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  • 1. Brus, David
    et al.
    Skrabalova, Lenka
    Herrmann, Erik
    Olenius, Tinja
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för miljövetenskap och analytisk kemi. University of Helsinki, Finland.
    Travnickova, Tereza
    Makkonen, Ulla
    Merikanto, Joonas
    Temperature-Dependent Diffusion of H2SO4 in Air at Atmospherically Relevant Conditions: Laboratory Measurements Using Laminar Flow Technique2017Inngår i: Atmosphere, ISSN 2073-4433, E-ISSN 2073-4433, Vol. 8, nr 7, artikkel-id 132Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    We report flow tube measurements of the effective sulfuric acid diffusion coefficient at ranges of different relative humidities (from similar to 4 to 70%), temperatures (278, 288 and 298 K) and initial H2SO4 concentrations (from 1 x 10(6) to 1 x 10(8) molecules.cm(-3)). The measurements were carried out under laminar flow of humidified air containing trace amounts of impurities such as amines (few ppt), thus representing typical conditions met in Earth's continental boundary layer. The diffusion coefficients were calculated from the sulfuric acid wall loss rate coefficients that were obtained by measuring H2SO4 concentration continuously at seven different positions along the flow tube with a chemical ionization mass spectrometer (CIMS). The wall loss rate coefficients and laminar flow conditions were verified with additional computational fluid dynamics (CFD) model FLUENT simulations. The determined effective sulfuric acid diffusion coefficients decreased with increasing relative humidity, as also seen in previous experiments, and had a rather strong power dependence with respect to temperature, around proportional to T-5.6, which is in disagreement with the expected temperature dependence of similar to T-1.75 for pure vapours. Further clustering kinetics simulations using quantum chemical data showed that the effective diffusion coefficient is lowered by the increased diffusion volume of H2SO4 molecules via a temperature-dependent attachment of base impurities like amines. Thus, the measurements and simulations suggest that in the atmosphere the attachment of sulfuric acid molecules with base molecules can lead to a lower than expected effective sulfuric acid diffusion coefficient with a higher than expected temperature dependence.

  • 2. Elm, Jonas
    et al.
    Myllys, Nanna
    Olenius, Tinja
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för miljövetenskap och analytisk kemi.
    Halonen, Roope
    Kurtén, Theo
    Vehkamäki, Hanna
    Formation of atmospheric molecular clusters consisting of sulfuric acid and C8H12O6 tricarboxylic acid2017Inngår i: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 19, nr 6, s. 4877-4886Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    Using computational methods, we investigate the formation of atmospheric clusters consisting of sulfuric acid (SA) and 3-methyl-1,2,3-butanetricarboxylic acid (MBTCA), identified from a-pinene oxidation. The molecular structure of the clusters is obtained using three different DFT functionals (PW91, M06-2X and oB97X-D) with the 6-31++ G(d, p) basis set and the binding energies are calculated using a high level DLPNO-CCSD(T)/ Def2-QZVPP method. The stability of the clusters is evaluated based on the calculated formation free energies. The interaction between MBTCA and sulfuric acid is found to be thermodynamically favourable and clusters consisting of 2-3 MBTCA and 2-3 SA molecules are found to be particularly stable. There is a large stabilization of the cluster when the amount of sulfuric acid-carboxylic acid hydrogen bonded interactions is maximized. The reaction free energies for forming the (MBTCA) 2-3(SA) 2-3 clusters are found to be similar in magnitude to those of the formation of the sulfuric acid-dimethylamine cluster. Using cluster kinetics calculations we identify that the growth of the clusters is essentially limited by a weak formation of the largest clusters studied, implying that other stabilizing vapours are required for stable cluster formation and growth.

