Evidence for Diverse Biogeochemical Drivers of Boreal Forest New Particle Formation

Lawler, Michael J.; Rissanen, Matti; Ehn, Mikael; Mauldin, R. L.; Sarnela, Nina; Sipilä, Mikko; Smith, James N.

doi:10.1002/2017gl076394

Cited by 37 publications

(43 citation statements)

References 60 publications

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“…The average total mass concentration for the background period was determined to be 1.2 ± 0.8 µg m −3 . A similar trend in total mass concentration between background and polluted conditions was observed during the Southern Oxidant and Aerosol Study (SOAS), where larger particle mass concentrations were observed during times with polluted air mass influence and, when followed by a period of rainfall, smaller mass concentrations were observed (Liu and Russell, 2017). Occasional rainfall was seen during the background period, resulting in wet deposition of aerosol particles.…”

Section: Meteorological Data and Classification Of Air Massessupporting

confidence: 69%

“…A prior TDCIMS laboratory study linked the acetate ion fragment (m/z 59) to particulate carboxylic and dicarboxylic acids (Smith and Rathbone, 2008), which have been linked to the photochemical oxidation of both biogenic and anthropogenic compounds (Winkler et al, 2012). During the wet season in the Amazon Basin, specific dicarboxylic acids and tricarboxylic acids have been identified and proposed to have been formed from the oxidation of semi-volatile fatty acids and terpenes (Kubátová et al, 2000). Hydrogen oxalate, measured as m/z 89, was one of the two most abundant organic ions measured in ultrafine particles at both an urban and rural site in Helsinki, Finland (Pakkanen et al, 2000).…”

Section: Multivariate Analysis Of Tdcims and Ams Datamentioning

confidence: 99%

“…For example, TDCIMS measurements performed outside of Mexico City attribute about 90 % of the growth of freshly nucleated particles to oxidized organics . In the boreal forest of Finland, the contribution of oxidized organics is close to 100 %, and an analysis of composition suggests that marine emissions can play an important role in that process (Lawler et al, 2018). For the smallest particles measurable by TDCIMS, with diameters from 8 to 10 nm, between 23 % and 47 % of the constituents may be derived from organic salt formation, a reactive uptake mechanism that requires the presence of strong bases such as gasphase amines (Smith et al, 2010).…”

Section: Introductionmentioning

confidence: 99%

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Chemical composition of ultrafine aerosol particles in central Amazonia during the wet season

et al. 2019

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Abstract. Central Amazonia serves as an ideal location to study atmospheric particle formation, since it often represents nearly natural, pre-industrial conditions but can also experience periods of anthropogenic influence due to the presence of emissions from large metropolitan areas like Manaus, Brazil. Ultrafine (sub-100 nm diameter) particles are often observed in this region, although new particle formation events seldom occur near the ground despite being readily observed in other forested regions with similar emissions of volatile organic compounds (VOCs). This study focuses on identifying the chemical composition of ultrafine particles as a means of determining the chemical species and mechanisms that may be responsible for new particle formation and growth in the region. These measurements were performed during the wet season as part of the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) field campaign at a site located 70 km southwest of Manaus. A thermal desorption chemical ionization mass spectrometer (TDCIMS) characterized the most abundant compounds detected in ultrafine particles. Two time periods representing distinct influences on aerosol composition, which we label as “anthropogenic” and “background” periods, were studied as part of a larger 10 d period of analysis. Higher particle number concentrations were measured during the anthropogenic period, and modeled back-trajectory frequencies indicate transport of emissions from the Manaus metropolitan area. During the background period there were much lower number concentrations, and back-trajectory frequencies showed that air masses arrived at the site predominantly from the forested regions to the north and northeast. TDCIMS-measured constituents also show distinct differences between the two observational periods. Although bisulfate was detected in particles throughout the 10 d period, the anthropogenic period had higher levels of particulate bisulfate overall. Ammonium and trimethyl ammonium were positively correlated with bisulfate. The background period had distinct diurnal patterns of particulate cyanate and acetate, while oxalate remained relatively constant during the 10 d period. 3-Methylfuran, a thermal decomposition product of a particulate-phase isoprene epoxydiol (IEPOX), was the dominant species measured in the positive-ion mode. Principal component analysis (PCA) was performed on the TDCIMS-measured ion abundance and aerosol mass spectrometer (AMS) mass concentration data. Two different hierarchical clusters representing unique influences arise: one comprising ultrafine particulate acetate, hydrogen oxalate, cyanate, trimethyl ammonium and 3-methylfuran and another made up of ultrafine particulate bisulfate, chloride, ammonium and potassium. A third cluster separated AMS-measured species from the two TDCIMS-derived clusters, indicating different sources or processes in ultrafine aerosol particle formation compared to larger submicron-sized particles.

