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Tunable plasmonic lattices of silver nanocrystals

Description: Silver nanocrystals are ideal building blocks for plasmonicmaterials that exhibit a wide range of unique and potentially usefuloptical phenomena. Individual nanocrystals display distinct opticalscattering spectra and can be assembled into hierarchical structures thatcouple strongly to external electromagnetic fields. This coupling, whichis mediated by surface plasmons, depends on their shape and arrangement.Here we demonstrate the bottom-up assembly of polyhedral silvernanocrystals into macroscopic two-dimensional superlattices using theLangmuir-Blodgett technique. Our ability to control interparticlespacing, density, and packing symmetry allows for tunability of theoptical response over the entire visible range. This assembly strategyoffers a new, practical approach to making novel plasmonic materials forapplication in spectroscopic sensors, sub-wavelength optics, andintegrated devices that utilize field enhancement effects.
Date: February 18, 2008
Creator: Tao, Andrea; Sinsermsuksakul, Prasert & Yang, Peidong
Partner: UNT Libraries Government Documents Department

Multinozzle Emitter Arrays for Nanoelectrospray Mass Spectrometry

Description: Mass spectrometry (MS) is the enabling technology for proteomics and metabolomics. However, dramatic improvements in both sensitivity and throughput are still required to achieve routine MS-based single cell proteomics and metabolomics. Here, we report the silicon-based monolithic multinozzle emitter array (MEA), and demonstrate its proof-of-principle applications in high-sensitivity and high-throughput nanoelectrospray mass spectrometry. Our MEA consists of 96 identical 10-nozzle emitters in a circular array on a 3-inch silicon chip. The geometry and configuration of the emitters, the dimension and number of the nozzles, and the micropillar arrays embedded in the main channel, can be systematically and precisely controlled during the microfabrication process. Combining electrostatic simulation and experimental testing, we demonstrated that sharpened-end geometry at the stem of the individual multinozzle emitter significantly enhanced the electric fields at its protruding nozzle tips, enabling sequential nanoelectrospray for the high-density emitter array. We showed that electrospray current of the multinozzle emitter at a given total flow rate was approximately proportional to the square root of the number of its spraying-nozzles, suggesting the capability of high MS sensitivity for multinozzle emitters. Using a conventional Z-spray mass spectrometer, we demonstrated reproducible MS detection of peptides and proteins for serial MEA emitters, achieving sensitivity and stability comparable to the commercial capillary emitters. Our robust silicon-based MEA chip opens up the possibility of a fully-integrated microfluidic system for ultrahigh-sensitivity and ultrahigh-throughput proteomics and metabolomics.
Date: June 16, 2011
Creator: Mao, Pan; Wang, Hung-Ta; Yang, Peidong & Wang, Daojing
Partner: UNT Libraries Government Documents Department

Semiconductor Nanowires: What's Next?

Description: In this perspective, we take a critical look at the research progress within the nanowire community for the past decade. We discuss issues on the discovery of fundamentally new phenomena versus performance benchmarking for many of the nanowire applications. We also notice that both the bottom-up and top-down approaches have played important roles in advancing our fundamental understanding of this new class of nanostructures. Finally we attempt to look into the future and offer our personal opinions on what the future trends will be in nanowire research.
Date: April 28, 2010
Creator: Yang, Peidong; Yan, Ruoxue & Fardy, Melissa
Partner: UNT Libraries Government Documents Department

High Density n-Si/n-TiO2 Core/Shell Nanowire Arrays with Enhanced Photoactivity

Description: There are currently great needs to develop low-cost inorganic materials that can efficiently perform solar water splitting as photoelectrolysis of water into hydrogen and oxygen has significant potential to provide clean energy. We investigate the Si/TiO2 nanowire heterostructures to determine their potential for the photooxidation of water. We observed that highly dense Si/TiO2 core/shell nanowire arrays enhanced the photocurrent by 2.5 times compared to planar Si/TiO2 structure due to their low reflectance and high surface area. We also showed that n-Si/n-TiO2 nanowire arrays exhibited a larger photocurrent and open circuit voltage than p-Si/n-TiO2 nanowires due to a barrier at the heterojunction.
Date: November 15, 2008
Creator: Hwang, Yun Jeong; Boukai, Akram & Yang, Peidong
Partner: UNT Libraries Government Documents Department

