ALBERT

Description: The global climate system has experienced a series of drastic changes during the Cenozoic. These include the climate transformation in Asia, from a zonal pattern to a monsoon-dominant pattern, the disappearance of subtropical aridity related to a planetary circulation system and the onset of inland deserts in central Asia. Despite of the major advances in the last two decades in characterizing and understanding these climate phenomena, disagreements persist relative to the timing, behaviors and underlying causes. This paper addresses these issues mainly based on two lines of evidence. Firstly, we newly collected the available Cenozoic geological indicators of environment in China to compile the paleoenvironmental maps of ten intervals with a more detailed examination within the Oligocene and Miocene. In confirming the earlier observation that a zonal climate pattern was transformed into a monsoonal one, the new maps within the Miocene indicate that this major change was achieved by the early Miocene, roughly consistent with the onset of loess deposition in China. Although a monsoon-like regime would have existed in the Eocene, it was restricted in the tropical-subtropical regions. The observed latitudinal oscillations of the climate zones during the Paleogene are likely attributable to the imbalanced evolution of polar ice-sheets between the two hemispheres. Secondly, we examine the relevant depositional and soil-forming processes of the Miocene loess-soil sequences to determine the circulation characteristics with special emphasis given to the early Miocene. Continuous eolian deposition in the middle reaches of the Yellow River since the early Miocene firmly indicates the formation of inland deserts, which has been constantly maintained in the past 22 Ma. Inter-section grain-size gradients indicate northerly dust-carrying winds and source location, as is regarded as the main criteria of the Asian winter monsoon system. Meanwhile, the well-developed Luvisols evidence the existence of circulations from the ocean, which brought moisture to northern China. These imply the coexistence of two kinds of circulations, one from the ocean as moisture carrier and another from the inland deserts as dust transporter. The accretionary properties of the early Miocene paleosols, resulted from interactive soil-forming and dust deposition processes, evidence two seasonally alternative circulations, i.e. a monsoonal climate regime. The much stronger development of the early Miocene soils compared to those in the Quaternary loess indicates significantly stronger summer monsoons. These lines of evidence indicate a joint change in circulations and inland aridity by the early Miocene, and suggest a dynamic linkage of them. Our recent numerical experiments reconfirm the potential roles of Tibetan uplift and Paratethys shrinkage in triggering this major climate reorganization, as revealed in peer studies, but yielded more details about their combined scenarios. These two factors would have coacted with the help of South China Sea spreading. Although the realistic effects of each factor remain to be further discriminated, probably through more paleoaltimetrical and tectonic approaches, the Miocene loess record provides a vital insight that tectonics had evolved to a threshold by the early Miocene to cause this major climate reorganization in Asia.

Description: The global climate system experienced a series of drastic changes during the Cenozoic. In Asia, these include the climate transformation from a zonal pattern to a monsoon-dominated pattern, the disappearance of typical subtropical aridity, and the onset of inland deserts. Despite major advances in the last two decades in characterizing and understanding these climate phenomena, disagreements persist relative to the timing, behaviors and underlying causes. This paper addresses these issues mainly based on two lines of evidence. First, we compiled newly collected data from geological indicators of the Cenozoic environment in China as paleoenvironmental maps of ten intervals. In confirming the earlier observation that a zonal climate pattern was transformed into a monsoonal one, the maps within the Miocene indicate that this change was achieved by the early Miocene, roughly consistent with the onset of loess deposition in China. Although a monsoon-like regime would have existed in the Eocene, it was restricted to tropical-subtropical regions. The latitudinal oscillations of the climate zones during the Paleogene are likely attributable to the imbalance in evolution of polar ice-sheets between the two hemispheres. Secondly, we examine the relevant depositional and soil forming processes of the Miocene loess-soil sequences to determine the circulation characteristics with emphasis on the early Miocene. Continuous eolian deposition in the middle reaches of the Yellow River since the early Miocene firmly indicates the formation of inland deserts, which have been constantly maintained during the past 22 Ma. Grain-size gradients between loess sections indicate northerly dust-carrying winds from northern sources, a clear indication of an Asian winter monsoon system. Meanwhile, well-developed Luvisols show evidence that moisture from the oceans reached northern China. This evidence shows the coexistence of two kinds of circulations, one from the ocean carrying moisture and another from the inland deserts transporting dust. The formation of the early Miocene paleosols resulted from interactive soil forming and dust deposition processes in these two seasonally alternating monsoonal circulations. The much stronger development of the early Miocene soils compared to those in the Quaternary loess indicates that summer monsoons were either significantly stronger, more persistent through the year, or both. These lines of evidence indicate a joint change in circulation and inland aridity by the early Miocene and suggest a dynamic linkage of them. Our recent sensitivity tests with a general circulation model, along with relevant geological data, suggest that the onset of these contrasting wet/dry responses, as well as the change from the "planetary" subtropical aridity pattern to the "inland" aridity pattern, resulted from the combined effects of Tibetan uplift and withdrawal of the Paratethys seaway in central Asia, as suggested by earlier experiments. The spreading of South China Sea also helped to enhance the south-north contrast of humidity. The Miocene loess record provides a vital insight that these tectonic factors had evolved by the early Miocene to a threshold sufficient to cause this major climate reorganization in Asia.

