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At least 595 records · Page 33
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Phonon modulation of strongly coupled gold tetrahedral plasmonic nanoparticles and a carbocyanine J-aggregate

Coupling exciton and plasmon excitations to form polaritons are of great interest for manipulating energy transfer at the nanoscale via the formation of hybrid light–matter states. In this study, we successfully couple gold tetrahedral nanoparticles with the J-aggregate forming dye 5,5′,6,6′-tetrachloro-1,1′-diethyl-3,3′-di(4-sulfobutyl)-benzimidazolocarbocyanine (TDBC) to form a strongly coupled colloidal polariton system with a Rabi splitting energy of ∼206 meV. These gold tetrahedra exhibit coherent phonon modes upon photoexcitation, which produce transient oscillations of the LSPR energy for isolated tetrahedra. Transient absorption measurements of the polariton system were performed and show how these coherent phonon modes influence the polariton states’ extinction. We found that the oscillation period increases by 0.5 ± 0.14 ps upon surface deposition of TDBC dye, demonstrating LSPR sensitivity to the refractive index environment. Shifts in the plasmon resonance due to the coherent phonon modes transiently alters LSPR alignment with the J-aggregate exciton peak, resulting in shifts of the hybrid polariton states’ oscillator strength.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Tamper indicating gold nanocup plasmonic films

The spectral signature of nanoplasmonic films are both robust and tailorable with optical responses ranging from the visible to the near-infrared. We present the development of flexible, elastomeric nanoplasmonic films consisting of periodic arrays of gold nanocups as tamper indicating films. Gold nanocups have polarization-sensitive optical properties that may be manufactured into films that offer unique advantages for tamper indication. These flexible films can be made quickly and at low-cost using commercially available monodisperse polystyrene nanospheres through self-assembly followed by plasma etching, metal deposition, and lift-off from a sacrificial substrate. Polarization- and angle-dependent optical spectroscopic measurements were performed to characterize the fabricated films. Furthermore, using polarization-sensitive hyperspectral imaging, we demonstrate how these films can be applied to tamper indication and counterfeit resistance applications.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Hybrid-PIC modeling of laser-plasma interactions and hot electron generation in gold hohlraum walls

The walls of the hohlraum used in experiments at the national ignition facility are heated by laser beams with intensities ∼1015 W/cm2, a wavelength of ∼1/3 μm, and pulse lengths on the order of a ns, with collisional absorption believed to be the primary heating mechanism. X-rays generated by the hot ablated plasma at the gold walls are then used to implode a target in the hohlraum interior. In addition to the collisional absorption of laser energy at the walls, non-linear laser-plasma interactions (LPI), such as stimulated Raman scattering and two plasmon decay, are believed to generate a population of supra-thermal electrons which, if present in the hohlraum, can have a deleterious effect on target implosion. We describe results of hohlraum modeling using a hybrid particle-in-cell code. To enable this work, new particle-based algorithms for a multiple-ion magneto-hydrodynamic (MHD) treatment, and a particle-based ray-tracing model were developed. The use of such hybrid methods relaxes the requirement to resolve the laser wavelength, and allows for relatively large-scale hohlraum simulations with a reasonable number of cells. But the non-linear effects which are believed to be the cause of hot electron generation can only be captured by fully kinetic simulations with good resolution of the laser wavelength. For this reason, we employ a two-tiered approach to hohlraum modeling. Large-scale simulations of the collisional absorption process can be conducted using the fast quasi-neutral MHD algorithm with fluid particle species. From these simulations, we can observe the time evolution of the hohlraum walls and characterize the density and temperature profiles. From these results, we can transition to smaller-scale highly resolved simulations using traditional kinetic particle-in-cell methods, from which we can fully model all of the non-linear laser-plasma interactions, as well as assess the details of the electron distribution function. We find that vacuum hohlraums should be stable to both two plasmon decay and stimulated Raman scattering instabilities for intensities ≤1015 W/cm2. In gas-filled hohlraums, shocks may be induced in the blowoff gold plasma, which leads to more complex density and temperatures profiles. The resulting effect on LPI stability depends strongly on the details of the profile, and it is possible for the gas-filled hohlraum to become unstable to two plasmon decay at 1015 W/cm2 if the quarter-critical surface reaches temperatures exceeding 1 keV.

