217 research outputs found
Simulating the influence of primary biological aerosol particles on clouds by heterogeneous ice nucleation
Primary ice formation, which is an important process for mixed-phase clouds with an impact on their lifetime, radiative balance, and hence the climate, strongly depends on the availability of ice-nucleating particles (INPs). Supercooled droplets within these clouds remain liquid until an INP immersed in or colliding with the droplet reaches its activation temperature. Only a few aerosol particles are acting as INPs and the freezing efficiency varies among them. Thus, the fraction of supercooled water in the cloud depends on the specific properties and concentrations of the INPs. Primary biological aerosol particles (PBAPs) have been identified as very efficient INPs at high subzero temperatures, but their very low atmospheric concentrations make it difficult to quantify their impact on clouds.
Here we use the regional atmospheric model COSMO–ART to simulate the heterogeneous ice nucleation by PBAPs during a 1-week case study on a domain covering Europe. We focus on three highly ice-nucleation-active PBAP species, Pseudomonas syringae bacteria cells and spores from the fungi Cladosporium sp. and Mortierella alpina. PBAP emissions are parameterized in order to represent the entirety of bacteria and fungal spores in the atmosphere. Thus, only parts of the simulated PBAPs are assumed to act as INPs. The ice nucleation parameterizations are specific for the three selected species and are based on a deterministic approach. The PBAP concentrations simulated in this study are within the range of previously reported results from other modeling studies and atmospheric measurements. Two regimes of PBAP INP concentrations are identified: a temperature-limited and a PBAP-limited regime, which occur at temperatures above and below a maximal concentration at around −10 ∘C, respectively. In an ensemble of control and disturbed simulations, the change in the average ice crystal concentration by biological INPs is not statistically significant, suggesting that PBAPs have no significant influence on the average state of the cloud ice phase. However, if the cloud top temperature is below −15 ∘C, PBAP can influence the cloud ice phase and produce ice crystals in the absence of other INPs. Nevertheless, the number of produced ice crystals is very low and it has no influence on the modeled number of cloud droplets and hence the cloud structure
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An algal enzyme required for biosynthesis of the most abundant marine carotenoids.
Fucoxanthin and its derivatives are the main light-harvesting pigments in the photosynthetic apparatus of many chromalveolate algae and represent the most abundant carotenoids in the world's oceans, thus being major facilitators of marine primary production. A central step in fucoxanthin biosynthesis that has been elusive so far is the conversion of violaxanthin to neoxanthin. Here, we show that in chromalveolates, this reaction is catalyzed by violaxanthin de-epoxidase-like (VDL) proteins and that VDL is also involved in the formation of other light-harvesting carotenoids such as peridinin or vaucheriaxanthin. VDL is closely related to the photoprotective enzyme violaxanthin de-epoxidase that operates in plants and most algae, revealing that in major phyla of marine algae, an ancient gene duplication triggered the evolution of carotenoid functions beyond photoprotection toward light harvesting
Twin-plate Ice Nucleation Assay (TINA) with infrared detection for high-throughput droplet freezing experiments with biological ice nuclei in laboratory and field samples
For efficient analysis and characterization of biological ice nuclei under
immersion freezing conditions, we developed the Twin-plate Ice Nucleation Assay
(TINA) for high-throughput
droplet freezing experiments, in which the temperature profile and freezing
of each droplet is tracked by an infrared detector. In the fully automated
setup, a couple of independently cooled aluminum blocks carrying two 96-well
plates and two 384-well plates, respectively, are available to study ice
nucleation and freezing events simultaneously in hundreds of microliter-range
droplets (0.1–40 µL). A cooling system with two refrigerant
circulation loops is used for high-precision temperature control (uncertainty
 < 0.2 K), enabling measurements over a wide range of temperatures
( ∼  272–233 K) at variable cooling rates (up to 10 K min−1).The TINA instrument was tested and characterized in experiments with
bacterial and fungal ice nuclei (IN) from Pseudomonas syringae (Snomax®) and Mortierella alpina, exhibiting freezing curves in good agreement with literature
data. Moreover, TINA was applied to investigate the influence of chemical
processing on the activity of biological IN, in particular the effects of
oxidation and nitration reactions. Upon exposure of
Snomax® to O3 and NO2, the cumulative
number of IN active at 270–266 K decreased by more than 1 order of
magnitude. Furthermore, TINA was used to study aqueous extracts of
atmospheric aerosols, simultaneously investigating a multitude of samples
that were pre-treated in different ways to distinguish different kinds of
IN. For example, heat treatment and filtration indicated that most
biological IN were larger than 5 µm. The results confirm that TINA is
suitable for high-throughput experiments and efficient analysis of
biological IN in laboratory and field samples.</p
Ice Nucleation Activity of Perfluorinated Organic Acids.
