Changes In Aerosol Concentrations Research Articles

Biomass burning aerosol as a modulator of the droplet number in the southeast Atlantic region

Abstract. The southeastern Atlantic (SEA) and its associated cloud deck, off the west coast of central Africa, is an area where aerosol–cloud interactions can have a strong radiative impact. Seasonally, extensive biomass burning (BB) aerosol plumes from southern Africa reach this area. The NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) study focused on quantitatively understanding these interactions and their importance. Here we present measurements of cloud condensation nuclei (CCN) concentration, aerosol size distribution, and characteristic vertical updraft velocity (w∗) in and around the marine boundary layer (MBL) collected by the NASA P-3B aircraft during the August 2017 ORACLES deployment. BB aerosol levels vary considerably but systematically with time; high aerosol concentrations were observed in the MBL (800–1000 cm−3) early on, decreasing midcampaign to concentrations between 500 and 800 cm−3. By late August and early September, relatively clean MBL conditions were sampled (<500 cm−3). These data then drive a state-of-the-art droplet formation parameterization from which the predicted cloud droplet number and its sensitivity to aerosol and dynamical parameters are derived. Droplet closure was achieved to within 20 %. Droplet formation sensitivity to aerosol concentration, w∗, and the hygroscopicity parameter, κ, vary and contribute to the total droplet response in the MBL clouds. When aerosol concentrations exceed ∼900 cm−3 and maximum supersaturation approaches 0.1 %, droplet formation in the MBL enters a velocity-limited droplet activation regime, where the cloud droplet number responds weakly to CCN concentration increases. Below ∼500 cm−3, in a clean MBL, droplet formation is much more sensitive to changes in aerosol concentration than to changes in vertical updraft. In the competitive regime, where the MBL has intermediate pollution (500–800 cm−3), droplet formation becomes much more sensitive to hygroscopicity (κ) variations than it does in clean and polluted conditions. Higher concentrations increase the sensitivity to vertical velocity by more than 10-fold. We also find that characteristic vertical velocity plays a very important role in driving droplet formation in a more polluted MBL regime, in which even a small shift in w∗ may make a significant difference in droplet concentrations. Identifying regimes where droplet number variability is driven primarily by updraft velocity and not by aerosol concentration is key for interpreting aerosol indirect effects, especially with remote sensing. The droplet number responds proportionally to changes in characteristic velocity, offering the possibility of remote sensing of w∗ under velocity-limited conditions.

Aerosol–cloud closure study on cloud optical properties using remotely piloted aircraft measurements during a BACCHUS field campaign in Cyprus

Abstract. In the framework of the EU-FP7 BACCHUS (impact of Biogenic versus Anthropogenic emissions on Clouds and Climate: towards a Holistic UnderStanding) project, an intensive field campaign was performed in Cyprus (March 2015). Remotely piloted aircraft system (RPAS), ground-based instruments, and remote-sensing observations were operating in parallel to provide an integrated characterization of aerosol–cloud interactions. Remotely piloted aircraft (RPA) were equipped with a five-hole probe, pyranometers, pressure, temperature and humidity sensors, and measured vertical wind at cloud base and cloud optical properties of a stratocumulus layer. Ground-based measurements of dry aerosol size distributions and cloud condensation nuclei spectra, and RPA observations of updraft and meteorological state parameters are used here to initialize an aerosol–cloud parcel model (ACPM) and compare the in situ observations of cloud optical properties measured by the RPA to those simulated in the ACPM. Two different cases are studied with the ACPM, including an adiabatic case and an entrainment case, in which the in-cloud temperature profile from RPA is taken into account. Adiabatic ACPM simulation yields cloud droplet number concentrations at cloud base (approximately 400 cm−3) that are similar to those derived from a Hoppel minimum analysis. Cloud optical properties have been inferred using the transmitted fraction of shortwave radiation profile measured by downwelling and upwelling pyranometers mounted on a RPA, and the observed transmitted fraction of solar radiation is then compared to simulations from the ACPM. ACPM simulations and RPA observations shows better agreement when associated with entrainment compared to that of an adiabatic case. The mean difference between observed and adiabatic profiles of transmitted fraction of solar radiation is 0.12, while this difference is only 0.03 between observed and entrainment profiles. A sensitivity calculation is then conducted to quantify the relative impacts of 2-fold changes in aerosol concentration, and updraft to highlight the importance of accounting for the impact of entrainment in deriving cloud optical properties, as well as the ability of RPAs to leverage ground-based observations for studying aerosol–cloud interactions.

