Environmental chemistry through intelligent atmospheric data analysis

Gross, Deborah S.; Atlas, Robert; Rzeszotarski, Jeffrey M.; Turetsky, Emma; Christensen, Janara; Benzaid, Sami; Olson, J.; Smith, Thomas; Steinberg, Leah E.; Sulman, Jon; Ritz, Anna; Anderson, Benjamin; Nelson, C. N.; Musicant, David R.; Chen, Lei; Snyder, David C.; Schauer, James J.

doi:10.1016/j.envsoft.2009.12.001

Cited by 56 publications

(36 citation statements)

References 49 publications

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“…Over 1.2 million single particle mass spectra were generated by the ATOFMS during the sampling period and clustered using the K-means algorithm (K = 80), described in detail elsewhere (Gross et al, 2010;Healy et al, 2009Healy et al, , 2010. Clusters exhibiting very similar average mass spectra (including those with the same major ions but varying relative signal intensities), comparable temporal trends and size distributions were merged.…”

Section: Atofms Data Analysismentioning

confidence: 99%

Sources and mixing state of summertime background aerosol in the north-western Mediterranean basin

et al. 2017

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Abstract. An aerosol time-of-flight mass spectrometer (ATOFMS) was employed to provide real-time single particle mixing state and thereby source information for aerosols impacting the western Mediterranean basin during the ChArMEx-ADRIMED and SAF-MED campaigns in summer 2013. The ATOFMS measurements were made at a ground-based remote site on the northern tip of Corsica.Twenty-seven distinct ATOFMS particle classes were identified and subsequently grouped into eight general categories: EC-rich (elemental carbon), K-rich, Na-rich, amines, OC-rich (organic carbon), V-rich, Fe-rich and Carich particles. Mass concentrations were reconstructed for the ATOFMS particle classes and found to be in good agreement with other co-located quantitative measurements (PM 1 , black carbon (BC), organic carbon, sulfate mass and ammonium mass). Total ATOFMS reconstructed mass (PM 2.5 ) accounted for 70-90 % of measured PM 10 mass and was comprised of regionally transported fossil fuel (EC-rich) and biomass burning (K-rich) particles. The accumulation of these transported particles was favoured by repeated and extended periods of air mass stagnation over the western Mediterranean during the sampling campaigns. The single particle mass spectra proved to be valuable source markers, allowing the identification of fossil fuel and biomass burning combustion sources, and was therefore highly complementary to quantitative measurements made by Particle into Liquid Sampler ion chromatography (PILS-IC) and an aerosol chemical speciation monitor (ACSM), which have demonstrated that PM 1 and PM 10 were comprised predominantly of sulfate, ammonium and OC. Good temporal agreement was observed between ATOFMS EC-rich and K-rich particle mass concentrations and combined mass concentrations of BC, sulfate, ammonium and low volatility oxygenated organic aerosol (LV-OOA). This combined information suggests that combustion of fossil fuels and biomass produced primary EC-and OC-containing particles, which then accumulated ammonium, sulfate and alkylamines during regional transport.Three other sources were also identified: local biomass burning, marine and shipping. Local combustion particlesPublished by Copernicus Publications on behalf of the European Geosciences Union. (emitted in Corsica) contributed little to PM 2.5 particle number and mass concentrations but were easily distinguished from regional combustion particles. Marine emissions comprised fresh and aged sea salt: the former was detected mostly during a 5-day event during which it accounted for 50-80 % of sea salt aerosol mass, while the latter was detected throughout the sampling period. Dust was not efficiently detected by the ATOFMS, and support measurements showed that it was mainly in the PM 2.5-10 fraction. Shipping particles, identified using markers for heavy fuel oil combustion, were associated with regional emissions and represented only a small fraction of PM 2.5 particle number and mass concentration at the site.

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Section: Atofms Data Analysismentioning

confidence: 99%

Sources and mixing state of summertime background aerosol in the north-western Mediterranean basin

et al. 2017

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“…A Kmeans algorithm (K = 80), as described in detail by Healy et al (2010) and Gross et al (2010), was used to classify aerosol mass spectra into different particle classes. More than 40 distinct ATOFMS particle classes were identified and subsequently grouped into 8 general categories for clar- ity.…”

Section: Aerosol Chemical Compositionmentioning

confidence: 99%

Overview of the Chemistry-Aerosol Mediterranean Experiment/Aerosol Direct Radiative Forcing on the Mediterranean Climate (ChArMEx/ADRIMED) summer 2013 campaign

