Post-industrial increases in atmospheric black carbon (BC) have a large but uncertain warming contribution to Earth's climate. Particle size and mixing state determine the solar absorption efficiency ...of BC and also strongly influence how effectively BC is removed, but they have large uncertainties. Here we use a multiple-mixing-state global aerosol microphysics model and show that the sensitivity (range) of present-day BC direct radiative effect, due to current uncertainties in emission size distributions, is amplified 5-7 times (0.18-0.42 W m
) when the diversity in BC mixing state is sufficiently resolved. This amplification is caused by the lifetime, core absorption, and absorption enhancement effects of BC, whose variability is underestimated by 45-70% in a single-mixing-state model representation. We demonstrate that reducing uncertainties in emission size distributions and how they change in the future, while also resolving modeled BC mixing state diversity, is now essential when evaluating BC radiative effects and the effectiveness of BC mitigation on future temperature changes.
Feedbacks between the global dust cycle and the climate system might have amplified past climate changes. Yet, it remains unclear what role the dust-climate feedback will play in future anthropogenic ...climate change. Here, we estimate the direct dust-climate feedback, arising from changes in the dust direct radiative effect (DRE), using a simple theoretical framework that combines constraints on the dust DRE with a series of climate model results. We find that the direct dust-climate feedback is likely in the range of -0.04 to +0.02 Wm
K
, such that it could account for a substantial fraction of the total aerosol feedbacks in the climate system. On a regional scale, the direct dust-climate feedback is enhanced by approximately an order of magnitude close to major source regions. This suggests that it could play an important role in shaping the future climates of Northern Africa, the Sahel, the Mediterranean region, the Middle East, and Central Asia.
Metal dissolution from atmospheric aerosol deposition to the oceans is important in enhancing and inhibiting phytoplankton growth rates and modifying plankton community structure, thus impacting ...marine biogeochemistry. Here we review the current state of knowledge on the causes and effects of the leaching of multiple trace metals from natural and anthropogenic aerosols. Aerosol deposition is considered both on short timescales over which phytoplankton respond directly to aerosol metal inputs, as well as longer timescales over which biogeochemical cycles are affected by aerosols.
Mineral dust acts both as a tracer and a forcing agent of climate change. Past dust variability, imprinted in paleodust records from natural archives, offers the unique opportunity to reconstruct the ...global dust cycle within a range of possibilities that plausibly encompass future variations in response to climate change and land-cover and land-use changes. Dust itself has direct and indirect feedbacks on the climate system, through impacts on the atmosphere radiative budget and the carbon cycle. Starting from well-constrained reconstructions of the present and past dust cycle, we focus on quantifying dust direct impacts on the atmospheric radiation. We discuss the intrinsic effects of dust onto climate, and how changes in the global dust budget and surface conditions modulate the effective impacts on surface temperatures and precipitation. Most notably, the presence of dust tends to enhance the West African monsoon and warm the Arctic. We also highlight how different choices in terms of dust optical properties and size distributions may yield opposite results, and what are the observational constraints we can use to make an informed choice of model parameters. Finally, we discuss how dust variability might have influenced ongoing climate transitions in the past. In particular we found that a reduction in dust load, along with a reduced cryosphere cover, acted to offset Arctic warming during the deglaciation, potentially playing a role in shaping the Northern Hemisphere deglacial dynamics.
Even though desert dust is the most abundant aerosol by mass in Earth’s atmosphere, atmospheric models 25 struggle to accurately represent its spatial and temporal distribution. These model errors ...are partially caused byfundamental difficulties in simulating dust emission in coarse-resolution models and in accurately representing dust microphysical properties. Here we mitigate these problems by developing a new methodology that yields an improved representation of the global dust cycle. We present an analytical framework that uses inverse modeling to integrate an ensemble of global model simulations with observational constraints on the dust size distribution, 30 extinction efficiency, and regional dust aerosol optical depth. We then compare the inverse model results against independent measurements of dust surface concentration and deposition flux and find that errors are reduced by approximately a factor of two relative to current model simulations of the Northern Hemisphere dust cycle. The inverse model results show smaller improvements in the less dusty Southern Hemisphere, most likely because both the model simulations and the observational constraints used in the inverse model are less accurate. On a global 35 basis, we find that the emission flux of dust with geometric diameter up to 20 μm (PM20) is approximately 5,000 Tg/year, which is greater than most models account for. This larger PM20 dust flux is needed to match observational constraints showing a large atmospheric loading of coarse dust. We obtain gridded data sets of dust emission, vertically integrated loading, dust aerosol optical depth, (surface) concentration, and wet and dry deposition fluxes that are resolved by season and particle size. As our results indicate that this data set is more accurate than current 40 model simulations and the MERRA-2 dust reanalysis product, it can be used to improve quantifications of dust impacts on the Earth system.