  • 3.
    Julin, Jan
    et al.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för miljövetenskap och analytisk kemi. University of Eastern Finland, Finland.
    Murphy, Benjamin N.
    Patoulias, David
    Fountoukis, Christos
    Olenius, Tinja
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för miljövetenskap och analytisk kemi.
    Pandis, Spyros N.
    Riipinen, Ilona
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för miljövetenskap och analytisk kemi.
    Impacts of Future European Emission Reductions on Aerosol Particle Number Concentrations Accounting for Effects of Ammonia, Amines, and Organic Species2018Inngår i: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 52, nr 2, s. 692-700Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    Although they are currently unregulated, atmospheric ultrafine particles (<100 nm) pose health risks because of, e.g., their capability to penetrate deep into the respiratory system. Ultrafine particles, often minor contributors to atmospheric particulate mass, typically dominate aerosol particle number concentrations. We simulated the response of particle number concentrations over Europe to recent estimates of future emission reductions of aerosol particles and their precursors. We used the chemical transport model PMCAMx-UF, with novel updates including state-of-the-art descriptions of ammonia and dimethylamine new particle formation (NPF) pathways and the condensation of organic compounds onto particles. These processes had notable impacts on atmospheric particle number concentrations. All three emission scenarios (current legislation, optimized emissions, and maximum technically feasible reductions) resulted in substantial (10-50%) decreases in median particle number concentrations over Europe. Consistent reductions were predicted in Central Europe, while Northern Europe exhibited smaller reductions or even increased concentrations. Motivated by the improved NPF descriptions for ammonia and methylamines, we placed special focus on the potential to improve air quality by reducing agricultural emissions,, which are a major source of these species. Agricultural emission controls showed promise in reducing ultrafine particle number concentrations, although the change is nonlinear with particle size.

  • 4.
    Kontkanen, Jenni
    et al.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för miljövetenskap och analytisk kemi. University of Helsinki, Finland.
    Olenius, Tinja
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för miljövetenskap och analytisk kemi.
    Kulmala, Markku
    Riipinen, Ilona
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för miljövetenskap och analytisk kemi.
    Exploring the potential of nano-Kohler theory to describe the growth of atmospheric molecular clusters by organic vapors using cluster kinetics simulations2018Inngår i: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 18, nr 18, s. 13733-13754Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    Atmospheric new particle formation (NPF) occurs by the formation of nanometer-sized molecular clusters and their subsequent growth to larger particles. NPF involving sulfuric acid, bases and oxidized organic compounds is an important source of atmospheric aerosol particles. One of the mechanisms suggested to depict this process is nano-Kohler theory, which describes the activation of inorganic molecular clusters to growth by a soluble organic vapor. In this work, we studied the capability of nano-Kohler theory to describe the initial growth of atmospheric molecular clusters by simulating the dynamics of a cluster population in the presence of a sulfuric acid-base mixture and an organic compound. We observed nano-Kohler-type activation in our simulations when the saturation ratio of the organic vapor and the ratio between organic and inorganic vapor concentrations were in a suitable range. However, nano-Kohler theory was unable to predict the exact size at which the activation occurred in the simulations. In some conditions, apparent cluster growth rate (GR) started to increase close to the activation size determined from the simulations. Nevertheless, because the behavior of GR is also affected by other dynamic processes, GR alone cannot be used to deduce the cluster growth mechanism.

  • 5. Kontkanen, Jenni
    et al.
    Olenius, Tinja
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för miljövetenskap och analytisk kemi.
    Lehtipalo, Katrianne
    Vehkamäki, Hanna
    Kulmala, Markku
    Lehtinen, Kari E. J.
    Growth of atmospheric clusters involving cluster-cluster collisions: comparison of different growth rate methods2016Inngår i: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 16, nr 9, s. 5545-5560Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    We simulated the time evolution of atmospheric cluster concentrations in a one-component system where not only do clusters grow by condensation of monomers, but cluster-cluster collisions also significantly contribute to the growth of the clusters. Our aim was to investigate the consistency of the growth rates of sub-3aEuro-nm clusters determined with different methods and the validity of the common approach to use them to estimate particle formation rates. We compared the growth rate corresponding to particle fluxes (FGR), the growth rate derived from the appearance times of clusters (AGR), and the growth rate calculated based on irreversible vapor condensation (CGR). We found that the relation between the different growth rates depends strongly on the external conditions and the properties of the model substance. The difference between the different growth rates was typically highest at the smallest, sub-2aEuro-nm sizes. FGR was generally lower than AGR and CGR; at the smallest sizes the difference was often very large, while at sizes larger than 2aEuro-nm the growth rates were closer to each other. AGR and CGR were in most cases close to each other at all sizes. The difference between the growth rates was generally lower in conditions where cluster concentrations were high, and evaporation and other losses were thus less significant. Furthermore, our results show that the conventional method used to determine particle formation rates from growth rates may give estimates far from the true values. Thus, care must be taken not only in how the growth rate is determined but also in how it is applied.

