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Articles 1 - 30 of 135

Full-Text Articles in Physics

Complex Oscillatory Decrease With Size In Diffusivity Of {100}-Epitaxially Supported 3d Fcc Metal Nanoclusters, King C. Lai, James W. Evans Oct 2019

Complex Oscillatory Decrease With Size In Diffusivity Of {100}-Epitaxially Supported 3d Fcc Metal Nanoclusters, King C. Lai, James W. Evans

Ames Laboratory Accepted Manuscripts

Diffusion and coalescence of supported 3D metal nanoclusters (NCs) leads to Smoluchowski Ripening (SR), a key pathway for catalyst degradation. Variation of the NC diffusion coefficient, DN, with size N (in atoms) controls SR kinetics. Traditionally, a form DN ∼ N−β was assumed consistent with mean-field analysis. However, KMC simulation of a stochastic model for diffusion of {100}-epitaxially supported fcc NCs mediated by surface diffusion reveals instead a complex oscillatory decrease of DN with N. Barriers for surface diffusion of metal atoms across and between facets, along step edges, etc., in this model are selected to accurately capture behavior ...


Nonlinearity In The Dark: Broadband Terahertz Generation With Extremely High Efficiency, Ming Fang, Nian-Hai Shen, Wei E. I. Sha, Zhixiang Huang, Thomas Koschny, Costas M. Soukoulis Jan 2019

Nonlinearity In The Dark: Broadband Terahertz Generation With Extremely High Efficiency, Ming Fang, Nian-Hai Shen, Wei E. I. Sha, Zhixiang Huang, Thomas Koschny, Costas M. Soukoulis

Ames Laboratory Accepted Manuscripts

Plasmonic metamaterials and metasurfaces offer new opportunities in developing high performance terahertz emitters and detectors beyond the limitations of conventional nonlinear materials. However, simple meta-atoms for second-order nonlinear applications encounter fundamental trade-offs in the necessary symmetry breaking and local-field enhancement due to radiation damping that is inherent to the operating resonant mode and cannot be controlled separately. Here we present a novel concept that eliminates this restriction obstructing the improvement of terahertz generation efficiency in nonlinear metasurfaces based on metallic nanoresonators. This is achieved by combining a resonant dark-state metasurface, which locally drives nonlinear nanoresonators in the near field, with ...


On Loss Compensation, Amplification And Lasing In Metallic Metamaterials, Sotiris Droulias, Thomas Koschny, Maria Kafesaki, Costas M. Soukoulis Jan 2019

On Loss Compensation, Amplification And Lasing In Metallic Metamaterials, Sotiris Droulias, Thomas Koschny, Maria Kafesaki, Costas M. Soukoulis

Ames Laboratory Accepted Manuscripts

The design of metamaterials, which are artificial materials that can offer unique electromagnetic properties, is based on the excitation of strong resonant modes. Unfortunately, material absorption—mainly due to their metallic parts—can damp their resonances and hinder their operation. Incorporating a gain material can balance these losses, but this must be performed properly, as a reduced or even eliminated absorption does not guarantee loss compensation. Here we examine the possible regimes of interaction of a gain material with a passive metamaterial and show that background amplification and loss compensation are two extreme opposites, both of which can lead to ...


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

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

Chemistry Publications

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


Squeezed Nanocrystals: Equilibrium Configuration Of Metal Clusters Embedded Beneath The Surface Of A Layered Material, Scott E. Julien, Ann Lii-Rosales, Kai-Tak Wan, Yong Han, Michael C. Tringides, James W. Evans, Patricia A. Thiel Jan 2019

Squeezed Nanocrystals: Equilibrium Configuration Of Metal Clusters Embedded Beneath The Surface Of A Layered Material, Scott E. Julien, Ann Lii-Rosales, Kai-Tak Wan, Yong Han, Michael C. Tringides, James W. Evans, Patricia A. Thiel

Chemistry Publications

Shapes of functional metallic nanocrystals, typically synthesized either free in solution or supported on surfaces, are key for controlling properties. Here, we consider a novel new class of metallic nanocrystals, copper islands embedded near the surface of graphite, which can be considered a model system for metals embedded beneath surfaces of layered materials, or beneath supported membranes. We develop a continuum elasticity (CE) model for the equilibrium shape of these islands, and compare its predictions with experimental data. The CE model incorporates appropriate surface energy, adhesion energies, and strain energy. The agreement between the CE model and the data is ...