A global assessment of precipitation chemistry and deposition has been carried out under the direction of the World Meteorological Organization (WMO) Global Atmosphere Watch (GAW) Scientific Advisory ...Group for Precipitation Chemistry (SAG-PC). The assessment addressed three questions: (1) what do measurements and model estimates of precipitation chemistry and wet, dry and total deposition of sulfur, nitrogen, sea salt, base cations, organic acids, acidity, and phosphorus show globally and regionally? (2) has the wet deposition of major ions changed since 2000 (and, where information and data are available, since 1990) and (3) what are the major gaps and uncertainties in our knowledge? To that end, regionally-representative measurements for two 3-year-averaging periods, 2000–2002 and 2005–2007, were compiled worldwide. Data from the 2000–2002 averaging period were combined with 2001 ensemble-mean modeling results from 21 global chemical transport models produced in Phase 1 of the Coordinated Model Studies Activities of the Task Force on Hemispheric Transport of Air Pollution (TF HTAP). The measurement data and modeling results were used to generate global and regional maps of major ion concentrations in precipitation and deposition. A major product of the assessment is a database of quality assured ion concentration and wet deposition data gathered from regional and national monitoring networks. The database is available for download from the World Data Centre for Precipitation Chemistry (http://wdcpc.org/). The assessment concludes that global concentrations and deposition of sulfur and nitrogen are reasonably well characterized with levels generally highest near emission sources and more than an order of magnitude lower in areas largely free of anthropogenic influences. In many parts of the world, wet deposition of reduced nitrogen exceeds that of oxidized nitrogen and is increasing. Sulfur and nitrogen concentrations and deposition in North America and Europe have declined significantly in line with emission reduction policies. Major regions of the world, including South America, the more remote areas of North America, much of Asia, Africa, Oceania, polar regions, and all of the oceans, are inadequately sampled for all of the major ions in wet and dry deposition, and particularly so for phosphorus, organic forms of nitrogen, and weak acids including carbonates and organic acids. Measurement-based inferential estimates of dry deposition are limited to sulfur and some nitrogen in only a few regions of the world and methods are highly uncertain. The assessment concludes with recommendations to address major gaps and uncertainties in global ion concentration and deposition measurements.
•Assessed the global distribution of precipitation composition and deposition of major ions.•Produced a global data set of quality assured wet deposition monitoring data for 2000–2002 and 2005–2007.•Generated global wet deposition maps of major ions combining measurement and modeling results.•Established that sulfur and nitrogen wet deposition is highest in parts of Asia, Europe and eastern North America.•Determined that major gaps in wet and dry deposition monitoring exist globally.
This work reports on the current status of the global modeling of iron (Fe)
deposition fluxes and atmospheric concentrations and the analyses of the
differences between models, as well as between ...models and observations. A
total of four global 3-D chemistry transport (CTMs) and general circulation
(GCMs) models participated in this intercomparison, in the framework of
the United Nations Joint Group of Experts on the Scientific Aspects of Marine
Environmental Protection (GESAMP) Working Group 38, “The Atmospheric Input
of Chemicals to the Ocean”. The global total Fe (TFe) emission strength in
the models is equal to ∼72 Tg Fe yr−1 (38–134 Tg Fe yr−1)
from mineral dust sources and around 2.1 Tg Fe yr−1 (1.8–2.7 Tg Fe yr−1)
from combustion processes (the sum of anthropogenic
combustion/biomass burning and wildfires). The mean global labile Fe (LFe)
source strength in the models, considering both the primary emissions and the
atmospheric processing, is calculated to be 0.7 (±0.3) Tg Fe yr−1,
accounting for both mineral dust and combustion aerosols. The
mean global deposition fluxes into the global ocean are estimated to be in the range
of 10–30 and 0.2–0.4 Tg Fe yr−1 for TFe and LFe, respectively,
which roughly corresponds to a respective 15 and 0.3 Tg Fe yr−1 for the multi-model ensemble model mean. The model intercomparison analysis indicates that the representation of the
atmospheric Fe cycle varies among models, in terms of both the magnitude of
natural and combustion Fe emissions as well as the complexity of atmospheric
processing parameterizations of Fe-containing aerosols. The model comparison
with aerosol Fe observations over oceanic regions indicates that most models
overestimate surface level TFe mass concentrations near dust source
regions and tend to underestimate the low concentrations observed in remote
ocean regions. All models are able to simulate the tendency of higher Fe
concentrations near and downwind from the dust source regions, with the mean
normalized bias for the Northern Hemisphere (∼14), larger
than that of the Southern Hemisphere (∼2.4) for the ensemble model
mean. This model intercomparison and model–observation comparison study
reveals two critical issues in LFe simulations that require further
exploration: (1) the Fe-containing aerosol size distribution and (2) the
relative contribution of dust and combustion sources of Fe to labile Fe in
atmospheric aerosols over the remote oceanic regions.
