scholarly journals Vertical distribution of ozone and VOCs in the low boundary layer of Mexico City

2007 ◽  
Vol 7 (4) ◽  
pp. 12751-12779 ◽  
Author(s):  
E. Velasco ◽  
C. Márquez ◽  
E. Bueno ◽  
R. M. Bernabé ◽  
A. Sánchez ◽  
...  

Abstract. The evolution of ozone and 13 volatile organic compounds (VOCs) in the boundary layer of Mexico City was investigated during 2000–2004 to improve our understanding of the complex interactions between those trace gases and meteorological variables, and their influence on the air quality of a polluted megacity. A tethered balloon, fitted with electrochemical and meteorological sondes, was used to obtain detailed vertical profiles of ozone and meteorological parameters up to 1000 m above ground during part of the diurnal cycle (02:00–18:00 h). VOCs samples were collected up to 200 m by pumping air to canisters with a Teflon tube attached to the tether line. Overall, features of these profiles were found to be consistent with a simple picture of nighttime trapping of ozone in an upper residual layer and of VOCs in a shallow unstable layer above the ground. After sunrise an ozone balance is determined by photochemical production, entrainment from the upper residual layer and destruction by titration with NO, delaying the ground-level ozone rise by 2 h. The subsequent evolution of the conductive boundary layer and vertical distribution of pollutants are discussed in terms of the energy balance, the presence of turbulence and the atmospheric stability.

2008 ◽  
Vol 8 (12) ◽  
pp. 3061-3079 ◽  
Author(s):  
E. Velasco ◽  
C. Márquez ◽  
E. Bueno ◽  
R. M. Bernabé ◽  
A. Sánchez ◽  
...  

Abstract. The evolution of ozone (O3) and 13 volatile organic compounds (VOCs) in the boundary layer of Mexico City was investigated during 2000–2004 to improve our understanding of the complex interactions between those trace gases and meteorological variables, and their influence on the air quality of a polluted megacity. A tethered balloon, fitted with electrochemical and meteorological sondes, was used to obtain detailed vertical profiles of O3 and meteorological parameters up to 1000 m above ground during part of the diurnal cycle (02:00–18:00 h). VOCs samples were collected up to 200 m by pumping air to canisters with a Teflon tube attached to the tether line. Overall, features of these profiles were found to be consistent with the formation of an upper residual layer during nighttime carrying over a fraction of the O3 from the previous day that contributes to the background concentration in surrounding regions. At the same time the release of heat stored in the urban surface forms a shallow unstable layer close to the ground, where the nocturnal emissions are trapped. After sunrise an O3 balance is determined by photochemical production, entrainment from the upper residual layer and destruction by titration with nitric oxide, delaying the ground-level O3 rise by 2 h. The subsequent evolution of the conductive boundary layer and vertical distribution of pollutants are discussed in terms of the energy balance, the presence of turbulence and the atmospheric stability.


2020 ◽  
Author(s):  
Wanyu Zhao ◽  
Hong Ren ◽  
Kimitaka Kawamura ◽  
Huiyun Du ◽  
Xueshun Chen ◽  
...  

