, 458, and 110 nm erbium-doped crystalline yttria (Er{sup +3}:Y{sub 2}O{sub 3}) films deposited via atomic layer deposition was measured using the 3ω method at room temperature. Thermal conductivity results show 16-fold increase in thermal conductivity from 0.49 W m{sup −1}K{sup −1} to 8 W m{sup −1}K{sup −1} upon post deposition annealing, partially due to the suppression of the number of the -OH/H{sub 2}O bonds in the films after annealing. Thermal conductivity of the annealed film was ∼70% lower than undoped bulk single crystal yttria. The cumulative interface thermal resistivity of substrate-Er{sup +3}:Y{sub 2}O{sub 3}-metal heater was determined tomore » be ∼2.5 × 10{sup −8} m{sup 2} K/W.« less

Effects of Substrate and Post-Growth Treatments on the Microstructure and Properties of ZnO Thin Films Prepared by Atomic Layer Deposition

NASA Astrophysics Data System (ADS)

Haseman, Micah; Saadatkia, P.; Winarski, D. J.; Selim, F. A.; Leedy, K. D.; Tetlak, S.; Look, D. C.; Anwand, W.; Wagner, A.

2016-12-01

Aluminum-doped zinc oxide (ZnO:Al) thin films were synthesized by atomic layer deposition on silicon, quartz and sapphire substrates and characterized by x-ray diffraction (XRD), high-resolution scanning electron microscopy, optical spectroscopy, conductivity mapping, Hall effect measurements and positron annihilation spectroscopy. XRD showed that the as-grown films are of single-phase ZnO wurtzite structure and do not contain any secondary or impurity phases. The type of substrate was found to affect the orientation and degree of crystallinity of the films but had no effect on the defect structure or the transport properties of the films. High conductivity of 10-3 Ω cm, electron mobility of 20 cm2/Vs and carrier density of 1020 cm-3 were measured in most films. Thermal treatments in various atmospheres induced a large effect on the thickness, structure and electrical properties of the films. Annealing in a Zn and nitrogen environment at 400°C for 1 h led to a 16% increase in the thickness of the film; this indicates that Zn extracts oxygen atoms from the matrix and forms new layers of ZnO. On the other hand, annealing in a hydrogen atmosphere led to the emergence of an Al2O3 peak in the XRD pattern, which implies that hydrogen and Al atoms compete to occupy Zn sites in the ZnO lattice. Only ambient air annealing had an effect on film defect density and electrical properties, generating reductions in conductivity and electron mobility. Depth-resolved measurements of positron annihilation spectroscopy revealed short positron diffusion lengths and high concentrations of defects in all as-grown films. However, these defects did not diminish the electrical conductivity in the films.

Two-dimensional antimonene single crystals grown by van der Waals epitaxy.

PubMed

Ji, Jianping; Song, Xiufeng; Liu, Jizi; Yan, Zhong; Huo, Chengxue; Zhang, Shengli; Su, Meng; Liao, Lei; Wang, Wenhui; Ni, Zhenhua; Hao, Yufeng; Zeng, Haibo

2016-11-15

Unlike the unstable black phosphorous, another two-dimensional group-VA material, antimonene, was recently predicted to exhibit good stability and remarkable physical properties. However, the synthesis of high-quality monolayer or few-layer antimonenes, sparsely reported, has greatly hindered the development of this new field. Here, we report the van der Waals epitaxy growth of few-layer antimonene monocrystalline polygons, their atomical microstructure and stability in ambient condition. The high-quality, few-layer antimonene monocrystalline polygons can be synthesized on various substrates, including flexible ones, via van der Waals epitaxy growth. Raman spectroscopy and transmission electron microscopy reveal that the obtained antimonene polygons have buckled rhombohedral atomic structure, consistent with the theoretically predicted most stable β-phase allotrope. The very high stability of antimonenes was observed after aging in air for 30 days. First-principle and molecular dynamics simulation results confirmed that compared with phosphorene, antimonene is less likely to be oxidized and possesses higher thermodynamic stability in oxygen atmosphere at room temperature. Moreover, antimonene polygons show high electrical conductivity up to 10 4  S m -1 and good optical transparency in the visible light range, promising in transparent conductive electrode applications.

Two-dimensional antimonene single crystals grown by van der Waals epitaxy

PubMed Central

Ji, Jianping; Song, Xiufeng; Liu, Jizi; Yan, Zhong; Huo, Chengxue; Zhang, Shengli; Su, Meng; Liao, Lei; Wang, Wenhui; Ni, Zhenhua; Hao, Yufeng; Zeng, Haibo

2016-01-01

Unlike the unstable black phosphorous, another two-dimensional group-VA material, antimonene, was recently predicted to exhibit good stability and remarkable physical properties. However, the synthesis of high-quality monolayer or few-layer antimonenes, sparsely reported, has greatly hindered the development of this new field. Here, we report the van der Waals epitaxy growth of few-layer antimonene monocrystalline polygons, their atomical microstructure and stability in ambient condition. The high-quality, few-layer antimonene monocrystalline polygons can be synthesized on various substrates, including flexible ones, via van der Waals epitaxy growth. Raman spectroscopy and transmission electron microscopy reveal that the obtained antimonene polygons have buckled rhombohedral atomic structure, consistent with the theoretically predicted most stable β-phase allotrope. The very high stability of antimonenes was observed after aging in air for 30 days. First-principle and molecular dynamics simulation results confirmed that compared with phosphorene, antimonene is less likely to be oxidized and possesses higher thermodynamic stability in oxygen atmosphere at room temperature. Moreover, antimonene polygons show high electrical conductivity up to 104 S m−1 and good optical transparency in the visible light range, promising in transparent conductive electrode applications. PMID:27845327

Phonon impedance matching: minimizing interfacial thermal resistance of thin films

NASA Astrophysics Data System (ADS)

Polanco, Carlos; Zhang, Jingjie; Ghosh, Avik

2014-03-01

The challenge to minimize interfacial thermal resistance is to allow a broad band spectrum of phonons, with non-linear dispersion and well defined translational and rotational symmetries, to cross the interface. We explain how to minimize this resistance using a frequency dependent broadening matrix that generalizes the notion of acoustic impedance to the whole phonon spectrum including symmetries. We show how to ``match'' two given materials by joining them with a single atomic layer, with a multilayer material and with a graded superlattice. Atomic layer ``matching'' requires a layer with a mass close to the arithmetic mean (or spring constant close to the harmonic mean) to favor high frequency phonon transmission. For multilayer ``matching,'' we want a material with a broadening close to the geometric mean to maximize transmission peaks. For graded superlattices, a continuous sequence of geometric means translates to an exponentially varying broadening that generates a wide-band antireflection coating for both the coherent and incoherent limits. Our results are supported by ``first principles'' calculations of thermal conductance for GaAs / Gax Al1 - x As / AlAs thin films using the Non-Equilibrium Greens Function formalism coupled with Density Functional Perturbation Theory. NSF-CAREER (QMHP 1028883), NSF-IDR (CBET 1134311), XSEDE.

Kinetic model for thin film stress including the effect of grain growth

NASA Astrophysics Data System (ADS)

Chason, Eric; Engwall, A. M.; Rao, Z.; Nishimura, T.

2018-05-01

Residual stress during thin film deposition is affected by the evolution of the microstructure. This can occur because subsurface grain growth directly induces stress in the film and because changing the grain size at the surface affects the stress in new layers as they are deposited. We describe a new model for stress evolution that includes both of these effects. It is used to explain stress in films that grow with extensive grain growth (referred to as zone II) so that the grain size changes throughout the thickness of the layer as the film grows. Equations are derived for different cases of high or low atomic mobility where different assumptions are used to describe the diffusion of atoms that are incorporated into the grain boundary. The model is applied to measurements of stress and grain growth in evaporated Ni films. A single set of model parameters is able to explain stress evolution in films grown at multiple temperatures and growth rates. The model explains why the slope of the curvature measurements changes continuously with thickness and attributes it to the effect of grain size on new layers deposited on the film.

Methods of producing armor systems, and armor systems produced using such methods

DOEpatents

Chu, Henry S; Lillo, Thomas M; McHugh, Kevin M

2013-02-19

An armor system and method involves providing a core material and a stream of atomized coating material that comprises a liquid fraction and a solid fraction. An initial layer is deposited on the core material by positioning the core material in the stream of atomized coating material wherein the solid fraction of the stream of atomized coating material is less than the liquid fraction of the stream of atomized coating material on a weight basis. An outer layer is then deposited on the initial layer by positioning the core material in the stream of atomized coating material wherein the solid fraction of the stream of atomized coating material is greater than the liquid fraction of the stream of atomized coating material on a weight basis.

Synthesis of layer-tunable graphene: A combined kinetic implantation and thermal ejection approach

DOE PAGES

Wang, Gang; Zhang, Miao; Liu, Su; ...

2015-05-04

Layer-tunable graphene has attracted broad interest for its potentials in nanoelectronics applications. However, synthesis of layer-tunable graphene by using traditional chemical vapor deposition (CVD) method still remains a great challenge due to the complex experimental parameters and the carbon precipitation process. Herein, by performing ion implantation into a Ni/Cu bilayer substrate, the number of graphene layers, especially single or double layer, can be controlled precisely by adjusting the carbon ion implant fluence. The growth mechanism of the layer-tunable graphene is revealed by monitoring the growth process is observed that the entire implanted carbon atoms can be expelled towards the substratemore » surface and thus graphene with designed layer number can be obtained. Such a growth mechanism is further confirmed by theoretical calculations. The proposed approach for the synthesis of layer-tunable graphene offers more flexibility in the experimental conditions. Being a core technology in microelectronics processing, ion implantation can be readily implemented in production lines and is expected to expedite the application of graphene to nanoelectronics.« less

A new nonlinear optical silicate carbonate K2Ca[Si2O5](CO3) with a hybrid structure of kalsilite and soda-like layered fragments

NASA Astrophysics Data System (ADS)

Belokoneva, Elena L.; Stefanovich, Sergey Yu.; Volkov, Anatoly S.; Dimitrova, Olga V.

2016-10-01

Single crystals of a new silicate carbonate, K2Ca[Si2O5](CO3), have been synthesized in a multi-components hydrothermal solution with a pH value close to neutral and a high concentration of a carbonate mineralizer. The new compound has an axial structure (s.g. P6322) with unit cell parameters a = 5.04789 (15), c = 17.8668 (6) Å. Pseudosymmetry of the structure corresponds to s.g. P63/mmc which is broken only by one oxygen position. The structure consists of two layered fragments: one of the type of the mineral kalsilite (KAlSiO4) and the other of the high-temperature soda-like α-Na2CO3, Ca substituting for Na. The electro-neutral layer K2[Si2O5] (denoted K) as well as the layer Ca(CO3) (denoted S) may separately correspond to individual structures. In K2Ca[Si2O5](CO3) the S-K layers are connected together via Ca-O interactions between Ca atoms from the carbonate layer and apical O atoms from the silicate one, and also via K-O interlayer interactions. A hypothetical acentric structure, sp.gr. P-62c, is predicted on the basis of the order-disorder theory. It presents another symmetrical option for the arrangement of K-layers relative to S-layers. The K,Ca-silicate-carbonate powder produces a moderate SHG signal that is two times larger that of the α-quartz powder standard and close to other silicates with acentric structures and low electronic polarizability.

Properties of Surface-Modification Layer Generated by Atomic Hydrogen Annealing on Poly(ethylene naphthalate) Substrate

NASA Astrophysics Data System (ADS)

Heya, Akira; Matsuo, Naoto

2008-01-01

The surface of a poly(ethylene naphthalate) (PEN) substrate was modified by atomic hydrogen annealing (AHA). In this method, a PEN substrate was exposed to atomic hydrogen generated by cracking hydrogen molecules on heated tungsten wire. The properties of the surface-modification layer by AHA were evaluated by spectroscopic ellipsometry. It is found that the thickness of the modified layer was 5 nm and that the modification layer has a low refractive index compared with the PEN substrate. The modification layer relates to the reduction reaction of the PEN substrate by AHA.

Atomic-order thermal nitridation of group IV semiconductors for ultra-large-scale integration

NASA Astrophysics Data System (ADS)

Murota, Junichi; Le Thanh, Vinh

2015-03-01

One of the main requirements for ultra-large-scale integration (ULSI) is atomic-order control of process technology. Our concept of atomically controlled processing for group IV semiconductors is based on atomic-order surface reaction control in Si-based CVD epitaxial growth. On the atomic-order surface nitridation of a few nm-thick Ge/about 4 nm-thick Si0.5Ge0.5/Si(100) by NH3, it is found that N atoms diffuse through nm-order thick Ge layer into Si0.5Ge0.5/Si(100) substrate and form Si nitride, even at 500 °C. By subsequent H2 heat treatment, although N atomic amount in Ge layer is reduced drastically, the reduction of the Si nitride is slight. It is suggested that N diffusion in Ge layer is suppressed by the formation of Si nitride and that Ge/atomic-order N layer/Si1-xGex/Si (100) heterostructure is formed. These results demonstrate the capability of CVD technology for atomically controlled nitridation of group IV semiconductors for ultra-large-scale integration. Invited talk at the 7th International Workshop on Advanced Materials Science and Nanotechnology IWAMSN2014, 2-6 November, 2014, Ha Long, Vietnam.

Pulsed-Plasma Physical Vapor Deposition Approach Toward the Facile Synthesis of Multilayer and Monolayer Graphene for Anticoagulation Applications.

PubMed

Vijayaraghavan, Rajani K; Gaman, Cezar; Jose, Bincy; McCoy, Anthony P; Cafolla, Tony; McNally, Patrick J; Daniels, Stephen

2016-02-01

We demonstrate the growth of multilayer and single-layer graphene on copper foil using bipolar pulsed direct current (DC) magnetron sputtering of a graphite target in pure argon atmosphere. Single-layer graphene (SG) and few-layer graphene (FLG) films are deposited at temperatures ranging from 700 °C to 920 °C within <30 min. We find that the deposition and post-deposition annealing temperatures influence the layer thickness and quality of the graphene films formed. The films were characterized using atomic force microscopy (AFM), scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), and optical transmission spectroscopy techniques. Based on the above studies, a diffusion-controlled mechanism was proposed for the graphene growth. A single-step whole blood assay was used to investigate the anticoagulant activity of graphene surfaces. Platelet adhesion, activation, and morphological changes on the graphene/glass surfaces, compared to bare glass, were analyzed using fluorescence microscopy and SEM techniques. We have found significant suppression of the platelet adhesion, activation, and aggregation on the graphene-covered surfaces, compared to the bare glass, indicating the anticoagulant activity of the deposited graphene films. Our production technique represents an industrially relevant method for the growth of SG and FLG for various applications including the biomedical field.

