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At least 397 records · Page 22

All sources NASA NTRS DOE OSTI

DOE OSTI2021

Fast attenuation of high-frequency acoustic waves in bicontinuous nanoporous gold

We studied the formation and attenuation of GHz elastic waves in free-standing nanoporous gold films by MeV ultrafast electron diffraction and finite element simulations. By tracing the evolution of the high frequency acoustic waves in time domain, we found that the bicontinuous nanoporous structure in nanoporous gold films results in three-dimensionally acoustic response with low coherence, leading to fast attenuation of the elastic waves in comparison with solid gold films. The morphologically dominated dynamics indicates the nanoporosity plays an important role in the high-frequency acoustic energy relaxation, which shines a light on the applications of dealloyed nanoporous materials in nanodevices and sensors as GHz and THz acoustic filters and dampers.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Synthesis of TiO{sub 2} nanoparticles decorated with gold nanoclusters using pulsed laser ablation in liquid

Amorphous spherical titanium dioxide (TiO{sub 2}) nanoparticles, decorated gold nanoparticles, are shown to be formed under irradiation of commercial TiO{sub 2} nanopowders dispersed in aqueous solution of hydrogen tetrachloroaurate (HAuCl{sub 4}) by second-harmonic nanosecond pulses of an Nd : YAG laser. It is found that these hybrid nanostructures are formed during laser-induced remelting of the initial nanoparticles, stimulated by gold nanoclusters (providing more efficient absorption of visible laser radiation by titanium dioxide) recovered on their surface. The morphology and chemical composition of the newly formed hybrid nanomaterials are investigated in detail by electron microscopy, Raman spectroscopy, and energy-dispersive analysis. It is shown that the average size and number of gold nanoparticles recovered on the TiO{sub 2} surface can be controlled by varying the concentration ratio of the initial nanomaterial and HAuCl{sub 4}. A spectroscopic analysis of light scattering by single hybrid nanoparticles and the results of numerical calculation of the structure of electromagnetic fields near their surface indicate good prospects of these hybrid nanomaterials for various applications in modern optics, optoelectronics, and nanophotonics; for example, for designing chemo- and biosensor platforms and new-generation solar cells. (nanoparticles)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2021

Polymorphism of gold under laser-based ramp compression to 690 GPa

The high-pressure behavior and polymorphism of gold has attracted strong recent interest from theory as well as from both static and dynamic experiments. In this study, gold was dynamically ramp-compressed to 690 GPa via laser ablation using the Omega Laser Facility (U. Rochester) in order to investigate the stability regions of this noble metal's polymorphs. Here, stresses were determined from measurements of surface or interface velocities by laser interferometry. In situ X-ray diffraction was carried out to constrain the structure and density. The ambient face-centered-cubic (fcc) phase was observed at 162 GPa, followed by a mixed phase region consisting of the fcc and body-centeredcubic (bcc). The presence of only the bcc phase was observed between 377 and 690 GPa. Our results are consistent with recent shock compression experiments and demonstrate that gold transforms to the bcc phase under conditions of both ramp and shock loading.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2017

Instability of the topological surface state in Bi 2 Se 3 upon deposition of gold

Momentum-resolved photoemission spectroscopy indicates the instability of the Dirac surface state upon deposition of gold on the (0001) surface of the topological insulator Bi 2 Se 3 . Based on the structure model derived from extended x-ray absorption fine structure experiments showing that gold atoms substitute bismuth atoms, first-principles calculations provide evidence that a gap appears due to hybridization of the surface state with gold d states near the Fermi level. Here, our findings provide insights into the mechanisms affecting the stability of the surface state.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2017

Neutron transfer in the C 13 + Au 197 reaction from gold isotope residuals

Residual gold nuclei were produced in this paper via neutron transfer at multiple energies using a 130-MeV 13 C beam incident on a stacked-foil target consisting of alternating layers of 197 Au and 27 Al. Production cross sections, over an energy range of 56 to 129 MeV, for seven gold isotopes and two gold isomers were determined through activation analysis. By using the Wilczynski binary transfer model with a modified version of the recoil formula and a standard evaporation model, we were able to reproduce the isotopic production cross sections at high beam energy, with some disagreement at lower beam energies. Finally, this limiting angular momentum model does not predict the transfer of sufficient angular momentum to reproduce the observed isomeric populations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2019

