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Sökning: WFRF:(Hallquist Mattias)

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31.
  • Emanuelsson, Eva U., et al. (författare)
  • Formation of anthropogenic secondary organic aerosol (SOA) and its influence on biogenic SOA properties
  • 2012
  • Ingår i: Atmospheric Chemistry and Physics Discussions. - : Copernicus Publications. - 1680-7367 .- 1680-7375. ; 12:8, s. 20311-20350
  • Tidskriftsartikel (refereegranskat)abstract
    • Secondary organic aerosol (SOA) formation from mixed anthropogenic and biogenic precursors has been studied exposing reaction mixtures to natural sunlight in the SAPHIR chamber in Jülich, Germany. Several experiments with exclusively anthro- 5 pogenic precursors were performed to establish a relationship between yield and organic aerosol mass loading for the atmospheric relevant range of aerosol loads of 0.01 to 10 μgm−3. The yields (0.5–9 %) were comparable to previous data and further used for the detailed evaluation of the mixed biogenic and anthropogenic experiments. For the mixed experiments a number of different oxidation schemes were addressed. The 10 reactivity, the sequence of addition, and the amount of the precursors influenced the SOA properties. Monoterpene oxidation products, including carboxylic acids and dimer esters were identified in the aged aerosol at levels comparable to ambient air. OH radicals were measured by Laser Induced Fluorescence, which allowed for establishing relations of aerosol properties and composition to the experimental OH dose. Further 15 more, the OH measurements in combination with the derived yields for anthropogenic SOA enabled application of a simplified model to calculate the chemical turnover of the anthropogenic precursor and corresponding anthropogenic contribution to the mixed aerosol. The estimated anthropogenic contributions were ranging from small (8 %) up to significant fraction (>50 %) providing a suitable range to study the effect of aerosol 20 composition on the aerosol volatility (volume fraction remaining at 343 K: 0.86–0.94). The anthropogenic aerosol had higher oxygen to carbon ratio O/C and was less volatile than the biogenic fraction. However, in order to produce significant amount of anthropogenic SOA the reaction mixtures needed a higher OH dose that also increased O/C and provided a less volatile aerosol. A strong positive correlation was found between 25 changes in volatility and O/C with the exception during dark hours where the SOA volatility decreased while O/C did not change significantly. This change in volatility under dark conditions is likely due to chemical or morphological changes not affecting O/C.
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32.
  • Emanuelsson, Eva U., et al. (författare)
  • Formation of anthropogenic secondary organic aerosol (SOA) and its influence on biogenic SOA properties
  • 2013
  • Ingår i: Atmos. Chem. Phys.. - : Copernicus Publications. - 1680-7324. ; 13:5, s. 2837-2855
  • Tidskriftsartikel (refereegranskat)abstract
    • Secondary organic aerosol (SOA) formation from mixed anthropogenic and biogenic precursors has been studied exposing reaction mixtures to natural sunlight in the SAPHIR chamber in Jülich, Germany. In this study aromatic compounds served as examples of anthropogenic volatile organic compound (VOC) and a mixture of α-pinene and limonene as an example for biogenic VOC. Several experiments with exclusively aromatic precursors were performed to establish a relationship between yield and organic aerosol mass loading for the atmospheric relevant range of aerosol loads of 0.01 to 10 μg m−3. The yields (0.5 to 9%) were comparable to previous data and further used for the detailed evaluation of the mixed biogenic and anthropogenic experiments. For the mixed experiments a number of different oxidation schemes were addressed. The reactivity, the sequence of addition, and the amount of the precursors influenced the SOA properties. Monoterpene oxidation products, including carboxylic acids and dimer esters were identified in the aged aerosol at levels comparable to ambient air. OH radicals were measured by Laser Induced Fluorescence, which allowed for establishing relations of aerosol properties and composition to the experimental OH dose. Furthermore, the OH measurements in combination with the derived yields for aromatic SOA enabled application of a simplified model to calculate the chemical turnover of the aromatic precursor and corresponding anthropogenic contribution to the mixed aerosol. The estimated anthropogenic contributions were ranging from small (≈8%) up to significant fraction (>50%) providing a suitable range to study the effect of aerosol composition on the aerosol volatility (volume fraction remaining (VFR) at 343 K: 0.86–0.94). The aromatic aerosol had higher oxygen to carbon ratio O/C and was less volatile than the biogenic fraction. However, in order to produce significant amount of aromatic SOA the reaction mixtures needed a higher OH dose that also increased O/C and provided a less volatile aerosol. The SOA yields, O/C, and f44 (the mass fraction of CO2+ ions in the mass spectra which can be considered as a measure of carboxylic groups) in the mixed photo-chemical experiments could be described as linear combinations of the corresponding properties of the pure systems. For VFR there was in addition an enhancement effect, making the mixed aerosol significantly less volatile than what could be predicted from the pure systems. A strong positive correlation was found between changes in volatility and O/C with the exception during dark hours where the SOA volatility decreased while O/C did not change significantly. Thus, this change in volatility under dark conditions as well as the anthropogenic enhancement is due to chemical or morphological changes not affecting O/C.
