scholarly journals Revisiting particle dry deposition and its role in radiative effect estimates

2020 ◽  
Vol 117 (42) ◽  
pp. 26076-26082
Author(s):  
Ethan W. Emerson ◽  
Anna L. Hodshire ◽  
Holly M. DeBolt ◽  
Kelsey R. Bilsback ◽  
Jeffrey R. Pierce ◽  
...  
Keyword(s):  
Dry Deposition ◽  
Radiative Forcing ◽  
Particle Deposition ◽  
Climate Models ◽  
Transport Model ◽  
Cloud Condensation Nuclei ◽  
Measurement Techniques ◽  
Chemical Transport ◽  
Radiative Effect ◽  
Accumulation Mode

Wet and dry deposition remove aerosols from the atmosphere, and these processes control aerosol lifetime and thus impact climate and air quality. Dry deposition is a significant source of aerosol uncertainty in global chemical transport and climate models. Dry deposition parameterizations in most global models were developed when few particle deposition measurements were available. However, new measurement techniques have enabled more size-resolved particle flux observations. We combined literature measurements with data that we collected over a grassland in Oklahoma and a pine forest in Colorado to develop a dry deposition parameterization. We find that relative to observations, previous parameterizations overestimated deposition of the accumulation and Aitken mode particles, and underestimated in the coarse mode. These systematic differences in observed and modeled accumulation mode particle deposition velocities are as large as an order of magnitude over terrestrial ecosystems. As accumulation mode particles form most of the cloud condensation nuclei (CCN) that influence the indirect radiative effect, this model-measurement discrepancy in dry deposition alters modeled CCN and radiative forcing. We present a revised observationally driven parameterization for regional and global aerosol models. Using this revised dry deposition scheme in the Goddard Earth Observing System (GEOS)-Chem chemical transport model, we find that global surface accumulation-mode number concentrations increase by 62% and enhance the global combined anthropogenic and natural aerosol indirect effect by −0.63 W m−2. Our observationally constrained approach should reduce the uncertainty of particle dry deposition in global chemical transport models.

Effects of Dry Deposition on Surface Ozone over South Asia Inferred from a Regional Chemical Transport Model

2020 ◽  
Vol 4 (2) ◽  
pp. 321-327 ◽  
Author(s):  
Amit Sharma ◽  
Narendra Ojha ◽  
Tabish U. Ansari ◽  
Som K. Sharma ◽  
Andrea Pozzer ◽  
...  
Keyword(s):  
South Asia ◽  
Dry Deposition ◽  
Transport Model ◽  
Surface Ozone ◽  
Chemical Transport ◽  
Chemical Transport Model

scholarly journals Machine learning uncovers aerosol size information from chemistry and meteorology to quantify potential cloud-forming particles

2021 ◽  
Author(s):  
Arshad Nair ◽  
Fangqun Yu ◽  
Pedro Campuzano Jost ◽  
Paul DeMott ◽  
Ezra Levin ◽  
...  
Keyword(s):  
Climate Change ◽  
Machine Learning ◽  
Radiative Forcing ◽  
Climate Models ◽  
Cloud Condensation Nuclei ◽  
Global Climate Models ◽  
Aerosol Composition ◽  
Airborne Measurements ◽  
Aerosol Cloud ◽  
Aerosol Cloud Interactions

Abstract Cloud condensation nuclei (CCN) are mediators of aerosol–cloud interactions, which contribute to the largest uncertainty in climate change prediction. Here, we present a machine learning/artificial intelligence model that quantifies CCN from variables of aerosol composition, atmospheric trace gases, and meteorology. Comprehensive multi-campaign airborne measurements, covering varied physicochemical regimes in the troposphere, confirm the validity of and help probe the inner workings of this machine learning model: revealing for the first time that different ranges of atmospheric aerosol composition and mass correspond to distinct aerosol number size distributions. Machine learning extracts this information, important for accurate quantification of CCN, additionally from both chemistry and meteorology. This can provide a physicochemically explainable, computationally efficient, robust machine learning pathway in global climate models that only resolve aerosol composition; potentially mitigating the uncertainty of effective radiative forcing due to aerosol–cloud interactions (ERFaci) and improving confidence in assessment of anthropogenic contributions and climate change projections.

