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Diffusion kinetics of proton-induced ^(21)Ne, ^3He, and ^4He in quartz

Shuster, David L. and Farley, Kenneth A. (2005) Diffusion kinetics of proton-induced ^(21)Ne, ^3He, and ^4He in quartz. Geochimica et Cosmochimica Acta, 69 (9). pp. 2349-2359. ISSN 0016-7037. http://resolver.caltech.edu/CaltechAUTHORS:20121120-135218509

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Abstract

A natural quartz sample free of mineral and fluid inclusions was irradiated with a 200 MeV proton beam to produce spallogenic ^(21)Ne, ^3He and ^4He. Temperature-dependent diffusivities of these three nuclides were then determined simultaneously by high precision stepped-heating and noble gas mass spectrometry. The outward mobility of proton-induced nuclides reflects diffusion through the quartz lattice. In the studied range of 70 to 400°C the helium diffusion coefficients exceed those of neon by 5–7 orders of magnitude. The implied diffusion parameters E_a = 153.7 ± 1.5 (kJ/mol) and ln(D_o/a^2) = 15.9 ± 0.3 (ln(s^(−1))) and E_a = 84.5 ± 1.2 (kJ/mol) and ln(D_o/a^2) = 11.1 ± 0.3 (ln(s^(−1))) for proton-induced ^(21)Ne and ^3He, respectively, indicate that cosmogenic neon will be quantitatively retained in inclusion-free quartz at typical Earth surface temperatures whereas cosmogenic helium will not. However, the neon diffusion parameters also indicate that diffusive loss needs to be considered for small (<1 mm) quartz grains that have experienced elevated temperatures. Since natural quartz often contains fluid inclusions which may enhance noble gas retentivity, these parameters likely represent an end-member case of purely solid-state diffusion. The ∼70 kJ/mol higher activation energy for neon diffusion compared to helium diffusion likely represents an energy barrier related to its ∼13% greater diameter and provides a fundamental constraint with which to test theories of solid state diffusion. The diffusion parameters for proton-induced ^4He are indistinguishable from those for ^3He, providing no evidence for the commonly expected inverse square root of the mass diffusion relationship between isotopes. We also find preliminary indication that increased exposure to radiation may enhance neon and helium retentivity in quartz at low temperatures.


Item Type:Article
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http://dx.doi.org/10.1016/j.gca.2004.11.002DOIUNSPECIFIED
http://www.sciencedirect.com/science/article/pii/S0016703704008555PublisherUNSPECIFIED
Additional Information:© 2005 Elsevier Ltd. Received June 2, 2004; accepted in revised form November 2, 2004. Associate editor: R. Wieler. We thank G. Rossman for providing the quartz sample, D. Burnett for helpful input, and J. Sisterson and E. Cascio for their expertise with the irradiation. The reviews and comments of Rainer Wieler, Tom Trull, Tibor Dunai and an anonymous referee led to improvement of the manuscript and the additional low dose experiment. This work was supported by the National Science Foundation and by a N.S.F. Graduate Research Fellowship to D.L.S.
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NSF Graduate Research FellowshipUNSPECIFIED
Record Number:CaltechAUTHORS:20121120-135218509
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20121120-135218509
Official Citation:David L. Shuster, Kenneth A. Farley, Diffusion kinetics of proton-induced 21Ne, 3He, and 4He in quartz, Geochimica et Cosmochimica Acta, Volume 69, Issue 9, 1 May 2005, Pages 2349-2359, ISSN 0016-7037, 10.1016/j.gca.2004.11.002. (http://www.sciencedirect.com/science/article/pii/S0016703704008555)
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:35577
Collection:CaltechAUTHORS
Deposited By: Ruth Sustaita
Deposited On:20 Nov 2012 22:07
Last Modified:20 Nov 2012 22:07

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