Small-scale mixing processes enhancing troposphere-to-stratosphere transport by pyro-cumulonimbus storms

Abstract. Deep convection induced by large forest fires is an efficient mechanism for transport of aerosol particles and trace gases into the upper troposphere and lower stratosphere (UT/LS). For many pyro-cumulonimbus clouds (pyroCbs) as well as other cases of severe convection without fire forcing, radiometric observations of cloud tops in the thermal infrared (IR) reveal characteristic structures, featuring a region of relatively high brightness temperatures (warm center) surrounded by a U-shaped region of low brightness temperatures. We performed a numerical simulation of a specific case study of pyroCb using a non-hydrostatic cloud resolving model with a two-moment cloud microphysics p…

Comparing airborne and satellite retrievals of cloud optical thickness and particle effective radius using a spectral radiance ratio technique: two case studies for cirrus and deep convective clouds

Solar radiation reflected by cirrus and deep convective clouds (DCCs) was measured by the Spectral Modular Airborne Radiation Measurement System (SMART) installed on the German High Altitude and Long Range Research Aircraft (HALO) during the Mid-Latitude Cirrus (ML-CIRRUS) and the Aerosol, Cloud, Precipitation, and Radiation Interaction and Dynamic of Convective Clouds System – Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modelling and to the Global Precipitation Measurement (ACRIDICON-CHUVA) campaigns. On particular flights, HALO performed measurements closely collocated with overpasses of the Moderate Resolution Imaging Spectroradiometer (…

230Th/U dating of Last Interglacial brain corals from Bonaire (southern Caribbean) using bulk and theca wall material

Abstract We compared the suitability of two skeletal materials of the Atlantic brain coral Diploria strigosa for 230Th/U-dating: the commonly used bulk material comprising all skeletal elements and the denser theca wall material. Eight fossil corals of presumably Last Interglacial age from Bonaire, southern Caribbean Sea, were investigated, and several sub-samples were dated from each coral. For four corals, both the ages and the activity ratios of the bulk material and theca wall agree within uncertainty. Three corals show significantly older ages for their bulk material than for their theca wall material as well as substantially elevated 232Th content and (230Th/238U) ratios. The bulk mat…

HONO Emissions from Soil Bacteria as a Major Source of Atmospheric Reactive Nitrogen

From Soil to Sky Trace gases emitted either through the activity of microbial communities or from abiotic reactions in the soil influence atmospheric chemistry. In laboratory column experiments using several soil types, Oswald et al. (p. 1233 ) showed that soils from arid regions and farmlands can produce substantial quantities of nitric oxide (NO) and nitrous acid (HONO). Ammonia-oxidizing bacteria are the primary source of HONO at comparable levels to NO, thus serving as an important source of reactive nitrogen to the atmosphere.

In-situ high spatial resolution LA-MC-ICPMS 230Th/U dating enables detection of small-scale age inversions in speleothems

Abstract We present an in-situ method for Th and U isotope measurements by laser ablation multi-collector inductively coupled plasma mass spectrometry (LA-MC-ICPMS) to determine possible age inversions of stalagmites, using a 213 nm Nd:YAG laser connected to an MC-ICPMS. Due to the low ion beam intensity of 230 Th (20–120 counts per second, cps), we carefully optimized the operating parameters to get highest possible ion beam intensities, i.e., laser fluence (25 J cm −2 ), spot size (110 μm), pulse repetition rate (20 Hz), scan speed (4 μm s −1 ), integration time (1000 s), and He and Ar gas flow (∼0.9 L min −1 and ∼0.6 L min −1 respectively). A precision (2 relative standard error, 2RSE) o…

Primary biological aerosol particles in the atmosphere: a review

Atmospheric aerosol particles of biological origin are a very diverse group of biological materials and structures, including microorganisms, dispersal units, fragments and excretions of biological organisms. In recent years, the impact of biological aerosol particles on atmospheric processes has been studied with increasing intensity, and a wealth of new information and insights has been gained. This review outlines the current knowledge on major categories of primary biological aerosol particles (PBAP): bacteria and archaea, fungal spores and fragments, pollen, viruses, algae and cyanobacteria, biological crusts and lichens and others like plant or animal fragments and detritus. We give a…

Modelling the optical properties of fresh biomass burning aerosol produced in a smoke chamber: results from the EFEU campaign