Display omitted
► Globally 148 regional studies reviewed; average wind speed trend
=
∼−0.014
m
s
−1
a
−1. ► Globally 55 pan evaporation studies were reviewed; average trend
=
−3.19
mm
a
−2. ► ...Twenty-six crop reference evapotranspiration studies reviewed; average trend
=
−1.31
mm
a
−2. ► Globally 36 studies confirmed wind speed importance when assessing evaporation trends. ► Influence of wind speeds trends on actual evaporation depends on limiting factor.
In a globally warming climate, observed rates of atmospheric evaporative demand have declined over recent decades. Several recent studies have shown that declining rates of evaporative demand are primarily governed by trends in the aerodynamic component (primarily being the combination of the effects of wind speed (
u) and atmospheric humidity) and secondarily by changes in the radiative component. A number of these studies also show that declining rates of observed near-surface
u (termed ‘stilling’) is the primary factor contributing to declining rates of evaporative demand. One objective of this paper was to review and synthesise the literature to assess whether stilling is a globally widespread phenomenon. We analysed 148 studies reporting terrestrial
u trends from across the globe (with uneven and incomplete spatial distribution and differing periods of measurement) and found that the average trend was −0.014
m
s
−1
a
−1 for studies with more than 30 sites observing data for more than 30
years, which confirmed that stilling was widespread. Assuming a linear trend this constitutes a −0.7
m
s
−1 change in
u over 50
years. A second objective was to confirm the declining rates of evaporative demand by reviewing papers reporting trends in measured pan evaporation (
E
pan) and estimated crop reference evapotranspiration (
ET
o); average trends were −3.19
mm
a
−2 (
n
=
55) and −1.31
mm
a
−2 (
n
=
26), respectively. A third objective was to assess the contribution to evaporative demand trends that the four primary meteorological variables (being
u; atmospheric humidity; radiation; and air temperature) made. The results from 36 studies highlighted the importance of
u trends. We also quantified the sensitivity of rates of evaporative demand to changes in
u and how the relative contributions of the aerodynamic and radiative components change seasonally over the globe. Our review: (i) shows that terrestrial stilling is widespread across the globe; (ii) confirms declining rates of evaporative demand; and (iii) highlights the contribution
u has made to these declining evaporative rates. Hence we advocate that assessing evaporative demand trends requires consideration of all four primary meteorological variables (being
u, atmospheric humidity, radiation and air temperature). This is particularly relevant for long-term water resource assessment because changes in
u exert greater influence on energy-limited water-yielding catchments than water-limited ones.
A key Earth system science question is the role of atmospheric deposition in supplying vital nutrients to the phytoplankton that form the base of marine food webs. Industrial and vehicular pollution, ...wildfires, volcanoes, biogenic debris, and desert dust all carry nutrients within their plumes throughout the globe. In remote ocean ecosystems, aerosol deposition represents an essential new source of nutrients for primary production. The large spatiotemporal variability in aerosols from myriad sources combined with the differential responses of marine biota to changing fluxes makes it crucially important to understand where, when, and how much nutrients from the atmosphere enter marine ecosystems. This review brings together existing literature, experimental evidence of impacts, and new atmospheric nutrient observations that can be compared with atmospheric and ocean biogeochemistry modeling. We evaluate the contribution and spatiotemporal variability of nutrient-bearing aerosols from desert dust, wildfire, volcanic, and anthropogenic sources, including the organic component, deposition fluxes, and oceanic impacts.
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