Structure of chemical elements deposited with atmospheric precipitation in the north of the European territory of Russia derived with multivariate analysis methods

Data on deposition density of Ag, Al, As, B, Ba, Bi, Br, Ca, Cd, Co, Cr, Cs, Cu, Fe, K, Li, Mg, Mn, Mo, Na, Ni, P, Pb, Rb, S, Sb, Si, Sn, Sr, Th, Tl, U, V, Zn, Cl^?, NO ₃ ^? , and SO4 ₄ ^2? in atmospheric precipitation were derived at 11 observation stations in the northern part of the European territory of Russia (ETR). Three sets (factors) of chemical indices that are mutually independent and determine the precipitation chemical content over that territory were revealed by using the hierarchical factor analysis of deposited density of chemical ingredients studied. These are two first-order factors: one is presented with the elements of a “marine” origin; the second is associated with biogenic elements. The second-order factor is formed by the ingredients characteristic of the combustion products of different fossil fuels. The structure and space-time distribution of factors are considered. The discriminant and cluster analyses allowed to classify the observation stations considered by the atmospheric precipitation chemistry and to show that Amderma, Vorkuta, Arkhangelsk, and Kargopol stations mostly differ from each other.     

Wet deposition of precipitation chemistry during 2005–2009 at a remote site (Nam Co Station) in central Tibetan Plateau

Chemical compositions of precipitation samples collected from a remote and high elevation site (Nam Co Station, 30°46.44??N, 90°59.31??E, 4730?m?a.s.l.) in central Tibetan Plateau (TP, hereafter) from August 2005 to August 2009 are investigated. During the study period, Ca²⁺ and HCO ₃ ^- have the highest concentrations among ions and are the dominant cation and anion in precipitation, taking 27.46?% and 30.84?% to the total ions respectively. Empirical Orthogonal Functions (EOFs) analyses reveal that crustal aerosol inputs significantly contributed to the loading of Ca²⁺, Mg²⁺, SO ₄ ^2- and HCO ₃ ^- in precipitation, while lake salt plays a major source of K⁺ and Cl^-. Seasonal variations of ionic wet deposition fluxes show high values during monsoon seasons due to large precipitation amount. Among the cations, annual Ca²⁺ flux is the largest (86.26?eq hm^?2), Na⁺ and NH ₄ ⁺ fluxes are following. Among anions, HCO ₃ ^- has the highest flux (98.66?eq hm^?2) while that of NO ₃ ^- is the lowest. Annual wet deposition of nitrogen has varied considerably with the average value of 0.70?kg?ha^?1 a^?1 at Nam Co Station. About 80?% of total nitrogen flux occurs during the monsoon seasons when precipitation is concentrated, in which NH ₄ ⁺ and NO ₃ ^- contributed to 61?% and 39?% of the total nitrogen deposition. Thus, our ionic concentrations and wet deposition fluxes in precipitation can provide a useful dataset to assess atmospheric environment and its impacts on ecosystem in the inland TP.     

Chemistry of rainwater and aerosols over Bay of Bengal during CTCZ program

For the first time, simultaneous study on physical and chemical characteristics of PM₁₀, PM_2.5, and rainwater chemistry was attempted over the Bay of Bengal in monsoon season of 2009. The aerosols and rainwater samples were collected onboard ship ‘SK-261, ORV Sagar Kanya’ during Oceanographic Observations in the Northern Bay of Bengal under the Continental Tropical Convergence Zone (CTCZ) program conducted during 16 July to 19 Aug 2009. Aerosol samples collected by PM₁₀ and PM_2.5 were analyzed for various water soluble (Na⁺, K⁺, Ca²⁺, Mg²⁺, NH ₄ ⁺ , Cl^?, SO ₄ ^2? and NO ₃ ^? and acid soluble (Fe²⁺, Al³⁺, Zn²⁺, Mn³⁺ and Ni²⁺) ionic constituents. The pH of rainwater varied from 5.10 to 7.04. Chloride ions contributed most to the total ion concentration in aerosol and rainwater, followed by Na⁺. Significant contributions of SO ₄ ^2? , NO ₃ ^? and NH ₄ ⁺ found in PM_2.5, PM₁₀ and high concentrations of TSP and non sea-salt SO ₄ ^2? over the mid-ocean is attributed to the long range transport of anthropogenic pollution from the Indian continent. The scavenging ratio was maximum for coarse particles such as Ca²⁺ and minimum for fine particles like NH ₄ ⁺ _.     