Abstract. Vertical distribution of dicarboxylic acids, oxoacids, α-dicarbonyls, and other organic tracer compounds in fine aerosols (PM2.5) was investigated from the ground surface (8 m) to 260 m at a 325-meter meteorological tower in Beijing in the summer of 2015. Results showed that the concentrations of oxalic acid (C2), the predominant diacid, were more abundant at 120 m (210 ± 154 ng m−3) and 260 m (220 ± 140 ng m−3) than those at the ground level (160 ± 90 ng m−3). Concentrations of phthalic acid (Ph) decreased with the increase of heights, demonstrating that the vehicular exhausts at the ground surface was the main contributor. Positive correlations were noteworthy for C2/total diacids with mass ratios of C2 to main oxoacids (Pyr, ωC2) and α-dicarbonyls (Gly, MeGly) in polluted days (0.42 ≤ r2 ≤ 0.65), especially at the ground level. In clean days, the ratios of carbon content in oxalic acid to water soluble organic carbon (C2-C/WSOC) showed larger values at 120 m and 260 m than those at the ground surface. However, in polluted days, the C2-C/WSOC ratio mainly reached its maximum at the ground level. These phenomena may indicate the enhanced contribution of aqueous-phase oxidation to oxalic acid in polluted days. Combined with the influence of wind field, total diacids, oxoacids and α-dicarbonyls decreased by 22 %–58 % under the control on anthropogenic activities during the 2015 Victory Parade period. Furthermore, the PMF results showed that the secondary formation routes (secondary sulfate formation and secondary nitrate formation) were the dominant contributors (37–44 %) to organic acids, followed by biomass burning (25–30 %) and motor vehicles (18–24 %). In this study, the organic acids at the ground level were largely associated with local traffic emissions, while the long-range atmospheric transport followed by photochemical aging contributed more to diacids and related compounds in the boundary layer over Beijing than the ground surface.


2020 ◽  
Vol 20 (11) ◽  
pp. 6435-6453 ◽  
Author(s):  
Shengzhen Zhou ◽  
Luolin Wu ◽  
Junchen Guo ◽  
Weihua Chen ◽  
Xuemei Wang ◽  
...  

Abstract. Many studies have recently been done on understanding the sources and formation mechanisms of atmospheric aerosols at ground level. However, vertical profiles and sources of size-resolved particulate matter within the urban boundary layer are still lacking. In this study, vertical distribution characteristics of size-segregated particles were investigated at three observation platforms (ground level, 118 m, and 488 m) on the 610 m high Canton Tower in Guangzhou, China. Size-segregated aerosol samples were simultaneously collected at the three levels in autumn and winter. Major aerosol components, including water-soluble ions, organic carbon, and elemental carbon, were measured. The results showed that daily average fine-particle concentrations generally decreased with height. Concentrations of sulfate and ammonium in fine particles displayed shallow vertical gradients, and nitrate concentrations increased with height in autumn, while the chemical components showed greater variations in winter than in autumn. The size distributions of sulfate and ammonium in both seasons were characterized by a dominant unimodal mode with peaks in the size range of 0.44–1.0 µm. In autumn, the nitrate size distribution was bimodal, peaking at 0.44–1.0 and 2.5–10 µm, while in winter it was unimodal, implying that the formation mechanisms for nitrate particles were different in the two seasons. Our results suggest that the majority of the sulfate and nitrate is formed from aqueous-phase reactions, and we attribute coarse-mode nitrate formation at the measurement site to the heterogeneous reactions of gaseous nitric acid on existing sea-derived coarse particles in autumn. Case studies further showed that atmospheric aqueous-phase and heterogeneous reactions could be important mechanisms for sulfate and nitrate formation, which, in combination with adverse weather conditions such as temperature inversion and calm wind, led to haze formation during autumn and winter in the Pearl River Delta (PRD) region.


2019 ◽  
Author(s):  
Fanhao Meng ◽  
Min Qin ◽  
Ke Tang ◽  
Jun Duan ◽  
Wu Fang ◽  
...  