Simulation of the responses of rainstorm in the Yangtze River Middle Reaches to changes in anthropogenic aerosol emissions

The model WRF-Chem sensitivity simulation experiments with changing intensity of anthropogenic emissions sources were applied to simulate a rainstorm process in the Yangtze River Middle Reaches (YRMR) during June 18–19, 2018 to study the responses of clouds and precipitation in the rainstorm to changes in aerosol concentrations in this region. The simulation experiments revealed that the aerosol-cloud interaction during low and high emission phases tended to inhibit and to enhance the precipitation process with the precipitation peak lagging 1–2 h. In the later period of rainstorm, high concentrations of aerosols improved precipitation efficiency significantly, resulting in more centralized clusters of intense precipitation. The cloud droplet number concentrations and cloud water contents demonstrated an increasing logarithmic relationship with increasing PM2.5 concentrations. The PM2.5 concentration of about 25 μg/m3 was estimated as the response threshold of cloud droplet number concentrations from sharp to smooth changes. Before and after the peak precipitation, the relationship between the average precipitation rates and PM2.5 concentrations presented an inverse power function. Aerosol-induced precipitation changes were sensitive to ambient relative humidity (RH). When 80% ≤ RH < 85%, the response of precipitation to aerosol emissions was in equilibrium. When RH < 80% or RH > 85% increasing anthropogenic aerosol emissions tended to inhibit or enhance precipitation, especially in the case of low (high) aerosol emissions.

Rapid transition in winter aerosol composition in Beijing from 2014 to 2017: response to clean air actions

Abstract. The clean air actions implemented by the Chinese government in 2013 have led to significantly improved air quality in Beijing. In this work, we combined the in situ measurements of the chemical components of submicron particles (PM1) in Beijing during the winters of 2014 and 2017 and a regional chemical transport model to investigate the impact of clean air actions on aerosol chemistry and quantify the relative contributions of anthropogenic emissions, meteorological conditions, and regional transport to the changes in aerosol chemical composition from 2014 to 2017. We found that the average PM1 concentration in winter in Beijing decreased by 49.5 % from 2014 to 2017 (from 66.2 to 33.4 µg m−3). Sulfate exhibited a much larger decline than nitrate and ammonium, which led to a rapid transition from sulfate-driven to nitrate-driven aerosol pollution during the wintertime. Organic aerosol (OA), especially coal combustion OA, and black carbon also showed large decreasing rates, indicating the effective emission control of coal combustion and biomass burning. The decreased sulfate contribution and increased nitrate fraction were highly consistent with the much faster emission reductions in sulfur dioxide (SO2) due to phasing out coal in Beijing compared to reduction in nitrogen oxides emissions estimated by bottom-up inventory. The chemical transport model simulations with these emission estimates reproduced the relative changes in aerosol composition and suggested that the reduced emissions in Beijing and its surrounding regions played a dominant role. The variations in meteorological conditions and regional transport contributed much less to the changes in aerosol concentration and its chemical composition during 2014–2017 compared to the decreasing emissions. Finally, we speculated that changes in precursor emissions possibly altered the aerosol formation mechanisms based on ambient observations. The observed explosive growth of sulfate at a relative humidity (RH) greater than 50 % in 2014 was delayed to a higher RH of 70 % in 2017, which was likely caused by the suppressed sulfate formation through heterogeneous reactions due to the decrease in SO2 emissions. Thermodynamic simulations showed that the decreased sulfate and nitrate concentrations have lowered the aerosol water content, particle acidity, and ammonium particle fraction. The results in this study demonstrate the response of aerosol chemistry to the stringent clean air actions and identify that the anthropogenic emission reductions are a major driver, which could help to further guide air pollution control strategies in China.

