M. Kulmala, D. Aliaga, Santeri Tuovinen, Runlong Cai, H. Junninen, Chao Yan, Federico Bianchi, Yafang Cheng, Aijun Ding, Doug Worsnop, T. Petäjä, K. Lehtipalo, P. Paasonen, V. Kerminen
{"title":"Opinion: A paradigm shift in investigating the general characteristics of atmospheric new particle formation using field observations","authors":"M. Kulmala, D. Aliaga, Santeri Tuovinen, Runlong Cai, H. Junninen, Chao Yan, Federico Bianchi, Yafang Cheng, Aijun Ding, Doug Worsnop, T. Petäjä, K. Lehtipalo, P. Paasonen, V. Kerminen","doi":"10.5194/ar-2-49-2024","DOIUrl":"https://doi.org/10.5194/ar-2-49-2024","url":null,"abstract":"Abstract. Atmospheric new particle formation (NPF) and associated production of secondary particulate matter dominate aerosol particle number concentrations and submicron particle mass loadings in many environments globally. Our recent investigations show that atmospheric NPF produces a significant amount of particles on days when no clear NPF event has been observed/identified. Furthermore, it has been observed in different environments all around the world that growth rates of nucleation mode particles vary little, usually much less than the measured concentrations of condensable vapors. It has also been observed that the local clustering, which in many cases acts as a starting point of regional new particle formation (NPF), can be described with the formation of intermediate ions at the smallest sizes. These observations, together with a recently developed ranking method, lead us to propose a paradigm shift in atmospheric NPF investigations. In this opinion paper, we will summarize the traditional approach of describing atmospheric NPF and describe an alternative method, covering both particle formation and initial growth. The opportunities and remaining challenges offered by the new approach are discussed.\u0000","PeriodicalId":511317,"journal":{"name":"Aerosol Research","volume":"25 7","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140375436","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Marie Kathrine Mikkelsen, Jesper Liisberg, Maarten M. J. W. van Herpen, Kurt V. Mikkelsen, M. S. Johnson
{"title":"Photocatalytic chloride-to-chlorine conversion by ionic iron in aqueous aerosols: a combined experimental, quantum chemical, and chemical equilibrium model study","authors":"Marie Kathrine Mikkelsen, Jesper Liisberg, Maarten M. J. W. van Herpen, Kurt V. Mikkelsen, M. S. Johnson","doi":"10.5194/ar-2-31-2024","DOIUrl":"https://doi.org/10.5194/ar-2-31-2024","url":null,"abstract":"Abstract. Prior aerosol chamber experiments show that the ligand-to-metal charge transfer absorption in iron(III) chlorides can lead to the production of chlorine (Cl2/Cl). Based on this mechanism, the photocatalytic oxidation of chloride (Cl−) in mineral dust–sea spray aerosols was recently shown to be the largest source of chlorine over the North Atlantic. However, there has not been a detailed analysis of the mechanism that includes the aqueous formation equilibria and the absorption spectra of the iron chlorides nor has there been an analysis of which iron chloride is the main chromophore. Here we present the results of experiments measuring the photolysis of FeCl3 ⋅ 6H2O in specific wavelength bands, an analysis of the absorption spectra of FeCln3-n (n=1 … 4) made using density functional theory, and the results of an aqueous-phase model that predicts the abundance of the iron chlorides with changes in pH and iron concentrations. Transition state analysis is used to determine the energy thresholds of the dissociations of the species. Based on a speciation model with conditions extending from dilute water droplets and acidic seawater droplets to brine and salty crust, as well as the absorption rates and dissociation thresholds, we find that FeCl2+ is the most important species for chlorine production for a wide range of conditions. The mechanism was found to be active in the range of 400 to 530 nm, with a maximum around 440 nm. We conclude that iron chlorides will form in atmospheric aerosols from the combination of iron(III) cations with chloride and that they will be activated by sunlight, generating chlorine (Cl2/Cl) from chloride (Cl−) in a process that is catalytic in both chlorine and iron.