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Register a new userAccelerated alpha-decay of 232U isotope achieved by exposure of its aqueous solution with gold nanoparticles to laser radiation
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Experimental results are presented on laser-induced accelerated alpha-decay of Uranium-232 nuclei under laser exposure of Au nanoparticles in aqueous solutions of its salt. It is demonstrated that the decrease of alpha-activity strongly depends on the peak intensity of the laser radiation in the liquid and is highest at several terawatt per square centimeter. The decrease of alpha-activity of the exposed solutions is accompanied by the deviation of gamma-activities of daughter nuclides of Uranium-232 from their equilibrium values. Possible mechanisms of the laser influence on the alpha-activity are discussed on the basis of the amplification of the electric field of laser wave on metallic nanoparticles.
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We report the generation of molecular hydrogen from water by laser irradiation, without any electrodes and photocatalysts. A near infrared pulsed nanosecond laser is used for exposure of colloidal solution of Au nanoparticles suspended in water. Laser exposure of the colloidal solution results in formation of plasma of laser breakdown of liquid and emission of H2. The rate of H2 emission depends critically on the energy of laser pulses. There is a certain threshold in laser fluence in liquid (around 50 J/cm2) below which plasma disappears and H2 emission stops. H2 emission from colloidal solution of Au nanoparticles in ethanol is higher than that from similar water colloid. It is found that formation of plasma and emission of H2 or D2 can be induced by laser exposure of pure liquids, either H2O or D2O, respectively. The results are interpreted as water molecules splitting by direct electron impact from breakdown plasma.
Influence of permanent magnetic field up to 7.5 T on plasma emission and laser-assisted Au nanoparticles fragmentation in water is experimentally studied. It is found that presence of magnetic field causes the breakdown plasma emission to start earlier regarding to laser pulse. Field presence also accelerates the fragmentation of nanoparticles down to a few nanometers. Dependence of Au NPs fragmentation rate in water on magnetic field intensity is investigated. The results are discussed on the basis of laser-induced plasma interaction with magnetic field.
The performance of gold nanoparticles (NPs) in applications depends critically on the structure of the NP-solvent interface, at which the electrostatic surface polarization is one of the key characteristics that affects hydration, ionic adsorption, and electrochemical reactions. Here, we demonstrate significant effects of explicit metal polarizability on the solvation and electrostatic properties of bare gold NPs in aqueous electrolyte solutions of sodium salts of various anions (Cl$^-$, BF$_4$$^-$, PF$_6$$^-$, Nip$^-$(nitrophenolate), and 3- and 4-valent hexacyanoferrate (HCF)), using classical molecular dynamics simulations with a polarizable core-shell model of the gold atoms. We find considerable spatial heterogeneity of the polarization and electrostatic potentials on the NP surface, mediated by a highly facet-dependent structuring of the interfacial water molecules. Moreover, ion-specific, facet-dependent ion adsorption leads to large alterations of the interfacial polarization. Compared to non-polarizable NPs, polarizability modifies water local dipole densities only slightly, but has substantial effects on the electrostatic surface potentials, and leads to significant lateral redistributions of ions on the NP surface. Besides, interfacial polarization effects on the individual monovalent ions cancel out in the far field, and effective Debye-Huckel surface potentials remain essentially unaffected, as anticipated from continuum `image-charge concepts. Hence, the explicit charge response of metal NPs is crucial for the accurate description and interpretation of interfacial electrostatics (as, e.g., for charge transfer and interface polarization in catalysis and electrochemistry).
We study the solvation and electrostatic properties of bare gold (Au) nanoparticles (NPs) of $1$-$2$ nm in size in aqueous electrolyte solutions of sodium salts of various anions with large physicochemical diversity (Cl$^-$, BF$_4$$^-$, PF$_6$$^-$, Nip$^-$(nitrophenolate), 3- and 4-valent hexacyanoferrate (HCF)) using nonpolarizable, classical molecular dynamics computer simulations. We find a substantial facet selectivity in the adsorption structure and spatial distribution of the ions at the Au-NPs: while sodium and some of the anions (e.g., Cl$^-$, HCF$^{3-}$) adsorb more at the `edgy (100) and (110) facets of the NPs, where the water hydration structure is more disordered, other ions (e.g., BF$_4$$^-$, PF$_6$$^-$, Nip$^-$) prefer to adsorb strongly on the extended and rather flat (111) facets. In particular, Nip$^-$, which features an aromatic ring in its chemical structure, adsorbs strongly and perturbs the first water monolayer structure on the NP (111) facets substantially. Moreover, we calculate adsorptions, radially-resolved electrostatic potentials, as well as the far-field effective electrostatic surface charges and potentials by mapping the long-range decay of the calculated electrostatic potential distribution onto the standard Debye-Huckel form. We show how the extrapolation of these values to other ionic strengths can be performed by an analytical Adsorption-Grahame relation between effective surface charge and potential. We find for all salts negative effective surface potentials in the range from $-10$ mV for NaCl down to about $-80$ mV for NaNip, consistent with typical experimental ranges for the zeta-potential. We discuss how these values depend on the surface definition and compare them to the explicitly calculated electrostatic potentials near the NP surface, which are highly oscillatory in the $pm 0.5$ V range.
The formation of stable products of water decomposition under laser exposure of aqueous colloidal solutions of nanoparticles is experimentally studied. Laser exposure of colloidal solutions leads to formation of H2, O2, and H2O2. The dependence of the yield of these products depends on the energy density of laser radiation inside the liquid and concentration of nanoparticles. The ratio H2/O2 depends on laser fluence and is shifted towards H2. There are at least to sources of H2O2, namely, laser-induced breakdown plasma and ultrasound induced by laser pulses in the liquid. The formation of both H2 and O2 is tentatively assigned to direct dissociation of H2O molecules by electron impact from laser-induced plasma.
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