Trends in remote PM2.5 residual mass across the United States: Implications for aerosol mass reconstruction in the IMPROVE network

The Interagency Monitoring of Protected Visual Environments (IMPROVE) network collects aerosol samples for gravimetric and composition analysis in support of the Environmental Protection Agency's Regional Haze Rule and for long-term trend studies and model evaluations. Reconstructing PM2.5 mass or extinction from composition measurements requires assumptions of the molecular form of the individual species assumed to compose the bulk of PM2.5 mass. The IMPROVE reconstruction algorithm includes sulfate as ammonium sulfate, nitrate as ammonium nitrate, organic mass calculated with an assumed organic carbon (OC) to organic mass (OM) multiplier (OM/OC) of 1.8, elemental carbon, fine dust assuming common mineral oxides in soil, and sea salt calculated from chloride. Comparisons of reconstructed fine mass (RCFM) to PM2.5 gravimetric fine mass (FM) provide a check on these assumptions as well as help identify possible biases in gravimetric or speciated measurements. Significant changes in aerosol concentration and composition have occurred over time, leading to decreased FM across the United States. However, within the IMPROVE network, annual mean FM and RCFM have decreased at different rates from 2005 through 2016 (−29% versus −43%, respectively), causing the network median residuals (FM − RCFM) to increase by 0.49 μg m−3 over the 12-year period. The residual shifted from mostly negative before 2011 to mostly positive after 2011, with a strong summer peak. A multiple linear regression analysis indicated that FM biases increased due to the presence of particle-bound water (PBW) after 2011, associated with increased laboratory relative humidity during weighing. Results also suggested that the OM/OC ratio increased across the network after 2011, unrelated to the influence of PBW. While temporal behavior in the OM/OC ratio was similar across the network and for all seasons, values were highest in the East and during summer. Fine dust also appeared to be underestimated by ∼20%. Identifying the source of the trends in the FM residual is essential for accurately estimating contributions by individual species to RCFM and visibility degradation.

Influence of particle concentration and residence time on the efficiency of nanoparticulate collection by electrostatic precipitation

The influence of gas velocity on the efficiency of electrostatic precipitators has previously been discussed exclusively in terms of the gas residence time, even when there are changes in aerosol concentration. Therefore, the aim of this work was to separately evaluate the influences of residence time and concentration by performing sets of experimental tests with KCl nanoparticles in a wire-plate electrostatic precipitator. A proportional increase in the nanoparticles flow rate with increase of the gas stream mitigated dilution effects, allowing exclusive evaluation of the effect of residence time on efficiency.

The response of a simulated mesoscale convective system to increased aerosol pollution: Part II: Derecho characteristics and intensity in response to increased pollution

