Browsing by Subject "new particle formation"

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  • Mohr, Claudia; Lopez-Hilfiker, Felipe D.; Yli-Juuti, Taina; Heitto, Arto; Lutz, Anna; Hallquist, Mattias; D'Ambro, Emma L.; Rissanen, Matti P.; Hao, Liqing; Schobesberger, Siegfried; Kulmala, Markku; Mauldin III, Roy L.; Makkonen, Ulla; Sipilä, Mikko; Petäjä, Tuukka; Thornton, Joel A. (2017)
    We present ambient observations of dimeric monoterpene oxidation products (C16-20HyO6-9) in gas and particle phases in the boreal forest in Finland in spring 2013 and 2014, detected with a chemical ionization mass spectrometer with a filter inlet for gases and aerosols employing acetate and iodide as reagent ions. These are among the first online dual-phase observations of such dimers in the atmosphere. Estimated saturation concentrations of 10(-15) to 10(-6)mu gm(-3) (based on observed thermal desorptions and group-contribution methods) and measured gas-phase concentrations of 10(-3) to 10(-2)mu gm(-3) (similar to 10(6)-10(7)moleculescm(-3)) corroborate a gas-phase formation mechanism. Regular new particle formation (NPF) events allowed insights into the potential role dimers may play for atmospheric NPF and growth. The observationally constrained Model for Acid-Base chemistry in NAnoparticle Growth indicates a contribution of similar to 5% to early stage particle growth from the similar to 60 gaseous dimer compounds. Plain Language Summary Atmospheric aerosol particles influence climate and air quality. We present new insights into how emissions of volatile organic compounds from trees are transformed in the atmosphere to contribute to the formation and growth of aerosol particles. We detected for the first time over a forest, a group of organic molecules, known to grow particles, in the gas phase at levels far higher than expected. Previous measurements had only measured them in the particles. This finding provides guidance on how models of aerosol formation and growth should describe their appearance and fate in the atmosphere.
  • Lu, Yiqun; Liu, Ling; Ning, An; Yang, Gan; Liu, Yiliang; Kurten, Theo; Vehkamäki, Hanna; Zhang, Xiuhui; Wang, Lin (2020)
    Sulfuric acid (SA)-dimethylamine (DMA)-H2O cluster formation has been proven to be responsible for a significant part of new particle formation (NPF) in a Chinese megacity. However, the possible involvement of common atmospheric acids in the subsequent growth of SA-DMA clusters remains elusive. We simulated formation and growth of clusters using atmospheric relevant concentrations of SA, DMA, and trifluoroacetic acid (TFA), a commonly observed atmospheric perfluorocarboxylic acid, using Density Functional Theory combined with Atmospheric Cluster Dynamics Code. The presence of TFA leads to complex cluster formation routes and an enhancement of NPF rates by up to 2.3 ([TFA] = 5.0 x 10(6) molecules cm(-3), [SA] = 1.0 x 10(6) molecules cm(-3), and [DMA] = 1.5 x 10(9) molecules cm(-3)). The agreement of (SA)(1)center dot(DMA)(1-2)center dot(TFA)(1) concentrations between simulations and ambient measurements during NPF events validates model predictions and implies that perfluorocarboxylic acids could potentially boost atmospheric SA-DMA NPF rates.
  • Clusius, Petri (Helsingin yliopisto, 2020)
    This thesis presents the Atmospherically Relevant Chemistry and Aerosol Box Model (ARCA box), which is used for simulating atmospheric chemistry and the time evolution of aerosol particles and the formation of stable molecular clusters. The model can be used for example in solving of the concentrations of atmospheric trace gases formed from some predefined precursors, simulation and design of smog chamber experiments or indoor air quality estimation. The backbone of ARCAs chemical library comes from Master Chemical Mechanism (MCM), extended with Peroxy Radical Autoxidation Mechanism (PRAM), and is further extendable with any new reactions. Molecular clustering is simulated with the Atmospheric Cluster Dynamics Code (ACDC). The particle size distribution is represented with two alternative methods whose size and grid density are fully configurable. The evolution of the particle size distribution due to the condensation of low volatile organic vapours and the Brownian coagulation is simulated using established kinetic and thermodynamic theories. The user interface of ARCA differs considerably from the previous comparable models. The model has a graphical user interface which improves its usability and repeatability of the simulations. The user interface increases the potential of ARCA being used also outside the modelling community, for example in the experimental atmospheric sciences or by authorities.
