Evaluation of convective boundary layer height estimates using radars operating at different frequency bands

Knowledge of the atmospheric boundary layer state and evolution is important for understanding air pollution and low-level cloud development, among other things. There are a number of instruments and methods that are currently used to estimate boundary layer height (BLH). However, no single instrument is capable of providing BLH measurements in all weather conditions. We proposed a method to derive a daytime convective BLH using clear air echoes in radar observations and investigated the consistency of these retrievals between different radar frequencies. We utilized data from three vertically pointing radars that are available at the SMEAR II station in Finland, i.e. the C band (5 GHz), Ka band (35 GHz) and W band (94 GHz). The Ka- or W-band cloud radars are an integral part of cloud profiling stations of pan-European Aerosol, Clouds and Trace Gases Research Infrastructure (ACTRIS). Our method will be utilized at ACTRIS stations to serve as an additional estimate of the BLH during summer months. During this period, insects and Bragg scatter are often responsible for clear air echoes recorded by weather and cloud radars. To retrieve a BLH, we suggested a mechanism to separate passive and independently flying insects that works for all analysed frequency bands. At the lower frequency (the C band) insect scattering has been separated from Bragg scattering using a combination of the radar reflectivity factor and linear depolarization ratio. Retrieved values of the BLH from all radars are in a good agreement when compared to the BLH obtained with the co-located HALO Doppler lidar and ERA5 reanalysis data set. Our method showed some underestimation of the BLH after nighttime heavy precipitation yet demonstrated a potential to serve as a reliable method to obtain a BLH during clear-sky days. Additionally, the entrainment zone was observed by the C-band radar above the CBL in the form of a Bragg scatter layer. Aircraft observations of vertical profiles of potential temperature and water vapour concentration, collected in the vicinity of the radar, demonstrated some agreement with the Bragg scatter layer.Peer reviewe

Investigation of new particle formation mechanisms and aerosol processes at Marambio Station, Antarctic Peninsula

Understanding chemical processes leading to the formation of atmospheric aerosol particles is crucial to improve our capabilities in predicting the future climate. However, those mechanisms are still inadequately characterized, especially in polar regions. In this study, we report observations of neutral and charged aerosol precursor molecules and chemical cluster composition (qualitatively and quantitatively), as well as air ions and aerosol particle number concentrations and size distributions from the Marambio research station (64 degrees 15' S, 56 degrees 38' W), located north of the Antarctic Peninsula. We conducted measurements during the austral summer, between 15 January and 25 February 2018. The scope of this study is to characterize new particle formation (NPF) event parameters and connect our observations of gas-phase compounds with the formation of secondary aerosols to resolve the nucleation mechanisms at the molecular scale. NPF occurred on 40% of measurement days. All NPF events were observed during days with high solar radiation, mostly with above-freezing temperatures and with low relative humidity. The averaged formation rate for 3 nm particles (J(3)) was 0.686 cm(-3) s(-1), and the average particle growth rate (GR(3.8-12 nm)) was 4.2 nm h(-1). Analysis of neutral aerosol precursor molecules showed measurable concentrations of iodic acid (IA), sulfuric acid (SA), and methane sulfonic acid (MSA) throughout the entire measurement period with significant increase in MSA and SA concentrations during NPF events. We highlight SA as a key contributor to NPF processes, while IA and MSA likely only contribute to particle growth. Mechanistically, anion clusters containing ammonia and/or dimethylamine (DMA) and SA were identified, suggesting significant concentration of ammonia and DMA as well. Those species are likely contributing to NPF events since SA alone is not sufficient to explain observed nucleation rates. Here, we provide evidence of the marine origin of the measured chemical precursors and discuss their potential contribution to the aerosol phase.Peer reviewe

An evaluation of new particle formation events in Helsinki during a Baltic Sea cyanobacterial summer bloom

