scholarly journals Supplementary material to "α-pinene secondary organic aerosol at low temperature: Chemical composition and implications for particle viscosity"

Author(s):  
Wei Huang ◽  
Harald Saathoff ◽  
Aki Pajunoja ◽  
Xiaoli Shen ◽  
Karl-Heinz Naumann ◽  
...  
2017 ◽  
Author(s):  
Wei Huang ◽  
Harald Saathoff ◽  
Aki Pajunoja ◽  
Xiaoli Shen ◽  
Karl-Heinz Naumann ◽  
...  

Abstract. Chemical composition and viscosity of secondary organic aerosol (SOA) from α-pinene (C10H16) ozonolysis were investigated for low temperature conditions (223 K). Two types of experiments were performed using two simulation chambers at the Karlsruhe Institute of Technology, the Aerosol Preparation and Characterization chamber (APC), and the Aerosol Interaction and Dynamics in the Atmosphere chamber (AIDA). Experiment type 1 simulated SOA formation at upper tropospheric conditions: SOA was generated in the AIDA chamber directly at 223 K, 61 % relative humidity (RH) (experiment termed cold humid, CH), or for comparison at 6 % RH (experiment termed cold dry, CD) conditions. Experiment type 2 simulated SOA uplifting: SOA was formed in the APC chamber at room temperature (296 K), <1 % RH (experiment termed warm dry, WD) or 21 % RH (experiment termed warm humid, WH) conditions, and then partially transferred to the AIDA chamber kept at 223 K, and 61 % RH (WDtoCH) or 30 % RH (WHtoCH), respectively. Precursor concentrations varied between 0.7 and 2.2 ppm α-pinene, and 2.3 and 1.8 ppm ozone for type 1 and type 2 experiments, respectively. Among other instrumentation, a chemical ionization mass spectrometer (CIMS) with filter inlet for gases and aerosols (FIGAERO), deploying I- as reagent ion, was used for SOA chemical composition analysis. For type 1 experiments with lower α-pinene concentration and cold SOA formation temperature (223 K), smaller particles of 100–300 nm vacuum aerodynamic diameter (dva) and higher mass fractions (>40 %) of adducts (molecules with more than 10 carbon atoms) of α-pinene oxidation products were observed. For type 2 experiments with higher α-pinene concentration and warm SOA formation temperature (296 K), larger particles (~500 nm dva) with smaller mass fractions of adducts (<35 %) were produced. We also observed differences (up to 20 ºC) in maximum desorption temperature (Tmax) of individual compounds desorbing from the particles deposited on the FIGAERO Teflon filter for different experiments, indicating that Tmax is not purely a function of a compound's vapor pressure or volatility, but is also influenced by diffusion limitations within the particles (particle viscosity), interactions between particles deposited on the filter (particle matrix), and/or particle mass on the filter. Highest Tmax were observed for SOA under dry conditions and with higher adduct mass fraction; lowest Tmax for SOA under humid conditions and with lowest adduct mass fraction. The observations indicate that particle viscosity may be influenced by intra- and inter-molecular hydrogen bonding between oligomers, and particle water uptake, even under such low temperature conditions. Our results suggest that particle physicochemical properties such as viscosity and oligomer content mutually influence each other, and that variation in Tmax of particle desorptions may provide implications for particle viscosity and particle matrix effects. The differences in particle physicochemical properties observed between our different experiments demonstrate the importance of taking experimental conditions into consideration when interpreting data from laboratory studies or using them as input in climate models.


2018 ◽  
Vol 18 (4) ◽  
pp. 2883-2898 ◽  
Author(s):  
Wei Huang ◽  
Harald Saathoff ◽  
Aki Pajunoja ◽  
Xiaoli Shen ◽  
Karl-Heinz Naumann ◽  
...  