  • 6. Myllys, Nanna
    et al.
    Chee, Sabrina
    Olenius, Tinja
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för miljövetenskap och analytisk kemi.
    Lawler, Michael
    Smith, James
    Molecular-Level Understanding of Synergistic Effects in Sulfuric Acid-Amine-Ammonia Mixed Clusters2019Inngår i: Journal of Physical Chemistry A, ISSN 1089-5639, E-ISSN 1520-5215, Vol. 123, nr 12, s. 2420-2425Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    The abundance and basicity of a stabilizing base have shown to be key factors in sulfuric acid driven atmospheric new-particle formation. However, since experiments indicate that a low concentration of ammonia enhances particle formation from sulfuric acid and dimethylamine, which is a stronger base, there must be additional factors affecting the particle formation efficiency. Using quantum chemistry, we provide a molecular-level explanation for the synergistic effects in sulfuric acid-dimethylamine-ammonia cluster formation. Because of the capability of ammonia to form more intermolecular interactions than dimethylamine, it can act as a bridge-former in sulfuric acid-dimethylamine clusters. In many cluster compositions, ammonia is more likely to be protonated than dimethylamine, although it is a weaker base. By nanoparticle formation rate simulations, we show that due to the synergistic effects, ammonia can increase the particle formation rate by up to 5 orders of magnitude compared to the two-component sulfuric acid-amine system.

  • 7. Myllys, Nanna
    et al.
    Kubecka, Jakub
    Besel, Vitus
    Alfaouri, Dina
    Olenius, Tinja
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för miljövetenskap och analytisk kemi.
    Norman Smith, James
    Passananti, Monica
    Role of base strength, cluster structure and charge in sulfuric-acid-driven particle formation2019Inngår i: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 19, nr 15, s. 9753-9768Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    In atmospheric sulfuric-acid-driven particle formation, bases are able to stabilize the initial molecular clusters and thus enhance particle formation. The enhancing potential of a stabilizing base is affected by different factors, such as the basicity and abundance. Here we use weak (ammonia), medium strong (dimethylamine) and very strong (guanidine) bases as representative atmospheric base compounds, and we systematically investigate their ability to stabilize sulfuric acid clusters. Using quantum chemistry, we study proton transfer as well as intermolecular interactions and symmetry in clusters, of which the former is directly related to the base strength and the latter to the structural effects. Based on the theoretical cluster stabilities and cluster population kinetics modeling, we provide molecular-level mechanisms of cluster growth and show that in electrically neutral particle formation, guanidine can dominate formation events even at relatively low concentrations. However, when ions are involved, charge effects can also stabilize small clusters for weaker bases. In this case the atmospheric abundance of the bases becomes more important, and thus ammonia is likely to play a key role. The theoretical findings are validated by cluster distribution experiments, as well as comparisons to previously reported particle formation rates, showing a good agreement.

