A simple model for the time evolution of the condensation sink in the atmosphere for intermediate Knudsen numbers

Transformation of the mass flux towards the particle from the kinetic regime to the continuum regime is often described by the Fuchs-Sutugin coefficient. Kinetic regime can be obtained as a limiting case when only one term of the expansion of the Fuchs-Sutugin coefficient at small 1/Kn is considered. Here we take the two first terms into account, and get a mass flux which agrees well with the full mass flux down to Kn similar to 0.5. This procedure allows an analytical solution of the condensation equation valid for the range of intermediate Knudsen numbers to be obtained. The expansion is further applied to analytically calculate the condensation sink. The formula for the condensation sink is tested against field observations. The relative contribution of different aerosol modes to the condensation sink is discussed. Furthermore, we present a simple model describing the coupled dynamics of the condensing vapour and the condensation sink. The model gives reasonable predictions of condensation sink dynamics during the periods of the aerosol modes' growth by condensation in the atmosphere.Peer reviewe

Estimation of sulfuric acid concentration using ambient ion composition and concentration data obtained with atmospheric pressure interface time-of-flight ion mass spectrometer

Sulfuric acid (H2SO4, SA) is the key compound in atmospheric new particle formation. Therefore, it is crucial to observe its concentration with sensitive instrumentation, such as chemical ionisation (CI) inlets coupled to atmospheric pressure interface time-of-flight (APi-TOF) mass spectrometers. However, there are environmental conditions for which and physical reasons why chemical ionisation cannot be used, for example in certain remote places or during flight measurements with limitations regarding chemicals. Here, we propose a theoretical method to estimate the SA concentration based on ambient ion composition and concentration measurements that are achieved by APi-TOF alone. We derive a theoretical expression to estimate the SA concentration and validate it with accurate CI-APi-TOF observations. Our validation shows that the developed estimate works well during daytime in a boreal forest (R-2 = 0.85); however, it underestimates the SA concentration in, e.g. the Antarctic atmosphere during new particle formation events where the dominating pathway for nucleation involves sulfuric acid and a base (R-2 = 0.48).Peer reviewe

Atmospheric new particle formation and growth : review of field observations

This review focuses on the observed characteristics of atmospheric new particle formation (NPF) in different environments of the global troposphere. After a short introduction, we will present a theoretical background that discusses the methods used to analyze measurement data on atmospheric NPF and the associated terminology. We will update on our current understanding of regional NPF, i.e. NPF taking simultaneously place over large spatial scales, and complement that with a full review on reported NPF and growth rates during regional NPF events. We will shortly review atmospheric NPF taking place at sub-regional scales. Since the growth of newly-formed particles into larger sizes is of great current interest, we will briefly discuss our observation-based understanding on which gaseous compounds contribute to the growth of newly-formed particles, and what implications this will have on atmospheric cloud condensation nuclei formation. We will finish the review with a summary of our main findings and future outlook that outlines the remaining research questions and needs for additional measurements.Peer reviewe

Comprehensive analysis of particle growth rates from nucleation mode to cloud condensation nuclei in boreal forest

Growth of aerosol particles to sizes at which they can act as cloud condensation nuclei (CCN) is a crucial factor in estimating the current and future impacts of aerosol-cloud-climate interactions. Growth rates (GRs) are typically determined for particles with diameters (d(P)) smaller than 40 nm immediately after a regional new particle formation (NPF) event. These growth rates are often taken as representatives for the particle growth to CCN sizes (d(P) > 50-100 nm). In modelling frameworks, the concentration of the condensable vapours causing the growth is typically calculated with steady state assumptions, where the condensation sink (CS) is the only loss term for the vapours. Additionally, the growth to CCN sizes is represented with the condensation of extremely low-volatility vapours and gas-particle partitioning of semi-volatile vapours. Here, we use a novel automatic method to determine growth rates from below 10 nm to hundreds of nanometres from a 20-year-long particle size distribution (PSD) data set in boreal forest. With this method, we are able to detect growth rates also at times other than immediately after a NPF event. We show that the GR increases with an increasing oxidation rate of monoterpenes, which is closely coupled with the ambient temperature. Based on our analysis, the oxidation reactions of monoterpenes with ozone, hydroxyl radical and nitrate radical all are capable of producing vapours that contribute to the particle growth in the studied size ranges. We find that GR increases with particle diameter, resulting in up to 3-fold increases in GRs for particles with d(P) similar to 100 nm in comparison to those with d(P) similar to 10 nm. We use a single particle model to show that this increase in GR can be explained with aerosol-phase reactions, in which semi-volatile vapours form non-volatile dimers. Finally, our analysis reveals that the GR of particles with d(P) <100 nm is not limited by the condensation sink, even though the GR of larger particles is. Our findings suggest that in the boreal continental environment, the formation of CCN from NPF or sub-100 nm emissions is more effective than previously thought and that the formation of CCN is not as strongly self-limiting a process as the previous estimates have suggested.Peer reviewe