Thoma, C.↗
DOE OSTI2019

Monitoring the growth dynamics of colloidal gold-silver core-shell nanoparticles using in situ second harmonic generation and extinction spectroscopy

The growth dynamics of gold-silver core-shell (Au@Ag) nanoparticles are studied using in situ time-dependent second harmonic generation (SHG) and extinction spectroscopy to investigate the nanoparticle shell formation. The silver shell is grown by reduction of silver cations onto a 14 nm gold core using ascorbic acid in colloidal aqueous solution under varying reaction concentrations producing Au@Ag nanoparticles of final sizes ranging from 51 to 78 nm in diameter. The in situ extinction spectra show a rapid increase in intensity on the timescale of 5–6 s with blue shifting and narrowing of the plasmonic peak during the silver shell formation. The in situ SHG signals show an abrupt rise at early times of the reaction, followed by a time-dependent biexponential decrease, where the faster SHG lifetime corresponds to the timescale of the shell growth, and where the slower SHG lifetime is attributed to changes in the nanoparticle surface charge density. A large enhancement in the SHG signal at early stages of the reaction is caused by plasmonic hot spots due to the nanoparticle surface morphology, which becomes smoother as the reaction proceeds. The final extinction spectra are compared to finite-difference time-domain (FDTD) calculations, showing general agreement with experiment, where the plasmon peak red shifts and increases in spectral width as the silver shell thickness increases. These in situ SHG and extinction spectroscopy results, combined with FDTD calculations, help characterize the complicated processes involved in colloidal nanoparticle shell formation in real time for developing potential plasmon-enhanced nanomaterial applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Investigation of heat transport using directly driven gold spheres

Recently, heat transport was investigated using a directly driven beryllium sphere [Farmer et al., Phys. Plasmas 27, 082701 (2020)]. Models that overly restrict heat transport were rejected. This paper extends work to directly driven gold spheres where radiation loss is more important. Here, gold coated spheres are directly driven at the OMEGA laser facility at intensities of 5×10 14 W/cm 2 . Plasma conditions, laser coupling, and x-ray flux are all measured. Additionally, comparisons to 2D radiation-hydrodynamic simulations are performed. Simulations use three common heat transport models: local transport with flux limiters of f = 0.15 and f = 0.03, and the nonlocal Schurtz–Nicolai–Busquet (SNB) model. It is shown that both the SNB model and f = 0.15 match the measured plasma conditions with the SNB model better capturing the temporal evolution of electron temperature. The f = 0.03 model predicts too low of an electron density and too hot of a temperature. The measured scattered light is roughly 6% of the incident energy, the f = 0.15 and SNB models predict 0.5% uncoupled light, and f = 0.03, 38% uncoupled light. The x-ray fluxes in the f = 0.15 and SNB simulations rise too quickly and are just outside the measurement's error, while the x-ray flux in the f = 0.03 simulation is low by a factor of two-three. For these reasons, the f = 0.03 model is rejected.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

The action-integral and energy to explode short gold wires in ambient air

This paper is about electrically induced explosions of short (1 mm) and thin (38 μm diameter) gold bridgewires in ambient air and contrasts this behavior with that observed for longer wires in a vacuum used in applications such as Z-pinch systems. The action-integral (the time integral of the wire current squared) and energy-to-burst are measured using high current discharge systems. It is found that in contrast to some reports, the action-integral to burst is not a constant for a specific wire geometry and material but, instead, is a function of the rate of current change in the wire around the time of burst and the related metric of the current flux at burst. Furthermore, it is found that the accuracy of the constant action-integral to burst approximation is dependent on the discharge system used. Short gold wires such as these have relevancy to exploding bridgewire detonators.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Ultrafast electron dynamics in platinum and gold thin films driven by optical and terahertz fields

