Climate change is causing pronounced shifts during winter in the US, including shortening the snow season, reducing snowpack, and altering the timing and volume of snowmelt-related runoff. These changes in winter precipitation patterns affect in-stream freeze-thaw cycles, including ice and snow cover, and can trigger direct and indirect effects on in-stream physical, chemical, and biological processes in similar to 60% of river basins in the Northern Hemisphere. We used high-resolution, multi-parameter data collected in a headwater stream and its local environment (climate and soil) to determine interannual variability in physical, chemical, and biological signals in a montane stream during the winter of an El Nino and a La Nina year. We observed similar to 77% greater snow accumulation during the El Nino year, which caused the formation of an ice dam that shifted the system from a primarily lotic to a lentic environment. Water chemistry and stream metabolism parameters varied widely between years. They featured anoxic conditions lasting over a month, with no observable gross primary production (GPP) occurring under the ice and snow cover in the El Nino year. In contrast, dissolved oxygen and GPP remained relatively high during the winter months of the La Nina year. These redox and metabolic changes driven by changes in winter precipitation have significant implications for water chemistry and biological functioning beyond the winter. Our study suggests that as snow accumulation and hydrologic conditions shift during the winter due to climate change, hot-spots and hot-moments for biogeochemical processing may be reduced, with implications for the downstream movement of nutrients and transported materials.
Aviation emissions are responsible for an estimated 24,000 premature mortalities annually and 3.5% of anthropogenic radiative forcing (RF). Emissions of nitrogen and sulfur oxides (NOx and SOx) contribute to these impacts. However, the relative contributions and mechanisms linking these emissions to formation and impacts of secondary aerosols (as opposed to direct aerosol emissions) have not been quantified, including how short-lived aerosol precursors at altitude can increase surface-level aerosol concentrations. We apply global chemistry transport modeling to identify and quantify the different chemical pathways to aerosol formation from aviation emissions, including the resulting impact on radiative forcing. We estimate a net aerosol radiative forcing of -8.3 mWm(-2), of which -0.67 and -7.8 mWm(-2) result from nitrate and sulfate aerosols respectively. We find that aviation NOx causes -1.7 mWm(-2) through nitrate aerosol forcing but also -1.6 mWm(-2) of sulfate aerosol forcing by promoting oxidation of SO2 to sulfate aerosol. This accounts for 21% of the total sulfate forcing, and oxidation of SO2 due to aviation NOx is responsible for 47% of the net aviation NOx attributable RF. Aviation NOx emissions in turn account for 41% of net aviation-aerosol-attributable RF (non-contrail). This is due to ozone-mediated oxidation of background sulfur and the 'nitrate bounce-back' effect, which reduces the net impact of sulfur emissions. The ozone-mediated mechanism also explains the ability of cruise aviation emissions to significantly affect surface aerosol concentrations. We find that aviation NOx emissions cause 72% of aviation-attributable, near-surface aerosol loading by mass, compared to 27% from aviation SOx emissions and less than 0.1% from direct emission of black carbon. We conclude that aviation NOx and SOx emissions are the dominant cause of aviation-attributable secondary inorganic aerosol radiative forcing, and that conversion of background aerosol precursors at all altitudes is amplified by enhanced production of aviation attributable oxidants at cruise altitudes.
Global aviation operations contribute to anthropogenic climate change via a complex set of processes that lead to a net surface warming. Of importance are aviation emissions of carbon dioxide (CO2), nitrogen oxides (NOx), water vapor, soot and sulfate aerosols, and increased cloudiness due to contrail formation. Aviation grew strongly over the past decades (1960-2018) in terms of activity, with revenue passenger kilometers increasing from 109 to 8269 billion km yr(-1), and in terms of climate change impacts, with CO2 emissions increasing by a factor of 6.8 to 1034 Tg CO2 yr(-1). Over the period 2013-2018, the growth rates in both terms show a marked increase. Here, we present a new comprehensive and quantitative approach for evaluating aviation climate forcing terms. Both radiative forcing (RF) and effective radiative forcing (ERF) terms and their sums are calculated for the years 2000-2018. Contrail cirrus, consisting of linear contrails and the cirrus cloudiness arising from them, yields the largest positive net (warming) ERF term followed by CO2 and NOx emissions. The for-mation and emission of sulfate aerosol yields a negative (cooling) term. The mean contrail cirrus ERF/RF ratio of 0.42 indicates that contrail cirrus is less effective in surface warming than other terms. For 2018 the net aviation ERF is +100.9 milliwatts (mW) m(-2) (5-95% likelihood range of (55, 145)) with major contributions from contrail cirrus (57.4 mW m(-2)), CO2 (34.3 mW m(-2)), and NOx (17.5 mW m(-2)). Non-CO2 terms sum to yield a net positive (warming) ERF that accounts for more than half (66%) of the aviation net ERF in 2018. Using normalization to aviation fuel use, the contribution of global aviation in 2011 was calculated to be 3.5 (4.0, 3.4) % of the net anthropogenic ERF of 2290 (1130, 3330) mW m(-2). Uncertainty distributions (5%, 95%) show that non-CO2 forcing terms contribute about 8 times more than CO2 to the uncertainty in the aviation net ERF in 2018. The best estimates of the ERFs from aviation aerosol-cloud interactions for soot and sulfate remain undetermined. CO2-warming-equivalent emissions based on global warming potentials (GWP* method) indicate that aviation emissions are currently warming the climate at approximately three times the rate of that associated with aviation CO2 emissions alone. CO2 and NOx aviation emissions and cloud effects remain a continued focus of anthropogenic climate change research and policy discussions.