A better characterisation of the optical properties of biomass burning aerosol as a function of the burning conditions is required in order to quantify their effects on climate and atmospheric chemistry. Controlled laboratory combustion experiments with different fuel types were carried out at the combustion facility of the Max Planck Institute for Chemistry (Mainz, Germany) as part of the "Impact of Vegetation Fires on the Composition and Circulation of the Atmosphere" (EFEU) project. The combustion conditions were monitored with concomitant CO<sub>2</sub> and CO measurements. The mass scattering efficiencies of 8.9±0.2 m<sup>2</sup> g<sup&gt…

Simulation of a biomass-burning plume: Comparison of model results with observations

[1] We have simulated the dynamical evolution of the plume from a prescribed biomass fire, using the active tracer high- resolution atmospheric model (ATHAM). Initialization parameters were set to reflect the conditions during the fire. The model results are compared with airborne remote-sensing and in situ measurements of the plume. ATHAM reproduces the injection height (250-600 m) and the horizontal extent of the plume (similar to4 km) with good accuracy. The aerosol mass concentrations are underestimated but still in the range of the observations. Remaining differences between the model results and the measurements are attributed to limited meteorological and fire emission information. A…

Comparing Airborne and Satellite Retrievals of Optical and Microphysical Properties of Cirrus and Deep Convective Clouds using a Radiance Ratio Technique

Abstract. Solar radiation reflected by cirrus and deep convective clouds (DCCs) was measured by the Spectral Modular Airborne Radiation Measurement System (SMART) installed on the German HALO (High Altitude and Long Range Research Aircraft) during the ML-CIRRUS and the ACRIDICON-CHUVA campaigns. In particular flights, HALO performed closely collocated measurements with overpasses of the Moderate Resolution Imaging Spectroradiometer (MODIS) on board of Aqua satellite. Based on the nadir upward radiance, the optical thickness τ and bulk particle effective radius reff of cirrus and DCC are retrieved using a radiance ratio algorithm which considers the cloud thermodynamic phase, the cloud verti…

The Palaeoanthropocene – The beginnings of anthropogenic environmental change

Abstract As efforts to recognize the Anthropocene as a new epoch of geological time are mounting, the controversial debate about the time of its beginning continues. Here, we suggest the term Palaeoanthropocene for the period between the first, barely recognizable, anthropogenic environmental changes and the industrial revolution when anthropogenically induced changes of climate, land use and biodiversity began to increase very rapidly. The concept of the Palaeoanthropocene recognizes that humans are an integral part of the Earth system rather than merely an external forcing factor. The delineation of the beginning of the Palaeoanthropocene will require an increase in the understanding and …

High efficacy of face masks explained by characteristic regimes of airborne SARS-CoV-2 virus abundance

Abstract Airborne transmission is an important transmission pathway for viruses, including SARS-CoV-2. Regions with a higher proportion of people wearing masks show better control of COVID-19, but the effectiveness of masks is still under debate due to their limited and variable efficiencies in removing respiratory particles. Here, we analyze experimental data and perform model calculations to show that this contrast can be explained by the different regimes of abundance of particles and viruses. Because of the large number of particles exhaled during human respiration and vocalization, indoor environments are usually in a particle-rich regime which means that masks cannot prevent the inhal…

Control of solute concentrations in cloud and fog water by liquid water content

We measured the concentrations of Cl^−, NO_3^−, and SO_4^(2−) in atmospheric cloudwater collected with a passive collector from a remote marine site and the concentrations of Cl^−, NO_3^−, SO_4^(2−), Na^+ and NH_4^+ in cloudwater from a continental site. At the continental site, an active rotating arm collector was employed for cloudwater collection. At both locations, we observed an inverse relationship between the measured ion concentrations and the liquid water content of the clouds. The product of the observed concentrations and the liquid water content, the cloudwater loading, was found to be nearly constant. A study of published cloudwater data showed that at the majority of the exami…

The ACRIDICON-CHUVA campaign: Studying tropical deep convective clouds and precipitation over Amazonia using the new German research aircraft HALO

Abstract Between 1 September and 4 October 2014, a combined airborne and ground-based measurement campaign was conducted to study tropical deep convective clouds over the Brazilian Amazon rain forest. The new German research aircraft, High Altitude and Long Range Research Aircraft (HALO), a modified Gulfstream G550, and extensive ground-based instrumentation were deployed in and near Manaus (State of Amazonas). The campaign was part of the German–Brazilian Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems–Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (Global Precipitatio…