A theoretical study for mechanical contact between carbon nanotubes

NASA Astrophysics Data System (ADS)

Takagi, Yoshiteru; Uda, Tsuyoshi; Ohno, Takahisa

2005-03-01

We have theoretically investigated motions of single-walled carbon nanotubes (SWNTs) which are mounted on a flat substrate layer of SWNTs by tight-binding molecular dynamics simulations. One of the most interesting motions is the conversion of force and torque, where the force and torque acting initially on the mounted tube finally results in the lateral motion and rolling of the supporting tubes in the substrate. This motion is well understood in terms of the total energy surface of the SWNT/SWNT system. It is suggested that an undulation of the total energy surface plays a role as an atomic-scale gear tooth in the field of nanomechanics, in spite of the atomically smooth surface of SWNT.

Stability, resolution, and ultra-low wear amplitude modulation atomic force microscopy of DNA: Small amplitude small set-point imaging

NASA Astrophysics Data System (ADS)

Santos, Sergio; Barcons, Victor; Christenson, Hugo K.; Billingsley, Daniel J.; Bonass, William A.; Font, Josep; Thomson, Neil H.

2013-08-01

A way to operate fundamental mode amplitude modulation atomic force microscopy is introduced which optimizes stability and resolution for a given tip size and shows negligible tip wear over extended time periods (˜24 h). In small amplitude small set-point (SASS) imaging, the cantilever oscillates with sub-nanometer amplitudes in the proximity of the sample, without the requirement of using large drive forces, as the dynamics smoothly lead the tip to the surface through the water layer. SASS is demonstrated on single molecules of double-stranded DNA in ambient conditions where sharp silicon tips (R ˜ 2-5 nm) can resolve the right-handed double helix.

Calculated Properties of Fully Hydrogenated Single Layers of BN, BC2N, and Graphene: Graphane and Its BN-Containing Analogues

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

Averill, Frank; Morris, James R; Cooper, Valentino R

2009-01-01

Carbon is an attractive material for hydrogen adsorption, due to its light weight, variety of structures, and ability to both physisorb and chemisorb hydrogen. Recently, fully hydrogenated graphene layers ( graphane ) have been predicted to exist [J.O. Sofo et al., Phys. Rev. B 75, 15340 (2007)], and experimentally observed [D.C. Elias et al., Science 323, 610 (2009)]. In this work, we examine analogues of graphane, in particular BNH2 and BC2NH4. Unlike graphene, these materials have a band gap without hydrogenation. Our results indicate that the hydrogenation product of BN is metastable: the fully hydrogenated compound BNH2 is higher inmore » energy than hexagonal BN sheets plus H2 molecules, in sharp contrast with graphane. We find that BC2NH4 is energetically very close to hexagonal BC2N+2H2 molecules. Furthermore our examination of the relative binding strengths of rows of symmetry related hydrogen atoms on BC2NH4shows that this compound is marginally higher in energy than BC2NH2 plus an H2 molecule, with the hydrogen atoms in BC2NH2 absorbed on the carbon sites. These remaining hydrogen atoms are not as strongly bound as in graphane, indicating that the average hydrogen chemisorption energy is controllable by changing the carbon content in the B-C-N layer.« less

Characterization of plasma-enhanced atomic layer deposition of Al{sub 2}O{sub 3} using dimethylaluminum isopropoxide

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

Yang, Jialing; Eller, Brianna S.; Nemanich, Robert J.

2014-03-15

In this research, Al{sub 2}O{sub 3} films were grown by remote plasma-enhanced atomic layer deposition using a nonpyrophoric precursor, dimethylaluminum isopropoxide (DMAI), and oxygen plasma. After optimization, the growth rate was determined to be ∼1.5 Å/cycle within a growth window of 25–220 °C; the higher growth rate than reported for thermal atomic layer deposition was ascribed to the higher reactivity of the plasma species compared with H{sub 2}O and the adsorption of active oxygen at the surface, which was residual from the oxygen plasma exposure. Both effects enhance DMAI chemisorption and increase the saturation density. In addition, a longer oxygen plasma timemore » was required at room temperature to complete the reaction and decrease the carbon contamination below the detection limit of x-ray photoemission spectroscopy. The properties of the subsequent Al{sub 2}O{sub 3} films were measured for different temperatures. When deposited at 25 °C and 200 °C, the Al{sub 2}O{sub 3} films demonstrated a single Al-O bonding state as measured by x-ray photoemission spectroscopy, a similar band gap of 6.8±0.2 eV as determined by energy loss spectroscopy, a similar index of refraction of 1.62±0.02 as determined by spectroscopic ellipsometry, and uniform growth with a similar surface roughness before and after growth as confirmed by atomic force microscopy. However, the room temperature deposited Al{sub 2}O{sub 3} films had a lower mass density (2.7 g/cm{sup 3} compared with 3.0 g/cm{sup 3}) and a higher atomic ratio of O to Al (2.1 compared with 1.6) as indicated by x-ray reflectivity and Rutherford backscattering spectroscopy, respectively.« less

Constructing oxide interfaces and heterostructures by atomic layer-by-layer laser molecular beam epitaxy

NASA Astrophysics Data System (ADS)

Lei, Qingyu; Golalikhani, Maryam; Davidson, Bruce A.; Liu, Guozhen; Schlom, Darrell G.; Qiao, Qiao; Zhu, Yimei; Chandrasena, Ravini U.; Yang, Weibing; Gray, Alexander X.; Arenholz, Elke; Farrar, Andrew K.; Tenne, Dmitri A.; Hu, Minhui; Guo, Jiandong; Singh, Rakesh K.; Xi, Xiaoxing

2017-12-01

Advancements in nanoscale engineering of oxide interfaces and heterostructures have led to discoveries of emergent phenomena and new artificial materials. Combining the strengths of reactive molecular-beam epitaxy and pulsed-laser deposition, we show here, with examples of Sr1+xTi1-xO3+δ, Ruddlesden-Popper phase Lan+1NinO3n+1 (n = 4), and LaAl1+yO3(1+0.5y)/SrTiO3 interfaces, that atomic layer-by-layer laser molecular-beam epitaxy significantly advances the state of the art in constructing oxide materials with atomic layer precision and control over stoichiometry. With atomic layer-by-layer laser molecular-beam epitaxy we have produced conducting LaAlO3/SrTiO3 interfaces at high oxygen pressures that show no evidence of oxygen vacancies, a capability not accessible by existing techniques. The carrier density of the interfacial two-dimensional electron gas thus obtained agrees quantitatively with the electronic reconstruction mechanism.

Semiconducting behavior of substitutionally doped bilayer graphene

NASA Astrophysics Data System (ADS)

Mousavi, Hamze; Khodadadi, Jabbar; Grabowski, Marek

2018-02-01

In the framework of the Green's functions approach, random tight-binding model and using the coherent potential approximation, electronic characteristics of the bilayer graphene are investigated by exploring various forms of substitutional doping of a single or both layers of the system by either boron and (or) nitrogen atoms. The results for displacement of the Fermi level resemble the behavior of acceptor or donor doping in a conventional semiconductor, dependent on the impurity type and concentration. The particular pattern of doping of just one layer with one impurity type is most efficient for opening a gap within the energy bands which could be tuned directly by impurity concentration. Doping both layers at the same time, each with one impurity type, leads to an anomaly whereby the gap decreases with increasing impurity concentration.

High temperature interface superconductivity

DOE PAGES

Gozar, A.; Bozovic, I.

2016-01-20

High-T c superconductivity at interfaces has a history of more than a couple of decades. In this review we focus our attention on copper-oxide based heterostructures and multi-layers. We first discuss the technique, atomic layer-by-layer molecular beam epitaxy (ALL-MBE) engineering, that enabled High-T c Interface Superconductivity (HT-IS), and the challenges associated with the realization of high quality interfaces. Then we turn our attention to the experiments which shed light on the structure and properties of interfacial layers, allowing comparison to those of single-phase films and bulk crystals. Both ‘passive’ hetero-structures as well as surface-induced effects by external gating are discussed.more » Here, we conclude by comparing HT-IS in cuprates and in other classes of materials, especially Fe-based superconductors, and by examining the grand challenges currently laying ahead for the field.« less

A nitride-based epitaxial surface layer formed by ammonia treatment of silicene-terminated ZrB{sub 2}

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

Wiggers, F. B., E-mail: F.B.Wiggers@utwente.nl; Van Bui, H.; Schmitz, J.

We present a method for the formation of an epitaxial  surface layer involving B, N, and Si atoms on a ZrB{sub 2}(0001) thin film on Si(111). It has the potential to be an insulating growth template for 2D semiconductors. The chemical reaction of NH{sub 3} molecules with the silicene-terminated ZrB{sub 2}  surface was characterized by synchrotron-based, high-resolution core-level photoelectron spectroscopy and low-energy electron diffraction. In particular, the dissociative chemisorption of NH{sub 3} at 400 °C leads to surface  nitridation, and subsequent annealing up to 830 °C results in a solid phase reaction with the ZrB{sub 2} subsurface layers. In this way, amore » new nitride-based epitaxial  surface layer is formed with hexagonal symmetry and a single in-plane crystal orientation.« less

Landau quantization of Dirac fermions in graphene and its multilayers

NASA Astrophysics Data System (ADS)

Yin, Long-Jing; Bai, Ke-Ke; Wang, Wen-Xiao; Li, Si-Yu; Zhang, Yu; He, Lin

2017-08-01

When electrons are confined in a two-dimensional (2D) system, typical quantum-mechanical phenomena such as Landau quantization can be detected. Graphene systems, including the single atomic layer and few-layer stacked crystals, are ideal 2D materials for studying a variety of quantum-mechanical problems. In this article, we review the experimental progress in the unusual Landau quantized behaviors of Dirac fermions in monolayer and multilayer graphene by using scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS). Through STS measurement of the strong magnetic fields, distinct Landau-level spectra and rich level-splitting phenomena are observed in different graphene layers. These unique properties provide an effective method for identifying the number of layers, as well as the stacking orders, and investigating the fundamentally physical phenomena of graphene. Moreover, in the presence of a strain and charged defects, the Landau quantization of graphene can be significantly modified, leading to unusual spectroscopic and electronic properties.

Water desalination with a single-layer MoS2 nanopore

PubMed Central

Heiranian, Mohammad; Farimani, Amir Barati; Aluru, Narayana R.

2015-01-01

Efficient desalination of water continues to be a problem facing the society. Advances in nanotechnology have led to the development of a variety of nanoporous membranes for water purification. Here we show, by performing molecular dynamics simulations, that a nanopore in a single-layer molybdenum disulfide can effectively reject ions and allow transport of water at a high rate. More than 88% of ions are rejected by membranes having pore areas ranging from 20 to 60 Å2. Water flux is found to be two to five orders of magnitude greater than that of other known nanoporous membranes. Pore chemistry is shown to play a significant role in modulating the water flux. Pores with only molybdenum atoms on their edges lead to higher fluxes, which are ∼70% greater than that of graphene nanopores. These observations are explained by permeation coefficients, energy barriers, water density and velocity distributions in the pores. PMID:26465062

Water desalination with a single-layer MoS2 nanopore

NASA Astrophysics Data System (ADS)

Heiranian, Mohammad; Farimani, Amir Barati; Aluru, Narayana R.

2015-10-01

Efficient desalination of water continues to be a problem facing the society. Advances in nanotechnology have led to the development of a variety of nanoporous membranes for water purification. Here we show, by performing molecular dynamics simulations, that a nanopore in a single-layer molybdenum disulfide can effectively reject ions and allow transport of water at a high rate. More than 88% of ions are rejected by membranes having pore areas ranging from 20 to 60 Å2. Water flux is found to be two to five orders of magnitude greater than that of other known nanoporous membranes. Pore chemistry is shown to play a significant role in modulating the water flux. Pores with only molybdenum atoms on their edges lead to higher fluxes, which are ~70% greater than that of graphene nanopores. These observations are explained by permeation coefficients, energy barriers, water density and velocity distributions in the pores.

Water desalination with a single-layer MoS2 nanopore.

PubMed

Heiranian, Mohammad; Farimani, Amir Barati; Aluru, Narayana R

2015-10-14

Efficient desalination of water continues to be a problem facing the society. Advances in nanotechnology have led to the development of a variety of nanoporous membranes for water purification. Here we show, by performing molecular dynamics simulations, that a nanopore in a single-layer molybdenum disulfide can effectively reject ions and allow transport of water at a high rate. More than 88% of ions are rejected by membranes having pore areas ranging from 20 to 60 Å(2). Water flux is found to be two to five orders of magnitude greater than that of other known nanoporous membranes. Pore chemistry is shown to play a significant role in modulating the water flux. Pores with only molybdenum atoms on their edges lead to higher fluxes, which are ∼ 70% greater than that of graphene nanopores. These observations are explained by permeation coefficients, energy barriers, water density and velocity distributions in the pores.

2D- and 3D SIMS investigations on hot-pressed steel powder HS 6-5-3-8.

PubMed

Rosner, M; Pöckl, G; Danninger, H; Hutter, H

2002-10-01

Processing of steel with powder metallurgical methods such as sintering or hot-pressing have proven to be a powerful tool for the production of industrial parts and for components in the automotive industry. Series of steel-powders (HS 6-5-3-8) produced by gas atomization has been hot-pressed in a graphite tube at temperatures from 820 degrees C to 1050 degrees C. The samples have been characterized with a Secondary Electron Microscope (SEM) due to their porosity and then investigated with 2D- and 3D- SIMS. The spatial distribution of the non-metallic impurities and the covering oxide layer of the single particles has been traced dependent to the pressing temperature. Powders pressed at temperatures higher than 880 degrees C exhibited different precipitation behavior of the impurities and an excessive loss of the covering oxide layer of the single powder particles.