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Section: Meteorological Data and Classification Of Air Massessupporting

confidence: 69%

Section: Multivariate Analysis Of Tdcims and Ams Datamentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Chemical composition of ultrafine aerosol particles in central Amazonia during the wet season

et al. 2019

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“…The mainstream smoke sampling train was composed of a series of dedicated instruments including a scanning mobility particle sizer (SMPS; TSI) to measure size distribution of particles, a CO monitor (Thermo Fisher Scientific, model 48i) and two mass spectrometers measuring the volatiles (PTR-ToF-MS, model 8000, Ionicon Analytik) (Jordan et al 2009) and the particle chemical composition (TDCIMS) (Lawler et al 2018;Smith et al 2004). All details of the instrumentation operation are given in SI.…”

Section: Methodsmentioning

confidence: 99%

Chemical characterization of nanoparticles and volatiles present in mainstream hookah smoke

Perraud

Lawler

Malecha

et al. 2019

Aerosol Science and Technology

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Waterpipe smoking is becoming more popular worldwide and there is a pressing need to better characterize the exposure of smokers to chemical compounds present in the mainstream smoke. We report real-time measurements of mainstream smoke for carbon monoxide, volatile organic compounds and nanoparticle size distribution and chemical composition using a custom dilution flow tube. A conventional tobacco mixture, a dark leaf unwashed tobacco, and a nicotine-free herbal tobacco were studied. Results show that carbon monoxide is present in the mainstream smoke and originates primarily from the charcoal used to heat the tobacco. Online measurements of volatile organic compounds in mainstream smoke showed an overwhelming contribution from glycerol and its decomposition products. Gas phase analysis also showed that very little filtration of the gas phase products is provided by the percolation of mainstream smoke through water. Waterpipe smoking generated high concentrations of 4-100 nm nanoparticles, which were mainly composed of sugar derivatives and especially abundant in the first 10 min of the smoking session. These measured emissions of volatiles and particles are compared with those from a reference cigarette (3R4F) and represent the equivalent of the emission of one or more entire cigarettes for a single puff of hookah smoke. Considerations related to the health impacts of waterpipe smoking are discussed.

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“…For example, TDCIMS measurements performed outside of Mexico City attribute about 90% of the growth of freshly nucleated particles to oxidized organics . In the Boreal forest of Finland, the contribution of oxidized organics is close to 100% and an analysis of composition suggests that marine emissions can play an important role in that process (Lawler et al, 2018). For the smallest particles measureable by TDCIMS, with diameters from 8 to 10 nm, between 23% to 47% of the constituents may be derived from organic salt formation, a reactive uptake mechanism that requires the presence of strong bases such as gas phase amines (Smith et al, 2010).…”

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confidence: 99%

Chemical composition of ultrafine aerosol particles in central Amazonia during the wet season

Glicker¹,

Ortega²,

Sá³

et al. 2019

Preprint

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Abstract. Central Amazonia serves as an ideal location to study atmospheric particle formation since it often can be characterized as representing natural, pre-industrial conditions but can also experience periods of anthropogenic influence due to the presence of emissions from large metropolitan areas like Manaus, Brazil. Ultrafine (sub-100 nm diameter) particles are often observed in this region, although new particle formation events seldom occur near the ground despite being readily observed in other forested regions with similar emissions. This study focuses on identifying the chemical composition of ultrafine particles as a means of determining the chemical species and mechanisms that may be responsible for new particle formation and growth in the region. These measurements were performed during the wet season as part of the GoAmazon2014/5 field campaign at a site located 70 km southwest of Manaus. A Thermal Desorption Chemical Ionization Mass Spectrometer (TDCIMS) measured the concentrations of the most abundant compounds detected in ultrafine particles. Two time periods representing distinct influences on aerosol composition, which we label as anthropogenic and background periods, were studied as part of a larger ten-day period of analysis. The anthropogenic period saw higher particle number concentrations and modeled back-trajectories indicate transport of emissions from the Manaus metropolitan area. The background period saw much lower number concentrations and back-trajectories showed that air masses arrived at the site predominantly from the forested regions to the north and northeast. TDCIMS-measured constituents also show distinct differences between the two observational periods. Although bisulfate was detected in particles during the ten-day period, the anthropogenic period had increased levels of particulate bisulfate overall. Additionally, with larger fractions of bisulfate observed, increased fractions of ammonium and trimethyl ammonium were observed. The background period had distinct diurnal patterns of particulate organic nitrogen species and acetate, while oxalate remained relatively constant during the ten-day period. 3-Methylfuran, a thermal decomposition product of particulate phase isoprene epoxydiol (IEPOX), was the dominant species measured in the positive ion mode. Principal Component Analysis (PCA) was performed on the TDCIMS-measured ion abundance and Aerosol Mass Spectrometer (AMS) mass concentration data. Two different hierarchical clusters representing unique influences arise: one relating ultrafine particulate acetate, hydrogen oxalate, organic nitrogen species, trimethyl ammonium and 3-methylfuran with each other and ultrafine particulate bisulfate, chloride, ammonium and potassium. A third cluster separated AMS-measured species from the two TDCIMS-derived clusters, indicating different sources or processes in ultrafine aerosol particle formation compared to submicron-sized particles.

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Evidence for Diverse Biogeochemical Drivers of Boreal Forest New Particle Formation

Cited by 37 publications

References 60 publications

Chemical composition of ultrafine aerosol particles in central Amazonia during the wet season

Chemical composition of ultrafine aerosol particles in central Amazonia during the wet season

Chemical characterization of nanoparticles and volatiles present in mainstream hookah smoke

Chemical composition of ultrafine aerosol particles in central Amazonia during the wet season

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