Measurement of sulfur isotope ratios in micrometer-sized samples by NanoSIMS

Abstract Sulfur isotope ratios of atmospheric aerosol particles can provide detailed information with regard to the origin and the transport of sulfur in the environment. The new Cameca NanoSIMS 50 ion microprobe technique permits analysis of individual aerosol particles with volumes down to 0.5 μm 3 and a precision for δ 34 S of 3–10‰ (2 σ ). This technique will set new standards in the analysis of isotope ratios in atmospheric aerosol. For the first time it is possible to directly compare chemical and isotopic composition of individual aerosol particles, identify internal and external mixtures and investigate reactions of anthropogenic gases with natural aerosol such as sea salt and miner…

Non-Matrix-Matched Calibration for the Multi-Element Analysis of Geological and Environmental Samples Using 200 nm Femtosecond LA-ICP-MS: A Comparison with Nanosecond Lasers

LA-ICP-MS is one of the most promising techniques for in situ analysis of geological and environmental samples. However, there are some limitations with respect to measurement accuracy, in particular for volatile and siderophile/chalcophile elements, when using non-matrix-matched calibration. We therefore investigated matrix-related effects with a new 200 nm femtosecond (fs) laser ablation system (NWRFemto200) using reference materials with different matrices and spot sizes from 10 to 55 μm. We also performed similar experiments with two nanosecond (ns) lasers, a 193 nm excimer (ESI NWR 193) and a 213 nm Nd:YAG (NWR UP-213) laser. The ion intensity of the 200 nm fs laser ablation was much l…

230Th/U-dating of carbonate deposits from ancient aqueducts

Abstract Carbonate deposits in aqueducts, known as calcareous sinter, can reach a considerable thickness and are commonly annually laminated. Environmental and palaeoclimate proxies measured in calcareous sinter samples, such as stable oxygen and carbon isotopes and trace elements, can provide important high-resolution information on hydrological conditions, temperature, and local precipitation in the catchment area of an aqueduct. In order to utilize the proxy data for palaeoclimate reconstruction, the sinter deposits must be dated by annual laminae counting and more precisely by 230 Th/U-dating. The major problem of 230 Th/U-dating of calcareous sinter in aqueducts is the relatively large…

Whole-Ocean Changes in Silica and Ge/Si Ratios During the Last Deglacial Deduced From Long-Lived Giant Glass Sponges

Size Matters More Than Chemistry for Cloud-Nucleating Ability of Aerosol Particles

Size-resolved cloud condensation nuclei (CCN) spectra measured for various aerosol types at a non-urban site in Germany showed that CCN concentrations are mainly determined by the aerosol number size distribution. Distinct variations of CCN activation with particle chemical composition were observed but played a secondary role. When the temporal variation of chemical effects on CCN activation is neglected, variation in the size distribution alone explains 84 to 96% of the variation in CCN concentrations. Understanding that particles' ability to act as CCN is largely controlled by aerosol size rather than composition greatly facilitates the treatment of aerosol effects on cloud physics in re…

Microanalytical methods for in-situ high-resolution analysis of rock varnish at the micrometer to nanometer scale

Abstract A wide range of analytical techniques were used to investigate rock varnish from different locations (Negev, Israel; Knersvlakte, South Africa; Death Valley and Mojave Desert, California): a 200 nm-femtosecond laser ablation-inductively coupled plasma-mass spectrometer (LA-ICP-MS), an electron probe microanalyzer (EPMA), focused ion beam (FIB) slicing, and scanning transmission X-ray microscopy–near edge X-ray absorption fine structure spectroscopy (STXM–NEXAFS). This combination enables comprehensive high-spatial-resolution analysis of rock varnish. Femtosecond LA-ICP-MS and EPMA were used for quantitative determination of element concentrations. In-situ measurements were conducte…

Radical Formation by Fine Particulate Matter Associated with Highly Oxygenated Molecules

Highly oxygenated molecules (HOMs) play an important role in the formation and evolution of secondary organic aerosols (SOA). However, the abundance of HOMs in different environments and their relation to the oxidative potential of fine particulate matter (PM) are largely unknown. Here, we investigated the relative HOM abundance and radical yield of laboratory-generated SOA and fine PM in ambient air ranging from remote forest areas to highly polluted megacities. By electron paramagnetic resonance and mass spectrometric investigations, we found that the relative abundance of HOMs, especially the dimeric and low-volatility types, in ambient fine PM was positively correlated with the formatio…

Improved constraints on open-system processes in fossil reef corals by combined Th/U, Pa/U and Ra/Th dating: A case study from Aqaba, Jordan

Abstract Here we present 230Th/U, 231Pa/U as well as 226Ra/230Th isotope ratios from five fossil reef corals of Last Interglacial origin from the Gulf of Aqaba, Northern Red Sea. The results show clear evidence for open-system behaviour with strongly elevated δ234U values and U concentrations indicating post-depositional U addition. The combined application of all isotope systems enables us to better constrain the nature and timing of the open-system processes than only based on the 230Th/U data. Quantitative modelling of the diagenetic processes allowed us to reproduce the trends in the isotope ratios. Two of the five corals were probably affected by two separate phases of U addition with …

Face masks effectively limit the probability of SARS-CoV-2 transmission.