Magnetic and electronic properties of single-walled Mo2C nanotube: a first-principles study

NASA Astrophysics Data System (ADS)

Jalil, Abdul; Sun, Zhongti; Wang, Dayong; Wu, Xiaojun

2018-04-01

The structural, electronic, and magnetic properties of single-walled Mo2C nanotubes are investigated by using first-principles calculations. We establish that single-walled Mo2C nanotubes can be rolled up from a graphene-like Mo2C monolayer with H- or T-type phase, i.e. H-Mo2C and T-Mo2C nanotubes. The armchair-type T-Mo2C nanotubes are more energetically stable than H-Mo2C nanotubes with the same diameter, while zigzag-type H-Mo2C nanotubes are more energetically stable than T-Mo2C nanotubes. In particular, (8, 0) H-Mo2C nanotube are more stable than Mo2C monolayer due to structural deformation. All Mo2C nanotubes are magnetic metals, independent of their chirality, and the magnetic moments of Mo atoms in the outer layer are larger than the inner. The ionic and metallic bonds in Mo2C nanotubes and delocalized electrons around Mo atoms lead to the versatile electronic and magnetic properties in them, endowing them potential applications in catalysts and electronics.

Magnetic and electronic properties of single-walled Mo2C nanotube: a first-principles study.

PubMed

Jalil, Abdul; Sun, Zhongti; Wang, Dayong; Wu, Xiaojun

2018-04-18

The structural, electronic, and magnetic properties of single-walled Mo 2 C nanotubes are investigated by using first-principles calculations. We establish that single-walled Mo 2 C nanotubes can be rolled up from a graphene-like Mo 2 C monolayer with H- or T-type phase, i.e. H-Mo 2 C and T-Mo 2 C nanotubes. The armchair-type T-Mo 2 C nanotubes are more energetically stable than H-Mo 2 C nanotubes with the same diameter, while zigzag-type H-Mo 2 C nanotubes are more energetically stable than T-Mo 2 C nanotubes. In particular, (8, 0) H-Mo 2 C nanotube are more stable than Mo 2 C monolayer due to structural deformation. All Mo 2 C nanotubes are magnetic metals, independent of their chirality, and the magnetic moments of Mo atoms in the outer layer are larger than the inner. The ionic and metallic bonds in Mo 2 C nanotubes and delocalized electrons around Mo atoms lead to the versatile electronic and magnetic properties in them, endowing them potential applications in catalysts and electronics.

Electronic Structure Control of Sub-nanometer 1D SnTe via Nanostructuring within Single-Walled Carbon Nanotubes.

PubMed

Vasylenko, Andrij; Marks, Samuel; Wynn, Jamie M; Medeiros, Paulo V C; Ramasse, Quentin M; Morris, Andrew J; Sloan, Jeremy; Quigley, David

2018-05-25

Nanostructuring, e. g., reduction of dimensionality in materials, offers a viable route toward regulation of materials electronic and hence functional properties. Here, we present the extreme case of nanostructuring, exploiting the capillarity of single-walled carbon nanotubes (SWCNTs) for the synthesis of the smallest possible SnTe nanowires with cross sections as thin as a single atom column. We demonstrate that by choosing the appropriate diameter of a template SWCNT, we can manipulate the structure of the quasi-one-dimensional (1D) SnTe to design electronic behavior. From first principles, we predict the structural re-formations that SnTe undergoes in varying encapsulations and confront the prediction with TEM imagery. To further illustrate the control of physical properties by nanostructuring, we study the evolution of transport properties in a homologous series of models of synthesized and isolated SnTe nanowires varying only in morphology and atomic layer thickness. This extreme scaling is predicted to significantly enhance thermoelectric performance of SnTe, offering a prospect for further experimental studies and future applications.

Structural properties and diffusion processes of the Cu 3Au (0 0 1) surface

NASA Astrophysics Data System (ADS)

Wang, Fang; Zhang, Jian-Min; Zhang, Yan; Ji, Vincent

2010-09-01

The surface relaxation and surface energy of both the mixed AuCu and pure Cu terminated Cu 3Au (0 0 1) surfaces are simulated and calculated by using the modified analytical embedded-atom method. We find that the mixed AuCu termination is energetically preferred over the pure Cu termination thereby the mono-vacancy diffusion is also investigated in the topmost few layers of the mixed AuCu terminated Cu 3Au (0 0 1) surface. In the mixed AuCu terminated surface the relaxed Au atoms are raised above Cu atoms for 0.13 Å in the topmost layer. All the surface atoms displace outwards, this effect occurs in the first three layers and changes the first two inter-layer spacing. For mono-vacancy migration in the first layer, the migration energies of Au and Cu mono-vacancy via two-type in-plane displace: the nearest neighbor jump (NNJ) and the second nearest neighbor jump (2NNJ), are calculated and the results show that the NNJ requires a much lower energy than 2NNJ. For the evolution of the energy requirements for successive nearest neighbor jumps (SNNJ) along three different paths: circularity, zigzag and beeline, we find that the circularity path is preferred over the other two paths due to its minimum energy barriers and final energies. In the second layer, the NN jumps in intra- and inter-layer of the Cu mono-vacancy are investigated. The calculated energy barriers and final energies show that the vacancy prefer jump up to a proximate Cu site. This replacement between the Cu vacancy in the second layer and Cu atom in the first layer is remunerative for the Au atoms enrichment in the topmost layer.

Anisotropic Growth of Otavite on Calcite: Implications for Heteroepitaxial Growth Mechanisms

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

Riechers, Shawn L.; Kerisit, Sebastien N.

Elucidating how cation intermixing can affect the mechanisms of heteroepitaxial growth in aqueous media has remained a challenging endeavor. Toward this goal, in situ atomic force microscopy was employed to image the heteroepitaxial growth of otavite (CdCO3) at the (10-14) surface of calcite (CaCO3) single crystals in static aqueous conditions. Heteroepitaxial growth proceeded via spreading of three-dimensional (3D) islands and two-dimensional (2D) atomic layers at low and high initial saturation levels, respectively. Experiments were carried out as a function of applied force and imaging mode thus enabling determination of growth mechanisms unaltered by imaging artifacts. This approach revealed the significantmore » anisotropic nature of heteroepitaxial growth on calcite in both growth modes and its dependence on supersaturation, intermixing, and substrate topography. The 3D islands not only grew preferentially along the [42-1] direction relative to the [010] direction, resulting in rod-like surface precipitates, but also showed clear preference for growth from the island end rich in obtuse/obtuse kink sites. Pinning to step edges was observed to often reverse this tendency. In the 2D growth mode, the relative velocities of acute and obtuse steps were observed to switch between the first and second atomic layers. This phenomenon stemmed from the significant Cd-Ca intermixing in the first layer, despite bulk thermodynamics predicting the formation of almost pure otavite. Composition effects were also responsible for the inability of 3D islands to grow on 2D layers in cases where both modes were observed to occur simultaneously. Overall, the AFM images highlighted the effects of intermixing on heteroepitaxial growth, particularly how it can induce thickness-dependent growth mechanisms at the nanoscale.« less

Oxidation precursor dependence of atomic layer deposited Al2O3 films in a-Si:H(i)/Al2O3 surface passivation stacks.

PubMed

Xiang, Yuren; Zhou, Chunlan; Jia, Endong; Wang, Wenjing

2015-01-01

In order to obtain a good passivation of a silicon surface, more and more stack passivation schemes have been used in high-efficiency silicon solar cell fabrication. In this work, we prepared a-Si:H(i)/Al2O3 stacks on KOH solution-polished n-type solar grade mono-silicon(100) wafers. For the Al2O3 film deposition, both thermal atomic layer deposition (T-ALD) and plasma enhanced atomic layer deposition (PE-ALD) were used. Interface trap density spectra were obtained for Si passivation with a-Si films and a-Si:H(i)/Al2O3 stacks by a non-contact corona C-V technique. After the fabrication of a-Si:H(i)/Al2O3 stacks, the minimum interface trap density was reduced from original 3 × 10(12) to 1 × 10(12) cm(-2) eV(-1), the surface total charge density increased by nearly one order of magnitude for PE-ALD samples and about 0.4 × 10(12) cm(-2) for a T-ALD sample, and the carrier lifetimes increased by a factor of three (from about 10 μs to about 30 μs). Combining these results with an X-ray photoelectron spectroscopy analysis, we discussed the influence of an oxidation precursor for ALD Al2O3 deposition on Al2O3 single layers and a-Si:H(i)/Al2O3 stack surface passivation from field-effect passivation and chemical passivation perspectives. In addition, the influence of the stack fabrication process on the a-Si film structure was also discussed in this study.

Atomic-scale electrochemistry on the surface of a manganite

DOE PAGES

Vasudevan, Rama K.; Tselev, Alexander; Baddorf, Arthur P.; ...

2015-04-09

The doped manganese oxides (manganites) have been widely studied for their colossal magnetoresistive effects, for potential applications in oxide spintronics, electroforming in resistive switching devices, and are materials of choice as cathodes in modern solid oxide fuel cells. However, little experimental knowledge of the dynamics of the surfaces of perovskite manganites at the atomic scale exists. Here, through in-situ scanning tunnelling microscopy (STM), we demonstrate atomic resolution on samples of La 0.625Ca 0.375MnO 3 grown on (001) SrTiO 3 by pulsed laser deposition (PLD). Furthermore, by applying triangular DC waveforms of increasing amplitude to the STM tip, and measuring themore » tunnelling current, we demonstrate the ability to both perform and monitor surface electrochemical processes at the atomic level, including, for the first time in a manganite, formation of single and multiple oxygen vacancies, disruption of the overlying manganite layers, and removal and deposition of individual atomic units or clusters. Our work paves the way for better understanding of surface oxygen reactions in these systems.« less

Interacting dark resonances with plasmonic meta-molecules

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

Jha, Pankaj K.; Mrejen, Michael; Kim, Jeongmin

2014-09-15

Dark state physics has led to a variety of remarkable phenomena in atomic physics, quantum optics, and information theory. Here, we investigate interacting dark resonance type physics in multi-layered plasmonic meta-molecules. We theoretically demonstrate that these plasmonic meta-molecules exhibit sub-natural spectral response, analogous to conventional atomic four-level configuration, by manipulating the evanescent coupling between the bright and dark elements (plasmonic atoms). Using cascaded coupling, we show nearly 4-fold reduction in linewidth of the hybridized resonance compared to a resonantly excited single bright plasmonic atom with same absorbance. In addition, we engineered the geometry of the meta-molecules to realize efficient intramolecularmore » excitation transfer with nearly 80%, on resonant excitation, of the total absorption being localized at the second dark plasmonic atom. An analytical description of the spectral response of the structure is presented with full electrodynamics simulations to corroborate our results. Such multilayered meta-molecules can bring a new dimension to higher quality factor plasmonic resonance, efficient excitation transfer, wavelength demultiplexing, and enhanced non-linearity at nanoscale.« less

Atomic and Excitonic Stability in Dirac Materials: A White Dwarf Perspective

NASA Astrophysics Data System (ADS)

Velizhanin, Kirill

2014-03-01

Dirac materials - systems where the low-energy spectrum of electronic excitations can be understood via solving the Dirac equation - draw a great amount of attention of the scientific community lately due to their enormous application potential and interesting basic physics. Examples of such materials include carbon nanotubes, graphene and, more recently, single-layer transition metal dichalcogenides. One surprising application of Dirac materials is their use as a platform to simulate various atomic and high-energy physics ``on a chip.'' For example, graphene has been recently used to ``mimic'' an atomic collapse of superheavy atoms [Y. Wang et al, Science, 340, 734, 2013]. In this talk I will discuss an unexpected similarity between atomic and excitonic collapse in Dirac materials and the limit of stability of such exotic astrophysical objects as degenerate stars (e.g., white dwarfs, neutron stars). Various aspects of this similarity, e.g., an application of the concept of the Chandrasekhar limit to the exciton stability in transition metal dichalcogenides, will be discussed. This work was performed under the NNSA of the U.S. DOE at LANL under Contract No. DE-AC52-06NA25396.

Quantum chemical investigation on the role of Li adsorbed on anatase (101) surface nano-materials on the storage of molecular hydrogen.

PubMed

Srinivasadesikan, V; Raghunath, P; Lin, M C

2015-06-01

Lithiation of TiO2 has been shown to enhance the storage of hydrogen up to 5.6 wt% (Hu et al. J Am Chem Soc 128:11740-11741, 2006). The mechanism for the process is still unknown. In this work we have carried out a study on the adsorption and diffusion of Li atoms on the surface and migration into subsurface layers of anatase (101) by periodic density functional theory calculations implementing on-site Coulomb interactions (DFT+U). The model consists of 24 [TiO2] units with 11.097 × 7.655 Å(2) surface area. Adsorption energies have been calculated for different Li atoms (1-14) on the surface. A maximum of 13 Li atoms can be accommodated on the surface at two bridged O, Ti-O, and Ti atom adsorption sites, with 83 kcal mol(-1) adsorption energy for a single Li atom adsorbed between two bridged O atoms from where it can migrate into the subsurface layer with 27 kcal mol(-1) energy barrier. The predicted adsorption energies for H2 on the lithiated TiO2 (101) surface with 1-10 Li atoms revealed that the highest adsorption energies occurred on 1-Li, 5-Li, and 9-Li surfaces with 3.5, 4.4, and 7.6 kcal mol(-1), respectively. The values decrease rapidly with additional H2 co-adsorbed on the lithiated surfaces; the maximum H2 adsorption on the 9Li-TiO2(a) surface was estimated to be only 0.32 wt% under 100 atm H2 pressure at 77 K. The result of Bader charge analysis indicated that the reduction of Ti occurred depending on the Li atoms covered on the TiO2 surface.

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.

Photoinduced Nonlinear Mixing of Terahertz Dipole Resonances in Graphene Metadevices.

