ORCID Profile
0000-0003-2525-160X
Current Organisation
NASA Jet Propulsion Laboratory
Does something not look right? The information on this page has been harvested from data sources that may not be up to date. We continue to work with information providers to improve coverage and quality. To report an issue, use the Feedback Form.
Publisher: Elsevier BV
Date: 04-2015
Publisher: Copernicus GmbH
Date: 19-12-2013
DOI: 10.5194/ACP-13-12451-2013
Abstract: Abstract. In situ airborne measurements were made over eastern Canada in summer 2011 as part of the BORTAS experiment (Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites). In this paper we present observations of greenhouse gases (CO2 and CH4) and other biomass burning tracers (CO, HCN and CH3CN), both climatologically and through case studies, as recorded on board the FAAM BAe-146 research aircraft. Vertical profiles of CO2 were generally characterised by depleted boundary layer concentrations relative to the free troposphere, consistent with terrestrial biospheric uptake. In contrast, CH4 concentrations were found to rise with decreasing altitude due to strong local and regional surface sources. BORTAS observations were found to be broadly comparable with both previous measurements in the region during the regional burning season and with reanalysed composition fields from the EU Monitoring Atmospheric Composition and Change (MACC) project. We use coincident tracer–tracer correlations and a Lagrangian trajectory model to characterise and differentiate air mass history of intercepted plumes. In particular, CO, HCN and CH3CN were used to identify air masses that have been recently influenced by biomass burning. Examining in idual cases we were able to quantify emissions from biomass burning. Using both near-field ( 1 day) and far-field ( 1 day) s ling, boreal forest fire plumes were identified throughout the troposphere. Fresh plumes from fires in northwestern Ontario yield emission factors for CH4 and CO2 of 8.5 ± 0.9 g (kg dry matter)−1 and 1512 ± 185 g (kg dry matter)−1, respectively. We have also investigated the efficacy of calculating emission factors from far-field s ling, in which there might be expected to be limited mixing with background and other characteristic air masses, and we provide guidance on best practice and limitations in such analysis. We have found that for measurements within plumes that originated from fires in northwestern Ontario 2–4 days upwind, emission factors can be calculated that range between 1618 ± 216 and 1702 ± 173 g (kg dry matter)−1 for CO2 and 1.8 ± 0.2 and 6.1 ± 1 g (kg dry matter)−1 for CH4.
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1EA00041A
Abstract: Tropospheric ozone (O 3 ) negatively impacts human health and is also a greenhouse gas.
Publisher: American Meteorological Society
Date: 05-2015
DOI: 10.1175/BAMS-D-12-00245.1
Abstract: Air quality and heat are strong health drivers, and their accurate assessment and forecast are important in densely populated urban areas. However, the sources and processes leading to high concentrations of main pollutants, such as ozone, nitrogen dioxide, and fine and coarse particulate matter, in complex urban areas are not fully understood, limiting our ability to forecast air quality accurately. This paper introduces the Clean Air for London (ClearfLo www.clearflo.ac.uk) project’s interdisciplinary approach to investigate the processes leading to poor air quality and elevated temperatures. Within ClearfLo, a large multi-institutional project funded by the U.K. Natural Environment Research Council (NERC), integrated measurements of meteorology and gaseous, and particulate composition/loading within the atmosphere of London, United Kingdom, were undertaken to understand the processes underlying poor air quality. Long-term measurement infrastructure installed at multiple levels (street and elevated), and at urban background, curbside, and rural locations were complemented with high-resolution numerical atmospheric simulations. Combining these (measurement–modeling) enhances understanding of seasonal variations in meteorology and composition together with the controlling processes. Two intensive observation periods (winter 2012 and the Summer Olympics of 2012) focus upon the vertical structure and evolution of the urban boundary layer chemical controls on nitrogen dioxide and ozone production—in particular, the role of volatile organic compounds and processes controlling the evolution, size, distribution, and composition of particulate matter. The paper shows that mixing heights are deeper over London than in the rural surroundings and that the seasonality of the urban boundary layer evolution controls when concentrations peak. The composition also reflects the seasonality of sources such as domestic burning and biogenic emissions.
