This paper examines the representativeness of ground-based in situ measurements for the planetary boundary layer (PBL) and conducts a closure study between airborne in situ and ground-based lidar ...measurements up to an altitude of 2300 m. The related measurements were carried out in a field campaign within the framework of the High-Definition Clouds and Precipitation for Advancing Climate Prediction (HD(CP)2) Observational Prototype Experiment (HOPE) in September 2013 in a rural background area of central Europe.The helicopter-borne probe ACTOS (Airborne Cloud and Turbulence Observation System) provided measurements of the aerosol particle number size distribution (PNSD), the aerosol particle number concentration (PNC), the number concentration of cloud condensation nuclei (CCN-NC), and meteorological atmospheric parameters (e.g., temperature and relative humidity). These measurements were supported by the ground-based 3+2 wavelength polarization lidar system PollyXT, which provided profiles of the particle backscatter coefficient (σbsc) for three wavelengths (355, 532, and 1064 nm). Particle extinction coefficient (σext) profiles were obtained by using a fixed backscatter-to-extinction ratio (also lidar ratio, LR). A new approach was used to determine profiles of CCN-NC for continental aerosol. The results of this new approach were consistent with the airborne in situ measurements within the uncertainties.In terms of representativeness, the PNSD measurements on the ground showed a good agreement with the measurements provided with ACTOS for lower altitudes. The ground-based measurements of PNC and CCN-NC are representative of the PBL when the PBL is well mixed. Locally isolated new particle formation events on the ground or at the top of the PBL led to vertical variability in the cases presented here and ground-based measurements are not entirely representative of the PBL. Based on Mie theory (Mie, 1908), optical aerosol properties under ambient conditions for different altitudes were determined using the airborne in situ measurements and were compared with the lidar measurements. The investigation of the optical properties shows that on average the airborne-based particle light backscatter coefficient is 50.1 % smaller for 1064 nm, 27.4 % smaller for 532 nm, and 29.5 % smaller for 355 nm than the measurements of the lidar system. These results are quite promising, since in situ measurement-based Mie calculations of the particle light backscattering are scarce and the modeling is quite challenging. In contrast, for the particle light extinction coefficient we found a good agreement. The airborne-based particle light extinction coefficient was just 8.2 % larger for 532 nm and 3 % smaller for 355 nm, for an assumed LR of 55 sr. The particle light extinction coefficient for 1064 nm was derived with a LR of 30 sr. For this wavelength, the airborne-based particle light extinction coefficient is 5.2 % smaller than the lidar measurements. For the first time, the lidar ratio of 30 sr for 1064 nm was determined on the basis of in situ measurements and the LR of 55 sr for 355 and 532 nm wavelength was reproduced for European continental aerosol on the basis of this comparison. Lidar observations and the in situ based aerosol optical properties agree within the uncertainties. However, our observations indicate that a determination of the PNSD for a large size range is important for a reliable modeling of aerosol particle backscattering.
Abstract Novel observations of aerosol and clouds by means of ground-based remote sensing have been performed in Antarctica over the Ekström ice shelf on the coast of Dronning Maud Land at Neumayer ...Station III (70.67°S, 8.27°W) from January to December 2023. The deployment of OCEANET-Atmosphere remote-sensing observatory in the framework of the Continuous Observations of Aerosol-cLoud interAction (COALA) campaign brought ACTRIS aerosol and cloud profiling capabilities next to meteorological and air chemistry in-situ observations at the Antarctic station. We present an overview of the site, the instrumental setup and data analysis strategy and introduce 3 scientific highlights from austral fall and winter, namely: 1. Observations of a persistent mixed-phase cloud embedded in a plume of marine aerosol. Remote-sensing-based retrievals of cloud-relevant aerosol properties and cloud microphysical parameters confirm that the free-tropospheric mixed phase cloud layer formed in an aerosol-limited environment. 2. Two extraordinary warm air intrusions. One with intense snowfall produced the equivalent of 10% of the yearly snow accumulation, a second one with record-breaking maximum temperatures and heavy icing due to supercooled drizzle. 3. Omnipresent aerosol layers in the stratosphere. Our profiling capabilities could show that 50% of the 500-nm aerosol optical depth of 0.06 was caused by stratospheric aerosol, while the troposphere was usually pristine. As demonstrated by these highlights, the one-year COALA observations will serve as a reference dataset for the vertical structure of aerosol and clouds above the region, enabling future observational and modeling studies to advance understanding of atmospheric processes in Antarctica.
