Title: Krypton storage capacity of the Earth's lower mantle

Abstract

Noble gases are important geochemical tracers allowing reconstructing global volatile cycles in Earth's reservoirs. To constrain these fundamental processes, precise data on their partitioning behavior at deep Earth conditions are needed. Such data are only available at moderate pressures up to 25 GPa due to experimental challenges. We have investigated the possibility of noble gas storage in the Earth's lower mantle up to 115 GPa. We studied the incorporation of krypton in the second most abundant lower mantle mineral (Mg_1-x,Fe_x)O (ferropericlase) as well as in liquid metal-alloys by performing experiments up to 115 GPa and 3700 K using the laser-heated diamond anvil cell coupled to post-mortem EMPA analysis and X-ray absorption spectroscopy. The results reveal that, at these extreme conditions, up to 3 wt.% of krypton can be stored in (Mg_1-x,Fe_x)O and 3000 ppm in the Fe-rich liquid metal. For both phases the storage capacities increase with pressure (between 40 GPa and 60 GPa) at a constant high temperature of 2300 K. Fpc has never been considered as a NG host, despite being the second most abundant mineral in the Earth's LM. Using recent accurate compressibility data, we demonstrate that a substitution of krypton into the anion site of (Mg_1-x,Fe_x)Omore » in form of neutral oxygen Schottky defects at diluted lower mantle conditions is possible. This noble gas incorporation mechanism is in agreement with a previous study on bridgmanite. We show that (Mg_1-x,Fe_x)O exhibits higher noble gas storage capacities than bridgmanite through the lower mantle using lattice strain modeling and including experimental solubility and thermoelastic data for neon, argon, krypton and xenon. We also demonstrate that both phases exhibit the highest solubilities for argon and krypton. We used the solubility data from lattice strain modeling to predict noble gas abundances stored in the solid lower mantle after magma ocean crystallization. The modeled abundances show apparent similarities with estimates for the deep noble gas reservoir that are based on either 3He abundances in ocean island basalts or radiogenic 40Ar abundances in the bulk Earth. This strongly indicates that the crystalline lower mantle may play an important role as deep noble gas storage reservoir. We propose, based on considerations on noble gas replenishment from the lower mantle to the atmosphere, that the lower mantle can only contribute to a small fraction of the present-day atmospheric noble gases. This suggests that the lower mantle is an un-degassed reservoir.« less

Authors:

Rosa, A. ^[1]; Bouhifd, M. A. ^[2]; Morard, G. ^[3]; Briggs, R. ^[4]; Garbarino, G. ^[1]; Irifune, T. ^[5]; Mathon, O. ^[1]; Pascarelli, S. ^[1]

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+ Show Author Affiliations

1. European Synchrotron Radiation Facility (ESRF), Grenoble (France)
2. Clermont Auvergne Univ., Clermont-Ferrand (France)
3. Sorbonne Univ., Paris (France)
4. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
5. Ehime Univ., Matsuyama (Japan)

Publication Date:

2019-12-19

Research Org.:

Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Org.:

USDOE National Nuclear Security Administration (NNSA)

OSTI Identifier:

1597224

Alternate Identifier(s):

OSTI ID: 1775735

Report Number(s):

LLNL-JRNL-799861
Journal ID: ISSN 0012-821X; 1002037

Grant/Contract Number:  

AC52-07NA27344

Resource Type:

Accepted Manuscript

Journal Name:

Earth and Planetary Science Letters

Additional Journal Information:

Journal Volume: 532; Journal Issue: C; Journal ID: ISSN 0012-821X

Publisher:

Elsevier

Country of Publication:

United States

Language:

English

Subject:

58 GEOSCIENCES; Physics; Geosciences; deep noble gas reservoir; lower mantle minerals; iron melts; krypton; partitioning; laser-heated diamond anvil cell