  • 8. Myllys, Nanna
    et al.
    Olenius, Tinja
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för miljövetenskap och analytisk kemi.
    Kurtén, Theo
    Vehkamäki, Hanna
    Riipinen, Ilona
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för miljövetenskap och analytisk kemi.
    Elm, Jonas
    Effect of Bisulfate, Ammonia, and Ammonium on the Clustering of Organic Acids and Sulfuric Acid2017Inngår i: Journal of Physical Chemistry A, ISSN 1089-5639, E-ISSN 1520-5215, Vol. 121, nr 25, s. 4812-4824Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    We investigate the effect of the bisulfate anion HSO4-, ammonium cation NH4+, and ammonia NH3 on the clustering of sulfuric acid and pinic acid or 3-methyl-1,2,3-butanetricarboxylic acid (MBTCA). The systems were chosen based on their expected relevance in atmospheric new particle formation. Using quantum chemical methods together with kinetic calculations, we study the ability of these compounds to enhance cluster formation and growth. The cluster structures are obtained and frequencies are calculated using three different DFT functionals (M06-2X, PW91, and omega B97X-D) with the 6-31++G(d,p) basis set. The electronic energies are corrected using an accurate DLPNO-CCSD(T)/def2-QZVPP level of theory. The evaporation rates are evaluated based on the calculated Gibbs free energies. The interaction between the ions and sulfuric acid or carboxylic acid group is strong, and thereby small two-component ionic clusters are found to be very stable against evaporation. The presence of bisulfate stimulates the cluster formation through addition of the sulfuric acid, whereas the presence of ammonium favors the addition of organic acids. Bisulfate and ammonium enhance the first steps of cluster formation; however, at atmospheric conditions further cluster growth is limited due to the weak interaction and fast evaporation of the larger three-component clusters. On the basis of our results it is therefore unlikely that the studied organic acids and sulfuric acid, even together with bisulfate, ammonia, or ammonium can drive new-particle formation via clustering mechanisms. Other mechanisms such as chemical reactions are needed to explain observed new-particle formation events in the presence of oxidized organic compounds resembling the acids studied here.

  • 9. Myllys, Nanna
    et al.
    Ponkkonen, Tuomo
    Passananti, Monica
    Elm, Jonas
    Vehkämaki, Hanna
    Olenius, Tinja
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för miljövetenskap och analytisk kemi.
    Guanidine: A Highly Efficient Stabilizer in Atmospheric New-Particle Formation2018Inngår i: Journal of Physical Chemistry A, ISSN 1089-5639, E-ISSN 1520-5215, Vol. 122, nr 20, s. 4717-4729Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    The role of a strong organobase, guanidine, in sulfuric acid-driven new-particle formation is studied using state-of-the-art quantum chemical methods and molecular cluster formation simulations. Cluster formation mechanisms at the molecular level are resolved, and theoretical results on cluster stability are confirmed with mass spectrometer measurements. New-particle formation from guanidine and sulfuric acid molecules occurs without thermodynamic barriers under studied conditions, and clusters are growing close to a 1:1 composition of acid and base. Evaporation rates of the most stable clusters are extremely low, which can be explained by the proton transfers and symmetrical cluster structures. We compare the ability of guanidine and dimethylamine to enhance sulfuric acid-driven particle formation and show that more than 2000-fold concentration of dimethylamine is needed to yield as efficient particle formation as in the case of guanidine. At similar conditions, guanidine yields 8 orders of magnitude higher particle formation rates compared to dimethylamine. Highly basic compounds such as guanidine may explain experimentally observed particle formation events at low precursor vapor concentrations, whereas less basic and more abundant bases such as ammonia and amines are likely to explain measurements at high concentrations.

  • 10.
    Olenius, Tinja
    et al.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för miljövetenskap och analytisk kemi.
    Halonen, Roope
    Kurtén, Theo
    Henschel, Henning
    Kupiainen-Määtä, Oona
    Ortega, Ismael K.
    Jen, Coty N.
    Vehkamäki, Hanna
    Riipinen, Ilona
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för miljövetenskap och analytisk kemi.
    New particle formation from sulfuric acid and amines: Comparison of monomethylamine, dimethylamine, and trimethylamine2017Inngår i: Journal of Geophysical Research - Atmospheres, ISSN 2169-897X, E-ISSN 2169-8996, Vol. 122, nr 13, s. 7103-7118Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    Amines are bases that originate from both anthropogenic and natural sources, and they are recognized as candidates to participate in atmospheric aerosol particle formation together with sulfuric acid. Monomethylamine, dimethylamine, and trimethylamine (MMA, DMA, and TMA, respectively) have been shown to enhance sulfuric acid-driven particle formation more efficiently than ammonia, but both theory and laboratory experiments suggest that there are differences in their enhancing potentials. However, as quantitative concentrations and thermochemical properties of different amines remain relatively uncertain, and also for computational reasons, the compounds have been treated as a single surrogate amine species in large-scale modeling studies. In this work, the differences and similarities of MMA, DMA, and TMA are studied by simulations of molecular cluster formation from sulfuric acid, water, and each of the three amines. Quantum chemistry-based cluster evaporation rate constants are applied in a cluster population dynamics model to yield cluster concentrations and formation rates at boundary layer conditions. While there are differences, for instance, in the clustering mechanisms and cluster hygroscopicity for the three amines, DMA and TMA can be approximated as a lumped species. Formation of nanometer-sized particles and its dependence on ambient conditions is roughly similar for these two: both efficiently form clusters with sulfuric acid, and cluster formation is rather insensitive to changes in temperature and relative humidity. Particle formation from sulfuric acid and MMA is weaker and significantly more sensitive to ambient conditions. Therefore, merging MMA together with DMA and TMA introduces inaccuracies in sulfuric acid-amine particle formation schemes.

