Search Results
Vertical profiles of aerosol mass concentration derived by unmanned airborne in situ and remote sensing instruments during dust events
In situ measurements using unmanned aerial vehicles (UAVs) and remote sensing observations can independently provide dense vertically resolved measurements of atmospheric aerosols, information which is strongly required in climate models. In both cases, inverting the recorded signals to useful information requires assumptions and constraints, and this can make the comparison of the results difficult. Here we compare, for the first time, vertical profiles of the aerosol mass concentration derived from light detection and ranging (lidar) observations and in situ measurements using an optical particle counter on board a UAV during moderate and weak Saharan dust episodes. Agreement between the two measurement methods was within experimental uncertainty for the coarse mode (i.e. particles having radii > 0.5 μm), where the properties of dust particles can be assumed with good accuracy. This result proves that the two techniques can be used interchangeably for determining the vertical profiles of aerosol concentrations, bringing them a step closer towards their systematic exploitation in climate models.
GARRLiC and LIRIC: Strengths and limitations for the characterization of dust and marine particles along with their mixtures
The Generalized Aerosol Retrieval from Radiometer and Lidar Combined data algorithm (GARRLiC) and the LIdar-Radiometer Inversion Code (LIRIC) provide the opportunity to study the aerosol vertical distribution by combining ground-based lidar and sun-photometric measurements. Here, we utilize the capabilities of both algorithms for the characterization of Saharan dust and marine particles, along with their mixtures, in the south-eastern Mediterranean during the CHARacterization of Aerosol mixtures of Dust and Marine origin Experiment (CHARADMExp). Three case studies are presented, focusing on dust-dominated, marinedominated and dust-marine mixing conditions. GARRLiC and LIRIC achieve a satisfactory characterization for the dust-dominated case in terms of particle microphysical properties and concentration profiles. The marine-dominated and the mixture cases are more challenging for both algorithms, although GARRLiC manages to provide more detailed microphysical retrievals compared to AERONET, while LIRIC effectively discriminates dust and marine particles in its concentration profile retrievals. The results are also compared with modelled dust and marine concentration profiles and surface in situ measurements.
Sensitivity of polar stratospheric ozone loss to uncertainties in chemical reaction kinetics
The impact and significance of uncertainties in model calculations of stratospheric ozone loss resulting from known uncertainty in chemical kinetics parameters is evaluated in trajectory chemistry simulations for the Antarctic and Arctic polar vortices. The uncertainty in modeled ozone loss is derived from Monte Carlo scenario simulations varying the kinetic (reaction and photolysis rate) parameters within their estimated uncertainty bounds. Simulations of a typical winter/spring Antarctic vortex scenario and Match scenarios in the Arctic produce large uncertainty in ozone loss rates and integrated seasonal loss. The simulations clearly indicate that the dominant source of model uncertainty in polar ozone loss is uncertainty in the Cl2O 2 photolysis reaction, which arises from uncertainty in laboratory-measured molecular cross sections at atmospherically important wavelengths. This estimated uncertainty in JCl 2O2 from laboratory measurements seriously hinders our ability to model polar ozone loss within useful quantitative error limits. Atmospheric observations, however, suggest that the Cl2O2 photolysis uncertainty may be less than that derived from the lab data. Comparisons to Match, South Pole ozonesonde, and Aura Microwave Limb Sounder (MLS) data all show that the nominal recommended rate simulations agree with data within uncertainties when the Cl2O2 photolysis error is reduced by a factor of two, in line with previous in situ ClOx measurements. Comparisons to simulations using recent cross sections from Pope et al. (2007) are outside the constrained error bounds in each case. Other reactions producing significant sensitivity in polar ozone loss include BrO + ClO and its branching ratios. These uncertainties challenge our confidence in modeling polar ozone depletion and projecting future changes in response to changing halogen emissions and climate. Further laboratory, theoretical, and possibly atmospheric studies are needed.
Biomass burning and urban emission impacts in the Andes Cordillera region based on in situ measurements from the Chacaltaya observatory, Bolivia (5240a.s.l.)