Perfluorinated acids (PFAs) are widely used synthetic chemical compounds, highly resistant to environmental
degradation. The widespread PFA contamination in remote regions such as the High Arctic implies currently not understood long-range atmospheric transport pathways. Here, we report that perfluorooctanoic acid (PFOA) initiates heterogeneous ice nucleation at temperatures as high as −16 °C. In contrast, the eight-carbon octanoic acid, perfluorooctanesulfonic acid, and deprotonated PFOA showed poor ice nucleating capabilities. The ice nucleation ability of PFOA correlates with the formation of a PFOA monolayer at the air−water interface, suggesting a mechanism in which the aligned hydroxyl groups of the carboxylic acid moieties provide a lattice matching to ice. The ice nucleation capabilities of fluorinated compounds like PFOA might be relevant for cloud glaciation in the atmosphere and the removal of these persistent pollutants by wet deposition.MaxWater initiative from the Max Planck SocietyYe
Simulating the influence of primary biological aerosol particles on clouds by heterogeneous ice nucleation
Primary ice formation,
which is an important process for mixed-phase clouds with an impact on their
lifetime, radiative balance, and hence the climate, strongly depends on the
availability of ice-nucleating particles (INPs). Supercooled droplets within
these clouds remain liquid until an INP immersed in or colliding with the
droplet reaches its activation temperature. Only a few aerosol particles are
acting as INPs and the freezing efficiency varies among them. Thus, the
fraction of supercooled water in the cloud depends on the specific properties
and concentrations of the INPs. Primary biological aerosol particles (PBAPs)
have been identified as very efficient INPs at high subzero temperatures, but
their very low atmospheric concentrations make it difficult to quantify their
impact on clouds.Here we use the regional atmospheric model COSMO–ART to simulate the
heterogeneous ice nucleation by PBAPs during a 1-week case study on a domain
covering Europe. We focus on three highly ice-nucleation-active PBAP species,
Pseudomonas syringae bacteria cells and spores from the fungi
Cladosporium sp. and Mortierella alpina. PBAP emissions are
parameterized in order to represent the entirety of bacteria and fungal
spores in the atmosphere. Thus, only parts of the simulated PBAPs are assumed
to act as INPs. The ice nucleation parameterizations are specific for the
three selected species and are based on a deterministic approach. The PBAP
concentrations simulated in this study are within the range of previously
reported results from other modeling studies and atmospheric measurements.
Two regimes of PBAP INP concentrations are identified: a temperature-limited
and a PBAP-limited regime, which occur at temperatures above and below a
maximal concentration at around −10 °C, respectively. In an
ensemble of control and disturbed simulations, the change in the average ice
crystal concentration by biological INPs is not statistically significant,
suggesting that PBAPs have no significant influence on the average state of
the cloud ice phase. However, if the cloud top temperature is below −15 °C, PBAP can influence the cloud ice phase and produce ice
crystals in the absence of other INPs. Nevertheless, the number of produced
ice crystals is very low and it has no influence on the modeled number of
cloud droplets and hence the cloud structure.</p
Oligomerization and Nitration of the Grass Pollen Allergen Phl p 5 by Ozone, Nitrogen Dioxide, and Peroxynitrite: Reaction Products, Kinetics, and Health Effects
The allergenic and inflammatory potential of proteins can be enhanced by chemical modification upon exposure to atmospheric or physiological oxidants. The molecular mechanisms and kinetics of such modifications, however, have not yet been fully resolved. We investigated the oligomerization and nitration of the grass pollen allergen Phl p 5 by ozone (O(3)), nitrogen dioxide (NO(2)), and peroxynitrite (ONOO(–)). Within several hours of exposure to atmospherically relevant concentration levels of O(3) and NO(2), up to 50% of Phl p 5 were converted into protein oligomers, likely by formation of dityrosine cross-links. Assuming that tyrosine residues are the preferential site of nitration, up to 10% of the 12 tyrosine residues per protein monomer were nitrated. For the reaction with peroxynitrite, the largest oligomer mass fractions (up to 50%) were found for equimolar concentrations of peroxynitrite over tyrosine residues. With excess peroxynitrite, the nitration degrees increased up to 40% whereas the oligomer mass fractions decreased to 20%. Our results suggest that protein oligomerization and nitration are competing processes, which is consistent with a two-step mechanism involving a reactive oxygen intermediate (ROI), as observed for other proteins. The modified proteins can promote pro-inflammatory cellular signaling that may contribute to chronic inflammation and allergies in response to air pollution
Membranes Are Decisive for Maximum Freezing Efficiency of Bacterial Ice Nucleators
Ice-nucleating proteins (INPs) from Pseudomonas syringae are among
the most active ice nucleators known, enabling ice formation at temperatures close to
the melting point of water. The working mechanisms of INPs remain elusive, but their
ice nucleation activity has been proposed to depend on the ability to form large INP
aggregates. Here, we provide experimental evidence that INPs alone are not sufficient
to achieve maximum freezing efficiency and that intact membranes are critical. Ice
nucleation measurements of phospholipids and lipopolysaccharides show that these
membrane components are not part of the active nucleation site but rather enable
INP assembly. Substantially improved ice nucleation by INP assemblies is observed
for deuterated water, indicating stabilization of assemblies by the stronger hydrogen
bonds of D2O. Together, these results show that the degree of order/disorder and the
