scholarly journals Physical and chemical properties of the regional mixed layer of Mexico's Megapolis Part II: evaluation of measured and modeled trace gases and particle size distributions

2012 ◽  
Vol 12 (21) ◽  
pp. 10161-10179 ◽  
Author(s):  
C. Ochoa ◽  
D. Baumgardner ◽  
M. Grutter ◽  
J. Allan ◽  
J. Fast ◽  
...  

Abstract. This study extends the work of Baumgardner et al. (2009) in which measurements of trace gases and particles, at a remote, high altitude mountain site, 60 km from Mexico City were analyzed with respect to the origin of the air masses. In the current evaluation, the temperature, water vapor mixing ratio (WMR), ozone (O3), carbon monoxide (CO), sulfur dioxide (SO2) and acyl peroxy nitrate (APN) are simulated with the WRF-Chem chemical transport model and compared with the measurements at the mountain site. Comparisons between the model and measurements are also evaluated for particle size distributions (PSDs) of the mass concentrations of sulfate, nitrate, ammonium and organic mass (OM). The model predictions of the diurnal trends in temperature, WMR and trace gases were generally well correlated; 13 of the 18 correlations were significant at a confidence level of <0.01. Less satisfactory were the average hourly differences between model and measurements that showed predicted values within expected, natural variation for only 10 of the 18 comparisons. The model performed best when comparing with the measurements during periods when the air originated from the east. In that case all six of the parameters being compared had average differences between the model and measurements less than the expected standard deviation. For the cases when the air masses are from the southwest or west northwest, only two of the comparisons from each case showed differences less than the expected standard deviation. The differences appear to be a result of an overly rapid growth of the boundary layer predicted by the model and too much dilution. There also is more O3 being produced, most likely by photochemical production, downwind of the emission sources than is predicted by the model. The measured and modeled PSD compare very well with respect to their general shape and the diameter of the peak concentrations. The spectra are log normally distributed with most of the mass in the accumulation mode centered at 200 ± 20 nm and little observed or predicted changes with respect to the time when the RML is above the Altzomoni research station. Only the total mass changes with time and air mass origin. The invariability of average diameter of the accumulation mode suggests that there is very little growth of the particles by condensation or coagulation after six hours of aging downwind of the major sources of anthropogenic emissions in Mexico's Megapolis. This could greatly simplify parameterization in climate models although it is not known at this time if this invariance can be extended to other megacity regions.

2012 ◽  
Vol 12 (4) ◽  
pp. 9813-9856
Author(s):  
C. Ochoa ◽  
D. Baumgardner ◽  
M. Grutter ◽  
J. Allan ◽  
J. Fast ◽  
...  

Abstract. This study extends the work of Baumgardner et al. (2009) in which measurements of trace gases and particles, at a remote, high altitude mountain site, 60 km from Mexico City were analyzed with respect to the origin of the air masses. In the current evaluation, the temperature, water vapor, ozone (O3), carbon monoxide (CO), acyl peroxy nitrate (APN) and particle size distributions (PSDs) of the mass concentrations of sulfate, nitrate, ammonium and organic mass (OM) were simulated with the WRF-Chem chemical transport model and compared with the measurements at the mountain site. The model predictions of the diurnal trends of the gases were well correlated with the measurements before the regional mixed layer (RML) reached the measurement site but underestimated the concentration after that time. The differences are caused by an over rapid growth of the boundary layer by the model and too much dilution. There also is more O3 being actually produced by photochemical production downwind of the emission sources than predicted by the model. The measured and modeled PSDs compare very well with respect to their general shape and diameter of the peak concentrations. The spectra are lognormal with most of the mass in the accumulation mode and the geometric diameter centered at 200±20 nm, showing little observed or predicted change with respect to the time when the RML is above the Altzomoni research station. Only the total mass changed with time and air mass origin. The invariability of average diameter of the accumulation mode suggests that there is very little growth of the particles by condensation or coagulation past about six hours of aging downwind of the major sources of anthropogenic emissions in Mexico's Megapolis. This could greatly simplify parameterization in climate models although it is not known at this time if this invariance can be extended to other megacity regions.