Publisher: Copernicus GmbH
Date: 09-02-2015
Abstract: Abstract. Chemical modelling studies have been conducted over north-western Europe in summer conditions, showing that night-time dinitrogen pentoxide (N2O5) heterogeneous reactive uptake is important regionally in modulating particulate nitrate and has a~modest influence on oxidative chemistry. Results from Weather Research and Forecasting model with Chemistry (WRF-Chem) model simulations, run with a detailed volatile organic compound (VOC) gas-phase chemistry scheme and the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) sectional aerosol scheme, were compared with a series of airborne gas and particulate measurements made over the UK in July 2010. Modelled mixing ratios of key gas-phase species were reasonably accurate (correlations with measurements of 0.7–0.9 for NO2 and O3). However modelled loadings of particulate species were less accurate (correlation with measurements for particulate sulfate and ammonium were between 0.0 and 0.6). Sulfate mass loadings were particularly low (modelled means of 0.5–0.7 μg kg−1air, compared with measurements of 1.0–1.5 μg kg−1air). Two flights from the c aign were used as test cases – one with low relative humidity (RH) (60–70%), the other with high RH (80–90%). N2O5 heterogeneous chemistry was found to not be important in the low-RH test case but in the high-RH test case it had a strong effect and significantly improved the agreement between modelled and measured NO3 and N2O5. When the model failed to capture atmospheric RH correctly, the modelled NO3 and N2O5 mixing ratios for these flights differed significantly from the measurements. This demonstrates that, for regional modelling which involves heterogeneous processes, it is essential to capture the ambient temperature and water vapour profiles. The night-time NO3 oxidation of VOCs across the whole region was found to be 100–300 times slower than the daytime OH oxidation of these compounds. The difference in contribution was less for alkenes (× 80) and comparable for dimethylsulfide (DMS). However the suppression of NO3 mixing ratios across the domain by N2O5 heterogeneous chemistry has only a very slight, negative, influence on this oxidative capacity. The influence on regional particulate nitrate mass loadings is stronger. Night-time N2O5 heterogeneous chemistry maintains the production of particulate nitrate within polluted regions: when this process is taken into consideration, the daytime peak (for the 95th percentile) of PM10 nitrate mass loadings remains around 5.6 μg kg−1air, but the night-time minimum increases from 3.5 to 4.6 μg kg−1air. The sustaining of higher particulate mass loadings through the night by this process improves model skill at matching measured aerosol nitrate diurnal cycles and will negatively impact on regional air quality, requiring this process to be included in regional models.
Publisher: Elsevier BV
Date: 12-2015
Publisher: Copernicus GmbH
Date: 10-12-2014
DOI: 10.5194/ACP-14-13159-2014
Abstract: Abstract. Airborne and ground-based measurements of methane (CH4), carbon dioxide (CO2) and boundary layer thermodynamics were recorded over the Fennoscandian landscape (67–69.5° N, 20–28° E) in July 2012 as part of the MAMM (Methane and other greenhouse gases in the Arctic: Measurements, process studies and Modelling) field c aign. Employing these airborne measurements and a simple boundary layer box model, net regional-scale (~ 100 km) fluxes were calculated to be 1.2 ± 0.5 mg CH4 h−1 m−2 and −350 ± 143 mg CO2 h−1 m−2. These airborne fluxes were found to be relatively consistent with seasonally averaged surface chamber (1.3 ± 1.0 mg CH4 h−1 m−2) and eddy covariance (1.3 ± 0.3 mg CH4 h−1 m−2 and −309 ± 306 mg CO2 h−1 m−2) flux measurements in the local area. The internal consistency of the aircraft-derived fluxes across a wide swath of Fennoscandia coupled with an excellent statistical comparison with local seasonally averaged ground-based measurements demonstrates the potential scalability of such localised measurements to regional-scale representativeness. Comparisons were also made to longer-term regional CH4 climatologies from the JULES (Joint UK Land Environment Simulator) and HYBRID8 land surface models within the area of the MAMM c aign. The average hourly emission flux output for the summer period (July–August) for the year 2012 was 0.084 mg CH4 h−1 m−2 (minimum 0.0 and maximum 0.21 mg CH4 h−1 m−2) for the JULES model and 0.088 mg CH4 h−1 m−2 (minimum 0.0008 and maximum 1.53 mg CH4 h−1 m−2) for HYBRID8. Based on these observations both models were found to significantly underestimate the CH4 emission flux in this region, which was linked to the under-prediction of the wetland extents generated by the models.
Publisher: American Geophysical Union (AGU)
Date: 13-12-2016
DOI: 10.1002/2016JD026006
Publisher: Elsevier BV
Date: 09-2014
Publisher: Elsevier BV
Date: 12-2014
Publisher: Elsevier BV
Date: 12-2014
Publisher: American Geophysical Union (AGU)
Date: 06-2015
DOI: 10.1002/2014JD022629
Publisher: Elsevier BV
Date: 06-2015
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D0FD00080A
Abstract: We study the anthropogenic and biogenic contributions to organic aerosol.
