Ozone and PAN Formation Inside and Outside of the Berlin Plume — Process Analysis and Numerical Process Simulation

Corsmeier, U.; Kalthoff, Norbert; Vogel, Bernhard; Hammer, Maria; Fiedler, F.; Kottmeier, C.; Volz‐Thomas, A.; Konrad, S.; Glaser, K.; Neininger, B.; Lehning, M.; Jaeschke, W.; Memmesheimer, M.; Rappenglück, Bernhard; Jakobi, Gert

doi:10.1007/978-94-010-0399-5_13

Cited by 23 publications

(34 citation statements)

References 35 publications

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“…Since the model system KAMM/DRAIS has been described in detail in previous papers Hammer et al, 2002) and has been extensively validated against observations in the past Nester et al, 1995;Fiedler et al, 2000;Corsmeier et al, 2002;Hammer et al, 2002) we only give a short summary with the focus on the aerosol model MADEsoot (Riemer et al, 2003b).…”

Section: Model Descriptionmentioning

confidence: 99%

Soot aging time scales in polluted regions during day and night

Riemer

Vogel²,

Vogel³

2004

Atmos. Chem. Phys.

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171

184

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Abstract. The aging of soot is one of the key uncertainties in the estimation of both the direct and indirect climate effect. While freshly emitted soot is initially hydrophobic and externally mixed, it can be transferred into an internal mixture by coagulation, condensation or photochemical processes. These aging processes affect the hygroscopic qualities and hence the growth behaviour, the optical properties and eventually the lifetime of the soot particles. However, due to computational limits the aging of soot in global climate models is often only parameterised by an estimated turnover rate resulting in a lifetime of soot of several days. Hence, the aging process of soot is one of the key uncertainties governing the burden and effect of black carbon. In this study, we discuss the time scale on which diesel soot is transferred from an external to an internal mixture based on the results of our simulations with a comprehensive mesoscale model. For daytime conditions during summer condensation of sulphuric acid is dominant and the aging process occurs on a time scale of τ =8 h close to the sources and τ =2 h above the source region. During winter comparable time scales are found but ammonium nitrate becomes more important. During night time condensation is not effective. Then coagulation is the most important aging process and our results show time scales between 10 h and 40 h.

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Section: Model Descriptionmentioning

confidence: 99%

Soot aging time scales in polluted regions during day and night

Riemer

Vogel²,

Vogel³

2004

Atmos. Chem. Phys.

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171

184

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“…All important trace gases (NO x , NO y , O 3 , biogenic/anthropogenic VOC's, etc.) and meteorological parameters (temperature, wind direction, wind speed and relative humidity) were monitored by various groups at this station (Becker, 2001;Corsmeier et al, 2002;Volz-Thomas et al, 2001. Measurements of hydrogen peroxide, organic peroxides, carbonyl compounds, and organic acids at Pabstthum over a period of the whole BERLIOZ campaign are discussed by Grossmann et al (2001).…”

Section: Introductionmentioning

confidence: 99%

Hydrogen Peroxide, Organic Peroxides and Higher Carbonyl Compounds Determined during the BERLIOZ Campaign

Moortgat

Grossmann

Boddenberg

et al. 2002

Tropospheric Chemistry

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Abstract. Gas-phase H 2 O 2 , organic peroxides and carbonyl compounds were determined at various sites from Mid-July to early August 1998 during the BERLIOZ campaign in Germany. The sites were located northwest of Berlin and were chosen to determine pollutants downwind of the city emissions during a summer smog episode. Hydrogen peroxide (H 2 O 2 ), methyl hydroperoxide (MHP, CH 3 OOH) and occasionally hydroxymethyl hydroperoxide (HMHP, HOCH 2 OOH) were quantified in air samples by commercial fluorimetric methods and classical HPLC with post-column derivatisation by horseradish peroxidase/p-hydroxyphenyl acetic acid and fluorimetric detection. Carbonyl compounds were determined in ambient air by a novel method based on O-pentafluorobenzyl hydroxylamine as derivatisation agent. Mixing ratio profiles of the hydroperoxides and the carbonyl compounds are reported for the intensive phase of the campaign, 20-21 July, 1998. Peroxides showed pronounced diurnal variations with peak mixing ratios in the early afternoon. At times, a second maximum was observed in the late afternoon. The major part of the H 2 O 2 was formed through recombination reactions of HO 2 radicals, but there is some evidence that H 2 O 2 is also formed from ozonolysis of anthropogenic and/or biogenic alkenes. Diurnal variations of mixing ratios of various carbonyl compounds are reported: alkanals (C 2 to C 10 , isobutanal), unsaturated carbonyl compounds (methacrolein, methylvinylketone, acrolein), hydroxycarbonyl (glycolaldehyde, hydroxyacetone) and dicarbonyl compounds (glyoxal, methylglyoxal, biacetyl), aromatic compounds (benzaldehyde, o-and m-tolylaldehyde) and pinonaldehyde.

