ALBERT

Description: Measurements of particle formation following the gas phase oxidation of volatile organic compounds (VOCs) emitted by Scots pine (Pinus sylvestris L.) seedlings are reported. Particle nucleation and condensational growth both from ozone (O3) and hydroxyl radical (OH) initiated oxidation of pine emissions (about 20–120 ppb) were investigated in a~smog chamber. During experiments, tetramethylethylene (TME) and 2-butanol were added to control the concentrations of O3 and OH. Particle nucleation and condensational growth rates were interpreted with a chemical kinetics model. Scots pine emissions mainly included α-pinene, β-pinene, Δ3-carene, limonene, myrcene, β-phellandrene and isoprene, composing more than 95% of total emissions. Modeled OH concentration in the O3+OH induced experiments was at a level of ~106 molecular cm−3. Our results demonstrate that OH-initiated oxidation of VOCs plays an important role in the nucleation process during the initial new particle formation stage. The highest average nucleation rate of 360 cm−3 s−1 was observed for the OH-dominated nucleation events and the lowest aerosol mean formation rate less than 0.5 cm−3 s−1 for the case with only O3 present as an oxidant. On the other hand, ozonolysis of monoterpenes appears to be much more efficient to the aerosol growth process following nucleation. Higher contributions of more oxygenated products to the SOA mass loadings from OH-dominating oxidation systems were found as compared to the ozonolysis systems. Comparison of mass and volume distributions from the aerosol mass spectrometer and differential mobility analyzer yields estimated effective density of these SOA to be 1.34±0.06 g cm−3 with the OH plus O3 initiated oxidation systems and 1.38±0.03 g cm−3 with the ozonolysis dominated chemistry.

Description: Biogenic volatile organic compounds (VOCs) are a significant source of global secondary organic aerosol (SOA); however, quantifying their aerosol forming potential remains a challenge. This study presents smog chamber laboratory work, focusing on SOA formation via oxidation of the emissions of two dominant tree species from boreal forest area, Scots pine (Pinus sylvestris L.) and Norway spruce (Picea abies), by hydroxyl radical (OH) and ozone (O3). Oxidation of α-pinene was also studied as a reference system. Tetramethylethylene (TME) and 2-butanol were added to control OH and O3 levels, thereby allowing SOA formation events to be categorized as resulting from either OH-dominated or O3-initiated chemistry. SOA mass yields from α-pinene are consistent with previous studies while the yields from the real plant emissions are generally lower than that from α-pinene, varying from 1.9% at an aerosol mass loading of 0.69 μg m−3 to 17.7% at 26.0 μg m−3. Mass yields from oxidation of real plant emissions are subject to the interactive effects of the molecular structures of plant emissions and their reaction chemistry with OH and O3, which lead to variations in condensable product volatility. SOA formation can be reproduced with a two-product gas-phase partitioning absorption model in spite of differences in the source of oxidant species and product volatility in the real plant emission experiments. Condensable products from OH-dominated chemistry showed a higher volatility than those from O3-initiated systems during aerosol growth stage. Particulate phase products became less volatile via aging process which continued after input gas-phase oxidants had been completely consumed.

Description: Measurements of particle formation following the gas phase oxidation of volatile organic compounds (VOCs) emitted by Scots pine (Pinus sylvestris L.) seedlings are reported. Particle formation and condensational growth both from ozone (O3) and hydroxyl radical (OH) initiated oxidation of pine emissions (about 20-120 ppb) were investigated in a smog chamber. During experiments, tetramethylethylene (TME) and 2-butanol were added to control the concentrations of O3 and OH. Particle formation and condensational growth rates were interpreted with a chemical kinetic model. Scots pine emissions mainly included α-pinene, β-pinene, Δ3-carene, limonene, myrcene and β-phellandrene, composing more than 95% of total emissions. Modeled OH concentrations in the O3- and OH-induced experiments were on the order of ~106 molecules cm−3. Our results demonstrate that OH-initiated oxidation of VOCs plays an important role in the nucleation process during the initial new particle formation stage. The highest average particle formation rate of 360 cm−3 s−1 was observed for the OH-dominated nucleation events and the lowest formation rate of less than 0.5 cm−3 s−1 was observed for the case with only O3 present as an oxidant. In contrast to the particle formation process, ozonolysis of monoterpenes appears to be much more efficient to the aerosol growth process following nucleation. Higher contributions of more oxygenated products to the SOA mass loadings from OH-dominated oxidation systems were found as compared to the ozonolysis systems. Comparison of mass and volume distributions from the aerosol mass spectrometer and differential mobility analyzer yields estimated SOA effective densities of 1.34±0.06 g cm−3 for the OH+O3 oxidation systems and 1.38±0.03 g cm−3 for the O3 dominated chemistry.