Several studies have investigated new particle formation (NPF) events from various sites ranging from pristine locations, including forest sites, to urban areas. However, there is still a dearth of studies investigating NPF processes and subsequent aerosol growth in coastal yet semi-urban sites, where the tropospheric layer is a concoction of biogenic and anthropogenic gases and particles. The investigation of factors leading to NPF becomes extremely complex due to the highly dynamic meteorological conditions at the coastline especially when combined with both continental and oceanic weather conditions. Herein, we engage in a comprehensive study of particle number size distributions and aerosol-forming precursor vapors at the coastal semi-urban site in Helsinki, Finland. The measurement period, 25 June-18 August 2019, was timed with the recurring cyanobacterial summer bloom in the Baltic Sea region and coastal regions of Finland. Our study recorded several regional/local NPF and aerosol burst events during this period. Although the overall anthropogenic influence on sulfuric acid (SA) concentrations was low during the measurement period, we observed that the regional or local NPF events, characterized by SA concentrations on the order of 10(7) molec. cm(-3), occurred mostly when the air mass traveled over the land areas. Interestingly, when the air mass traveled over the Baltic Sea, an area enriched with algae and cyanobacterial blooms, high iodic acid (IA) concentration coincided with an aerosol burst or a spike event at the measurement site. Further, SA-rich bursts were seen when the air mass traveled over the Gulf of Bothnia, enriched with cyanobacterial blooms. The two most important factors affecting aerosol precursor vapor concentrations, and thus the aerosol formation, were speculated to be (1) the type of phytoplankton species and intensity of bloom present in the coastal regions of Finland and the Baltic Sea and (2) the wind direction. During the events, most of the growth of sub-3 nm particles was probably due to SA, rather than IA or methane sulfonic acid (MSA); however much of the particle growth remained unexplained indicative of the strong role of organics in the growth of particles, especially in the 3-7 nm particle size range. Further studies are needed to explore the role of organics in NPF events and the potential influence of cyanobacterial blooms in coastal locations.Peer reviewe

Diurnal evolution of negative atmospheric ions above the boreal forest : from ground level to the free troposphere

At SMEAR II research station in Hyytiala, located in the Finnish boreal forest, the process of new particle formation and the role of ions has been investigated for almost 20 years near the ground and at canopy level. However, above SMEAR II, the vertical distribution and diurnal variation of these different atmospheric ions are poorly characterized. In this study, we assess the atmospheric ion composition in the stable boundary layer, residual layer, mixing layer, and free troposphere, and the evolution of these atmospheric ions due to photochemistry and turbulent mixing through the day. To measure the vertical profile of atmospheric ions, we developed a tailored set-up for online mass spectrometric measurements, capable of being deployed in a Cessna 172 with minimal modifications. Simultaneously, instruments dedicated to aerosol properties made measurements in a second Cessna. We conducted a total of 16 measurement flights in May 2017, during the spring, which is the most active new particle formation season. A flight day typically consisted of three distinct flights through the day (dawn, morning, and afternoon) to observe the diurnal variation and at different altitudes (from 100 to 3200 m above ground), to capture the boundary layer development from the stable boundary layer, residual layer to mixing layer, and the free troposphere. Our observations showed that the ion composition is distinctly different in each layer and depends on the air mass origin and time of the day. Before sunrise, the layers are separated from each other and have their own ion chemistry. We observed that the ions present within the stable layer are of the same composition as the ions measured at the canopy level. During daytime when the mixing layer evolved and the compounds are vertically mixed, we observed that highly oxidized organic molecules are distributed to the top of the boundary layer. The ion composition in the residual layer varies with each day, showing similarities with either the stable boundary layer or the free troposphere. Finally, within the free troposphere, we detected a variety of carboxylic acids and ions that are likely containing halogens, originating from the Arctic Sea.Peer reviewe

Vertical profiles of sub-3nm particles over the boreal forest

This work presents airborne observations of sub-3 nm particles in the lower troposphere and investigates new particle formation (NPF) within an evolving boundary layer (BL). We studied particle concentrations together with supporting gas and meteorological data inside the planetary BL over a boreal forest site in Hyytiala, southern Finland. The analysed data were collected during three flight measurement campaigns: May-June 2015, August 2015 and April-May 2017, including 27 morning and 26 afternoon vertical profiles. As a platform for the instrumentation, we used a Cessna 172 aircraft. The analysed flight data were collected horizontally within a 30 km distance from SMEAR II in Hyytiala and vertically from 100 m above ground level up to 2700 m. The number concentration of 1.5-3 nm particles was observed to be, on average, the highest near the forest canopy top and to decrease with increasing altitude during the mornings of NPF event days. This indicates that the precursor vapours emitted by the forest play a key role in NPF in Hyytiala. During daytime, newly formed particles were observed to grow in size and the particle population became more homogenous within the well-mixed BL in the afternoon. During undefined days with respect to NPF, we also detected an increase in concentration of 1.5-3 nm particles in the morning but not their growth in size, which indicates an interrupted NPF process during these undefined days. Vertical mixing was typically stronger during the NPF event days than during the undefined or non-event days. The results shed light on the connection between boundary layer dynamics and NPF.Peer reviewe