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33.
  • Emanuelsson, Eva U., et al. (författare)
  • Influence of Humidity, Temperature, and Radicals on the Formation and Thermal Properties of Secondary Organic Aerosol (SOA) from Ozonolysis of β-Pinene
  • 2013
  • Ingår i: Journal of Physical Chemistry A. - : American Chemical Society (ACS). - 1089-5639 .- 1520-5215. ; 117:40, s. 10346 - 10358
  • Tidskriftsartikel (refereegranskat)abstract
    • The influence of water and radicals on SOAs produced by β-pinene ozonolysis was investigated at 298 and 288 K using a laminar flow reactor. A volatility tandem differential mobility analyzer (VTDMA) was used to measure the evaporation of the SOA, enabling the parametrization of its volatility properties. The parameters extracted included the temperature at which 50% of the aerosol had evaporated (TVFR0.5) and the slope factor (SVFR). An increase in SVFR indicates a broader distribution of vapor pressures for the aerosol constituents. Reducing the reaction temperature increased SVFR and decreased TVFR0.5 under humid conditions but had less effect on TVFR0.5 under dry conditions. In general, higher water concentrations gave lower TVFR0.5 values, more negative SVFR values, and a reduction in total SOA production. The radical conditions were changed by introducing OH scavengers to generate systems with and without OH radicals and with different [HO2]/[RO2] ratios. The presence of a scavenger and lower [HO2]/[RO2] ratio reduced SOA production. Observed changes in SVFR values could be linked to the more complex chemistry that occurs in the absence of a scavenger and indicated that additional HO2 chemistry gives products with a wider range of vapor pressures. Updates to existing ozonolysis mechanisms with routes that describe the observed responses to water and radical conditions for monoterpenes with endocyclic and exocyclic double bonds are discussed.
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36.
  • Faxon, Cameron, et al. (författare)
  • Characterization of organic nitrate constituents of secondary organic aerosol (SOA) from nitrate-radical-initiated oxidation of limonene using high-resolution chemical ionization mass spectrometry
  • 2018
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 18, s. 5467-5481
  • Tidskriftsartikel (refereegranskat)abstract
    • The gas-phase nitrate radical (NO 3 • ) initiated oxidation of limonene can produce organic nitrate species with varying physical properties. Low-volatility products can contribute to secondary organic aerosol (SOA) formation and organic nitrates may serve as a NO x reservoir, which could be especially important in regions with high biogenic emissions. This work presents the measurement results from flow reactor studies on the reaction of NO 3 • with limonene using a High-Resolution Time-of-Flight Chemical Ionization Mass Spectrometer (HR-ToF-CIMS) combined with a Filter Inlet for Gases and AEROsols (FIGAERO). Major condensed-phase species were compared to those in the Master Chemical Mechanism (MCM) limonene mechanism, and many non-listed species were identified. The volatility properties of the most prevalent organic nitrates in the produced SOA were determined. Analysis of multiple experiments resulted in the identification of several dominant species (including C 10 H 15 NO 6 , C 10 H 17 NO 6 , C 8 H 11 NO 6 , C 10 H 17 NO 7 , and C 9 H 13 NO 7 ) that occurred in the SOA under all conditions considered. Additionally, the formation of dimers was consistently observed and these species resided almost completely in the particle phase. The identities of these species are discussed, and formation mechanisms are proposed. Cluster analysis of the desorption temperatures corresponding to the analyzed particle-phase species yielded at least five distinct groupings based on a combination of molecular weight and desorption profile. Overall, the results indicate that the oxidation of limonene by NO 3 • produces a complex mixture of highly oxygenated monomer and dimer products that contribute to SOA formation.