\u0000","PeriodicalId":511317,"journal":{"name":"Aerosol Research","volume":"26 10","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140229839","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Opinion: Should high-resolution differential mobility analyzers be used in mainstream aerosol studies?","authors":"J. Fernández de la Mora","doi":"10.5194/ar-2-21-2024","DOIUrl":"https://doi.org/10.5194/ar-2-21-2024","url":null,"abstract":"Abstract. Differential mobility analyzers (DMAs) are widely used instruments to measure the size distributions of submicron aerosols. High-resolution DMAs (HRDMAs) are defined here as plain DMAs maintaining a steady flow over an unusually broad range of sheath gas flow rates Q. HRDMAs, first developed by Georg Reischl's group, have existed for a long time. However, they have not been widely adopted, except in the size range below 10 nm, often in new particle formation studies. Here we question the commonly held view that HRDMAs are necessarily complex, bulky and expensive machines, mainly of interest in exotic applications outside mainstream aerosol research. Rather, many studies central to aerosol research could be carried out with HRDMAs with considerable advantage in size range, resolution, sensitivity and measurement speed. DMA manufacturers will hopefully take the challenge of developing commercial HRDMAs of complexity and cost comparable to those of today's commercial instruments, adapted for broad use by aerosol scientists, though with greatly improved flexibility and performance. Some of the technical challenges that still need to be overcome are discussed, such as the development of high-flow condensation counter detectors, and the control of high sample and sheath gas flow rates.\u0000","PeriodicalId":511317,"journal":{"name":"Aerosol Research","volume":"284 5","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140427651","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
J. Sulo, J. Enroth, A. Pajunoja, J. Vanhanen, K. Lehtipalo, T. Petäjä, M. Kulmala
{"title":"Pushing nano-aerosol measurements towards a new decade – technical note on the Airmodus particle size magnifier 2.0","authors":"J. Sulo, J. Enroth, A. Pajunoja, J. Vanhanen, K. Lehtipalo, T. Petäjä, M. Kulmala","doi":"10.5194/ar-2-13-2024","DOIUrl":"https://doi.org/10.5194/ar-2-13-2024","url":null,"abstract":"Abstract. Accurate measurement of the size distribution of sub-10 nm aerosol particles is still a challenge. Here we introduce a novel version of the Airmodus particle size magnifier (PSM 2.0), which is a condensation-particle-counter-based instrument with a sizing range of 1–12 nm. The extended size range compared to the earlier PSM version enables the direct detection of forming clusters and particles as well as the study of their growth processes without the challenges related to particle charging. It also gives an overlap between the activation size distribution measurements with the PSM and mobility size distribution measurements with conventional mobility particle sizers. We compared the performance of PSM 2.0 to that of a mobility particle size spectrometer, the original A10 particle size magnifier, and a Neutral cluster and Air Ion Spectrometer (NAIS) during field measurements. Also, calibration results were compared against the A10 instrument. The results show that PSM 2.0 is able to activate sub-2 nm clusters and that the concentration and size distribution between 2–12 nm compare well, especially with the NAIS.\u0000","PeriodicalId":511317,"journal":{"name":"Aerosol Research","volume":"253 ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140445959","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Evaluation of a Partector Pro for atmospheric particle number size distribution and number concentration measurements at an urban background site","authors":"C. Asbach, A. Todea, Heinz Kaminski","doi":"10.5194/ar-2-1-2024","DOIUrl":"https://doi.org/10.5194/ar-2-1-2024","url":null,"abstract":"Abstract. Particle number size distributions, total number concentrations and mean particle sizes have been measured for 70 d at an urban background site in Mülheim-Styrum, Germany, with a handheld Partector Pro of the first generation and a TSI mobility particle size spectrometer (MPSS). The aim of the study was to evaluate the performance of the Partector Pro against the MPSS. The results show that the size distributions, measured with the Partector Pro, agree with the MPSS mostly within ± 25 % for particle sizes between 10 and 113.5 nm, whereas higher, systematic differences were observed for larger particles. The measurement accuracy was shown to be dependent on the geometric mean diameter and the geometric standard deviation of the aerosol. Best results were found for the most abundant size distributions with geometric mean particle diameters ≥ 30 nm and geometric standard deviations larger than 1.8. The total number concentration, measured by the Partector Pro, was found to be in excellent agreement with the MPSS with a slope of the linear fit of 0.9977 and a regression coefficient of R2=0.9956. The agreement of the geometric mean particle diameter, determined with the Partector Pro and the MPSS was good but moderately dependent on the particle size distribution. For mean particle sizes between 20 and 50 nm, the bias was within ±15 %. Higher deviations of up to 30 % were observed when the geometric mean particle sizes exceeded 70 nm and when the geometric standard deviations exceeded approximately 2.7.\u0000","PeriodicalId":511317,"journal":{"name":"Aerosol Research","volume":" 7","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139617211","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}