Environmental monitoring involves the quantification of microscopic cells and particles such as algae, plant cells, pollen, or fungal spores. Traditional methods using conventional microscopy require ...expert knowledge, are time‐intensive and not well‐suited for automated high throughput. Multispectral imaging flow cytometry (MIFC) allows measurement of up to 5000 particles per second from a fluid suspension and can simultaneously capture up to 12 images of every single particle for brightfield and different spectral ranges, with up to 60x magnification. The high throughput of MIFC has high potential for increasing the amount and accuracy of environmental monitoring, such as for plant‐pollinator interactions, fossil samples, air, water or food quality that currently rely on manual microscopic methods. Automated recognition of particles and cells is also possible, when MIFC is combined with deep‐learning computational techniques. Furthermore, various fluorescence dyes can be used to stain specific parts of the cell to highlight physiological and chemical features including: vitality of pollen or algae, allergen content of individual pollen, surface chemical composition (carbohydrate coating) of cells, DNA‐ or enzyme‐activity staining. Here, we outline the great potential for MIFC in environmental research for a variety of research fields and focal organisms. In addition, we provide best practice recommendations.
The marine aerosol arriving at Barbados (Ragged Point) was characterized during two 3-week long measurement periods in November 2010 and April 2011, in the context of the measurement campaign CARRIBA ...(Cloud, Aerosol, Radiation and tuRbulence in the trade wInd regime over BArbados). Through a comparison between ground-based and airborne measurements it was shown that the former are representative of the marine boundary layer at least up to cloud base. In general, total particle number concentrations (Ntotal) ranged from as low as 100 up to 800 cm−3, while number concentrations for cloud condensation nuclei (NCCN) at a supersaturation of 0.26 % ranged from some 10 to 600 cm−3. Ntotal and NCCN depended on the air mass origin. Three distinct types of air masses were found. One type showed elevated values for both Ntotal and NCCN and could be attributed to long-range transport from Africa, by which biomass burning particles from the Sahel region and/or mineral dust particles from the Sahara were advected. The second and third type both had values for NCCN below 200 cm−3 and a clear minimum in the particle number size distribution (NSD) around 70 to 80 nm (Hoppel minimum). While for one of these two types the accumulation mode was dominating (albeit less so than for air masses advected from Africa), the Aitken mode dominated the other and contributed more than 50 % of all particles. These Aitken mode particles likely were formed by new particle formation no more than 3 days prior to the measurements. Hygroscopicity of particles in the CCN size range was determined from CCN measurements to be κ = 0.66 on average, which suggests that these particles contain mainly sulfate and do not show a strong influence from organic material, which might generally be the case for the months during which measurements were made. The average κ could be used to derive NCCN from measured number size distributions, showing that this is a valid approach to obtain NCCN. Although the total particulate mass sampled on filters was found to be dominated by Na+ and Cl−, this was found to be contributed by a small number of large particles ( > 500 nm, mostly even in the super-micron size range). Based on a three-modal fit, a sea spray mode observed in the NSDs was found to contribute 90 % to the total particulate mass but only 4 to 10 % to Ntotal and up to 15 % to NCCN. This is in accordance with finding no correlation between Ntotal and wind speed.