  • Kivekäs, Niku; Carpman, Jimmie; Roldin, Pontus; Leppa, Johannes; O'Connor, Ewan; Kristensson, Adam; Asmi, Eija (2016)
    Field observations of new particle formation and the subsequent particle growth are typically only possible at a fixed measurement location, and hence do not follow the temporal evolution of an air parcel in a Lagrangian sense. Standard analysis for determining formation and growth rates requires that the time-dependent formation rate and growth rate of the particles are spatially invariant; air parcel advection means that the observed temporal evolution of the particle size distribution at a fixed measurement location may not represent the true evolution if there are spatial variations in the formation and growth rates. Here we present a zero-dimensional aerosol box model coupled with one-dimensional atmospheric flow to describe the impact of advection on the evolution of simulated new particle formation events. Wind speed, particle formation rates and growth rates are input parameters that can vary as a function of time and location, using wind speed to connect location to time. The output simulates measurements at a fixed location; formation and growth rates of the particle mode can then be calculated from the simulated observations at a stationary point for different scenarios and be compared with the 'true' input parameters. Hence, we can investigate how spatial variations in the formation and growth rates of new particles would appear in observations of particle number size distributions at a fixed measurement site. We show that the particle size distribution and growth rate at a fixed location is dependent on the formation and growth parameters upwind, even if local conditions do not vary. We also show that different input parameters used may result in very similar simulated measurements. Erroneous interpretation of observations in terms of particle formation and growth rates, and the time span and areal extent of new particle formation, is possible if the spatial effects are not accounted for.
  • Lawler, Michael J.; Rissanen, Matti P.; Ehn, Mikael; Mauldin, R. Lee; Sarnela, Nina; Sipilä, Mikko; Smith, James N. (2018)
    New particle formation (NPF) is an important contributor to particle number in many locations, but the chemical drivers for this process are not well understood. Daytime NPF events occur regularly in the springtime Finnish boreal forest and strongly impact aerosol abundance. In April 2014 size-resolved chemical measurements of ambient nanoparticles were made using the Time-of-Flight Thermal Desorption Chemical ionization Mass Spectrometer and we report results from two NPF events. While growth overall was dominated by terpene oxidation products, newly formed 20-70nm particles showed enhancement in apparent alkanoic acids. The events occurred on days with rapid transport of marine air, which correlated with low background aerosol loading and higher gas phase methanesulfonic acid levels. These results are broadly consistent with previous studies on Nordic NPF but indicate that further attention should be given to the sources and role of non-terpenoid organics and the possible contribution of transported marine compounds in this process. Plain Language Summary Clouds are an enormously important part of the climate system because they control the radiation entering and leaving the Earth. Clouds form as water condenses onto small particles called cloud condensation nuclei. These particles can be directly emitted from the Earth's surface, like sea spray, for example, or they can form in the atmosphere out of precursor gases. We have measured the composition of these atmosphere-formed particles to understand better how this process works in the Nordic boreal forest. We found that a diverse mix of processes and molecules are likely involved, possibly including the transport of materials from the ocean. While these results will ultimately lead to a better understanding of ocean-land-cloud interactions, they currently indicate that more work is needed to learn the processes involved.
  • Sahyoun, Maher; Freney, Evelyn; Brito, Joel; Duplissy, Jonathan; Gouhier, Mathieu; Colomb, Aurélie; Dupuy, Regis; Bourianne, Thierry; Nowak, John B.; Yan, Chao; Petäjä, Tuukka; Kulmala, Markku; Schwarzenboeck, Alfons; Planche, Céline; Sellegri, Karine (2019)
    Abstract Volcanic emissions can significantly affect the Earth's radiation budget by emitting aerosol particles and gas-phase species that can result in the new particle formation (NPF). These particles can scatter solar radiation or modify cloud properties, with consequences on health, weather, and climate. To our knowledge, this is the first dedicated study detailing how gas-phase precursors emitted from volcanic plumes can influence the NPF. A series of airborne measurements were performed around the Etna and Stromboli volcanoes within the framework of the CLerVolc and STRAP projects. The ATR-42 aircraft was equipped with a range of instrumentation allowing the measurement of particle number concentration in diameter range above 2.5 nm, and gaseous species to investigate the aerosol dynamics and the processes governing the NPF and their growth within the volcanic plumes. We demonstrate that NPF occurs within the volcanic plumes in the Free Troposphere (FT) and Boundary Layer (BL). Typically, the NPF events were more pronounced in the FT, where the condensational sink was up to two orders of magnitude smaller and the temperature was ~20°C lower than in the BL. Within the passive volcanic plume, the concentration of sulfur dioxide, sulfuric acid, and N2.5 were as high as 92 ppbV, 5.65?108 and 2.4?105 cm?3, respectively. Using these measurements, we propose a new parameterization for NPF rate (J2.5) within the passive volcanic plume in the FT. These results can be incorporated into mesoscale models to better assess the impact of the particle formed by natural processes, i.e. volcanic plumes, on climate.