Description: We analyzed the seasonal variations of energy balance components over three different surfaces: irrigated cropland (Yingke, YK), alpine meadow (A'rou, AR), and spruce forest (Guantan, GT). The energy balance components were measured using eddy covariance (EC) systems and a large aperture scintillometer (LAS) in the Heihe River Basin, China, in 2008 and 2009. We also determined the source areas of the EC and LAS measurements with a footprint model for each site and discussed the differences between the sensible heat fluxes measured with EC and LAS at AR. The results show that the main EC source areas were within a radius of 250 m at all of the sites. The main source area for the LAS (with a path length of 2390 m) stretched along a path line approximately 2000 m long and 700 m wide. The surface characteristics in the source areas changed with the season at each site, and there were characteristic seasonal variations in the energy balance components at all of the sites. The sensible heat flux was the main term of the energy budget during the dormant season. During the growing season, however, the latent heat flux dominated the energy budget, and an obvious "oasis effect" was observed at YK. The sensible heat fluxes measured by LAS at AR were larger than those measured by EC at the same site. This difference seems to be caused by the so-called energy imbalance phenomenon, the heterogeneity of the underlying surfaces, and the difference between the source areas of the LAS and EC measurements.

Description: The Yellow Sea, surrounded by East China and the Korea Peninsula, is a potentially important receptor for anthropogenic mercury (Hg) emissions from East Asia. However, there is little documentation about the distribution and cycle of Hg in this marine system. During the cruise covering the Yellow Sea in July 2010, gaseous elemental mercury (GEM or Hg(0)) in the atmosphere, total Hg (THg), reactive Hg (RHg) and dissolved gaseous mercury (DGM, largely Hg(0)) in the waters were measured aboard the R/V Kexue III. The mean (±SD) concentration of GEM over the entire cruise was 2.61 ± 0.50 ng m−3 (range: 1.68 to 4.34 ng m−3), which were generally higher than other open oceans. The spatial distribution of GEM generally reflected a clear gradient with high levels near the coast of East China and low levels in open waters, suggesting the significant atmospheric Hg outflow from East China. The mean concentration of THg in the surface waters was 1.69 ± 0.35 ng l−1 and the RHg accounted for a considerable fraction of THg (RHg: 1.08 ± 0.28 ng l−1, %RHg/THg = 63.9%). The mean concentration of DGM in the surface waters was 63.9 ± 13.7 pg l−1 and always suggested the supersaturation of Hg(0) in the surface waters with respect to Hg(0) in the atmosphere (the degree of saturation: 7.8 ± 2.3 with a range of 3.6–14.0). The mean Hg(0) flux at the air-sea interface was estimated to be 18.3 ± 11.8 ng m−2 h−1 based on a two-layer exchange model. The high wind speed and DGM levels induced the extremely high Hg(0) emission rates. Measurements at three stations showed no clear vertical patterns of DGM, RHg and THg in the water column. Overall, the elevated Hg levels in the Yellow Sea compared with other open oceans suggested that the human activity has influenced the oceanic Hg cycle downwind of East Asia.