scholarly journals Concentrations and source regions of light absorbing impurities in snow/ice in northern Pakistan and their impact on snow albedo

2017 ◽  
Author(s):  
Chaman Gul ◽  
Siva Praveen Puppala ◽  
Shichang Kang ◽  
Bhupesh Adhikary ◽  
Yulan Zhang ◽  
...  
Keyword(s):  
Radiative Forcing ◽  
Transport Model ◽  
Chemical Transport ◽  
Small Contribution ◽  
Northern Pakistan ◽  
Chemical Transport Model ◽  
Transport Modelling ◽  
Snow Albedo ◽  
Source Regions ◽  
Snow And Ice

Abstract. Black carbon (BC), water-insoluble organic carbon (OC), and mineral dust are important particulate impurities in snow and ice, which significantly reduce albedo and accelerate melting. Surface snow and ice samples were collected from the Karakoram–Himalayan region of northern Pakistan during 2015 and 2016 in summer (six glaciers), autumn (two glaciers), and winter (six mountain valleys). The average BC concentration overall was 2130 ± 1560 ngg−1 in summer samples, 2883 ± 3439 ngg−1 in autumn samples, and 992 ± 883 ngg−1 in winter samples. The average water insoluble OC concentration overall was 1839 ± 1108 ngg−1 in summer samples, 1423 ± 208 ngg−1 in autumn samples, and 1342 ± 672 ngg−1 in winter samples. The overall concentration of BC, OC, and dust in aged snow samples collected during the summer campaign was higher than the concentration in ice samples. The values are relatively high compared to reports by others for the Himalayas and Tibetan Plateau. This is probably the result of taking more representative samples at lower elevation where deposition is higher and the effects of ageing and enrichment more marked. A reduction in snow albedo of 0.1–8.3 % for fresh snow and 0.9–32.5 % for aged snow was calculated for selected solar zenith angles during day time using the Snow, Ice, and Aerosol Radiation (SNICAR) model. Daily mean albedo was reduced by 0.07–12.0 %. The calculated radiative forcing ranged from 0.16 to 43.45 Wm−2 depending on snow type, solar zenith angle, and location. The potential source regions of the deposited pollutants were identified using spatial variance in wind vector maps, emission inventories coupled with backward air trajectories, and simple region tagged chemical transport modelling. Central, South, and West Asia were the major sources of pollutants during the sampling months, with only a small contribution from East Asia. Analysis based on the Weather Research and Forecasting (WRF-STEM) chemical transport model identified a significant contribution (more than 70 %) from South Asia at selected sites. Research into the presence and effect of pollutants in the glaciated areas of Pakistan is economically significant because the surface water resources in the country mainly depend on the rivers (the Indus and its tributaries) that flow from this glaciated area.

scholarly journals Coupling between surface ozone and leaf area index in a chemical transport model: strength of feedback and implications for ozone air quality and vegetation health

2018 ◽  
Vol 18 (19) ◽  
pp. 14133-14148 ◽  
Author(s):  
Shan S. Zhou ◽  
Amos P. K. Tai ◽  
Shihan Sun ◽  
Mehliyar Sadiq ◽  
Colette L. Heald ◽  
...  
Keyword(s):  
Air Quality ◽  
Leaf Area Index ◽  
Leaf Area ◽  
Dry Deposition ◽  
Transport Model ◽  
Surface Ozone ◽  
Chemical Transport ◽  
Chemical Transport Model ◽  
Area Index ◽  
Ozone Levels

