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The absorption Ångström exponent (AAE) is an important aerosol optical parameter used for aerosol characterization and apportionment studies. The AAE of black carbon (BC) particles is widely accepted to be 1.0, although observational estimates give quite a wide range of 0.6–1.3. With considerable uncertainties related to observations, a numerical study is a powerful method, if not the only one, to provide a better and more accurate understanding on BC AAE. This study calculates BC AAE using realistic particle geometries based on fractal aggregate and an accurate numerical optical model (namely the multiple-sphere T-matrix method), and considers bulk properties of an ensemble of BC particles following lognormal size distributions. At odds with the expectations, BC AAE is not 1.0, even when BC is assumed to have small sizes and a wavelength-independent refractive index. With a wavelength-independent refractive index, the AAE of fresh BC is approximately 1.05 and relatively insensitive to particle size. For BC with geometric mean diameters larger than 0.12 µm, BC AAE becomes smaller when BC particles are aged (compact structures or coated by other non-absorptive materials). For coated BC, we prescribe the coating fraction variation based on a laboratory study, where smaller BC cores are shown to develop larger coating fractions than those of bigger BC cores. For both compact and coated BC, the AAE is highly sensitive to particle size distribution, ranging from approximately 0.8 to even over 1.4 with wavelength-independent refractive index. When the refractive index is allowed to vary with wavelength, a feature with observational backing, the BC AAE may show an even wider range. For different BC morphologies, we derive simple empirical equations on BC AAE based on our numerical results, which can serve as a guide for the response of BC AAE to BC size and refractive index. Due to its complex influences, the effects of BC geometry is better to be discussed at certain BC properties, i.e., known size and refractive index.

This study aims at quantifying the ice nucleation properties of desert dust in the Saharan Air Layer (SAL), the warm, dry and dust-laden layer that expands from North Africa to the Americas. By measuring close to the dust's emission source, before aging processes during the transatlantic advection potentially modify the dust properties, the study fills a gap between in situ measurements of dust ice nucleating particles (INPs) far away from the Sahara and laboratory studies of ground-collected soil. Two months of online INP concentration measurements are presented, which were part of the two CALIMA campaigns at the Izaña observatory in Tenerife, Spain (2373 m a.s.l.), in the summers of 2013 and 2014. INP concentrations were measured in the deposition and condensation mode at temperatures between 233 and 253 K with the Portable Ice Nucleation Chamber (PINC). Additional aerosol information such as bulk chemical composition, concentration of fluorescent biological particles as well as the particle size distribution was used to investigate observed variations in the INP concentration. The concentration of INPs was found to range between 0.2 std L−1 in the deposition mode and up to 2500 std L−1 in the condensation mode at 240 K. It correlates well with the abundance of aluminum, iron, magnesium and manganese (R: 0.43–0.67) and less with that of calcium, sodium or carbonate. These observations are consistent with earlier results from laboratory studies which showed a higher ice nucleation efficiency of certain feldspar and clay minerals compared to other types of mineral dust. We find that an increase of ammonium sulfate, linked to anthropogenic emissions in upwind distant anthropogenic sources, mixed with the desert dust has a small positive effect on the condensation mode INP per dust mass ratio but no effect on the deposition mode INP. Furthermore, the relative abundance of biological particles was found to be significantly higher in INPs compared to the ambient aerosol. Overall, this suggests that atmospheric aging processes in the SAL can lead to an increase in ice nucleation ability of mineral dust from the Sahara. INP concentrations predicted with two common parameterization schemes, which were derived mostly from atmospheric measurements far away from the Sahara but influenced by Asian and Saharan dust, were found to be higher based on the aerosol load than we observed in the SAL, further suggesting aging effects of INPs in the SAL.

Atmospheric aerosol particles like mineral dust, volcanic ash and combustion particles can reduce Earth's snow and ice albedo considerably even by very small amounts of deposited particle mass. In this study, a new laboratory method is applied to measure the spectral light absorption coefficient of airborne particles that are released from fresh snow samples by an efficient nebulizing system. Three-wavelength photoacoustic absorption spectroscopy is combined with refractory black carbon (BC) mass analysis to determine the snow mass-specific and BC mass-specific absorption cross sections. Fullerene soot in water suspensions are used for the characterization of the method and for the determination of the mass-specific absorption cross section of this BC reference material. The analysis of 31 snow samples collected after fresh snowfall events at a high-altitude Alpine research station reveals a significant discrepancy between the measured snow mass-specific absorption cross section and the cross section that is expected from the BC mass data, indicating that non-BC light-absorbing particles are present in the snow. Mineral dust and brown carbon (BrC) are identified as possible candidates for the non-BC particle mass based on the wavelength dependence of the measured absorption. For one sample this result is confirmed by environmental scanning electron microscopy and by single-particle fluorescence measurements, which both indicate a high fraction of biogenic and organic particle mass in the sample.

