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Large Sulfur-Isotope Anomaly in Nonvolcanic Sulfate Aerosol and Its Implications for the Archean Atmosphere

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Large Sulfur-Isotope Anomaly in Nonvolcanic Sulfate Aerosol and Its Implications for the Archean Atmosphere Large sulfur-isotope anomaly in nonvolcanic sulfate aerosol and its implications for the Archean atmosphere Robina Shaheena, Mariana M. Abaunzaa, Teresa L. Jacksona, Justin McCabea,b, Joël Savarinoc,d, and Mark H. Thiemensa,1 aDepartment of Chemistry and Biochemistry, University of California, San Diego, La Jolla, CA 92093; bPacific Ridge School, Carlsbad, CA 92009; cLaboratoire de Glaciologie et de Géophysique de l’Environnement, Centre National de la Recherche Scientifique, Unité Mixte de Recherche 5183, F-38041 Grenoble, France; and dLaboratoire de Glaciologie et de Géophysique de l’Environnement, Université Grenoble Alpes, Unité Mixte de Recherche 5183, F-38041 Grenoble, France † Edited by Barbara J. Finlayson-Pitts, University of California, Irvine, CA, and approved July 18, 2014 (received for review April 8, 2014) Sulfur-isotopic anomalies have been used to trace the evolution of (1980–2002) have recently revealed how ENSO-driven changes oxygen in the Precambrian atmosphere and to document past affect the global transport and transformation of sulfate aero- volcanic eruptions. High-precision sulfur quadruple isotope sols from the troposphere to the stratosphere and across hemi- measurements of sulfate aerosols extracted from a snow pit at spheres (10). the South Pole (1984–2001) showed the highest S-isotopic anoma- lies (Δ33S =+1.66‰ and Δ36S =+2‰) in a nonvolcanic (1998–1999) Results and Discussion period, similar in magnitude to Pinatubo and Agung, the largest 2- The highest SO4 concentration in snow [154 parts per billion volcanic eruptions of the 20th century. The highest isotopic anom- (ppb)] is observed after volcanic activity (Pinatubo, June 1991; aly may be produced from a combination of different stratospheric Cerro Hudson, August 1991). The addition of volcanic sulfate to the sources (sulfur dioxide and carbonyl sulfide) via SOx photochemis- try, including photoexcitation and photodissociation. The source of stratospheric baseline sulfate aerosol (or background sulfate aerosol SI Appendix anomaly is linked to super El Niño Southern Oscillation (ENSO) (1997– as defined in , Section 2) produced a significant de- 1998)-induced changes in troposphere–stratosphere chemistry and crease in heavy sulfur isotopes. The baseline sulfate aerosol value of 34 dynamics. The data possess recurring negative S-isotope anoma- δ SBG= 12‰ dropped to ∼3‰ (Fig. 1A) following the Pinatubo lies (Δ36S = −0.6 ± 0.2‰) in nonvolcanic and non-ENSO years, thus eruption, and δ33S, δ36S tracked this isotopic trend. The contribu- requiring a second source that may be tropospheric. The genera- tion of sea salt sulfate at the South Pole is <9%, indicating long- tion of nonvolcanic S-isotopic anomalies in an oxidizing atmo- range transported aerosol to be the main sulfate component (10). A sphere has implications for interpreting Archean sulfur deposits broad range in δ33S(1.61–11.32‰), δ34S(2–20‰), and δ36S(2.8– used to determine the redox state of the paleoatmosphere. 37‰)valuesforthesamplingtimeperiodindicatestheorigin of sulfate aerosols from various sulfur sources and chemical and UV photolysis | sulfur isotopes dynamical processes. A significant positive correlation of δ34S ulfur is a ubiquitous element on Earth. Its multiple valence − + Significance Sstates (S 2 to S 6) permit it to participate in a range of photochemical, geochemical, and biochemical processes, and its four stable isotope (32S, 33S, 34S, and 36S) allow tracing of chemical The highest S-isotope anomaly is observed in a nonvolcanic reactions at a molecular level. Multiple sulfur isotopes (δ33S, δ34S, period, and the magnitude of anomaly is similar to the largest ‡ and δ36S) and concomitant anomalies (Δ33S and Δ36S) in paleo- volcanic eruptions of the 20th century. S-quadruple isotope sediments [>2.5 giga-annum (Ga)] have been used to trace the data provided the first evidence of how super El Niño Southern Oscillation (ENSO) events (1997–1998) have affected the trans- EARTH, ATMOSPHERIC, origin and evolution of life and rise of oxygen in the Earth’s AND PLANETARY SCIENCES paleoclimatic history (1–3). In the present atmosphere, the port and transformation of aerosols to the stratosphere; thus, concentration of sulfate in ice cores and associated S-isotope record of paleo-ENSO events of this magnitude can be traced anomalies has served as a forensic tool to help understand the with the S-isotopic anomaly. High-resolution and high-precision dynamics of volcanic emissions, such as transport and trans- S-isotopic fingerprinting also revealed that the tropospheric formation of sulfur to the stratosphere and its impact on ozone sulfate produced during fossil-fuel and biomass burning con- 2- tributes to the stratospheric sulfate aerosol layer, a contribution chemistry (4–7). The low concentration of sulfate (SO4 )inice cores during volcanically quiescent periods and associated ana- previously unrecognized. The distribution