Low hygroscopic scattering enhancement of boreal aerosol and the implications for a columnar optical closure study

Ambient aerosol particles can take up water and thus change their optical properties depending on the hygroscopicity and the relative humidity (RH) of the surrounding air. Knowledge of the hygroscopicity effect is of crucial importance for radiative forcing calculations and is also needed for the comparison or validation of remote sensing or model results with in situ measurements. Specifically, particle light scattering depends on RH and can be described by the scattering enhancement factor f(RH), which is defined as the particle light scattering coefficient at defined RH divided by its dry value (RH <30-40 %). Here, we present results of an intensive field campaign carried out in summer 2013 at the SMEAR II station at Hyytiala, Finland. Ground-based and airborne measurements of aerosol optical, chemical and microphysical properties were conducted. The f(RH) measured at ground level by a humidified nephelometer is found to be generally lower (e.g. 1.63 +/- 0.22 at RH = 85% and lambda = 525 nm) than observed at other European sites. One reason is the high organic mass fraction of the aerosol encountered at Hyytiala to which f(RH) is clearly anti-correlated (R-2 approximate to 0.8). A simplified parametrization of f(RH) based on the measured chemical mass fraction can therefore be derived for this aerosol type. A trajectory analysis revealed that elevated values of f(RH) and the corresponding elevated inorganic mass fraction are partially caused by transported hygroscopic sea spray particles. An optical closure study shows the consistency of the ground-based in situ measurements. Our measurements allow to determine the ambient particle light extinction coefficient using the measured f(RH). By combining the ground-based measurements with intensive aircraft measurements of the particle number size distribution and ambient RH, columnar values of the particle extinction coefficient are determined and compared to columnar measurements of a co-located AERONET sun photometer. The water uptake is found to be of minor importance for the column-averaged properties due to the low particle hygroscopicity and the low RH during the daytime of the summer months. The in situ derived aerosol optical depths (AOD) clearly correlate with directly measured values of the sun photometer but are substantially lower compared to the directly measured values (factor of similar to 2-3). The comparison degrades for longer wavelengths. The disagreement between in situ derived and directly measured AOD is hypothesized to originate from losses of coarse and fine mode particles through dry deposition within the canopy and losses in the in situ sampling lines. In addition, elevated aerosol layers (above 3 km) from long-range transport were observed using an aerosol lidar at Kuopio, Finland, about 200 km east-northeast of Hyytiala. These elevated layers further explain parts of the disagreement.Peer reviewe

Refined classification and characterization of atmospheric new-particle formation events using air ions

Atmospheric new-particle formation (NPF) is a worldwide-observed phenomenon that affects the human health and the global climate. With a growing network of global atmospheric measurement stations, efforts towards investigating NPF have increased. In this study, we present an automated method to classify days into four categories including NPF events, non-events and two classes in between, which then ensures reproducibility and minimizes the hours spent on manual classification. We applied our automated method to 10 years of data collected at the SMEAR II measurement station in Hyytiälä, southern Finland using a Neutral cluster and Air Ion Spectrometer (NAIS). In contrast to the traditionally applied classification methods, which categorize days into events and non-events and ambiguous days as undefined days, our method is able to classify the undefined days as it accesses the initial steps of NPF at sub-3&thinsp;nm sizes. Our results show that, on ∼24&thinsp;% of the days in Hyytiälä, a regional NPF event occurred and was characterized by nice weather and favourable conditions such as a clear sky and low condensation sink. Another class found in Hyytiälä is the transported event class, which seems to be NPF carried horizontally or vertically to our measurement location and it occurred on 17&thinsp;% of the total studied days. Additionally, we found that an ion burst, wherein the ions apparently fail to grow to larger sizes, occurred on 18&thinsp;% of the days in Hyytiälä. The transported events and ion bursts were characterized by less favourable ambient conditions than regional NPF events and thus experienced interrupted particle formation or growth. Non-events occurred on 41&thinsp;% of the days and were characterized by complete cloud cover and high relative humidity. Moreover, for regional NPF events occurring at the measurement site, the method identifies the start time, peak time and end time, which helps us focus on variables within an exact time window to better understand NPF at a process level. Our automated method can be modified to work in other measurement locations where NPF is observed.</p

