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At least 721 records · Page 40

A closer look at the physical and optical properties of gold nanostars: an experimental and computational study

A combined experimental and computational study was carried out to design a semi-empirical method to determine the volume, surface area, and extinction coefficients of gold nanostars. The values obtained were confirmed by reconstructing the nanostar 3D topography through high-tilt TEM tomography and introducing the finite elements in COMSOL Multiphysics through which we have also calculated the morphology-dependent extinction coefficient. We have, for the first time, modeled the heat losses of a real, experimentally synthesized nanostar, and found the plasmon resonances to be in excellent agreement with those obtained experimentally. Furthermore, we believe that our approach could substantially improve the applicability of this remarkable nanomaterial.

36 MATERIALS SCIENCE↗

Catalytic Oxidation of Propane over Palladium Alloyed with Gold: An Assessment of the Chemical and Intermediate Species

Understanding the catalytic oxidation of propane is important for developing catalysts not only for catalytic oxidation of hydrocarbons in emission systems but also for selective oxidation in the chemical processing industry. For palladium-based catalysts, little is known about the identification of the chemical or intermediate species involved in propane oxidation. We describe herein findings of an investigation of the catalytic oxidation of propane over supported palladium nanoalloys with different compositions of gold (Pd n Au 100–n ), focusing on probing the chemical or intermediate species on the catalysts in correlation with the bimetallic composition and the alloying phase structure. In addition to an enhanced catalytic activity, a strong dependence of the catalytic activity on the bimetallic composition was revealed, displaying an activity maximum at a Pd : Au ratio of 50 : 50 in terms of reaction temperature. This dependence is also reflected by its dependence on the thermochemical treatment conditions. While the activity for nanoalloys with n ~ 50 showed little change after the thermochemical treatment under oxygen, the activities for nanoalloys with n < 50 and n > 50 showed opposite trends. Importantly, this catalytic synergy is linked to the subtle differences of chemical and intermediate species which have been identified for the catalysts with different bimetallic compositions by in situ measurements using diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). For the catalytic oxidation of propane over the highly-active catalyst with a Pd : Au ratio of 50 : 50, the major species identified include acetate and bicarbonate, showing subtle differences in comparison with the identification of bicarbonate and formate for the catalyst with <50% Au (with a lower activity) and the absence of apparent species for the catalyst with >50% Au (activity is largely absent). The alloying of 50% Au in Pd is believed to increase the oxophilicity of Pd, which facilitates the first carbon–carbon bond cleavage and oxygenation of propane. Finally, the implications of the findings on the catalytic synergy of Pd alloyed with Au and the design of active Pd alloy catalysts are also discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Electrolytic gold plating, stripping, and ion transport dynamics through a solid-state iodide perovskite

The pronounced electrochemical reactivity between halide perovskites and metal electrodes can introduce mobile extrinsic metal ions which can cause device instability or enable novel functionalities. Here we systematically investigate the kinetics of gold cation (Au + ) migration in indium tin oxide (ITO)/methylammonium lead triiodide (MAPbI 3 )/Au model devices under long-term potentiostatic biasing. Scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and density functional theory (DFT) analyses reveal that Au + ions, electrochemically generated at the Au anode, traverse the perovskite layer with diffusion coefficients on the order of 10 −11 to 10 −10 cm 2 s −1 and are subsequently reduced at the cathode as Au 0 clusters, resembling metal plating behavior in electrolytic cells and solid-state batteries during charging. Furthermore, reversing the applied bias strips the plated Au 0 , revealing reversibility suitable for bipolar resistive switching devices and providing direct evidence of the electrochemical and ionic nature of Au transport within the perovskite matrix. Quantitatively determining diffusion coefficients and ion concentrations provides foundational inputs for future drift-diffusion modelling opportunities and allows us to relate our findings to implications on long term operation of devices like photovoltaic modules. These results clearly demonstrate the solid-state electrochemical nature of perovskite devices, highlight methods to be more quantitative about ion transport properties, provide and emphasize the importance of disentangling electro-, photo-, photoelectrochemical processes for understanding device performance and unlocking new functionalities.

14 SOLAR ENERGY↗

Synthesis of nanocrystalline thin films of gold on the surface of GaSb by swift heavy ion

Thin films of gold ({approx}100 nm thick) were deposited on p-type GaSb substrates. These samples were irradiated with 100 MeV Fe{sup 7+}ions for the fluence of 1 Multiplication-Sign 10{sup 13} and 1 Multiplication-Sign 10{sup 14} ions cm{sup -2}. After irradiation, samples were characterized using AFM, UV-VIS -NIR, X-Ray Diffraction techniques. AFM studies showed the presence of clusters on the surface of GaSb. R.M.S. roughness of the sample was found to increase w.r.t ion fluence. Absorption coefficient obtained from the Ultra violet - Visible NIR (UV-VIS -NIR) spectra of the samples irradiated with various fluences compared with non irradiated GaSb. The annealing experiment showed a significant improvement in the absorption coefficient after rapid thermal annealing at temperature of 400 Degree-Sign C. X-Ray Diffraction study reveals different orientations of Au film.