Ice crystal chain aggregates—linear structures of conjoined monomer crystals—have previously been observed in strongly electrified deep convection, likely forming via electric‐field‐enhanced aggregation. The NASA Investigation of Microphysics and Precipitation for Atlantic Coast‐Threatening Snowstorms field campaign conducted aircraft‐based sampling of cold‐season storms using cloud probes. These measurements reveal chain aggregates in weakly electrified winter storms. Chain aggregates were identified in 28 of 34 research flights from 2020 to 2023 (∼10% of total P‐3 flight time), spanning −38°C to +2.5°C and 1.5–9.7 km. High‐resolution Cloud Particle Imager and Particle Habit Imaging and Polar Scattering imagery revealed sublimation signatures on chain aggregates, consistent across instruments. The widespread occurrence of chain aggregates in weakly electrified clouds suggests alternative formation pathways than electric‐field‐enhanced aggregation.

Ice clouds in the tropical tropopause layer have a key role in dehydrating air that is entering the stratosphere. Cloud-chamber measurements suggest that their high humidity can be explained if heterogeneous ice nucleation on glassy aerosols is a significant nucleation mechanism in this region. Ice clouds in the tropical tropopause layer play a key role in dehydrating air as it enters the stratosphere 1 , 2 . However, in situ measurements show that water vapour within these clouds is unexpectedly supersaturated 3 , 4 , 5 ; normally the growth of ice crystals rapidly quenches supersaturation 3 . The high in-cloud humidity may be related to the low number of ice crystals found in these clouds 4 , 6 , but low ice number densities are inconsistent with standard models of cirrus cloud formation involving homogeneous freezing of liquid aerosols 7 . Aqueous aerosols rich in organic matter are ubiquitous in the atmosphere 8 , 9 , and under cirrus conditions they are known to become glassy 10 , 11 , that is, amorphous, non-crystalline solids. Here we report experiments in a cloud simulation chamber that demonstrate heterogeneous nucleation of ice on glassy solution droplets. Cirrus residues measured in situ showed ice nuclei rich in oxidized organic matter 12 , consistent with heterogeneous nucleation on glassy aerosols. In addition, using a one-dimensional cirrus model, we show that nucleation on glassy aerosols may explain low ice crystal numbers and high in-cloud humidity in the tropical tropopause layer. We propose that heterogeneous nucleation on glassy aerosols is an important mechanism for ice nucleation in the tropical tropopause layer.

The Arctic CLoud Observations Using airborne measurements during polar Day (ACLOUD) campaign was carried out north-west of Svalbard (Norway) between 23 May and 6 June 2017. The objective of ACLOUD was to study Arctic boundary layer and mid-level clouds and their role in Arctic amplification. Two research aircraft (Polar 5 and 6) jointly performed 22 research flights over the transition zone between open ocean and closed sea ice. Both aircraft were equipped with identical instrumentation for measurements of basic meteorological parameters, as well as for turbulent and radiative energy fluxes. In addition, on Polar 5 active and passive remote sensing instruments were installed, while Polar 6 operated in situ instruments to characterize cloud and aerosol particles as well as trace gases. A detailed overview of the specifications, data processing, and data quality is provided here. It is shown that the scientific analysis of the ACLOUD data benefits from the coordinated operation of both aircraft. By combining the cloud remote sensing techniques operated on Polar 5, the synergy of multi-instrument cloud retrieval is illustrated. The remote sensing methods were validated using truly collocated in situ and remote sensing observations. The data of identical instruments operated on both aircraft were merged to extend the spatial coverage of mean atmospheric quantities and turbulent and radiative flux measurement. Therefore, the data set of the ACLOUD campaign provides comprehensive in situ and remote sensing observations characterizing the cloudy Arctic atmosphere. All processed, calibrated, and validated data are published in the World Data Center PANGAEA as instrument-separated data subsets (Ehrlich et al., 2019b, https://doi.org/10.1594/PANGAEA.902603).