PubMed

In, Chihun; Kim, Hyeon-Don; Min, Bumki; Choi, Hyunyong

2016-02-17

The first experimental demonstration of nonlinear terahertz difference-frequency generation in a hybrid graphene metadevice is reported. Decades of research have revealed that terahertz-wave generation is impossible in single-layer graphene. This limitation is overcome and nonlinear terahertz generation by ultra-short optical pulse injection is demonstrated. This device is an essential step toward atomically thin, nonlinear terahertz optoelectronic components. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Classical Gradual-Channel Modeling of Graphene Field-Effect Transistors (FETs)

DTIC Science & Technology

2010-08-01

29  1 1. Introduction Over the past 60 years, a large number of papers have been written about the properties of graphene (1...strongly covalent features of its atomic bonding, properties that it inherits from the semimetal graphite. Indeed, the earliest papers on graphene (2...simplicity of this “single-layer graphite” model, the picture of graphene that evolved from these papers is one of extreme complexity. This is

Synthesis and characterization of two layered aluminophosphates, ( T) 2HAl 2P 3O 12 ( T=2-BuNH 3+) and ( T)H 2Al 2P 3O 12 ( T=pyH +)

NASA Astrophysics Data System (ADS)

Chippindale, Ann M.; Powell, Anthony V.; Bull, Lucy M.; Jones, Richard H.; Cheetham, Anthony K.; Thomas, John M.; Xu, Ruren

1992-01-01

Two new aluminophosphates, ( T) 2HAl 2P 3O 12 ( T=2-BuNH 3+) ( I) and ( T)H 2Al 2P 3O 12 ( T=pyH +) ( II) with the same framework stoichiometry but different layer structures have been prepared under nonaqueous conditions and the structures determined by single-crystal X-ray diffraction. Compound ( I) crystallizes in the monoclinic space group P2 1/ c ( Z=4), with lattice parameters a=9.261(1) b=8.365(6), c=27.119(4) Å, β=91.50(1)δ, and V=2100.1 Å 3 ( R=0.072 and R w=0.090). The structure consists of Al-and P-centered tetrahedra linked to form layers. Protonated 2-butylamine molecules are located in the interlayer spaces and hydrogen bonded to the layers through NH 3+ groups. Weak hydrophobic van der Waals' interactions between alkyl groups of the 2-BuNH 3+ cations hold the layers together. Compound ( II) crystallizes in the triclinic space group P-1 ( Z=2), with a=8.574(2), b=8.631(3), c=10.371(2) Å, α=81.84(3), β=87.53(2), γ=69.07(2)δ, and V=709.49Å 3 ( R=0.039 and R w=0.052). The structure contains tetrahedrally coordinated P atoms and both tetrahedral and trigonal pyramidal Al atoms linked to form layers which are held together through hydrogen bonding, creating cavities in which pyH + cations reside.

Quantitative Raman spectrum and reliable thickness identification for atomic layers on insulating substrates.

PubMed

Li, Song-Lin; Miyazaki, Hisao; Song, Haisheng; Kuramochi, Hiromi; Nakaharai, Shu; Tsukagoshi, Kazuhito

2012-08-28

We demonstrate the possibility in quantifying the Raman intensities for both specimen and substrate layers in a common stacked experimental configuration and, consequently, propose a general and rapid thickness identification technique for atomic-scale layers on dielectric substrates. Unprecedentedly wide-range Raman data for atomically flat MoS(2) flakes are collected to compare with theoretical models. We reveal that all intensity features can be accurately captured when including optical interference effect. Surprisingly, we find that even freely suspended chalcogenide few-layer flakes have a stronger Raman response than that from the bulk phase. Importantly, despite the oscillating intensity of specimen spectrum versus thickness, the substrate weighted spectral intensity becomes monotonic. Combined with its sensitivity to specimen thickness, we suggest this quantity can be used to rapidly determine the accurate thickness for atomic layers.

Dopant Distribution in Atomic Layer Deposited ZnO:Al Films Visualized by Transmission Electron Microscopy and Atom Probe Tomography.

PubMed

Wu, Yizhi; Giddings, A Devin; Verheijen, Marcel A; Macco, Bart; Prosa, Ty J; Larson, David J; Roozeboom, Fred; Kessels, Wilhelmus M M

2018-02-27

The maximum conductivity achievable in Al-doped ZnO thin films prepared by atomic layer deposition (ALD) is limited by the low doping efficiency of Al. To better understand the limiting factors for the doping efficiency, the three-dimensional distribution of Al atoms in the ZnO host material matrix has been examined on the atomic scale using a combination of high-resolution transmission electron microscopy (TEM) and atom probe tomography (APT). Although the Al distribution in ZnO films prepared by so-called "ALD supercycles" is often presented as atomically flat δ-doped layers, in reality a broadening of the Al-dopant layers is observed with a full-width-half-maximum of ∼2 nm. In addition, an enrichment of the Al at grain boundaries is observed. The low doping efficiency for local Al densities > ∼1 nm -3 can be ascribed to the Al solubility limit in ZnO and to the suppression of the ionization of Al dopants from adjacent Al donors.

Dopant Distribution in Atomic Layer Deposited ZnO:Al Films Visualized by Transmission Electron Microscopy and Atom Probe Tomography

PubMed Central

2018-01-01

The maximum conductivity achievable in Al-doped ZnO thin films prepared by atomic layer deposition (ALD) is limited by the low doping efficiency of Al. To better understand the limiting factors for the doping efficiency, the three-dimensional distribution of Al atoms in the ZnO host material matrix has been examined on the atomic scale using a combination of high-resolution transmission electron microscopy (TEM) and atom probe tomography (APT). Although the Al distribution in ZnO films prepared by so-called “ALD supercycles” is often presented as atomically flat δ-doped layers, in reality a broadening of the Al-dopant layers is observed with a full-width–half-maximum of ∼2 nm. In addition, an enrichment of the Al at grain boundaries is observed. The low doping efficiency for local Al densities > ∼1 nm–3 can be ascribed to the Al solubility limit in ZnO and to the suppression of the ionization of Al dopants from adjacent Al donors. PMID:29515290

Dynamic layer rearrangement during growth of layered oxide films by molecular beam epitaxy

DOE PAGES

Lee, J. H.; Luo, G.; Tung, I. C.; ...

2014-08-03

The A n+1B nO 3n+1 Ruddlesden–Popper homologous series offers a wide variety of functionalities including dielectric, ferroelectric, magnetic and catalytic properties. Unfortunately, the synthesis of such layered oxides has been a major challenge owing to the occurrence of growth defects that result in poor materials behaviour in the higher-order members. To understand the fundamental physics of layered oxide growth, we have developed an oxide molecular beam epitaxy system with in situ synchrotron X-ray scattering capability. We present results demonstrating that layered oxide films can dynamically rearrange during growth, leading to structures that are highly unexpected on the basis of themore » intended layer sequencing. Theoretical calculations indicate that rearrangement can occur in many layered oxide systems and suggest a general approach that may be essential for the construction of metastable Ruddlesden–Popper phases. Lastly, we demonstrate the utility of the new-found growth strategy by performing the first atomically controlled synthesis of single-crystalline La 3Ni 2O 7.« less

Single-crystalline aluminum film for ultraviolet plasmonic nanolasers

PubMed Central

Chou, Bo-Tsun; Chou, Yu-Hsun; Wu, Yen-Mo; Chung, Yi-Cheng; Hsueh, Wei-Jen; Lin, Shih-Wei; Lu, Tien-Chang; Lin, Tzy-Rong; Lin, Sheng-Di

2016-01-01

Significant advances have been made in the development of plasmonic devices in the past decade. Plasmonic nanolasers, which display interesting properties, have come to play an important role in biomedicine, chemical sensors, information technology, and optical integrated circuits. However, nanoscale plasmonic devices, particularly those operating in the ultraviolet regime, are extremely sensitive to the metal and interface quality. Thus, these factors have a significant bearing on the development of ultraviolet plasmonic devices. Here, by addressing these material-related issues, we demonstrate a low-threshold, high-characteristic-temperature metal-oxide-semiconductor ZnO nanolaser that operates at room temperature. The template for the ZnO nanowires consists of a flat single-crystalline Al film grown by molecular beam epitaxy and an ultrasmooth Al2O3 spacer layer synthesized by atomic layer deposition. By effectively reducing the surface plasmon scattering and metal intrinsic absorption losses, the high-quality metal film and the sharp interfaces formed between the layers boost the device performance. This work should pave the way for the use of ultraviolet plasmonic nanolasers and related devices in a wider range of applications. PMID:26814581

Homoepitaxial growth of metal halide crystals investigated by reflection high-energy electron diffraction

DOE PAGES

Chen, Pei; Kuttipillai, Padmanaban S.; Wang, Lili; ...

2017-01-10

Here, we report the homoepitaxial growth of a metal halide on single crystals investigated with in situ reflection high-energy electron diffraction (RHEED) and ex situ atomic force microscopy (AFM). Epitaxial growth of NaCl on NaCl (001) is explored as a function of temperature and growth rate which provides the first detailed report of RHEED oscillations for metal halide growth. Layer-by-layer growth is observed at room temperature accompanied by clear RHEED oscillations while the growth mode transitions to an island (3D) mode at low temperature. At higher temperatures (>100 °C), RHEED oscillations and AFM data indicate a transition to a step-flowmore » growth mode. To show the importance of such metal halide growth, green organic light-emitting diodes (OLEDs) are demonstrated using a doped NaCl film with a phosphorescent emitter as the emissive layer. This study demonstrates the ability to perform in situ and non-destructive RHEED monitoring even on insulating substrates and could enable doped single crystals and crystalline substrates for a range of optoelectronic applications.« less

Few-layer nanoplates of Bi 2 Se 3 and Bi 2 Te 3 with highly tunable chemical potential.

PubMed

Kong, Desheng; Dang, Wenhui; Cha, Judy J; Li, Hui; Meister, Stefan; Peng, Hailin; Liu, Zhongfan; Cui, Yi

2010-06-09

A topological insulator (TI) represents an unconventional quantum phase of matter with insulating bulk band gap and metallic surface states. Recent theoretical calculations and photoemission spectroscopy measurements show that group V-VI materials Bi(2)Se(3), Bi(2)Te(3), and Sb(2)Te(3) are TIs with a single Dirac cone on the surface. These materials have anisotropic, layered structures, in which five atomic layers are covalently bonded to form a quintuple layer, and quintuple layers interact weakly through van der Waals interaction to form the crystal. A few quintuple layers of these materials are predicted to exhibit interesting surface properties. Different from our previous nanoribbon study, here we report the synthesis and characterizations of ultrathin Bi(2)Te(3) and Bi(2)Se(3) nanoplates with thickness down to 3 nm (3 quintuple layers), via catalyst-free vapor-solid (VS) growth mechanism. Optical images reveal thickness-dependent color and contrast for nanoplates grown on oxidized silicon (300 nm SiO(2)/Si). As a new member of TI nanomaterials, ultrathin TI nanoplates have an extremely large surface-to-volume ratio and can be electrically gated more effectively than the bulk form, potentially enhancing surface state effects in transport measurements. Low-temperature transport measurements of a single nanoplate device, with a high-k dielectric top gate, show decrease in carrier concentration by several times and large tuning of chemical potential.

Improved Gate Dielectric Deposition and Enhanced Electrical Stability for Single-Layer MoS2 MOSFET with an AlN Interfacial Layer.

PubMed

Qian, Qingkai; Li, Baikui; Hua, Mengyuan; Zhang, Zhaofu; Lan, Feifei; Xu, Yongkuan; Yan, Ruyue; Chen, Kevin J

2016-06-09

Transistors based on MoS2 and other TMDs have been widely studied. The dangling-bond free surface of MoS2 has made the deposition of high-quality high-k dielectrics on MoS2 a challenge. The resulted transistors often suffer from the threshold voltage instability induced by the high density traps near MoS2/dielectric interface or inside the gate dielectric, which is detrimental for the practical applications of MoS2 metal-oxide-semiconductor field-effect transistor (MOSFET). In this work, by using AlN deposited by plasma enhanced atomic layer deposition (PEALD) as an interfacial layer, top-gate dielectrics as thin as 6 nm for single-layer MoS2 transistors are demonstrated. The AlN interfacial layer not only promotes the conformal deposition of high-quality Al2O3 on the dangling-bond free MoS2, but also greatly enhances the electrical stability of the MoS2 transistors. Very small hysteresis (ΔVth) is observed even at large gate biases and high temperatures. The transistor also exhibits a low level of flicker noise, which clearly originates from the Hooge mobility fluctuation instead of the carrier number fluctuation. The observed superior electrical stability of MoS2 transistor is attributed to the low border trap density of the AlN interfacial layer, as well as the small gate leakage and high dielectric strength of AlN/Al2O3 dielectric stack.

Black phosphorus saturable absorber for ultrashort pulse generation

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

Sotor, J., E-mail: jaroslaw.sotor@pwr.edu.pl; Sobon, G.; Abramski, K. M.

Low-dimensional materials, due to their unique and versatile properties, are very interesting for numerous applications in electronics and optoelectronics. Recently rediscovered black phosphorus, with a graphite-like layered structure, can be effectively exfoliated up to the single atomic layer called phosphorene. Contrary to graphene, it possesses a direct band gap controllable by the number of stacked atomic layers. For those reasons, black phosphorus is now intensively investigated and can complement or replace graphene in various photonics and electronics applications. Here, we demonstrate that black phosphorus can serve as a broadband saturable absorber and can be used for ultrashort optical pulse generation.more » The mechanically exfoliated ∼300 nm thick layers of black phosphorus were transferred onto the fiber core, and under pulsed excitation at 1560 nm wavelength, its transmission increases by 4.6%. We have demonstrated that the saturable absorption of black phosphorus is polarization sensitive. The fabricated device was used to mode-lock an Er-doped fiber laser. The generated optical solitons with the 10.2 nm bandwidth and 272 fs duration were centered at 1550 nm. The obtained results unambiguously show that black phosphorus can be effectively used for ultrashort pulse generation with performances similar or even better than currently used graphene or carbon nanotubes. This application of black phosphorus proves its great potential to future practical use in photonics.« less

Hybrid phosphorene/graphene nanocomposite as an anode material for Na-ion batteries: a first-principles study

NASA Astrophysics Data System (ADS)

Wang, Linxia; Jiang, Zhiqiang; Li, Wei; Gu, Xiao; Huang, Li

2017-04-01

The potential application of the hybrid phosphorene/graphene (P/G) composites as an anode material in Na-ion batteries (NIBs) has been explored based on first-principles calculations. The calculated elastic constants reveal that the P/G has an ultrahigh stiffness, which can effectively suppress the undesirable structural deformation during the sodiation and desodiation cycles. Na atoms can strongly bind with the phosphorene single-layer (SP), double-layer (DP), and their composites with graphene (SP/G, DP/G, G/DP/G), and can even cause a sliding between the layers when the DP/G accommodate more Na atoms. The migration of Na in P/G is anisotropic with the minimum energy path along the zigzag channel. The low diffusion barriers of only about several tens of meV ensure the high mobility of Na within the layers, and thus lead to rapid charge/discharge capacity of P/G. The electronic structures show that the hybrid P/G becomes metallic with the Na incorporation, which contributes to the good electric conductivity in P/G. We further demonstrate that the average open circuit voltage (OCV) of DP/G is 0.53 V, which is comparable to other anode materials. These results suggest that P/G composites hold great potential to be a good anode material in NIBs.

