Life cycle of a cloud condensation nucleus, CCN

The research conducted and presented herein concentrates primarily on the life cycle of a cloud condensation nucleus CCN. The primary motivation of the work is the importance of CCN in the global aerosol-cloud-climate system, and focus is placed on the production of CCN, their behaviour in the atmosphere and their properties with respect to CCN activation, as well as the removal pathways. The work presented in this thesis covers measurements performed at 16 locations around the world. The results further corroborated the notion that atmospheric new particle formation NPF is an important and widespread source of CCN in the atmosphere. The number of newly formed CCN from NPF depends on many factors, including, but not limited to, biogenic and anthropogenic emissions, frequency of NPF events, nucleation and growth rates and pre-existing CCN concentrations; method of calculation also affects the estimate of NPF contribution to CCN budgets. Highest relative increase in CCN as a result of NPF was observed at a clean remote location in Northern Finland, where in the summer the number concentration of particles above 50 nm in diameter N50 can increase by as much as 800%. Highest absolute increases in NCCN as a result of NPF (up to 3500 particles cm 3 for N50) were found at a dry savannah location of Botsalano in South Africa. In Hyytiälä Type I nucleation events were found to always, at the very least, double NCCN concentrations. It was found that in many environments around the world a rather similar fraction of aerosols activated into cloud droplets at any given level of supersaturation S, and a simple linear parameterisation is provided for an easy calculation of annual mean CCN concentration NCCN based only on total number concentration NCN and the desired S. At the majority of studied locations hygroscopicity was found to increase with size, with accumulation mode hygroscopicity parameter κ values being significantly larger than Aitken mode κ at some locations. Depending on the focus and desired accuracy, the use of κ values as a function of particle dry size rather than the assumption of a size-independent κ should preferably be considered. The photochemistry, aging processes, atmospheric NPF and other atmospheric processes occurring on a diurnal scale were found to affect the CCN activation and hygroscopic properties of Aitken mode aerosol only. The hygroscopicity of the accumulation mode aerosol is more affected by processes occurring on a time scale of a few days to months, e.g. long range transport and seasonal variation in vegetation activity. Below-cloud scavenging by snow was found to be an inefficient mechanism of CCN removal from the atmosphere compared to, e.g., in-cloud scavenging. Additionally, nucleation and Aitken mode particles are scavenged by snow more efficiently that CCN-sized aerosol. No apparent difference in the scavenging efficiency of snow was observed between a rural and an urban site in Southern Finland. Ambient relative humidity was found to correlate positively with the scavenging efficiency of snow, and a new parameterisation for calculating snow scavenging coefficients based on both particle dry size and relative humidity is presented. A reconsideration of the purpose, the focus and the motivation for the cloud condensation nuclei counter CCNC measurements at the SMEAR II is needed if they are to be continued with reasonable, interesting and exciting output

Condensation/immersion mode ice-nucleating particles in a boreal environment

Ice-nucleating particle (INP) measurements were performed in the boreal environment of southern Finland at the Station for Measuring Ecosystem-Atmosphere Relations (SMEAR II) in the winter-spring of 2018. Measurements with the Portable Ice Nucleation Chamber (PINC) were conducted at 242 K and 105 % relative humidity with respect to water. The median INP number concentration [INP] during a 6-week measurement period was 13 L-1. The [INP] spanned 3 orders of magnitude and showed a general increase from mid-February until early April. No single dominant local or regional sources of INPs in the boreal environment of southern Finland could be identified. Rather, it is hypothesised that the INPs detected at SMEAR II are a result of long-range transport and dilution of INPs sourced far from the measurement site. Despite high variability, the measured [INP] values fall within the range expected for the [INP] measured elsewhere under similar thermodynamic conditions. The [INP] did not correlate with any of the examined parameters during the entire field campaign, indicating that no one single parameter can be used to predict the [INP] at the measurement location during the examined time period. The absence of a correlation across the entire field campaign also suggests that a variety of particles act as INPs at different times, although it was indirectly determined that ambient INPs are most likely within the size range of 0.1-0.5 mu m in diameter on average. On shorter timescales, several particle species correlated well with the [INP]. Depending on the meteorological conditions, black carbon (BC), supermicron biological particles and sub-0.1 mu m particles, most likely nanoscale biological fragments such as ice-nucleating macromolecules (INMs), correlated with the INP signal. However, an increase in the concentration of any of these particle species may not necessarily lead to the increase in the [INP]; the reasons for this remain unknown. Limitations of the instrumental set-up and the necessity for future field INP studies are addressed.Peer reviewe

