资源环境科技发展态势分析平台

Chemical composition, size distributions, and degree of oligomerization of secondary organic aerosol (SOA) from alpha-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 223K 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 alpha-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 alpha-pinene concentrations and cold SOA formation temperature (223 K), smaller particles of 100-300 nm vacuum aerodynamic diameter (d(va)/and higher mass fractions (> 40 %) of adducts (molecules with more than 10 carbon atoms) of alpha-pinene oxidation products were observed. For type 2 experiments with higher alpha-pinene concentrations and warm SOA formation temperature (296 K), larger particles (similar to 500 nm d(va)/with smaller mass fractions of adducts (< 35 %) were produced.

We also observed differences (up to 20 degrees C) in maximum desorption temperature (T-max/of individual compounds desorbing from the particles deposited on the FIGAERO Teflon filter for different experiments, indicating that T-max 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 T max were observed for SOA under dry conditions and with higher adduct mass fraction; lowest T-max 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 T-max 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.