scholarly journals Aerosol ageing in an urban plume – implications for climate and health

2010 ◽  
Vol 10 (8) ◽  
pp. 18731-18780 ◽  
Author(s):  
P. Roldin ◽  
E. Swietlicki ◽  
A. Massling ◽  
A. Kristensson ◽  
J. Löndahl ◽  
...  

Abstract. The climate and health effects downwind of an urban area resulting from gaseous and particulate emissions within the city are as yet inadequately quantified. The aim of this work was to estimate these effects for Malmö city in Southern Sweden (population 280 000). The chemical and physical particle properties were simulated with a model for Aerosol Dynamics, gas phase CHEMistry and radiative transfer calculations (ADCHEM) following the trajectory movement from upwind Malmö, through the urban background environment and finally tens and hundreds of kilometers downwind Malmö. The model results were validated with measurements of the particle number size distribution and chemical composition. The total particle number concentration 50 km (~3 h) downwind in the center of the Malmö plume is about 3800 cm−3 and the Malmö contribution is roughly 35%. Condensation of nitric acid, ammonium and to a smaller extent oxidized organic compounds formed from the emissions in Malmö increases the secondary aerosol formation with a maximum of 0.6–0.7 μg/m3 6 to 18 h downwind of Malmö. The secondary mass contribution dominates over the primary soot contribution from Malmö already 2 to 3 h after the emissions and gives an enhanced total top of the atmosphere direct or indirect aerosol shortwave radiative forcing in the center of the urban plume ranging from −0.3 to −2.3 W m−2 depending on the distance from Malmö, and the cloud properties. It also gives an increased respiratory tract deposited mass dose, which increases with the distance downwind Malmö.

2011 ◽  
Vol 11 (12) ◽  
pp. 5897-5915 ◽  
Author(s):  
P. Roldin ◽  
E. Swietlicki ◽  
A. Massling ◽  
A. Kristensson ◽  
J. Löndahl ◽  
...  

Abstract. The climate effects downwind of an urban area resulting from gaseous and particulate emissions within the city are as yet inadequately quantified. The aim of this work was to estimate these effects for Malmö city in southern Sweden (population 280 000). The chemical and physical particle properties were simulated with a model for Aerosol Dynamics, gas phase CHEMistry and radiative transfer calculations (ADCHEM) following the trajectory movement from upwind of Malmö, through the urban background environment and finally tens and hundreds of kilometers downwind of Malmö. The model results were evaluated using measurements of the particle number size distribution and chemical composition. The total particle number concentration 50 km (~ 3 h) downwind, in the center of the Malmö plume, is about 3700 cm−3 of which the Malmö contribution is roughly 30%. Condensation of nitric acid, ammonium and to a smaller extent oxidized organic compounds formed from the emissions in Malmö increases the secondary aerosol formation with a maximum of 0.7–0.8 μg m−3 6 to 18 h downwind of Malmö. The secondary mass contribution dominates over the primary soot contribution from Malmö already 3 to 4 h downwind of the emission sources and contributes to an enhanced total surface direct or indirect aerosol shortwave radiative forcing in the center of the urban plume ranging from −0.3 to −3.3 W m−2 depending on the distance from Malmö, and the specific cloud properties.


2014 ◽  
Vol 14 (6) ◽  
pp. 3083-3093 ◽  
Author(s):  
M. Fiebig ◽  
D. Hirdman ◽  
C. R. Lunder ◽  
J. A. Ogren ◽  
S. Solberg ◽  
...  

Abstract. This article investigates the annual cycle observed in the Antarctic baseline aerosol scattering coefficient, total particle number concentration, and particle number size distribution (PNSD), as measured at Troll Atmospheric Observatory. Mie theory shows that the annual cycles in microphysical and optical aerosol properties have a common cause. By comparison with observations at other Antarctic stations, it is shown that the annual cycle is not a local phenomenon, but common to central Antarctic baseline air masses. Observations of ground-level ozone at Troll as well as backward plume calculations for the air masses arriving at Troll demonstrate that the baseline air masses originate from the free troposphere and lower stratosphere region, and descend over the central Antarctic continent. The Antarctic summer PNSD is dominated by particles with diameters <100 nm recently formed from the gas-phase despite the absence of external sources of condensible gases. The total particle volume in Antarctic baseline aerosol is linearly correlated with the integral insolation the aerosol received on its transport pathway, and the photooxidative production of particle volume is mostly limited by photooxidative capacity, not availability of aerosol precursor gases. The photooxidative particle volume formation rate in central Antarctic baseline air is quantified to 207 ± 4 μm3/(MJ m). Further research is proposed to investigate the applicability of this number to other atmospheric reservoirs, and to use the observed annual cycle in Antarctic baseline aerosol properties as a benchmark for the representation of natural atmospheric aerosol processes in climate models.