Masking out air sharing The effectiveness of masks in preventing the transmission of severe acute respiratory syndrome coronavirus 2 has been debated since the beginning of the COVID-19 pandemic. One important question is whether masks are effective despite the forceful expulsion of respiratory matter during coughing and sneezing. Cheng et al. convincingly show that most people live in conditions in which the airborne virus load is low. The probability of infection changes nonlinearly with the amount of respiratory matter to which a person is exposed. If most people in the wider community wear even simple surgical masks, then the probability of an encounter with a virus particle is even fur…

Do organics contribute to small particle formation in the Amazonian upper troposphere?

3-D cloud-resolving model simulations including explicit aerosol physics and chemistry are compared with observations of upper tropospheric (12 km) aerosol size distributions over the Amazon Basin. ...

Aerosol concentrations determine the height of warm rain and ice initiation in convective clouds over the Amazon basin

Abstract. We have investigated how pollution aerosols affect the height above cloud base of rain and ice hydrometeor initiation and the subsequent vertical evolution of cloud droplet size and number concentrations in growing convective cumulus. For this purpose we used in-situ data of hydrometeor size distributions measured with instruments mounted on HALO (High Altitude and Long Range Research Aircraft) during the ACRIDICON-CHUVA campaign over the Amazon during September 2014. The results show that the height of rain initiation by collision and coalescence processes (Dr, in units of meters above cloud base) is linearly correlated with the number concentration of droplets (Nd in cm−3) nucle…

Aerosol Chemistry Resolved by Mass Spectrometry: Linking Field Measurements of Cloud Condensation Nuclei Activity to Organic Aerosol Composition.

Aerosol hygroscopic properties were linked to its chemical composition by using complementary online mass spectrometric techniques in a comprehensive chemical characterization study at a rural mountaintop station in central Germany in August 2012. In particular, atmospheric pressure chemical ionization mass spectrometry ((-)APCI-MS) provided measurements of organic acids, organosulfates, and nitrooxy-organosulfates in the particle phase at 1 min time resolution. Offline analysis of filter samples enabled us to determine the molecular composition of signals appearing in the online (-)APCI-MS spectra. Aerosol mass spectrometry (AMS) provided quantitative measurements of total submicrometer or…

Investigation of matrix effects in 193nm laser ablation-inductively coupled plasma-mass spectrometry analysis using reference glasses of different transparencies

Abstract The degree of transparency of glasses, which depends on the Fe content, may influence the ablation behavior during laser ablation-inductively coupled plasma-mass spectrometry (LA-ICP-MS) analysis. To test possible matrix effects when using a 193 nm Nd:YAG laser, we have analyzed transparent and opaque NIST, BAM and USGS reference glasses. These reference materials are ideal for such investigations, because they are well characterized, most elements are homogeneously distributed at the micrometer scale, and their Fe content varies over a very large range, from 16 to 130,000 μg g− 1. Our measurements show that the fractionation factors of refractory and volatile lithophile elements, …

Speleothem δ13C record suggests enhanced spring/summer drought in south-eastern Spain between 9.7 and 7.8 ka – A circum-Western Mediterranean anomaly?

South-eastern Spain is one of the driest regions in Europe and thus, prone to drought. Terrestrial climate records covering the late Glacial and Holocene from this area are sparse. Here, we present a flowstone record from Cueva Victoria, south-eastern Spain, which covers the late Glacial (15 ka) to the mid-Holocene (7 ka) including the Younger Dryas (YD). Between the onset of the Bølling/Allerød (B/A) and the early Holocene, flowstone δ18O values progressively decrease in accordance with sea-surface temperatures in the Alboran Sea, indicating an increase in precipitation in south-eastern Spain and a supra-regional signal of North Atlantic temperature change. At the same time, decreasing δ13…

Hydroxylamine released by nitrifying microorganisms is a precursor for HONO emission from drying soils