Mesoscale Convective Systems (MCS) are important contributors to rainfall as well as producers of severe weather such as hail, tornados, and straight-line wind events known as derechos. In this study, different aerosol concentrations and their effects on a derecho event are examined by simulating a case study, the 8 May 2009 “Super-Derecho”, using the Regional Atmospheric Modeling System (RAMS), a cloud-resolving model with sophisticated aerosol and cloud microphysics. Three simulations were conducted that differed in the initial aerosol concentrations, spatial distribution and chemical composition as derived from output of GEOS-Chem, a 3D chemical transport model. In order to understand the impact of changes in aerosol concentrations on the derecho characteristics, the dynamical processes that produced the strong surface wind were determined by performing back-trajectory analysis during two periods of the simulated storm: the development and the onset of dissipation. A time dependent and non-monotonic trend was found between the intensity of the derecho and the increased aerosol concentrations that served as cloud condensation nuclei. During the formation period of the MCS, the non-monotonic trend was attributed to the microphysical impact of aerosol loading on the intensity of the cold pool; that is, the impact of aerosols on both the melting and evaporation rates of hydrometeors. The subsequent intensity changes within the cold pool modified the balance between the horizontal vorticity generated by the cold pool and that of the environment, thereby impacting the orientation of the convective updraft at the leading line. This, in turn, altered the primary flow that contributed to the formation of the derecho-strength surface winds. The simulation with no anthropogenic aerosols exhibited the strongest cold pool and the primary flow was associated with a descending rear inflow jet that produced the derecho winds over a larger region. The simulation with the highest amount of anthropogenic aerosols featured a stronger mesovortex and the derecho winds were primarily due to stronger convective downbursts. As the simulated storm matured, the changes in the derecho winds were found to be associated with the strength of the mesovortex at the gust front. During the period when the simulated storm began to dissipate, the non-monotonic trend in derecho intensity was associated with a non-monotonic response in mesovortex strength to increased aerosol concentrations. A moderate increase in aerosol concentrations led to the formation of a weaker mesovortex while a greater increase in aerosol concentration led to the formation of a stronger mesovortex. The formation of a stronger mesovortex was found to increase the contribution of the derecho winds following a convective downburst associated with an “up-down” downdraft trajectory.

A Study on Parameterization of the Beijing Winter Heavy Haze Events Associated with Height of Pollution Mixing Layer

North China Plain, Beijing, Tianjin, and Hebei province are the major areas facing the decreasing air quality and frequent pollution events in the recent years. Identifying the effect of meteorological conditions on changes in aerosol concentration and the mechanism for forming such heavy pollution in North China Plain has become the focus of scientific research. The influence of atmospheric boundary layer characteristics on air quality has become the focus of attention and research. However, the boundary layer describes that the influences of air pollution have sometimes been duplicated and confused with each other in some of the studies. It is necessary to pay attention to some extent, raising awareness of related pollution mixing layer. The conclusions of the study include the following:(1)The lowered height of pollution mixing layer (H_PML) was favorable for the increase of the PM2.5density. The lowered height of pollution mixing layer had significant impacts on formation of severe haze.(2)A statistical analysis of large-scale heavy pollution cases in eastern China shows that the H_PML parameters have significant contributions.(3)The feedback effect of the high value of the convection inhibition (CIN), which is unfavorable to vertical diffusion of pollution, causes further reduction of H_PML, resulting in cumulative pollution again.

Winter monsoon variability and its impact on aerosol concentrations in East Asia

We investigate the relationship between winter aerosol concentrations over East Asia and variability in the East Asian winter monsoon (EAWM) using GEOS-Chem 3-D global chemical transport model simulations and ground-based aerosol concentration data. We find that both observed and modeled surface aerosol concentrations have strong relationships with the intensity of the EAWM over northern (30–50°N, 100–140°E) and southern (20–30°N, 100–140°E) East Asia. In strong winter monsoon years, compared to weak winter monsoon years, lower and higher surface PM2.5 concentrations by up to 25% are shown over northern and southern East Asia, respectively. Analysis of the simulated results indicates that the southward transport of aerosols is a key process controlling changes in aerosol concentrations over East Asia associated with the EAWM. Variability in the EAWM is found to play a major role in interannual variations in aerosol concentrations; consequently, changes in the EAWM will be important for understanding future changes in wintertime air quality over East Asia.

Implications of RCP emissions on future PM2.5 air quality and direct radiative forcing over China