2021 ◽  
Author(s):  
Matthias Karl ◽  
Liisa Pirjola ◽  
Tiia Grönholm ◽  
Mona Kurppa ◽  
Srinivasan Anand ◽  
...  

Abstract. Numerical models are needed for evaluating aerosol processes in the atmosphere in state-of-the-art chemical transport models, urban-scale dispersion models and climatic models. This article describes a publicly available aerosol dynamics model MAFOR (Multicomponent Aerosol FORmation model; version 2.0); we address the main structure of the model, including the types of operation and the treatments of the aerosol processes. The main advantage of MAFOR v2.0 is the consistent treatment of both the mass- and number-based concentrations of particulate matter. An evaluation of the model is also presented, against a high-resolution observational dataset in a street canyon located in the centre of Helsinki (Finland) during an afternoon traffic rush hour on 13 December 2010. The experimental data included measurements at different locations in the street canyon of ultrafine particles, black carbon, and fine particulate mass PM1. This evaluation has also included an intercomparison with the corresponding predictions of two other prominent aerosol dynamics models, AEROFOR and SALSA. All three models fairly well simulated the decrease of the measured total particle number concentrations with increasing distance from the vehicular emission source. The MAFOR model reproduced the evolution of the observed particle number size distributions more accurately than the other two models. The MAFOR model also predicted the variation of the concentration of PM1 better than the SALSA model. We also analysed the relative importance of various aerosol processes based on the predictions of the three models. As expected, atmospheric dilution dominated over other processes; dry deposition was the second most significant process. Numerical sensitivity tests with the MAFOR model revealed that the uncertainties associated with the properties of the condensing organic vapours affected only the size range of particles smaller than 10 nm in diameter. These uncertainties do not therefore affect significantly the predictions of the whole of the number size distribution and the total number concentration. The MAFOR model version 2 is well documented and versatile to use, providing a range of alternative parametrizations for various aerosol processes. The model includes an efficient numerical integration of particle number and mass concentrations, an operator-splitting of processes, and the use of a fixed sectional method. The model could be used as a module in various atmospheric and climatic models.


2019 ◽  
Author(s):  
Rebecca Jackson ◽  
Albert Gabric ◽  
Roger Cropp ◽  
Matthew Woodhouse

Abstract. Coral reefs are being threatened by global climate change, with ocean warming and acidification, compounded by declining water quality in many coastal systems, adversely affecting coral health and cover. This is of great concern as coral reefs provide numerous ecosystem, economic and social services. Corals are also recognized as being amongst the strongest individual sources of natural atmospheric sulfur, through stress-induced emissions of dimethylsulfide (DMS). In the clean marine boundary layer, biogenic sulfates contribute to new aerosol formation and the growth of existing particles, with important implications for the radiative balance. Evidence suggests that DMS is not only directly involved in the coral stress response, alleviating oxidative stress, but may create an ocean thermostat which suppresses sea surface temperature (SST) through changes to aerosol and cloud properties. This review provides a summary of the current major threats facing coral reefs and describes the role of dimethylated sulfur compounds in coral physiology and climate. The role of coral reefs as a source of climatically important compounds is an emerging topic of research however, the window of opportunity to understand the complex biogeophysical processes involved is closing with ongoing degradation of the world's coral reefs. The greatest uncertainty in our estimates of radiative forcing and climate change are derived from natural aerosol sources, such as marine DMS, which constitutes the largest flux of oceanic reduced sulfur to the atmosphere. Gaining a better understanding of the role of coral reef DMS emissions is crucial to predicting the future climate of our planet.


2010 ◽  
Vol 10 (4) ◽  
pp. 8553-8594 ◽  
Author(s):  
F. Wang ◽  
P. Roldin ◽  
A. Massling ◽  
A. Kristensson ◽  
E. Swietlicki ◽  
...  