This study documents and analyses a 4-year continuous record of aerosol optical properties measured at the Global Atmosphere Watch (GAW) station of Chacaltaya (CHC; 5240a.s.l.), in Bolivia. Records of particle light scattering and particle light absorption coefficients are used to investigate how the high Andean Cordillera is affected by both long-range transport and by the fast-growing agglomeration of La Paz-El Alto, located approximately 20km away and 1.5km below the sampling site. The extended multi-year record allows us to study the properties of aerosol particles for different air mass types, during wet and dry seasons, also covering periods when the site was affected by biomass burning in the Bolivian lowlands and the Amazon Basin. The absorption, scattering, and extinction coefficients (median annual values of 0.74, 12.14, and 12.96Mm-1 respectively) show a clear seasonal variation with low values during the wet season (0.57, 7.94, and 8.68Mm-1 respectively) and higher values during the dry season (0.80, 11.23, and 14.51Mm-1 respectively). The record is driven by variability at both seasonal and diurnal scales. At a diurnal scale, all records of intensive and extensive aerosol properties show a pronounced variation (daytime maximum, night-time minimum), as a result of the dynamic and convective effects. The particle light absorption, scattering, and extinction coefficients are on average 1.94, 1.49, and 1.55 times higher respectively in the turbulent thermally driven conditions than the more stable conditions, due to more efficient transport from the boundary layer. Retrieved intensive optical properties are significantly different from one season to the other, reflecting the changing aerosol emission sources of aerosol at a larger scale. Using the wavelength dependence of aerosol particle optical properties, we discriminated between contributions from natural (mainly mineral dust) and anthropogenic (mainly biomass burning and urban transport or industries) emissions according to seasons and local circulation. The main sources influencing measurements at CHC are from the urban area of La Paz-El Alto in the Altiplano and from regional biomass burning in the Amazon Basin. Results show a 28% to 80% increase in the extinction coefficients during the biomass burning season with respect to the dry season, which is observed in both tropospheric dynamic conditions. From this analysis, long-term observations at CHC provide the first direct evidence of the impact of biomass burning emissions of the Amazon Basin and urban emissions from the La Paz area on atmospheric optical properties at a remote site all the way to the free troposphere. © Author(s) 2019.
Detecting impacts of extreme events with ecological in situ monitoring networks
Extreme hydrometeorological conditions typically impact ecophysiological processes on land. Satellite-based observations of the terrestrial biosphere provide an important reference for detecting and describing the spatiotemporal development of such events. However, in-depth investigations of ecological processes during extreme events require additional in situ observations. The question is whether the density of existing ecological in situ networks is sufficient for analysing the impact of extreme events, and what are expected event detection rates of ecological in situ networks of a given size. To assess these issues, we build a baseline of extreme reductions in the fraction of absorbed photosynthetically active radiation (FAPAR), identified by a new event detection method tailored to identify extremes of regional relevance. We then investigate the event detection success rates of hypothetical networks of varying sizes. Our results show that large extremes can be reliably detected with relatively small networks, but also reveal a linear decay of detection probabilities towards smaller extreme events in log–log space. For instance, networks with ≈ 100 randomly placed sites in Europe yield a ≥ 90 % chance of detecting the eight largest (typically very large) extreme events; but only a ≥ 50 % chance of capturing the 39 largest events. These findings are consistent with probability-theoretic considerations, but the slopes of the decay rates deviate due to temporal autocorrelation and the exact implementation of the extreme event detection algorithm. Using the examples of AmeriFlux and NEON, we then investigate to what degree ecological in situ networks can capture extreme events of a given size. Consistent with our theoretical considerations, we find that today's systematically designed networks (i.e. NEON) reliably detect the largest extremes, but that the extreme event detection rates are not higher than would be achieved by randomly designed networks. Spatio-temporal expansions of ecological in situ monitoring networks should carefully consider the size distribution characteristics of extreme events if the aim is also to monitor the impacts of such events in the terrestrial biosphere.
