How to reliably detect molecular clusters and nucleation mode particles with Neutral cluster and Air Ion Spectrometer (NAIS)

To understand the very first steps of atmospheric particle formation and growth processes, information on the size where the atmospheric nucleation and cluster activation occurs, is crucially needed. The current understanding of the concentrations and dynamics of charged and neutral clusters and particles is based on theoretical predictions and experimental observations. This paper gives a standard operation procedure (SOP) for Neutral cluster and Air Ion Spectrometer (NAIS) measurements and data processing. With the NAIS data, we have improved the scientific understanding by (1) direct detection of freshly formed atmospheric clusters and particles, (2) linking experimental observations and theoretical framework to understand the formation and growth mechanisms of aerosol particles, and (3) parameterizing formation and growth mechanisms for atmospheric models. The SOP provides tools to harmonize the world-wide measurements of small clusters and nucleation mode particles and to verify consistent results measured by the NAIS users. The work is based on discussions and interactions between the NAIS users and the NAIS manufacturer.Peer reviewe

On the accuracy of ion measurements using a neutral cluster and air ion spectrometer

Here, we present a calibration of the Neutral cluster and Air Ion Spectrometer (NAIS, Airel Ltd.) for the size and concentration of ions in the mobility-diameter size-range 0.98-29.1 nm. Previous studies raised accuracy issues in size and concentration determination and highlighted the importance of used data inversion algorithm. Therefore, we investigated the performance of the NAIS by using five inversion methods. The presented results illustrate that the size information given by the NAIS is very accurate, regardless of the version of the data inversion. The number concentrations determined by the NAIS were 15%-30% too low especially at the lower end of the measurement size range (<5 nm), whereas concentrations at diameters 19.6 nm and larger were overestimated by up to 8%. With the correction presented in this study, the uncertainty of the ion concentration measurement of the NAIS can be reduced to less than 10%, allowing the NAIS to be used in quantitative ion cluster studies and more accurate determination of formation and growth rates.Peer reviewe

Characteristics of new-particle formation at three SMEAR stations

We analyzed the size distributions of atmospheric aerosol particles measured during 2013-2014 at Varrio (SMEAR I) in northern Finland, Hyytiala (SMEAR II) in southern Finland and Jarvselja (SMEAR-Estonia) in Estonia. The stations are located on a transect spanning from north to south over 1000 km and they represent different environments ranging from subarctic to the hemi-boreal. We calculated the characteristics of new-particle-formation events, such as the frequency of events, growth rate of nucleation mode particles, condensation and coagulation sinks, formation rate of 2 nm and 3 nm particles, and source rate of condensable vapors. We observed 59, 185 and 108 new-particle-formation events at Varrio, Hyytiala and Jarvselja, respectively. The frequency of the observed events showed an annual variation with a maximum in spring. The analysis revealed size dependence of growth rate at all locations. We found that the growth rate and source rate of a condensable vapor were the highest in Jarvselja and the lowest in Varrio. The condensation sink and particle formation rate were of a similar magnitude at Hyytiala and Jarvselja, but several times smaller at Varrio. Tracking the origin of air masses revealed that the number concentration of nucleation mode particles (3-25 nm) varied from north to south, with the highest concentrations at Jarvselja and lowest at Varrio. Trajectory analysis indicated that new-particle-formation events are large-scale phenomena that can take place concurrently at distant stations located even 1000 km apart. We found a total of 26 days with new-particle-formation events occurring simultaneously at all three stations.Peer reviewe

The legacy of Finnish-Estonian air ion and aerosol workshops

Atmospheric air ions, clusters and aerosol particles participate in a variety of atmospheric processes and considerably affect e.g. global climate and human health. When measured, air ions as well as atmospheric clusters and particles have been observed to be present practically always and everywhere. In this overview, we present a brief summary of the main achievements and legacy of the series of workshops organized mainly by the University of Helsinki and the University of Tartu. The legacy covers the development and standardization of new instruments, such as ion spectrometers, mass spectrometers and aerosol particle counters, as well as work toward theoretical understanding of new-particle formation and evolution of atmospheric clusters. One important legacy is the establishment of the SMEAR-Estonia station at Jarvselja.Peer reviewe

Atmospheric ions and nucleation: A review of observations

This review is based on ca. 250 publications, from which 92 published data on the temporal and spatial variation of the concentration of small ions (<1.6nm in diameter) in the atmosphere, chemical composition, or formation and growth rates of sub-3nm ions. The small ions exist all the time in the atmosphere, and the average concentrations of positive and negative small ions are typically 200–2500 cm−3. However, concentrations up to 5000 cm−3 have been observed. The results are in agreement with observations of ion production rates in the atmosphere. Concentrations of small ions increased in the early morning hours due to night time inversion, which leads to accumulation of radon. We also summarised observations on the conversion of small ions to intermediate ions, which can act as embryos for new atmospheric aerosol particles. Those observations include the formation rates (J2[ion]) of 2-nm intermediate ions, growth rates (GR[ion]) of sub-3nm ions, and information on the chemical composition of the ions. Unfortunately, there were only a few studies which presented J2[ion] and GR[ion]. Based on the publications, the formation rates of 2-nm ions were 0–1.1 cm−3 s−1, while the total 2-nm particle formation rates varied between 0.001 and 60 cm−3 s−1. The ionmediated processes were observed to dominate when the total particle formation rates were small, and, accordingly the importance of ion-induced mechanisms decreased with increasing total 2-nm particle formation rates. Furthermore, small ions were observed to activate for growth earlier than neutral nanometer-sized particles and at lower saturation ratio of condensing vapours.Non peer reviewe