Description: Understanding the particle number size distributions in diversified atmospheric environments is important in order to design mitigation strategies related to submicron particles and their effects on regional air quality, haze and human health. In this study, we conducted 15 different field measurement campaigns between 2007 and 2011 at 13 individual sites in China, including five urban sites, four regional sites, three coastal/background sites and one ship cruise measurement along eastern coastline of China. Size resolved particles were measured in the 15–600 nm size range. The median particle number concentrations (PNCs) were found to vary in the range of 1.1−2.2 × 104 cm−3 at urban sites, 0.8−1.5 × 104 cm−3 at regional sites, 0.4−0.6 × 104 cm−3 at coastal/background sites, and 0.5 × 104 cm−3 during cruise measurement. Peak diameters at each of these sites varied greatly from 24 to 115 nm. Particles in the 15–25 nm (nucleation mode), 25–100 nm (Aitken mode) and 100–600 nm (accumulation mode) range showed different characteristics at each sites, indicating the features of primary emissions and secondary formation in these diversified atmospheric environments. Diurnal variations show a build-up of accumulation mode particles belt at regional sites, suggesting the contribution of regional secondary aerosol pollution. Frequencies of new particle formation (NPF) events were much higher at urban and regional sites than at coastal sites and during cruise measurement. The average growth rates (GRs) of nucleation mode particles were 8.0–10.9 nm h−1 at urban sites, 7.4–13.6 nm h−1 at regional sites and 2.8–7.5 nm h−1 at coastal sites and during cruise measurement. The high gaseous precursors and strong oxidation at urban and regional sites not only favored the formation of particles, but also accelerated the growth rate of the nucleation mode particles. No significant difference in condensation sink (CS) during NPF days were observed among different site types, suggesting that the NPF events in background areas were more influenced by the pollutant transport. In addition, average contributions of NPF events to potential cloud condensation nuclei (CCN) at 0.2% super-saturation in the afternoon of all sampling days were calculated as 11% and 6% at urban sites and regional sites, respectively. On the other hand, NPF events at coastal sites and during cruise measurement had little impact on potential production of CCN. This study provides a large data set of particle size distribution in diversified atmosphere of China, improving our general understanding of emission, secondary formation, new particle formation and corresponding CCN activity of submicron aerosols in Chinese environments.

Description: Heterogeneous processes on dust particles are important for understanding the chemistry and radiative balance of the atmosphere. This paper investigates an intense Asian dust storm episode observed at Mount Heng (1269 m a.s.l.) in southern China on 24–26 April 2009. A set of aerosol and trace gas data collected during the study was analyzed to investigate their chemical evolution and heterogeneous photochemistry as the dust traveled to southern China. Results show that the mineral dust arriving at Mt. Heng experienced significant modifications during transport, with large enrichments in secondary species (sulfate, nitrate, and ammonium) compared with the dust composition collected at an upwind mountain top site (Mount Hua). A photochemical age "clock" (−Log10(NOx/NOy)) was employed to quantify the atmospheric processing time. The result indicates an obvious increase in the abundance of secondary water-soluble ions in dust particles with the air mass atmospheric processing time. Based on the observations, a 4-stage evolution process is proposed for carbonate-containing Asian dust, starting from fresh dust to particles coated with hydrophilic and acidic materials. Daytime-enhanced nitrite formation on the dust particles was also observed, which indicates the recent laboratory result of the TiO2 photocatalysis of NO2 as a potential source of nitrite and nitrous acid.

Description: Visibility degradation is a pervasive and urgent environmental problem in China. The occurrence of low visibility events is frequent in the North China Plain, where the aerosol loading is quite high and aerosols are strongly hygroscopic. A parameterization of light extinction (Kex) for low visibilities on hazy days is proposed in this paper, based on visibility, relative humidity (RH), aerosol hygroscopic growth factors and particle number size distributions measured during the Haze in China (HaChi) Project. Observational results show that a high aerosol volume concentration is responsible for low visibility at RH 〈90%; while for RH 〉90%, decrease of visibility is mainly influenced by the increase of RH. The parameterization of Kex is developed on the basis of aerosol volume concentrations and RH, taking into accounts the sensitivity of visibility to the two factors and the availability of corresponding data. The extinction coefficients calculated with the parameterization schemes agree well with the directly measured values.

Description: A three-dimensional variational data assimilation (3-DVAR) algorithm for aerosols in a WRF/Chem model is presented. The WRF/Chem model uses the MOSAIC (Model for Simulating Aerosol Interactions and Chemistry) scheme, which explicitly treats eight major species (elemental/black carbon, organic carbon, nitrate, sulfate, chloride, ammonium, sodium and the sum of other inorganic, inert mineral and metal species) and represents size distributions using a sectional method with four size bins. The 3-DVAR scheme is formulated to take advantage of the MOSAIC scheme in providing comprehensive analyses of species concentrations and size distributions. To treat the large number of state variables associated with the MOSAIC scheme, this 3-DVAR algorithm first determines the analysis increments of the total mass concentrations of the eight species, defined as the sum of the mass concentrations across all size bins, and then distributes the analysis increments over four size bins according to the background error variances. The number concentrations for each size bin are adjusted based on the ratios between the mass and number concentrations of the background state. Additional flexibility is incorporated to further lump the eight mass concentrations, and five lumped species are used in the application presented. The system is evaluated using the analysis and prediction of PM2.5 in the Los Angeles basin during the CalNex 2010 field experiment, with assimilation of surface PM2.5 and speciated concentration observations. The results demonstrate that the data assimilation significantly reduces the errors in comparison with a simulation without data assimilation and improved forecasts of the concentrations of PM2.5 as well as individual species for up to 24 h. Some implementation difficulties and limitations of the system are discussed.