Here, we investigate the ultrafast electron dynamics triggered by terahertz and optical pulses in thin platinum and gold films by probing their transient optical reflectivity. The response of the platinum film to an intense terahertz pulse is similar to the optically induced one and can be described by a two-temperature model with a 20% larger electron–phonon coupling for the terahertz-driven dynamics compared to the optically induced one, ascribed to an additional nonthermal electron–phonon coupling contribution. Surprisingly, gold films exhibit a much smaller terahertz pulse-induced reflectivity change and with a sign opposite to the optical case. Additionally we explain this remarkable observation with field emission of electrons due to Fowler–Nordheim tunneling, enabled in samples with thicknesses below the structural percolation threshold, where nanostructuring promotes near-field enhancement. Our results provide a fundamental insight into the ultrafast processes relevant to modern electro- and magneto-optical applications.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Signature of a pair of Majorana zero modes in superconducting gold surface states

Under certain conditions, a fermion in a superconductor can separate in space into two parts known as Majorana zero modes, which are immune to decoherence from local noise sources and are attractive building blocks for quantum computers. Promising experimental progress has been made to demonstrate Majorana zero modes in materials with strong spin–orbit coupling proximity coupled to superconductors. Here we report signatures of Majorana zero modes in a material platform utilizing the surface states of gold. Using scanning tunneling microscope to probe EuS islands grown on top of gold nanowires, we observe two well-separated zero-bias tunneling conductance peaks aligned along the direction of the applied magnetic field, as expected for a pair of Majorana zero modes. This platform has the advantage of having a robust energy scale and the possibility of realizing complex designs using lithographic methods.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Self-assembly of large-scale crack-free gold nanoparticle films using a ‘drain-to-deposit’ strategy

Gold nanoparticles are widely studied due to the ease of controlled synthesis, facile surface modification, and interesting physical properties. However, a technique for depositing large-area, crack-free monolayers on solid substrates is lacking. Herein is presented a method for accomplishing this. Spherical gold nanoparticles were synthesized as an aqueous dispersion. Assembly into monolayers and ligand exchange occurred simultaneously at an organic/aqueous interface. Then the monolayer film was deposited onto arbitrary solid substrates by slowly pumping out the lower, aqueous phase. This allowed the monolayer film (and liquid–liquid interface) to descend without significant disturbance, eventually reaching substrates contained in the aqueous phase. The resulting macroscopic quality of the films was found to be superior to films transferred by Langmuir techniques. The surface plasmon resonance and Raman enhancement of the films were evaluated and found to be uniform across the surface of each film.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2019

Silver and gold doped hydroxyapatite nanocomposites for enhanced bone regeneration

In this work, we report the osteogenic potential of silver (Ag), gold (Au), or silver–gold doped hydroxyapatite nanoparticles (Ag-Au-HA) in zebrafish (ZF) jawbone regeneration (JBR) model. The hydroxyapatite (HA, Ca 10 (PO 4 ) 6 (OH) 2 ), Ag-HA, Au-HA, and Ag-Au-HA nanomaterials were synthesized by the co-precipitation procedure. The surface structures of Ag-HA, Au-HA, HA, and Ag-Au-HA were analysed by scanning electron microscopy, transmission-electron microscopy (TEM), x-ray diffraction, Fourier transform infrared (FTIR), UV–vis, energy dispersive x-ray spectroscopy (EDS), elemental mapping, and laser fluorescent spectroscopy. The TEM and EDS analysis confirmed that the Ag and Au are associated with the surface of HA nanoparticle. The chemical structure of HA, Ag-HA, Au-HA, and Ag-Au-HA nanoparticles was validated by FTIR and EDS analysis. We observed that Ag and Au are associated with HA nanoparticles by electrostatic, wander wall, and electrostatic and H-bonding interaction. The effect of Ag-HA, Au-HA, and Ag-Au-HA nanoparticles on bone regeneration was confirmed by ZF JBR model. The significant growth of ZF bone regeneration was observed in Ag-Au-HA nanoparticles as compared with HA, Ag-HA, and Au-HA nanoparticles. In conclusion, these results indicating a therapeutic potential of Ag-Au-HA compositions suggest these nanomaterials would be excellent for bone regeneration and fracture healing.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Emergence of liquid following laser melting of gold thin films