AbstractSevere PM2.5 air pollution in China and the First Grand National Standard (FGNS), implemented in 2016 (annual PM2.5 concentration target of less than 35 µg m−3), necessitate urgent reduction strategies. This study applied the nested‐grid version of the Goddard Earth Observing System (GEOS) chemical transport model (GEOS‐Chem) to quantify 2000–2050 changes in PM2.5 air quality and related direct radiative forcing (DRF) in China, based on future emission changes under the representative concentration pathway (RCP) scenarios of RCP2.6, RCP4.5, RCP6.0, and RCP8.5. In the near term (2000–2030), a projected maximum increase in PM2.5 concentrations of 10–15 µg m−3 is found over east China under RCP6.0 and RCP8.5 and less than 5 µg m−3 under RCP2.6 and RCP4.5. In the long term (2000–2050), PM2.5 pollution clearly improves, and the largest decrease in PM2.5 concentrations of 15–30 µg m−3 is over east China under all RCPs except RCP6.0. Focusing particularly on highly polluted regions, we find that Beijing‐Tianjin‐Hebei (BTH) wintertime PM2.5 concentrations meeting the FGNS occur after 2040 under RCP2.6, RCP4.5, and RCP8.5, and summertime PM2.5 concentrations reach this goal by 2030 under RCP2.6 and RCP4.5. In Sichuan Basin (SCB), wintertime PM2.5 concentrations below the FGNS occur only in 2050 under RCP2.6 and RCP4.5, although future summertime PM2.5 will be well controlled. The difficulty in controlling future PM2.5 concentrations relates to unmitigated high levels of nitrate, although NOx and SO2 emissions show substantial reductions during 2020–2040. The changes in aerosol concentrations lead to positive aerosol DRF over east China (20°–45°N, 100°–125°E) by 1.22, 1.88, and 0.66 W m−2 in 2050 relative to 2000 under RCP2.6, RCP4.5, and RCP8.5, respectively. When considering both health and climate effects of PM2.5 over China, for example, PM2.5 concentrations averaged over east China under RCP4.5 (RCP2.6) decrease by 54% (43%) in 2050 relative to 2000, but at the cost of warming with DRF of 1.88 (1.22) W m−2. Our results indicate that it will be possible to mitigate future PM2.5 pollution in China, but it will likely take two decades for polluted regions such as BTH and SCB to meet the FGNS, based on all RCP scenarios. At the same time, the consequent warming effects from reduced aerosols are also significant and inevitable.

Impact of meteorology on fine aerosols at Lucas Heights, Australia

Ion Beam Analysis (IBA) techniques were used to assign nine years of PM2.5 observations to seven source types, at Lucas Heights, a topographically complex urban fringe site of Sydney. The highest contributions to total PM2.5 were from motor vehicles (Autos, 26.3%), secondary sulfur (2ndryS, 23.7%), a mixture of industry and aged sea air (IndSaged, 20.6%), and smoke (Smoke, 13.7%). The Autos contribution was highest in winter, whereas 2ndryS was highest in summer, indicating that mitigation measures targeting SO2 release in summer and vehicle exhaust in winter would be most effective in reducing the PM2.5 concentrations at this site. Since concentrations of particulate matter can be significantly affected by local meteorology, generalised additive model (GAM) techniques were employed to investigate relationships between PM2.5 source types and meteorological conditions. The GAM predictors used included: time (seasonal to inter-annual variations), mixing layer depth, temperature, relative humidity, wind speed, wind direction, and atmospheric pressure. Meteorological influences on PM2.5 variability were found to be 58% for soil dust, 46% for Autos, 41% for total PM2.5, and 35% for 2ndryS. Effects were much smaller for other source types. Temperature was found to be an important variable for the determination of total PM2.5, 2ndryS, IndSaged, Soil and Smoke, indicating that future changes in temperature are likely to have an associated change in aerosol concentrations. However, the impact on different source types varied. Temperature had the highest impact on 2ndryS (sometimes more than a factor of 4 increase for temperatures above 25 °C compared to temperatures under 10 °C) and IndSaged, being predominantly secondary aerosols formed in the atmosphere from precursors, whereas wind speed and wind direction were more important for the determination of vehicle exhaust and fresh sea salt concentrations. The marginal effect of relative humidity on 2ndryS increased up to relative humidity of 70–80% and then plateaued, confirming previous findings that (NH4)2SO4 is present in the solid phase below relative humidity of about 80%.

Interannual variation of springtime biomass burning in Indochina: Regional differences, associated atmospheric dynamical changes, and downwind impacts.

