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Synthesis and Properties of Au Hydride
Author(s) -
Sil Devika,
Lane Christopher,
Glor Ethan,
Gilroy Kyle D.,
Sylla Safiya,
Barbiellini Bernardo,
Markiewicz Robert,
Hajfathalian Maryam,
Neretina Svetlana,
Bansil Arun,
Fakhraai Zahra,
Borguet Eric
Publication year - 2019
Publication title -
chemistryselect
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.437
H-Index - 34
ISSN - 2365-6549
DOI - 10.1002/slct.201900925
Subject(s) - hydride , surface plasmon resonance , dissociation (chemistry) , plasmon , surface plasmon , chemical physics , blueshift , materials science , colloidal gold , nanoparticle , hydrogen , chemistry , photochemistry , nanotechnology , optoelectronics , photoluminescence , organic chemistry
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 ZZ‐component of the dielectric tensor undergoes a blue shift of 28 nm from a hydrogen free peak at 574 nm.