et al. 2016

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Abstract. The Chemistry-Aerosol Mediterranean Experiment (ChArMEx; http://charmex.lsce.ipsl.fr) is a collaborative research program federating international activities to investigate Mediterranean regional chemistry-climate interactions. A special observing period (SOP-1a) including intensive airborne measurements was performed in the framework of the Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region (ADRIMED) project during the Mediterranean dry season over the western and central Mediterranean basins, with a focus on aerosol-radiation measurements and their modeling. The SOP-1a took place from 11 June to 5 July 2013. Airborne measurements were made by both the ATR-42 and F-20 French research aircraft operated from Sardinia (Italy) and instrumented for in situ and remote-sensing measurements, respectively, and by sounding and drifting balloons, launched in Minorca. The experimental setup also involved several ground-based measurement sites on islands including two ground-based reference stations in Corsica and Lampedusa and secondary monitoring sites in Minorca and Sicily. Additional measurements including lidar profiling were also performed on alert during aircraft operations at EARLINET/ACTRIS stations at Granada and Barcelona in Spain, and in southern Italy. Remote-sensing aerosol products from satellites (MSG/SEVIRI, MODIS) and from the AERONET/PHOTONS network were also used. Dedicated meso-scale and regional modeling experiments were performed in relation to this observational effort. We provide here an overview of the different surface and aircraft observations deployed during the ChArMEx/ADRIMED period and of associated modeling studies together with an analysis of the synoptic conditions that determined the aerosol emission and transport. Meteorological conditions observed during this campaign (moderate temperatures and southern flows) were not favorable to producing high levels of atmospheric pollutants or intense biomass burning events in the region. However, numerous mineral dust plumes were observed during the campaign, with the main sources located in Morocco, Algeria and Tunisia, leading to aerosol optical depth (AOD) values ranging between 0.2 and 0.6 (at 440 nm) over the western and central Mediterranean basins. One important point of this experiment concerns the direct observations of aerosol extinction onboard the ATR-42, using the CAPS system, showing local maxima reaching up to 150 M m −1 within the dust plume. Non-negligible aerosol extinction (about 50 M m −1 ) has also been observed within the marine boundary layer (MBL). By combining the ATR-42 extinction coefficient observations with absorption and scattering measurements, we performed a complete optical closure revealing excellent agreement with estimated optical properties. This additional information on extinction properties has allowed calculation of the dust single scattering albedo (SSA) with a high level of confidence over the western Mediterranean. Our results show a moderate variability from 0....

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“…During the three week campaign 558 740 ATOFMS single particle mass spectra were generated and subsequently imported into ENCHILADA (Environmental Chemistry through Intelligent Data Analysis), a freeware single particle data analysis software package (Gross et al, 2010) and clustered using the K-means algorithm (MacQueen, 1967), (K = 50). ENCHILADA has been previously used to classify ATOFMS mass spectra generated from ambient particles at sites in Switzerland and East St. Louis, Illinois (Herich et al, 2008;Snyder et al, 2009).…”

Section: Atofms Data Analysismentioning

confidence: 99%

Source apportionment of PM<sub>2.5</sub> in Cork Harbour, Ireland using a combination of single particle mass spectrometry and quantitative semi-continuous measurements

et al. 2010

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Abstract. An aerosol time-of-flight mass spectrometer (ATOFMS) was deployed for the measurement of the size resolved chemical composition of single particles at a site in Cork Harbour, Ireland for three weeks in August 2008. The ATOFMS was co-located with a suite of semi-continuous instrumentation for the measurement of particle number, elemental carbon (EC), organic carbon (OC), sulfate and particulate matter smaller than 2.5 µm in diameter (PM 2.5 ). The temporality of the ambient ATOFMS particle classes was subsequently used in conjunction with the semi-continuous measurements to apportion PM 2.5 mass using positive matrix factorisation. The synergy of the single particle classification procedure and positive matrix factorisation allowed for the identification of six factors, corresponding to vehicular traffic, marine, long-range transport, various combustion, domestic solid fuel combustion and shipping traffic with estimated contributions to the measured PM 2.5 mass of 23%, 14%, 13%, 11%, 5% and 1.5% respectively. Shipping traffic was found to contribute 18% of the measured particle number (20-600 nm mobility diameter), and thus may have important implications for human health considering the size and composition of ship exhaust particles. The positive matrix factorisation procedure enabled a more refined interpretation of the single particle results by providing source contributions to PM 2.5 mass, while the single particle data enabled the identification of additional factors not possible with typical semi-continuous measurements, including local shipping traffic.

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Environmental chemistry through intelligent atmospheric data analysis

Cited by 56 publications

References 49 publications

Sources and mixing state of summertime background aerosol in the north-western Mediterranean basin

Sources and mixing state of summertime background aerosol in the north-western Mediterranean basin

Overview of the Chemistry-Aerosol Mediterranean Experiment/Aerosol Direct Radiative Forcing on the Mediterranean Climate (ChArMEx/ADRIMED) summer 2013 campaign

Source apportionment of PM<sub>2.5</sub> in Cork Harbour, Ireland using a combination of single particle mass spectrometry and quantitative semi-continuous measurements

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Environmental chemistry through intelligent atmospheric data analysis

Cited by 56 publications

References 49 publications

Sources and mixing state of summertime background aerosol in the north-western Mediterranean basin

Sources and mixing state of summertime background aerosol in the north-western Mediterranean basin

Overview of the Chemistry-Aerosol Mediterranean Experiment/Aerosol Direct Radiative Forcing on the Mediterranean Climate (ChArMEx/ADRIMED) summer 2013 campaign

Source apportionment of PM&lt;sub&gt;2.5&lt;/sub&gt; in Cork Harbour, Ireland using a combination of single particle mass spectrometry and quantitative semi-continuous measurements

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Source apportionment of PM<sub>2.5</sub> in Cork Harbour, Ireland using a combination of single particle mass spectrometry and quantitative semi-continuous measurements