Effect Of (Poly)Electrolytes On The Interfacial Assembly Of Peg Functionalized Gold Nanoparticles, Srikanth Nayak, Max Fieg, Wenjie Wang, Wei Bu, Surya Mallapragada, David Vaknin Jan 2019

Effect Of (Poly)Electrolytes On The Interfacial Assembly Of Peg Functionalized Gold Nanoparticles, Srikanth Nayak, Max Fieg, Wenjie Wang, Wei Bu, Surya Mallapragada, David Vaknin

Chemical and Biological Engineering Publications

We report on the effect of interpolymer complexes (IPCs) of poly(acrylic acid) (PAA) with poly(ethylene glycol) functionalized Au nanoparticles (PEG-AuNPs) as they assemble at the vapor-liquid interface, using surface sensitive synchrotron X-ray scattering techniques. Depending on the suspension pH, PAA functions both as a weak polyelectrolyte and a hydrogen bond donor, and these two roles affect the interfacial assembly of PEG-AuNPs differently. Above its isoelectric point, we find that PAA leads to the formation of a PEG-AuNPs monolayer at the interface with hexagonal structure. In the presence of high concentration of HCl (i.e., below the isoelectric point ...


Imaging Stress And Magnetism At High Pressures Using A Nanoscale Quantum Sensor, S. Hsieh, P. Bhattacharyya, C. Zu, T. Mittiga, T. J. Smart, F. Machado, B. Kobrin, T. O. Hohn, N. Z. Rui, Mehdi Kamrani, S. Chatterjee, S. Choi, M. Zaletel, V. V. Struzhkin, J. E. Moore, Valery I. Levitas, R. Jeanloz, N. Y. Yao Dec 2018

Imaging Stress And Magnetism At High Pressures Using A Nanoscale Quantum Sensor, S. Hsieh, P. Bhattacharyya, C. Zu, T. Mittiga, T. J. Smart, F. Machado, B. Kobrin, T. O. Hohn, N. Z. Rui, Mehdi Kamrani, S. Chatterjee, S. Choi, M. Zaletel, V. V. Struzhkin, J. E. Moore, Valery I. Levitas, R. Jeanloz, N. Y. Yao

Aerospace Engineering Publications

Pressure alters the physical, chemical and electronic properties of matter. The development of the diamond anvil cell (DAC) enables tabletop experiments to investigate a diverse landscape of high-pressure phenomena ranging from the properties of planetary interiors to transitions between quantum mechanical phases. In this work, we introduce and utilize a novel nanoscale sensing platform, which integrates nitrogen-vacancy (NV) color centers directly into the culet (tip) of diamond anvils. We demonstrate the versatility of this platform by performing diffraction-limited imaging (~600 nm) of both stress fields and magnetism, up to pressures ~30 GPa and for temperatures ranging from 25-340 K. For ...


Improved Gas Sensing Performance Of Ald Azo 3-D Coated Zno Nanorods, P. Lin, X. Chen, K. Zhang, H. Baumgart Dec 2018

Improved Gas Sensing Performance Of Ald Azo 3-D Coated Zno Nanorods, P. Lin, X. Chen, K. Zhang, H. Baumgart

Electrical & Computer Engineering Faculty Publications

This paper reports an enhancement on the sensing performance of ZnO nanorod ethanol sensors with a new approach by utilizing nested coatings of Aluminum doped ZnO (AZO) thin films by Atomic Layer Deposition (ALD) technology. ZnO nanorods were grown by the hydrothermal method with the ZnO seed layer synthesized on Silicon wafers by ALD. To enhance the sensing performance of ZnO nanorod ethanol sensors, multiple coated AZO thin film 3-D coatings were deposited on the surface of the intrinsic ZnO nanorods by ALD.To investigate the sensing performance of the ZnO nanorods sensor for the detection of ethanol vapor, a ...