Increases of wet deposition at remote sites in Japan from 1991 to 2009

Temporal trends in wet deposition of major ions were explored at nationwide remote sites in Japan from April 1991 to March 2009 by using the seasonal Kendall slope estimator and the nonparametric seasonal Kendall test. For the trend analysis, datasets from eight remote sites (Rishiri, Echizenmisaki, Oki, Ogasawara, Shionomisaki, Goto, Yakushima, and Amami) were selected from the Japanese Acid Deposition Survey (JADS) conducted by the Ministry of the Environment. Deposition of H⁺ has been increasing at remote sites in Japan on a national scale. Significant (p????0.05) increases in H⁺ deposition were detected with changes of +3?C+9?%?year^?1 at seven sites, while insignificant increases were observed at one site. Depositions of non-sea salt (nss)-SO ₄ ^2? and NO ₃ ^? significantly increased at four and six sites, respectively, with changes of +1?C+3?%?year^?1. Significant increases in precipitation at four sites would have contributed to the increase in depositions of H⁺, nss-SO ₄ ^2? , and NO ₃ ^? . The emission trends of SO₂ and NO_x did not corresponded to the deposition trends of nss-SO ₄ ^2? and NO ₃ ^? . The different trends indicated that temporal variation of precipitation amount trend dominated the deposition trends.     

Anthropogenic sulphate aerosols and large Cl-deficit in marine atmospheric boundary layer of tropical Bay of Bengal

Our long-term study provides an unequivocal evidence for near-quantitative (80–100%) depletion of chloride from sea-salts in the marine atmospheric boundary layer (MABL) of tropical Bay of Bengal. During the late NE-monsoon (Jan-Mar), continental outflow from south and south-east Asia dominate the wide-spread dispersal of pollutants over the Bay of Bengal. Among anthropogenic constituents, SO ₄ ^2? (range: 0.6–35 μg m^?3) is the most dominant. The non-sea-salt SO ₄ ^2? (nss-SO ₄ ^2? ) constitutes a major fraction (55–65%) of the aerosol water-soluble ionic composition (WSIC), whereas contribution of NO ₃ ^? is relatively minor. The magnitude of Cl-deficit (with respect to its sea-salt proportion) exhibits linear increase with the excess-nss-SO ₄ ^2? (excess over NH ₄ ⁺ ). We propose that displacement of HCl from sea-salt aerosols by H₂SO₄ is a dominant reaction mechanism for the chloride-depletion. These results also suggest that sea-salts could serve as a potential sink for anthropogenic SO₂ in the downwind polluted marine environment. Furthermore, loss of hydrogen chloride, representing a large source of reactive chlorine, has implications to the oxidant chemistry in the MABL (oxidation of hydrocarbons and dimethyl sulphide).     

In-cloud and below-cloud scavenging of aerosol ionic species over a tropical rural atmosphere in India

The temporal variation in concentrations of major water soluble ionic species has been studied from several rain events occurred over Gadanki (13.5 °N, 79.2 °E), located in tropical semi arid region in southern India. The contribution from rain-out (in cloud) and wash-out (below cloud) processes to the total removal of ionic species by rain events is also estimated using the pattern of variations of ionic species within an individual event. A number of rain samples were collected from each rain event during June–November in 2006, 2007 and 2008. On average, nearly 20% of the total NH ₄ ⁺ and non-sea SO ₄ ^2? is removed by in-cloud scavenging, suggesting that their removal by “below cloud” washout is relatively dominant. In contrast Na⁺, Ca²⁺, Mg²⁺, NO ₃ ^? and sea-SO ₄ ^2? are mainly removed by below-cloud scavenging or wash-out process. A significant variation in the acidity was observed within rain events with successive precipitation showing higher acidity at the final stage of the precipitation due to partial neutralization of non-sea SO ₄ ^2? . Overall, greater influence of both terrestrial and anthropogenic sources is recorded in the rain events compared to that from marine sources.     