AbstractNitrous acid (HONO) is an important precursor of the hydroxyl radical (OH), the atmosphere´s primary oxidant. An unknown strong daytime source of HONO is required to explain measurements in ambient air. Emissions from soils are one of the potential sources. Ammonia-oxidizing bacteria (AOB) have been identified as possible producers of these HONO soil emissions. However, the mechanisms for production and release of HONO in soils are not fully understood. In this study, we used a dynamic soil-chamber system to provide direct evidence that gaseous emissions from nitrifying pure cultures contain hydroxylamine (NH2OH), which is subsequently converted to HONO in a heterogeneous reaction w…

Observed and Simulated Variability of Droplet Spectral Dispersion in Convective Clouds Over the Amazon

In this study, the variability of the spectral dispersion of droplet size distributions (DSDs) in convective clouds is investigated. Analyses are based on aircraft measurements of growing cumuli near the Amazon basin, and on numerical simulations of an idealized ice‐free cumulus. In cleaner clouds, the relative dispersion ϵ, defined as the ratio of the standard deviation to the mean value of the droplet diameter, is negatively correlated with the ratio of the cloud water content (qc) to the adiabatic liquid water content (qa), while no strong correlation between ϵ and qc/qa is seen in polluted clouds. Bin microphysics numerical simulations suggest that these contrasting behaviors are associ…

Comparing calculated microphysical properties of tropical convective clouds at cloud base with measurements during the ACRIDICON-CHUVA campaign

Abstract. Reliable aircraft measurements of cloud microphysical properties are essential for understanding liquid convective cloud formation. In September 2014, the properties of convective clouds were measured with a Cloud Combination Probe (CCP), a Cloud and Aerosol Spectrometer (CAS-DPOL), and a cloud condensation nuclei (CCN) counter on board the HALO (High Altitude and Long Range Research Aircraft) aircraft during the ACRIDICON-CHUVA campaign over the Amazon region. An intercomparison of the cloud drop size distributions (DSDs) and the cloud water content derived from the different instruments generally shows good agreement within the instrumental uncertainties. The objective of this s…

Sensitivities of Amazonian clouds to aerosols and updraft speed

Abstract. The effects of aerosol particles and updraft speed on warm-phase cloud microphysical properties are studied in the Amazon region as part of the ACRIDICON-CHUVA experiment. Here we expand the sensitivity analysis usually found in the literature by concomitantly considering cloud evolution, putting the sensitivity quantifications into perspective in relation to in-cloud processing, and by considering the effects on droplet size distribution (DSD) shape. Our in situ aircraft measurements over the Amazon Basin cover a wide range of particle concentration and thermodynamic conditions, from the pristine regions over coastal and forested areas to the southern Amazon, which is highly poll…

Sulfur isotope ratio measurements of individual sulfate particles by NanoSIMS

Abstract The sulfur isotopic compositions of barite (BaSO4), anhydrite (CaSO4), gypsum (CaSO4·2H2O), mascagnite ((NH4)2SO4), thenardite (Na2SO4), boetite (K2SO4), epsomite (MgSO4·7H2O), magnesium sulfate (MgSO4·xH2O) and cysteine (an amino acid) were determined with a Cameca NanoSIMS 50 ion microprobe employing a Cs+ primary ion beam and measuring negative secondary ions. This ion microprobe permits the analysis of sulfur isotope ratios in sulfates on 0.001–0.5 ng of sample material, enabling the analysis of individual S-bearing particles with diameters as small as 500 nm. The grain-to-grain reproducibility of measurements is typically 5‰ (1σ) for micron-sized grains,

Geochemical insights into the relationship of rock varnish and adjacent mineral dust fractions

Abstract Rock varnishes are μm-thin, dark, manganese(Mn)-rich crusts that accrete in the order of few μm/ka on weathering-resistant lithologies. Although these crusts can form in all climates, they are best known in arid to semi-arid settings. Aeolian dust is understood as a major contributor to the distinct trace metal and REE enrichments in rock varnish. However, the exact proportions of abiotic and biotic formation mechanisms that may explain the oxidation-reactions of Mn2+ to Mn4+, present as Mn oxyhydroxides in the varnish, are still a matter of ongoing debate. We present here the first systematic study of trace element enrichment processes between the uppermost layer of the varnish se…

Comparing parameterized versus measured microphysical properties of tropical convective cloud bases during the ACRIDICON–CHUVA campaign