One-Dimensional Anomalous Diffusion of Gold Nanoparticles in a Polymer Melt

We investigated the dynamics of polymer-grafted gold nanoparticles loaded into polymer melts using x-ray photon correlation spectroscopy. For low molecular weight host matrix polymer chains, normal isotropic diffusion of the gold nanoparticles is observed. For larger molecular weights, anomalous diffusion of the nanoparticles is observed that can be described by ballistic motion and generalized Levy walks, similar to those often used to discuss the dynamics of jammed systems. Under certain annealing conditions, the diffusion is one-dimensional and related to the direction of heat flow during annealing and is associated with an dynamic alignment of the host polymer chains. Molecular dynamics simulations of a single gold nanoparticle diffusing in a partially aligned polymer network semiquantitatively reproduce the experimental results to a remarkable degree. Here, the results help to showcase how nanoparticles can under certain circumstances move rapidly in polymer networks.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Large spin-to-charge conversion in ultrathin gold-silicon multilayers

Investigation of the spin Hall effect in gold has triggered increasing interest over the past decade, since gold combines the properties of a large bulk spin-diffusion length and strong interfacial spin-orbit coupling. However, discrepancies between the values of the spin Hall angle of gold reported in the literature have brought into question the microscopic origin of the spin Hall effect in Au. Here, we investigate the thickness dependence of the effective spin-charge conversion efficiency in single Au films and ultrathin Au/Si multilayers by nonlocal transport and spin-torque ferromagnetic resonance measurements. We show that the inferred effective spin-charge conversion efficiency is strongly enhanced in ultrathin Au/Si multilayers, reaching exceedingly large values of 0.99 ± 0.34 when the thickness of the individual Au layers is scaled down to 2 nm. These findings reveal the coexistence of a strong interfacial spin-to-charge conversion effect, which becomes dominant in ultrathin Au, and bulk spin Hall effect with a relatively low bulk spin Hall angle of 0.012 ± 0.005. Furthermore, our experimental results suggest the key role of the intrinsic spin Hall effect enhancement along with a strong interfacial spin-orbit coupling-related effect in the large spin-to-charge conversion in ultrathin Au.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Annealing of focused ion beam damage in gold microcrystals: an in situ Bragg coherent X-ray diffraction imaging study

Focused ion beam (FIB) techniques are commonly used to machine, analyse and image materials at the micro- and nanoscale. However, FIB modifies the integrity of the sample by creating defects that cause lattice distortions. Methods have been developed to reduce FIB-induced strain; however, these protocols need to be evaluated for their effectiveness. Here, non-destructive Bragg coherent X-ray diffraction imaging is used to study the in situ annealing of FIB-milled gold microcrystals. Two non-collinear reflections are simultaneously measured for two different crystals during a single annealing cycle, demonstrating the ability to reliably track the location of multiple Bragg peaks during thermal annealing. The thermal lattice expansion of each crystal is used to calculate the local temperature. This is compared with thermocouple readings, which are shown to be substantially affected by thermal resistance. To evaluate the annealing process, each reflection is analysed by considering facet area evolution, cross-correlation maps of the displacement field and binarized morphology, and average strain plots. The crystal's strain and morphology evolve with increasing temperature, which is likely to be caused by the diffusion of gallium in gold below ~280°C and the self-diffusion of gold above ~280°C. The majority of FIB-induced strains are removed by 380–410°C, depending on which reflection is being considered. These observations highlight the importance of measuring multiple reflections to unambiguously interpret material behaviour.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2018

Gold Code-Phase-Shift Keying: A Power and Bandwidth Efficient Communication Scheme for Smart Buildings