Nanomeeter-aerosooli mõõtmistehnoloogia arendamine

Väitekirja elektrooniline versioon ei sisalda publikatsioone.Aerosooliosakeste teket nukleatsiooni teel ja nende järgnevat kasvu on jälgitud kõikjal maailmas. Tekkinud osakesed on algselt nanomeetri suurused, kuid võimelised kasvama ja seejärel osalema pilvetekkes, muutma kiirgusbilanssi ja lõpuks mõjutama Maa kliimat. Samuti võivad nano-osakesed mõjuda inimeste tervisele. Aerosooliosakeste tekke uurimise vastu on suur huvi, kuid nanomeetrisuuruste osakeste mõõtmine atmosfääris on keerukas. Osakeste tekke uurimiseks sobib hästi nanomeeter-aerosooli ja õhuioonide spektromeeter (NAIS, välja töötatud AS Airel, Eesti). Seade kasutab elektrilise aerosooli spektromeetria põhimõtet, et mõõta nii elektriliselt laetud osakeste (aero-ioonide) või ka laadimata osakeste suurusspektreid. Spektromeeter on suuteline töötama kaua hooldusvabalt väga erinevates keskkondades -- nii reostunud kesklinnast, kui ka kaugetes metsades. Seade on väljatöötatud aeroioonide spektromeetri (AIS) baasil. NAIS tööpõhimõte seisneb aersooli laadimises unipolaarses koroona ioonide väljas ja paralleelses elektrilises liikuvusanalüüsis. NAIS-il on kaks paljukanalilist elektrilist liikuvusanalüsaatorit, üks positiivsete ja teine negatiivsete laengute detekteerimiseks. Aerosool klassifitseeritakse ja mõõdetakse mõlemas analüsaatoris samaaegselt, kummaski 21 elektromeetriga. Seade mõõdab ioonide (laetud osakeste, klasterioonide) liikuvusjaotust vahemikus 3.2 – 0.0013 cm/V/s ja aerosooliosakeste suurusjaotust vahemikus 2.0 – 40 nm. Hetkel on üle maailma käigus üle kümne NAIS mõõteseadme. Väitekiri põhineb NAIS spektromeeter arendusel. Kirjeldatakse seadme matemaatilisi ja tehnilisi põhimõtteid. Tutvustatakse uut edasiarendatud NAIS mudelit – nn. “Lendav NAIS”', mis on suuteline sooritama mõõtmisi lennukilt laias kõrgustevahemikus. Uue seadme parandatud töökindlus, paindlikkus ja mõõtmiskiirus tulevad kasuks ka tavapärastel “maistel” atmosfäärimõõtmistel.Formation of aerosol by the nucleation of particles and their subsequent growth has been observed in the atmosphere almost everywhere around the world. The formed particles, initially of nanometer size, may grow further, participate in cloud formation, influence the radiation balance and ultimately climate. On local scales, these particles can affect atmospheric visibility and human health. There is a growing interest in studying new particle formation. However, it is difficult to measure aerosol particles in the size range of a few nanometers under atmospheric conditions. An instrument that is well suited for such measurements is the Nanometer aerosol and Air Ion Spectrometer (NAIS, developed by Airel Ltd., Estonia) which uses the principle of electrical aerosol spectrometry to measure the size distributions of naturally charged particles (ions) of both polarities as well as uncharged particles. The NAIS has been specifically designed for atmospheric nanometer aerosol monitoring. It can operate for long periods in a wide range of ambient conditions from polluted downtown to remote forest. It is based on the Air Ion Spectrometer (AIS). The NAIS uses unipolar corona charging and parallel electrical mobility analysis. The instrument contains two identical multichannel electrical mobility analyzer columns: one for positive, one for negative ions. The aerosol is synchronously mobility-classified in the mobility analyzers and measured with an array of 21 electrometers per column. The NAIS measures the distribution of ions (charged particles and cluster ions) in the electric mobility range from 3.2 to 0.0013 cm/V/s and the distribution of aerosol particles in the size range from 2.0 to 40 nm. There are more than ten NAIS instruments in use today around the world. The thesis focuses on the development of the NAIS. The mathematical and technical principles of the instrument are presented. An updated version of the instrument is introduced – the so called “Airborne NAIS”, which is capable of operating on board an aircraft at varying altitudes. The better reliability, adaptability and measurement speed improve regular ground based measurements as well