  • Deng, Yange; Kagami, Sara; Ogawa, Shuhei; Kawana, Kaori; Nakayama, Tomoki; Kubodera, Ryo; Adachi, Kouji; Hussein, Tareq; Miyazaki, Yuzo; Mochida, Michihiro (2018)
    The formation of biogenic secondary organic aerosols (BSOAs) in forest environments is potentially important to cloud formation via changes of the cloud condensation nuclei (CCN) activity of aerosols. In this study, the CCN activation of submicrometer aerosols and their chemical compositions and size distributions were measured at a midlatitude forest site in Japan during the summer of 2014 to assess the hygroscopicity of the organic aerosols and their contributions to the local CCN concentrations. The mean number concentrations of the condensation nuclei and CCN at supersaturation (SS) conditions of 0.11-0.80% were 1,238 and 166-740cm(-3), respectively. Organic aerosols and sulfate dominated the submicrometer aerosol mass concentrations. The particle hygroscopicity increased with increases in particle diameters. The hygroscopicity parameter for the organics, (org), was positively correlated with the atomic O to C ratio. The product of (org) and the volume fraction of OA was 0.12, accounting for 38% of the water uptake by aerosol particles. The hygroscopicity parameter of the locally formed fresh BSOA was estimated to be 0.09. The contribution of OA to the CCN number concentration, which was assessed by subtracting the CCN concentration of the hypothetical inorganic aerosols from that of the ambient aerosols, was 50-182cm(-3) for the SS range of 0.11-0.80%. The increase of the CCN number concentrations per 1-g/m(3) increase of the BSOA was 23-299cm(-3) at 0.11-0.80% SS. The contribution of the BSOA to the CCN number concentration can be enhanced by new particle formation. Plain Language Summary Some of the particles suspended in the atmosphere can absorb water vapors around them and act as nuclei to form cloud droplets. These particles are called cloud condensation nuclei (CCN), the quantification of which is important for climate forcing prediction. The ability of a particle to absorb water is referred to as hygroscopicity, which is governed by the chemical composition. Volatile organic vapors emitted by vegetation (i.e., biogenic volatile organic compound) after chemical reactions in the atmosphere can either condense onto existing particles or participate in the formation of new particles and thus change the aerosol chemical composition. The aerosol component originated from biogenic volatile organic compounds, named biogenic secondary organic aerosol (BSOA), is an important constituent of CCN on a global scale. However, the hygroscopicity of BSOA and its contribution to CCN are not understood well. We performed measurements of the hygroscopicity and chemical composition of aerosol particles in a forest in Japan. Based on the observation, we calculated the hygroscopicity of the BSOA formed in the forest and quantified the contribution of the BSOA to the CCN number concentrations. An enhancement of the contribution of BSOA to the CCN number concentrations by new particle formation is suggested, which is an important subject of future studies.