Electronic structure imperfections and chemical bonding at graphene interfaces

NASA Astrophysics Data System (ADS)

Schultz, Brian Joseph

The manifestation of novel phenomena upon scaling to finite size has inspired a paradigm shift in materials science that takes advantage of the distinctive electrical and physical properties of nanomaterials. Remarkably, the simple honeycomb arrangement of carbon atoms in a single atomic layer has become renowned for exhibiting never-before-seen electronic and physical phenomena. This archetypal 2-dimensional nanomaterial is known as graphene, a single layer of graphite. Early reports in the 1950's eluded to graphene-like nanostructures that were evidenced from exfoliation of oxidized graphite followed by chemical reduction, absorbed carbon on transition metals, and thermal decomposition of SiC. Furthermore, the earliest tight binding approximation calculations in the 1950's held clues that a single-layer of graphite would behave drastically different than bulk graphite. Not until 2004, when Giem and Novoselov first synthesized graphene by mechanical exfoliation from highly-oriented pyrolytic graphite did the field of graphene-based research bloom within the scientific community. Since 2004, the availability and relatively straight forward synthesis of single-layer graphene (SLG) enabled the observation of remarkable phenomena including: massless Dirac fermions, extremely high mobilities of its charge carriers, room temperature half-integer quantum Hall effect, the Rashba effect, and the potential for ballistic conduction over macroscopic distances. These enticing electronic properties produce the drive to study graphene for use in truly nanoscale electrical interconnects, integrated circuits, transparent conducting electrodes, ultra-high frequency transistors, and spintronic devices, just to name a few. Yet, for almost all real world applications graphene will need to be interfaced with other materials, metals, dielectrics, organics, or any combination thereof that in turn are constituted from various inorganic and organic components. Interfacing graphene, a nanomaterial with lateral dimensions in the hundreds of microns if not larger, with a corresponding atomic vertical thickness poses significant difficulties. Graphene's unique structure is dominated by surface area or potentially hybridized interfaces; consequently, the true realization of this remarkable nanomaterial in device constructs relies on engineering graphene interfaces at the surface in order to controllably mold the electronic structure. Near-edge X-ray absorption fine-structure (NEXAFS) spectroscopy and the transmission mode analogue scanning transmission X-ray microscopy (STXM) are particularly useful tools to study the unoccupied states of graphene and graphene interfaces. In addition, polarized NEXAFS and STXM studies provide information on surface orientation, bond sterics, and the extent of substrate alignment before and after interfacial hybridization. The work presented in this dissertation is fundamentally informed by NEXAFS and STXM measurements on graphene/metal, graphene/dielectric, and graphene/organic interfaces. We start with a general review of the electronic structure of freestanding graphene and graphene interfaces in Chapter 1. In Chapter 2, we investigate freestanding single-layer graphene via STXM and NEXAFS demonstrating that electronic structure heterogeneities from synthesis and processing are ubiquitous in 2-dimensional graphene. We show the mapping of discrete charge transfer regions as a result of doped impurities that decorate the surfaces of graphene and that transfer processing imparts local electronic corrugations or ripples. In corroboration with density functional theory, definitive assignments to the spectral features, global steric orientations of the localized domains, and quantitative charge transfer schemes are evidenced. In the following chapters, we deliberately (Chapter 3) incorporate substitutional nitrogen into reduced graphene oxide to induce C--N charge redistribution and improve global conductivity, (Chapter 4) fabricate graphene/metal interfaces and metal/graphene/metal sandwich structures evidencing classical anisotropic umpolung chemistry from carbon pz-orbrital charge pinning, and (Chapter 5) engineer graphene/dielectric interfaces showing electron depletion from carbon atoms at the HfO2/graphene interface. The fabrication of graphene interfaces remains a critical gap for successful commercialization of graphene-based devices, yet we demonstrate that interfacial hybridization, anisotropic charge redistribution, local chemical bonding, and discrete electronic hybridization regimes play a critical role in the electronic structure at graphene interfaces.

Dimensional Effects on the Charge Density Waves in Ultrathin Films of TiSe 2

DOE PAGES

Chen, P.; Chan, Y. -H.; Wong, M. -H.; ...

2016-09-20

Charge density wave (CDW) formation in solids is a critical phenomenon involving the collective reorganization of the electrons and atoms in the system into a wave structure, and it is expected to be sensitive to the geometric constraint of the system at the nanoscale. Here, we study the CDW transition in TiSe 2, a quasi-two-dimensional layered material, to determine the effects of quantum confinement and changing dimensions in films ranging from a single layer to multilayers. Of key interest is the characteristic length scale for the transformation from a two-dimensional case to the three-dimensional limit. Angle-resolved photoemission (ARPES) measurements ofmore » films with thicknesses up to six layers reveal substantial variations in the energy structure of discrete quantum well states; however, the temperature-dependent band-gap renormalization converges at just three layers. The results indicate a layer-dependent mixture of two transition temperatures and a very-short-range CDW interaction within a three-dimensional framework.« less

Two-dimensional triangular lattice and its application to lithium-intercalated layered compounds

NASA Astrophysics Data System (ADS)

Decerqueira, R. O.

1982-08-01

Good rechargeable batteries are being searched for use in electric vehicles and in energy storage during off-peak consumption periods and from solar sources. The interest in lithium intercalation compounds has been recently enhanced by the search for such batteries. The process of intercalation of lithium in several transition metal dichalcogenides can provide an emf of several volts. The progress achieved in the last decade in the investigation of these intercalates has been facilitated by the availability of the dichalcogenides as single crystals and by their chemical stability. The transition-metal dichalcogenides and their Li-intercalates are studied, with emphasis on the Li/su xTa/sub yTi/sub l-y/S2 series. The interactions between the Li atoms and the applicability of a lattice gas model to the problem of ordering of these atoms is discussed. A formulation is presented of the cluster-variation aproximation to the lattice gas problem. The single-site and the nearest-neighbor triangle basic clusters are considered as models for Li/sub x TiS2. Also a theory is presented for the effects of a random distribution of different species of host atoms, as in Ta/sub y/Ti/sub l-y/S2.

Sinter-Resistant Platinum Catalyst Supported by Metal-Organic Framework

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

Kim, In Soo; Li, Zhanyong; Zheng, Jian

Installed on the zirconia nodes of a metal-organic framework (MOF) NU-1000 via targeted vapor-phase synthesis. The catalytic Pt clusters, site-isolated by organic linkers, are shown to exhibit high catalytic activity for ethylene hydrogenation while exhibiting resistance to sintering up to 200 degrees C. In situ IR spectroscopy reveals the presence of both single atoms and few-atom clusters that depend upon synthesis conditions. Operando X-ray absorption spectroscopy and Xray pair distribution analyses reveal unique changes in chemical bonding environment and cluster size stability while on stream. Density functional theory calculations elucidate a favorable reaction pathway for ethylene hydrogenation with the novelmore » catalyst. These results provide evidence that atomic layer deposition (ALD) in MOFs is a versatile approach to the rational synthesis of size-selected clusters, including noble metals, on a high surface area support.« less

Atomically Thin Mesoporous Nanomesh of Graphitic C₃N₄ for High-Efficiency Photocatalytic Hydrogen Evolution.

PubMed

Han, Qing; Wang, Bing; Gao, Jian; Cheng, Zhihua; Zhao, Yang; Zhang, Zhipan; Qu, Liangti

2016-02-23

Delamination of layer materials into two-dimensional single-atom sheets has induced exceptional physical properties, including large surface area, ultrahigh intrinsic carrier mobility, pronounced changes in the energy band structure, and other properties. Here, atomically thin mesoporous nanomesh of graphitic carbon nitride (g-C3N4) is fabricated by solvothermal exfoliation of mesoporous g-C3N4 bulk made from thermal polymerization of freeze-drying assembled Dicyandiamide nanostructure precursor. With the unique structural advantages for aligned energy levels, electron transfer, light harvesting, and the richly available reaction sites, the as-prepared monolayer of mesoporous g-C3N4 nanomesh exhibits a superior photocatalytic hydrogen evolution rate of 8510 μmol h(-1) g(-1) under λ > 420 nm and an apparent quantum efficiency of 5.1% at 420 nm, the highest of all the metal-free g-C3N4 nanosheets photocatalysts.

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

Susarla, Sandhya; Kochat, Vidya; Kutana, Alex

Transition metal dichalcogenide (TMD) alloys form a broad class of two-dimensional (2D) layered materials with tunable bandgaps leading to interesting optoelectronic applications. In the bottom-up approach of building these atomically thin materials, atomic doping plays a crucial role. Here we demonstrate a single step CVD (chemical vapor deposition) growth procedure for obtaining binary alloys and heterostructures by tuning atomic composition. We show that a minute doping of tin during the growth phase of the Mo 1–xW xS 2 alloy system leads to formation of lateral and vertical heterostructure growth. High angle annular dark field scanning transmission electron microscopy (HAADF-STEM) imagingmore » and density functional theory (DFT) calculations also support the modified stacking and growth mechanism due to the nonisomorphous Sn substitution. Our experiments demonstrate the possibility of growing heterostructures of TMD alloys whose spectral responses can be desirably tuned for various optoelectronic applications.« less

Small angle neutron and X-ray studies of carbon structures with metal atoms

NASA Astrophysics Data System (ADS)

Lebedev, V. T.; Szhogina, A. A.; Bairamukov, V. Yu

2017-05-01

Encapsulation of metal atoms inside carbon single-wall cages or within multi-layer cells has been realized using molecular precursors and high temperature processes transforming them into desirable structures. Endohedral fullerenols Fe@C60(OH)X with 3d-metal (iron) have been studied by SANS in aqueous solutions where they form stable globular clusters with radii R C ∼ 10-12 nm and aggregation numbers N C ∼ 104. This self-assembly is a crucial feature of paramagnetic fullerenols as perspective contrast agents for Magneto-Resonance Imaging in medicine. Cellular carbon-metal structures have been created by the pyrolysis of diphthalocyanines of lanthanides and actinides. It was established that these ultra porous matrices consist of globular cells of molecular precursor size (∼ 1 nm) which are aggregated into superstructures. This provides retain of metal atoms inside matrices which may serve for safety storage of spent fuel of nuclear power plants.

A two-dimensional organic–inorganic hybrid compound, poly[(ethylenediamine)tri-μ-oxido-oxidocopper(II)molybdenum(VI)

PubMed Central

Gun, Ozgul; VanDerveer, Don; Emirdag-Eanes, Mehtap

2008-01-01

A new organic–inorganic two-dimensional hybrid compound, [CuMoO4(C2H8N2)], has been hydro­thermally synthesized at 443 K. The unit cell contains layers composed of CuN2O4 octa­hedra and MoO4 tetra­hedra. Corner-sharing MoO4 and CuN2O4 polyhedra form CuMoO4 bimetallic sites that are joined together through O atoms, forming an edge-sharing Cu2Mo2O4 chain along the c axis. The one-dimensional chains are further linked through bridging O atoms that join the Cu and Mo atoms into respective chains along the b axis, thus establishing layers in the bc plane. The ethyl­enediamine ligand is coordinated to the Cu atom through its two N atoms and is oriented perpendicularly to the two-dimensional –Cu—O—Mo– layers. The average distance between adjacent layers, as calculated by consideration of the closest and furthest distances between two layers, is 8.7 Å. The oxidation states of the Mo and Cu atoms of VI and II, respectively, were confirmed by bond-valence sum calculations. PMID:21200997

Epitaxial layers of 2122 BCSCO superconductor thin films having single crystalline structure

NASA Technical Reports Server (NTRS)

Pandey, Raghvendra K. (Inventor); Raina, Kanwal K. (Inventor); Solayappan, Narayanan (Inventor)

1995-01-01

A substantially single phase, single crystalline, highly epitaxial film of Bi.sub.2 CaSr.sub.2 Cu.sub.2 O.sub.8 superconductor which has a T.sub.c (zero resistance) of 83K is provided on a lattice-matched substrate with no intergrowth. This film is produced by a Liquid Phase Epitaxy method which includes the steps of forming a dilute supercooled molten solution of a single phase superconducting mixture of oxides of Bi, Ca, Sr, and Cu having an atomic ratio of about 2:1:2:2 in a nonreactive flux such as KCl, introducing the substrate, e.g., NdGaO.sub.3, into the molten solution at 850.degree. C., cooling the solution from 850.degree. C. to 830.degree. C. to grow the film and rapidly cooling the substrate to room temperature to maintain the desired single phase, single crystalline film structure.

Laser-assisted atom probe tomography of four paired poly-Si/SiO2 multiple-stacks with each thickness of 10 nm

NASA Astrophysics Data System (ADS)

Kwak, C.-M.; Seol, J.-B.; Kim, Y.-T.; Park, C.-G.