Advanced communications, sensors and controls play an important role in reducing the energy consumption of smart buildings. Wireless sensors have been recently deployed in buildings to provide monitoring and control of several devices such as heating, ventilation, and air-conditioning (HVAC) and lighting systems. In this paper, we present a low-power bandwidth-efficient communication scheme that can be driven by energy harvesting in self-powered wireless sensors. The proposed communication scheme is based on Gold code-phase-shift keying (CPSK) spread-spectrum signaling that improves both transmitter range and power consumption. We present our efforts toward exploring the design, implementation, and performance evaluation of a hardware prototypic Gold CPSK spread-spectrum radio transceiver. Experimental testing in addition to end-to-end system-level simulation-based studies are conducted to evaluate the performance of the Gold CPSK transceiver in terms of receiver sensitivity, coverage range, average probability of bit-error over standard Gaussian and Rayleigh fading-type channels, and multiple access capabilities. The specific engineering tradeoffs are also discussed.

Killough, Stephen M.↗

DOE OSTI2014

SU-E-T-231: Measurements of Gold Nanoparticle-Mediated Proton Dose Enhancement Due to Particle-Induced X-Ray Emission and Activation Products Using Radiochromic Films and CdTe Detector

Purpose: There have been several reports of enhanced cell-killing and tumor regression when tumor cells and mouse tumors were loaded with gold nanoparticles (GNPs) prior to proton irradiation. While particle-induced xray emission (PIXE), Auger electrons, secondary electrons, free radicals, and biological effects have been suggested as potential mechanisms responsible for the observed GNP-mediated dose enhancement/radiosensitization, there is a lack of quantitative analysis regarding the contribution from each mechanism. Here, we report our experimental effort to quantify some of these effects. Methods: 5-cm-long cylindrical plastic vials were filled with 1.8 mL of either water or water mixed with cylindrical GNPs at the same gold concentration (0.3 mg Au/g) as used in previous animal studies. A piece of EBT2 radiochromic film (30-µm active-layer sandwiched between 80/175-µm outer-layers) was inserted along the long axis of each vial and used to measure dose enhancement due to PIXE from GNPs. Vials were placed at center-of-modulation (COM) and 3-cm up-/down-stream from COM and irradiated with 5 different doses (2–10 Gy) using 10-cm-SOBP 160-MeV protons. After irradiation, films were cleaned and read to determine the delivered dose. A vial containing spherical GNPs (20 mg Au/g) was also irradiated, and gamma-rays from activation products were measured using a cadmium-telluride (CdTe) detector. Results: Film measurements showed no significant dose enhancement beyond the experimental uncertainty (∼2%). There was a detectable activation product from GNPs, but it appeared to contribute to dose enhancement minimally (<0.01%). Conclusion: Considering the composition of EBT2 film, it can be inferred that gold characteristic x-rays from PIXE and their secondary electrons make insignificant contribution to dose enhancement. The current investigation also suggests negligible dose enhancement due to activation products. Thus, previously-reported GNP-mediated proton dose enhancement/radiosensitization needs to be attributed to one or more of the other mechanisms listed earlier. Supported in part by NIH/NCI grant R01CA155446;This investigation was supported in part by NIH/NCI grant R01CA155446.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2015

MO-FG-BRA-02: Modulation of Clinical Orthovoltage X-Ray Spectrum Further Enhances Radiosensitization of Cancer Cells Targeted with Gold Nanoparticles