Abstract. Tropospheric ozone is an air pollutant that substantially harms vegetation and is also strongly dependent on various vegetation-mediated processes. The interdependence between ozone and vegetation may constitute feedback mechanisms that can alter ozone concentration itself but have not been considered in most studies to date. In this study we examine the importance of dynamic coupling between surface ozone and leaf area index (LAI) in shaping ozone air quality and vegetation. We first implement an empirical scheme for ozone damage on vegetation in the Community Land Model (CLM) and simulate the steady-state responses of LAI to long-term exposure to a range of prescribed ozone levels (from 0 to 100 ppb). We find that most plant functional types suffer a substantial decline in LAI as ozone level increases. Based on the CLM-simulated results, we develop and implement in the GEOS-Chem chemical transport model a parameterization that computes fractional changes in monthly LAI as a function of local mean ozone levels. By forcing LAI to respond to ozone concentrations on a monthly timescale, the model simulates ozone–LAI coupling dynamically via biogeochemical processes including biogenic volatile organic compound (VOC) emissions and dry deposition, without the complication from meteorological changes. We find that ozone-induced damage on LAI can lead to changes in ozone concentrations by −1.8 to +3 ppb in boreal summer, with a corresponding ozone feedback factor of −0.1 to +0.6 that represents an overall self-amplifying effect from ozone–LAI coupling. Substantially higher simulated ozone due to strong positive feedbacks is found in most tropical forests, mainly due to the ozone-induced reductions in LAI and dry deposition velocity, whereas reduced isoprene emission plays a lesser role in these low-NOx environments. In high-NOx regions such as the eastern US, Europe, and China, however, the feedback effect is much weaker and even negative in some regions, reflecting the compensating effects of reduced dry deposition and reduced isoprene emission (which reduces ozone in high-NOx environments). In remote, low-LAI regions, including most of the Southern Hemisphere, the ozone feedback is generally slightly negative due to the reduced transport of NOx–VOC reaction products that serve as NOx reservoirs. This study represents the first step to accounting for dynamic ozone–vegetation coupling in a chemical transport model with ramifications for a more realistic joint assessment of ozone air quality and ecosystem health.

scholarly journals Contrasting the direct radiative effect and direct radiative forcing of aerosols

2014 ◽  
Vol 14 (11) ◽  
pp. 5513-5527 ◽  
Author(s):  
C. L. Heald ◽  
D. A. Ridley ◽  
J. H. Kroll ◽  
S. R. H. Barrett ◽  
K. E. Cady-Pereira ◽  
...  
Keyword(s):  
Energy Balance ◽  
Radiative Forcing ◽  
Transport Model ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
Radiative Effect ◽  
Chemical Transport Model ◽  
Anthropogenic Aerosols ◽  
Anthropogenic Aerosol ◽  
Direct Radiative Forcing

Abstract. The direct radiative effect (DRE) of aerosols, which is the instantaneous radiative impact of all atmospheric particles on the Earth's energy balance, is sometimes confused with the direct radiative forcing (DRF), which is the change in DRE from pre-industrial to present-day (not including climate feedbacks). In this study we couple a global chemical transport model (GEOS-Chem) with a radiative transfer model (RRTMG) to contrast these concepts. We estimate a global mean all-sky aerosol DRF of −0.36 Wm−2 and a DRE of −1.83 Wm−2 for 2010. Therefore, natural sources of aerosol (here including fire) affect the global energy balance over four times more than do present-day anthropogenic aerosols. If global anthropogenic emissions of aerosols and their precursors continue to decline as projected in recent scenarios due to effective pollution emission controls, the DRF will shrink (−0.22 Wm−2 for 2100). Secondary metrics, like DRE, that quantify temporal changes in both natural and anthropogenic aerosol burdens are therefore needed to quantify the total effect of aerosols on climate.

scholarly journals Effects of aerosol dynamics and gas–particle conversion on dry deposition of inorganic reactive nitrogen in a temperate forest