We report on the Azores Stratocumulus Measurements of Radiation, Turbulence and Aerosols (ACORES) campaign, which took place around Graciosa and Pico Islands/Azores in July 2017. The main objective ...was to investigate the vertical distribution of aerosol particles, stratocumulus microphysical and radiative properties, and turbulence parameters in the eastern North Atlantic. The vertical exchange of mass, momentum, and energy between the free troposphere (FT) and the cloudy marine boundary layer (MBL) was explored over a range of scales from submeters to kilometers. To cover these spatial scales with appropriate measurements, helicopter-borne observations with unprecedented high resolution were realized using the Airborne Cloud Turbulence Observation System (ACTOS) and Spectral Modular Airborne Radiation Measurement System–Helicopter-Borne Observations (SMART-HELIOS) instrumental payloads. The helicopter-borne observations were combined with ground-based aerosol measurements collected at two continuously running field stations on Pico Mountain (2,225 m above sea level, in the FT), and at the Atmospheric Radiation Measurement (ARM) station on Graciosa (at sea level). First findings from the ACORES observations we are discussing in the paper are as follows: (i) we have observed a high variability of the turbulent cloud-top structure on horizontal scales below 100 m with local temperature gradients of up to 4 K over less than 1 m vertical distance, (ii) we have collected strictly collocated radiation measurements supporting the relevance of small-scale processes by revealing significant inhomogeneities in cloud-top brightness temperature to scales well below 100 m, and (iii) we have concluded that aerosol properties are completely different in the MBL and FT with often-complex stratification and frequently observed burst-like new particle formation.
The Southern Ocean is a critical component of Earth's climate system, but its remoteness makes it challenging to develop a holistic understanding of its processes from the small scale to the large ...scale. As a result, our knowledge of this vast region remains largely incomplete. The Antarctic Circumnavigation Expedition (ACE, austral summer 2016/2017) surveyed a large number of variables describing the state of the ocean and the atmosphere, the freshwater cycle, atmospheric chemistry, and ocean biogeochemistry and microbiology. This circumpolar cruise included visits to 12 remote islands, the marginal ice zone, and the Antarctic coast. Here, we use 111 of the observed variables to study the latitudinal gradients, seasonality, shorter-term variations, geographic setting of environmental processes, and interactions between them over the duration of 90 d. To reduce the dimensionality and complexity of the dataset and make the relations between variables interpretable we applied an unsupervised machine learning method, the sparse principal component analysis (sPCA), which describes environmental processes through 14 latent variables. To derive a robust statistical perspective on these processes and to estimate the uncertainty in the sPCA decomposition, we have developed a bootstrap approach. Our results provide a proof of concept that sPCA with uncertainty analysis is able to identify temporal patterns from diurnal to seasonal cycles, as well as geographical gradients and “hotspots” of interaction between environmental compartments. While confirming many well known processes, our analysis provides novel insights into the Southern Ocean water cycle (freshwater fluxes), trace gases (interplay between seasonality, sources, and sinks), and microbial communities (nutrient limitation and island mass effects at the largest scale ever reported). More specifically, we identify the important role of the oceanic circulations, frontal zones, and islands in shaping the nutrient availability that controls biological community composition and productivity; the fact that sea ice controls sea water salinity, dampens the wave field, and is associated with increased phytoplankton growth and net community productivity possibly due to iron fertilisation and reduced light limitation; and the clear regional patterns of aerosol characteristics that have emerged, stressing the role of the sea state, atmospheric chemical processing, and source processes near hotspots for the availability of cloud condensation nuclei and hence cloud formation. A set of key variables and their combinations, such as the difference between the air and sea surface temperature, atmospheric pressure, sea surface height, geostrophic currents, upper-ocean layer light intensity, surface wind speed and relative humidity played an important role in our analysis, highlighting the necessity for Earth system models to represent them adequately. In conclusion, our study highlights the use of sPCA to identify key ocean–atmosphere interactions across physical, chemical, and biological processes and their associated spatio-temporal scales. It thereby fills an important gap between simple correlation analyses and complex Earth system models. The sPCA processing code is available as open-access from the following link: https://renkulab.io/gitlab/ACE-ASAID/spca-decomposition (last access: 29 March 2021). As we show here, it can be used for an exploration of environmental data that is less prone to cognitive biases (and confirmation biases in particular) compared to traditional regression analysis that might be affected by the underlying research question.
Polar environments are among the fastest changing regions on the planet. It is a crucial time to make significant improvements in our understanding of how ocean and ice biogeochemical processes are ...linked with the atmosphere. This is especially true over Antarctica and the Southern Ocean where observations are severely limited and the environment is far from anthropogenic influences. In this commentary, we outline major gaps in our knowledge, emerging research priorities, and upcoming opportunities and needs. We then give an overview of the large-scale measurement campaigns planned across Antarctica and the Southern Ocean in the next 5 years that will address the key issues. Until we do this, climate models will likely continue to exhibit biases in the simulated energy balance over this delicate region. Addressing these issues will require an international and interdisciplinary approach which we hope to foster and facilitate with ongoing community activities and collaborations.