Reverse-Engineering Of Graphene On Metal Surfaces: A Case Study Of Embedded Ruthenium, Ann Lii-Rosales, Yong Han, Ka Man Yu, Dapeng Jing, Nathaniel Anderson, David Vaknin, Michael C. Tringides, James W. Evans, Michael S. Altman, Patricia A. Thiel Oct 2018

Reverse-Engineering Of Graphene On Metal Surfaces: A Case Study Of Embedded Ruthenium, Ann Lii-Rosales, Yong Han, Ka Man Yu, Dapeng Jing, Nathaniel Anderson, David Vaknin, Michael C. Tringides, James W. Evans, Michael S. Altman, Patricia A. Thiel

Chemistry Publications

Using scanning tunneling microscopy, x-ray photoelectron spectroscopy, and x-ray absorption spectroscopy, we show that Ru forms metallic nanoislands on graphite, covered by a graphene monolayer. These islands are air-stable, contain 2–4 layers of Ru, and have diameters on the order of 10 nm. To produce these nanoislands two conditions must be met during synthesis. The graphite surface must be ion-bombarded, and subsequently held at an elevated temperature (1000–1180 K) during Ru deposition. A coincidence lattice forms between the graphene overlayer and the Ru island top. Its characteristics—coincidence lattice constant, corrugation amplitude, and variation of carbon lattice appearance ...


No2- And No3- Enhance Cold Atmospheric Plasma Induced Cancer Cell Death By Generation Of Onoo-, Dehui Xu, Qingjie Cui, Yujing Xu, Zhijie Liu, Zeyu Chen, Wenjie Xia, Hao Zhang, Dingxin Liu, Hailan Chen, Michael G. Kong Oct 2018

No2- And No3- Enhance Cold Atmospheric Plasma Induced Cancer Cell Death By Generation Of Onoo-, Dehui Xu, Qingjie Cui, Yujing Xu, Zhijie Liu, Zeyu Chen, Wenjie Xia, Hao Zhang, Dingxin Liu, Hailan Chen, Michael G. Kong

Bioelectrics Publications

Cold atmospheric plasma (CAP) is a rapidly developed technology that has been widely applied in biomedicine especially in cancer treatment. Due to the generation of various active species in plasma, CAP could induce various tumor cells death and showed a promising potential in cancer therapy. To enhance the biological effects of gas plasma, changing the discharging parameters is the most commonly used method, yet increasing discharging power will lead to a higher possibility of simultaneously damage surrounding tissues. In this study, by adding nontoxic concentration of additional nitrite and nitrate in the medium, we found that anti-tumor effect of CAP ...


Growing Signals From The Noise: Challenging Nuclei In Materials Dnp, Frédéric A. Perras, Takeshi Kobayashi, Marek Pruski Sep 2018

Growing Signals From The Noise: Challenging Nuclei In Materials Dnp, Frédéric A. Perras, Takeshi Kobayashi, Marek Pruski

Ames Laboratory Accepted Manuscripts

The polarization of nuclear spins by dynamic nuclear polarization (DNP) has redefined the sensitivity limits of solid‐state (SS) NMR spectroscopy. Materials science has been arguably one of the key beneficiaries of the recent remarkable advances of the technique, which included low‐temperature magic angle spinning (MAS), modern gyrotrons, and biradical agents for polarization transfer via the cross‐effect. In many classes of materials, DNP offers the capability of selectively sensitizing progressively smaller surface and interfacial regions of materials and eliciting responses from previously undetectable nuclei, with no detrimental effect on resolution. We review the most recent applications of DNP ...


Finite-Size Effects In Metasurface Lasers Based On Resonant Dark States, Sotiris Droulias, Thomas Koschny, Costas M. Soukoulis Aug 2018

Finite-Size Effects In Metasurface Lasers Based On Resonant Dark States, Sotiris Droulias, Thomas Koschny, Costas M. Soukoulis

Ames Laboratory Accepted Manuscripts

The quest for subwavelength coherent light sources has recently led to the exploration of dark-mode based surface lasers, which allow for independent adjustment of the lasing state and its coherent radiation output. To understand how this unique design performs in real experiments, we need to consider systems of finite size and quantify finite-size effects not present in the infinite dark-mode surface laser model. Here we find that, depending on the size of the system, distinct and even counterintuitive behavior of the lasing state is possible, determined by a balanced competition between multiple loss channels, including dissipation, intentional out-coupling of coherent ...