Publisher: American Chemical Society (ACS)
Date: 15-08-2008
DOI: 10.1021/JA804165Q
Abstract: Carbonyl oxide species play a key role in tropospheric oxidation of organic molecules and in low-temperature combustion processes. In the late 1940s, Criegee first postulated the participation of carbonyl oxides, now often called "Criegee intermediates," in ozonolysis of alkenes. However, despite decades of effort, no gas phase Criegee intermediate has before been observed. As a result, knowledge of gas phase carbonyl oxide reactions has heretofore been inferred by indirect means, with derived rate coefficients spanning orders of magnitude. We have directly detected the primary Criegee intermediate, formaldehyde oxide (CH2OO), in the chlorine-initiated gas-phase oxidation of dimethyl sulfoxide (DMSO). This work not only establishes that the Criegee intermediate is formed in DMSO oxidation also but opens the possibility for explicit kinetics studies on this critical atmospheric species.
Publisher: Royal Society of Chemistry (RSC)
Date: 2013
DOI: 10.1039/C3FD00048F
Abstract: Carbonyl oxides ("Criegee intermediates"), formed in the ozonolysis of alkenes, are key species in tropospheric oxidation of organic molecules and their decomposition provides a non-photolytic source of OH in the atmosphere (Johnson and Marston, Chem. Soc. Rev., 2008, 37, 699, Harrison et al, Sci, Total Environ., 2006, 360, 5, Gäb et al., Nature, 1985, 316, 535, ref. 1-3). Recently it was shown that small Criegee intermediates, C.I.'s, react far more rapidly with SO2 than typically represented in tropospheric models, (Welz, Science, 2012, 335, 204, ref. 4) which suggested that carbonyl oxides could have a substantial influence on the atmospheric oxidation of SO2. Oxidation of 502 is the main atmospheric source of sulphuric acid (H2SO4), which is a critical contributor to aerosol formation, although questions remain about the fundamental nucleation mechanism (Sipilä et al., Science, 2010, 327, 1243, Metzger et al., Proc. Natl. Acad. Sci. U. S. A., 2010 107, 6646, Kirkby et al., Nature, 2011, 476, 429, ref. 5-7). Non-absorbing atmospheric aerosols, by scattering incoming solar radiation and acting as cloud condensation nuclei, have a cooling effect on climate (Intergovernmental Panel on Climate Change (IPCC), Climate Change 2007: The Physical Science Basis, Cambridge University Press, 2007, ref. 8). Here we explore the effect of the Criegees on atmospheric chemistry, and demonstrate that ozonolysis of alkenes via the reaction of Criegee intermediates potentially has a large impact on atmospheric sulphuric acid concentrations and consequently the first steps in aerosol production. Reactions of Criegee intermediates with SO2 will compete with and in places dominate over the reaction of OH with SO2 (the only other known gas-phase source of H2SO4) in many areas of the Earth's surface. In the case that the products of Criegee intermediate reactions predominantly result in H2SO4 formation, modelled particle nucleation rates can be substantially increased by the improved experimentally obtained estimates of the rate coefficients of Criegee intermediate reactions. Using both regional and global scale modelling, we show that this enhancement is likely to be highly variable spatially with local hot-spots in e.g. urban outflows. This conclusion is however contingent on a number of remaining uncertainties in Criegee intermediate chemistry.
Publisher: Wiley
Date: 25-03-2014
DOI: 10.1002/ASL2.496
Publisher: Elsevier BV
Date: 07-2015
Publisher: Elsevier BV
Date: 10-2015
Publisher: Elsevier BV
Date: 11-2011
Publisher: Copernicus GmbH
Date: 09-01-2012
Abstract: Abstract. Gas-phase ethene ozonolysis experiments were conducted at room temperature to determine formic acid yields as a function of relative humidity (RH) using the integrated EXTreme RAnge chamber-Chemical Ionisation Mass Spectrometry technique, employing a CH3I ionisation scheme. RHs studied were , 11, 21, 27, 30 % and formic acid yields of (0.07±0.01) and (0.41±0.07) were determined at % RH and 30 % RH respectively, showing a strong water dependence. It has been possible to estimate the ratio of the rate coefficient for the reaction of the Criegee biradical, CH2OO with water compared with decomposition. This analysis suggests that the rate of reaction with water ranges between 1×10−12–1×10−15 cm3 molecule−1 s−1 and will therefore dominate its loss with respect to bimolecular processes in the atmosphere. Global model integrations suggest that this reaction between CH2OO and water may dominate the production of HC(O)OH in the atmosphere.
Publisher: American Chemical Society (ACS)
Date: 07-01-2021
Location: United States of America
Location: United Kingdom of Great Britain and Northern Ireland
Location: United Kingdom of Great Britain and Northern Ireland
Location: United Kingdom of Great Britain and Northern Ireland
No related grants have been discovered for Carl Percival.