  • Lee, Shan-Hu; Gordon, Hamish; Yu, Huan; Lehtipalo, Katrianne; Haley, Ryan; Li, Yixin; Zhang, Renyi (2019)
    New particle formation (NPF) represents the first step in the complex processes leading to formation of cloud condensation nuclei. Newly formed nanoparticles affect human health, air quality, weather, and climate. This review provides a brief history, synthesizes recent significant progresses, and outlines the challenges and future directions for research relevant to NPF. New developments include the emergence of state-of-the-art instruments that measure prenucleation clusters and newly nucleated nanoparticles down to about 1 nm; systematic laboratory studies of multicomponent nucleation systems, including collaborative experiments conducted in the Cosmics Leaving Outdoor Droplets chamber at CERN; observations of NPF in different types of forests, extremely polluted urban locations, coastal sites, polar regions, and high-elevation sites; and improved nucleation theories and parameterizations to account for NPF in atmospheric models. The challenges include the lack of understanding of the fundamental chemical mechanisms responsible for aerosol nucleation and growth under diverse environments, the effects of SO2 and NOx on NPF, and the contribution of anthropogenic organic compounds to NPF. It is also critical to develop instruments that can detect chemical composition of particles from 3 to 20 nm and improve parameterizations to represent NPF over a wide range of atmospheric conditions of chemical precursor, temperature, and humidity. Plain Language Summary In the atmosphere, invisible to the human eye, there are many microscopic particles, or nanoparticles, that affect human health, air quality, and climate. We do not fully understand the chemical processes that allow these fine particles to form and be suspended in the air nor how they influence heat flow in Earth's atmosphere. Laboratory experiments, field observations, and modeling simulations have all shown different results for how these particles behave. These inconsistencies make it difficult to accurately represent the processes of new particle formation in regional and global atmospheric models. Scientists still need to develop instruments that can measure the smallest range of nanoparticles and to find ways to describe particle formation that allow for differences in temperature, humidity, and level of pollution.
  • Lehmusjärvi, Tuuli (Helsingin yliopisto, 2022)
    The effects of atmospheric aerosol particles on Earth’s radiative balance are mainly cooling, which is mostly due their indirect effects with clouds. In the Arctic more than half of the cloud condensation nuclei (CCN) production is originated from secondary aerosols, and to further the understanding of Arctic climate and its changes due to the global warming, it is necessary to better understand the secondary aerosol processes there. Highly oxygenated organic molecules (HOM) are known to be important for the formation and especially for the growth of newly formed secondary aerosols to climate relevant sizes. Because of the low volatilities of HOM, they can condense onto the smallest particles, which is crucial for the growth of the new particles. Volatile organic compounds (VOC), especially monoterpenes, are known to be sources of HOM in boreal forest, but in the Arctic where the vegetation is scarce the sources of HOM have not yet been identified. The processes related to secondary aerosol formation in the Arctic are still not fully understood. Especially the observations of HOM and their sources are lacking. Recent studies in Ny-Ålesund, Svalbard showed that multiple aerosol precursors are found to be present in the Arctic atmosphere, as well as contributing to the early stages of the formation of secondary particles. However, more molecular scale observations of aerosol precursors are still needed to form a full picture of the Arctic climate processes. In this thesis, the different aerosol precursors and their contributions to the new particle formations in high Arctic location Ny-Ålesund, Svalbard were analysed. Chemical compositions of HOM were identified for the first time from Arctic atmosphere, and their contributions to new particle formation in high Arctic location were investigated. Because of the high concentrations of HOM during the observed NPF events, it can be suggested that they were contributing to the nucleation of aerosol particles. Particle growth rate calculation shows that the HOM present in the study site were responsible for up to 50% of the total growth of the newly formed particles. VOC flux measurements done in same location were also analysed, and Arctic tundra in Svalbard was found out to be a source of at least four different VOC. Furthermore, the identified HOM were linked to the VOC flux measurements, suggesting a possible link between Arctic VOC and HOM.
  • Wu, Hao; Li, Zhanqing; Li, Hanqing; Luo, Kun; Wang, Yuying; Yan, Peng; Hu, Fei; Zhang, Fang; Sun, Yele; Shang, Dongjie; Liang, Chunsheng; Zhang, Dongmei; Wei, Jing; Wu, Tong; Jin, Xiaoai; Fan, Xinxin; Cribb, Maureen; Fischer, Marc L.; Kulmala, Markku; Petäjä, Tuukka (2021)
    A new mechanism of new particle formation (NPF) is investigated using comprehensive measurements of aerosol physicochemical quantities and meteorological variables made in three continents, including Beijing, China; the Southern Great Plains site in the USA; and SMEAR II Station in Hyytiala, Finland. Despite the considerably different emissions of chemical species among the sites, a common relationship was found between the characteristics of NPF and the stability intensity. The stability parameter (zeta = Z/L, where Z is the height above ground and L is the Monin-Obukhov length) is found to play an important role; it drops significantly before NPF as the atmosphere becomes more unstable, which may serve as an indicator of nucleation bursts. As the atmosphere becomes unstable, the NPF duration is closely related to the tendency for turbulence development, which influences the evolution of the condensation sink. Presumably, the unstable atmosphere may dilute pre-existing particles, effectively reducing the condensation sink, especially at coarse mode to foster nucleation. This new mechanism is confirmed by model simulations using a molecular dynamic model that mimics the impact of turbulence development on nucleation by inducing and intensifying homogeneous nucleation events.