Potential Of Mean Force For Two Nanocrystals: Core Geometry And Size, Hydrocarbon Unsaturation, And Universality With Respect To The Force Field, Curt Waltmann, Nathan Horst, Alex Travesset Jul 2018

Potential Of Mean Force For Two Nanocrystals: Core Geometry And Size, Hydrocarbon Unsaturation, And Universality With Respect To The Force Field, Curt Waltmann, Nathan Horst, Alex Travesset

Ames Laboratory Accepted Manuscripts

We present a detailed analysis of the interaction between two nanocrystals capped with ligands consisting of hydrocarbon chains by united atom molecular dynamics simulations. We analyze large cores (up to 10 nm in diameter) and ligands with unsaturated carbon bonds (oleic acid) and we investigate the accuracy of the computed potential of mean force by comparing different force fields. We also analyze the vortices that determine the bonding, including the case of asymmetric nanocrystals, and discuss effects related to the intrinsic anisotropy of the core. Overall our results are in agreement with the predictions of the recently proposed orbifold topological ...


Two-Dimensional Crystallization Of Poly(N-Isopropylacrylamide)-Capped Gold Nanoparticles, Wenjie Wang, Jack J. Lawrence, Wei Bu, Honghu Zhang, David Vaknin Jun 2018

Two-Dimensional Crystallization Of Poly(N-Isopropylacrylamide)-Capped Gold Nanoparticles, Wenjie Wang, Jack J. Lawrence, Wei Bu, Honghu Zhang, David Vaknin

Ames Laboratory Accepted Manuscripts

Surface-sensitive X-ray reflectivity and grazing incidence small-angle X-ray scattering reveal the structure of polymer-capped-gold nanoparticles (AuNPs that are grafted with poly(N-isopropylacrylamide); PNIPAM–AuNPs) as they self-assemble and crystallize at the aqueous suspension/vapor interface. Citrate-stabilized AuNPs (5 and 10 nm in nominal diameter) are ligand-exchanged by 6 kDa PNIPAM-thiol to form corona brushes around the AuNPs that are highly stable and dispersed in aqueous suspensions. Surprisingly, no clear evidence of thermosensitive effect on surface enrichment or self-assembly of the PNIPAM–AuNPs is observed in the 10–35 °C temperature range. However, addition of simple salts (in this case ...


Tailoring Bandgap Of Perovskite Batio3 By Transition Metals Co-Doping For Visible-Light Photoelectrical Applications: A First-Principles Study, Fan Yang, Liang Yang, Changzhi Ai, Pengcheng Xie, Shiwei Lin, Cai-Zhuang Wang, Xihong Lu Jun 2018

Tailoring Bandgap Of Perovskite Batio3 By Transition Metals Co-Doping For Visible-Light Photoelectrical Applications: A First-Principles Study, Fan Yang, Liang Yang, Changzhi Ai, Pengcheng Xie, Shiwei Lin, Cai-Zhuang Wang, Xihong Lu

Ames Laboratory Accepted Manuscripts

The physical and chemical properties of V-M″ and Nb-M″ (M″ is 3d or 4d transition metal) co-doped BaTiO3were studied by first-principles calculation based on density functional theory. Our calculation results show that V-M″ co-doping is more favorable than Nb-M″ co-doping in terms of narrowing the bandgap and increasing the visible-light absorption. In pure BaTiO3, the bandgap depends on the energy levels of the Ti 3d and O 2p states. The appropriate co-doping can effectively manipulate the bandgap by introducing new energy levels interacting with those of the pure BaTiO3. The optimal co-doping effect comes from the ...


Probing Magnetism In 2d Van Der Waals Crystalline Insulators Via Electron Tunneling, D. R. Klein, D. Macneill, J. L. Lado, D. Soriano, E. Navarro-Moratalla, K. Watanabe, T. Taniguchi, S. Manni, Paul C. Canfield, J. Fernández-Rossier, P. Jarillo-Herrero Jun 2018

Probing Magnetism In 2d Van Der Waals Crystalline Insulators Via Electron Tunneling, D. R. Klein, D. Macneill, J. L. Lado, D. Soriano, E. Navarro-Moratalla, K. Watanabe, T. Taniguchi, S. Manni, Paul C. Canfield, J. Fernández-Rossier, P. Jarillo-Herrero

Ames Laboratory Accepted Manuscripts

Magnetic insulators are a key resource for next-generation spintronic and topological devices. The family of layered metal halides promises varied magnetic states, including ultrathin insulating multiferroics, spin liquids, and ferromagnets, but device-oriented characterization methods are needed to unlock their potential. Here, we report tunneling through the layered magnetic insulator CrI3 as a function of temperature and applied magnetic field. We electrically detect the magnetic ground state and interlayer coupling and observe a field-induced metamagnetic transition. The metamagnetic transition results in magnetoresistances of 95, 300, and 550% for bilayer, trilayer, and tetralayer CrI3 barriers, respectively. We further measure inelastic tunneling spectra ...


