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1.
Environ Sci Technol ; 52(11): 6126-6136, 2018 06 05.
Article in English | MEDLINE | ID: mdl-29745225

ABSTRACT

Riverine dissolved sulfate (SO42-) sulfur and oxygen isotope variations reflect their controls such as SO42- reduction and reoxidation, and source mixing. However, unconstrained temporal variability of riverine SO42- isotope compositions due to short sampling durations may lead to mischaracterization of SO42- sources, particularly for the pyrite-derived sulfate load. We measured the sulfur and triple-oxygen isotopes (δ34S, δ18O, and Δ'17O) of Mississippi River SO42- with biweekly sampling between 2009 and 2013 to test isotopic variability and constrain sources. Sulfate δ34S and δ18O ranged from -6.3‰ to -0.2‰ and -3.6‰ to +8.8‰, respectively. Our sampling period captured the most severe flooding and drought in the Mississippi River basin since 1927 and 1956, respectively, and a first year of sampling that was unrepresentative of long-term average SO42-. The δ34SSO4 data indicate pyrite-derived SO42- sources are 74 ± 10% of the Mississippi River sulfate budget. Furthermore, pyrite oxidation is implicated as the dominant process supplying SO42- to the Mississippi River, whereas the Δ'17OSO4 data shows 18 ± 9% of oxygen in this sulfate is sourced from air O2.


Subject(s)
Rivers , Sulfates , Environmental Monitoring , Iron , Mississippi , Oxygen Isotopes , Sulfides , Sulfur , Sulfur Isotopes
2.
Sci Adv ; 3(11): eaao6741, 2017 11.
Article in English | MEDLINE | ID: mdl-29159288

ABSTRACT

Molecular nitrogen (N2) comprises three-quarters of Earth's atmosphere and significant portions of other planetary atmospheres. We report a 19 per mil (‰) excess of 15N15N in air relative to a random distribution of nitrogen isotopes, an enrichment that is 10 times larger than what isotopic equilibration in the atmosphere allows. Biological experiments show that the main sources and sinks of N2 yield much smaller proportions of 15N15N in N2. Electrical discharge experiments, however, establish 15N15N excesses of up to +23‰. We argue that 15N15N accumulates in the atmosphere because of gas-phase chemistry in the thermosphere (>100 km altitude) on time scales comparable to those of biological cycling. The atmospheric 15N15N excess therefore reflects a planetary-scale balance of biogeochemical and atmospheric nitrogen chemistry, one that may also exist on other planets.

3.
Sci Adv ; 3(1): e1602365, 2017 Jan.
Article in English | MEDLINE | ID: mdl-28097222

ABSTRACT

Establishing the age of the Moon is critical to understanding solar system evolution and the formation of rocky planets, including Earth. However, despite its importance, the age of the Moon has never been accurately determined. We present uranium-lead dating of Apollo 14 zircon fragments that yield highly precise, concordant ages, demonstrating that they are robust against postcrystallization isotopic disturbances. Hafnium isotopic analyses of the same fragments show extremely low initial 176Hf/177Hf ratios corrected for cosmic ray exposure that are near the solar system initial value. Our data indicate differentiation of the lunar crust by 4.51 billion years, indicating the formation of the Moon within the first ~60 million years after the birth of the solar system.

4.
Science ; 351(6272): 493-6, 2016 Jan 29.
Article in English | MEDLINE | ID: mdl-26823426

ABSTRACT

Earth and the Moon are shown here to have indistinguishable oxygen isotope ratios, with a difference in Δ'(17)O of -1 ± 5 parts per million (2 standard error). On the basis of these data and our new planet formation simulations that include a realistic model for primordial oxygen isotopic reservoirs, our results favor vigorous mixing during the giant impact and therefore a high-energy, high-angular-momentum impact. The results indicate that the late veneer impactors had an average Δ'(17)O within approximately 1 per mil of the terrestrial value, limiting possible sources for this late addition of mass to the Earth-Moon system.

5.
Science ; 338(6114): 1583-7, 2012 Dec 21.
Article in English | MEDLINE | ID: mdl-23258889

ABSTRACT

Doppler weather radar imaging enabled the rapid recovery of the Sutter's Mill meteorite after a rare 4-kiloton of TNT-equivalent asteroid impact over the foothills of the Sierra Nevada in northern California. The recovered meteorites survived a record high-speed entry of 28.6 kilometers per second from an orbit close to that of Jupiter-family comets (Tisserand's parameter = 2.8 ± 0.3). Sutter's Mill is a regolith breccia composed of CM (Mighei)-type carbonaceous chondrite and highly reduced xenolithic materials. It exhibits considerable diversity of mineralogy, petrography, and isotope and organic chemistry, resulting from a complex formation history of the parent body surface. That diversity is quickly masked by alteration once in the terrestrial environment but will need to be considered when samples returned by missions to C-class asteroids are interpreted.

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