The objective of this study is to validate parameterizations that were recently developed for satellite retrievals of cloud condensation nuclei supersaturation spectra, NCCN(S), at cloud base alongside more traditional parameterizations connecting NCCN(S) with cloud base updrafts and drop concentrations. This was based on the HALO aircraft measurements during the ACRIDICON–CHUVA campaign over the Amazon region, which took place in September 2014. The properties of convective clouds were measured with a cloud combination probe (CCP), a cloud and aerosol spectrometer (CAS-DPOL), and a CCN counter onboard the HALO aircraft. An intercomparison of the cloud drop size distributions (DSDs) and the…

Cloud droplet number closure for tropical convective clouds during the ACRIDICON–CHUVA campaign

The main objective of the ACRIDICON-CHUVA (Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems–Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the Global Precipitation measurements) campaign in September 2014 was the investigation of aerosol-cloud-interactions in the Amazon Basin. Cloud properties near cloud base of growing convective cumuli were characterized by cloud droplet size distribution measurements using a cloud combination probe (CCP) and a cloud and aerosol spectrometer (CAS-DPOL). In the current study, an adiabatic parcel model was used to perform cloud droplet number (N…

Accurate trace element analysis of speleothems and biogenic calcium carbonates by LA-ICP-MS

The high spatial resolution of laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) microanalysis of speleothems and biogenic calcium carbonates makes it possible to improve our understanding of past climatic conditions. However, there are analytical problems associated with this method, such as molecular interferences, elemental fractionation, and mass-load-dependent matrix effects, when using NIST silicate reference glasses for calibration. Our study with a sector-field ICP-MS shows that many masses are affected by interferences, such as 24Mg+ by 48Ca++ or 31P+ by 15N16O+. Elemental fractionation and mass-load-dependent matrix effects have been detected for both 213 and…

Linear relationship between effective radius and precipitation water content near the top of convective clouds

Quantifying the precipitation within clouds is a crucial challenge to improve our current understanding of the Earth’s hydrological cycle. We have investigated the relationship between the effective radius of droplets and ice particles (re) and precipitation water content (PWC) measured by cloud probes near the top of growing convective cumuli. The data for this study were collected by aircraft measurements in clean and polluted conditions over the Amazon Basin and over the western tropical Atlantic in September 2014. Our results indicate a threshold of re ∼ 13 μm for warm rain initiation in convective clouds, which is in agreement with previous studies. In…

Reorganization of the North Atlantic Oscillation during early Holocene deglaciation

Laurentide ice-sheet retreat continued into the mid-Holocene. Speleothem-based precipitation records suggest the cessation of melt led to the establishment of the present precipitation patterns associated with the North Atlantic Oscillation. The North Atlantic Oscillation is the dominant atmospheric pressure mode in the North Atlantic region and affects winter temperature and precipitation in the Mediterranean, northwest Europe, Greenland, and Asia1. The index1 that describes the sea-level pressure difference between Iceland and the Azores is correlated with a dipole precipitation pattern over northwest Europe and northwest Africa. How the North Atlantic Oscillation will develop as the Gree…

Enhanced organic mass fraction and decreased hygroscopicity of cloud condensation nuclei (CCN) during new particle formation events

In a forested near-urban location in central Germany, the CCN efficiency of particles smaller than 100 nm decreases significantly during periods of new particle formation. This results in an increase of average activation diameters, ranging from 5 to 8% at supersaturations of 0.33% and 0.74%, respectively. At the same time, the organic mass fraction in the sub-100-nm size range increases from approximately 2/3 to 3/4. This provides evidence that secondary organic aerosol (SOA) components are involved in the growth of new particles to larger sizes, and that the reduced CCN efficiency of small particles is caused by the low hygroscopicity of the condensing material. The observed dependence of…

The challenge of simulating the sensitivity of the Amazonian clouds microstructure to cloud condensation nuclei number concentrations

The realistic representation of cloud-aerosol interactions is of primary importance for accurate climate model projections. The investigation of these interactions in strongly contrasting clean and polluted atmospheric conditions in the Amazon area has been one of the motivations for several field observations, including the airborne Aerosol, Cloud, Precipitation, and Radiation Interactions and DynamIcs of CONvective cloud systems – Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (Global Precipitation Measurement) (ACRIDICON-CHUVA) campaign based in Manaus, Brazil in September 2014. In this work we combine in situ …