Abstract. The production of HONO on aerosol surfaces and ground surfaces in urban atmosphere is of interests. However, ground surface measurement commonly in our society is not able to distinguish these two parts. Here, for the first time, we reported high-resolution vertical profile measurements of HONO and NO2 in urban Beijing at night using an incoherent broadband cavity enhanced absorption spectrometer (IBBCEAS) amounted on a movable container which attached to a meteorological tower of 325 m high. The mixing ratios of HONO during one haze episode (E1), the clean episode (C2) and another haze episode (E3) were 4.26 ± 2.08, 0.83 ± 0.65, and 3.54 ± 0.91 ppb, respectively. High-resolution vertical profiles revealed that the vertical distribution of HONO is consistent with stratification and layering in the nocturnal urban atmosphere below 250 m. Direct emissions from combustion processes contributed 51.1 % to ambient HONO concentration at night. The HONO production from the heterogeneous conversion of NO2 on the aerosol surfaces cannot explain HONO vertical measurements at night, indicating that the heterogeneous reaction of NO2 on ground surfaces dominated the nocturnal HONO production. The nocturnal HONO in the boundary layer is primarily derived from the heterogeneous conversion of NO2 at ground level and direct emissions; it is then transported throughout the column by vertical convection. ϕNO2 → HONO, the HONO yield from deposited NO2, is used to evaluate HONO production from the heterogeneous conversion of NO2 at night. The derived ϕNO2 → HONO values on 9 (C2), 10 (C2) and 11 December (E3) were 0.10, 0.08, and 0.09, respectively, indicating a significant production of HONO from heterogeneous reaction of NO2 at ground level. The similar ϕNO2 → HONO values measured during clean and haze episodes suggest that the heterogeneous conversion potential of NO2 at ground level is consistent at night. Furthermore, the dry deposition loss of HONO to the ground surface and vertical mixing effects associated with convection reached a near steady state at midnight on 11–12 December, indicating that significant quantities of HONO are deposited to the ground surface at night, and the ground surface is the source and sink of HONO at night.


2016 ◽  
Vol 16 (17) ◽  
pp. 10831-10845 ◽  
Author(s):  
Marie Boichu ◽  
Isabelle Chiapello ◽  
Colette Brogniez ◽  
Jean-Christophe Péré ◽  
Francois Thieuleux ◽  
...  

Abstract. The 2014–2015 Holuhraun lava-flood eruption of Bárðarbunga volcano (Iceland) emitted prodigious amounts of sulfur dioxide into the atmosphere. This eruption caused a large-scale episode of air pollution throughout Western Europe in September 2014, the first event of this magnitude recorded in the modern era. We gathered chemistry-transport simulations and a wealth of complementary observations from satellite sensors (OMI, IASI), ground-based remote sensing (lidar, sunphotometry, differential optical absorption spectroscopy) and ground-level air quality monitoring networks to characterize both the spatial-temporal distributions of volcanic SO2 and sulfate aerosols as well as the dynamics of the planetary boundary layer. Time variations of dynamical and microphysical properties of sulfate aerosols in the aged low-tropospheric volcanic cloud, including loading, vertical distribution, size distribution and single scattering albedo, are provided. Retrospective chemistry-transport simulations at low horizontal resolution (25 km  ×  25 km) capture the correct temporal dynamics of this far-range air pollution event but fail to reproduce the correct magnitude of SO2 concentration at ground-level. Simulations at higher spatial resolution, relying on two nested domains with finest resolution of 7.3 km  ×  7.3 km, improve substantially the far-range vertical distribution of the volcanic cloud and subsequently the description of ground-level SO2 concentrations. However, remaining discrepancies between model and observations are shown to result from an inaccurate representation of the planetary boundary layer (PBL) dynamics. Comparison with lidar observations points out a systematic under-estimation of the PBL height by the model, whichever the PBL parameterization scheme. Such a shortcoming impedes the capture of the overlying Bárðarbunga cloud into the PBL at the right time and in sufficient quantities. This study therefore demonstrates the key role played by the PBL dynamics in accurately modelling large-scale volcanogenic air pollution.