2020 ◽  
Vol 20 (8) ◽  
pp. 4933-4949 ◽  
Author(s):  
Genki Katata ◽  
Kazuhide Matsuda ◽  
Atsuyuki Sorimachi ◽  
Mizuo Kajino ◽  
Kentaro Takagi
Keyword(s):  
Dry Deposition ◽  
Particle Deposition ◽  
Chemical Transport ◽  
Reactive Nitrogen ◽  
Surface Model ◽  
Deposition Flux ◽  
Transport Models ◽  
Inorganic Particles ◽  
Aerosol Dynamics ◽  
Chemical Transport Models

Abstract. Dry deposition has an impact on nitrogen status in forest environments. However, the mechanism for the high dry-deposition rates of fine nitrate particles (NO3-) observed in forests remains unknown and is thus a potential source of error in chemical transport models (CTMs). Here, we modified and applied a multilayer land surface model coupled with dry-deposition and aerosol dynamic processes for a temperate mixed forest in Japan. This represents the first application of such a model to ammonium nitrate (NH4NO3) gas–particle conversion (gpc) and the aerosol water uptake of reactive nitrogen compounds. Thermodynamics, kinetics, and dry deposition for mixed inorganic particles are modeled by a triple-moment modal method. Data for inorganic mass and size-resolved total number concentrations measured by a filter pack and electrical low-pressure impactor in autumn were used for model inputs and subsequent numerical analysis. The model successfully reproduces turbulent fluxes observed above the canopy and vertical micrometeorological profiles noted in our previous studies. The sensitivity tests with and without gpc demonstrated clear changes in the inorganic mass and size-resolved total number concentrations within the canopy. The results also revealed that within-canopy evaporation of NH4NO3 under dry conditions significantly enhances the deposition flux of fine-NO3- and fine-NH4+ particles, while reducing the deposition flux of nitric acid gas (HNO3). As a result of the evaporation of particulate NH4NO3, the calculated daytime mass flux of fine NO3- over the canopy was 15 times higher in the scenario of “gpc” than in the scenario of “no gpc”. This increase caused high contributions from particle deposition flux (NO3- and NH4+) to total nitrogen flux over the forest ecosystem (∼39 %), although the contribution of NH3 was still considerable. A dry-deposition scheme coupled with aerosol dynamics may be required to improve the predictive accuracy of chemical transport models for the surface concentration of inorganic reactive nitrogen.

scholarly journals Combined assimilation of IASI and MLS observations to constrain tropospheric and stratospheric ozone in a global chemical transport model

2013 ◽  
Vol 13 (8) ◽  
pp. 21455-21505
Author(s):  
E. Emili ◽  
B. Barret ◽  
S. Massart ◽  
E. Le Flochmoen ◽  
A. Piacentini ◽  
...  
Keyword(s):  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
Transport Model ◽  
Stratospheric Ozone ◽  
Chemical Transport ◽  
Free Troposphere ◽  
Chemical Transport Model ◽  
Ozone Monitoring Instrument ◽  
Global Chemical Transport Model ◽  
The Impact

Abstract. Accurate and temporally resolved fields of free-troposphere ozone are of major importance to quantify the intercontinental transport of pollution and the ozone radiative forcing. In this study we examine the impact of assimilating ozone observations from the Microwave Limb Sounder (MLS) and the Infrared Atmospheric Sounding Interferometer (IASI) in a global chemical transport model (MOdèle de Chimie Atmosphérique à Grande Échelle, MOCAGE). The assimilation of the two instruments is performed by means of a variational algorithm (4-D-VAR) and allows to constrain stratospheric and tropospheric ozone simultaneously. The analysis is first computed for the months of August and November 2008 and validated against ozone-sondes measurements to verify the presence of observations and model biases. It is found that the IASI Tropospheric Ozone Column (TOC, 1000–225 hPa) should be bias-corrected prior to assimilation and MLS lowermost level (215 hPa) excluded from the analysis. Furthermore, a longer analysis of 6 months (July–August 2008) showed that the combined assimilation of MLS and IASI is able to globally reduce the uncertainty (Root Mean Square Error, RMSE) of the modeled ozone columns from 30% to 15% in the Upper-Troposphere/Lower-Stratosphere (UTLS, 70–225 hPa) and from 25% to 20% in the free troposphere. The positive effect of assimilating IASI tropospheric observations is very significant at low latitudes (30° S–30° N), whereas it is not demonstrated at higher latitudes. Results are confirmed by a comparison with additional ozone datasets like the Measurements of OZone and wAter vapour by aIrbus in-service airCraft (MOZAIC) data, the Ozone Monitoring Instrument (OMI) total ozone columns and several high-altitude surface measurements. Finally, the analysis is found to be little sensitive to the assimilation parameters and the model chemical scheme, due to the high frequency of satellite observations compared to the average life-time of free-troposphere/low-stratosphere ozone.