On measurements of aerosol particles and greenhouse gases in Siberia and future research needs

The role of the world's boreal forest for our understanding of the climate system is indisputable. Due to the large area covered, the forest's biophysical (e.g. surface energy balance, albedo) and biogeochemical (e.g. bidirectional exchange of greenhouse gases or aerosol precursors) processes are known to affect today's climate, and will need to be accounted for in studies of climate feedbacks in response to anthropogenic warming. However, observations that are needed to develop and evaluate terrestrial and climate models are still relatively scarce, especially for the Siberian part of the boreal forest. Here, we present a short overview of aerosol and greenhouse gas measurements over Siberia, aiming to also survey a large fraction of the existing literature in Russian. We aim to highlight areas of least data coverage and argue that, due to the importance of Siberia in the global climate system, a coordinated research program is needed to address some of the open research questions: The Pan Siberian Experiment

Airborne measurements over the boreal forest of southern Finland during new particle formation events in 2009 and 2010

Peer reviewe

Cloud condensation nuclei production associated with atmospheric nucleation : a synthesis based on existing literature and new results

This paper synthesizes the available scientific information connecting atmospheric nucleation with subsequent cloud condensation nuclei (CCN) formation. We review both observations and model studies related to this topic, and discuss the potential climatic implications. We conclude that CCN production associated with atmospheric nucleation is both frequent and widespread phenomenon in many types of continental boundary layers, and probably also over a large fraction of the free troposphere. The contribution of nucleation to the global CCN budget spans a relatively large uncertainty range, which, together with our poor understanding of aerosol-cloud interactions, results in major uncertainties in the radiative forcing by atmospheric aerosols. In order to better quantify the role of atmospheric nucleation in CCN formation and Earth System behavior, more information is needed on (i) the factors controlling atmospheric CCN production and (ii) the properties of both primary and secondary CCN and their interconnections. In future investigations, more emphasis should be put on combining field measurements with regional and large-scale model studies.Peer reviewe

Heavy alcohol drinking and subclinical echocardiographic abnormalities of structure and function.

OBJECTIVE: The aim of the study is to assess changes in heart structure and function associated with heavy alcohol use by comparing echocardiographic indices in a population-based sample to those in patients admitted to an inpatient facility with severe alcohol problems. METHODS AND RESULTS: We used data from the Know Your Heart study (2015-2017) which is a cross-sectional study that recruited 2479 participants aged 35-69 years from the general population of the city of Arkhangelsk in Northwest Russia and 278 patients from the Arkhangelsk Regional Psychiatric Hospital with a primary diagnosis related to chronic alcohol use (narcology clinic subsample). The drinking patterns of the population-based sample were characterised in detail. We used regression models controlling for age, sex, smoking, education and waist to hip ratio to evaluate the differences in echocardiographic indices in participants with different drinking patterns. The means of left ventricular end-diastolic diameter and indexed left atrial systolic diameter were increased among heavy drinkers (narcology clinic subsample), while mean left ventricular ejection fraction was decreased in this group compared with the population-based sample. In contrast, the harmful and hazardous drinkers in the population-based sample did not differ from non-problem drinkers with respect to echocardiographic indices of systolic and diastolic function. CONCLUSIONS: Extremely heavy drinking is associated with a specific set of structural and functional abnormalities of the heart that may be regarded as precursors of alcohol-related dilated cardiomyopathy

Influence of biogenic emissions from boreal forests on aerosol-cloud interactions