2011 ◽  
Vol 11 (12) ◽  
pp. 5719-5744 ◽  
Author(s):  
W. R. Sessions ◽  
H. E. Fuelberg ◽  
R. A. Kahn ◽  
D. M. Winker

Abstract. The Weather Research and Forecasting Model (WRF) is considered a "next generation" mesoscale meteorology model. The inclusion of a chemistry module (WRF-Chem) allows transport simulations of chemical and aerosol species such as those observed during NASA's Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) in 2008. The ARCTAS summer deployment phase during June and July coincided with large boreal wildfires in Saskatchewan and Eastern Russia. One of the most important aspects of simulating wildfire plume transport is the height at which emissions are injected. WRF-Chem contains an integrated one-dimensional plume rise model to determine the appropriate injection layer. The plume rise model accounts for thermal buoyancy associated with fires and local atmospheric stability. This paper describes a case study of a 10 day period during the Spring phase of ARCTAS. It compares results from the plume model against those of two more traditional injection methods: Injecting within the planetary boundary layer, and in a layer 3–5 km above ground level. Fire locations are satellite derived from the GOES Wildfire Automated Biomass Burning Algorithm (WF_ABBA) and the MODIS thermal hotspot detection. Two methods for preprocessing these fire data are compared: The prep_chem_sources method included with WRF-Chem, and the Naval Research Laboratory's Fire Locating and Monitoring of Burning Emissions (FLAMBE). Results from the simulations are compared with satellite-derived products from the AIRS, MISR and CALIOP sensors. When FLAMBE provides input to the 1-D plume rise model, the resulting injection heights exhibit the best agreement with satellite-observed injection heights. The FLAMBE-derived heights are more realistic than those utilizing prep_chem_sources. Conversely, when the planetary boundary layer or the 3–5 km a.g.l. layer were filled with emissions, the resulting injection heights exhibit less agreement with observed plume heights. Results indicate that differences in injection heights produce different transport pathways. These differences are especially pronounced in area of strong vertical wind shear and when the integration period is long.


2015 ◽  
Vol 8 (4) ◽  
pp. 1657-1671 ◽  
Author(s):  
L. Haszpra ◽  
Z. Barcza ◽  
T. Haszpra ◽  
Zs. Pátkai ◽  
K. J. Davis

Abstract. Planetary boundary layer (PBL) CO2 mole fraction data are needed by transport models and carbon budget models as both input and reference for validation. The height of in situ CO2 mole fraction measurements is usually different from that of the model levels where the data are needed; data from short towers, in particular, are difficult to utilize in atmospheric models that do not simulate the surface layer well. Tall-tower CO2 mole fraction measurements observed at heights ranging from 10 to 115 m above ground level at a rural site in Hungary and regular airborne vertical mole fraction profile measurements (136 vertical profiles) above the tower allowed us to estimate how well a tower of a given height could estimate the CO2 mole fraction above the tower in the PBL. The statistical evaluation of the height-dependent bias between the real PBL CO2 mole fraction profile (measured by the aircraft) and the measurement at a given elevation above the ground was performed separately for the summer and winter half years to take into account the different dynamics of the lower troposphere and the different surface CO2 flux in the different seasons. The paper presents (1) how accurately the vertical distribution of CO2 in the PBL can be estimated from the measurements on the top of a tower of height H; (2) how tall of a tower would be needed for the satisfaction of different requirements on the accuracy of the estimation of the CO2 vertical distribution; (3) how accurate of a CO2 vertical distribution estimation can be expected from the existing towers; and (4) how much improvement can be achieved in the accuracy of the estimation of CO2 vertical distribution by applying the virtual tall-tower concept.


2010 ◽  
Vol 10 (1) ◽  
pp. 327-360 ◽  
Author(s):  
B. Wehner ◽  
H. Siebert ◽  
A. Ansmann ◽  
F. Ditas ◽  
P. Seifert ◽  
...  

Abstract. Aerosol particle measurements in the atmospheric boundary layer performed by a helicopter-borne measurement payload and by a lidar system from a case study during the IMPACT field campaign in Cabauw (NL) are presented. Layers of increased number concentrations of ultrafine particles were observed in the residual layer, indicating relatively recent new-particle formation. These layers were characterized by a sub-critical Richardson number and concomitant increased turbulence. Turbulent mixing is likely to lead to local supersaturation of possible precursor gases which are essential for new particle formation. Observed peaks in the number concentrations of ultrafine particles at ground level are connected to the new particle formation in the residual layer by boundary layer development and vertical mixing.