Rainwater Chemistry and Wet Deposition over the Wet Savanna Ecosystem of Lamto (Côte d'Ivoire)

From the IGAC-DEBITS Africa network (IDAF), data sets on precipitation chemistry collected from the ‘wet savanna ecosystem’ site of Lamto (Côte d'Ivoire), are analyzed (1995–2002). Inorganic (Ca^{2 +}, Mg^{2 +}, Na⁺, K⁺, NH₄ ⁺, Cl^?, SO₄ ^{2 ?}, NO₃ ^?) and organic (HCOO^?, CH₃COO^?) ions content were determined using Ion Chromatography. The analyzed 631 rainfall events represent 8420.9 mm of rainfall from a 9631.1 mm total. The precipitation chemistry at Lamto is influenced by four main sources: natural biogenic emissions from savanna soils (NO _x and NH₃), biomass burning (savanna and domestic fires), terrigeneous particles emissions from dry savanna soils, and marine compounds embedded in the summer monsoon. The inter-annual variability of the weighted volume mean concentration of chemical species linked with wet deposition fluctuates by ～ 20% over the period. Ammonium concentration is found to be the highest (17.6 μ eq.l^{? 1}) from all IDAF sites belonging to the West Africa ecosystems. Ammonia sources are from domestic animals, fertilizers and biomass burning. In spite of the high potential acidity of 30.5 μ eq.l^{? 1} from NO₃ ^?, SO₄ ^{2 ?}, HCOO^? and CH₃COO^?, a relatively weak acidity is measured: 6.9 μ eq.l^{? 1}. The 40% acid neutralization is explained by the acid gas – alkaline soil particles interaction. The remaining neutralization is from inclusion of gaseous ammonia. When results from Lamto, are compared with those from Banizoumbou (dry savanna) and Zoetele (equatorial forest), a regional view for wet tropospheric chemistry processes is obtained. The high concentration of the particulate phase in precipitation emphasizes the importance of multiphases processes between gases and particles in the atmospheric chemistry of the West Africa ecosystems. For example, the nss Ca^{2 +} precipitation content, main indicator of terrigeneous particles, goes from 30.8 μ eq.l^{? 1} in dry savanna to 9.2 μ eq.l^{? 1} at Lamto and 8.9 μ eq.l^{? 1} in the Cameroon forest. A similar gradient is obtained for rainfall mineral particles precipitation content with contribution of 80% in dry savanna, 40% in wet savanna, and 20% in the equatorial forest.     

Atmospheric ionic species in PM2.5 and PM1 aerosols in the ambient air of eastern central India

This study elucidates the characteristics of ambient PM_2.5 (fine) and PM₁ (submicron) samples collected between July 2009 and June 2010 in Raipur, India, in terms of water soluble ions, i.e. Na⁺, NH ₄ ⁺ , K⁺, Mg²⁺, Ca²⁺, Cl^?, NO ₃ ^? and SO ₄ ^2? . The total number of PM_2.5 and PM₁ samples collected with eight stage cascade impactor was 120. Annual mean concentrations of PM_2.5 and PM₁ were 150.9?±?78.6 μg/m³ and 72.5?±?39.0 μg/m³, respectively. The higher particulate matter (PM) mass concentrations during the winter season are essentially due to the increase of biomass burning and temperature inversion. Out of above 8 ions, the most abundant ions were SO ₄ ^2? , NO ₃ ^? and NH ₄ ⁺ for both PM_2.5 and PM₁ aerosols; their average concentrations were 7.86?±?5.86 μg/m³, 3.12?±?2.63 μg/m³ and 1.94?±?1.28 μg/m³ for PM_2.5, and 5.61?±?3.79 μg/m³, 1.81?±?1.21 μg/m³ and 1.26?±?0.88 μg/m³ for PM₁, respectively. The major secondary species SO ₄ ^2? , NO ₃ ^? and NH ₄ ⁺ accounted for 5.81%, 1.88% and 1.40% of the total mass of PM_2.5 and 11.10%, 2.68%, and 2.48% of the total mass of PM₁, respectively. The source identification was conducted for the ionic species in PM_2.5 and PM₁ aerosols. The results are discussed by the way of correlations and principal component analysis. Spearman correlation indicated that Cl^? and K⁺ in PM_2.5 and PM₁ can be originated from similar type of sources. Principal component analysis reveals that there are two major sources (anthropogenic and natural such as soil derived particles) for PM_2.5 and PM₁ fractions.     