Hygroscopic properties of secondary organic aerosol (SOA) formed by photooxidation of different concentrations (10-27 or 220-270 ppb) of alpha-pinene precursor were investigated at different relative ...humidities (RH) using a hygroscopicity tandem differential mobility analyzer (HTDMA, RH=95-97%) and using the mobile version of the Leipzig Aerosol Cloud Interaction Simulator (LACIS-mobile, RH=98-99.3%). In addition, the cloud condensation nuclei (CCN) activity was measured applying two CCN counters (CCNC). An apparent single-hygroscopicity parameter, kappa, of approximately 0.09, approximately 0.07-0.13, and approximately 0.02-0.04 was derived from CCNC, HTDMA and LACIS data, respectively, assuming the surface tension of pure water. Closure between HTDMA and CCNC data was achieved within experimental uncertainty, whereas closure between LACIS and CCNC was only achieved by assuming a concentration-dependent surface tension reduction, consequently resulting in lower CCNC-derived kappa values. Comparing different experimental techniques at varying precursor concentrations in more detail reveals further open questions. Varying precursor concentration influences hygroscopic growth factors at subsaturated RH, while it has no effect on the CCN activation. This difference in behaviour might be caused by precursor concentration-dependent surface tension depression or changing droplet solution concentration dependence of the water activity coefficient with varying SOA composition. Furthermore, evidence was found that the SOA might need several seconds to reach the equilibrium growth factor at high RH.
The Arctic is sensitive to cloud radiative forcing. Due to the limited number of aerosols present throughout much of the year, cloud formation is susceptible to the presence of cloud condensation ...nuclei and ice nucleating particles (INPs). Primary biological aerosol particles (PBAP) contribute to INPs and can impact cloud phase, lifetime, and radiative properties. We present yearlong observations of hyperfluorescent aerosols (HFA), tracers for PBAP, conducted with a Wideband Integrated Bioaerosol Sensor, New Electronics Option during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition (October 2019–September 2020) in the central Arctic. We investigate the influence of potential anthropogenic and natural sources on the characteristics of the HFA and relate our measurements to INP observations during MOSAiC. Anthropogenic sources influenced HFA during the Arctic haze period. But surprisingly, we also found sporadic “bursts” of HFA with the characteristics of PBAP during this time, albeit with unclear origin. The characteristics of HFA between May and August 2020 and in October 2019 indicate a strong contribution of PBAP to HFA. Notably from May to August, PBAP coincided with the presence of INPs nucleating at elevated temperatures, that is, >−9°C, suggesting that HFA contributed to the “warm INP” concentration. The air mass residence time and area between May and August and in October were dominated by the open ocean and sea ice, pointing toward PBAP sources from within the Arctic Ocean. As the central Arctic changes drastically due to climate warming with expected implications on aerosol–cloud interactions, we recommend targeted observations of PBAP that reveal their nature (e.g., bacteria, diatoms, fungal spores) in the atmosphere and in relevant surface sources, such as the sea ice, snow on sea ice, melt ponds, leads, and open water, to gain further insights into the relevant source processes and how they might change in the future.
Cloud condensation nuclei (CCN) number concentrations alongside with submicrometer particle number size distributions and particle chemical composition have been measured at atmospheric observatories ...of the Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS) as well as other international sites over multiple years. Here, harmonized data records from 11 observatories are summarized, spanning 98,677 instrument hours for CCN data, 157,880 for particle number size distributions, and 70,817 for chemical composition data. The observatories represent nine different environments, e.g., Arctic, Atlantic, Pacific and Mediterranean maritime, boreal forest, or high alpine atmospheric conditions. This is a unique collection of aerosol particle properties most relevant for studying aerosol-cloud interactions which constitute the largest uncertainty in anthropogenic radiative forcing of the climate. The dataset is appropriate for comprehensive aerosol characterization (e.g., closure studies of CCN), model-measurement intercomparison and satellite retrieval method evaluation, among others. Data have been acquired and processed following international recommendations for quality assurance and have undergone multiple stages of quality assessment.
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