E. Herrmann

Emission Rates Due to Indoor Activities: Indoor Aerosol Model Development, Evaluation, and Applications

This study presents an indoor aerosol model based on size-resolved and multi-compartment approach. The current indoor aerosol model is also developed with a semi-empirical technique to estimate the emission rates due to indoor sources of aerosol particles. We present in this study a methodology to predict and estimate the best-fit input parameters for the current indoor aerosol model. The performance of the current indoor aerosol model in its single-compartment form was evaluated against previously measured indoor-outdoor aerosol data sets from an office room with mechanical ventilation and a family house with natural ventilation. The indoor aerosol model simulations show that the current methodology used to predict the best-fit input parameters to the indoor aerosol model is efficient. As expected, the penetration factor, aerosol particle deposition, and ventilation rate are the most important parameters in the indoor-outdoor relationship of aerosol particles transport. The emission rate analysis showed that fine aerosol particles production was as high as 26 particle/cm 3 s during wood burning in a fireplace. The emission rate was about eight times this value during grilling in a fireplace and sauna heating. Indoor activities take place in another room may significantly increase the aerosol particle concentrations in other rooms in the building. Therefore, it is recommended to use extra air cleaners in houses to reduce the number concentrations of emitted aerosol particles. The quantitative and qualitative results obtained by the current indoor aerosol model in this study are building and condition specific. Applying the current model to a broad range of conditions and previously measured indoor-outdoor aerosol data sets provides better understanding of aerosol particle characteristics indoors, especially regarding the aerosol particles produced during different indoor activities.

A computational fluid dynamics approach to nucleation in the water-sulfuric acid system.

This study presents a computational fluid dynamics modeling approach to investigate the nucleation in the water-sulfuric acid system in a flow tube. On the basis of an existing experimental setup (Brus, D.; Hyvärinen, A.-P.; Viisanen, Y.; Kulmala, M.; Lihavainen, H. Atmos. Chem. Phys. 2010, 10, 2631-2641), we first establish the effect of convection on the flow profile. We then proceed to simulate nucleation for relative humidities of 10, 30, and 50% and for sulfuric acid concentration between 10(9) to 3 x 10(10) cm(-3). We describe the nucleation zone in detail and determine how flow rate and relative humidity affect its characteristics. Experimental nucleation rates are compared to rates gained from classical binary and kinetic nucleation theory as well as cluster activation theory. For low RH values, kinetic theory yields the best agreement with experimental results while binary nucleation best reproduces the experimental nucleation behavior at 50% relative humidity. Particle growth is modeled for an example case at 50% relative humidity. The final simulated diameter is very close to the experimental result.

Predicting abundance and variability of ice nucleating particles in precipitation at the high-altitude observatory Jungfraujoch

Abstract. Nucleation of ice affects the properties of clouds and the formation of precipitation. Quantitative data on how ice nucleating particles (INPs) determine the distribution, occurrence and intensity of precipitation are still scarce. INPs active at −8 °C (INPs−8) were observed for 2 years in precipitation samples at the High-Altitude Research Station Jungfraujoch (Switzerland) at 3580 m a.s.l. Several environmental parameters were scanned for their capability to predict the observed abundance and variability of INPs−8. Those singularly presenting the best correlations with observed number of INPs−8 (residual fraction of water vapour, wind speed, air temperature, number of particles with diameter larger than 0.5 µm, season, and source region of particles) were implemented as potential predictor variables in statistical multiple linear regression models. These models were calibrated with 84 precipitation samples collected during the first year of observations; their predictive power was successively validated on the set of 15 precipitation samples collected during the second year. The model performing best in calibration and validation explains more than 75 % of the whole variability of INPs−8 in precipitation and indicates that a high abundance of INPs−8 is to be expected whenever high wind speed coincides with air masses having experienced little or no precipitation prior to sampling. Such conditions occur during frontal passages, often accompanied by precipitation. Therefore, the circumstances when INPs−8 could be sufficiently abundant to initiate the ice phase in clouds may frequently coincide with meteorological conditions favourable to the onset of precipitation events.

Re-evaluation of the Pressure Effect for Nucleation in Laminar Flow Diffusion Chamber Experiments with Fluent and the Fine Particle Model

This study is an investigation of the effect of total pressure on homogeneous nucleation rates of n-butanol in helium and n-pentanol in helium and argon in a laminar flow diffusion chamber (LFDC). To verify earlier findings, experimental data was re-evaluated using the computational fluid dynamics (CFD) software FLUENT in combination with the fine particle model (FPM) for aerosol dynamics calculations. This approach has been introduced in an earlier paper [Herrmann, E.; Lihavainen, H.; Hyvarinen, A.-P.; Riipinen, I.; Wilck, M.; Stratmann, F.; Kulmala, M. J. Phys. Chem. A 2006, 110, 12448]. As a result of our evaluation, a flaw in the femtube2 code was found which had been used in the original data analysis [Hyvarinen, A.-P.; Brus, D.; Zdimal, V.; Smolik, J.; Kulmala, M.; Viisanen, Y.; Lihavainen, H. J. Chem. Phys. 2006, 124, 224304]. The FLUENT analysis yielded a weak positive pressure effect for the nucleation of n-butanol in helium at low nucleation temperatures (265-270 K). n-Pentanol in helium showed a positive pressure effect at all temperatures (265-290 K), while the effect for the nucleation of n-pentanol in argon was negative at high temperatures (280 and 285 K) and positive at lower nucleation temperatures (265 K). These findings support results gained with the corrected femtube2 model. In this study, we also carried out a detailed comparison of FLUENT and femtube2 modeling results, especially focusing on the calculation of temperature and saturation ratio at nucleation rate maximum (T(nuc) and S(nuc), respectively) in both models.