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“…During the afternoon hours, the net production rates are nearly the same in the regions 1 and 2, whereas the rate is obviously lower in region 3. During the afternoon the ozone net production in the urban plume reaches a level of about 6.5±1.0 ppb/h, as derived from aircraft measurements on the downwind side of the city (Corsmeier et al, 2002). The aircraft flew at different levels in the lower mixing layer (layer 3 in our mass balance calculations), and it crossed regions 2 and 3 several times.…”

Section: Simulationsmentioning

confidence: 63%

“…The grid size for this simulation was 18 km. Only the ozone profile at the upper levels (1.5-5 km) was modified in line with the measurements carried out by the IBUF aircraft (Corsmeier et al, 2002). The emission data for this episode were provided by IER, Stuttgart.…”

Section: Simulationsmentioning

confidence: 99%

Sensitivity analysis by the adjoint chemistry transport model DRAISfor an episode in the Berlin Ozone (BERLIOZ) experiment

Nester¹,

Panitz²

2006

Atmos. Chem. Phys.

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Abstract. The Berlin Ozone Experiment (BERLIOZ) was carried out in summer 1998. One of its purposes was the evaluation of Chemistry Transport Models (CTM). CTM KAMM/DRAIS was one of the models considered. The data of 20 July were selected for evaluation. On that day, a pronounced ozone plume developed downwind of the city. Evaluation showed that the KAMM/DRAIS model is able to reproduce the meteorological and ozone data observed, except at farther distances (60-80 km) downwind of the city. In that region, the DRAIS model underestimates the measured ozone concentrations by 10-15 ppb, approximately.Therefore, this study was conducted to detect possible reasons for this deviation. A comprehensive sensitivity analysis was carried out to determine the most relevant model parameters. The adjoint DRAIS model was developed for this purpose, because for this study the application of this model is the most effective method of calculating the sensitivities. The least squares of the measured and simulated ozone concentrations between 08:00 UTC and 16:00 UTC at two stations 30 km and 70 km downwind of the city centre were chosen as distance function. The model parameters considered in this study are the complete set of initial and boundary species concentrations, emissions, and reaction rates, respectively. A sensitivity ranking showing the relevance of the individual parameters in the set is determined for each parameter set.In order to find out which modification in the parameter sets most reduces the cost function, simplified 4-D data assimilation was carried out. The result of this data assimilation shows that modifications of the reaction rates provide the best agreement between the measured and the simulated ozone concentrations at both stations. However, the modified reaction rates seem to be unrealistic for the whole simulation period. Therefore, the good agreement should not be overesCorrespondence to: H.-J. Panitz (panitz@imk.fzk.de) timated. The agreement is still acceptable when the parameters in the other sets are modified together. The investigation demonstrates that an analysis of this type can help to explain inconsistencies between observations and simulations. But in the case considered here the inconsistencies cannot be explained by an error in only one parameter set.

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Ozone and PAN Formation Inside and Outside of the Berlin Plume — Process Analysis and Numerical Process Simulation

Abstract: found in previous studies. The low PAN formation on 20 July, was mainly restricted by the moderate nonmethane hydrocarbon levels, whereas high PAN concentrations of 3.0 ppb on 21 July, are caused by local production in the boundary layer and by large scale advection aloft.

Cited by 23 publications

References 35 publications

Soot aging time scales in polluted regions during day and night

Soot aging time scales in polluted regions during day and night

Hydrogen Peroxide, Organic Peroxides and Higher Carbonyl Compounds Determined during the BERLIOZ Campaign

Sensitivity analysis by the adjoint chemistry transport model DRAISfor an episode in the Berlin Ozone (BERLIOZ) experiment

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