2017-02-01

For the past 10 years, laser-assisted atom probe tomography (APT) analysis has been performed to quantify the near-atomic scale distribution of elements and their local chemical compositions within interfaces that determine the design, processing, and properties of virtually all materials. However, the nature of the occurring laser-induced emission at the surface of needle-shaped sample is highly complex and it has been an ongoing challenge to understand the surface-related interactions between laser-sources and tips containing non-conductive oxides for a robust and reliable analysis of multiple-stacked devices. Here, we find that the APT analysis of four paired poly-Si/SiO2 (conductive/non-conductive) multiple stacks with each thickness of 10 nm is governed by experimentally monitoring three experimental conditions, such as laser-beam energies ranged from 30 to 200 nJ, analysis temperatures varying with 30-100 K, and the inclination of aligned interfaces within a given tip toward analysis direction. Varying with laser-energy and analysis temperature, a drastic compositional ratio of doubly charged Si ions to single charged Si ions within conductive poly-Si layers is modified, as compared with ones detected in the non-conductive layers. Severe distorted APT images of multiple stacks are also inevitable, especially at the conductive layers, and leading to a lowering of the successful analysis yields. This lower throughput has been overcome though changing the inclination of interfaces within a given tip to analysis direction (planar interfaces parallel to the tip axis), but significant deviations in chemical compositions of a conductive layer counted from those of tips containing planar interfaces perpendicular to the tip axis are unavoidable owing to the Si2, SiH2O, and Si2O ions detected, for the first time, within poly-Si layers.

Implementation of atomic layer etching of silicon: Scaling parameters, feasibility, and profile control

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

Ranjan, Alok, E-mail: alok.ranjan@us.tel.com; Wang, Mingmei; Sherpa, Sonam D.

2016-05-15

Atomic or layer by layer etching of silicon exploits temporally segregated self-limiting adsorption and material removal steps to mitigate the problems associated with continuous or quasicontinuous (pulsed) plasma processes: selectivity loss, damage, and profile control. Successful implementation of atomic layer etching requires careful choice of the plasma parameters for adsorption and desorption steps. This paper illustrates how process parameters can be arrived at through basic scaling exercises, modeling and simulation, and fundamental experimental tests of their predictions. Using chlorine and argon plasma in a radial line slot antenna plasma source as a platform, the authors illustrate how cycle time, ionmore » energy, and radical to ion ratio can be manipulated to manage the deviation from ideality when cycle times are shortened or purges are incomplete. Cell based Monte Carlo feature scale modeling is used to illustrate profile outcomes. Experimental results of atomic layer etching processes are illustrated on silicon line and space structures such that iso-dense bias and aspect ratio dependent free profiles are produced. Experimental results also illustrate the profile control margin as processes move from atomic layer to multilayer by layer etching. The consequence of not controlling contamination (e.g., oxygen) is shown to result in deposition and roughness generation.« less

Prenucleation Induced by Crystalline Substrates

NASA Astrophysics Data System (ADS)

Men, H.; Fan, Z.

2018-04-01

Prenucleation refers to the phenomenon of atomic ordering in the liquid adjacent to the substrate/liquid interface at temperatures above the liquidus. In this paper, we have systematically investigated and holistically quantified the prenucleation phenomenon as a function of temperature and the lattice misfit between the substrate and the solid, using molecular dynamics (MD) simulations. Our results have confirmed that at temperatures above the liquidus, the atoms in the liquid at the interface may exhibit pronounced atomic ordering, manifested by atomic layering normal to the interface, in-plane atomic ordering parallel to the interface, and the formation of a 2-dimensional (2D) ordered structure (a few atomic layers in thickness) on the substrate surface. Holistic quantification of such atomic ordering at the interface has revealed that the atomic layering is independent of lattice misfit and is only slightly enhanced by reducing temperature while both in-plane atomic ordering and the formation of the 2D ordered structure are significantly enhanced by reducing the lattice misfit and/or temperature. This substrate-induced atomic ordering in the liquid may have a significant influence on the subsequent heterogeneous nucleation process.

Positron Annihilation Induced Auger and Gamma Spectroscopy of Catalytically Important Surfaces

NASA Astrophysics Data System (ADS)

Weiss, A. H.; Nadesalingam, M. P.; Sundaramoorthy, R.; Mukherjee, S.; Fazleev, N. G.

2006-10-01

The annihilation of positrons with core electrons results in unique signatures in the spectra of Auger-electron and annihilation-gamma rays that can be used to make clear chemical identification of atoms at the surface. Because positrons implanted at low energies are trapped with high efficiency in the image-correlation well where they are localized just outside the surface it is possible to use annihilation induced Auger and Gamma signals to probe the surfaces of solids with single atomic layer depth resolution. In this talk we will report recent applications of Positron Annihilation Induced Auger Electron Spectroscopy (PAES) and Auger-Gamma Coincidence Spectroscopy (AGCS) to the study of surface structure and surface chemistry. Our research has demonstrated that PAES spectra can provide new information regarding the composition of the top-most atomic layer. Applications of PAES to the study of catalytically important surfaces of oxides and wide band-gap semiconductors including TiO2, SiO2,Cu2O, and SiC will be presented. We conclude with a discussion of the use of Auger-Gamma and Gamma-Gamma coincidence spectroscopy for the study of surfaces at pressures closer to those found in practical chemical reactors. Research supported by the Welch Foundation Grant Number Y-1100.

Single-Atom Single-Photon Quantum Interface

NASA Astrophysics Data System (ADS)

Moehring, David; Bochmann, Joerg; Muecke, Martin; Specht, Holger; Weber, Bernhard; Wilk, Tatjana; Rempe, Gerhard

2008-05-01

By combining atom trapping techniques and cavity cooling schemes we are able to trap a single neutral atom inside a high-finesse cavity for several tens of seconds. We show that our coupled atom-cavity system can be used to generate single photons in a controlled way. With our long trapping times and high single-photon production efficiency, the non-classical properties of the emitted light can be shown in the photon correlations of a single atom. In a similar atom-cavity setup, we investigate the interface between atoms and photons by entangling a single atom with a single photon emitted into the cavity and by further mapping the quantum state of the atom onto a second single photon. These schemes are intrinsically deterministic and establish the basic element required to realize a distributed quantum network with individual atoms at rest as quantum memories and single flying photons as quantum messengers. This work was supported by the Deutsche Forschungsgemeinschaft, and the European Union SCALA and CONQUEST programs. D. L. M. acknowledges support from the Alexander von Humboldt Foundation.

Atomic and electronic structure of the CdTe(111)B–(2√3 × 4) orthogonal surface

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

Bekenev, V. L., E-mail: bekenev@ipms.kiev.ua; Zubkova, S. M.

2017-01-15

The atomic and electronic structure of four variants of Te-terminated CdTe(111)B–(2√3 × 4) orthogonal polar surface (ideal, relaxed, reconstructed, and reconstructed with subsequent relaxation) are calculated ab initio for the first time. The surface is modeled by a film composed of 12 atomic layers with a vacuum gap of ~16 Å in the layered superlattice approximation. To close Cd dangling bonds on the opposite side of the film, 24 fictitious hydrogen atoms with a charge of 1.5 electrons each are added. Ab initio calculations are performed using the Quantum Espresso program based on density functional theory. It is demonstrated thatmore » relaxation leads to splitting of the four upper layers. The band energy structures and total and layer-by-layer densities of electronic states for the four surface variants are calculated and analyzed.« less

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

Hossain, M. Anwar; Center for Crystal Science and Technology, University of Yamanashi, Miyamae 7-32, Kofu, Yamanashi 400-8511; Tanaka, Isao

We studied thermoelectric properties of YB{sub 41}Si{sub 1.3} single crystals grown by the floating zone method. The composition of the grown crystal was confirmed by electron probe micro-analysis. We have determined the growth direction for the first time for these borosilicides, and discovered relatively large anisotropy in electrical properties. We measured the electrical resistivity and Seebeck coefficient along [510] (the growth direction) and [052] directions and we found that this crystal exhibits strong electrical anisotropy with a maximum of more than 8 times. An interesting layered structural feature is revealed along [510] with dense boron cluster layers and yttrium layers,more » with conductivity enhanced along this direction. We obtained 3.6 times higher power factor along [510] compared to that along [052]. Although the ZT of the present system is low, anisotropy in the thermoelectric properties of a boride was reported for the first time, and can be a clue in developing other boride systems also. - Graphical abstract: The growth direction ([510]) was determined for the first time in YB{sub 41}Si{sub 1.3} single crystals and revealed an interesting layered feature of boron clusters and metal atoms, along which the electrical conductivity and thermoelectric power factor was strongly enhanced. - Highlights: • We have grown YB{sub 41}Si{sub 1.3} single crystals by the floating zone method. • Growth direction of [510] determined for first time in REB{sub 41}Si{sub 1.2}. • Electrical resistivity was strongly anisotropic with possible enhancement along metal layers. • The obtained power factor along [510] is 3.6 times higher than that along [052].« less

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.

Direct synthesis of large area graphene on insulating substrate by gallium vapor-assisted chemical vapor deposition

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

Murakami, Katsuhisa, E-mail: k.murakami@bk.tsukuba.ac.jp; Hiyama, Takaki; Kuwajima, Tomoya

2015-03-02

A single layer of graphene with dimensions of 20 mm × 20 mm was grown directly on an insulating substrate by chemical vapor deposition using Ga vapor catalysts. The graphene layer showed highly homogeneous crystal quality over a large area on the insulating substrate. The crystal quality of the graphene was measured by Raman spectroscopy and was found to improve with increasing Ga vapor density on the reaction area. High-resolution transmission electron microscopy observations showed that the synthesized graphene had a perfect atomic-scale crystal structure within its grains, which ranged in size from 50 nm to 200 nm.

Effect of atomic monolayer insertions on electric-field-induced rotation of magnetic easy axis

NASA Astrophysics Data System (ADS)

Tsujikawa, M.; Haraguchi, S.; Oda, T.

2012-04-01

We have investigated the electric field (EF) effect on the magnetic anisotropy energy (MAE) in the thin films MgO/M/Fe/Au(001) and MgO/Fe/M(001) (M = Pd, Pt, and Au) by means of first-principles density-functional calculations. We find that the MAE varies linearly with the EF and investigate the change in slope of the MAE as a function of the EF as the buffer layer is changed. We find that a single monatomic buffer layer may be useful for devices that use EF-modified MAE. We simulate the critical EF for easy-axis rotation and discuss interface effects of Mg/Fe and Fe/Au on MAE.

Sharp chemical interface in epitaxial Fe{sub 3}O{sub 4} thin films

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

Gálvez, S.; Rubio-Zuazo, J., E-mail: rubio@esrf.fr; Salas-Colera, E.

Chemically sharp interface was obtained on single phase single oriented Fe{sub 3}O{sub 4} (001) thin film (7 nm) grown on NiO (001) substrate using oxygen assisted molecular beam epitaxy. Refinement of the atomic structure, stoichiometry, and oxygen vacancies were determined by soft and hard x-ray photoelectron spectroscopy, low energy electron diffraction and synchrotron based X-ray reflectivity, and X-ray diffraction. Our results demonstrate an epitaxial growth of the magnetite layer, perfect iron stoichiometry, absence of oxygen vacancies, and the existence of an intermixing free interface. Consistent magnetic and electrical characterizations are also shown.

Carbon Nanotube Microarrays Grown on Nanoflake Substrates

NASA Technical Reports Server (NTRS)

Schmidt, Howard K.; Hauge, Robert H.; Pint, Cary; Pheasant, Sean

2013-01-01

This innovation consists of a new composition of matter where single-walled carbon nanotubes (SWNTs) are grown in aligned arrays from nanostructured flakes that are coated in Fe catalyst. This method of growth of aligned SWNTs, which can yield well over 400 percent SWNT mass per unit substrate mass, exceeds current yields for entangled SWNT growth. In addition, processing can be performed with minimal wet etching treatments, leaving aligned SWNTs with superior properties over those that exist in entangled mats. The alignment of the nanotubes is similar to that achieved in vertically aligned nanotubes, which are called "carpets. " Because these flakes are grown in a state where they are airborne in a reactor, these flakes, after growing SWNTs, are termed "flying carpets. " These flakes are created in a roll-to-roll evaporator system, where three subsequent evaporations are performed on a 100-ft (approx. =30-m) roll of Mylar. The first layer is composed of a water-soluble "release layer, " which can be a material such as NaCl. After depositing NaCl, the second layer involves 40 nm of supporting layer material . either Al2O3 or MgO. The thickness of the layer can be tuned to synthesize flakes that are larger or smaller than those obtained with a 40-nm deposition. Finally, the third layer consists of a thin Fe catalyst layer with a thickness of 0.5 nm. The thickness of this layer ultimately determines the diameter of SWNT growth, and a layer that is too thick will result in the growth of multiwalled carbon nanotubes instead of single-wall nanotubes. However, between a thickness of 0.5 nm to 1 nm, single-walled carbon nanotubes are known to be the primary constituent. After this three-layer deposition process, the Mylar is rolled through a bath of water, which allows catalyst-coated flakes to detach from the Mylar. The flakes are then collected and dried. The method described here for making such flakes is analogous to that which is used to make birefringent ink that is coated on U.S. currency. After deposition, the growth is carried out in a hot-filament chemical vapor deposition apparatus. A tungsten hot filament placed in the flow of H2 at a temperature greater than 1,600 C creates atomic hydrogen, which serves to reduce the Fe catalyst into a metallic state. The catalyst can now precipitate SWNTs in the presence of growth gases. The gases used for the experiments reported are C2H2, H2O, and H2, at rates of 2, 2, and 400 standard cubic centimeters per minute (sccm), respectively. In order to retain the flakes, a cage is constructed by spot welding stainless steel or copper mesh to form an enclosed area, in which the flakes are placed prior to growth. This allows growth gases and atomic hydrogen to reach the flakes, but does not allow the flakes, which rapidly nucleate SWNTs, to escape from the cage.

Quantized edge modes in atomic-scale point contacts in graphene

NASA Astrophysics Data System (ADS)

Kinikar, Amogh; Phanindra Sai, T.; Bhattacharyya, Semonti; Agarwala, Adhip; Biswas, Tathagata; Sarker, Sanjoy K.; Krishnamurthy, H. R.; Jain, Manish; Shenoy, Vijay B.; Ghosh, Arindam

2017-07-01

The zigzag edges of single- or few-layer graphene are perfect one-dimensional conductors owing to a set of gapless states that are topologically protected against backscattering. Direct experimental evidence of these states has been limited so far to their local thermodynamic and magnetic properties, determined by the competing effects of edge topology and electron-electron interaction. However, experimental signatures of edge-bound electrical conduction have remained elusive, primarily due to the lack of graphitic nanostructures with low structural and/or chemical edge disorder. Here, we report the experimental detection of edge-mode electrical transport in suspended atomic-scale constrictions of single and multilayer graphene created during nanomechanical exfoliation of highly oriented pyrolytic graphite. The edge-mode transport leads to the observed quantization of conductance close to multiples of G0 = 2e2/h. At the same time, conductance plateaux at G0/2 and a split zero-bias anomaly in non-equilibrium transport suggest conduction via spin-polarized states in the presence of an electron-electron interaction.