X-ray structural science is undergoing a revolution driven by the emergence of X-ray Free-electron Laser (XFEL) facilities. The structures of crystalline solids can now be studied on the picosecond time scale relevant to phonons, atomic vibrations which travel at acoustic velocities. In the work presented here, X-ray diffuse scattering is employed to characterize the time dependence of the liquid phase emerging from femtosecond laser-induced melting of polycrystalline gold thin films using an XFEL. In a previous analysis of Bragg peak profiles, we showed the supersonic disappearance of the solid phase and presented a model of pumped hot electrons carrying energy from the gold surface to scatter at internal grain boundaries. This generates melt fronts propagating relatively slowly into the crystal grains. By conversion of diffuse scattering to a partial X-ray pair distribution function, we demonstrate that it has the characteristic shape obtained by Fourier transformation of the measured F ( Q ). The diffuse signal fraction increases with a characteristic rise-time of 13 ps, roughly independent of the incident pump fluence and consequent final liquid fraction. This suggests the role of further melt-front nucleation processes beyond grain boundaries.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Revealing Three-Dimensional Morphology in Nanoporous Gold Using Three-Dimensional X-Ray Fresnel Coherent Diffractive Imaging Tomography

Nanoporous metals fabricated by dealloying have a unique bi-continuous, sponge-like porous structure with ultra-high surface area. The unique properties of these materials, especially nanoporous gold, have numerous potential applications in sensors and actuators and in energy-related applications such as catalytic materials, super-capacitors, and battery supports. The degree of porosity and size of the metal ligaments are critical parameters that determine many properties and thus govern the functionalities of nanoporous metals in many applications including energy storage and conversion. Additionally, we used Fresnel coherent diffractive imaging combined with tomographic reconstruction to quantify the nanoscale three-dimensional spatial distribution and homogeneity of the porosity and ligament size within a bulk sample of nanoporous gold. The average porosity and its standard deviation along the axial direction through the sample were determined, as well as the characteristic feature size and its standard deviation. The result shows that free corrosion is an effective way to create homogeneous nanoporous metals with sample sizes on the order of 1 µm.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Efficient Coupling and Transport of a Surface Plasmon at 780 nm in a Gold Nanostructure

We studied plasmonic nanostructures in single-crystal gold with scanning electron and femtosecond photoemission electron microscopies. We designed an integrated laser coupling and nanowire waveguide structure by focused ion beam lithography in single-crystal gold flakes. The photoemission results show that the laser field is efficiently coupled into a propagating surface plasmon by a simple hole structure and propagates efficiently in an adjacent nano-bar waveguide. A strong local field is created by the propagating surface plasmon at the nano-bar tip. A similar structure, with a decreased waveguide width and thickness, displayed significantly more intense photoemission indicating enhanced local electric field at the sharper tip.