Future surface mass balance of the Antarctic ice sheet and its influence on sea level change, simulated by a regional atmospheric climate model

A regional atmospheric climate model with multi-layer snow module (RACMO2) is forced at the lateral boundaries by global climate model (GCM) data to assess the future climate and surface mass balance (SMB) of the Antarctic ice sheet (AIS). Two different GCMs (ECHAM5 until 2100 and HadCM3 until 2200) and two different emission scenarios (A1B and E1) are used as forcing to capture a realistic range in future climate states. Simulated ice sheet averaged 2 m air temperature (T_2m) increases (1.8–3.0 K in 2100 and 2.4–5.3 K in 2200), simultaneously and with the same magnitude as GCM simulated T_2m. The SMB and its components increase in magnitude, as they are directly influenced by the temperature increase. Changes in atmospheric circulation around Antarctica play a minor role in future SMB changes. During the next two centuries, the projected increase in liquid water flux from rainfall and snowmelt, together 60–200 Gt year^?1, will mostly refreeze in the snow pack, so runoff remains small (10–40 Gt year^?1). Sublimation increases by 25–50 %, but remains an order of magnitude smaller than snowfall. The increase in snowfall mainly determines future changes in SMB on the AIS: 6–16 % in 2100 and 8–25 % in 2200. Without any ice dynamical response, this would result in an eustatic sea level drop of 20–43 mm in 2100 and 73–163 mm in 2200, compared to the twentieth century. Averaged over the AIS, a strong relation between $\Updelta$ SMB and $\Updelta\hbox{T}_{2{\rm m}}$ of 98 ± 5 Gt w.e. year^?1 K^?1 is found.     

Time-scale and state dependence of the carbon-cycle feedback to climate

Climate and atmospheric CO₂ concentration are intimately coupled in the Earth system: CO₂ influences climate through the greenhouse effect, but climate also affects CO₂ through its impact on the amount of carbon stored on land and in the ocean. The change in atmospheric CO₂ as a response to a change in temperature ( $\varDelta CO_{2}/\varDelta T$ ) is a useful measure to quantify the feedback between the carbon cycle and climate. Using an ensemble of experiments with an Earth system model of intermediate complexity we show a pronounced time-scale dependence of $\varDelta CO_{2}/\varDelta T$ . A maximum is found on centennial scales with $\varDelta CO_{2}/\varDelta T$ values for the model ensemble in the range 5–12 ppm °C^?1, while lower values are found on shorter and longer time scales. These results are consistent with estimates derived from past observations. Up to centennial scales, the land carbon response to climate dominates the CO₂ signal in the atmosphere, while on longer time scales the ocean becomes important and eventually dominates on multi-millennial scales. In addition to the time-scale dependence, modeled $\varDelta CO_{2}/\varDelta T$ show a distinct dependence on the initial state of the system. In particular, on centennial time-scales, high $\varDelta CO_{2}/\varDelta T$ values are correlated with high initial land carbon content. A similar relation holds also for the CMIP5 models, although for $\varDelta CO_{2}/\varDelta T$ computed from a very different experimental setup. The emergence of common patterns like this could prove to usefully constrain the climate–carbon cycle feedback.     

Hourly estimation of soil heat flux density at the soil surface with three models and two field methods

Heat flux density at the soil surface (G ₀) was evaluated hourly on a vegetal cover 0.08 m high, with a leaf area index of 1.07 m² m^?2, during daylight hours, using Choudhury et al. (Agric For Meteorol 39:283–297, 1987) ( $ G_0^{\text{rn}} $ ), Santanello and Friedl (J Appl Meteorol 42:851–862, 2003) ( $ G_0^{\text{s}} $ ), and force-restore ( $ G_0^{\text{fr}} $ ) models and the plate calorimetry methodology ( $ G_0^{\text{pco}} $ ), where the gradient calorimetry methodology (G _0R ) served as a reference for determining G ₀. It was found that the peak of G _0R was at 1 p.m., with values that ranged between 60 and 100 W m^?2 and that the G ₀/Rn relation varied during the day with values close to zero in the early hours of the morning and close to 0.25 in the last hours of daylight. The $ G_0^{\text{s}} $ model presented the best performance, followed by the $ G_0^{\text{rn}} $ and $ G_0^{\text{fr}} $ models. The plate calorimetry methodology showed a similar behavior to that of the gradient calorimetry referential methodology.     