Aerosol-driven droplet concentrations dominate coverage and water of oceanic low-level clouds

Science ◽  
2019 ◽  
Vol 363 (6427) ◽  
pp. eaav0566 ◽  
Author(s):  
Daniel Rosenfeld ◽  
Yannian Zhu ◽  
Minghuai Wang ◽  
Youtong Zheng ◽  
Tom Goren ◽  
...  
Keyword(s):  
Radiative Forcing ◽  
Cloud Cover ◽  
Climate Models ◽  
Cloud Condensation Nuclei ◽  
Climate Forcing ◽  
Present Climate ◽  
Cloud Radiative Forcing ◽  
Cloud Properties ◽  
Aerosol Effects ◽  
Meteorological Effects

A lack of reliable estimates of cloud condensation nuclei (CCN) aerosols over oceans has severely limited our ability to quantify their effects on cloud properties and extent of cooling by reflecting solar radiation—a key uncertainty in anthropogenic climate forcing. We introduce a methodology for ascribing cloud properties to CCN and isolating the aerosol effects from meteorological effects. Its application showed that for a given meteorology, CCN explains three-fourths of the variability in the radiative cooling effect of clouds, mainly through affecting shallow cloud cover and water path. This reveals a much greater sensitivity of cloud radiative forcing to CCN than previously reported, which means too much cooling if incorporated into present climate models. This suggests the existence of compensating aerosol warming effects yet to be discovered, possibly through deep clouds.

scholarly journals Concentrations and source regions of light-absorbing particles in snow/ice in northern Pakistan and their impact on snow albedo

2018 ◽  
Vol 18 (7) ◽  
pp. 4981-5000 ◽  
Author(s):  
Chaman Gul ◽  
Siva Praveen Puppala ◽  
Shichang Kang ◽  
Bhupesh Adhikary ◽  
Yulan Zhang ◽  
...  
Keyword(s):  
Radiative Forcing ◽  
Transport Model ◽  
Chemical Transport ◽  
The Tibetan Plateau ◽  
Small Contribution ◽  
Northern Pakistan ◽  
Chemical Transport Model ◽  
Snow Albedo ◽  
Source Regions ◽  
Snow And Ice

Abstract. Black carbon (BC), water-insoluble organic carbon (OC), and mineral dust are important particles in snow and ice which significantly reduce albedo and accelerate melting. Surface snow and ice samples were collected from the Karakoram–Himalayan region of northern Pakistan during 2015 and 2016 in summer (six glaciers), autumn (two glaciers), and winter (six mountain valleys). The average BC concentration overall was 2130 ± 1560 ng g−1 in summer samples, 2883 ± 3439 ng g−1 in autumn samples, and 992 ± 883 ng g−1 in winter samples. The average water-insoluble OC concentration overall was 1839 ± 1108 ng g−1 in summer samples, 1423 ± 208 ng g−1 in autumn samples, and 1342 ± 672 ng g−1 in winter samples. The overall concentration of BC, OC, and dust in aged snow samples collected during the summer campaign was higher than the concentration in ice samples. The values are relatively high compared to reports by others for the Himalayas and the Tibetan Plateau. This is probably the result of taking more representative samples at lower elevation where deposition is higher and the effects of ageing and enrichment are more marked. A reduction in snow albedo of 0.1–8.3 % for fresh snow and 0.9–32.5 % for aged snow was calculated for selected solar zenith angles during daytime using the Snow, Ice, and Aerosol Radiation (SNICAR) model. The daily mean albedo was reduced by 0.07–12.0 %. The calculated radiative forcing ranged from 0.16 to 43.45 W m−2 depending on snow type, solar zenith angle, and location. The potential source regions of the deposited pollutants were identified using spatial variance in wind vector maps, emission inventories coupled with backward air trajectories, and simple region-tagged chemical transport modeling. Central, south, and west Asia were the major sources of pollutants during the sampling months, with only a small contribution from east Asia. Analysis based on the Weather Research and Forecasting (WRF-STEM) chemical transport model identified a significant contribution (more than 70 %) from south Asia at selected sites. Research into the presence and effect of pollutants in the glaciated areas of Pakistan is economically significant because the surface water resources in the country mainly depend on the rivers (the Indus and its tributaries) that flow from this glaciated area.