2008 ◽  
Vol 8 (22) ◽  
pp. 6729-6738 ◽  
Author(s):  
N. Kalivitis ◽  
W. Birmili ◽  
M. Stock ◽  
B. Wehner ◽  
A. Massling ◽  
...  

Abstract. Atmospheric particle size distributions were measured on Crete island, Greece in the Eastern Mediterranean during an intensive field campaign between 28 August and 20 October, 2005. Our instrumentation combined a differential mobility particle sizer (DMPS) and an aerodynamic particle sizer (APS) and measured number size distributions in the size range 0.018 μm–10 μm. Four time periods with distinct aerosol characteristics were discriminated, two corresponding to marine and polluted air masses, respectively. In marine air, the sub-μm size distributions showed two particle modes centered at 67 nm and 195 nm having total number concentrations between 900 and 2000 cm−3. In polluted air masses, the size distributions were mainly unimodal with a mode typically centered at 140 nm, with number concentrations varying between 1800 and 2900 cm−3. Super-μm particles showed number concentrations in the range from 0.01 to 2.5 cm−3 without any clear relation to air mass origin. A small number of short-lived particle nucleation events were recorded, where the calculated particle formation rates ranged between 1.1–1.7 cm−3 s−1. However, no particle nucleation and growth events comparable to those typical for the continental boundary layer were observed. Particles concentrations (Diameter <50 nm) were low compared to continental boundary layer conditions with an average concentration of 300 cm−3. The production of sulfuric acid and its subsequently condensation on preexisting particles was examined with the use of a simplistic box model. These calculations suggested that the day-time evolution of the Aitken particle population was governed mainly by coagulation and that particle formation was absent during most days.


2008 ◽  
Vol 8 (2) ◽  
pp. 6571-6601
Author(s):  
N. Kalivitis ◽  
W. Birmili ◽  
M. Stock ◽  
B. Wehner ◽  
A. Massling ◽  
...  

Abstract. Atmospheric particle size distributions were measured on Crete island, Greece in the Eastern Mediterranean during an intensive field campaign between 28 August and 20 October 2005. Our instrumentation combined a differential mobility particle sizer (DMPS) and an aerodynamic particle sizer (APS) and measured number size distributions in the size range 0.018 μm–10 μm. Four time periods with distinct aerosol characteristics were discriminated, two corresponding to marine and polluted air masses, respectively. In marine air, the sub-μm size distributions showed two particle modes centered at 67 nm and 195 nm having total number concentrations between 900 and 2000 cm−3. In polluted air masses, the size distributions were mainly unimodal with a mode typically centered at 140 nm, with number concentrations varying between 1800 and 2900 cm−3. Super-μm particles showed number concentrations in the range from 0.01 to 2.5 cm−3 without any clear relation to air mass origin. A small number of short-lived particle nucleation events were recorded, where the calculated particle formation rates ranged between 1.1–1.7 cm−3 s−1. However, no particle nucleation and growth events comparable to those typical for the continental boundary layer were observed. Particles concentrations (Diameter <50 nm) were low compared to continental boundary layer conditions with an average concentration of 300 cm−3. The production of sulfuric acid and its subsequently condensation on preexisting particles was examined with the use of a simplistic box model. These calculations suggested that the day-time evolution of the Aitken particle population was governed mainly by coagulation and that particle formation was absent during most days.


2017 ◽  
Vol 17 (22) ◽  
pp. 13605-13624 ◽  
Author(s):  
Berto Paul Lee ◽  
Hao Wang ◽  
Chak Keung Chan