Many Body Effects And Icosahedral Order In Superlattice Self-Assembly, Tommy Waltmann, Curt Waltmann, Nathan Horst, Alex Travesset Jun 2018

Many Body Effects And Icosahedral Order In Superlattice Self-Assembly, Tommy Waltmann, Curt Waltmann, Nathan Horst, Alex Travesset

Ames Laboratory Accepted Manuscripts

We elucidate how nanocrystals “bond” to form ordered structures. For that purpose we consider nanocrystal configurations consisting of regular polygons and polyhedra, which are the motifs that constitute single component and binary nanocrystal superlattices, and simulate them using united atom models. We compute the free energy and quantify many body effects, i.e., those that cannot be accounted for by pair potential (two-body) interactions, further showing that they arise from coalescing vortices of capping ligands. We find that such vortex textures exist for configurations with local coordination number ≤6. For higher coordination numbers, vortices are expelled and nanocrystals arrange in ...


The Crystal Facet-Dependent Electrochemical Performance Of Tio2 Nanocrystals For Heavy Metal Detection: Theoretical Prediction And Experimental Proof, Jianjun Liao, Fan Yang, Cai-Zhuang Wang, Shiwei Lin May 2018

The Crystal Facet-Dependent Electrochemical Performance Of Tio2 Nanocrystals For Heavy Metal Detection: Theoretical Prediction And Experimental Proof, Jianjun Liao, Fan Yang, Cai-Zhuang Wang, Shiwei Lin

Ames Laboratory Accepted Manuscripts

Tailored design/fabrication of electroanalytical materials with highly-active exposed crystal planes is of great importance for the development of electrochemical sensing. In this work, combining experimental and theoretical efforts, we reported a facile strategy to fabricate TiO2 nanocrystals with tunable electrochemical performance for heavy metal detection. Density functional theory (DFT) calculations indicated that TiO2 (001) facet showed relative larger adsorption energy and lower diffusion energy barrier toward heavy metal ions, which is favorable for obtaining better electrochemical stripping behaviors. Based on this prediction, a series of TiO2 nanocrystals with different ratios of exposed (001) and (101) facets were synthesized. Electrochemical ...


Investigating Phase Transition Temperatures Of Size Separated Gadolinium Silicide Magnetic Nanoparticles, Shivakumar G. Hunagund, Shane M. Harstad, Ahmed A. El-Gendy, Shalbh Gupta, Vitalij K. Pecharsky, Ravi L. Hadimani May 2018

Investigating Phase Transition Temperatures Of Size Separated Gadolinium Silicide Magnetic Nanoparticles, Shivakumar G. Hunagund, Shane M. Harstad, Ahmed A. El-Gendy, Shalbh Gupta, Vitalij K. Pecharsky, Ravi L. Hadimani

Ames Laboratory Accepted Manuscripts

Gadolinium silicide (Gd5Si4) nanoparticles (NPs) exhibit different properties compared to their parent bulk materials due to finite size, shape, and surface effects. NPs were prepared by high energy ball-milling of the as-cast Gd5Si4ingot and size separated into eight fractions using time sensitive sedimentation in an applied dc magnetic field with average particle sizes ranging from 700 nm to 82 nm. The largest Gd5Si4 NPs order ferromagnetically at 316 K. A second anomaly observed at 110 K can be ascribed to a Gd5Si3 impurity. As the particle sizes decrease, the volume fraction of Gd5Si3 phase increases at the expense of the ...


