The multiple hydrogen location near an alpha-Fe vacancy

S. SIMONETTI, C. PISTONESI, A. JUAN, G. BRIZUELA

JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS

Elsevier

Lugar: Amsterdam. Netherlands; Año: 2005 p. 1240 - 1246

0022-3697

The interaction between 10 hydrogen atoms and a a-Fe structure having a vacancy (V) has been studied using a cluster model and a semi-empirical theoretical method. The energy of the system was calculated by the atom superposition and electron delocalization molecular orbital method. The electronic structure was studied using the concept of density of states and crystal orbital overlap population curves. For the study of a sequential absorption, the hydrogen atoms were positioned in their energy minima configurations, near to the tetrahedral sites neighboring the vacancy, except the last H atom that was located far from the vacancy. The energy difference for H agglomeration was also computed. The vacancy-Hn complexes become less stable than VH species for more than three hydrogen’s. The changes in the electronic structure of Fe atoms near the vacancy were also analyzed. The interactions mainly involve Fe 3d and 4s atomic orbitals. The contribution of Fe p orbitals is much less important. The Fe–Fe bond weakened as new Fe–H and H–H pairs were formed. The effect of H atoms is limited to its first Fe neighbors. The detrimental effect of H atoms on the Fe–Fe bonds can be related to the mechanism for embrittlement in a-Fe.Hn complexes become less stable than VH species for more than three hydrogen’s. The changes in the electronic structure of Fe atoms near the vacancy were also analyzed. The interactions mainly involve Fe 3d and 4s atomic orbitals. The contribution of Fe p orbitals is much less important. The Fe–Fe bond weakened as new Fe–H and H–H pairs were formed. The effect of H atoms is limited to its first Fe neighbors. The detrimental effect of H atoms on the Fe–Fe bonds can be related to the mechanism for embrittlement in a-Fe.