Abstract. Mass-concentration-based particle size distributions measured by a high-resolution aerosol mass spectrometer were systematically analyzed to assess long and short-term temporal characteristics of ambient particle size distributions sampled at a typical urban environment close to emission sources and a suburban coastal site representing a regional and local pollution receptor location in Hong Kong. Measured distributions were bimodal and deconvoluted into submodes, which were analyzed for day-to-day variations and diurnal variations. Traffic and cooking emissions at the urban site contributed substantially to particle mass in both modes, while notable decreases in mass median diameters were limited to the morning rush hour. Inorganic particle components displayed varying diurnal behavior, including nocturnal nitrate formation and daytime photochemical formation evident in both modes. Suburban particle size distributions exhibited notable seasonal disparities with differing influence of local formation, particularly in spring and summer, and transport which dominated in the fall season leading to notably higher sulfate and organic accumulation-mode particle concentrations. Variations in particle mixing state were evaluated by comparison of interspecies mass median diameter trends at both measurement sites. Internal mixing was prevalent in the accumulation mode in spring at the urban site, while greater frequency of time periods with external mixing of particle populations comprising different fractions of organic constituents was observed in summer. At the suburban site, sulfate and nitrate in the accumulation mode more frequently exhibited differing particle size distributions in all seasons, signifying a greater extent of external mixing. At the urban site, periods of greater submicron inorganic mass concentrations were more likely to be caused by increases in both Aitken- and accumulation-mode particle mass in summer, while at the suburban receptor location, organic and nitrate Aitken-mode particle mass contributed more regularly to higher total submicron species mass concentrations in most seasons (spring, summer, and winter).


2016 ◽  
Author(s):  
Daniel Neumann ◽  
Volker Matthias ◽  
Johannes Bieser ◽  
Armin Aulinger ◽  
Markus Quante

Abstract. Atmospheric sea salt particles affect chemical and physical processes in the atmosphere. They provide surface area for condensation and reaction of nitrogen, sulfur, and organic species and are a vehicle of transport for these species. Additionally, HCl is released from sea salt. Hence, sea salt has a relevant impact on air quality, particularly in coastal regions with high anthropogenic emissions such as in the North Sea region. Therefore, the integration of sea salt emissions in modeling studies in these regions is necessary. However, it was found that sea salt concentrations are not represented with necessary accuracy in some situations. In this study, three sea salt emission parameterizations depending on different combinations of wind speed, salinity, sea surface temperature, and wave data were implemented and compared: GO03 (Gong, 2003), SP13 (Spada et al., 2013), and OV14 (Ovadnevaite et al., 2014). The aim is to improve modeled atmospheric sea salt concentrations by identifying the parameterization that predicts the sea salt PM10 mass concentrations at different distances to the source regions most accurately and that represents atmospheric sea salt particle size distributions most appropriately in the region under consideration. While the GO03 emissions yielded overestimations in the PM10 concentrations at coastal stations and underestimations of those at inland stations, OV14 emissions, vice versa, led to underestimations at coastal stations and overestimations at inland stations. Because of differently shaped particle size distributions of the GO03 and OV14 emission cases, the deposition velocity of the coarse particles differs between both cases which yields this distinct behavior at inland and coast stations. PM10 concentrations produced by the SP13 emissions generally overestimated measured concentrations. With respect to the size distribution, OV14 produced most accurate coarse particle concentrations, whereas GO03 produced most accurate fine particle concentrations. Overall, GO03 and OV14 produced most accurate results, but both parameterizations still reveal weaknesses in some situations.


1993 ◽  
Vol 115 (3) ◽  
pp. 523-526 ◽  
Author(s):  
J. R. Ferguson ◽  
D. E. Stock

A method is presented to estimate the effects of a polydisperse particle size distribution on the measured turbulent dispersion of particles. In addition, the analysis provides a means to estimate the standard deviation of the size distribution for which a class of particles may be considered monodisperse. If monodisperse particles are unavailable because of practical considerations (e.g., the required standard deviation of particle size is too small to obtain a sufficient quantity) then the method provides a means to correct the data of near monodisperse size distributions to reflect the dispersion of monodisperse particles.


2014 ◽  
Vol 14 (8) ◽  
pp. 4327-4348 ◽  
Author(s):  
D. C. S. Beddows ◽  
M. Dall'Osto ◽  
R. M. Harrison ◽  
M. Kulmala ◽  
A. Asmi ◽  
...  