Electroosmotic Flow Of Viscoelastic Fluid In A Nanoslit, Lanju Mei, Hongna Zhang, Hongxia Meng, Shizhi Qian Mar 2018

Electroosmotic Flow Of Viscoelastic Fluid In A Nanoslit, Lanju Mei, Hongna Zhang, Hongxia Meng, Shizhi Qian

Mechanical & Aerospace Engineering Faculty Publications

The electroosmotic flow (EOF) of viscoelastic fluid in a long nanoslit is numerically studied to investigate the rheological property effect of Linear Phan-Thien-Tanner (LPTT) fluid on the fully developed EOF. The non-linear Poisson-Nernst-Planck equations governing the electric potential and the ionic concentration distribution within the channel are adopted to take into account the effect of the electrical double layer (EDL), including the EDL overlap. When the EDL is not overlapped, the velocity profiles for both Newtonian and viscoelastic fluids are plug-like and increase sharply near the charged wall. The velocity profile resembles that of pressure-driven flow when the EDL is ...


Nanostructural Origin Of Semiconductivity And Large Magnetoresistance In Epitaxial Nico2O4/Al2O3 Thin Films, Congmian Zhen, Xiaozhe Zhang, Wengang Wei, Wenzhe Guo, Ankit Pant, Xiaoshan Xu, Jian Shen, Li Ma, Denglu Hou Mar 2018

Nanostructural Origin Of Semiconductivity And Large Magnetoresistance In Epitaxial Nico2O4/Al2O3 Thin Films, Congmian Zhen, Xiaozhe Zhang, Wengang Wei, Wenzhe Guo, Ankit Pant, Xiaoshan Xu, Jian Shen, Li Ma, Denglu Hou

Xiaoshan Xu Papers

Despite low resistivity (~1 mΩ cm), metallic electrical transport has not been commonly observed in inverse spinel NiCo2O4, except in certain epitaxial thin films. Previous studies have stressed the effect of valence mixing and the degree of spinel inversion on the electrical conduction of NiCo2O4 films. In this work, we studied the effect of nanostructural disorder by comparing the NiCo2O4 epitaxial films grown on MgAl2O4 (1 1 1) and on Al2O3 (0 0 1) substrates. Although the optimal growth conditions are similar for the NiCo ...


Effects Of Grain Boundary Disorder On Yield Strength, Valery Borovikov, Mikhail I. Mendelev, Alexander H. King Jan 2018

Effects Of Grain Boundary Disorder On Yield Strength, Valery Borovikov, Mikhail I. Mendelev, Alexander H. King

Materials Science and Engineering Publications

It was recently reported that segregation of Zr to grain boundaries (GB) in nanocrystalline Cu can lead to the formation of disordered intergranular films [1,2]. In this study we employ atomistic computer simulations to study how the formation of these films affects the dislocation nucleation from the GBs. We found that full disorder of the grain boundary structure leads to the suppression of dislocation emission and significant increase of the yield stress. Depending on the solute concentration and heat-treatment, however, a partial disorder may also occur and this aids dislocation nucleation rather than suppressing it, resulting in elimination of ...


Shear Driven Formation Of Nano-Diamonds At Sub-Gigapascals And 300 K, Yang Gao, Yanzhang Ma, Qi An, Valery I. Levitas, Yanyan Zhang, Biao Feng, Jharna Chaudhuri, William A. Goddard Jan 2018

Shear Driven Formation Of Nano-Diamonds At Sub-Gigapascals And 300 K, Yang Gao, Yanzhang Ma, Qi An, Valery I. Levitas, Yanyan Zhang, Biao Feng, Jharna Chaudhuri, William A. Goddard

Materials Science and Engineering Publications

The transformation pathways of carbon at high pressures are of broad interest for synthesis of novel materials and for revealing the Earth's geological history. We have applied large plastic shear on graphite in rotational anvils to form hexagonal and nanocrystalline cubic diamond at extremely low pressures of 0.4 and 0.7 GPa, which are 50 and 100 times lower than the transformation pressures under hydrostatic compression and well below the phase equilibrium. Large shearing accompanied with pressure elevation to 3 GPa also leads to formation of a new orthorhombic diamond phase. Our results demonstrate new mechanisms and new ...


