ALBERT

Description: Sulfuric acid, amines and oxidized organics have been found to be important compounds in the nucleation and initial growth of atmospheric particles. Because of the challenges involved in determining the chemical composition of objects with very small mass, however, the properties of the freshly nucleated particles and the detailed pathways of their formation processes are still not clear. In this study, we focus on a challenging size range, i.e. particles that have grown to diameters of 10 and 15 nm following nucleation, and measure their water uptake. Water uptake constrains their chemical composition. We use a nanometer-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) at subsaturated conditions (ca. 90 % relative humidity at 293 K) to measure the hygroscopicity of particles during the seventh Cosmics Leaving OUtdoor Droplets (CLOUD7) experiments performed at CERN in 2012. In CLOUD7, the hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from α-pinene oxidation. The hygroscopicity parameter κ decreased with increasing particle size indicating decreasing acidity of particles. No clear effect of the sulfuric acid monomer concentrations on the hygroscopicities of 10 nm particles produced from sulfuric acid and dimethylamine was observed, whereas the hygroscopicity of 15 nm particles sharply decreased with decreasing sulfuric acid monomer concentrations. In particular, when the concentrations of sulfuric acid was 5.1 × 106 molecules cm−3 in the gas phase, and the dimethylamine mixing ratio was 11.8 ppt, the measured κ of 15 nm particles was 0.31 ± 0.01 close to the value reported for dimethylamine sulfate (DMAS) (κDMAS ~ 0.28). Furthermore, the difference in κ between sulfuric acid and sulfuric acid-dimethylamine experiments increased with increasing particle size. The κ values of particles in the presence of sulfuric acid and organics were much smaller than those of particles in the presence of sulfuric acid and dimethylamine. This suggests that the organics produced from α-pinene ozonolysis play a significant role in particle growth already at 10 nm sizes.

Description: Under certain conditions, secondary organic aerosol (SOA) particles can exist in the atmosphere in an amorphous solid or semi-solid state. To determine their relevance to processes such as ice nucleation or chemistry occurring within particles requires knowledge of the temperature and relative humidity (RH) range for SOA to exist in these states. In the CLOUD experiment at CERN, we deployed a new in-situ optical method to detect the viscosity of α-pinene SOA particles and measured their transition from the amorphous viscous to liquid state. The method is based on the depolarising properties of laboratory-produced non-spherical SOA particles and their transformation to non-depolarising spherical liquid particles during deliquescence. We found that particles formed and grown in the chamber developed an asymmetric shape through coagulation. A transition to spherical shape was observed as the RH was increased to between 35 % at −10 °C and 80 % at −38 °C, confirming previous calculations of the viscosity transition conditions. Consequently, α-pinene SOA particles exist in a viscous state over a wide range of ambient conditions, including the cirrus region of the free troposphere. This has implications for the physical, chemical and ice-nucleation properties of SOA and SOA-coated particles in the atmosphere.

Description: A method for retrieving cloud optical depth (τc) using a ground-based sky imager (USI) is presented. The Radiance Red-Blue Ratio (RRBR) method is motivated from the analysis of simulated images of various τc produced by a 3-D Radiative Transfer Model (3DRTM). From these images the basic parameters affecting the radiance and RBR of a pixel are identified as the solar zenith angle (θ0), τc, solar pixel angle/scattering angle (ϑs), and pixel zenith angle/view angle (ϑz). The effects of these parameters are described and the functions for radiance, Iλ(τc, θ0, ϑs, ϑz) and the red-blue ratio, RBR(τc, θ0, ϑs, ϑz) are retrieved from the 3DRTM results. RBR, which is commonly used for cloud detection in sky images, provides non-unique solutions for τc, where RBR increases with τc up to about τc = 1 (depending on other parameters) and then decreases. Therefore, the RRBR algorithm uses the measured Iλmeas(ϑs, ϑz), in addition to RBRmeas(ϑs, ϑz) to obtain a unique solution for τc. The RRBR method is applied to images taken by a USI at the Oklahoma Atmospheric Radiation Measurement program (ARM) site over the course of 220 days and validated against measurements from a microwave radiometer (MWR); output from the Min method for overcast skies, and τc retrieved by Beer's law from direct normal irradiance (DNI) measurements. A τc RMSE of 5.6 between the Min method and the USI are observed. The MWR and USI have an RMSE of 2.3 which is well within the uncertainty of the MWR. An RMSE of 0.95 between the USI and DNI retrieved τc is observed. The procedure developed here provides a foundation to test and develop other cloud detection algorithms.