During March and April, widespread burning occurs across farmlands in Indochina in preparation for planting at the monsoon onset. The resultant aerosols impact the air quality downwind. In this study, we investigate the climatic aspect of the interannual variation of springtime biomass burning in Indochina and its correlation with air quality at Mt. Lulin in Taiwan using long‐term (2005–2015) satellite and global reanalysis data. Based on empirical orthogonal function (EOF) analysis, we find that the biomass burning activities vary with two geographical regions: northern Indochina (the primary EOF mode) and southern Indochina (the secondary EOF mode). We determine that the variation of biomass burning over northern Indochina is significantly related with the change in aerosol concentrations at Mt. Lulin. This occurs following the change in the so‐called India‐Burma Trough in the lower and middle troposphere. When the India‐Burma Trough is intensified, a stronger northwesterly wind (to the west of the trough) transports the dryer air from higher latitude into northern Indochina, and this promotes local biomass burning activities. The increase in upward motion to the east of the intensified India‐Burma Trough lifts the aerosols, which are transported toward Taiwan by the increased low‐level westerly jet. Further diagnoses revealed the connection between the India‐Burma Trough and the South Asian jet's wave train pattern as well as the previous winter's El Niño–Southern Oscillation phase. This information highlights the role of the India‐Burma Trough in modulating northern Indochina biomass burning and possibly predicting aerosol transport to East Asia on the interannual time scale.

Characterization of cumulus cloud fields using trajectories in the center of gravity versus water mass phase space: 2. Aerosol effects on warm convective clouds

AbstractIn Part I of this work a 3‐D cloud tracking algorithm and phase space of center of gravity altitude versus cloud liquid water mass (CvM space) were introduced and described in detail. We showed how new physical insight can be gained by following cloud trajectories in the CvM space. Here this approach is used to investigate aerosol effects on cloud fields of warm cumuli. We show a clear effect of the aerosol loading on the shape and size of CvM clusters. We also find fundamental differences in the CvM space between simulations using bin versus bulk microphysical schemes, with the bin scheme precipitation expressing much higher sensitivity to changes in aerosol concentrations. Using the bin microphysical scheme, we find that the increase in cloud center of gravity altitude with increase in aerosol concentrations occurs for a wide range of cloud sizes. This is attributed to reduced sedimentation, increased buoyancy and vertical velocities, and increased environmental instability, all of which are tightly coupled to inhibition of precipitation processes and subsequent feedbacks of clouds on their environment. Many of the physical processes shown here are consistent with processes typically associated with cloud invigoration.

Meteorological and Aerosol Effects on Marine Stratocumulus

Abstract This study investigates the effects of meteorological conditions and aerosols on marine stratocumulus in the southeastern Pacific using the Weather Research and Forecasting (WRF) Model. Two regimes with different temperature and moisture conditions in the finest model domain are investigated. The western regime is around 87°–79°W, while the eastern regime is around 79°–71°W. In both regimes, cloud fraction, liquid water path (LWP), cloud thickness, and precipitation show significant diurnal cycles. Cloud fraction can be 0.83 during the night and down to 0.29 during the day in the western regime. The diurnal cycles in the eastern regime have smaller amplitudes but are still very strong. Stratocumulus properties also differ in the two regimes. Compared to the western regime, the eastern regime has lower temperature, higher relative humidity, and a more coupled boundary layer, leading to higher cloud fraction (by 0.11) and lower cloud-base height. The eastern regime also has lower inversion height that causes lower cloud-top height and thinner clouds and, hence, lower LWP and less precipitation. Cloud microphysical properties are very sensitive to aerosols in both regimes. Increasing aerosols greatly increase cloud number concentration, decrease cloud effective radius, and suppress precipitation. Cloud macrophysical properties (cloud fraction, LWP) are not sensitive to aerosols in either regime, most notably in the eastern regime where precipitation amount is less. The changes in cloud fraction and LWP caused by changes in aerosol concentrations are smaller than the changes in the diurnal cycle and the spatial variability between the two regimes.