Gong, Yu↗
DOE OSTI2015

SU-E-T-46: A Monte Carlo Investigation of Radiation Interactions with Gold Nanoparticles in Water for 6 MV, 85 KeV and 40 KeV Photon Beams

Purpose: To determine the effect of gold-nanoparticles (AuNPs) on energy deposition in water for different irradiation conditions. Methods: TOPAS version B12 Monte Carlo code was used to simulate energy deposition in water from monoenergetic 40 keV and 85 keV photon beams and a 6 MV Varian Clinac photon beam (IAEA phase space file, 10x10 cm{sup 2}, SSD 100 cm). For the 40 and 85 keV beams, monoenergetic 2x2 mm{sup 2} parallel beams were used to irradiate a 30x30x10 µm {sup 3} water mini-phantom located at 1.5 cm depth in a 30x30x50 cm{sup 3} water phantom. 5000 AuNPs of 50 nm diameter were randomly distributed inside the mini-phantom. Energy deposition was scored in the mini-phantom with the AuNPs’ material set to gold and then water. For the 6 MV beam, we created another phase space (PHSP) file on the surface of a 2 mm diameter sphere located at 1.5 cm depth in the water phantom. The PHSP file consisted of all particles entering the sphere including backscattered particles. Simulations were then performed using the new PHSP as the source with the mini-phantom centered in a 2 mm diameter water sphere in vacuum. The g4em-livermore reference list was used with “EMRangeMin/EMRangeMax = 100 eV/7 MeV” and “SetProductionCutLowerEdge = 990 eV” to create the new PHSP, and “SetProductionCutLowerEdge = 100 eV” for the mini-phantom simulations. All other parameters were set as defaults (“finalRange = 100 µm”). Results: The addition of AuNPs resulted in an increase in the mini-phantom energy deposition of (7.5 ± 8.7)%, (1.6 ± 8.2)%, and (−0.6 ± 1.1)% for 40 keV, 85 keV and 6 MV beams respectively. Conclusion: Enhanced energy deposition was seen at low photon energies, but decreased with increasing energy. No enhancement was observed for the 6 MV beam. Future work is required to decrease the statistical uncertainties in the simulations. This research is partially supported from institutional funds from the Center for Radiation Oncology Research, The University of Texas MD Anderson Cancer Center.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2015

SU-E-T-359: Emulation of Yb-169 Gamma-Ray Spectrum Using Metal-Filtered 250 KVp X-Rays for Pre-Clinical Studies of Gold Nanoparticle-Aided Radiation Therapy

Purpose: To develop an external beam surrogate of the Yb-169 brachytherapy source applying a filter-based spectrum modulation technique to 250 kVp x-rays. In-vitro/vivo studies performed with the modulated 250 kVp beam will help gauge the benefits of implementing gold nanoparticle-aided radiotherapy with the Yb-169 source. Methods: A previously validated MCNP5 model of the Phillips RT-250 orthovoltage unit was used to obtain the percentage depth dose (PDD) and filtered photon spectra for a variety of filtration and irradiation conditions. Photon spectra were obtained using the average flux F4 tally in air right after all collimation. A 30 x 30 x 30 cm{sup 3} water phantom was used to compute the PDD along the central axis (CAX) under the standards conditions of a 10 x 10 cm{sup 2} field size at 50 cm SSD. Cylindrical cells of 4 cm in diameter and the energy deposition F6 tally were used along the CAX to score the doses down to 20 cm depth. The number of particle history was set to 2 x 10{sup 8} in order to keep the relative uncertainty within each cell < 0.3%. The secondary electron spectrum within a gold-loaded tissue due to each photon spectrum was also calculated using EGSnrc and compared with that due to Yb-169 gamma rays. Results: Under the practical constraints for the spectrum modulation task, 250 kVp x-rays filtered by a 0.25 mm Erbium (Er) foil produced the best match with Yb-169 gamma rays, in terms of PDD and, more importantly, secondary electron spectrum. Conclusion: Modulation of 250kVp x-ray spectrum by an Er-filter was found effective in emulating the gamma ray spectrum of Yb-169. Possible benefits as predicted from the current MC model such as enhanced radiosensitization with the Er-filtered beam (as a surrogate of Yb-169) was confirmed with a separate in-vitro study. Supported by DOD/PCRP grant W81XWH-12-1-0198.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2016

Low Z target switching to increase tumor endothelial cell dose enhancement during gold nanoparticle-aided radiation therapy