Evaluation of wake influence on high-resolution balloon-sonde measurements
Balloons are used for various in situ measurements in the atmosphere. On turbulence measurements from rising balloons there is a potential for misinterpreting wake-created fluctuations in the trail of the balloon for atmospheric turbulence. These wake effects have an influence on temperature and humidity measurements from radiosondes as well. The primary aim of this study is to assess the likelihood for wake encounter on the payload below a rising balloon. Therefore, we present a tool for calculating this probability based on radiosonde wind data. This includes a retrieval of vertical winds from the radiosonde and an uncertainty analysis of the wake assessment. Our wake evaluation tool may be used for any balloon-gondola distance and provides a significant refinement compared to existing assessments. We have analysed wake effects for various balloon-gondola distances applying atmospheric background conditions from a set of 30 radiosondes. For a standard radiosonde we find an average probability for wake encounter of 28 %, pointing out the importance of estimating wake effects on sounding balloons. Furthermore, we find that even millimetre-sized objects in the payload can have significant effects on high-resolution turbulence measurements, if they are located upstream of the turbulence sensor. © Author(s) 2019. This work is distributed under.
Microphysical investigation of the seeder and feeder region of an Alpine mixed-phase cloud
The seeder-feeder mechanism has been observed to enhance orographic precipitation in previous studies. However, the microphysical processes active in the seeder and feeder region are still being understood. In this paper, we investigate the seeder and feeder region of a mixed-phase cloud passing over the Swiss Alps, focusing on (1) fallstreaks of enhanced radar reflectivity originating from cloud top generating cells (seeder region) and (2) a persistent lowlevel feeder cloud produced by the boundary layer circulation (feeder region). Observations were obtained from a multidimensional set of instruments including ground-based remote sensing instrumentation (Ka-band polarimetric cloud radar, microwave radiometer, wind profiler), in situ instrumentation on a tethered balloon system, and ground-based aerosol and precipitation measurements. The cloud radar observations suggest that ice formation and growth were enhanced within cloud top generating cells, which is consistent with previous observational studies. However, uncertainties exist regarding the dominant ice formation mechanism within these cells. Here we propose different mechanisms that potentially enhance ice nucleation and growth in cloud top generating cells (convective overshooting, radiative cooling, droplet shattering) and attempt to estimate their potential contribution from an ice nucleating particle perspective. Once ice formation and growth within the seeder region exceeded a threshold value, the mixedphase cloud became fully glaciated. Local flow effects on the lee side of the mountain barrier induced the formation of a persistent low-level feeder cloud over a small-scale topographic feature in the inner-Alpine valley. In situ measurements within the low-level feeder cloud observed the production of secondary ice particles likely due to the Hallett-Mossop process and ice particle fragmentation upon ice-ice collisions. Therefore, secondary ice production may have been partly responsible for the elevated ice crystal number concentrations that have been previously observed in feeder clouds at mountaintop observatories. Secondary ice production in feeder clouds can potentially enhance orographic precipitation.
Long-term in situ observations of biomass burning aerosol at a high altitude station in Venezuela – Sources, impacts and interannual variability
First long-term observations of South American biomass burning aerosol within the tropical lower free troposphere are presented. The observations were conducted between 2007 and 2009 at a high altitude station (4765 m a.s.l.) on the Pico Espejo, Venezuela. Sub-micron particle volume, number concentrations of primary particles and particle absorption were observed. Orographic lifting and shallow convection leads to a distinct diurnal cycle at the station. It enables measurements within the lower free troposphere during night-time and observations of boundary layer air masses during daytime and at their transitional regions. The seasonal cycle is defined by a wet rainy season and a dry biomass burning season. The particle load of biomass burning aerosol is dominated by fires in the Venezuelan savannah. Increases of aerosol concentrations could not be linked to long-range transport of biomass burning plumes from the Amazon basin or Africa due to effective wet scavenging of particles. Highest particle concentrations were observed within boundary layer air masses during the dry season. Ambient sub-micron particle volume reached 1.4±1.3 μm3 cm−3, refractory particle number concentrations (at 300 °C) 510±420 cm−3 and the absorption coefficient 0.91±1.2 Mm−1. The respective concentrations were lowest within the lower free troposphere during the wet season and averaged at 0.19±0.25 μm3 cm−3, 150±94 cm−3 and 0.15±0.26 Mm−1. A decrease of particle concentrations during the dry seasons from 2007–2009 could be connected to a decrease in fire activity in the wider region of Venezuela using MODIS satellite observations. The variability of biomass burning is most likely linked to the El Niño–Southern Oscillation (ENSO). Low biomass burning activity in the Venezuelan savannah was observed to follow La Niña conditions, high biomass burning activity followed El Niño conditions.