Spatial prediction model and its application to chemistry of atmospheric precipitation in Jordan

This study is concerned with the spatial variability of some wet atmospheric precipitation parameters such as; pH, conductivity (EC). The study also depicts the spatial variability of some ions (cations and anions) of atmospheric precipitation in Jordan such as, Ca²⁺, Mg²⁺, Na⁺ and K⁺, HCO₃⁻, Cl⁻, NO₃⁻ and SO₄²⁻. The basis of the work is to establish a relationship through the cumulative semivariogram technique between the distance ratios and the spatial dependence structure of the chemical composition of atmospheric precipitation. All semivariogram models are constructed in this study in order to understand the behavior of the spatial distribution. The spatial distributions of rainwater parameters show differences from station to station which is expressed in terms of angle, where the larger the angle the weaker the correlation. The semivariogram (SV) models are constructed to show the variation of the rainfall chemistry in Jordan. The SV models show weak correlation between mountain and leeside mountain stations, i.e. mountain and desert stations. On the other hand, good correlations are observed when transferring from south to north of the country. The larger is the found angle, the weaker is the correlation. For most of the SV model the correlation is found to be very weak between desert and mountainous locality. The Standard Regional Dependence Factor (SRDF) is used for prediction of the distribution of rain fall parameters. It shows the relative error between observed and predicted values of rainwater parameters. The overall regional relative error between the observed and estimated concentrations remains less than 15%.     

Beryllium-7 Deposition and Its Relation to Sulfate Deposition

Deposition of ⁷Be, a cosmogenic radionuclide, was observed at the Meteorological Research Institute in Tsukuba, Japan from 1986 to 1993 and compared with those of several chemical species observed in Tsukuba over the same period. We found a correlation between the monthly depositions of ⁷ Be and SO ₄ ² -, a major acidic species. The correlation was especially strong for late spring and fall, when both species had high depositional fluxes. This correlation was also observed in precipitation samples collected daily in 1992 at the same site. The cause of this correlation is discussed in connection with the fact that the stratospheric aerosol is composed largely of SO ₄ ² -. ⁷ Be is produced in the upper atmosphere, and detection of ⁷Be, especially in spring and fall in Japan, can be regarded as detection of stratospheric aerosol. However, we conclude that the bulk of the SO ₄ ² - observed did not have a stratospheric or an upper tropospheric origin. The correlation, therefore, may present a new question regarding acidic deposition: Why does the deposition of stratospheric aerosol in Japan coincide with that of nss-SO ₄ ² - originally from anthropogenic sources on the Earth's surface?     

Precipitation Chemistry in the Sahelian Savanna of Niger, Africa

Within the framework of the IDAF (IGAC DEBITS AFRICA) network, we present in this paper data on precipitation and aerosol chemistry in the semiarid savanna of the Sahelian region of Niger. An automatic wet-only precipitation collector was operated at the Banizoumbou station during the entire 1996 rainy season (June to September 1996). Inorganic (Na⁺, NH ₄ ⁺ , K⁺, Mg²⁺, Ca²⁺, Cl^-, NO ₃ ^- , SO ₄ ^2- ) and organic contents of the precipitation (HCOOH, CH₃COOH, C₂H₅COOH) were determined by Ion Chromatography (IC) in 29 rainfall events. Once per week, bulk particle samples were collected on the same site, and soluble water material was determined by IC. We examined the influence of atmospheric gas and particle sources on the precipitation and aerosol chemical contents. We established the influence of marine, terrigenous, and biogenic sources in the Sahelian region. The terrigenous signature is dominant and related to Sahelian soil erosion, with a high calcium content in precipitation (31.2 eq L^-1) and in aerosols (1.8 g m^-3). Two other signatures of atmospheric sources are highlighted by the relatively high nitrogenous (ammonium and nitrate) and organic contents (formate, acetate) in the precipitation. Ammonium (12.9 eq L^-1) and nitrate (12.3 eq L^-1) contents confirm respectively the biogenic source of ammonia released by domestic animal excreta in Niger and the natural emissions from semiarid savannas soils, perturbed by wild or domestic animal grazing. In spite of a high potential acidity given by nitrate, formate and acetate; a weak acidity (H⁺ (2.1 eq L^-1) is calculated from the mean pH of 5.67 measured. A statistical analysis of the aerosol chemical composition clearly indicates that nitrates are strongly correlated at the 1% level with terrigenous ions, i.e., Ca²⁺ and Mg²⁺ (0.95 < r < 1). We observed a similar relationship between all the terrigenous ions and nitrate in the precipitation. In the Sahelian region, alkaline soil dust representative of the terrigenous contribution interact, with gaseous nitrogenous and carbonaceous compounds, leading to the neutralization of acid gases and subsequent weak acidity in precipitation. Finally, taking into account the main chemical characteristics of Banizoumbou precipitations and aerosols, which demonstrate the importance of heterogeneous and multiphase chemical processes, we propose a conceptual model of the atmospheric chemistry in the Sahelian region.     