Nanowire-based All Oxide Solar Cells

Description: We present an all-oxide solar cell fabricated from vertically oriented zinc oxide nanowires and cuprous oxide nanoparticles. Our solar cell consists of vertically oriented n-type zinc oxide nanowires, surrounded by a film constructed from p-type cuprous oxide nanoparticles. Our solution-based synthesis of inexpensive and environmentally benign oxide materials in a solar cell would allow for the facile production of large-scale photovoltaic devices. We found that the solar cell performance is enhanced with the addition of an intermediate oxide insulating layer between the nanowires and the nanoparticles. This observation of the important dependence of the shunt resistance on the photovoltaic performance is widely applicable to any nanowire solar cell constructed with the nanowire array in direct contact with one electrode.
Date: December 7, 2008
Creator: Yang*, Benjamin D. Yuhas and Peidong & Yang, Peidong
Partner: UNT Libraries Government Documents Department

Localized Pd Overgrowth on Cubic Pt Nanocrystals for Enhanced Electrocatalytic Oxidation of Formic Acid

Description: Single crystalline surface such as (100), (111), (110) has been studied as an idealized platform for electrocatalytic reactions since the atomic arrangement affects a catalytic property. The secondary metal deposition on these surfaces also alters the catalytic property often showing improvement such as poisoning decrease. On the other hand, electrocatalysts used for practical purpose usually have a size on the order of nanometers. Therefore, linking the knowledge from single crystalline studies to nanoparticle catalysts is of enormous importance. Recently, the Pt nanoparticles which surface structure was preferentially oriented was synthesized and used as electrocatalysts. Here, we demonstrate a rational design of a binary metallic nanocatalyst based on the single crystalline study.
Date: December 14, 2007
Creator: Lee, Hyunjoo; Habas, Susan; Somorjai, Gabor & Yang, Peidong
Partner: UNT Libraries Government Documents Department

Single crystalline mesoporous silicon nanowires

Description: Herein we demonstrate a novel electroless etching synthesis of monolithic, single-crystalline, mesoporous silicon nanowire arrays with a high surface area and luminescent properties consistent with conventional porous silicon materials. The photoluminescence of these nanowires suggest they are composed of crystalline silicon with small enough dimensions such that these arrays may be useful as photocatalytic substrates or active components of nanoscale optoelectronic devices. A better understanding of this electroless route to mesoporous silicon could lead to facile and general syntheses of different narrow bandgap semiconductor nanostructures for various applications.
Date: August 18, 2009
Creator: Hochbaum, Allon; Dargas, Daniel; Hwang, Yun Jeong & Yang, Peidong
Partner: UNT Libraries Government Documents Department

Shaping metal nanocrystals through epitaxial seeded growth

Description: Morphological control of nanocrystals has becomeincreasingly important, as many of their physical and chemical propertiesare highly shape-dependent. Nanocrystal shape control for both single andmultiple material systems, however, remains fairly empirical andchallenging. New methods need to be explored for the rational syntheticdesign of heterostructures with controlled morphology. Overgrowth of adifferent material on well-faceted seeds, for example, allows for the useof the defined seed morphology to control nucleation and growth of thesecondary structure. Here, we have used highly faceted cubic Pt seeds todirect the epitaxial overgrowth of a secondary metal. We demonstrate thisconcept with lattice matched Pd to produce conformal shape-controlledcore-shell particles, and then extend it to lattice mismatched Au to giveanisotropic growth. Seeding with faceted nanocrystals may havesignificant potential towards the development of shape-controlledheterostructures with defined interfaces.
Date: February 17, 2008
Creator: Habas, Susan E.; Lee, Hyunjoo; Radmilovic, Velimir; Somorjai,Gabor A. & Yang, Peidong
Partner: UNT Libraries Government Documents Department

Sythesis of metal sulfide nanomaerials via thermal decomposition of single-source percursors

Description: In this report, we present a synthetic method for the formation of cuprous sulfide (Cu2S) and lead sulfide (PbS) nanomaterials directly on substrates from the thermolysis of single-source precursors. We find that the final morphology and arrangement of the nanomaterials may be controlled through the concentration of the dissolved precursors and choice of solvent. One-dimensional (1-D) morphologies may also be grown onto substrates with the addition of a metal catalyst layer through solution-liquid-solid (SLS) growth. These synthetic techniques may be expanded to other metal sulfide materials.
Date: June 3, 2010
Creator: Jen-La Plante, Ilan; Zeid, Tahani W.; Yang, Peidong & Mokari, Taleb
Partner: UNT Libraries Government Documents Department