scholarly journals Development of prognostic aerosol–cloud interactions combining a chemistry transport model and a regional climate model

2015 ◽  
Vol 8 (2) ◽  
pp. 897-933
Author(s):  
M. A. Thomas ◽  
M. Kahnert ◽  
C. Andersson ◽  
H. Kokkola ◽  
U. Hansson ◽  
...  
Keyword(s):  
Radiative Forcing ◽  
Climate Models ◽  
Climate Model ◽  
Transport Model ◽  
Regional Climate ◽  
Cloud Droplet ◽  
Microphysical Properties ◽  
Aerosol Effect ◽  
Aerosol Cloud Interactions ◽  
Set Up

Abstract. To reduce uncertainties and hence, to obtain a better estimate of aerosol (direct and indirect) radiative forcing, next generation climate models aim for a tighter coupling between chemistry transport models and regional climate models and a better representation of aerosol–cloud interactions. In this study, this coupling is done by first forcing the Rossby Center regional climate model, RCA4 by ERA-Interim lateral boundaries (LBCs) and SST using the standard CDNC (cloud droplet number concentration) formulation (hereafter, referred to as the "stand-alone RCA4 version" or "CTRL" simulation). In this simulation, the CDNCs are assigned fixed numbers based on if the underlying surface is land or oceanic. The meteorology from this simulation is then used to drive the chemistry transport model, MATCH which is coupled online with the aerosol dynamics model, SALSA. CDNC fields obtained from MATCH-SALSA are then fed back into a new RCA4 simulation. In this new simulation (referred to as "MOD" simulation), all parameters remain the same as in the first run except for the CDNCs provided by MATCH-SALSA. Simulations are carried out with this model set up for the period 2005–2012 over Europe and the differences in cloud microphysical properties and radiative fluxes as a result of local CDNC changes and possible model responses are analyzed. Our study shows substantial improvements in the cloud microphysical properties with the input of the MATCH-SALSA derived 3-D CDNCs compared to the stand-alone RCA4 version. This model set up improves the spatial, seasonal and vertical distribution of CDNCs with higher concentration observed over central Europe during summer half of the year and over Eastern Europe and Russia during the winter half of the year. Realistic cloud droplet radii (CD radii) values have been simulated with the maxima reaching 13 μm whereas in the stand-alone version, the values reached only 5 μm. A substantial improvement in the distribution of cloud liquid water path was observed when compared to the satellite retrievals from MODIS for the boreal summer months. The median and SD values from the "MOD" simulation are closer to observations than those obtained using the stand-alone RCA4 version. These changes resulted in a significant decrease in the total annual mean net fluxes at the top of the atmosphere (TOA) by −5 W m−2 over the domain selected in the study. The TOA net fluxes from the "MOD" simulation show a better agreement with the retrievals from CERES instrument. The aerosol indirect effects are evaluated based on 1900 emissions. Our simulations estimated the domain averaged annual mean total radiative forcing of −0.64 W m−2 with larger contribution from the first indirect aerosol effect than from the second indirect aerosol effect.

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