Variability of energy fluxes in relation to the net-radiation of urban and suburban areas: a case study

This paper addresses the relation between the net-radiation (Q ^*) and the ground heat flux (Q _G), the energy stored in the soil ( $\Updelta Q_{\rm S}$ ), and the residual of the energy partition (R = Q ^* ? Q _H  ? Q _E ) of urban and suburban areas of Oklahoma City, USA. These three forms of energy were observed or estimated from observations taken during Joint Urban 2003 Campaign. The database includes net-radiation, soil temperature, ground heat flux, and turbulent fluxes. In most cases the estimates of the energy stored in the soil were obtained by assuming roughly a certain type of soil and an effective soil depth. From the residuals it seems to be possible to distinguish the urban boundary layer from the suburban boundary layer when plotted as a function of net-radiation. Hysteresis coefficients were computed for fits of net-radiation against R, $\Updelta Q_{\rm S}$ and Q _G. In particular, the hysteresis patterns show that Q ^* vs. R represents clearer urban areas or suburban areas under the influence of an urban “plume”. On the other hand, hysteresis curves obtained from $\Updelta Q_{\rm S}$ or Q _G account for better the ground composition. A possible consequence is that the land use of urban areas could be roughly inferred from curve shapes such as Q ^* vs. R, or Q ^* versus another input variable representing the storage term. The objective is to show the variability of the subsurface-related energy fluxes across an urban area using these three different quantities and also to show that $\Updelta Q_{\rm S}, \,Q_{\rm G}$ , or R (and their corresponding hysteresis curves) are likely to be quantitatively different, which have not been clearly stated in the literature.     

Characterization of chemical properties of atmospheric aerosols over Anmyeon (South Korea), a super site under Global Atmosphere Watch

This paper reports aerosol chemical properties for the first time over a Korean Global Atmosphere Watch (GAW) supersite, Anmyeon (36°32′N; 126° 19′E), during 2003–2004 period. Total suspended Particulates (TSP) showed significant seasonal variation with consistent higher mass concentrations during spring season (average of up to 230?±?190 μg/m³). PM₁₀ also followed similar trend with higher concentrations during spring (average of up to 170?±?130 μg/m³) and showed reduced concentrations during summer. PM_2.5 showed a significant increase during summer (average of up to 60?±?25 μg/m³), which could be due to the influx of fine mode sea salt aerosols associated with the Changma front (summer monsoon). Chemical composition analysis showed enhanced presence of acidic fractions, majorly contributed by sulphates (SO ₄ ^2- ) and nitrates (NO ₃ ^- ) in TSP, PM₁₀ and PM_2.5 during different seasons. Enhanced presence of Calcium (Ca²⁺) was observed during sand storm days during spring. The high correlation obtained on matrix analysis between crustal ions and acidic ions suggests that the ionic compositions over the site are mainly contributed by terrestrial sources of similar origin. The neutralization factors has been estimated to find the extend of neutralization of acidicity by main basic components, and found to have higher value for Ammonium (up to 1.1) in different seasons, indicating significant neutralization of acidic components over the region by NH ₄ ⁺ . Back trajectory analysis has been performed during different seasons to constrain the possible sources of aerosol origin and the results are discussed in detail.     