Abstract. Cluster~analysis of particle number size distributions from~background sites across Europe~is presented. This generated a total of nine clusters of particle size distributions which could be further combined into two main groups, namely: a south-to-north category (four clusters) and a west-to-east category (five clusters). The first group was identified as most frequently being detected inside and around northern Germany and neighbouring countries, showing clear evidence of local afternoon nucleation and growth events that could be linked to movement of air masses from south to north arriving ultimately at the Arctic contributing to Arctic haze.~The second group of particle size spectra proved to have narrower size distributions and collectively showed a dependence of modal diameter upon the longitude of the site (west to east) at which they were most frequently detected.~These clusters indicated regional nucleation (at the coastal sites) growing to larger modes further inland. The apparent growth rate of the modal diameter was around 0.6–0.9 nm h−1. Four specific air mass back-trajectories were successively taken as case studies to examine in real time the evolution of aerosol size distributions across Europe. ~While aerosol growth processes can be observed as aerosol traverses Europe, the processes are often obscured by the addition of aerosol by emissions en route. This study revealed that some of the 24 stations exhibit more complex behaviour than others, especially when impacted by local sources or a variety of different air masses. Overall, the aerosol size distribution clustering analysis greatly simplifies the complex data set and allows a description of aerosol aging processes, which reflects the longer-term average development of particle number size distributions as air masses advect across Europe.


2008 ◽  
Vol 35 (1) ◽  
pp. 67-79 ◽  
Author(s):  
Shawn Clark ◽  
John Doering

The counter-rotating flume at the University of Manitoba was used to conduct a series of 21 laboratory experiments to investigate the effects of turbulence intensity on frazil ice formation and evolution. A detailed study of the velocity and turbulence intensity distributions within the counter-rotating flume was initially conducted using a constant-temperature anemometer equipped with a one-dimensional conical hot-film probe. Five levels of turbulence intensity were generated by five different sets of bed plates and flume wall rotation rates in order to study how turbulence affected the frazil particle size distributions and the statistics related to clear disk-shaped particles. It was found that a lognormal distribution could not be rejected when describing the frazil particle size distributions, regardless of the turbulence intensity of the water. The variation of the mean and standard deviation of particle diameter with turbulence intensity are well described by a parabolic shape. A preliminary equation to describe the variation of the mean and standard deviation of particle diameter as a function of turbulence intensity and time is presented.


2017 ◽  
Author(s):  
Berto P. Lee ◽  
Hao Wang ◽  
Chak K. Chan

Abstract. Mass concentration based particle size distributions measured by a high-resolution aerosol mass spectrometer were systematically analyzed to assess long and short-term temporal characteristics of ambient particle size distributions sampled at a typical urban environment close to emission sources and a suburban coastal site representing a regional and local pollution receptor location in Hong Kong. Measured distributions were bimodal and deconvoluted into submodes which were analyzed for day-to-day variations and diurnal variations. Traffic and cooking emissions at the urban site contributed substantially to particle mass in both modes, while notable decreases in mass median diameters were limited to the morning rush hour. Inorganic particle components displayed varying diurnal behavior, including nocturnal nitrate formation and daytime photochemical formation evident in both modes. Suburban particle size distributions exhibited notable seasonal disparities with differing influence of local formation, particularly in spring and summer, and transport which dominated in the fall season leading to notably higher sulfate and organic accumulation mode particle concentrations. Variations in particle mixing state were evaluated by comparison of inter-species mass median diameter trends at both measurement sites. Internal mixing was prevalent in the accumulation mode in spring at the urban site, while greater frequency of time periods with external mixing of particle populations comprising different fractions of organic constituents was observed in summer. At the suburban site, sulfate and nitrate in the accumulation mode more frequently exhibited differing particle size distributions in all seasons signifying a greater extent of external mixing. At the urban site, periods of greater submicron inorganic mass concentrations were more likely to be caused by increases in both Aitken and accumulation mode particle mass in summer, while at the suburban receptor location organic and nitrate Aitken mode particle mass contributed more regularly to higher total submicron species mass concentrations in most seasons (spring, summer and winter).


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