Absolute silicon molar mass measurements, the Avogadro constant and the redefinition of the kilogram

摘要

The results of an absolute silicon molar mass determination of two independent sets of samples from the highly ~(28)Si-enriched crystal (AV028) produced by the International Avogadro Coordination are presented and compared with results published by the Physikalisch-Technische Bundesanstalt (PTB, Germany), the National Research Council (NRC, Canada) and the National Metrology Institute of Japan (NMIJ, Japan). This study developed and describes significant changes to the published protocols for producing absolute silicon isotope ratios. The measurements were made at very high resolution on a multi-collector inductively coupled plasma mass spectrometer using tetramethylammonium hydroxide (TMAH) to dissolve and dilute all samples. The various changes in the measurement protocol and the use of TMAH resulted in significant improvements to the silicon isotope ratio precision over previously reported measurements and in particular, the robustness of the ~(29)Si/~(30)Si ratio of the AVO28 material. These new results suggest that a limited isotopic variability is present in the AVO28 material. The presence of this variability is at present singular and therefore its significance is not well understood. Fortunately, its magnitude is small enough so as to have an insignificant effect on the overall uncertainty of an Avogadro constant derived from the average molar mass of all four AVO28 silicon samples measured in this study. The NIST results confirm the AVO28 molar mass values reported by PTB and NMIJ and confirm that the virtual element-isotope dilution mass spectrometry approach to calibrated absolute isotope ratio measurements developed by PTB is capable of very high precision as well as accuracy. The Avogadro constant N_A and derived Planck constant h based on these measurements, together with their associated standard uncertainties, are 6.022 140 76(19) × 10~(23) mol~(-1) and 6.626 070 17(21) × 10~(-34) J s, respectively.