Effect of Aerosols on Freezing Drops, Hail, and Precipitation in a Midlatitude Storm

Abstract A midlatitude hail storm was simulated using a new version of the spectral bin microphysics Hebrew University Cloud Model (HUCM) with a detailed description of time-dependent melting and freezing. In addition to size distributions of drops, plate-, columnar-, and branch-type ice crystals, snow, graupel, and hail, new distributions for freezing drops as well as for liquid water mass within precipitating ice particles were implemented to describe time-dependent freezing and wet growth of hail, graupel, and freezing drops. Simulations carried out using different aerosol loadings show that an increase in aerosol loading leads to a decrease in the total mass of hail but also to a substantial increase in the maximum size of hailstones. Cumulative rain strongly increases with an increase in aerosol concentration from 100 to about 1000 cm−3. At higher cloud condensation nuclei (CCN) concentrations, the sensitivity of hailstones’ size and surface precipitation to aerosols decreases. The physical mechanism of these effects was analyzed. It was shown that the change in aerosol concentration leads to a change in the major mechanisms of hail formation and growth. The main effect of the increase in the aerosol concentration is the increase in the supercooled cloud water content. Accordingly, at high aerosol concentration, the hail grows largely by accretion of cloud droplets in the course of recycling in the cloud updraft zone. The main mechanism of hail formation in the case of low aerosol concentration is freezing of raindrops.

Global and regional climate impacts of future aerosol mitigation in an RCP6.0-like scenario in EC-Earth

Future changes in aerosol concentrations will influence the climate system over the coming decades. In this study we evaluate the equilibrium climate response to aerosol reductions in different parts of the world in 2050, using the global climate model EC-Earth. The aerosol concentrations are based on a set of scenarios similar to RCP6.0, developed using the IMAGE integrated assessment model and exploring stringent and weaker air pollution control. Reductions in aerosol concentrations lead to an increase in downward surface solar radiation under all-sky conditions in various parts of the world, especially in Asia where the local brightening may reach about 10 Wm−2. The associated increase in surface temperature may be as high as 0.5 °C. This signal is dominated by the reduced cooling effect of sulphate which in some areas is partially compensated by the decreased warming effect of black carbon. According to our simulations, the mitigation of BC may lead to decreases in mean summer surface temperature of up to 1 °C in central parts of North America and up to 0.3 °C in northern India. Aerosol reductions could significantly affect the climate at high latitudes especially in the winter, where temperature increases of up to 1 °C are simulated. In the Northern Hemisphere, this strong surface temperature response might be related to changes in circulation patterns and precipitation at low latitudes, which can give rise to a wave train and induce changes in weather patterns at high latitudes. Our model does not include a parameterization of aerosol indirect effects so that responses could be stronger in reality. We conclude that different, but plausible, air pollution control policies can have substantial local climate effects and induce remote responses through dynamic teleconnections.

Extensive closed cell marine stratocumulus downwind of Europe—A large aerosol cloud mediated radiative effect or forcing?

AbstractMarine stratocumulus clouds (MSC) cover large areas over the oceans and possess super sensitivity of their cloud radiative effect to changes in aerosol concentrations. Aerosols can cause transitions between regimes of fully cloudy closed cells and open cells. The possible role of aerosols in cloud cover has a big impact on the amount of reflected solar radiation from the clouds, thus potentially constitutes very large aerosol indirect radiative effect, which can exceed 100 Wm−2. It is hypothesized that continentally polluted clouds remain in closed cells regime for longer time from leaving continent and hence for longer distance away from land, thus occupying larger ocean areas with full cloud cover. Attributing this to anthropogenic aerosols would imply a very large negative radiative forcing with a significant climate impact. This possibility is confirmed by analyzing a detailed case study based on geostationary and polar‐orbiting satellite observations of the microphysical and dynamical evolution of MSC. We show that large area of closed cells was formed over the northeast Atlantic Ocean downwind of Europe in a continentally polluted air mass. The closed cells undergo cleansing process that was tracked for 3.5 days that resulted with a rapid transition from closed to open cells once the clouds started drizzling heavily. The mechanism leading to the eventual breakup of the clouds due to both meteorological and aerosol considerations is elucidated. We termed this cleansing and cloud breakup process maritimization. Further study is needed to assess the climatological significance of such situations.