Abstract. Aerosol particles in the submicrometer size range (PM1) have serious impacts on human health and climate. This work aims at studying the processes relevant for physical particle properties in and downwind Copenhagen and evaluating the capability of a detailed aerosol dynamics and chemistry model (ADCHEM) to describe the submicrometer aerosol dynamics in a complex urbanized region, subjected to a variety of important anthropogenic sources. The study area is the Oresund Region with Copenhagen (about 1.8 million people) as the major city, including the strait separating Denmark and Sweden with intense ship traffic. Modeled aerosol particle number size distributions and NOx concentrations are evaluated against ground-based measurements from two stations in the Copenhagen area in Denmark and one station in southern Sweden. The measured and modeled increments in NOx concentrations from rural background to the urban area showed satisfactory agreement, indicating that the estimated NOx emissions and modeled atmospheric dispersion are reasonable. For three out of five case studies, the modeled particle number concentrations and size distributions are in satisfactory agreement with the measurements at all stations along the trajectories. For the remaining cases the model significantly underestimates the particle number concentration over Copenhagen, but reaches acceptable agreement with the measurements at the downwind background station in Sweden. The major causes for this were identified as being the lack of spatial resolution in the meteorological data in describing boundary layer mixing heights and the uncertainty in the exact air mass trajectory path over Copenhagen. In addition, particle emission factors may also have been too low. It was shown that aerosol dynamics play a minor role from upwind to urban background, but are important 1–2 h downwind the city. Real-world size-resolved traffic number emission factors which take into account the initial ageing in the street canyon can be used to model traffic emissions in urban plume studies.


2012 ◽  
Vol 12 (5) ◽  
pp. 2399-2408 ◽  
Author(s):  
F. Yu ◽  
G. Luo ◽  
R. P. Turco ◽  
J. A. Ogren ◽  
R. M. Yantosca

Abstract. New particle formation contributes significantly to the number concentration of condensation nuclei (CN) as well as cloud CN (CCN), a key factor determining aerosol indirect radiative forcing of the climate system. Using a physics-based nucleation mechanism that is consistent with a range of field observations of aerosol formation, it is shown that projected increases in global temperatures could significantly inhibit new particle, and CCN, formation rates worldwide. An analysis of CN concentrations observed at four NOAA ESRL/GMD baseline stations since the 1970s and two other sites since 1990s reveals long-term decreasing trends that are consistent in sign with, but are larger in magnitude than, the predicted temperature effects. The possible reasons for larger observed long-term CN reductions at remote sites are discussed. The combined effects of rising temperatures on aerosol nucleation rates and other chemical and microphysical processes may imply substantial decreases in future tropospheric particle abundances associated with global warming, delineating a potentially significant feedback mechanism that increases Earth's climate sensitivity to greenhouse gas emissions. Further research is needed to quantify the magnitude of such a feedback process.


2011 ◽  
Vol 11 (10) ◽  
pp. 27913-27936
Author(s):  
F. Yu ◽  
G. Luo ◽  
R. P. Turco ◽  
J. A. Ogren ◽  
R. M. Yantosca

Abstract. New particle formation contributes significantly to the number concentration of condensation nuclei (CN) as well as cloud CN (CCN), a key factor determining aerosol indirect radiative forcing of the climate system. Using a physics-based nucleation mechanism that is consistent with a range of field observations of aerosol formation, it is shown that projected increases in global temperatures could significantly inhibit new particle, and CCN, formation rates worldwide. An analysis of CN concentrations observed at four NOAA ESRL/GMD baseline stations since the 1970s and two other sites since 1990s reveals long-term decreasing trends consistent with these predictions. The analysis also suggests, owing to larger observed CN reductions at remote sites than can be explained by the basic nucleation mechanism, that dimethylsulphide (DMS) emissions may be decreasing worldwide with increasing global temperatures, implying a positive DMS-based cloud feedback forcing of the climate ("CLAW"). The combined effects of rising temperatures on aerosol nucleation rates, and possibly on DMS emissions, may imply substantial decreases in future tropospheric particle abundances associated with global warming, delineating a potentially significant feedback mechanism that increases Earth's climate sensitivity to greenhouse gas emissions. Further research is needed to quantify the magnitude of such a feedback process.


2014 ◽  
Vol 14 (20) ◽  
pp. 27973-28018 ◽  
Author(s):  
L. Liao ◽  
M. Dal Maso ◽  
D. Mogensen ◽  
P. Roldin ◽  
A. Rusanen ◽  
...  

