Showing papers by "Pauli Paasonen published in 2017"

Estimating the atmospheric concentration of Criegee intermediates and their possible interference in a FAGE-LIF instrument

Abstract: . We analysed the extensive dataset from the HUMPPA-COPEC 2010 and the HOPE 2012 field campaigns in the boreal forest and rural environments of Finland and Germany, respectively, and estimated the abundance of stabilised Criegee intermediates (SCIs) in the lower troposphere. Based on laboratory tests, we propose that the background OH signal observed in our IPI-LIF-FAGE instrument during the aforementioned campaigns is caused at least partially by SCIs. This hypothesis is based on observed correlations with temperature and with concentrations of unsaturated volatile organic compounds and ozone. Just like SCIs, the background OH concentration can be removed through the addition of sulfur dioxide. SCIs also add to the previously underestimated production rate of sulfuric acid. An average estimate of the SCI concentration of ∼ 5.0 × 104 molecules cm−3 (with an order of magnitude uncertainty) is calculated for the two environments. This implies a very low ambient concentration of SCIs, though, over the boreal forest, significant for the conversion of SO2 into H2SO4. The large uncertainties in these calculations, owing to the many unknowns in the chemistry of Criegee intermediates, emphasise the need to better understand these processes and their potential effect on the self-cleaning capacity of the atmosphere.

Improving the simulation of global aerosol with size-segregated anthropogenic number emissions

Abstract: . Climate models are important tools that are used for generating climate change projections, in which aerosol-climate interactions are one of the main sources of uncertainties. In order to quantify aerosol-radiation and aerosol-cloud interactions, detailed input of anthropogenic aerosol number emissions is necessary. However, the anthropogenic aerosol number emissions are usually converted from the corresponding mass emissions in precompiled emission inventories through a very simplistic method depending uniquely on chemical composition, particle size and density, which are defined for a few very wide main source sectors. In this work, the anthropogenic particle number emissions converted from the AeroCom mass in the ECHAM-HAM climate model were replaced with the recently-formulated number emissions from the Greenhouse Gas and Air Pollution Interactions and Synergies (GAINS)-model, where the emission number size distributions vary, for example, with respect to the fuel and technology. A special attention in our analysis was put on accumulation mode particles (particle diameter d p > 100 nm) because of (i) their capability of acting as cloud condensation nuclei (CCN), thus forming cloud droplets and affecting Earth's radiation budget, and (ii) their dominant role in forming the coagulation sink and thus limiting the concentration of sub-100 nanometers particles. In addition, the estimates of anthropogenic CCN formation, and thus the forcing from aerosol-climate interactions are expected to be affected. Analysis of global particle number concentrations and size distributions reveal that GAINS implementation increases CCN concentration compared with AeroCom, with regional enhancement factors reaching values as high as 10. A comparison between modeled and observed concentrations shows that the increase in number concentration for accumulation mode particle agrees well with measurements, but it leads to a consistent underestimation of both nucleation mode and Aitken mode (d p > 100 nm) particle number concentrations. This suggests that revisions are needed in the new particle formation and growth schemes currently applied in global modeling frameworks.