Purpose: To assess the potential to amplify radiosensitization of cancer cells targeted with gold nanoparticles by augmenting selective spectral components of X-ray beam. Methods: Human prostate cancer cells were treated for 24h with gold nanorods conjugated to goserelin acetate or pegylated, systematically washed and irradiated with 250 kVp X-rays (25mA, 0.25mm Cu- filter, 8x8cm{sup 2} field size, 50cm SSD) with or without an additional 0.25 mm Erbium (Er) filter. As demonstrated in a companion Monte Carlo study, Er-filter acted as an external target to feed Erbium K-shell X-ray fluorescence photons (∼50 keV) into the 250 kVp beam. After irradiation, we performed measurements of clonogenic viability with doses between 0 -6Gy, irreparable DNA damage assay to measure double-strand breaks via γH2AX-foci staining, and production of stable reactive oxygen species (ROS). Results: The clonogenic assay for the group treated with conjugated nanoparticles showed radiosensitization enhancement factor (REF), calculated at the 10% survival fraction aisle, of (1.62±0.07) vs. (1.23±0.04) with/without the Er-filter in the 250 kVp beam, respectively. The group treated with pegylated nanoparticles, albeit retained in modest amounts within the cells, also showed statistically significant REF (1.13±0.09) when the Erbium filter was added to the beam. No significant radiosensitization was observed for other groups. Measurements of ROS levels showed increments of (1.9±0.2) vs. (1.4±0.1) for combined treatment with targeted nanoparticles and Er-filtered beam. γH2AX-foci showed 50% increase for the same treatment combination, confirming the enhanced radiosensitization in a consistent fashion. Conclusion: Our study demonstrates the feasibility of enhancing radiosensitization of cancer cells by combining actively targeted gold nanoparticles and modulating the X-ray spectrum in the desired energy range. The established technique will not only help develop strategies to maximize nanoparticle-mediated radiosensitization but also offer a convenient way to acquire unprecedented insights into the role of photon energy for the observed radiosensitization effects. Supported by DOD/PCRP grant W81XWH-12-1-0198.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2015

TU-F-CAMPUS-T-03: Enhancing the Tumor Specific Radiosensitization Using Molecular Targeted Gold Nanorods

Purpose: Gold nanoparticle (GNP) mediated radiosensitization has gained significant attention in recent years. However, the widely used passive targeting strategy requires high concentration of GNPs to induce the desired therapeutic effect, thus dampening the enthusiasm for clinical translation. The purpose of this study is to utilize a molecular targeting strategy to minimize the concentration of GNPs injected while simultaneously enhancing the tumor specific radiosensitization for an improved therapeutic outcome. Methods: Cetuximab (antibody specific to the epidermal growth factor receptor that is over-expressed in tumors) conjugated gold nanorods (cGNRs) was used for the tumor targeting. The binding affinity, internalization, and in vitro radiosensitization were evaluated using dark field microscopy, transmission electron microscopy, and clonogenic cell survival assay, respectively. In vivo biodistribution in tumor (HCT116-colorectal cancer cells) bearing mice were quantified using inductively coupled plasma mass spectrometry. In vivo radiosensitization potential was tested using 250-kVp x-rays and clinically relevant 6-MV radiation beams. Results: cGNRs displayed excellent cell-surface binding and internalization (∼31,000 vs 12,000/cell) when compared to unconjugated GNRs (pGNRs). In vitro, the dose enhancement factor at 10% survival (DEF10) was estimated as 1.06 and 1.17, respectively for both 250-kVp and 6-MV beams. In vivo biodistribution analysis revealed enhanced uptake of cGNRs in tumor (1.3 µg/g of tumor tissue), which is ∼1000-fold less than the reported values using passive targeting strategy. Nonetheless, significant radiosensitization was observed in vivo with cGNRs when compared to pGNRs, when irradiated with 250-kVp (tumor volume doubling time 35 days vs 25 days; p=0.002) and 6 MV (17 days vs 13 days; p=0.0052) beams. Conclusion: The enhanced radiosensitization effect observed with very low intratumoral concentrations of gold and megavoltage x-rays using the active targeting strategy holds promise for clinical translation of this strategy from a toxicity and cost-effectiveness perspective and could evolve as a paradigm-changing approach in the field of radiation oncology.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2016

Density Functional Investigation of the Inclusion of Gold Clusters on a CH 3 S Self-Assembled Lattice on Au(111)