Abstract. Chemical composition, size distributions, and degree of oligomerization of secondary organic aerosol (SOA) from α-pinene (C10H16) ozonolysis were investigated for low-temperature conditions (223 K). Two types of experiments were performed using two simulation chambers at the Karlsruhe Institute of Technology: the Aerosol Preparation and Characterization (APC) chamber, and the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) chamber. Experiment type 1 simulated SOA formation at upper tropospheric conditions: SOA was generated in the AIDA chamber directly at 223 K at 61 % relative humidity (RH; experiment termed “cold humid”, CH) and for comparison at 6 % RH (experiment termed “cold dry”, CD) conditions. Experiment type 2 simulated SOA uplifting: SOA was formed in the APC chamber at room temperature (296 K) and < 1 % RH (experiment termed “warm dry”, WD) or 21 % RH (experiment termed “warm humid”, WH) conditions, and then partially transferred to the AIDA chamber kept at 223 K, and 61 % RH (WDtoCH) or 30 % RH (WHtoCH), respectively. Precursor concentrations varied between 0.7 and 2.2 ppm α-pinene, and between 2.3 and 1.8 ppm ozone for type 1 and type 2 experiments, respectively. Among other instrumentation, a chemical ionization mass spectrometer (CIMS) coupled to a filter inlet for gases and aerosols (FIGAERO), deploying I− as reagent ion, was used for SOA chemical composition analysis. For type 1 experiments with lower α-pinene concentrations and cold SOA formation temperature (223 K), smaller particles of 100–300 nm vacuum aerodynamic diameter (dva) and higher mass fractions (> 40 %) of adducts (molecules with more than 10 carbon atoms) of α-pinene oxidation products were observed. For type 2 experiments with higher α-pinene concentrations and warm SOA formation temperature (296 K), larger particles (∼ 500 nm dva) with smaller mass fractions of adducts (< 35 %) were produced. We also observed differences (up to 20 ∘C) in maximum desorption temperature (Tmax) of individual compounds desorbing from the particles deposited on the FIGAERO Teflon filter for different experiments, indicating that Tmax is not purely a function of a compound's vapor pressure or volatility, but is also influenced by diffusion limitations within the particles (particle viscosity), interactions between particles deposited on the filter (particle matrix), and/or particle mass on the filter. Highest Tmax were observed for SOA under dry conditions and with higher adduct mass fraction; lowest Tmax were observed for SOA under humid conditions and with lower adduct mass fraction. The observations indicate that particle viscosity may be influenced by intra- and inter-molecular hydrogen bonding between oligomers, and particle water uptake, even under such low-temperature conditions. Our results suggest that particle physicochemical properties such as viscosity and oligomer content mutually influence each other, and that variation in Tmax of particle desorptions may have implications for particle viscosity and particle matrix effects. The differences in particle physicochemical properties observed between our different experiments demonstrate the importance of taking experimental conditions into consideration when interpreting data from laboratory studies or using them as input in climate models.


2020 ◽  
Author(s):  
Junling Li ◽  
Weigang Wang ◽  
Kun Li ◽  
Wenyu Zhang ◽  
Chao Peng ◽  
...  

Abstract. Environmental temperature plays a vital role in controlling chemical transformations that lead to the formation of secondary organic aerosol (SOA), and ultimately impact composition and optical properties of the aerosol particles. In this study, we investigate optical properties of n-dodecane secondary organic aerosol under two temperature conditions: 5 °C and 25 °C. It is shown that low temperature can enhance the real part of refractive index (RI) of the SOA at the wavelengths of 532 nm and 375 nm. Mass spectrometry analysis reveals that molecular composition of n-dodecane SOA is significantly modified by temperature: a large amount of oligomers are formed under low temperature condition, which lead to higher RI values. These findings will help improve our understanding of the chemical composition and optical properties of SOA under different temperature conditions, and provide another possible explanation of the low visibility during winter.


2020 ◽  
Vol 20 (13) ◽  
pp. 8123-8137 ◽  
Author(s):  
Junling Li ◽  
Weigang Wang ◽  
Kun Li ◽  
Wenyu Zhang ◽  
Chao Peng ◽  
...  

Abstract. Environmental temperature plays a vital role in controlling chemical transformations that lead to the formation of secondary organic aerosol (SOA) and ultimately impact the composition and optical properties of the aerosol particles. In this study, we investigated optical properties of n-dodecane SOA under two temperature conditions: 5 and 25 ∘C. It was shown that low-temperature conditions could enhance the real part of the refractive index (RI) of the SOA at wavelengths of 532 and 375 nm. Mass spectrometry analysis revealed that the molecular composition of n-dodecane SOA was significantly modified by temperature: a large amount of oligomers were formed under low-temperature conditions, which led to higher RI values. These findings will help improve our understanding of the chemical composition and optical properties of SOA under different temperature conditions and will provide one possible explanation for the low visibility in suburban areas during winter.


2006 ◽  
Vol 110 (31) ◽  
pp. 9665-9690 ◽  
Author(s):  
Jason D. Surratt ◽  
Shane M. Murphy ◽  
Jesse H. Kroll ◽  
Nga L. Ng ◽  
Lea Hildebrandt ◽  
...  

Sign in / Sign up

Export Citation Format

Share Document