of sulfur anomalies lytical challenges to analyze all four S-stable isotopes at high mimics the Archean isotope record, which is used to track the precision have restricted studies of the temporal distribution of origin and evolution of oxygen on earth. sulfur mass-independent signatures. Here, we present a high- – Author contributions: R.S., J.M., J.S., and M.H.T. designed research; R.S., M.M.A., and T.L.J. resolution seasonal record (1984 2001) of quadruple S-stable performed research; R.S., J.M., and M.H.T. contributed new reagents/analytic tools; R.S., isotopes and concomitant isotope anomalies of sulfate aerosols J.S., and M.H.T. analyzed data; and R.S. wrote the paper. extracted from a snow pit (1 × 1 m) at the South Pole (89.5° S, The authors declare no conflict of interest. † 17.3° W; 2,850 m) (8) to gain further insight into sources, pho- This Direct Submission article had a prearranged editor. tochemistry, and associated sulfur transformations of strato- 1To whom correspondence should be addressed. Email: [email protected]. spheric sulfate aerosols (SSAs). The time period encompasses This article contains supporting information online at www.pnas.org/lookup/suppl/doi:10. two major volcanic eruptions and three large El Niño Southern 1073/pnas.1406315111/-/DCSupplemental. ‡ Oscillation (ENSO) events. A recent study has attributed a global MIF. Here, delta denotes the ratio of the least abundant to the most abundant isotope warming hiatus (9) to a super ENSO event (1997–1998); therefore, {e.g., δ33S = [(33S)/(32S)sample/(33S)/(32S)std − 1) × 1,000]} relative to the same ratio in data from this period are timely for understanding changes in standard, which is Canyon Diablo Troilite (CDT) and expressed in parts per thousand (‰). Most natural processes fractionate S isotopes in proportion to mass differences and are stratospheric sulfate aerosol chemistry that play an important role in 33 34 36 34 described by δ S ≈ 0.515*δ S, and δ S ≈ 1.91*δ S, except UV photolysis of SO2. The mitigating global warming trends via scattering of incoming solar deviation from mass-dependent fractionation (MDF) is called anomalous or mass-inde- radiation. Oxygen triple isotope measurements of sulfate aerosols pendent fractionation (MIF) and quantified by Δ33S and Δ36S. www.pnas.org/cgi/doi/10.1073/pnas.1406315111 PNAS | August 19, 2014 | vol. 111 | no. 33 | 11979–11983 Downloaded by guest on September 27, 2021 wavelength is available in the present-day atmosphere, as will be discussed. The S-isotopic anomalies observed in volcanic sulfate aerosols are accompanied by a significant increase in sulfate concentration (4, 5, 11). The Pinatubo and Cerro Hudson eruptions in 1991 produced a factor of 3.7 sulfate concentration increase in the snow record. The observed unprecedented S-isotope anomaly is not accompanied by a massive Pinatubo-size increase in sulfate concentration, thus requiring new, or highly perturbed, chemical, photochemical, and dynamical processes. Our high-resolution, seasonally resolved sulfate aerosol data reveal 36 the presence of a negative S-isotope anomaly (Δ S(avg) ∼−0.6‰) during nonvolcanic and non-ENSO baseline periods (SI Appendix), suggesting the presence of a second isotopically anomalous sulfate source. The S-isotopic anomaly during these time periods is within the range reported for tropospheric sulfate aerosols (15) of Δ36S= −0.3‰ to −2‰ (Fig. 2B). In the present atmo- sphere, short UV is blocked by the O3 layer; thus, the negative anomaly in tropospheric sulfate aerosol cannot be attributed to short-wavelength SOx photolysis. Romero and Thiemens (15) suggested possible transport of stratospheric S-isotope anomaly to the troposphere at low and mid latitudes. Considering the tropospheric S burden (16) (SO2 from fossil-fuel combustion ∼ − − 78 Tg S·yr 1, biomass burning ∼ 2TgS·yr 1, and natural sources − ∼ 25 Tg S·yr 1), it is unlikely that even a 10% transport of SSA − (0.01 Tg S·yr 1) can produce such a significant isotopic change in tropospheric sulfate aerosols. Alternatively, a 0.01% transport of anomalous sulfate from the troposphere to stratosphere can cause a significant change (Δ36S = −0.9‰) in the isotopic com- position of SSA (SI Appendix), provided tropospheric sulfur is anomalous. Laboratory studies demonstrate that a negative S-iso- tope anomaly can be produced by nonphotochemical processes, such as primary sulfate produced during fossil-fuel combustion (Δ36S = −0.8‰ to −1.7‰) and biomass burning (Δ36S = −0.1‰ 33 34 36 to −2‰)(SI Appendix,TableS3) (17). The mechanism that gen- Fig. 1. (A) The concentration profile (1983–2000) of SO4 and δ S, δ S, δ S sulfate aerosol extracted from snow-pit samples at the South Pole. Note erates the negative anomaly in such processes is unknown (radical anticorrelation between SO4 concentration and S-stable isotopes of SO4 aerosol driven or recombination reactions may be operative, for example), after Pinatubo and Cerro Hudson eruptions. (B) Sulfur-isotope anomaly (Δ33S but, clearly, high-temperature sulfur oxidation processes are a via- and Δ36S) of sulfate aerosols extracted from the snow-pit samples at the South ble source for the tropospheric negative anomaly.
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