Optical vibrations of hydrogen in disordered palladium-gold alloys
Abstract
Description
In the fcc lattice of Pd, hydrogen occupies octahedral interstitial positions with cubic symmetry. One could therefore expect that in dilute solid H solutions in Pd the fundamental band of optical H vibrations should be reduced to a narrow line of 3-fold degenerate, non-interacting isotropic local oscillators. A few attempts to test this assumption by inelastic neutron scattering gave ambiguous results due to the very small limiting hydrogen concentration, x<0.001, of the PdH$_x$ solutions at low temperatures. We increased maximum x by alloying Pd with 20 at% Au and studied disordered Pd$_{0.8}$Au$_{0.2}$H$_{x}$ solutions with concentrations varying from x = 0.03 to 0.74. According to reported $^{197}$Au Mossbauer studies, hydrogen atoms in the Pd$_{0.8}$Au$_{0.2}$H$_{x}$ solutions with x < (0.8)^{6} = 0.26 can only occupy interstices having no Au neighbours. This abates the effect of H-Au interactions in the solutions with lower H concentrations and effectively prevents hydrogen clustering at low temperatures. Our INS investigation showed that the fundamental optical H band in both concentrated and dilute Pd$_{0.8}$Au$_{0.2}$H$_{x}$ solutions consists of a sharp peak with a broad shoulder towards higher energies. The shoulder shows no tendency to vanish with decreasing H concentration and amounts to approximately 0.44 integral intensity of the main peak in all studied samples. The optical band in infinitely diluted H solutions in Pd should therefore consist of a peak with a pronounced shoulder too. Implications for the isotopic effects in the hydrogen solubility in Pd are considered in the present paper.
3 pages, 3 figures, to be published in compendium "Physics of Extreme States of Matter - 2009" of XXIV International Conference on Interaction of Intense Energy Fluxes with Matter (accepted)
3 pages, 3 figures, to be published in compendium "Physics of Extreme States of Matter - 2009" of XXIV International Conference on Interaction of Intense Energy Fluxes with Matter (accepted)