Synthesis and Properties of Au Hydride

Abstract

The generation of chemical species from gases, noble metals and light interacting with localized surface plasmons represents a new paradigm for achieving low energy sustainable reaction pathways. Here, we demonstrate that the dissociation reaction of H 2 meditated by the decay of localized surface plasmons of gold nanoparticles leads to the generation of a new material as detected by a change in the optical properties of the gold nanostructures. The effective permittivity measured by in situ spectroscopic ellipsometry shows a blue-shift of 0.02 eV in the surface plasmon resonance, demonstrating the plausible formation of a metastable gold hydride layer on the surface of nanoparticles following the dissociation of H 2 . The formation of this gold hydride through the interaction of gold with atomic H is supported by first-principles simulations. These calculations do not indicate a significant charge transfer upon hydrogenation of the (111) surface but rather large Friedel charge oscillations within the gold layer. Moreover, our blue-shift is produced by the formation of a hydride leading to changes in critical band gaps in the electronic structure. For a coverage of 11%, the calculated peak of the imaginary part of the ZZcomponent of the dielectric tensor undergoes a blue shift of 28 nm from a hydrogen free peak at 574 nm.[a] Dr.

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Structural Properties of Nanometer‐Sized Gold Nanoparticles on a Silicon Substrate

“…[14][15][16] Although it is possible to prepare extremely small Au NPs down to sub-nanometer size, their catalytic activity, however, does not always grow monotonically with decreasing size. [17] Sil et al [18] used first-principles calculations in connection with in situ spectroscopic ellipsometry to provide a method for studying the bonding between Au NPs and hydrogen driven by plasmons. [19] Recent studies show that the structure of nano-systems at the atomic scale can be obtained by using simulations and experiments along the lines suggested by Billinge & Levin.…”

“…[ 14–16 ] Although it is possible to prepare extremely small Au NPs down to sub‐nanometer size, their catalytic activity, however, does not always grow monotonically with decreasing size. [ 17 ] Sil et al [ 18 ] used first‐principles calculations in connection with in situ spectroscopic ellipsometry to provide a method for studying the bonding between Au NPs and hydrogen driven by plasmons. [ 19 ]…”