Bioaerosols in the Earth system: Climate, health, and ecosystem interactions

Abstract Aerosols of biological origin play a vital role in the Earth system, particularly in the interactions between atmosphere, biosphere, climate, and public health. Airborne bacteria, fungal spores, pollen, and other bioparticles are essential for the reproduction and spread of organisms across various ecosystems, and they can cause or enhance human, animal, and plant diseases. Moreover, they can serve as nuclei for cloud droplets, ice crystals, and precipitation, thus influencing the hydrological cycle and climate. The sources, abundance, composition, and effects of biological aerosols and the atmospheric microbiome are, however, not yet well characterized and constitute a large gap i…

Linear relationship between effective radius and precipitation water content near the top of convective clouds: measurement results from ACRIDICON–CHUVA campaign

Quantifying the precipitation within clouds is a crucial challenge to improve our current understanding of the Earth's hydrological cycle. We have investigated the relationship between the effective radius of droplets and ice particles (re) and precipitation water content (PWC) measured by cloud probes near the top of growing convective cumuli. The data for this study were collected during the ACRIDICON–CHUVA campaign on the HALO research aircraft in clean and polluted conditions over the Amazon Basin and over the western tropical Atlantic in September 2014. Our results indicate a threshold of re∼13 µm for warm rain initiation in convective clouds, which is in agreement with previous studie…

Cloud droplet formation at the base of tropical convective clouds: closure between modeling and measurement results of ACRIDICON–CHUVA

Aerosol–cloud interactions contribute to the large uncertainties in current estimates of climate forcing. We investigated the effect of aerosol particles on cloud droplet formation by model calculations and aircraft measurements over the Amazon and over the western tropical Atlantic during the ACRIDICON–CHUVA campaign in September 2014. On the HALO (High Altitude Long Range Research) research aircraft, cloud droplet number concentrations (Nd) were measured near the base of clean and polluted growing convective cumuli using a cloud combination probe (CCP) and a cloud and aerosol spectrometer (CAS-DPOL). An adiabatic parcel model was used to perform cloud droplet number closure studies for fl…

Three-dimensional solar radiation effects on the actinic flux field in a biomass-burning plume

[1] Three-dimensional (3-D) solar radiative transfer models describe radiative transfer under inhomogeneous atmospheric conditions more accurately than the commonly used one-dimensional (1-D) radiative transfer models that assume horizontal homogeneity of the atmosphere. Here results of 3-D radiative transfer simulations for a biomass-burning plume are presented and compared with local one-dimensional (l-1-D) simulations, i.e., 1-D simulations in every column of the model domain. The spatial distribution of the aerosol particles was derived from a 3-D atmospheric transport simulation. We studied the impact of 3-D radiative effects on the actinic flux within the plume center. The differences…

FeMnOx-1: A new microanalytical reference material for the investigation of Mn–Fe rich geological samples

Suitable Mn-Fe rich microanalytical reference materials (MRMs) as calibration material for laser ablation-inductively coupled plasma mass spectrometry (LA-ICPMS) have not been available. The United States Geological Survey (USGS) in collaboration with the Max Planck Institute for Chemistry has prepared a synthetic MRM, FeMnOx-1, with elevated mass fractions of MnO (25 g/100 g), Fe2O3 (8.5 g/100 g) and high mass fractions of 25 trace elements varying between 200 and 5000 mg/kg. This new MRM has been designed as calibration material for a wide range of different Mn-Fe deposits, such as desert/rock varnish, ocean crusts and nodules as well as Mn accumulations in soils and lakes. Small-scale an…

Trace element variability in single ostracod valves as a proxy for hydrochemical change in Nam Co, central Tibet, during the Holocene

Ostracod shells, belonging to three taxa (Leucocytherella sinensis Huang, 1982, ?Leucocythere dorsotuberosa Huang, 1982 and ?L. dorsotuberosa f. postilirata sensu Pang, 1985), were collected from two sediment cores from Lake Nam Co, on the central Tibetan Plateau. Two variants of LA–ICP–MS (laser ablation–inductively coupled plasma–mass spectrometry), spot and line-scan analyses, were used to investigate trace element concentrations (Mg, Sr, Ba, U and rare earth elements [REEs]) in single ostracod shells. The results suggest that the line-scan method can provide better precision than the spot analysis and is therefore preferred. No significant difference in trace element composition between…

Characterization and differentiation of rock varnish types from different environments by microanalytical techniques

© 2017 Elsevier B.V. We investigated rock varnishes collected from several locations and environments worldwide by a broad range of microanalytical techniques. These techniques were selected to address the challenges posed by the chemical and structural complexity within the micrometer- to nanometer-sized structures in these geological materials. Femtosecond laser ablation-inductively coupled plasma-mass spectrometry (fs LA-ICP-MS), scanning transmission X-ray microscopy-near edge X-ray adsorption fine structure spectroscopy (STXM-NEXAFS) in combination with scanning electron microscopy (SEM) of focused ion beam (FIB) ultra-thin (100–200 nm) sections, conventional and polarization microscop…