Single crystalline mesoporous silicon nanowires

Description: Herein we demonstrate a novel electroless etching synthesis of monolithic, single-crystalline, mesoporous silicon nanowire arrays with a high surface area and luminescent properties consistent with conventional porous silicon materials. These porous nanowires also retain the crystallographic orientation of the wafer from which they are etched. Electron microscopy and diffraction confirm their single-crystallinity and reveal the silicon surrounding the pores is as thin as several nanometers. Confocal fluorescence microscopy showed that the photoluminescence (PL) of these arrays emanate from the nanowires themselves, and their PL spectrum suggests that these arrays may be useful as photocatalytic substrates or active components of nanoscale optoelectronic devices.
Date: August 4, 2009
Creator: Hochbaum, A.I.; Gargas, Daniel; Jeong Hwang, Yun & Yang, Peidong
Partner: UNT Libraries Government Documents Department

Room-temperature Formation of Hollow Cu2O Nanoparticles

Description: Monodisperse Cu and Cu2O nanoparticles (NPs) are synthesized using tetradecylphosphonic acid as a capping agent. Dispersing the NPs in chloroform and hexane at room temperature results in the formation of hollow Cu2O NPs and Cu@Cu2O core/shell NPs, respectively. The monodisperse Cu2O NPs are used to fabricate hybrid solar cells with efficiency of 0.14percent under AM 1.5 and 1 Sun illumination.
Date: January 18, 2010
Creator: Hung, Ling-I; Tsung, Chia-Kuang; Huang, Wenyu & Yang, Peidong
Partner: UNT Libraries Government Documents Department

Self-assembly of uniform polyhedral silver nanocrystals into densest packings and exotic superlattices

Description: Understanding how polyhedra pack into extended arrangements is integral to the design and discovery of crystalline materials at all length scales. Much progress has been made in enumerating and characterizing the packing of polyhedral shapes, and the self-assembly of polyhedral nanocrystals into ordered superstructures. However, directing the self-assembly of polyhedral nanocrystals into densest packings requires precise control of particle shape, polydispersity,interactions and driving forces. Here we show with experiment and computer simulation that a range of nanoscale Ag polyhedra can self-assemble into their conjectured densest packings. When passivated with adsorbing polymer, the polyhedra behave as quasi-hard particles and assemble into millimetre-sized three-dimensional supercrystals by sedimentation.We also show, by inducing depletion attraction through excess polymer in solution, that octahedra form an exotic superstructure with complex helical motifs rather than the densest Minkowski lattice. Such large-scale Ag supercrystals may facilitate the design of scalable three-dimensional plasmonic metamaterials for sensing, nanophotonics, and photocatalysis.
Date: March 1, 2011
Creator: Henzie, Joel; Grunwald, Michael; Widmer-Cooper, Asaph; Geissler, Phillip L. & Yang, Peidong
Partner: UNT Libraries Government Documents Department

Near-Monodisperse Ni-Cu Bimetallic Nanocrystals of Variable Composition: Controlled Synthesis and Catalytic Activity for H2 Generation

Description: Near-monodisperse Ni{sub 1-x}Cu{sub x} (x = 0.2-0.8) bimetallic nanocrystals were synthesized by a one-pot thermolysis approach in oleylamine/1-octadecene, using metal acetylacetonates as precursors. The nanocrystals form large-area 2D superlattices, and display a catalytic synergistic effect in the hydrolysis of NaBH{sub 4} to generate H{sub 2} at x = 0.5 in a strongly basic medium. The Ni{sub 0.5}Cu{sub 0.5} nanocrystals show the lowest activation energy, and also exhibit the highest H{sub 2} generation rate at 298 K.
Date: July 22, 2008
Creator: Zhang, Yawen; Huang, Wenyu; Habas, Susan E.; Kuhn, John N.; Grass, Michael E.; Yamada, Yusuke et al.
Partner: UNT Libraries Government Documents Department

Tunable nanowire nonlinear optical probe

Description: One crucial challenge for subwavelength optics has been thedevelopment of a tunable source of coherent laser radiation for use inthe physical, information, and biological sciences that is stable at roomtemperature and physiological conditions. Current advanced near-fieldimaging techniques using fiber-optic scattering probes1,2 have alreadyachieved spatial resolution down to the 20-nm range. Recently reportedfar-field approaches for optical microscopy, including stimulatedemission depletion (STED)3, structured illumination4, and photoactivatedlocalization microscopy (PALM)5, have also enabled impressive,theoretically-unlimited spatial resolution of fluorescent biomolecularcomplexes. Previous work with laser tweezers6-8 has suggested the promiseof using optical traps to create novel spatial probes and sensors.Inorganic nanowires have diameters substantially below the wavelength ofvisible light and have unique electronic and optical properties9,10 thatmake them prime candidates for subwavelength laser and imagingtechnology. Here we report the development of an electrode-free,continuously-tunable coherent visible light source compatible withphysiological environments, from individual potassium niobate (KNbO3)nanowires. These wires exhibit efficient second harmonic generation(SHG), and act as frequency converters, allowing the local synthesis of awide range of colors via sum and difference frequency generation (SFG,DFG). We use this tunable nanometric light source to implement a novelform of subwavelength microscopy, in which an infrared (IR) laser is usedto optically trap and scan a nanowire over a sample, suggesting a widerange of potential applications in physics, chemistry, materials science,and biology.
Date: February 18, 2008
Creator: Nakayama, Yuri; Pauzauskie, Peter J.; Radenovic, Aleksandra; Onorato, Robert M.; Saykally, Richard J.; Liphardt, Jan et al.
Partner: UNT Libraries Government Documents Department