An extensive data set for in situ microphysical characterization of low-level clouds in a Finnish sub-Arctic site

Continuous, semi-long-term, ground-based in situ cloud measurements were conducted during eight Pallas Cloud Experiments (PaCEs) held in autumn between 2004 and 2019. Those campaigns were carried out in the Finnish sub-Arctic region at the Sammaltunturi station (67 degrees 58'24"N, 24 degrees 06'58"E; 560ma.m.s.l.), the part of the Pallas Atmosphere-Ecosystem Supersite and Global Atmosphere Watch (GAW) program. Two cloud spectrometer ground setups and a weather station were installed on the roof of the station to measure in situ cloud properties and several meteorological variables. Thus, the obtained data sets include the size distribution of cloud droplets as a measured cloud parameter along with the air temperature, dew point temperature, humidity, pressure, horizontal wind speed and direction, (global solar) sun radiation, and visibility at the station. Additionally, the number concentration, effective diameter, median volume diameter, and liquid water content from each instrument were derived. The presented data sets provide a insight into microphysics of low-level clouds in subArctic conditions over a wide range of temperatures (-25.8 to 8.8 degrees C). The data are available in the Finnish Meteorological Institute (FMI) open data repository for each campaign and each cloud spectrometer ground setup individually: https://doi.org/10.23728/FMI-B2SHARE.988739D21B824C709084E88ED6C6D54B (Doulgeris et al., 2021).Peer reviewe

A Finnish Meteorological Institute-Aerosol Cloud Interaction Tube (FMI-ACIT) : Experimental setup and tests of proper operation

The Finnish Meteorological Institute-Aerosol Cloud Interaction Tube (FMI-ACIT) is a multi-purpose instrument for investigating atmospherically relevant interactions between aerosol particles and water vapor under defined laboratory conditions. This work introduces an experimental setup of FMI-ACIT for investigation of the aerosol activation and the droplet growth under supersaturated conditions. Several simulations and experimental tests were conducted to find out what the proper operational parameters are. To verify the ability of FMI-ACIT to perform as a cloud condensation nuclei (CCN) counter, activation experiments were executed using size selected ammonium sulfate [(NH4)(2)SO4] particles in the size range of 10-300 nm. Supersaturations from 0.18% to 1.25% were tested by experiments with different temperature gradients. Those showed that FMI-ACIT can effectively measure CCN in this range. Measured droplet size distributions at supersaturations 0.18% and 1.25% are in good agreement with those determined by a droplet growth model. Published by AIP Publishing.Peer reviewe

Intermediate ions as a strong indicator of new particle formation bursts in a boreal forest

Secondary aerosol formation from gas-phase precursors is a frequent phenomenon occurring in a boreal environment. Traditionally, this process is identified visually from observational data on total and ion number size distributions. Here, we introduce a new, objective classification method for the new particle formation events based on measured intermediate-ion concentrations. The intermediate-ion concentration is a suitable indicator of new particle formation, because it is linked to the atmospheric new particle formation. The concentration of intermediate ions is typically very low (below 5 cm(-3)) when there is no new particle formation or precipitation events occurring. In this study, we analysed concentrations of negative intermediate ions at the Station for Measuring Ecosystem Atmosphere Relations (SMEAR II) in Hyytiala, Finland, during the years 2003-2013. We found that the half-hour median concentration of negative intermediate ions in sizes 2-4 nm was > 20 cm(-3) during 77.5% of event days classified by traditional method. The corresponding value was 92.3% in the case of 2-7 nm negative ions. In addition, the intermediate-ion concentration varied seasonally in a similar manner as the number of event days, peaking in the spring. A typical diurnal variation of the intermediate-ion concentration resembled that of the particle concentration during the event days. We developed here a new method for classifying new particle formation events based on intermediate-ion concentrations. The new method is complementary to the traditional event analysis and it can also be used as an automatic way of determining new particle formation events from large data sets.Peer reviewe