assembly size are critically important in determining the extent to which bacterial
INPs can facilitate ice nucleation.We thank L. Reichelt, N. Bothen, and N. M. Kropf for technical assistance. The TOC graphic and Figures 1 and 2B were created using BioRender.com.Ye
Water uptake of subpollen aerosol particles: Hygroscopic growth, cloud condensation nuclei activation, and liquid-liquid phase separation
Pollen grains emitted from vegetation can release subpollen particles (SPPs) that contribute to the fine fraction of atmospheric aerosols and may act as cloud condensation nuclei (CCN), ice nuclei (IN), or aeroallergens. Here, we investigate and characterize the hygroscopic growth and CCN activation of birch, pine, and rapeseed SPPs. A high-humidity tandem differential mobility analyzer (HHTDMA) was used to measure particle restructuring and water uptake over a wide range of relative humidity (RH) from 2 % to 99.5 %, and a continuous flow CCN counter was used for size-resolved measurements of CCN activation at supersaturations (S) in the range of 0.2 % to 1.2 %. For both subsaturated and supersaturated conditions, effective hygroscopicity parameters, κ, were obtained by Köhler model calculations. Gravimetric and chemical analyses, electron microscopy, and dynamic light scattering measurements were performed to characterize further properties of SPPs from aqueous pollen extracts such as chemical composition (starch, proteins, DNA, and inorganic ions) and the hydrodynamic size distribution of water-insoluble material. All investigated SPP samples exhibited a sharp increase of water uptake and κ above ∼95 % RH, suggesting a liquid–liquid phase separation (LLPS). The HHTDMA measurements at RH >95 % enable closure between the CCN activation at water vapor supersaturation and hygroscopic growth at subsaturated conditions, which is often not achieved when hygroscopicity tandem differential mobility analyzer (HTDMA) measurements are performed at lower RH where the water uptake and effective hygroscopicity may be limited by the effects of LLPS. Such effects may be important not only for closure between hygroscopic growth and CCN activation but also for the chemical reactivity, allergenic potential, and related health effects of SPPs
Hospital admission and risk assessment associated to exposure of fungal bioaerosols at a municipal landfill using statistical models
The object of this research to determine the statistical relationship
and degree of association between variables: hospital admission days and
diagnostic (disease) potentially associated to fungal bioaerosols exposure.
Admissions included acute respiratory infections, atopic dermatitis, pharyngitis
and otitis. Statistical analysis was done using Statgraphics Centurion XVI
software. In addition, was estimated the occupational exposure to fungal aerosols in stages of a landfill using BIOGAVAL method and represented by Golden
Surfer XVI program. Biological risk assessment with sentinel microorganism A.
fumigatus and Penicillium sp, indicated that occupational exposure to fungal
aerosols is Biological action level. Preventive measures should be taken to
reduce the risk of acquiring acute respiratory infections, dermatitis or other skin
infections
Spectral Intensity Bioaerosol Sensor (SIBS): an instrument for spectrally resolved fluorescence detection of single particles in real time
Primary biological aerosol particles (PBAPs) in the atmosphere are highly relevant
for the Earth system, climate, and public health. The analysis of PBAPs,
however, remains challenging due to their high diversity and large
spatiotemporal variability. For real-time PBAP analysis, light-induced
fluorescence (LIF) instruments have been developed and widely used in
laboratory and ambient studies. The interpretation of fluorescence data from
these instruments, however, is often limited by a lack of spectroscopic
information. This study introduces an instrument – the Spectral Intensity
Bioaerosol Sensor (SIBS; Droplet Measurement Technologies (DMT), Longmont,
CO, USA) – that resolves fluorescence spectra for single particles and thus
promises to expand the scope of fluorescent PBAP quantification and
classification.
The SIBS shares key design components with the latest versions of the
Wideband Integrated Bioaerosol Sensor (WIBS) and the findings presented here
are also relevant for the widely deployed WIBS-4A and WIBS-NEO as well as
other LIF instruments. The key features of the SIBS and the findings of this
study can be summarized as follows.
Particle sizing yields reproducible linear responses for particles in the
range of 300 nm to 20 µm. The lower sizing limit is significantly
smaller than for earlier commercial LIF instruments (e.g., WIBS-4A and the
Ultraviolet Aerodynamic Particle Sizer; UV-APS), expanding the analytical
scope into the accumulation-mode size range.
Fluorescence spectra are recorded for two excitation wavelengths (λex=285 and 370 nm) and a wide range of emission wavelengths
(λmean=302–721 nm) with a resolution of 16
detection channels, which is higher than for most other commercially
available LIF bioaerosol sensors.
Fluorescence spectra obtained for 16 reference compounds confirm that the
SIBS provides sufficient spectral resolution to distinguish major modes of
molecular fluorescence. For example, the SIBS resolves the spectral
difference between bacteriochlorophyll and chlorophyll a and b.
A spectral correction of the instrument-specific detector response is
essential to use the full fluorescence emission range.
Asymmetry factor (AF) data were assessed and were found to provide only
limited analytical information.
In test measurements with ambient air, the SIBS worked reliably and yielded
characteristically different spectra for single particles in the coarse mode
with an overall fluorescent particle fraction of ∼4 %
(3σ threshold), which is consistent with earlier studies in
comparable environments.</ul
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