36 MATERIALS SCIENCE↗

Probing confined acoustic phonons in free standing small gold nanoparticles

Polarized and depolarized spectra from gold (Au) nanoparticles of different sizes are investigated in the small size range, between 3 and 7 nm, using low frequency Raman spectroscopy. Acoustic vibrations of the free-standing Au nanoparticles are demonstrated with frequencies ranging from 5 to 35 cm{sup -1}, opening the way to the development of the acoustic resonators. A blue shift in the phonon peaks along with the broadening is observed with a decrease in particle size. Comparison of the measured frequencies with vibrational dynamics calculation and an examination as from the transmission electron microscopy results ascertain that the low frequency phonon modes are due to acoustic phonon quantization. Our results show that the observed low frequency Raman scattering originates from the spherical (l = 0) and quadrupolar (l = 2) vibrations of the spheroidal mode due to plasmon mediated acoustic vibrations in Au nanoparticles.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Inhomogeneous Si-doping of gold-seeded InAs nanowires grown by molecular beam epitaxy

We have investigated in situ Si doping of InAs nanowires grown by molecular beam epitaxy from gold seeds. The effectiveness of n-type doping is confirmed by electrical measurements showing an increase of the electron density with the Si flux. We also observe an increase of the electron density along the nanowires from the tip to the base, attributed to the dopant incorporation on the nanowire facets whereas no detectable incorporation occurs through the seed. Furthermore, the Si incorporation strongly influences the lateral growth of the nanowires without giving rise to significant tapering, revealing the complex interplay between axial and lateral growth.

36 MATERIALS SCIENCE↗

Formation of uniformly sized gold nanoparticles over graphene by MeV electron beam irradiation for transparent conducting films

Highly flexible, transparent, and conducting sheet was fabricated by decoration of uniformly sized gold nanoparticles (Au NPs) with high-density on large-area graphene by MeV electron beam irradiation (MEBI) at room temperature under ambient conditions. The Au NPs with an average size of 13.6 ± 3.5 nm were clearly decorated on the graphene after MEBI with an irradiation energy of 1.0 MeV. The sheet resistances of the Au NPs/graphene significantly decreased. For the Au NPs/trilayer graphene, the sheet resistance reached to ∼45 Ω/sq, and the optical transmittance was ∼90.2% which is comparable to that of conventional indium tin oxide film.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Third-order nonlinear optical response of colloidal gold nanoparticles prepared by sputtering deposition

The nonlinear optical responses of gold nanoparticles dispersed in castor oil produced by sputtering deposition were investigated, using the thermally managed Z-scan technique. Particles with spherical shape and 2.6 nm of average diameter were obtained and characterized by transmission electron microscopy and small angle X-ray scattering. This colloid was highly stable, without the presence of chemical impurities, neither stabilizers. It was observed that this system presents a large refractive third-order nonlinear response and a negligible nonlinear absorption. Moreover, the evaluation of the all-optical switching figures of merit demonstrated that the colloidal nanoparticles prepared by sputtering deposition have a good potential for the development of ultrafast photonic devices.

36 MATERIALS SCIENCE↗

Ultrafast and steady-state laser heating effects on electron relaxation and phonon coupling mechanisms in thin gold films

We study the scattering mechanisms driving electron-phonon relaxation in thin gold films via pump-probe time-domain thermoreflectance. Electron-electron scattering can enhance the effective rate of electron-phonon relaxation when the electrons are out of equilibrium with the phonons. In order to correctly and consistently infer electron-phonon coupling factors in films on different substrates, we must account for the increase in steady-state lattice temperature due to laser heating. Our data provide evidence that a thermalized electron population will not directly exchange energy with the substrate during electron-phonon relaxation, whereas this pathway can exist between a non-equilibrium distribution of electrons and a non-metallic substrate.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Fabrication of gold nanostructures through pulsed laser interference patterning

In this Letter, we report on the experimental development and computational modeling of a simple, one-step method for the fabrication of diverse 2D and 3D periodic nanostructures derived from gold films on silicon substrates and over areas spanning 1 cm{sup 2}. These nanostructures can be patterned on films of thickness ranging from 50 nm to 500 nm with pulsed interfering laser beams. A finite volume-based inhomogeneous multiphase model of the process shows reasonable agreement with the experimentally obtained topographies and provides insights on the flow physics including normal and radial expansion that results in peeling of film from the substrate.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

High pressure melting curves of silver, gold and copper

In this work, based on the Lindemann's formula of melting and the pressure-dependent Grüneisen parameter, we have investigated the pressure effect on melting temperature of silver, gold and copper metals. The analytical expression of melting temperature as a function of volume compression has been derived. Our results are compared with available experimental data as well as with previous theoretical studies and the good and reasonable agreements are found. We also proposed the potential of this approach on predicting melting of copper at very high pressure.