In this paper, the Photoacoustic Aerosol Absorption Spectrometer (PAAS-4λ) is introduced. PAAS-4λ was specifically developed for long-term monitoring tasks in (unattended) air quality stations. It uses four wavelengths coupled to a single acoustic resonator in a compact and robust set-up. The instrument has been thoroughly characterized and carefully calibrated in the laboratory using NO2/air mixtures and Nigrosin aerosol. It has an ultimate 1σ detection limit below 0.1 Mm−1, at a measurement precision and accuracy of 3 % and 10 %, respectively. In order to demonstrate the PAAS-4λ suitability for long-term monitoring tasks, the instrument is currently validated at the air quality monitoring station Pallas in Finland, about 140 km north of the Arctic circle. A total of 11 months of PAAS-4λ data from this deployment are presented and discussed in terms of instrument performance. Intercomparisons with the filter-based photometers of a continuous soot monitoring system (COSMOS), the Multi-Angle Absorption Photometer (MAAP), and Aethalometer (AE33) demonstrate the capabilities and value of PAAS-4λ, as well as for the validation of the widely used filter-based instruments.

The spectral light-absorbing behavior of carbonaceous aerosols varies depending on the chemical composition and structure of the particles. A new single-cavity three-wavelength photoacoustic spectrometer was developed and characterized for measuring absorption coefficients at three wavelengths across the visible spectral range. In laboratory studies, several types of soot with different organic content were generated by a diffusion flame burner and were investigated for changes in mass-specific absorption cross section (MAC) values, absorption and scattering Ångström exponents (αabs and αsca), and single scattering albedo (ω). By increasing the organic carbonaceous (OC) content of the aerosol from 50 to 90 % of the total carbonaceous mass, for 660 nm nearly no change of MAC was found with increasing OC content. In contrast, for 532 nm a significant increase, and for 445 nm a strong increase of MAC was found with increasing OC content of the aerosol. Depending on the OC content, the Ångström exponents of absorption and scattering as well as the single scattering albedo increased. These laboratory results were compared to a field study at a traffic-dominated urban site, which was also influenced by residential wood combustion. For this site a daily average value of αabs(445–660) of 1.9 was found.

A new instrument for the quantification of light absorption by particles collected on filters has been developed to address long standing environmental questions about light-absorbing particles in air, water, and on snow and ice. The Light Absorption Heating Method (LAHM) uses temperature changes when filters are exposed to light to quantify absorption. Through the use of calibration standards, the observed temperature response of unknown materials can be related to the absorption cross section of the substance collected on the filter. Here, we present a detailed description of the instrument and calibration. The results of the calibration tests using a common surrogate for black carbon, Fullerene soot, show that the instrument provides stable results even when exposed to adverse laboratory conditions, and that there is little drift in the instrument over longer periods of time. Calibration studies using Fullerene soot suspended in water, airborne propane soot, as well as atmospheric particulates show consistent results for absorption cross section when using accepted values for the mass absorption cross section of the soot and when compared to results from a 3-wavelength photoacoustic instrument. While filter sampling cannot provide the time resolution of other instrumentation, the LAHM instrument fills a niche where time averaging is reasonable and high-cost instrumentation is not available. The optimal range of absorption cross sections for LAHM is from 0.1 to 5.0 cm2 (~1.0–50.0 µg soot) for 25 mm filters and 0.4 to 20 cm2 (4.0–200.0 µg soot) for 47 mm filters, with reduced sensitivity to higher values.

Potential impacts of lightning-induced plasma on cloud ice formation and precipitation have been a subject of debate for decades. Here, we report on the interaction of laser-generated plasma channels with water and ice clouds observed in a large cloud simulation chamber. Under the conditions of a typical storm cloud, in which ice and supercooled water coexist, no direct influence of the plasma channels on ice formation or precipitation processes could be detected. Under conditions typical for thin cirrus ice clouds, however, the plasma channels induced a surprisingly strong effect of ice multiplication. Within a few minutes, the laser action led to a strong enhancement of the total ice particle number density in the chamber by up to a factor of 100, even though only a 10 ⁻⁹ fraction of the chamber volume was exposed to the plasma channels. The newly formed ice particles quickly reduced the water vapor pressure to ice saturation, thereby increasing the cloud optical thickness by up to three orders of magnitude. A model relying on the complete vaporization of ice particles in the laser filament and the condensation of the resulting water vapor on plasma ions reproduces our experimental findings. This surprising effect might open new perspectives for remote sensing of water vapor and ice in the upper troposphere.