Sub-10 nm Platinum Nanocrystals with Size and Shape Control: Catalytic Study for Ethylene and Pyrrole Hydrogenation

Description: Platinum nanocubes and nanopolyhedra with tunable size from 5 to 9 nm were synthesized by controlling the reducing rate of metal precursor ions in a one-pot polyol synthesis. A two-stage process is proposed for the simultaneous control of size and shape. In the first stage, the oxidation state of the metal ion precursors determined the nucleation rate and consequently the number of nuclei. The reaction temperature controlled the shape in the second stage by regulation of the growth kinetics. These well-defined nanocrystals were loaded into MCF-17 mesoporous silica for examination of catalytic properties. Pt loadings and dispersions of the supported catalysts were determined by elemental analysis (ICP-MS) and H2 chemisorption isotherms, respectively. Ethylene hydrogenation rates over the Pt nanocrystals were independent of both size and shape and comparable to Pt single crystals. For pyrrole hydrogenation, the nanocubes enhanced ring-opening ability and thus showed a higher selectivity to n-butylamine as compared to nanopolyhedra.
Date: March 2, 2009
Creator: Tsung, Chia-Kuang; Kuhn, John N.; Huang, Wenyu; Aliaga, Cesar; Hung, Ling-I; Somorjai, Gabor A. et al.
Partner: UNT Libraries Government Documents Department

Dendrimer Templated Synthesis of One Nanometer Rh and Pt Particles Supported on Mesoporous Silica: Catalytic Activity for Ethylene and Pyrrole Hydrogenation.

Description: Monodisperse rhodium (Rh) and platinum (Pt) nanoparticles as small as {approx}1 nm were synthesized within a fourth generation polyaminoamide (PAMAM) dendrimer, a hyperbranched polymer, in aqueous solution and immobilized by depositing onto a high-surface-area SBA-15 mesoporous support. X-ray photoelectron spectroscopy indicated that the as-synthesized Rh and Pt nanoparticles were mostly oxidized. Catalytic activity of the SBA-15 supported Rh and Pt nanoparticles was studied with ethylene hydrogenation at 273 and 293 K in 10 torr of ethylene and 100 torr of H{sub 2} after reduction (76 torr of H{sub 2} mixed with 690 torr of He) at different temperatures. Catalysts were active without removing the dendrimer capping but reached their highest activity after hydrogen reduction at a moderate temperature (423 K). When treated at a higher temperature (473, 573, and 673 K) in hydrogen, catalytic activity decreased. By using the same treatment that led to maximum ethylene hydrogenation activity, catalytic activity was also evaluated for pyrrole hydrogenation.
Date: May 9, 2008
Creator: Huang, Wenyu; Kuhn, John N.; Tsung, Chia-Kuang; Zhang, Yawen; Habas, Susan E.; Yang, Peidong et al.
Partner: UNT Libraries Government Documents Department

Sum frequency generation and catalytic reaction studies of the removal of the organic capping agents from Pt nanoparticles by UV-ozone treatment

Description: We report the structure of the organic capping layers of platinum colloid nanoparticles and their removal by UV-ozone exposure. Sum frequency generation vibrational spectroscopy (SFGVS) studies identify the carbon-hydrogen stretching modes on poly(vinylpyrrolidone) (PVP) and tetradecyl tributylammonium bromide (TTAB)-capped platinum nanoparticles. We found that the UV-ozone treatment technique effectively removes the capping layer on the basis of several analytical measurements including SFGVS, X-ray photoelectron spectroscopy, and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). The overall shape of the nanoparticles was preserved after the removal of capping layers, as confirmed by transmission electron microscopy (TEM). SFGVS of ethylene hydrogenation on the clean platinum nanoparticles demonstrates the existence of ethylidyne and di-{sigma}-bonded species, indicating the similarity between single-crystal and nanoparticle systems.
Date: December 10, 2009
Creator: Aliaga, Cesar; Park, Jeong Y.; Yamada, Yusuke; Lee, Hyun Sook; Tsung, Chia-Kuang; Yang, Peidong et al.
Partner: UNT Libraries Government Documents Department