Measurement report: Balloon-borne in situ profiling of Saharan dust over Cyprus with the UCASS optical particle counter
This paper presents measurements of mineral dust concentration in the diameter range from 0.4 to 14.0 µm with a novel balloon-borne optical particle counter, the Universal Cloud and Aerosol Sounding System (UCASS). The balloon launches were coordinated with ground-based active and passive remote-sensing observations and airborne in situ measurements with a research aircraft during a Saharan dust outbreak over Cyprus from 20 to 23 April 2017. The aerosol optical depth at 500 nm reached values up to 0.5 during that event over Cyprus, and particle number concentrations were as high as 50 cm−3 for the diameter range between 0.8 and 13.9 µm. Comparisons of the total particle number concentration and the particle size distribution from two cases of balloon-borne measurements with aircraft observations show reasonable agreement in magnitude and shape despite slight mismatches in time and space. While column-integrated size distributions from balloon-borne measurements and ground-based remote sensing show similar coarse-mode peak concentrations and diameters, they illustrate the ambiguity related to the missing vertical information in passive sun photometer observations. Extinction coefficient inferred from the balloon-borne measurements agrees with those derived from coinciding Raman lidar observations at height levels with particle number concentrations smaller than 10 cm−3 for the diameter range from 0.8 to 13.9 µm. An overestimation of the UCASS-derived extinction coefficient of a factor of 2 compared to the lidar measurement was found for layers with particle number concentrations that exceed 25 cm−3, i.e. in the centre of the dust plume where particle concentrations were highest. This is likely the result of a variation in the refractive index and the shape and size dependency of the extinction efficiency of dust particles along the UCASS measurements. In the future, profile measurements of the particle number concentration and particle size distribution with the UCASS could provide a valuable addition to the measurement capabilities generally used in field experiments that are focussed on the observation of coarse aerosols and clouds.
Aircraft-based observations of isoprene-epoxydiol-derived secondary organic aerosol (IEPOX-SOA) in the tropical upper troposphere over the Amazon region
During the ACRIDICON-CHUVA field project (September-October 2014; based in Manaus, Brazil) aircraft-based in situ measurements of aerosol chemical composition were conducted in the tropical troposphere over the Amazon using the High Altitude and Long Range Research Aircraft (HALO), covering altitudes from the boundary layer (BL) height up to 14.4km. The submicron non-refractory aerosol was characterized by flash-vaporization/electron impact-ionization aerosol particle mass spectrometry. The results show that significant secondary organic aerosol (SOA) formation by isoprene oxidation products occurs in the upper troposphere (UT), leading to increased organic aerosol mass concentrations above 10km altitude. The median organic mass concentrations in the UT above 10km range between 1.0 and 2.5μgm-3 (referring to standard temperature and pressure; STP) with interquartile ranges of 0.6 to 3.2μgm-3 (STP), representing 78% of the total submicron non-refractory aerosol particle mass. The presence of isoprene-epoxydiol-derived secondary organic aerosol (IEPOX-SOA) was confirmed by marker peaks in the mass spectra. We estimate the contribution of IEPOX-SOA to the total organic aerosol in the UT to be about 20%. After isoprene emission from vegetation, oxidation processes occur at low altitudes and/or during transport to higher altitudes, which may lead to the formation of IEPOX (one oxidation product of isoprene). Reactive uptake or condensation of IEPOX on preexisting particles leads to IEPOX-SOA formation and subsequently increasing organic mass in the UT. This organic mass increase was accompanied by an increase in the nitrate mass concentrations, most likely due to NOx production by lightning. Analysis of the ion ratio of NO+ to NO2+ indicated that nitrate in the UT exists mainly in the form of organic nitrate. IEPOX-SOA and organic nitrates are coincident with each other, indicating that IEPOX-SOA forms in the UT either on acidic nitrate particles forming organic nitrates derived from IEPOX or on already neutralized organic nitrate aerosol particles.