Composition and diurnal variability of the natural Amazonian aerosol

As part of the Large-Scale Biosphere-Atmosphere Experiment in Amazonia (LBA)-Cooperative LBA Airborne Regional Experiment (CLAIRE) 2001 campaign, separate day and nighttime aerosol samples were collected in July 2001 at a ground-based site in Amazonia, Brazil, in order to examine the composition and temporal variability of the natural “background” aerosol. A combination of analytical techniques was used to characterize the elemental and ionic composition of the aerosol. Major particle types larger than ∼0.5 μm were identified by electron and light microscopy. Both the coarse and fine aerosol were found to consist primarily of organic matter (∼70 and 80% by mass, respectively), with the coar…

Further evidence for CCN aerosol concentrations determining the height of warm rain and ice initiation in convective clouds over the Amazon basin

We have investigated how aerosols affect the height above cloud base of rain and ice hydrometeor initiation and the subsequent vertical evolution of cloud droplet size and number concentrations in growing convective cumulus. For this purpose we used in situ data of hydrometeor size distributions measured with instruments mounted on HALO aircraft during the ACRIDICON–CHUVA campaign over the Amazon during September 2014. The results show that the height of rain initiation by collision and coalescence processes (Dr, in units of meters above cloud base) is linearly correlated with the number concentration of droplets (Nd in cm−3) nucleated at cloud base (Dr ≈ 5 ⋅ Nd). Additional cloud processes…

Chemical separation and MC-ICPMS analysis of U, Th, Pa and Ra isotope ratios of carbonates

Diagenetic alteration of fossil reef corals may have severe effects on the reliability of 230Th/U-ages. The widely applied criteria introduced to test for the reliability of coral 230Th/U-ages are often not sufficient to identify all altered ages. The combination of 230Th/U- with 231Pa/U-dating has been suggested as a promising method to identify altered ages. Furthermore, 226Ra/230Th ratios can provide information about the diagenetic history during the last 10 000 years. Here we present a method to chemically separate U, Th, Pa and Ra from the same aliquot of a carbonate sample. The isotope ratios of our mixed U–Th–Pa–Ra spike are calibrated using a secular equilibrium material treated in…

Modeling of biomass smoke injection into the lower stratosphere by a large forest fire (Part I): reference simulation

Abstract. Wildland fires in boreal regions have the potential to initiate deep convection, so-called pyro-convection, due to their release of sensible heat. Under favorable atmospheric conditions, large fires can result in pyro-convection that transports the emissions into the upper troposphere and the lower stratosphere. Here, we present three-dimensional model simulations of the injection of fire emissions into the lower stratosphere by pyro-convection. These model simulations are constrained and evaluated with observations obtained from the Chisholm fire in Alberta, Canada, in 2001. The active tracer high resolution atmospheric model (ATHAM) is initialized with observations obtained by r…

Modeling of biomass smoke injection into the lower stratosphere by a large forest fire (Part II): Sensitivity studies

Abstract. The Chisholm forest fire that burned in Alberta, Canada, in May 2001 resulted in injection of substantial amounts of smoke into the lower stratosphere. We used the cloud-resolving plume model ATHAM (Active Tracer High resolution Atmospheric Model) to investigate the importance of different contributing factors to the severe intensification of the convection induced by the Chisholm fire and the subsequent injection of biomass smoke into the lower stratosphere. The simulations show strong sensitivity of the pyro-convection to background meteorology. This explains the observed coincidence of the convective blow-up of the fire plume and the passage of a synoptic cold front. Furthermor…

Environmentally relevant precursors of carbonyl sulfide in aquatic systems

Seawater solutions of environmentally relevant organosulfur compounds, commercial humic acid (HA), and natural dissolved organic matter (DOM) were incubated with and without UV light in order to determine the carbonyl sulfide (COS) producing capabilities of these compounds. COS dark- and photo-production rate constants were determined for dilute solutions of the organosulfur compounds (μmol l−1) and HA/DOM (mg l−1). Dissolved COS was determined using a purge and cryogenic trap method followed by GC/FPD detection. COS was produced in considerable amounts both non-photochemically and photochemically from the reduced form of free acid of glutathione (GSH) and photochemically from cysteine (CYS…