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37.
  • Flores, J. M., et al. (författare)
  • Evolution of the complex refractive index in the UV spectral region in ageing secondary organic aerosol
  • 2014
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 14:11, s. 5793-5806
  • Tidskriftsartikel (refereegranskat)abstract
    • The chemical and physical properties of secondary organic aerosol (SOA) formed by the photochemical degradation of biogenic and anthropogenic volatile organic compounds (VOC) are as yet still poorly constrained. The evolution of the complex refractive index (RI) of SOA, formed from purely biogenic VOC and mixtures of biogenic and anthropogenic VOC, was studied over a diurnal cycle in the SAPHIR photochemical outdoor chamber in Julich, Germany. The correlation of RI with SOA chemical and physical properties such as oxidation level and volatility was examined. The RI was retrieved by a newly developed broadband cavity-enhanced spectrometer for aerosol optical extinction measurements in the UV spectral region (360 to 420 nm). Chemical composition and volatility of the particles were monitored by a high-resolution time-of-flight aerosol mass spectrometer, and a volatility tandem differential mobility analyzer. SOA was formed by ozonolysis of either (i) a mixture of biogenic VOC (alpha-pinene and limonene), (ii) biogenic VOC mixture with subsequent addition of an anthropogenic VOC (p-xylene-d(10)), or (iii) a mixture of biogenic and anthropogenic VOC. The SOA aged by ozone/OH reactions up to 29.5 h was found to be non-absorbing in all cases. The SOA with p-xylene-d(10) showed an increase of the scattering component of the RI correlated with an increase of the O / C ratio and with an increase in the SOA density. There was a greater increase in the scattering component of the RI when the SOA was produced from the mixture of biogenic VOCs and anthropogenic VOC than from the sequential addition of the VOCs after approximately the same ageing time. The increase of the scattering component was inversely correlated with the SOA volatility. Two RI retrievals determined for the pure biogenic SOA showed a constant RI for up to 5 h of ageing. Mass spectral characterization shows the three types of the SOA formed in this study have a significant amount of semivolatile components. The influence of anthropogenic VOCs on the oxygenated organic aerosol as well as the atmospheric implications are discussed.
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38.
  • Grundström, Maria, 1979, et al. (författare)
  • Influence of atmospheric circulation patterns on urban air quality during the winter
  • 2015
  • Ingår i: Atmospheric Pollution Research. - 1309-1042. ; 6:2, s. 278-285
  • Tidskriftsartikel (refereegranskat)abstract
    • Relationships between urban nitrogen dioxide (NO2) and atmospheric circulation at two spatial scales were studied for Southern Sweden. Lamb Weather Types (LWT) describe the circulation (scale: thousands of kilometers) including non–directional (cyclonic and anticyclonic) and directional types depending on the wind direction. LWTs with low wind speeds (anticyclonic, NW and N) were associated with strongly elevated [NO2], between 46–52% of the daily averages of NO2 exceeded the 60 μg m–3 air quality standard (AQS) when occurring during these LWTs. The lowest fractions of exceedances of NO2 AQS were generally observed for LWTs E, S, SW and W. A larger scale circulation (several thousands of kilometers) was represented by the North Atlantic Oscillation (NAO) affecting meteorology over middle and high latitudes in the Northern Hemisphere. While a negative NAO index (NAOI) favors stagnant high pressure weather over Northern Europe, a positive NAOI is often associated with windy conditions. High [NO2] was found to be frequent under negative NAOI. Additionally, larger fractions of exceedances of NO2 AQS were observed for the majority of LWTs occurring at negative NAOI. It’s concluded that both LWTs and NAOI had partly independent effects on the urban air quality in a North European city. These circulation indices can be useful tools for air pollution risk assessment and forecasting.
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39.