Phenomenology of ultrafine particle concentrations and size distribution across urban Europe

The 2017-2019 hourly particle number size distributions (PNSD) from 26 sites in Europe and 1 in the US were evaluated focusing on 16 urban background (UB) and 6 traffic (TR) sites in the framework of Research Infrastructures services reinforcing air quality monitoring capacities in European URBAN & industrial areaS (RI-URBANS) project. The main objective was to describe the phenomenology of urban ultrafine particles (UFP) in Europe with a significant air quality focus. The varying lower size detection limits made it difficult to compare PN concentrations (PNC), particularly PN10-25, from different cities. PNCs follow a TR > UB > Suburban (SUB) order. PNC and Black Carbon (BC) progressively increase from Northern Europe to Southern Europe and from Western to Eastern Europe. At the UB sites, typical traffic rush hour PNC peaks are evident, many also showing midday-morning PNC peaks anti-correlated with BC. These peaks result from increased PN10-25, suggesting significant PNC contributions from nucleation, fumigation and shipping. Site types to be identified by daily and seasonal PNC and BC patterns are: (i) PNC mainly driven by traffic emissions, with marked correlations with BC on different time scales; (ii) marked midday/morning PNC peaks and a seasonal anti-correlation with PNC/BC; (iii) both traffic peaks and midday peaks without marked seasonal patterns. Groups (ii) and (iii) included cities with high insolation. PNC, especially PN25-800, was positively correlated with BC, NO2, CO and PM for several sites. The variable correlation of PNSD with different urban pollutants demonstrates that these do not reflect the variability of UFP in urban environments. Specific monitoring of PNSD is needed if nanoparticles and their associated health impacts are to be assessed. Implementation of the CEN-ACTRIS recommendations for PNSD measurements would provide comparable measurements, and measurements of <10 nm PNC are needed for full evaluation of the health effects of this size fraction

Inter-annual trends of ultrafine particles in urban Europe

Ultrafine particles (UFP, those with diameters ≤ 100 nm), have been reported to potentially penetrate deeply into the respiratory system, translocate through the alveoli, and affect various organs, potentially correlating with increased mortality. The aim of this study is to assess long-term trends (5–11 years) in mostly urban UFP concentrations based on measurements of particle number size distributions (PNSD). Additionally, concentrations of other pollutants and meteorological variables were evaluated to support the interpretations. PNSD datasets from 12 urban background (UB), 5 traffic (TR), 3 suburban background (SUB) and 1 regional background (RB) sites in 15 European cities and 1 in the USA were evaluated. The non-parametric Theil-Sen's method was used to detect monotonic trends. Meta-analyses were carried out to assess the overall trends and those for different environments. The results showed significant decreases in NO, NO2, BC, CO, and particle concentrations in the Aitken (25–100 nm) and the Accumulation (100–800 nm) modes, suggesting a positive impact of the implementation of EURO 5/V and 6/VI vehicle standards on European air quality. The growing use of Diesel Particle Filters (DPFs) might also have clearly reduced exhaust emissions of BC, PM, and the Aitken and Accumulation mode particles. However, as reported by prior studies, there remains an issue of poor control of Nucleation mode particles (smaller than 25 nm), which are not fully reduced with current DPFs, without emission controls for semi-volatile organic compounds, and might have different origins than road traffic. Thus, contrasting trends for Nucleation mode particles were obtained across the cities studied. This mode also affected the UFP and total PNC trends because of the high proportion of Nucleation mode particles in both concentration ranges. It was also found that the urban temperature increasing trends might have also influenced those of PNC, Nucleation and Aitken modes.</p

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