TY - JOUR
T1 - Helium diffusion in natural zircon
T2 - radiation damage, anisotropy, and the interpretation of zircon (U-TH)/He thermochronology
AU - Guenthner, William R.
AU - Reiners, Peter W.
AU - Ketcham, Richard A.
AU - Nasdala, Lutz
AU - Giester, Gerald
PY - 2013/3
Y1 - 2013/3
N2 - Accurate thermochronologic interpretation of zircon (U-Th)/He dates requires a realistic and practically useful understanding of He diffusion kinetics in natural zircon, ideally across the range of variation that characterize typically dated specimens. Here we present a series of date and diffusion measurements that document the importance of alpha dose, which we interpret to be correlated with accumulated radiation damage, on He diffusivity. This effect is manifest in both date-effective uranium (eU) correlations among zircon grains from single hand samples and in diffusion experiments on pairs of crystallographically oriented slabs of zircon with alpha doses ranging from ∼1016 to 1019 α/g. We interpret these results as due to two contrasting effects of radiation damage in zircon, both of which have much larger effects on He diffusivity and thermal sensitivity of the zircon (U-Th)/He system than crystallographic anisotropy. Between 1.2×1016 α/g and 1.4×1018α/g, the frequency factor, D0, measured in the c-axis parallel direction decreases by roughly four orders of magnitude, causing He diffusivity to decrease dramatically (for example by three orders of magnitude at temperatures between 140 and 220 °C). Above ∼2×1018α/g, however, activation energy decreases by a factor of roughly two, and diffusivity increases by about nine orders of magnitude by 8.2×1018α/g. We interpret these two trends with a model that describes the increasing tortuosity of diffusion pathways with progressive damage accumulation, which in turn causes decreases in He diffusivity at low damage. At high damage, increasing diffusivity results from damage zone interconnection and consequential shrinking of the effective diffusion domain size. Our model predicts that the bulk zircon (U-Th)/He closure temperature (Tc) increases from about 140 to 220 °C between alpha doses of 1016 to 1018 /g, followed by a dramatic decrease in Tc above this dose. Linking this parameterization to one describing damage annealing as a function of time and temperature, we can model the coevolution of damage, He diffusivity, and (U-Th)/He date of zircon. This model generates positive or negative date-eU correlations depending on the extent of damage in each grain and the date-eU sample's time-temperature history.
AB - Accurate thermochronologic interpretation of zircon (U-Th)/He dates requires a realistic and practically useful understanding of He diffusion kinetics in natural zircon, ideally across the range of variation that characterize typically dated specimens. Here we present a series of date and diffusion measurements that document the importance of alpha dose, which we interpret to be correlated with accumulated radiation damage, on He diffusivity. This effect is manifest in both date-effective uranium (eU) correlations among zircon grains from single hand samples and in diffusion experiments on pairs of crystallographically oriented slabs of zircon with alpha doses ranging from ∼1016 to 1019 α/g. We interpret these results as due to two contrasting effects of radiation damage in zircon, both of which have much larger effects on He diffusivity and thermal sensitivity of the zircon (U-Th)/He system than crystallographic anisotropy. Between 1.2×1016 α/g and 1.4×1018α/g, the frequency factor, D0, measured in the c-axis parallel direction decreases by roughly four orders of magnitude, causing He diffusivity to decrease dramatically (for example by three orders of magnitude at temperatures between 140 and 220 °C). Above ∼2×1018α/g, however, activation energy decreases by a factor of roughly two, and diffusivity increases by about nine orders of magnitude by 8.2×1018α/g. We interpret these two trends with a model that describes the increasing tortuosity of diffusion pathways with progressive damage accumulation, which in turn causes decreases in He diffusivity at low damage. At high damage, increasing diffusivity results from damage zone interconnection and consequential shrinking of the effective diffusion domain size. Our model predicts that the bulk zircon (U-Th)/He closure temperature (Tc) increases from about 140 to 220 °C between alpha doses of 1016 to 1018 /g, followed by a dramatic decrease in Tc above this dose. Linking this parameterization to one describing damage annealing as a function of time and temperature, we can model the coevolution of damage, He diffusivity, and (U-Th)/He date of zircon. This model generates positive or negative date-eU correlations depending on the extent of damage in each grain and the date-eU sample's time-temperature history.
KW - He diffusion
KW - Radiation damage
KW - Thermochronology
KW - Zircon
UR - http://www.scopus.com/inward/record.url?scp=84881315206&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=84881315206&partnerID=8YFLogxK
U2 - 10.2475/03.2013.01
DO - 10.2475/03.2013.01
M3 - Article
AN - SCOPUS:84881315206
SN - 0002-9599
VL - 313
SP - 145
EP - 198
JO - American Journal of Science
JF - American Journal of Science
IS - 3
ER -