2020 ◽  
Author(s):  
Josipa Milovac ◽  
Klaus Goergen ◽  
Jesus Fernandez ◽  
Kirsten Warrach-Sagi ◽  
Alvaro Lavin-Gullon ◽  
...  

<p>The evaluation of the first of its kind multi-model convection permitting - regional climate model (CP-RCM) ensemble, produced within the framework of the international CORDEX - Flagship Pilot Study on Convective phenomena over the Mediterranean (CORDEX-FPS-CEM), showed the improved spatial representation, frequency and extremes of precipitation compared to coarser resolution counterparts (Ban et al., submitted 2019). It is important, though, to keep in mind that the quality of each of such high resolution simulations strongly depend on the quality of the forcing used to drive the model.</p><p>In this work we investigate the impact of the land-surface forcing on the model representation of land-atmosphere (LA) feedback. For that we used the 2 Weather Research and Forecasting (WRF) settings from the CORDEX-FPS-CEM ensemble to run 4 simulations for 2 seasons (summer and fall), combining 2 sets of data for the land cover (MODIS and CORINE) and the top soil texture (FAO and HWSD). In such a way we generated two ensembles with 8 simulations for each season. Additionally we run 4 simulations with perturbed starting date for the summer season to obtain an additional 5-member ensemble to investigate the impact of the internal variability on the final results.</p><p>The objective of this study is to investigate the model sensitivity to (1) land-surface static forcing, (2) season, and (3) the model configuration. To quantify the strength of LA coupling for each grid, we use coupling metrics appropriate for seasonal time scales. We applied mixing diagram approach to investigate the impact of the land-surface changes on the boundary layer evolution. We also investigate the impact of these changes on the potential for convection triggering, and we calculate correlation matrices to quantify the impact on the strength of the land-atmosphere coupling.</p><p>Preliminary results show evident effects of the land surface changes on surface variables, boundary layer evolution, atmospheric stability and humidity in the lower atmosphere. Strength of the sensitivity to a specific change in the land-surface forcing depend on the model configuration: WRF with less sophisticated parameterization schemes is more sensitive to land use changes, while more sophisticated configuration shows higher sensitivity to the soil texture changes in representing boundary layer evolution. Furthermore, the WRF shows stronger coupling and therefore stronger sensitivity to the land surface changes in the summer season.</p><p>Acknowledgement: This work is partially funded by the Spanish Government R+D programme through grant INSIGNIA (CGL2016-79210-R) co-funded by the ERDF/FEDER.</p><p>References: Ban N., and coauthors: The first multi-model ensemble of regional climate simulations at kilometer-scale resolution, Part I: Evaluation of precipitation, (submitted to Climate Dynamics, 2019)</p>


2010 ◽  
Vol 10 (9) ◽  
pp. 4319-4330 ◽  
Author(s):  
B. Wehner ◽  
H. Siebert ◽  
A. Ansmann ◽  
F. Ditas ◽  
P. Seifert ◽  
...  

Abstract. Aerosol particle measurements in the atmospheric boundary layer performed by a helicopter-borne measurement payload and by a lidar system from a case study during the IMPACT field campaign in Cabauw (NL) are presented. Layers of increased number concentrations of ultrafine particles were observed in the residual layer, indicating relatively recent new-particle formation. These layers were characterized by a sub-critical Richardson number and concomitant increased turbulence. Turbulent mixing is likely to lead to local supersaturation of possible precursor gases which are essential for new particle formation. Observed peaks in the number concentrations of ultrafine particles at ground level are connected to the new particle formation in the residual layer by boundary layer development and vertical mixing.


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