Purpose: Previous studies have introduced gold nanoparticles as vascular-disrupting agents during radiation therapy. Crucial to this concept is the low energy photon content of the therapy radiation beam. The authors introduce a new mode of delivery including a linear accelerator target that can toggle between low Z and high Z targets during beam delivery. In this study, the authors examine the potential increase in tumor blood vessel endothelial cell radiation dose enhancement with the low Z target. Methods: The authors use Monte Carlo methods to simulate delivery of three different clinical photon beams: (1) a 6 MV standard (Cu/W) beam, (2) a 6 MV flattening filter free (Cu/W), and (3) a 6 MV (carbon) beam. The photon energy spectra for each scenario are generated for depths in tissue-equivalent material: 2, 10, and 20 cm. The endothelial dose enhancement for each target and depth is calculated using a previously published analytic method. Results: It is found that the carbon target increases the proportion of low energy (<150 keV) photons at 10 cm depth to 28% from 8% for the 6 MV standard (Cu/W) beam. This nearly quadrupling of the low energy photon content incident on a gold nanoparticle results in 7.7 times the endothelial dose enhancement as a 6 MV standard (Cu/W) beam at this depth. Increased surface dose from the low Z target can be mitigated by well-spaced beam arrangements. Conclusions: By using the fast-switching target, one can modulate the photon beam during delivery, producing a customized photon energy spectrum for each specific situation.

61 RADIATION PROTECTION AND DOSIMETRY↗
DOE OSTI2017

Enhanced Raman Scattering from NCM523 Cathodes Coated with Electrochemically Deposited Gold

Materials with the general composition LiMO2, where M is a mix of nickel, cobalt, and manganese, have been studied extensively as cathodes for lithium-based electrochemical cells. Some compositions, like LiNi0.5Co0.2Mn0.3O2 (NCM523), have already found application in commercial lithium-ion batteries. Pre-test and post-test analyses of these types of cathodes have benefited greatly from the use of Raman spectroscopy. Specifically, Raman spectroscopy can be used to investigate the phonons of the LiMO2 lattice. This is particularly useful for studies of the LiMO2 after it has been formed into the type of polymer-bonded laminate from which typical battery cathodes are cut. One of the problems that occurs in such studies is that the scattering from the LiMO2 phase gets progressively weaker as the nickel content increases. NCM523 poses one example of this behavior owing to the fact that half of the transition metal content is nickel. In this study we show that the intensity of the Raman scattering from the NCM523 phonons can be significantly increased by electroplating clusters of sub-micron gold particles on NCM523-containing laminate structures. The gold appears to plate somewhat selectively on the NCM523 particles in randomly sized clusters. These clusters stimulate the Raman scattering from the NCM523 to varying extents that can reach nearly 100 times the scattering intensity from uncoated pristine laminates.

cathode↗
DOE OSTI2019

Ultrabroadband infrared near-field spectroscopy and imaging of local resonators in percolative gold films

Percolation processes are ubiquitous in nature and are responsible for many critical phenomena such as first-order phase transitions and infectious epidemic networks. The optical properties of a percolative medium can generally be captured by the effective medium approximation (EMA) when the degree of percolation and the properties of the constituent materials are properly addressed. However, the important local collective responses of nanoclusters in the deep subwavelength regime are often only phenomenologically addressed in the standard EMA formalism. Additionally, a comprehensive method that measures local light–matter interactions and registers how the local responses influence global optical properties has yet to be established on a firm basis. In this paper, we use infrared nanoimaging/spectroscopy to investigate percolative gold films in the vicinity of the critical percolation threshold. We demonstrate experimentally and theoretically that the near-field spectra yield quantitative information of the characteristic length scale of the local gold clusters and their relative oscillator strengths. As a result, EMA analysis can be augmented with near-field nano-spectroscopy to yield better predictability of the far-field reflection spectrum at the corresponding spectral range.

36 MATERIALS SCIENCE↗