Interpolymer Complexation As A Strategy For Nanoparticle Assembly And Crystallization, Srikanth Nayak, Nathan Horst, Honghu Zhang, Wenjie Wang, Surya Mallapragada, Alex Travesset, David Vaknin Jan 2018

Interpolymer Complexation As A Strategy For Nanoparticle Assembly And Crystallization, Srikanth Nayak, Nathan Horst, Honghu Zhang, Wenjie Wang, Surya Mallapragada, Alex Travesset, David Vaknin

Chemical and Biological Engineering Publications

Controlled self-assembly of nanoparticles into ordered structures is a major step in fabricating nanotechnology based devices. Here, we report on the self-assembly of high quality superlattices of nanoparticles in aqueous suspensions induced via interpolymer complexation. Using small angle X-ray scattering, we demonstrate that the NPs crystallize into superlattices of FCC symmetry, initially driven by hydrogen bonding and subsequently by van der Waals forces between the complexed coronas of hydrogen-bonded polymers. We show that the lattice constant and crystal quality can be tuned by polymer concentration, suspension pH and the length of polymer chains. Interpolymer complexation to assemble nanoparticles is scalable ...


Ordered Networks Of Gold Nanoparticles Crosslinked By Dithiol‐Oligomers, Srikanth Nayak, Nathan Horst, Honghu Zhang, Wenjie Wang, Surya Mallapragada, Alex Travesset, David Vaknin Jan 2018

Ordered Networks Of Gold Nanoparticles Crosslinked By Dithiol‐Oligomers, Srikanth Nayak, Nathan Horst, Honghu Zhang, Wenjie Wang, Surya Mallapragada, Alex Travesset, David Vaknin

Chemical and Biological Engineering Publications

Controlled aggregation of nanoparticles into superlattices is a grand challenge in material science, where ligand based self‐assembly is the dominant route. Here, the self‐assembly of gold nanoparticles (AuNPs) that are crosslinked by water soluble oligo‐(ethylene glycol)‐dithiol (oEG‐dithiol) is reported and their 3D structure by small angle X‐ray scattering is determined. Surprisingly, a narrow region is found in the parameter space of dithiol linker‐length and nanoparticle size for which the crosslinked networks form short‐ranged FCC crystals. Using geometrical considerations and numerical simulations, the stability of the formed lattices is evaluated as a function ...


Diffusion Of Two-Dimensional Epitaxial Clusters On Metal (100) Surfaces: Facile Versus Nucleation-Mediated Behavior And Their Merging For Larger Sizes, King C. Lai, Da-Jiang Liu, James W. Evans Dec 2017

Diffusion Of Two-Dimensional Epitaxial Clusters On Metal (100) Surfaces: Facile Versus Nucleation-Mediated Behavior And Their Merging For Larger Sizes, King C. Lai, Da-Jiang Liu, James W. Evans

Ames Laboratory Accepted Manuscripts

For diffusion of two-dimensional homoepitaxial clusters of N atoms on metal (100) surfaces mediated by edge atom hopping, macroscale continuum theory suggests that the diffusion coefficient scales like DN∼N−β with β=3/2. However, we find quite different and diverse behavior in multiple size regimes. These include: (i) facile diffusion for small sizes N<9; (ii) slow nucleation-mediated diffusion with small β<1 for “perfect” sizes N=Np=L2 or L(L+1), for L=3,4, ... having unique ground-state shapes, for moderate sizes 9≤N≤O(102); the same also applies for N=Np+3, Np+4, ...(iii) facile diffusion but with large β>2 for N=Np+1 and Np+2 also for moderate sizes 9≤N≤O(102); (iv) merging of the above distinct branches and subsequent anomalous scaling with 1≲β<3/2, reflecting the quasifacetted structure of clusters, for larger N=O(102) to N=O(103); (v) classic scaling with β=3/2 for very large N=O(103) and above. The specified size ranges apply for typical model parameters. We focus on the moderate size regime where we show that diffusivity cycles quasiperiodically from the slowest branch for Np+3 (not Np) to the fastest branch for Np+1. Behavior is quantified by kinetic Monte Carlo simulation of an appropriate stochastic lattice-gas model. However, precise analysis must account for a strong enhancement of diffusivity for short time increments due to back correlation in the cluster motion. Further understanding of this enhancement, of anomalous size scaling behavior, and of the merging of various branches, is facilitated by combinatorial analysis of the number of the ground-state and low-lying excited state cluster configurations, and also of kink populations.