Inorganic particulate nitrate (p-NO3-), gaseous nitric acid (HNO3(g)) and nitrogen oxides (NOx = NO + NO2), as main atmospheric pollutants, have detrimental effects on human health and aquatic/terrestrial ecosystems. Referred to as the 'Third Pole' and the 'Water Tower of Asia', the Tibetan Plateau (TP) has attracted wide attention on its environmental changes. Here, we evaluated the oxidation processes of atmospheric nitrate as well as traced its potential sources by analyzing the isotopic compositions of nitrate (delta N-15, delta O-18, and Delta O-17) in the aerosols collected from the Mt. Everest region during April to September 2018. Over the entire sampling campaigns, the average of delta N-15(NO3-), delta O-18(NO3-), and Delta O-17(NO3-) was -5.1 +/- 2.3 parts per thousand, 66.7 +/- 10.2 parts per thousand, and 24.1 +/- 3.9 parts per thousand, respectively. The seasonal variation in Delta O-17(NO3-) indicates the relative importance of O-3 and HO2/RO2/OH in NOx oxidation processes among different seasons. A significant correlation between NO3- and Ca2+ and frequent dust storms in the Mt. Everest region indicate that initially, the atmospheric nitrate in this region might have undergone a process of settling; subsequently, it got re-suspended in the dust. Compared with the Delta O-17(NO3-) values in the northern TP, our observed significantly higher values suggest that spatial variations in atmospheric Delta O-17(NO3-) exist within the TP, and this might result from the spatial variations of the atmospheric O-3 levels, especially the stratospheric O-3, over the TP. The observed delta N-15(NO3-) values predicted remarkably low delta N-15 values in the NOx of the sources and the N isotopic fractionation plays a crucial role in the seasonal changes of delta N-15(NO3-). Combined with the results from the backward trajectory analysis of air mass, we suggest that the vehicle exhausts and agricultural activities in South Asia play a dominant role in determining the nitrate levels in the Mt. Everest region. (c) 2020 Elsevier Ltd. All rights reserved.
Black carbon (BC) is an important atmospheric aerosol constituent that affects the climate by absorbing (directly) the sunlight and modifying cloud characteristics (indirectly). Here, we present first time yearlong measurements of BC and carbon monoxide (CO) from an urban location of Guwahati located in the Brahmaputra River valley (BRV) in the northeast region of India from 1st July 2013 to 30th June 2014. Daily BC concentrations varied within the range of 2.86 to 11.56 mu g m(-3) with an annual average of 7.17 +/- 1.89 mu g m(-3), while, CO varied from 0.19 to 1.20 ppm with a mean value of 0.51 +/- 0.19 ppm during the study period. The concentrations of BC (8.37 mu g m(-3)) and CO (0.67 ppm) were similar to 39% and similar to 55% higher during the dry months (October to March) than the wet months (April to September) suggesting that seasonal changes in meteorology and emission sources play an important role in controlling these species. The seasonal Delta BC/Delta CO ratios were highest (lowest) in the pre-monsoon (winter) 18.1 +/- 1.4 mu g m(-3) ppmv(-1) (12.6 +/- 2.2 mu g m(-3) ppmv(-1)) which indicate the combustion of biofuel/biomass as well as direct emissions from fossil fuel during the pre-monsoon season. The annual BC emission was estimated to be 2.72 Gg in and around Guwahati which is about 44% lower than the mega city 'Delhi' (4.86 Gg). During the study period, the annual mean radiative forcing (RF) at the top of the atmosphere (TOA) for clear skies of BC was +9.5Wm(-2), however, the RF value at the surface (SFC) was -21.1 Wm(-2) which indicates the net warming and cooling effects, respectively. The highest RF at SFC was in the month of April (-30 Wm(-2)) which is coincident with the highest BC mass level. The BC atmospheric radiative forcing (ARF) was +30.16 (annualmean) Wm(-2) varying from +23.1 to +43.8 Wm(-2). The annualmean atmospheric heating rate (AHR) due to the BC aerosols was 0.86 K day(-1) indicates the enhancement in radiation effect over the study region. The Weather Research and Forecasting model coupled with Chemistry(WRF-Chem) captured the seasonal cycle of observed BC fairly well but underestimated the observed BC during the month of May-August. Model results show that BC at Guwahati is controlled mainly by anthropogenic emissions except during the pre-monsoon season when open biomass burning also makes a similar contribution. (C) 2016 Elsevier B.V. All rights reserved.