  • Grundström, Maria, 1979, et al. (författare)
  • Variation and co-variation of PM10, particle number concentration, NOx and NO2 in the urban air - Relationships with wind speed, vertical temperature gradient and weather type
  • 2015
  • Ingår i: Atmospheric Environment. - : Elsevier Ltd. - 1352-2310. ; 120, s. 317-327
  • Tidskriftsartikel (refereegranskat)abstract
    • Atmospheric ultrafine particles (UFP; diameter < 0.1 μm) represent a growing global health concern in urban environments and has a strong link to traffic related emissions. UFP is usually the dominating fraction of atmospheric particle number concentrations (PNC) despite being a minor part of total particle mass. The aim of this study was to empirically investigate the relationship between PNC and other air pollutants (NOX, NO2 and PM10) in the urban environment and their dependence on meteorology and weather type, using the Lamb Weather Type (LWT) classification scheme. The study was carried out in Gothenburg, Sweden, at an urban background site during April 2007-May 2008. It was found that daily average [PNC] correlated very well with [NOx] (R2 = 0.73) during inversion days, to a lesser extent with [NO2] (R2 = 0.58) and poorly with [PM10] (R2 = 0.07). Both PNC and NOx had similar response patterns to wind speed and to the strength of temperature inversions. PNC displayed two regimes, one strongly correlated to NOx and a second poorly correlated to NOx which was characterised by high wind speed. For concentration averages based on LWTs, the PNC-[NOx] relationship remained strong (R2 = 0.70) where the windy LWT W deviated noticeably. Exclusion of observations with wind speed >5 ms-1 or ΔT < 0 °C from LWTs produced more uniform and stronger relationships (R2 = 0.90; R2 = 0.93). Low wind speeds and positive vertical temperature gradients were most common during LWTs A, NW, N and NE. These weather types were also associated with the highest daily means of NOx (~30 ppb) and PNC (~10 000 # cm-3). A conclusion from this study is that NOx (but not PM10) is a good proxy for PNC especially during calm and stable conditions and that LWTs A, NW, N and NE are high risk weather types for elevated NOx and PNC. © 2015.
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40.
  • Guo, Y. D., et al. (författare)
  • Identification of highly oxygenated organic molecules and their role in aerosol formation in the reaction of limonene with nitrate radical
  • 2022
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 22:17, s. 11323-11346
  • Tidskriftsartikel (refereegranskat)abstract
    • Nighttime NO3-initiated oxidation of biogenic volatile organic compounds (BVOCs) such as monoterpenes is important for the atmospheric formation and growth of secondary organic aerosol (SOA), which has significant impact on climate, air quality, and human health. In such SOA formation and growth, highly oxygenated organic molecules (HOM) may be crucial, but their formation pathways and role in aerosol formation have yet to be clarified. Among monoterpenes, limonene is of particular interest for its high emission globally and high SOA yield. In this work, HOM formation in the reaction of limonene with nitrate radical (NO3) was investigated in the SAPHIR chamber (Simulation of Atmospheric PHotochemistry In a large Reaction chamber). About 280 HOM products were identified, grouped into 19 monomer families, 11 dimer families, and 3 trimer families. Both closed-shell products and open-shell peroxy radicals (RO2 center dot) 2 were observed, and many of them have not been reported previously. Monomers and dimers accounted for 47% and 47% of HOM concentrations, respectively, with trimers making up the remaining 6 %. In the most abundant monomer families, C10H15-17NO6-14, carbonyl products outnumbered hydroxyl products, indicating the importance of RO2 center dot termination by unimolecular dissociation. Both RO2 center dot autoxidation and alkoxy-peroxy pathways were found to be important processes leading to HOM. Time-dependent concentration profiles of monomer products containing nitrogen showed mainly second-generation formation patterns. Dimers were likely formed via the accretion reaction of two monomer RO2 center dot , and HOM-trimers via the accretion reaction between monomer RO2 center dot and dimer RO2 center dot. Trimers are suggested to play an important role in new particle formation (NPF) observed in our experiment. A HOM yield of 1.5%(+1.7%)(-0.7%) was estimated considering only first-generation products. SOA mass growth could be reasonably explained by HOM condensation on particles assuming irreversible uptake of ultra-low volatility organic compounds (ULVOCs), extremely low volatility organic compounds (ELVOCs), and low volatility organic compounds (LVOCs). This work provides evidence for the important role of HOM formed via the limonene +NO3 reaction in NPF and growth of SOA particles.
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