  • 11.
    Olenius, Tinja
    et al.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för miljövetenskap och analytisk kemi.
    Pichelstorfer, Lukas
    Stolzenburg, Dominik
    Winkler, Paul M.
    Lehtinen, Kari E. J.
    Riipinen, Ilona
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för miljövetenskap och analytisk kemi.
    Robust metric for quantifying the importance of stochastic effects on nanoparticle growth2018Inngår i: Scientific Reports, ISSN 2045-2322, E-ISSN 2045-2322, Vol. 8, artikkel-id 14160Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    Comprehensive representation of nanoparticle dynamics is necessary for understanding nucleation and growth phenomena. This is critical in atmospheric physics, as airborne particles formed from vapors have significant but highly uncertain effects on climate. While the vapor-particle mass exchange driving particle growth can be described by a macroscopic, continuous substance for large enough particles, the growth dynamics of the smallest nanoparticles involve stochastic fluctuations in particle size due to discrete molecular collision and decay processes. To date, there have been no generalizable methods for quantifying the particle size regime where the discrete effects become negligible and condensation models can be applied. By discrete simulations of sub-10 nm particle populations, we demonstrate the importance of stochastic effects in the nanometer size range. We derive a novel, theory-based, simple and robust metric for identifying the exact sizes where these effects cannot be omitted for arbitrary molecular systems. The presented metric, based on examining the second- and first-order derivatives of the particle size distribution function, is directly applicable to experimental size distribution data. This tool enables quantifying the onset of condensational growth without prior information on the properties of the vapors and particles, thus allowing robust experimental resolving of nanoparticle formation physics.

  • 12.
    Olenius, Tinja
    et al.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för miljövetenskap och analytisk kemi.
    Riipinen, Ilona
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för miljövetenskap och analytisk kemi.
    Molecular-resolution simulations of new particle formation: Evaluation of common assumptions made in describing nucleation in aerosol dynamics models2017Inngår i: Aerosol Science and Technology, ISSN 0278-6826, E-ISSN 1521-7388, Vol. 51, nr 4, s. 397-408Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    Aerosol dynamics models that describe the evolution of a particle distribution incorporate nucleation as a particle formation rate at a small size around a few nanometers in diameter. This rate is commonly obtained from molecular models that cover the distribution below the given formation size - although in reality the distribution of nanometer-sized particles cannot be unambiguously divided into separate sections of particle formation and growth. When incorporating nucleation, the distribution below the formation size is omitted, and the formation rate is assumed to be in a steady state. In addition, to reduce the modeled size range, the formation rate is often scaled to a larger size based on estimated growth and scavenging rates and the assumption that also the larger size is in a steady state. This work evaluates these assumptions by simulating sub-10 nm particle distributions in typical atmospheric conditions with an explicit molecular-resolution model. Particle formation is included either (1) dynamically, that is, the whole size range starting from single vapor molecules is modeled explicitly or (2) implicitly by using an input formation rate as is done in aerosol models. The results suggest that while each assumption can affect the outcome of new particle formation modeling, the most significant source of uncertainty affecting the formation rates and resulting nanoparticle concentrations is the steady-state assumption, which may lead to an overprediction of the concentrations by factors of approximately from two to even orders of magnitude. This can have implications for modeling and predicting atmospheric particle formation.

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