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• W2008148206 abstract "The nanoscale intergranular films that form in the sintering of ceramics often occur as adherent glassy phases separating the crystalline grains in the ceramic. Consequently, the properties of these films are often equal in importance to those of the constituent grains in determining the ceramic's properties. The measured characteristics of the silica-rich phase separating the crystalline grains in ${mathrm{Si}}_{3}{mathrm{N}}_{4}$ and many other ceramics are so reproducible that ${mathrm{SiO}}_{2}$ has become a model system for studies of intergranular films (IGF's). Recently, the influence of fluorine and chlorine dopants in ${mathrm{SiO}}_{2}$-rich IGF's in silicon nitride was precisely documented by experiment. Along with the expected similarities between the halogens, some dramatically contrasting effects were found. But the atomic-scale mechanisms distinguishing the effects F and Cl on IGF behavior have not been well understood. First-principles density functional calculations reported here provide a quantum-level description of how these dopant-host interactions affect the properties of IGF's, with specific modeling of F and Cl in the silica-rich IGF in silicon nitride. Calculations were carried out for the energetics, structural changes, and forces on the atoms making up a model cluster fragment of an ${mathrm{SiO}}_{2}$ intergranular film segment in silicon nitride with and without dopants. Results show that both anions participate in the breaking of bonds within the IGF, directly reducing the viscosity of the ${mathrm{SiO}}_{2}$-rich film and promoting decohesion. Observed differences in the way fluorine and chlorine affect IGF behavior become understandable in terms of the relative stabilities of the halogens as they interact with Si atoms that have lost one if their oxygen bridges." @default.
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• W2008148206 date "2002-01-24" @default.
• W2008148206 modified "2023-10-17" @default.
• W2008148206 title "First-principles study of the effects of halogen dopants on the properties of intergranular films in silicon nitride ceramics" @default.
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• W2008148206 doi "https://doi.org/10.1103/physrevb.65.064113" @default.
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