Ionic Depletion At The Crystalline Gibbs Layer Of Peg-Capped Gold Nanoparticle Brushes At Aqueous Surfaces, Wenjie Wang, Honghu Zhang, Surya Mallapragada, Alex Travesset, David Vaknin Dec 2017

Ionic Depletion At The Crystalline Gibbs Layer Of Peg-Capped Gold Nanoparticle Brushes At Aqueous Surfaces, Wenjie Wang, Honghu Zhang, Surya Mallapragada, Alex Travesset, David Vaknin

Ames Laboratory Accepted Manuscripts

In situ surface-sensitive x-ray diffraction and grazing incidence x-ray fluorescence spectroscopy (GIXFS) methods are combined to determine the ionic distributions across the liquid/vapor interfaces of thiolated-polyethylene-glycol–capped gold nanoparticle (PEG-AuNP) solutions. Induced by the addition of salts (i.e., Cs2SO4) to PEG-AuNPs solutions, two-dimensional hexagonal lattices of PEG-AuNPs form spontaneously at the aqueous surfaces, as is demonstrated by x-ray reflectivity and grazing incidence small-angle x-ray scattering. By taking advantage of element specificity with the GIXFS method, we find that the cation Cs+ concentration at the crystalline film is significantly reduced in parts of the PEG-AuNP film compared with that ...


Synergistic Interactions Of H2 And N2 With Molten Gallium In The Presence Of Plasma, Maria L. Carreon, Daniel F. Jaramillo-Cabanzo, Indira Chaudhuri, Madhu Menon, Mahendra K. Sunkara Dec 2017

Synergistic Interactions Of H2 And N2 With Molten Gallium In The Presence Of Plasma, Maria L. Carreon, Daniel F. Jaramillo-Cabanzo, Indira Chaudhuri, Madhu Menon, Mahendra K. Sunkara

Physics and Astronomy Faculty Publications

The present study examines the interaction of hydrogen and nitrogen plasmas with gallium in an effort to gain insights into the mechanisms behind the synergetic effect of plasma and a catalytic metal. Absorption/desorption experiments were performed, accompanied by theoretical-computational calculations. Experiments were carried out in a plasma-enhanced, Ga-packed, batch reactor and entailed monitoring the change in pressure at different temperatures. The results indicated a rapid adsorption/dissolution of the gas into the molten metal when gallium was exposed to plasma, even at a low temperature of 100 °C. The experimental observations, when hydrogen was used, indicate that gallium acts ...


Generalized Ellipsometry On Complex Nanostructures And Low-Symmetry Materials, Alyssa Mock Dec 2017

Generalized Ellipsometry On Complex Nanostructures And Low-Symmetry Materials, Alyssa Mock

Theses, Dissertations, and Student Research from Electrical & Computer Engineering

In this thesis, complex anisotropic materials are investigated and characterized by generalized ellipsometry. In recent years, anisotropic materials have gained considerable interest for novel applications in electronic and optoelectronic devices, mostly due to unique properties that originate from reduced crystal symmetry. Examples include white solid-state lighting devices which have become ubiquitous just recently, and the emergence of high-power, high-voltage electronic transistors and switches in all-electric vehicles. The incorporation of single crystalline material with low crystal symmetry into novel device structures requires reconsideration of existing optical characterization approaches. Here, the generalized ellipsometry concept is extended to include applications for materials with ...


Optical Absorption Properties Of Ge2–44 And P-Doped Ge Nanoparticles, Wei Qin, Wen-Cai Lu, Li-Zhen Zhao, Kai-Ming Ho, Cai-Zhuang Wang Dec 2017

Optical Absorption Properties Of Ge2–44 And P-Doped Ge Nanoparticles, Wei Qin, Wen-Cai Lu, Li-Zhen Zhao, Kai-Ming Ho, Cai-Zhuang Wang

Ames Laboratory Accepted Manuscripts

The optical absorption properties of non-crystalline and crystalline Ge nanoparticles with the sizes from ∼2.5 to 15 Å have been studied at the B3LYP/6-31G level using time-dependent density functional theory. Hydrogen passivation and phosphorus doping on some selected Ge nanoparticles were also calculated. With the increase of cluster size, the optical absorption spectra of the non-crystalline Ge nanoparticles change from many peaks to a continuous broad band and at the same time exhibit a systematic red-shift. Doping phosphorus also causes the absorption spectra to shift toward the lower energy region for both non-crystalline and crystalline Ge nanoparticles. The ...