Quantized edge modes in atomic-scale point contacts in graphene.

PubMed

Kinikar, Amogh; Phanindra Sai, T; Bhattacharyya, Semonti; Agarwala, Adhip; Biswas, Tathagata; Sarker, Sanjoy K; Krishnamurthy, H R; Jain, Manish; Shenoy, Vijay B; Ghosh, Arindam

2017-07-01

The zigzag edges of single- or few-layer graphene are perfect one-dimensional conductors owing to a set of gapless states that are topologically protected against backscattering. Direct experimental evidence of these states has been limited so far to their local thermodynamic and magnetic properties, determined by the competing effects of edge topology and electron-electron interaction. However, experimental signatures of edge-bound electrical conduction have remained elusive, primarily due to the lack of graphitic nanostructures with low structural and/or chemical edge disorder. Here, we report the experimental detection of edge-mode electrical transport in suspended atomic-scale constrictions of single and multilayer graphene created during nanomechanical exfoliation of highly oriented pyrolytic graphite. The edge-mode transport leads to the observed quantization of conductance close to multiples of G 0  = 2e 2 /h. At the same time, conductance plateaux at G 0 /2 and a split zero-bias anomaly in non-equilibrium transport suggest conduction via spin-polarized states in the presence of an electron-electron interaction.

Isolating and moving single atoms using silicon nanocrystals

DOEpatents

Carroll, Malcolm S.

2010-09-07

A method is disclosed for isolating single atoms of an atomic species of interest by locating the atoms within silicon nanocrystals. This can be done by implanting, on the average, a single atom of the atomic species of interest into each nanocrystal, and then measuring an electrical charge distribution on the nanocrystals with scanning capacitance microscopy (SCM) or electrostatic force microscopy (EFM) to identify and select those nanocrystals having exactly one atom of the atomic species of interest therein. The nanocrystals with the single atom of the atomic species of interest therein can be sorted and moved using an atomic force microscope (AFM) tip. The method is useful for forming nanoscale electronic and optical devices including quantum computers and single-photon light sources.

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

Lutzer, B.; Simsek, S.; Zimmermann, C.

In order to improve the electrical behaviour of metal-insulator-metal capacitors with ZrO{sub 2} insulator grown by Atomic Layer Deposition, the influence of the insertion of interfacial Cr layers between Pt electrodes and the zirconia is investigated. An improvement of the α-voltage coefficient of capacitance as low as 567 ppm/V{sup 2} is achieved for a single layer of Cr while maintaining a high capacitance density of 10.7 fF/μm{sup 2} and a leakage current of less than 1.2 × 10{sup −8} A/cm{sup 2} at +1 V. The role of the interface is discussed by means of X-ray photoelectron spectroscopy and high-resolution transmission electron microscopy showing themore » formation of Zr stabilized chromia oxide phase with a dielectric constant of 16.« less

Probing the dielectric response of the interfacial buffer layer in epitaxial graphene via optical spectroscopy

NASA Astrophysics Data System (ADS)

Hill, Heather M.; Rigosi, Albert F.; Chowdhury, Sugata; Yang, Yanfei; Nguyen, Nhan V.; Tavazza, Francesca; Elmquist, Randolph E.; Newell, David B.; Hight Walker, Angela R.

2017-11-01

Monolayer epitaxial graphene (EG) is a suitable candidate for a variety of electronic applications. One advantage of EG growth on the Si face of SiC is that it develops as a single crystal, as does the layer below, referred to as the interfacial buffer layer (IBL), whose properties include an electronic band gap. Although much research has been conducted to learn about the electrical properties of the IBL, not nearly as much work has been reported on the optical properties of the IBL. In this work, we combine measurements from Mueller matrix ellipsometry, differential reflectance contrast, atomic force microscopy, and Raman spectroscopy, as well as calculations from Kramers-Kronig analyses and density-functional theory, to determine the dielectric function of the IBL within the energy range of 1 eV to 8.5 eV.

IBIC characterisation of novel detectors for single atom doping of quantum computer devices

NASA Astrophysics Data System (ADS)

Yang, Changyi; Jamieson, David N.; Pakes, Chris I.; George, Damien P.; Hearne, Sean M.; Dzurak, Andrew S.; Gauja, Eric; Stanley, F.; Clark, R. G.

2003-09-01

Single ion implantation and online detection is highly desirable for the emerging application, in which single 31P ions need to be inserted in prefabricated silicon cells to construct solid-state quantum bits (qubits). In order to fabricate qubit arrays, we have developed novel detectors that employ detector electrodes adjacent to the prefabricated cells that can detect single keV ion strikes appropriate for the fabrication of shallow phosphorus arrays. The method utilises a high purity silicon substrate with very high resistivity, a thin SiO 2 surface layer, nanometer masks for the lateral positioning single phosphorus implantation, biased electrodes applied to the surface of the silicon and sensitive electronics that can detect the charge transient from single keV ion strikes. A TCAD (Technology Computer Aided Design) software package was applied in the optimisation of the device design and simulation of the detector performance. Here we show the characterisation of these detectors using ion beam induced charge (IBIC) with a focused 2 MeV He ions in a nuclear microprobe. The IBIC imaging method in a nuclear microprobe allowed us to measure the dead-layer thickness of the detector structure (required to be very thin for successful detection of keV ions), and the spatial distribution of the charge collection efficiency around the entire region of the detector. We show that our detectors have near 100% charge collection efficiency for MeV ions, extremely thin dead-layer thickness (about 7 nm) and a wide active region extending laterally from the electrodes (10-20 μm) where qubit arrays can be constructed. We demonstrate that the device can be successfully applied in the detection of keV ionisation energy from single events of keV X-rays and keV 31P ions.

Coherent single-atom superradiance

NASA Astrophysics Data System (ADS)

Kim, Junki; Yang, Daeho; Oh, Seung-hoon; An, Kyungwon

2018-02-01

Superradiance is a quantum phenomenon emerging in macroscopic systems whereby correlated single atoms cooperatively emit photons. Demonstration of controlled collective atom-field interactions has resulted from the ability to directly imprint correlations with an atomic ensemble. Here we report cavity-mediated coherent single-atom superradiance: Single atoms with predefined correlation traverse a high–quality factor cavity one by one, emitting photons cooperatively with the N atoms that have already gone through the cavity (N represents the number of atoms). Enhanced collective photoemission of N-squared dependence was observed even when the intracavity atom number was less than unity. The correlation among single atoms was achieved by nanometer-precision position control and phase-aligned state manipulation of atoms by using a nanohole-array aperture. Our results demonstrate a platform for phase-controlled atom-field interactions.

Electroplating and magnetostructural characterization of multisegmented Co54Ni46/Co85Ni15 nanowires from single electrochemical bath in anodic alumina templates

PubMed Central

2013-01-01

Highly hexagonally ordered hard anodic aluminum oxide membranes, which have been modified by a thin cover layer of SiO2 deposited by atomic layer deposition method, were used as templates for the synthesis of electrodeposited magnetic Co-Ni nanowire arrays having diameters of around 180 to 200 nm and made of tens of segments with alternating compositions of Co54Ni46 and Co85Ni15. Each Co-Ni single segment has a mean length of around 290 nm for the Co54Ni46 alloy, whereas the length of the Co85Ni15 segments was around 430 nm. The composition and crystalline structure of each Co-Ni nanowire segment were determined by transmission electron microscopy and selected area electron diffraction techniques. The employed single-bath electrochemical nanowire growth method allows for tuning both the composition and crystalline structure of each individual Co-Ni segment. The room temperature magnetic behavior of the multisegmented Co-Ni nanowire arrays is also studied and correlated with their structural and morphological properties. PMID:23735184

Insights into the Interactions of Amino Acids and Peptides with Inorganic Materials Using Single-Molecule Force Spectroscopy.

PubMed

Das, Priyadip; Duanias-Assaf, Tal; Reches, Meital

2017-03-06

The interactions between proteins or peptides and inorganic materials lead to several interesting processes. For example, combining proteins with minerals leads to the formation of composite materials with unique properties. In addition, the undesirable process of biofouling is initiated by the adsorption of biomolecules, mainly proteins, on surfaces. This organic layer is an adhesion layer for bacteria and allows them to interact with the surface. Understanding the fundamental forces that govern the interactions at the organic-inorganic interface is therefore important for many areas of research and could lead to the design of new materials for optical, mechanical and biomedical applications. This paper demonstrates a single-molecule force spectroscopy technique that utilizes an AFM to measure the adhesion force between either peptides or amino acids and well-defined inorganic surfaces. This technique involves a protocol for attaching the biomolecule to the AFM tip through a covalent flexible linker and single-molecule force spectroscopy measurements by atomic force microscope. In addition, an analysis of these measurements is included.

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

Ren, Xiaochen; Singh, Arunima K.; Fang, Lei

Impurity doping in two-dimensional (2D) materials can provide a route to tuning electronic properties, so it is important to be able to determine the distribution of dopant atoms within and between layers. Here we report the totnographic mapping of dopants in layered 2D materials with atomic sensitivity and subnanometer spatial resolution using atom, probe tomography (APT). Also, APT analysis shows that Ag dopes both Bi 2Se 3 and PbSe layers in (PbSe) 5(Bi 2Se 3) 3, and correlations :in the position of Ag atoms suggest a pairing across neighboring Bi 2Se 3 and PbSe layers. Finally, density functional theory (DFT)more » calculations confirm the favorability of substitutional-doping for both Pb and Bi and provide insights into the,observed spatial correlations in dopant locations.« less

Atomic force microscopy based nanoindentation study of onion abaxial epidermis walls in aqueous environment

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

Xi, Xiaoning; Tittmann, Bernhard; Kim, Seong H.

An atomic force microscopy based nanoindentation method was employed to study how the structure of cellulose microfibril packing and matrix polymers affect elastic modulus of fully hydrated primary plant cell walls. The isolated, single-layered abaxial epidermis cell wall of an onion bulb was used as a test system since the cellulose microfibril packing in this cell wall is known to vary systematically from inside to outside scales and the most abundant matrix polymer, pectin, can easily be altered through simple chemical treatments such as ethylenediaminetetraacetic acid and calcium ions. Experimental results showed that the pectin network variation has significant impactsmore » on the cell wall modulus, and not the cellulose microfibril packing.« less

Thermal effects in equilibrium surface segregation in a copper/10-atomic-percent-aluminum alloy using Auger electron spectroscopy

NASA Technical Reports Server (NTRS)

Ferrante, J.

1972-01-01

Equilibrium surface segregation of aluminum in a copper-10-atomic-percent-aluminum single crystal alloy oriented in the /111/ direction was demonstrated by using Auger electron spectroscopy. This crystal was in the solid solution range of composition. Equilibrium surface segregation was verified by observing that the aluminum surface concentration varied reversibly with temperature in the range 550 to 850 K. These results were curve fitted to an expression for equilibrium grain boundary segregation and gave a retrieval energy of 5780 J/mole (1380 cal/mole) and a maximum frozen-in surface coverage three times the bulk layer concentration. Analyses concerning the relative merits of sputtering calibration and the effects of evaporation are also included.

Graphenes in the absence of metals as carbocatalysts for selective acetylene hydrogenation and alkene hydrogenation

NASA Astrophysics Data System (ADS)

Primo, Ana; Neatu, Florentina; Florea, Mihaela; Parvulescu, Vasile; Garcia, Hermenegildo

2014-10-01

Catalysis makes possible a chemical reaction by increasing the transformation rate. Hydrogenation of carbon-carbon multiple bonds is one of the most important examples of catalytic reactions. Currently, this type of reaction is carried out in petrochemistry at very large scale, using noble metals such as platinum and palladium or first row transition metals such as nickel. Catalysis is dominated by metals and in many cases by precious ones. Here we report that graphene (a single layer of one-atom-thick carbon atoms) can replace metals for hydrogenation of carbon-carbon multiple bonds. Besides alkene hydrogenation, we have shown that graphenes also exhibit high selectivity for the hydrogenation of acetylene in the presence of a large excess of ethylene.

Direct synthesis of ultrathin SOI structure by extremely low-energy oxygen implantation

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

Hoshino, Yasushi, E-mail: yhoshino@kanagawa-u.ac.jp; Yachida, Gosuke; Inoue, Kodai

2016-06-15

We performed extremely low-energy {sup 16}O{sup +} implantation at 10 keV (R{sub p} ∼ 25 nm) followed by annealing aiming at directly synthesizing an ultrathin Si layer separated by a buried SiO{sub 2} layer in Si(001) substrates, and then investigated feasible condition of recrystallization and stabilization of the superficial Si and the buried oxide layer by significantly low temperature annealing. The elemental compositions were analyzed by Rutherford backscattering (RBS) and secondary ion mass spectroscopy (SIMS). The crystallinity of the superficial Si layer was quantitatively confirmed by ananlyzing RBS-channeling spectra. Cross-sectional morphologies and atomic configurations were observed by transmission electron microscopemore » (TEM). As a result, we succeeded in directly synthesizing an ultrathin single-crystalline silicon layer with ≤20 nm thick separated by a thin buried stoichiometric SiO{sub 2} layer with ≤20 nm thick formed by extremely low-energy {sup 16}O{sup +} implantation followed by surprisingly low temperature annealing at 1050{sup ∘} C.« less

Origins of Moiré Patterns in CVD-grown MoS2 Bilayer Structures at the Atomic Scales.