36 MATERIALS SCIENCE↗

Switching of localized surface plasmon resonance of gold nanoparticles on a GeSbTe film mediated by nanoscale phase change and modification of surface morphology

As a platform for active nanophotonics, localized surface plasmon resonance (LSPR) switching via interaction with a chalcogenide phase change material (GeSbTe) was investigated. We performed single-particle spectroscopy of gold nanoparticles placed on a GeSbTe thin film. By irradiation with a femtosecond pulsed laser for amorphization and a continuous wave laser for crystallization, significant switching behavior of the LSPR band due to the interaction of GeSbTe was observed. The switching mechanism was explained in terms of both a change in the refractive index and a modification of surface morphology accompanying volume expansion and reduction of GeSbTe.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Quantum optics with single nanodiamonds flying over gold films: Towards a Robust quantum plasmonics

A nanodiamond (ND) hosting nitrogen-vacancy (NV) color centers is attached on the apex of an optical tip for near-field microscopy. Its fluorescence is used to launch surface plasmon-polaritons (SPPs) in a thin polycrystalline gold film. It is shown that the quantum nature of the initial source of light is preserved after conversion to SPPs. This opens the way to a deterministic quantum plasmonics, where single SPPs can be injected at well-defined positions in a plasmonic device produced by top-down approaches.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Dimpling in critical current density vs. magnetic field angle in YBa{sub 2}Cu{sub 3}O{sub 7} films irradiated with 3-MeV gold ions

Magnetic-field-angle θ dependence of critical current density J{sub c} was measured in YBa{sub 2}Cu{sub 3}O{sub 7} films irradiated with 3-MeV gold ions. Such films were recently found to show large pinning force arising from point-like irradiation defects. A dimpled line-shape of J{sub c}(θ) and its variation with magnetic field strength were revealed that could be well described by a simple model based on flux-lattice shear and Blatter scaling. Our results strongly suggest that vortex elasticity and electron-mass anisotropy coordinately produce the characteristic J{sub c} anisotropy, called “shoulders,” in cuprate and iron-pnictide films.

36 MATERIALS SCIENCE↗

Effect of defocusing on picosecond laser-coupling into gold cones

Here, we show that defocusing of the laser in the interaction of a picosecond duration, 1.053 μm wavelength, high energy pulse with a cone-wire target does not significantly affect the laser energy coupling efficiency, but does result in a drop in the fast electron effective temperature. This may be beneficial for fast ignition, since not only were more electrons with lower energies seen in the experiment but also the lower prepulse intensity will reduce the amount of preplasma present on arrival of the main pulse, reducing the distance the hot electrons have to travel. We used the Vulcan Petawatt Laser at the Rutherford Appleton Laboratory and gold cone targets with approximately 1 mm long, 40 μm diameter copper wires attached to their tip. Diagnostics included a quartz crystal imager, a pair of highly oriented pyrolytic graphite crystal spectrometers and a calibrated CCD operating in the single photon counting regime, all of which looked at the copper K{sub α} emission from the wire. A short pulse optical probe, delayed 400 ps relative to the main pulse was employed to diagnose the extent of plasma expansion around the wire. A ray-tracing code modeled the change in intensity on the interior surface of the cone with laser defocusing. Using a model for the wire copper K{sub α} emission coupled to a hybrid Vlasov-Fokker-Planck code, we ran a series of simulations, holding the total energy in electrons constant whilst varying the electron temperature, which support the experimental conclusions.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Nonlinear contrast enhancement in photoacoustic molecular imaging with gold nanosphere encapsulated nanoemulsions

A composite contrast agent, a nanoemulsion bead with assembled gold nanospheres at the interface, is proposed to improve the specific contrast of photoacoustic molecular imaging. A phase transition in the bead's core is induced by absorption of a nanosecond laser pulse with a fairly low laser fluence (∼3.5 mJ/cm{sup 2}), creating a transient microbubble through dramatically enhanced thermal expansion. This generates nonlinear photoacoustic signals with more than 10 times larger amplitude compared to that of a linear agent with the same optical absorption. By applying a differential scheme similar to ultrasound pulse inversion, more than 40 dB contrast enhancement is demonstrated with suppression of background signals.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Anomalous patterns and nearly defect-free ripples produced by bombarding silicon and germanium with a beam of gold ions

We demonstrate that surface ripples with an exceptionally high degree of order can develop when germanium is bombarded with a broad beam of gold ions. In contrast, if silicon is sputtered with an Au{sup −} beam, patches of ripples with two distinct wave vectors can emerge. These types of order can be understood if the coupling between the surface morphology and composition is taken into account.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