  • Yan, Chao; Yin, Rujing; Lu, Yiqun; Dada, Lubna; Yang, Dongsen; Fu, Yueyun; Kontkanen, Jenni; Deng, Chenjuan; Garmash, Olga; Ruan, Jiaxin; Baalbaki, Rima; Schervish, Meredith; Cai, Runlong; Bloss, Matthew; Chan, Tommy; Chen, Tianzeng; Chen, Qi; Chen, Xuemeng; Chen, Yan; Chu, Biwu; Dällenbach, Kaspar; Foreback, Benjamin; He, Xucheng; Heikkinen, Liine; Jokinen, Tuija; Junninen, Heikki; Kangasluoma, Juha; Kokkonen, Tom; Kurppa, Mona; Lehtipalo, Katrianne; Li, Haiyan; Li, Hui; Li, Xiaoxiao; Liu, Yiliang; Ma, Qingxin; Paasonen, Pauli; Rantala, Pekka; Pileci, Rosaria E.; Rusanen, Anton; Sarnela, Nina; Simonen, Pauli; Wang, Shixian; Wang, Weigang; Wang, Yonghong; Xue, Mo; Yang, Gan; Yao, Lei; Zhou, Ying; Kujansuu, Joni; Petäjä, Tuukka; Nie, Wei; Ma, Yan; Ge, Maofa; He, Hong; Donahue, Neil M.; Worsnop, Douglas R.; Kerminen, Veli-Matti; Wang, Lin; Liu, Yongchun; Zheng, Jun; Kulmala, Markku; Jiang, Jingkun; Bianchi, Federico (2021)
    Intense and frequent new particle formation (NPF) events have been observed in polluted urban environments, yet the dominant mechanisms are still under debate. To understand the key species and governing processes of NPF in polluted urban environments, we conducted comprehensive measurements in downtown Beijing during January-March, 2018. We performed detailed analyses on sulfuric acid cluster composition and budget, as well as the chemical and physical properties of oxidized organic molecules (OOMs). Our results demonstrate that the fast clustering of sulfuric acid (H2SO4) and base molecules triggered the NPF events, and OOMs further helped grow the newly formed particles toward climate- and health-relevant sizes. This synergistic role of H2SO4, base species, and OOMs in NPF is likely representative of polluted urban environments where abundant H2SO4 and base species usually co-exist, and OOMs are with moderately low volatility when produced under high NOx concentrations.
  • Kulmala, Markku; Stolzenburg, Dominik; Dada, Lubna; Cai, Runlong; Kontkanen, Jenni; Yan, Chao; Kangasluoma, Juha; Ahonen, Lauri; Gonzalez-Carracedo, Loïc; Sulo, Juha; Tuovinen, Santeri Otto Luukas; Deng, Chenjuan; Li, Yiran; Lehtipalo, Katrianne; Lehtinen, Kari E. J.; Petäjä, Tuukka; Winkler, Paul M.; Jiang, Jingkun; Kerminen, Veli-Matti (2021)
    Atmospheric clusters play a key role in atmospheric new particle formation and they are a sensitive indicator for atmospheric chemistry. Both the formation and loss of atmospheric clusters include a complex set of interlinked physical and chemical processes, and therefore their dynamics is highly non-linear. Here we derive a set of simple equations to estimate the atmospheric cluster concentrations in size ranges of 1.5–2 nm and 2–3 nm as well as 3–6 nm aerosol particles. We compared the estimated concentrations with measured ones both in a boreal forest site (the SMEAR II station in Hyytiälä, Finland) and in an urban site (the AHL/BUCT station in Beijing, China). We made this comparison first for 3–6 nm particles, since in this size range observations are more reliable than at smaller sizes, and then repeated it for the 2–3 nm size range. Finally, we estimated cluster concentrations in the 1.5–2 nm size range. Our main finding is that the present observations are able to detect a major fraction of existing atmospheric clusters.