PubMed

Wang, Jin; Namburu, Raju; Dubey, Madan; Dongare, Avinash M

2018-06-21

The chemical vapor deposition (CVD)-grown two-dimensional molybdenum disulfide (MoS 2 ) structures comprise of flakes of few layers with different dimensions. The top layers are relatively smaller in size than the bottom layers, resulting in the formation of edges/steps across adjacent layers. The strain response of such few-layer terraced structures is therefore likely to be different from exfoliated few-layered structures with similar dimensions without any terraces. In this study, the strain response of CVD-grown few-layered MoS 2 terraced structures is investigated at the atomic scales using classic molecular dynamics (MD) simulations. MD simulations suggest that the strain relaxation of CVD-grown triangular terraced structures is observed in the vertical displacement of the atoms across the layers that results in the formation of Moiré patterns. The Moiré islands are observed to nucleate at the corners or edges of the few-layered structure and propagate inwards under both tensile and compressive strains. The nucleation of these islands is observed to happen at tensile strains of ~ 2% and at compressive strains of ~2.5%. The vertical displacements of the atoms and the dimensions of the Moiré islands predicted using the MD simulation are in excellent agreement with that observed experimentally.

Detailed line shape analysis of the C KVV Auger peak of two carbon allotropes measured using a time of flight positron annihilation induced Auger electron spectrometer

NASA Astrophysics Data System (ADS)

Fairchild, A. J.; Chirayath, V. A.; Chrysler, M. D.; Gladen, R. W.; Imam, S. K.; Koymen, A. R.; Weiss, A. H.

We report a detailed line shape analysis of the positron induced C KVV Auger line shape from highly oriented pyrolytic graphite (HOPG) and a single layer of graphene grown on polycrystalline Cu. A model consisting of the self-fold of the one-electron density of states including terms for hole-hole interactions, charge screening effects, and intrinsic loss mechanisms is compared to experimental C KVV line shapes measured using a positron induced Auger electron spectrometer (PAES). In traditional Auger spectroscopies which use an electron or photon to initiate the Auger process, extracting the relatively small Auger signal from the large secondary background can be quite difficult. Using a very low energy positron beam to create the core hole through an anti-matter matter annihilation entirely eliminates this background. Additionally, PAES has sensitivity to the top most atomic layer since the positron becomes trapped in an image potential well at the surface before annihilation. Therefore, the PAES signal from a single layer of graphene on polycrystalline Cu is primarily from the graphene overlayer with small contributions from the Cu substrate while the PAES signal from HOPG can be viewed as a single graphene layer with a graphite substrate. The influence of these two substrates on C KVV line shape is discussed. This work was supported by NSF Grant No. DMR 1508719 and DMR 1338130.

Improving Osteoblast Response In Vitro by a Nanostructured Thin Film with Titanium Carbide and Titanium Oxides Clustered around Graphitic Carbon.

PubMed

Longo, Giovanni; Ioannidu, Caterina Alexandra; Scotto d'Abusco, Anna; Superti, Fabiana; Misiano, Carlo; Zanoni, Robertino; Politi, Laura; Mazzola, Luca; Iosi, Francesca; Mura, Francesco; Scandurra, Roberto

2016-01-01

Recently, we introduced a new deposition method, based on Ion Plating Plasma Assisted technology, to coat titanium implants with a thin but hard nanostructured layer composed of titanium carbide and titanium oxides, clustered around graphitic carbon. The nanostructured layer has a double effect: protects the bulk titanium against the harsh conditions of biological tissues and in the same time has a stimulating action on osteoblasts. The aim of this work is to describe the biological effects of this layer on osteoblasts cultured in vitro. We demonstrate that the nanostructured layer causes an overexpression of many early genes correlated to proteins involved in bone turnover and an increase in the number of surface receptors for α3β1 integrin, talin, paxillin. Analyses at single-cell level, by scanning electron microscopy, atomic force microscopy, and single cell force spectroscopy, show how the proliferation, adhesion and spreading of cells cultured on coated titanium samples are higher than on uncoated titanium ones. Finally, the chemistry of the layer induces a better formation of blood clots and a higher number of adhered platelets, compared to the uncoated cases, and these are useful features to improve the speed of implant osseointegration. In summary, the nanostructured TiC film, due to its physical and chemical properties, can be used to protect the implants and to improve their acceptance by the bone.

4H-SiC p i n diodes grown by sublimation epitaxy in vacuum (SEV) and their application as microwave diodes

NASA Astrophysics Data System (ADS)

Camara, N.; Zekentes, K.; Zelenin, V. V.; Abramov, P. L.; Kirillov, A. V.; Romanov, L. P.; Boltovets, N. S.; Krivutsa, V. A.; Thuaire, A.; Bano, E.; Tsoi, E.; Lebedev, A. A.

2008-02-01

Sublimation epitaxy under vacuum (SEV) was investigated as a method for growing 4H-SiC epitaxial structures for p-i-n diode fabrication. The SEV-grown 4H-SiC material was investigated with scanning electron microscopy (SEM), atomic force microscopy (AFM), x-ray diffraction, photo-luminescence spectroscopy (PL), cathodo-luminescence (CL) spectroscopy, photocurrent method for carrier diffusion length determination, electro-luminescence microscopy (EL), deep level transient spectroscopy (DLTS), C-V profiling and Hall-effect measurements. When possible, the same investigation techniques were used in parallel with similar layers grown by chemical vapour deposition (CVD) epitaxy and the physical properties of the two kind of epitaxied layers were compared. p-i-n diodes were fabricated in parallel on SEV and CVD-grown layers and showed close electrical performances in dc mode in term of capacitance, resistance and transient time switching, despite the lower mobility and the diffusion length of the SEV-grown layers. X-band microwave switches based on the SEV-grown p-i-n diodes have been demonstrated with insertion loss lower than 4 dB and an isolation higher than 17 dB. These single-pole single-throw (SPST) switches were able to handle a pulsed power up to 1800 W in isolation mode, similar to the value obtained with switches incorporating diodes with CVD-grown layers.

Synthesis, structure, and bonding in K12Au21Sn4. A polar intermetallic compound with dense Au20 and open AuSn4 layers.

PubMed

Li, Bin; Kim, Sung-Jin; Miller, Gordon J; Corbett, John D

2009-12-07

The new phase K(12)Au(21)Sn(4) has been synthesized by direct reaction of the elements at elevated temperatures. Single crystal X-ray diffraction established its orthorhombic structure, space group Pmmn (No. 59), a = 12.162(2); b = 18.058(4); c = 8.657(2) A, V = 1901.3(7) A(3), and Z = 2. The structure consists of infinite puckered sheets of vertex-sharing gold tetrahedra (Au(20)) that are tied together by thin layers of alternating four-bonded-Sn and -Au atoms (AuSn(4)). Remarkably, the dense but electron-poorer blocks of Au tetrahedra coexist with more open and saturated Au-Sn layers, which are fragments of a zinc blende type structure that maximize tetrahedral heteroatomic bonding outside of the network of gold tetrahedra. LMTO band structure calculations reveal metallic properties and a pseudogap at 256 valence electrons per formula unit, only three electrons fewer than in the title compound and at a point at which strong Au-Sn bonding is optimized. Additionally, the tight coordination of the Au framework atoms by K plays an important bonding role: each Au tetrahedra has 10 K neighbors and each K atom has 8-12 Au contacts. The appreciably different role of the p element Sn in this structure from that in the triel members in K(3)Au(5)In and Rb(2)Au(3)Tl appears to arise from its higher electron count which leads to better p-bonding (valence electron concentrations = 1.32 versus 1.22).

Polymerization of a divalent/tetravalent metal-storing atom-mimicking dendrimer.

PubMed

Albrecht, Ken; Hirabayashi, Yuki; Otake, Masaya; Mendori, Shin; Tobari, Yuta; Azuma, Yasuo; Majima, Yutaka; Yamamoto, Kimihisa

2016-12-01

The phenylazomethine dendrimer (DPA) has a layer-by-layer electron density gradient that is an analog of the Bohr atom (atom mimicry). In combination with electron pair mimicry, the polymerization of this atom-mimicking dendrimer was achieved. The valency of the mimicked atom was controlled by changing the chemical structure of the dendrimer. By mimicking a divalent atom, a one-dimensional (1D) polymer was obtained, and by using a planar tetravalent atom mimic, a 2D polymer was obtained. These poly(dendrimer) polymers could store Lewis acids (SnCl 2 ) in their unoccupied orbitals, thus indicating that these poly(dendrimer) polymers consist of a series of nanocontainers.

Adhesion-dependent negative friction coefficient on chemically modified graphite at the nanoscale

NASA Astrophysics Data System (ADS)

Deng, Zhao; Smolyanitsky, Alex; Li, Qunyang; Feng, Xi-Qiao; Cannara, Rachel J.

2012-12-01

From the early tribological studies of Leonardo da Vinci to Amontons’ law, friction has been shown to increase with increasing normal load. This trend continues to hold at the nanoscale, where friction can vary nonlinearly with normal load. Here we present nanoscale friction force microscopy (FFM) experiments for a nanoscale probe tip sliding on a chemically modified graphite surface in an atomic force microscope (AFM). Our results demonstrate that, when adhesion between the AFM tip and surface is enhanced relative to the exfoliation energy of graphite, friction can increase as the load decreases under tip retraction. This leads to the emergence of an effectively negative coefficient of friction in the low-load regime. We show that the magnitude of this coefficient depends on the ratio of tip-sample adhesion to the exfoliation energy of graphite. Through both atomistic- and continuum-based simulations, we attribute this unusual phenomenon to a reversible partial delamination of the topmost atomic layers, which then mimic few- to single-layer graphene. Lifting of these layers with the AFM tip leads to greater deformability of the surface with decreasing applied load. This discovery suggests that the lamellar nature of graphite yields nanoscale tribological properties outside the predictive capacity of existing continuum mechanical models.

High-precision measurement of magnetic penetration depth in superconducting films

DOE PAGES

He, X.; Gozar, A.; Sundling, R.; ...

2016-11-01

We report that the magnetic penetration depth (λ) in thin superconducting films is usually measured by the mutual inductance technique. The accuracy of this method has been limited by uncertainties in the geometry of the solenoids and in the film position and thickness, by parasitic coupling between the coils, etc. Here, we present several improvements in the apparatus and the method. To ensure the precise thickness of the superconducting layer, we engineer the films at atomic level using atomic-layer-by-layer molecular beam epitaxy. In this way, we also eliminate secondary-phase precipitates, grain boundaries, and pinholes that are common with other depositionmore » methods and that artificially increase the field transmission and thus the apparent λ. For better reproducibility, the thermal stability of our closed-cycle cryocooler used to control the temperature of the mutual inductance measurement has been significantly improved by inserting a custom-built thermal conductivity damper. Next, to minimize the uncertainties in the geometry, we fused a pair of small yet precisely wound coils into a single sapphire block machined to a high precision. Lastly, the sample is spring-loaded to exactly the same position with respect to the solenoids. Altogether, we can measure the absolute value of λ with the accuracy better than ±1%.« less

Stability of surface and subsurface hydrogen on and in Au/Ni near-surface alloys

DOE PAGES

Celik, Fuat E.; Mavrikakis, Manos

2015-01-12

Periodic, self-consistent DFT-GGA (PW91) calculations were used to study the interaction of hydrogen atoms with the (111) surfaces of substitutional near-surface alloys (NSAs) of Au and Ni with different surface layer compositions and different arrangements of Au atoms in the surface layer. The effect of hydrogen adsorption on the surface and in the first and second subsurface layers of the NSAs was studied. Increasing the Au content in the surface layer weakens hydrogen binding on the surface, but strengthens subsurface binding, suggesting that the distribution of surface and subsurface hydrogen will be different than that on pure Ni(111). While themore » metal composition of the surface layer has an effect on the binding energy of hydrogen on NSA surfaces, the local composition of the binding site has a stronger effect. For example, fcc hollow sites consisting of three Ni atoms bind H nearly as strongly as on Ni(111), and fcc sites consisting of three Au atoms bind H nearly as weakly as on Au(111). Sites with one or two Au atoms show intermediate binding energies. The preference of hydrogen for three-fold Ni hollow sites alters the relative stabilities of different surface metal atom arrangements, and may provide a driving force for adsorbate-induced surface rearrangement.« less

Stability of Surface and Subsurface Hydrogen on and in Au/Ni Near-Surface Alloys

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

Celik, Fuat E.; Mavrikakis, Manos

2015-10-01

Periodic, self-consistent DFT-GGA (PW91) calculations were used to study the interaction of hydrogen atoms with the (111) surfaces of substitutional near-surface alloys (NSAs) of Au and Ni with different surface layer compositions and different arrangements of Au atoms in the surface layer. The effect of hydrogen adsorption on the surface and in the first and second subsurface layers of the NSAs was studied. Increasing the Au content in the surface layer weakens hydrogen binding on the surface, but strengthens subsurface binding, suggesting that the distribution of surface and subsurface hydrogen will be different than that on pure Ni(111). While themore » metal composition of the surface layer has an effect on the binding energy of hydrogen on NSA surfaces, the local composition of the binding site has a stronger effect. For example, fcc hollow sites consisting of three Ni atoms bind H nearly as strongly as on Ni(111), and fcc sites consisting of three Au atoms bind H nearly as weakly as on Au(111). Sites with one or two Au atoms show intermediate binding energies. The preference of hydrogen for three-fold Ni hollow sites alters the relative stabilities of different surface metal atom arrangements, and may provide a driving force for adsorbate-induced surface rearrangement.« less

Stability of surface and subsurface hydrogen on and in Au/Ni near-surface alloys

NASA Astrophysics Data System (ADS)

Celik, Fuat E.; Mavrikakis, Manos

2015-10-01

Periodic, self-consistent DFT-GGA (PW91) calculations were used to study the interaction of hydrogen atoms with the (111) surfaces of substitutional near-surface alloys (NSAs) of Au and Ni with different surface layer compositions and different arrangements of Au atoms in the surface layer. The effect of hydrogen adsorption on the surface and in the first and second subsurface layers of the NSAs was studied. Increasing the Au content in the surface layer weakens hydrogen binding on the surface, but strengthens subsurface binding, suggesting that the distribution of surface and subsurface hydrogen will be different than that on pure Ni(111). While the metal composition of the surface layer has an effect on the binding energy of hydrogen on NSA surfaces, the local composition of the binding site has a stronger effect. For example, fcc hollow sites consisting of three Ni atoms bind H nearly as strongly as on Ni(111), and fcc sites consisting of three Au atoms bind H nearly as weakly as on Au(111). Sites with one or two Au atoms show intermediate binding energies. The preference of hydrogen for three-fold Ni hollow sites alters the relative stabilities of different surface metal atom arrangements, and may provide a driving force for adsorbate-induced surface rearrangement.