We employ first-principles density functional theoretical calculations to address the inclusion of gold (Au) clusters in a well-packed CH 3 S self-assembled lattice. We compute CH 3 S adsorption energies to quantify the energetic stability of the self-assembly and gold adsorption and dissolution energies to characterize the structural stability of a series of Au clusters adsorbed at the SAM-Au interface. Our results indicate that the inclusion of Au clusters with less than four Au atoms in the SAM-Au interface enhances the binding of CH 3 S species. In contrast, larger Au clusters destabilize the self-assembly. We attribute this effect to the low-coordinated gold atoms in the cluster. For small clusters, these low-coordinated sites have significantly different electronic properties compared to larger islands, which makes the binding with the self-assembly energetically more favorable. Our results further indicate that Au clusters in the SAM-Au interface are thermodynamically unstable and they will tend to dissolve, producing Au adatoms incorporated in the self-assembly in the form of CH 3 S-Au-SCH 3 species. This is due to the strong S-Au bond which stabilizes single Au adatoms in the self-assembly. Our results provide solid insight into the impact of adatom islands at the CH 3 S-Au interface.

Allen, Darnel J.↗

DOE OSTI2018

Low Density Gold Nanowire Aerogels: Synthetic Control through Ligand Exchange

Gold nanowire aerogels have been formed through freeze casting aqueous suspensions of high quality gold nanowires (AuNW). Since the properties of the final aerogel are highly dependent upon the freeze casting conditions, moving from aqueous to organic suspensions would open a new parameter space for optimization of aerogel properties and processing conditions. In this study, the surface chemistry of gold nanowires was modified through ligand exchange in order to improve their colloidal stability in nonpolar organic solvents.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Unraveling the Effects of Melt–Mantle Interactions on the Gold Fertility of Magmas

The oxidation state of the Earth’s mantle and its partial melting products exert a key control on the behavior and distribution of sulfur and chalcophile and siderophile elements between the mantle and crust, underpinning models of ore deposit formation. Whether the oxidized nature of magmas is inherited from the asthenospheric mantle source or acquired during ascent and differentiation is vigorously debated, limiting our understanding of the mechanisms of extraction of sulfur and metals from the mantle. Here, we focused on the redox-sensitive behavior of sulfur in apatite crystallized from quenched alkaline basaltic melts preserved within a peridotite xenolith from the El Deseado Massif auriferous province in southern Patagonia. We took advantage of this unique setting to elucidate the redox evolution of melts during their ascent through the subcontinental lithospheric mantle (SCLM) and grasp the inner workings of the Earth’s mantle during gold metallogenesis. Our data reveal that an initially reduced silicate melt (ΔFMQ -2.2 to -1.2) was oxidized to ΔFMQ between 0 and 1.2 during percolation and interaction with the surrounding peridotite wall-rock (ΔFMQ 0 to +0.8). This process triggered changes in sulfur speciation and solubility in the silicate melt, boosting the potential of the melt to scavenge ore metals such as gold. We suggest that large redox gradients resulting from the interaction between ascending melts and the surrounding mantle can potentially modify the oxidation state of primitive melts and enhance their metallogenic fertility. Among other factors including an enriched metal source and favorable geodynamic conditions, redox gradients in the mantle may exert a first-order control on the global-scale localization of crustal provinces endowed with gold deposits.

58 GEOSCIENCES↗

NASA NTRS1967

Substituting gold for silver improves electrical connections

In attaching external leads to thin film sensors of platinum ribbon, liquid gold is applied to each end of the ribbon and the leads are soldered to the cured gold. The cured and soldered liquid gold shows no tendency to migrate and retains initial resistance characteristics when exposed to elevated temperatures.

Loyd, J. R.↗

NASA NTRS1972

Evidence for the negative work function associated with positrons in gold.

Observation that positrons which have been thermalized in various moderators and coated with approximately 200-A gold leave the gold surface with an energy which peaks between 0.75 and 2.90 eV. This energy is thought to be associated with a positron or 'negative' work function of gold.

Costello, D. G.↗

NASA NTRS1975

On the controversy about the direction of electrotransport in thin gold films

Annealed 'pure' gold films exhibit electromigration against the electron flow. In contrast, gold films deposited on a transition metal underlayer show mass flow in the same direction as the electron flow. Diffusion of the transition metal from the underlayer into the gold film, deduced from Auger analyses presented herein, is believed to be responsible for this reversal. A new experiment, utilizing an 'inverted temperature profile' gives unambiguous results on the direction of electrotransport.

Hummel, R. E.↗