Boreal forest acts as a carbon sink and contributes to the formation of secondary organic aerosols via emission of aerosol precursor compounds. However, these influences on the climate system are poorly quantified. Here we show direct observational evidence that aerosol emissions from the boreal forest biosphere influence warm cloud microphysics and cloud-aerosol interactions in a scale-dependent and highly dynamic manner. Analyses of in situ and ground-based remote-sensing observations from the SMEAR II station in Finland, conducted over eight months in 2014, reveal substantial increases in aerosol load over the forest one to three days after aerosol-poor marine air enters the forest environment. We find that these changes are consistent with secondary organic aerosol formation and, together with water-vapour emissions from evapotranspiration, are associated with changes in the radiative properties of warm, low-level clouds. The feedbacks between boreal forest emissions and aerosol-cloud interactions and the highly dynamic nature of these interactions in air transported over the forest over timescales of several days suggest boreal forests have the potential to mitigate climate change on a continental scale. Our findings suggest that even small changes in aerosol precursor emissions, whether due to changing climatic or anthropogenic factors, may substantially modify the radiative properties of clouds in moderately polluted environments. Emissions from the boreal forest biosphere can substantially increase aerosol load above the forest and influence the radiative properties of clouds, according to analysis of observations from a monitoring station in Finland.Peer reviewe

Adsorptive uptake of water by semisolid secondary organic aerosols

Aerosol climate effects are intimately tied to interactions with water. Here we combine hygroscopicity measurements with direct observations about the phase of secondary organic aerosol (SOA) particles to show that water uptake by slightly oxygenated SOA is an adsorption-dominated process under subsaturated conditions, where low solubility inhibits water uptake until the humidity is high enough for dissolution to occur. This reconciles reported discrepancies in previous hygroscopicity closure studies. We demonstrate that the difference in SOA hygroscopic behavior in subsaturated and supersaturated conditions can lead to an effect up to about 30% in the direct aerosol forcinghighlighting the need to implement correct descriptions of these processes in atmospheric models. Obtaining closure across the water saturation point is therefore a critical issue for accurate climate modeling.Peer reviewe

Measurement report : Introduction to the HyICE-2018 campaign for measurements of ice-nucleating particles and instrument inter-comparison in the Hyytiala boreal forest

The formation of ice particles in Earth's atmosphere strongly influences the dynamics and optical properties of clouds and their impacts on the climate system. Ice formation in clouds is often triggered heterogeneously by ice-nucleating particles (INPs) that represent a very low number of particles in the atmosphere. To date, many sources of INPs, such as mineral and soil dust, have been investigated and identified in the low and mid latitudes. Although less is known about the sources of ice nucleation at high latitudes, efforts have been made to identify the sources of INPs in the Arctic and boreal environments. In this study, we investigate the INP emission potential from high-latitude boreal forests in the mixed-phase cloud regime. We introduce the HyICE-2018 measurement campaign conducted in the boreal forest of Hyytiala, Finland, between February and June 2018. The campaign utilized the infrastructure of the Station for Measuring Ecosystem-Atmosphere Relations (SMEAR) II, with additional INP instruments, including the Portable Ice Nucleation Chamber I and II (PINC and PINCii), the SPectrometer for Ice Nuclei (SPIN), the Portable Ice Nucleation Experiment (PINE), the Ice Nucleation SpEctrometer of the Karlsruhe Institute of Technology (INSEKT) and the Microlitre Nucleation by Immersed Particle Instrument (mu L-NIPI), used to quantify the INP concentrations and sources in the boreal environment. In this contribution, we describe the measurement infrastructure and operating procedures during HyICE-2018, and we report results from specific time periods where INP instruments were run in parallel for inter-comparison purposes. Our results show that the suite of instruments deployed during HyICE-2018 reports consistent results and therefore lays the foundation for forthcoming results to be considered holistically. In addition, we compare measured INP concentrations to INP parameterizations, and we observe good agreement with the Tobo et al. (2013) parameterization developed from measurements conducted in a ponderosa pine forest ecosystem in Colorado, USA.Peer reviewe