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High Pressure Synthesis at the Origin of New Developments in Silicon Clathrate Physical-Chemistry

High Pressure Synthesis at the Origin of New Developments in...

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18th International Conference on High Pressure Science and Technology

作者： E.Reny S.Yamanaka C.Cros m.pouchard Department of Applied Chemistry Faculty of EngineeringHiroshima UniversityHigashi Hiroshima 739-8527Japan Japan Society for the Promotion of Science (JSPS Japan Department of Applied Chemistry Faculty of EngineeringHiroshima UniversityHigashi Hiroshima 739-8527 CRESTJapan Science and Technology Corporation (JSTJapan Institut de Chimie de la matiere Condensee de Bordeaux 33608 Pessac cedexFrance Institut de Chimie de la matiere Condensee de Bordeaux 33608 Pessac cedexFrance

＜正＞The network of type I silicon clathrate structures is an arrangement of fullerene-like Si20（Ih） and Si24（D6d） polyhedra connected via their pentagonal and hexagonal faces. These compounds crystallise in a cubic cell （Pm3n） where the two Si20 dodecahedra occupy the summits and the centre of the cube while six Si24 tetradekaidecahedra are situated on the faces. In the centre of these cages can be found guest atoms which are usually alkali or alkaline-earth elements （m）.（1,2）The corresponding ideal formula is therefore m8Si46. A representation of the ideal structure can be seen in figure 1. Up to recently, silicon clathrates could only be synthesised by two means: melting of stoichiometric mixture of the elements or thermal degradation of alkali or alkaline earth silicides under vacuum or argon flow. However, some compositions couldn’t be obtained in either ways. Recently, we attempted with great success the synthesis of clathrates using a High Pressure High Temperature （HPHT） technique. For example, two years ago, was successfully obtained for the first time, Ba8Si46 exhibiting superconducting properties with a Tc = 8K, highest ever obtained for sp3 silicon networks.（3） The increasing interest of the scientific community for clathrates, resulting mainly from the observed or speculated physical properties of such materials （superconductivity（3）, peculiar mechanical properties（4）, possible thermoelectric applications due to the guest atom rattling（5） etc.）, led us to explore the high pressure high temperature synthesis routein order to attempt the synthesis of other new silicon clathrates. We report in this presentation synthesis by HPHT of the first silicon clathrate compound doped with an electronegative element（6） Actually during the synthesis, the clathrate phase formation is in concurrence with other compounds as silicon iodides of type Silx. However it is possible to ’help’ the reaction by the addition of a crystalline seed to the starting

关键词： High Pressure High Temperature Synthesis Silicon Clathrate Iodine.

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