Atomic-level cotrol of the thermoelectric properties in polytypoid nanowires

Description: Thermoelectric materials have generated interest as a means of increasing the efficiency of power generation through the scavenging of waste heat. Materials containing nanometer-sized structural and compositional features can exhibit enhanced thermoelectric performance due to the decoupling of certain electrical and thermal properties, but the extent to which these features can be controlled is often limited. Here we report a simple synthesis of M{sub 2}O{sub 3}(ZnO){sub n} (M = In, Ga, Fe) nanowires with controllable polytypoid structures, where the nanostructured features are tuned by adjusting the amount of metal precursor. After the introduction of nanometer-scale features (individual atomic layers and alloying), thermal and electrical measurements on single In{sub 2-x}Ga{sub x}O3(ZnO){sub n} nanowires reveal a simultaneous improvement in all contributing factors to the thermoelectric figure of merit, indicating successful modification of the nanowire transport properties.
Date: October 23, 2010
Creator: Andrews, Sean C.; Fardy, Melissa A.; Moore, Michael C.; Aloni, Shaoul; Zhang, Minjuan; Radmilovic, Velimir et al.
Partner: UNT Libraries Government Documents Department

Holey Silicon as an Efficient Thermoelectric Material

Description: This work investigated the thermoelectric properties of thin silicon membranes that have been decorated with high density of nanoscopic holes. These ?holey silicon? (HS) structures were fabricated by either nanosphere or block-copolymer lithography, both of which are scalable for practical device application. By reducing the pitch of the hexagonal holey pattern down to 55 nm with 35percent porosity, the thermal conductivity of HS is consistently reduced by 2 orders of magnitude and approaches the amorphous limit. With a ZT value of 0.4 at room temperature, the thermoelectric performance of HS is comparable with the best value recorded in silicon nanowire system.
Date: September 30, 2010
Creator: Tang, Jinyao; Wang, Hung-Ta; Hyun Lee, Dong; Fardy, Melissa; Huo, Ziyang; Russell, Thomas P. et al.
Partner: UNT Libraries Government Documents Department

Oligo and Poly-thiophene/Zno Hybrid Nanowire Solar Cells

Description: We demonstrate the basic operation of an organic/inorganic hybrid single nanowire solar cell. End-functionalized oligo- and polythiophenes were grafted onto ZnO nanowires to produce p-n heterojunction nanowires. The hybrid nanostructures were characterized via absorption and electron microscopy to determine the optoelectronic properties and to probe the morphology at the organic/inorganic interface. Individual nanowire solar cell devices exhibited well-resolved characteristics with efficiencies as high as 0.036percent, Jsc = 0.32 mA/cm2, Voc = 0.4 V, and a FF = 0.28 under AM 1.5 illumination with 100 mW/cm2 light intensity. These individual test structures will enable detailed analysis to be carried out in areas that have been difficult to study in bulk heterojunction devices.
Date: November 3, 2009
Creator: Briseno, Alejandro L.; Holcombe, Thomas W.; Boukai, Akram I.; Garnett, Erik C.; Shelton, Steve W.; Frechet, Jean J. M. et al.
Partner: UNT Libraries Government Documents Department

Nanocrystal bilayer for tandem catalysis

Description: Supported catalysts are widely used in industry and can be optimized by tuning the composition and interface of the metal nanoparticles and oxide supports. Rational design of metal-metal oxide interfaces in nanostructured catalysts is critical to achieve better reaction activities and selectivities. We introduce here a new class of nanocrystal tandem catalysts that have multiple metal-metal oxide interfaces for the catalysis of sequential reactions. We utilized a nanocrystal bilayer structure formed by assembling platinum and cerium oxide nanocube monolayers of less than 10 nm on a silica substrate. The two distinct metal-metal oxide interfaces, CeO2-Pt and Pt-SiO2, can be used to catalyse two distinct sequential reactions. The CeO2-Pt interface catalysed methanol decomposition to produce CO and H2, which were subsequently used for ethylene hydroformylation catalysed by the nearby Pt-SiO2 interface. Consequently, propanal was produced selectively from methanol and ethylene on the nanocrystal bilayer tandem catalyst. This new concept of nanocrystal tandem catalysis represents a powerful approach towards designing high-performance, multifunctional nanostructured catalysts
Date: January 24, 2011
Creator: Yamada, Yusuke; Tsung, Chia Kuang; Huang, Wenyu; Huo, Ziyang; E.Habas, Susan E; Soejima, Tetsuro et al.
Partner: UNT Libraries Government Documents Department