There is a need to distinguish among sources of Hg to the atmosphere in order to more fully understand global Hg pollution. In this study we investigate whether coal deposits within the United States, China, and Russia-Kazakhstan, which are three of the five greatest coal-producing regions, have diagnostic Hg isotopic fingerprints that can be used to discriminate among Hg sources. We also investigate the Hg isotopic composition of modern organic soil horizons developed in areas distant from point sources of Hg in North America. Mercury stored in coal deposits displays a wide range of both mass dependent fractionation (MDF, delta202Hg) and mass independent fractionation (MIF, delta201Hg). delta202Hg varies in coals by 3 per thousand and delta201Hg varies by 0.9 per thousand. Combining these two Hg isotope signals results in what may be a unique isotopic "fingerprint" for many coal deposits. Mass independent fractionation of mercury has been demonstrated to occur during photochemical reactions of mercury. This suggests that Hg found in most coal deposits was subjected to photochemical reduction near the Earth's surface prior to deposition. The similarity in MDF and MIF of modern organic soils and coals from North America suggests that Hg deposition from coal may have imprinted an isotopic signature on soils. This research offers a new tool for characterizing mercury inputs from natural and anthropogenic sources to the atmosphere and provides new insights into the geochemistry of mercury in coal and soils.

Three ice cores to bedrock from the Dunde ice cap on the north-central Qinghai-Tibetan Plateau of China provide a detailed record of Holocene and Wisconsin-Würm late glacial stage (LGS) climate changes in the subtropics. The records reveal that LGS conditions were apparently colder, wetter, and dustier than Holocene conditions. The LGS part of the cores is characterized by more negative delta(18)O ratios, increased dust content, decreased soluble aerosol concentrations, and reduced ice crystal sizes than the Holocene part. These changes occurred rapidly approximately 10,000 years ago. In addition, the last 60 years were apparently one of the warmest periods in the entire record, equalling levels of the Holocene maximum between 6000 and 8000 years ago.

We present version 3.0 of the atmospheric chemistry box model CAABA/MECCA. In addition to a complete update of the rate coefficients to the most recent recommendations, a number of new features have been added: chemistry in multiple aerosol size bins; automatic multiple simulations reaching steady-state conditions; Monte-Carlo simulations with randomly varied rate coefficients within their experimental uncertainties; calculations along Lagrangian trajectories; mercury chemistry; more detailed isoprene chemistry; tagging of isotopically labeled species. Further changes have been implemented to make the code more user-friendly and to facilitate the analysis of the model results. Like earlier versions, CAABA/MECCA-3.0 is a community model published under the GNU General Public License

No abstract

The relative importance of north–south migrations of the intertropical convergence zone (ITCZ) versus El Niño-Southern Oscillation and its associated Pacific Walker Circulation (PWC) variability for past hydrological change in the western tropical Pacific is unclear. Here we show that north–south ITCZ migration was not the only mechanism of tropical Pacific hydrologic variability during the last millennium, and that PWC variability profoundly influenced tropical Pacific hydrology. We present hydrological reconstructions from Cattle Pond, Dongdao Island of the South China Sea, where multi-decadal rainfall and downcore grain size variations are correlated to the Southern Oscillation Index during the instrumental era. Our downcore grain size reconstructions indicate that this site received less precipitation during relatively warm periods, AD 1000–1400 and AD 1850–2000, compared with the cool period (AD 1400–1850). Including our new reconstructions in a synthesis of tropical Pacific records results in a spatial pattern of hydrologic variability that implicates the PWC.

Abstract. Biogenic aerosols are relevant for the Earth system, climate, and public health on local, regional, and global scales. Up to now, however, little is known about the diversity and biogeography of airborne microorganisms. We present the first DNA-based analysis of airborne fungi on global scales, showing pronounced geographic patterns and boundaries. In particular we find that the ratio of species richness between Basidiomycota and Ascomycota is much higher in continental air than in marine air. This may be an important difference between the "blue ocean" and "green ocean" regimes in the formation of clouds and precipitation, for which fungal spores can act as nuclei. Our findings also suggest that air flow patterns and the global atmospheric circulation are important for the understanding of global changes in biodiversity.

No abstract

Biomass burning is known to affect air quality, global carbon cycle, and climate. However, the extent to which biomass burning gases/aerosols are present on a global scale, especially in the marine atmosphere, is poorly understood. Here we report the molecular tracer levoglucosan concentrations in marine air from the Arctic Ocean through the North and South Pacific Ocean to Antarctica during burning season. Levoglucosan was found to be present in all regions at ng/m3 levels with the highest atmospheric loadings present in the mid-latitudes (30°–60° N and S), intermediate loadings in the Arctic, and lowest loadings in the Antarctic and equatorial latitudes. As a whole, levoglucosan concentrations in the Southern Hemisphere were comparable to those in the Northern Hemisphere. Biomass burning has a significant impact on atmospheric Hg and water-soluble organic carbon (WSOC) from pole-to-pole, with more contribution to WSOC in the Northern Hemisphere than in the Southern Hemisphere.