Satellite-based estimate of global aerosol–cloud radiative forcing by marine warm clouds

Changes in aerosol concentrations affect cloud albedo and Earth’s radiative balance. Aerosol radiative forcing from pre-industrial time to the present due to the effect of atmospheric aerosol levels on the micro- and macrophysics of clouds bears the largest uncertainty among external influences on climate change. Of all cloud forms, low-level marine clouds exert the largest impact on the planet’s albedo. For example, a 6% increase in the albedo of global marine stratiform clouds could offset the warming that would result from a doubling of atmospheric CO_2 concentrations. Marine warm cloud properties are thought to depend on aerosol levels and large-scale dynamic or thermodynamic states. Here we present a comprehensive analysis of multiple measurements from the A-Train constellation of Earth-observing satellites, to quantify the radiative forcing exerted by aerosols interacting with marine clouds. Specifically, we analyse observations of co-located aerosols and clouds over the world’s oceans for the period August 2006–April 2011, comprising over 7.3 million CloudSat single-layer marine warm cloud pixels. We find that thermodynamic conditions—that is, tropospheric stability and humidity in the free troposphere—and the state of precipitation act together to govern the cloud liquid water responses to the presence of aerosols and the strength of aerosol–cloud radiative forcing.

A permanent Raman lidar station in the Amazon: description, characterization, and first results

Abstract. A permanent UV Raman lidar station, designed to perform continuous measurements of aerosols and water vapor and aiming to study and monitor the atmosphere from weather to climatic time scales, became operational in the central Amazon in July 2011. The automated data acquisition and internet monitoring enabled extended hours of daily measurements when compared to a manually operated instrument. This paper gives a technical description of the system, presents its experimental characterization and the algorithms used for obtaining the aerosol optical properties and identifying the cloud layers. Data from one week of measurements during the dry season of 2011 were analyzed as a mean to assess the overall system capability and performance. Both Klett and Raman inversions were successfully applied. A comparison of the aerosol optical depth from the lidar and from a co-located Aerosol Robotic Network (AERONET) sun photometer showed a correlation coefficient of 0.86. By combining nighttime measurements of the aerosol lidar ratio (50–65 sr), back-trajectory calculations and fire spots observed from satellites, we showed that observed particles originated from biomass burning. Cirrus clouds were observed in 60% of our measurements. Most of the time they were distributed into three layers between 11.5 and 13.4 km a.g.l. The systematic and long-term measurements being made by this new scientific facility have the potential to significantly improve our understanding of the climatic implications of the anthropogenic changes in aerosol concentrations over the pristine Amazonia.

The signal of aerosol‐induced changes in sunshine duration records: A review of the evidence

AbstractAerosols play a significant yet complex and central role in the Earth's radiation budget, and knowledge of long‐term changes in the atmospheric turbidity induced by aerosols is therefore fundamental for a better understanding of climate change. However, there is little available information on changes in aerosol concentration in the atmosphere, especially prior to the 1980s. The present paper reviews publications reporting the suitability of sunshine duration records with regard to detecting changes in atmospheric aerosols. Some of the studies reviewed propose methods for estimating aerosol‐related magnitudes, such as turbidity, from sunshine deficit at approximately sunrise and sunset, when the impact of aerosols on the solar beam is more easily observed. In addition, there is abundant evidence that one cause of the decadal changes observed in sunshine duration records involves variations in atmospheric aerosol loading. Possible directions for future research are also suggested: in particular, detailed studies of the burn (not only its length but also its width) registered by means of Campbell‐Stokes sunshine recorders may provide a way of creating time series of atmospheric aerosol loading metrics dating back to over 120 years from the present.