Abstract. We used the MALTE-BOX model including near-explicit air chemistry and detailed aerosol dynamics to study the mechanisms of observed new particle formation events in the Jülich Plant Atmosphere Chamber. The modelled and measured H2SO4 (sulfuric acid) concentrations agreed within a factor of two. The modelled total monoterpene concentration was in line with PTR-MS observations, and we provided the distributions of individual isomers of terpenes, when no measurements were available. The aerosol dynamic results supported the hypothesis that H2SO4 is one of the critical compounds in the nucleation process. However, compared to kinetic H2SO4 nucleation, nucleation involving OH oxidation products of monoterpenes showed a better agreement with the measurements, with R2 up to 0.97 between modelled and measured total particle number concentrations. The nucleation coefficient for kinetic H2SO4 nucleation was 2.1 × 10−11 cm3 s−1, while the organic nucleation coefficient was 9.0 × 10−14 cm3 s−1. We classified the VOC oxidation products into two sub-groups including extremely low-volatility organic compounds (ELVOCs) and semi-volatile organic compounds (SVOCs). These ELVOCs and SVOCs contributed approximately equally to the particle volume production, whereas only ELVOCs made the smallest particles to grow in size. The model simulations revealed that the chamber walls constitute a major net sink of SVOCs on the first experiment day. However, the net wall SVOC uptake was gradually reduced because of SVOC desorption during the following days. Thus, in order to capture the observed temporal evolution of the particle number size distribution, the model needs to consider reversible gas-wall partitioning.


2013 ◽  
Vol 13 (9) ◽  
pp. 23057-23088
Author(s):  
M. Fiebig ◽  
D. Hirdman ◽  
C. R. Lunder ◽  
J. A. Ogren ◽  
S. Solberg ◽  
...  

Abstract. This article investigates the annual cycle observed in the Antarctic baseline aerosol scattering coefficient, total particle number concentration, and particle number size distribution (PNSD) as measured at Troll Atmospheric Observatory. Mie-theory shows that the annual cycles in microphysical and optical aerosol properties have a common cause. By comparison with observations at other Antarctic stations, it is shown that the annual cycle is not a local phenomenon, but common to Central Antarctic baseline air masses. Observations of ground-level ozone at Troll as well as backward plume calculations for the air masses arriving at Troll demonstrate that the baseline air masses originate from the free troposphere and lower stratosphere region, and descend over the Central Antarctic continent. The Antarctic summer PNSD is dominated by particles with diameters < 100 nm recently formed from the gas-phase despite the absence of external sources of condensible gases. The total particle volume in Antarctic baseline aerosol is linearly correlated with the integral insolation the aerosol received on its transport pathway, and the photooxidative production of particle volume is mostly limited by photooxidative capacity, not availability of aerosol precursor gases. The photooxidative particle volume formation rate in Central Antarctic baseline air is quantified to 207 ± 4 μm3/(MJ m). Further research is proposed to investigate the applicability of this number to other atmospheric reservoirs, and to use the observed annual cycle in Antarctic baseline aerosol properties as a benchmark for the representation of natural atmospheric aerosol processes in climate models.


Atmosphere ◽  
2021 ◽  
Vol 12 (3) ◽  
pp. 352
Author(s):  
Adelaide Dinoi ◽  
Daniel Gulli ◽  
Ivano Ammoscato ◽  
Claudia R. Calidonna ◽  
Daniele Contini

During the new coronavirus infection outbreak, the application of strict containment measures entailed a decrease in most human activities, with the consequent reduction of anthropogenic emissions into the atmosphere. In this study, the impact of lockdown on atmospheric particle number concentrations and size distributions is investigated in two different sites of Southern Italy: Lecce and Lamezia Terme, regional stations of the GAW/ACTRIS networks. The effects of restrictions are quantified by comparing submicron particle concentrations, in the size range from 10 nm to 800 nm, measured during the lockdown period and in the same period of previous years, from 2015 to 2019, considering three time intervals: prelockdown, lockdown and postlockdown. Different percentage reductions in total particle number concentrations are observed, −19% and −23% in Lecce and −7% and −4% in Lamezia Terme during lockdown and postlockdown, respectively, with several variations in each subclass of particles. From the comparison, no significant variations of meteorological factors are observed except a reduction of rainfall in 2020, which might explain the higher levels of particle concentrations measured during prelockdown at both stations. In general, the results demonstrate an improvement of air quality, more conspicuous in Lecce than in Lamezia Terme, during the lockdown, with a differed reduction in the concentration of submicronic particles that depends on the different types of sources, their distance from observational sites and local meteorology.


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