Description: Size-resolved and bulk activation properties of aerosols were measured at a regional/suburban site in the North China Plain (NCP), which is occasionally heavily polluted by anthropogenic aerosol particles and gases. A Cloud Condensation Nuclei (CCN) closure study is conducted with bulk CCN number concentration (NCCN) and calculated CCN number concentration based on the aerosol number size distribution and size-resolved activation properties. The observed CCN number concentration (NCCN-obs) are higher than those observed in other locations than China, with average NCCN-obs of roughly 2000, 3000, 6000, 10 000 and 13 000 cm−3 at supersaturations of 0.056, 0.083, 0.17, 0.35 and 0.70%, respectively. An inferred critical dry diameter (Dm) is calculated based on the NCCN-obs and aerosol number size distribution assuming homogeneous chemical composition. The inferred cut-off diameters are in the ranges of 190–280, 160–260, 95–180, 65–120 and 50–100 nm at supersaturations of 0.056, 0.083, 0.17, 0.35 and 0.7%, with their mean values 230.1, 198.4, 128.4, 86.4 and 69.2 nm, respectively. Size-resolved activation measurements show that most of the 300 nm particles are activated at the investigated supersaturations, while almost no particles of 30 nm are activated even at the highest supersaturation of 0.72%. The activation ratio increases with increasing supersaturation and particle size. The slopes of the activation curves for ambient aerosols are not as steep as those observed in calibrations with ammonium sulfate suggesting that the observed aerosols is an external mixture of more hygroscopic and hydrophobic particles. The calculated CCN number concentrations (NCCN-calc) based on the size-resolved activation ratio and aerosol number size distribution correlate well with the NCCN-obs, and show an average overestimation of 19%. Sensitivity studies of the CCN closure show that the NCCN at each supersaturation is well predicted with the campaign average of size-resolved activation curves. These results indicate that the aerosol number size distribution is critical in the prediction of possible CCN. The CCN number concentration can be reliably estimated using time-averaged, size-resolved activation efficiencies without accounting for the temporal variations.

Description: The Yellow Sea, surrounded by East China and the Korea Peninsula, is a potentially important receptor for anthropogenic mercury (Hg) emissions from East Asia. However, there is little documentation about the distribution and cycle of Hg in this marine system. During the cruise covering the Yellow Sea in July 2010, gaseous elemental mercury (GEM or Hg(0)) in the atmosphere, total Hg (THg), reactive Hg (RHg) and dissolved gaseous mercury (DGM, largely Hg(0)) in the waters were measured aboard the R/V Kexue III. The mean (±SD) concentration of GEM over the entire cruise was 2.61±0.50 ng m−3 (range: 1.68 to 4.34 ng m−3), which were generally higher than other open oceans. The spatial distribution of GEM generally reflected a clear gradient with high levels near the coast of East China and low levels in open waters, suggesting the significant atmospheric Hg outflow from East China. The mean concentration of THg in the surface waters was 1.69±0.35 ng l−1 and the RHg accounted for a considerable fraction of THg (RHg: 1.08±0.28 ng l−1, %RHg/THg=63.9%). The mean concentration of DGM in the surface waters was 63.9±13.7 pg l−1 and always suggested the supersaturation of Hg(0) in the surface waters with respect to Hg(0) in the atmosphere (the degree of saturation: 7.83±2.29 with a range of 3.58–14.00). The mean Hg(0) flux at the air-sea interface was estimated to be 22.58±14.56 ng m−2 h−1 based on a two-layer exchange model. The high wind speed and DGM levels induced the extremely high Hg(0) emission rates. Measurements at three selected stations showed no clear vertical patterns of all three species of Hg in the water column. Overall, the elevated Hg levels in the Yellow Sea compared with other open oceans suggested that the human activity has significantly influenced the oceanic Hg cycle downwind of East Asia.