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Table of contents
AKNOWLEDGEMENTS
SUMMARY
RESUME EN FRANCAIS
ABSTRACT
ORGANIZATION OF THE PRESENT WORK
Chapter A: INTRODUCTION (GEOCHEMISTRY)
I/ Noble gases in geosciences
1/ Helium
2/ Neon
3/ Argon
4/ Krypton
5/ Xenon
6/ Xe and Kr as nuclear fission products
II/ Evolution of the Earth-atmosphere system and noble gases
1/ Origin of noble gases
2/ Atmospheric loss
3/ Degassing processes
4/ Recycling at depth
III/ The ‘Missing Xenon’ and the Xenon Paradox
1/ The ‘Missing Xenon’
2/ Xe paradox
3/ Hypotheses to explain the ‘Missing Xenon’ and the Xenon paradox
Chapter B: STATE OF THE ART: XE REACTIVITY AND INCORPORATION IN EARTH’S RELEVANT MATERIALS
I/ Xe physical properties
1/ Noble gases atomic radii
2/ Diffusion and adsorption properties
3/ Xe phase diagram
4/ Xe in metallic phases at high P
II/ Xe in oxides and silicates
1/ Xe in clathrates (van der Waals bonds)
2/ Xe in stoichiometric oxides
3/ Xe as a minor or trace element in silicates
4/ Xe in silicate melts
III/ Prospects
Chapter C: EXPERIMENTAL METHODS
I/ High P-T generation
1/ Piston cylinder press and gas loading devices
2/ Diamond anvil-cell (DAC)
3/ Paris Edinburgh Press (PEP)
4/ P-T calibration
II/ In situ synchrotron-based probes at high P-T conditions…
1/ Synchrotron source
2/ X-ray absorption spectroscopy (XAS)
3/ X-ray diffraction on crystalline material
4/ Infrared (IR) spectroscopy
III/ Analytical methods
1/ Scanning Electron Microscopy (SEM)
2/ Transmission Electron Microscopy (TEM)
3/ Electron microprobe analyses (EMPA)
4/ Raman spectroscopy
IV/ Theoretical modelling of Xe incorporation in minerals
1/ Density functional theory (DFT) in condensed matter
2/ Infrared and Raman spectra modeling
3/ Computational details
4/ Previous modeling of Xe within the DFT framework
Chaper D: XE INCORPORATION IN OLIVINE
I/ Ex situ analyses
1/ Sample synthesis
2/ SEM / EMP analyses
II/ New constraints on Xe incorporation in olivine from First-principles calculations (Crépisson et al., 2018)
1/ Introduction
2/ Methods
3/ Results
a/ Reference compounds and pure forsterite
b/ Xe incorporation models
c/ Cell parameters vs. Xe concentration
d/ Raman spectra
4/ Conclusion
III/ In situ IR spectroscopy on Xe -bearing olivine
1/ Methods
2/ Results and discussion
IV/ New in situ X-ray diffraction on synthetic olivine
1/ Methods and samples
2/ Results and discussion
V/ Conclusion
Chapter E: XE INCORPORATION IN QUARTZ
I/ Sample synthesis
II/ The Xe-SiO2 system at moderate P and high T (submitted to G3)
1/ Methods
a/ X-ray diffraction
b/ Infrared spectroscopy
c/ Ab initio calculations
2/ Results and discussion
a/ Increase of unit-cell volume of quartz in presence of Xe
b/ A new (Xe,Si)O2 phase at high temperature
III/ Conclusion
Chapter F: XE INCORPORATION IN HIGH-TEMPERATURE FELDSPAR (SANIDINE)
I/ Ex situ analyses
1/ Sample synthesis
2/ SEM / TEM / EMP / Raman analyses
II/ In situ X-ray diffraction
1/ Methods and samples
2/ Results for dry sanidine
3/ Results for K-cymrite and sanidine at high water fugacity
III/ Conclusion
Chapter G: XE AND KR INCORPORATIONS IN FELDSPATHIC GLASS AND MELT
I/ Sample synthesis
II/ Kr environment in a feldspathic glass and melt: a high P-T XAS study (published in Chem. Geol.)
1/ Introduction
2/ Methods
a/ Sample: synthesis and characterization
b/ Experimental set-up
c/ X-ray diffraction and XAS measurements
d/ Processing of XAS data
3/ Results and Discussion
a/ XAS data at the Kr K-edge
b/ Resolving Kr environment in sanidine glass and melt
4/ Conclusion …
III/ In situ XAS study of Xe incorporation in a feldspathic glassy and crystalline sample
1/ Methods
2/ XAS at the Xe K-edge in sanidine (glass and crystal)
3/ Conclusion
Chapter H: GENERAL CONCLUSIONS AND PERSPECTIVES
REFERENCES
