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NASA NTRS1997

Third Order Optical Nonlinearity of Colloidal Metal Nanoclusters Formed by MeV Ion Implantation

We report the results of characterization of nonlinear refractive index of the composite material produced by MeV Ag ion implantation of LiNbO(sub 3) crystal (z-cut). The material after implantation exhibited a linear optical absorption spectrum with the surface plasmon peak near 430 nm attributed to the colloidal silver nanoclusters. Heat treatment of the material at 500 deg C caused a shift of the absorption peak to 550 nm. The nonlinear refractive index of the sample after heat treatment was measured in the region of the absorption peak with the Z-scan technique using a tunable picosecond laser source (4.5 ps pulse width).The experimental data were compared against the reference sample made of MeV Cu implanted silica with the absorption peak in the same region. The nonlinear index of the Ag implanted LiNbO(sub 3) sample produced at five times less fluence is on average two times greater than that of the reference.

Sarkisov, S. S.↗

DOE OSTI2021

Demonstration of a laser-driven, narrow spectral bandwidth x-ray source for collective x-ray scattering experiments

X-ray Thomson scattering (XRTS) is a powerful diagnostic technique that involves an x-ray source interacting with a dense plasma sample, resulting in a spectrum of elastically and inelastically scattered x-rays. Depending on the plasma conditions, one can measure a range of parameters from the resulting spectrum, including plasma temperature, electron density, and ionization state. To achieve sensitivity to collective electron oscillations, XRTS measurements require limited momentum transfer where the spectral separation of elastic and inelastic scattering is small. Such measurements require an x-ray probe source with a narrow bandwidth in order to reduce the spectral overlap between scattering contributions, allowing for the different features to be more precisely deconvolved. In this investigation, we discuss the theory behind how the bandwidth for a common XRTS probe, Zn He-α emission at 9 keV, can be reduced using a Cu K-edge filter.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

NASA NTRS1981

Intraband optical conductivity sigma/omega,T/ of Cu, Ag, and Au - Contribution from electron-electron scattering

The frequency and temperature dependence of the intraband optical conductivity of the noble metals Cu, Ag and Au is measured and contributions of electron-electron scattering are assessed. Optical measurements were performed at temperatures of 77, 295 and 425 K to obtain values of the Drude electron scattering rate with a linear dependence on temperature which may be attributed to electron-phonon scattering, and a quadratic dependence on photon energy, which is suggestive of electron-electron scattering but is a factor of two to three times greater than would be expected. Comparison of the optical data with dc electrical and thermal resistivity data which also show behavior attributed to electron-electron scattering reveals discrepancies of up to an order of magnitude. Other possible mechanisms for the frequency dependence, including absorptance, electron-surface plasmon interactions, a two-carrier model, and a structure dependence are considered, and it is concluded that the frequency dependence in the Drude scattering rates of the noble metals is not yet quantitatively understood

Parkins, G. R.↗

DOE OSTI2020

Nanoparticle-Enhanced Plasma Discharge Using Nanosecond High-Voltage Pulses

By discharging nanosecond high-voltage (5 kV) pulses across an insulating substrate containing Au, Pt, or Cu nanoparticles, a 3 order of magnitude (1000×) enhancement in the generation of plasma can be achieved through local field enhancement on the surface of the nanoparticles. The low-temperature nature of this transient plasma is crucial to maintaining the structural integrity of these delicate nanoparticles. These nanoparticles provide up to a 1000-fold enhancement in the generation of the plasma, which is localized to the surface of the nanoparticles where it is potentially useful (e.g., for catalysis). Additionally, we performed both time-domain and frequency-domain calculations of the electromagnetic response of the nanoparticles based on high-resolution transmission electron microscope (HRTEM) images, which show local field enhancement of the nanosecond high-voltage pulse on the order of 3×. Since the plasma initiation depends exponentially on the peak electric field strength, this 3-fold increase in the local electric field can result in a several orders of magnitude increases in the generation of plasma at a given applied external field strength. In order to rule out plasmon-resonance enhancement, which is often associated with small metal nanoparticles, we performed finite difference time domain (FDTD) simulations in the optical frequency domain, which show that the effect of plasmon resonance is negligible for Pt nanoparticles. We therefore attribute the nanoparticle-based enhancement to the generation of plasma (an electrostatic effect) rather than enhanced coupling of light from the near field to the far field via the plasmon resonance phenomenon (an optical effect).

36 MATERIALS SCIENCE↗

DOE OSTI2022

Stability of Polyethylene Glycol-Coated Copper Nanoparticles and Their Optical Properties

Oxidation is a corrosion reaction where the corroded metal forms an oxide. Prevention of oxidation at the nanoscale is critically important to retain the physicochemical properties of metal nanoparticles. In this work, we studied the stability of polyethylene glycol (PEG) coated copper nanoparticles (PEGylated CuNPs) against oxidation. The freshly-prepared PEGylated CuNPs mainly consist of metallic Cu which are quite stable in air although their surfaces are typically covered with a few monolayers of cuprous oxide. However, they are quickly oxidized in water due to the presence of protons that facilitate oxidation of the cuprous oxide to cupric oxide. PEG with carboxylic acid terminus could slightly delay the oxidation process compared to that with thiol terminus. It was found that a solvent with reducing power such as ethanol could greatly enhance the stability of PEGylated CuNPs by preventing further oxidation of the cuprous oxide to cupric oxide and thus retain the optical properties of CuNPs. The reducing environment also assists the galvanic replacement of these PEGylated CuNPs to form hollow nanoshells; however, they consist of ultra-small particle assemblies due to the co-reduction of gold precursor during the replacement reaction. As a result, these nanoshells do not exhibit strong optical properties in the near-infrared region. This study highlights the importance of solvent effects on PEGylated nonprecious metal nanoparticles against oxidation corrosion and its applications in preserving physicochemical properties of metallic nanostructures.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2025

De Nive Quinquangula: Pentagonal Snowflake Metal Nanocrystals as an Example of Emergence Phenomenon in Nanotechnology Complex Systems

The formation of snowflakes (SFL) is one of the most captivating phenomena in nature. The fabrication of multimetallic gold (Au) nanoparticles containing copper (Cu) and iron (Fe) is reported, which adopt snowflake-like morphology after nanoparticle aggregation. The synthesis of these snowflake-like Au microcrystals occurs mainly by kinetic control. In this process, a surfactant-assisted salt reduction method is employed on a heated substrate. Here, the metal salts react within seconds to form nanoparticles. This process results in a hierarchical structure with pseudo-pentagonal symmetry and chiroptical activity. We discuss how large superstructures emerge from nanoparticle aggregation, resembling natural snowflakes. However, unlike ice snowflakes, which exhibit hexagonal symmetry, the Au snowflakes display pentagonal symmetry. It is proposed that the formation of these snowflake-like microcrystals is the result of the complexity involved in the crystal growth process and represents an example of the phenomenon of emergence, which has become very significant in several fields of modern science, including physics, biology, chemistry, economics, philosophy, and poetry. The term emergent is used to evoke the collective behavior of a large number of microscopic constituents that is qualitatively different than the behaviors of the individual constituents.

36 MATERIALS SCIENCE↗