Description: Boreal forests are a major source of climate-relevant biogenic secondary organic aerosols (SOA) and will be greatly influenced by increasing temperature. Global warming is predicted to increase emissions of reactive biogenic volatile organic compounds (BVOC) from vegetation directly, but will also induce large-scale insect outbreaks, which significantly increase emissions of reactive BVOC. Thus, climate change factors could substantially accelerate the formation of biogenic SOA in the troposphere. In this study, we have combined results from field and laboratory experiments, satellite observations and global scale modelling in order to evaluate the effects of insect herbivory and large-scale outbreaks on SOA formation and the Earth's climate. Field measurements demonstrated 11-fold and 20-fold increases in monoterpene and sesquiterpene emissions, respectively, from damaged trees during a pine sawfly (Neodiprion sertifer) outbreak in eastern Finland. Laboratory chamber experiments showed that feeding by pine weevils (Hylobius abietis) increased VOC emissions from Scots pine and Norway spruce seedlings by 10–50 fold resulting in 200–1000 fold increases in SOA masses formed via ozonolysis. The influence of insect damage on aerosol concentrations in boreal forests was studied with a global chemical transport model GLOMAP and MODIS satellite observations. Global scale modelling was performed using a 10-fold increase in monoterpene emission rates and assuming 10% of the boreal forest area was experiencing outbreak. Results showed a clear increase in total particulate mass (local max. 480%) and cloud condensation nuclei concentrations (45%). Satellite observations indicated a two-fold increase in aerosol optical depth (AOD) over western Canada's pine forests in August during a bark beetle outbreak. These results suggest that more frequent insect outbreaks in a warming climate could result in substantial increase in biogenic SOA formation in the boreal zone and, thus, affect both aerosol direct and indirect forcing of climate at regional scales. The effect of insect outbreaks on VOC emissions and SOA formation should be considered in future climate predictions.

Description: Boreal forests are a major source of climate-relevant biogenic secondary organic aerosols (SOAs) and will be greatly influenced by increasing temperature. Global warming is predicted to not only increase emissions of reactive biogenic volatile organic compounds (BVOCs) from vegetation directly but also induce large-scale insect outbreaks, which significantly increase emissions of reactive BVOCs. Thus, climate change factors could substantially accelerate the formation of biogenic SOAs in the troposphere. In this study, we have combined results from field and laboratory experiments, satellite observations and global-scale modelling in order to evaluate the effects of insect herbivory and large-scale outbreaks on SOA formation and the Earth's climate. Field measurements demonstrated 11-fold and 20-fold increases in monoterpene and sesquiterpene emissions respectively from damaged trees during a pine sawfly (Neodiprion sertifer) outbreak in eastern Finland. Laboratory chamber experiments showed that feeding by pine weevils (Hylobius abietis) increased VOC emissions from Scots pine and Norway spruce seedlings by 10–50 fold, resulting in 200–1000-fold increases in SOA masses formed via ozonolysis. The influence of insect damage on aerosol concentrations in boreal forests was studied with a global chemical transport model GLOMAP and MODIS satellite observations. Global-scale modelling was performed using a 10-fold increase in monoterpene emission rates and assuming 10 % of the boreal forest area was experiencing outbreak. Results showed a clear increase in total particulate mass (local max. 480 %) and cloud condensation nuclei concentrations (45 %). Satellite observations indicated a 2-fold increase in aerosol optical depth over western Canada's pine forests in August during a bark beetle outbreak. These results suggest that more frequent insect outbreaks in a warming climate could result in substantial increase in biogenic SOA formation in the boreal zone and, thus, affect both aerosol direct and indirect forcing of climate at regional scales. The effect of insect outbreaks on VOC emissions and SOA formation should be considered in future climate predictions.

Description: Biogenic volatile organic compounds (VOCs) are a significant source of global secondary organic aerosol (SOA); however, quantifying their aerosol forming potential remains a challenge. This study presents smog chamber laboratory work, focusing on SOA formation via oxidation of the emissions of two dominant tree species from boreal forest area, Scots pine (Pinus sylvestris L.) and Norway spruce (Picea abies), by hydroxyl radical (OH) and ozone (O3). Oxidation of α-pinene was also studied as a reference system. Tetramethylethylene (TME) and 2-butanol were added to control OH and O3 levels, thereby allowing SOA formation events to be categorised as resulting from either OH-dominated or O3-initiated chemistry. SOA mass yields from α-pinene are consistent with previous studies while the yields from the real plant emissions are generally lower than that from α-pinene, varying from 1.9% at an aerosol mass loading of 0.69 μg m−3 to 13.6% at 32.8 μg m−3. Mass yields from oxidation of real plant emissions are subject to the interactive effects of the molecular structures of plant emissions and their reaction chemistry with OH and O3, which lead to variations in condensable product volatility. SOA formation can be reproduced with a two-product gas-phase partitioning absorption model in spite of differences in the source of oxidant species and product volatility in the real plant emission experiments. Condensable products from OH-dominated chemistry showed a higher volatility than those from O3-initiated systems during aerosol growth stage. Particulate phase products became less volatile via aging process which continued after input gas-phase oxidants had been completely consumed.