The isotopic composition of the new enriched silicon crystal Si28-31Pr11: maintaining the realization and dissemination of the mole and the kilogram via the XRCD method

Abstract

The molar mass and isotopic composition of a new silicon single crystal material (Si28-31Pr11) highly enriched in 28Si has been determined in the context of the x-ray crystal density method used for the realization and dissemination of the SI base units‒the mole and the kilogram. Isotope ratio measurements have been performed using a high-resolution multicollector-inductively coupled plasma mass spectrometer (MC-ICP-MS) with improved technical performance. By applying the Virtual-Element Isotope Dilution Mass Spectrometry method, different crystal areas enclosing the locations of two silicon spheres have been investigated with respect to the magnitude of tentative variations in the molar mass and isotopic composition of the respective samples as a function of their original location in the crystal ingot. In total, 18 subsamples from four different axial and several related radial positions have been characterized. An average molar mass M(Si28-31Pr11) = 27.976 941 464(41) g mol−1 corresponding to a relative combined uncertainty u c,rel(M(Si28-31Pr11)) = 1.4 × 10−9 was yielded. The average enrichment in 28Si of the crystal is expressed by the mean amount-of-substance fraction x(28Si) = 0.999 985 350(37). Two spheres were cut from the crystal ingot. The average molar masses of the spheres Si28kg_03_a and Si28kg_03_b are: M(Si28kg_03_a) = 27.976 941 467(43) g mol−1 and M(Si28kg_03_b) = 27.976 941 461(44) g mol−1, respectively. The results are discussed using uncertainty budgets according to the Guide to the expression of uncertainty in measurement. A homogeneous distribution of the molar mass throughout the crystal is suggested, qualifying it as a material for a primary standard–a silicon sphere–for the realization and dissemination of the mole and the kilogram. A comparison with enriched silicon crystals that are already available is given.