title: Multi-elemental Gd, Eu, Sm, Nd isotope ratio measurements by liquid chromatography coupled to MC-ICPMS with variable Faraday cup configurations during elution.
abstract: The high-precision isotopic characterization of actinides and fission products in nuclear samples is fundamental for various applications such as the management of spent nuclear fuel or the validation of neutronic calculation codes. However multi-elemental isotope ratio measurements by mass spectrometric techniques are hampered by the presence of both spectral and non-spectral interferences as complex sample matrices are encountered in such topics, but also due to the lack of high precision mass spectrometers able to cover the entire mass spectrum. This work describes a new LC-MC-ICPMS approach allowing simultaneous high-precision and multi-elemental isotope ratio measurements of four fission products of interest for nuclear issues (Nd, Sm, Eu, Gd) within a single elution run. Variable motorized Faraday cup configurations were successively used during a specifically designed elution procedure in order to take into account the non-natural Nd, Sm, Eu, Gd isotopic compositions encountered in irradiated nuclear samples. This new method, involving the relevant isotopic reference standard injection timings for on-line mass bias corrections, was validated by the analysis of a simulated fission product fraction from a235U-irradiated target. Reproducibilities better than 2‰ (k=2), comparable to those obtained by off-line measurements and the classic sample-standard bracketing mass bias correction approach, were obtained for all isotope ratios, except those involving isotopes with a transient signal peak apex lower than 100mV, for which the reproducibilities were comprised between 2‰ and 6‰.
authors.affiliation: DEN - Service d'Etudes Analytiques et de Réactivité des Surfaces (SEARS), CEA, Université Paris-Saclay, F-91191 Gif sur Yvette, France.
authors.forename: Florence
authors.initials: F
authors.lastname: Guéguen
authors.affiliation: DEN - Service d'Etudes Analytiques et de Réactivité des Surfaces (SEARS), CEA, Université Paris-Saclay, F-91191 Gif sur Yvette, France.
authors.forename: Anthony
authors.initials: A
authors.lastname: Nonell
authors.affiliation: DEN - Service d'Etudes Analytiques et de Réactivité des Surfaces (SEARS), CEA, Université Paris-Saclay, F-91191 Gif sur Yvette, France. Electronic address: helene.isnard@cea.fr.
authors.forename: Hélène
authors.initials: H
authors.lastname: Isnard
authors.affiliation: DEN - Service d'Etudes Analytiques et de Réactivité des Surfaces (SEARS), CEA, Université Paris-Saclay, F-91191 Gif sur Yvette, France.
authors.forename: Laurent
authors.initials: L
authors.lastname: Vio
authors.affiliation: DEN - Département de Physico-chimie (DPC), CEA, Université Paris-Saclay, F-91191 Gif sur Yvette, France.
authors.forename: Frédéric
authors.initials: F
authors.lastname: Chartier
keywords: Isotope ratios; LC-MC-ICPMS; Lanthanides; MC-ICPMS; Transient signal