Existing carbon offset protocols for improved cookstoves do not require emissions testing. They are based only on estimated reductions in the use of non-renewable biomass generated by a given stove, and use simplistic calculations to convert those fuel savings to imputed emissions of carbon dioxide (CO2). Yet recent research has shown that different cookstoves vary tremendously in their combustion quality, and thus in their emissions profiles of both CO2 and other products of incomplete combustion. Given the high global warming potential of some of these non-CO2 emissions, offset protocols that do not account for combustion quality may thus not be assigning either appropriate absolute or relative climate values to different technologies. We use statistical resampling of recent emissions studies to estimate the actual radiative forcing impacts of traditional and improved cookstoves. We compare the carbon offsets generated by protocols in the four carbon markets that currently accept cookstove offsets (Clean Development Mechanism, American Carbon Registry, Verified Carbon Standard, and Gold Standard) to a theoretical protocol that also accounts for emissions of carbonaceous aerosols and carbon monoxide, using appropriate statistical techniques to estimate emissions factor distributions from the literature. We show that current protocols underestimate the climate value of many improved cookstoves and fail to distinguish between (i.e., assign equal offset values to) technologies with very different climate impacts. We find that a comprehensive carbon accounting standard would generate significantly higher offsets for some improved cookstove classes than those generated by current protocols, and would create much larger separation between different cookstove classes. Finally, we provide compelling evidence for the inclusion of renewable biomass into current protocols, and propose guidelines for the statistics needed in future emissions tests in order to accurately estimate the climate impact (and thus offsets generated by) cookstoves and other household energy technologies.
Three global chemistry-transport models (CTM) are used to quantify the radiative forcing (RF) from aviation NOx emissions, and the resultant reductions in RF from coupling NOx to aerosols via heterogeneous chemistry. One of the models calculates the changes due to aviation black carbon (BC) and sulphate aerosols and their direct RF, as well as the BC indirect effect on cirrus cloudiness. The surface area density of sulphate aerosols is then passed to the other models to compare the resulting photochemical perturbations on NOx through heterogeneous chemical reactions. The perturbation on O-3 and CH4 (via OH) is finally evaluated, considering both short- and long-term O-3 responses. Ozone RF is calculated using the monthly averaged output of the three CTMs in two independent radiative transfer codes. According to the models, column ozone and CH4 lifetime changes due to coupled NOx/aerosol emissions are, on average, +0.56 Dobson Units (DU) and -1.1 months, respectively, for atmospheric conditions and aviation emissions representative of the year 2006, with an RF of +16.4 and -10.2 mW/m(2) for O-3 and CH4, respectively. Sulphate aerosol induced changes on ozone column and CH4 lifetime account for -0.028 DU and +0.04 months, respectively, with corresponding RFs of -0.63 and +0.36 mW/m(2). Soot-cirrus forcing is calculated to be 4.9 mW/m(2).
Fires impact atmospheric composition through their emissions, which range from long-lived gases to short-lived gases and aerosols. Effects are typically larger in the tropics and boreal regions but can also be substantial in highly populated areas in the northern mid-latitudes. In all regions, fire can impact air quality and health. Similarly, its effect on large-scale atmospheric processes, including regional and global atmospheric chemistry and climate forcing, can be substantial, but this remains largely unexplored. The impacts are primarily realised in the boundary layer and lower free troposphere but can also be noticeable in upper troposphere/lower stratosphere (UT/LS) region, for the most intense fires. In this review, we summarise the recent literature on findings related to fire impact on atmospheric composition, air quality and climate. We explore both observational and modelling approaches and present information on key regions and on the globe as a whole. We also discuss the current and future directions in this area of research, focusing on the major advances in emission estimates, the emerging efforts to include fire as a component in Earth system modelling and the use of modelling to assess health impacts of fire emissions.
This article presents the status of aerosols in India based on the research activities undertaken during last few decades in this region. Programs, like International Geophysical Year (IGY), Monsoon Experiment (MONEX), Indian Middle Atmospheric Program (IMAP) and recently conducted Indian Ocean Experiment (INDOEX), have thrown new lights on the role of aerosols in global change. INDOEX has proved that the effects of aerosols are no longer confined to the local levels but extend at regional as well as global scales due to occurrence of long range transportation of aerosols from source regions along with wind trajectories. The loading of aerosols in the atmosphere is on rising due to energy intensive activities for developmental processes and other anthropogenic activities. One of the significant observation of INDOEX is the presence of high concentrations of carbonaceous aerosols in the near persistent winter time haze layer over tropical Indian Ocean which have probably been emitted from the burning of fossil-fuels and biofuels in the source region. These have significant bearing on the radiative forcing in the region and, therefore, have potential to alter monsoon and hydrological cycles. In general, the SPM concentrations have been found to be on higher sides in ambient atmosphere in many Indian cities but the NOx concentrations have been found to be on lower side. Even in the haze layer over Indian Ocean and surrounding areas, the NOx concentrations have been reported to be low which is not conducive of O-3 formation in the haze/smog layer. The acid rain problem does not seem to exist at the moment in India because of the presence of neutralizing soil dust in the atmosphere. But the high particulate concentrations in most of the cities' atmosphere in India are of concern as it can cause deteriorated health conditions. (C) 2002 Elsevier Science Ltd. All rights reserved.