Continuous observations of water-soluble ions in PM2.5 at Mount Tai (1534 m a.s.l.) in central-eastern China

Near real-time measurements of PM_2.5 ionic compositions were performed at the summit of the highest mountain in the central-eastern plains in the spring and summer of 2007 in order to characterize aerosol composition and its interaction with clouds. The average concentrations of total water soluble ions were 27.5 and 36.7 μg?m^?3, accounting for 44% and 62% of the PM_2.5 mass concentration in the spring and summer, respectively. A diurnal pattern of SO ₄ ^2- , NH ₄ ⁺ and NO ₃ ^- was observed in both campaigns and attributed to the upslope/downslope transport of air mass and the development of the planetary boundary layer (PBL). The average SO₂ oxidation ratio (SOR) in summer was 57% (±27%), more than twice that in spring 24% (±16%); the fine nitrate oxidation ratio (NOR) was comparable in the two seasons (9?±?6% and 11?±?10% in summer and spring, respectively). This result indicates strong summertime production of sulfate aerosol. A principal component analysis shows that short-range and long-range transport of pollution, cloud processing, and crustal source were the main factors affecting the variability of the measured ions (and other trace gases and aerosols) at Mt. Tai. Strong indications of biomass burning were observed in summer. Cloud scavenging rates showed larger variations for different ions and in different cloud events. The elevated concentrations of the water soluble ions at Mt. Tai indicate serious aerosol pollution over the North China plain of eastern China.     

Climate change mitigation: trade-offs between delay and strength of action required

Climate change mitigation via a reduction in the anthropogenic emissions of carbon dioxide (CO₂) is the principle requirement for reducing global warming, its impacts, and the degree of adaptation required. We present a simple conceptual model of anthropogenic CO₂ emissions to highlight the trade off between delay in commencing mitigation, and the strength of mitigation then required to meet specific atmospheric CO₂ stabilization targets. We calculate the effects of alternative emission profiles on atmospheric CO₂ and global temperature change over a millennial timescale using a simple coupled carbon cycle-climate model. For example, if it takes 50 years to transform the energy sector and the maximum rate at which emissions can be reduced is ?2.5% $\text{year}^{-1}$ , delaying action until 2020 would lead to stabilization at 540 ppm. A further 20 year delay would result in a stabilization level of 730 ppm, and a delay until 2060 would mean stabilising at over 1,000 ppm. If stabilization targets are met through delayed action, combined with strong rates of mitigation, the emissions profiles result in transient peaks of atmospheric CO₂ (and potentially temperature) that exceed the stabilization targets. Stabilization at 450 ppm requires maximum mitigation rates of ?3% to ?5% $\text{year}^{-1}$ , and when delay exceeds 2020, transient peaks in excess of 550 ppm occur. Consequently tipping points for certain Earth system components may be transgressed. Avoiding dangerous climate change is more easily achievable if global mitigation action commences as soon as possible. Starting mitigation earlier is also more effective than acting more aggressively once mitigation has begun.     

Rainwater chemistry and bulk atmospheric deposition in a tropical semiarid ecosystem: the Brazilian Caatinga

We assessed the rainwater chemistry, the potential sources of its main inorganic components and bulk atmospheric deposition in a rural tropical semiarid region in the Brazilian Caatinga. Rainfall samples were collected during two wet seasons, one during an extremely dry year (2012) and one during a year with normal rainfall (2013). According to measurements of the main inorganic ions in the rainwater (H⁺, Na⁺, NH₄ ⁺, K⁺, Ca²⁺, Mg²⁺, Cl^?, NO₃ ^?, and SO₄ ^2?), no differences were observed in the total ionic charge between the two investigated wet seasons. However, Ca²⁺, K⁺, NH₄ ⁺ and NO₃ ^? were significant higher in the wetter year (p < 0.05) which was attributed to anthropogenic activities, such as organic fertilizer applications. The total ionic contents of the rainwater suggested a dominant marine contribution, accounting for 76 % and 58 % of the rainwater in 2012 and 2013, respectively. The sum of the non-sea-salt fractions of Cl^?, SO₄ ^2?, Mg²⁺, Ca²⁺ and K⁺ were 19 % and 33 % in 2012 and 2013, and the nitrogenous compounds accounted for 2.8 % and 6.0 % of the total ionic contents in 2012 and 2013, respectively. The ionic ratios suggested that Mg²⁺ was probably the main neutralizing constituent of rainwater acidity, followed by Ca²⁺. We observed a low bulk atmospheric deposition of all major rainwater ions during both wet seasons. Regarding nitrogen deposition, we estimated slightly lower annual inputs than previous global estimates. Our findings contribute to the understanding of rainfall chemistry in northeastern Brazil by providing baseline information for a previously unstudied tropical semiarid ecosystem.