ORCID Profile
0000-0003-4282-1264
Current Organisation
Wageningen University
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Publisher: Copernicus GmbH
Date: 31-10-2014
DOI: 10.5194/ACP-14-11525-2014
Abstract: Abstract. Vertical redistribution of HNO3 through large HNO3-containing particles associated with polar stratospheric clouds (PSCs) plays an important role in the chemistry of the Arctic winter stratosphere. During the RECONCILE (Reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interactions) c aign, apparently very large NAT (nitric acid trihydrate) particles were observed by the airborne in situ probe FSSP-100 (Molleker et al., 2014). Our analysis shows that the FSSP-100 observations associated with the flight on 25 January 2010 cannot easily be explained assuming compact spherical NAT particles due to much too short growing time at temperatures below the existence temperature of NAT (TNAT). State-of-the-art simulations using CLaMS (Chemical Lagrangian Model of the Stratosphere Grooß et al., 2014) suggest considerably smaller particles. We consider the hypothesis that the simulation reproduces the NAT particle masses in a realistic way, but that real NAT particles may have larger apparent sizes compared to compact spherical particles, e.g. due to non-compact morphology or aspheric shape. Our study focuses on the consequence that such particles would have reduced settling velocities compared to compact spheres, altering the vertical redistribution of HNO3. Utilising CLaMS simulations, we investigate the impact of reduced settling velocities of NAT particles on vertical HNO3 redistribution and compare the results with observations of gas-phase HNO3 by the airborne Fourier transform spectrometer MIPAS-STR associated with two RECONCILE flights. The MIPAS-STR observations confirm conditions consistent with denitrification by NAT particles for the flight on 25 January 2010 and show good agreement with the simulations within the limitations of the comparison. Best agreement is found if settling velocities between 100 and 50% relative to compact spherical particles are considered (slight preference for the 70% scenario). In contrast, relative settling velocities of 30% result in too weak vertical HNO3 redistribution. Sensitivity simulations considering temperature biases of ±1 K and multiplying the simulated nucleation rates by factors of 0.5 and 2.0 affect the comparisons to a similar extent, but result in no effective improvement compared to the reference scenario. Our results show that an accurate knowledge of the settling velocities of NAT particles is important for quantitative simulations of vertical HNO3 redistribution.
Publisher: Copernicus GmbH
Date: 02-02-2012
Abstract: Abstract. The photolysis rate constant of dichlorine peroxide (ClOOCl, ClO dimer) JClOOCl is a critical parameter in catalytic cycles destroying ozone (O3) in the polar stratosphere. In the atmospherically relevant wavelength region (λ 310 nm), significant discrepancies between laboratory measurements of ClOOCl absorption cross sections and spectra cause a large uncertainty in JClOOCl. Previous investigations of the consistency of published JClOOCl with atmospheric observations of chlorine monoxide (ClO) and ClOOCl have focused on the photochemical equilibrium between ClOOCl formation and photolysis, and thus could only constrain the ratio of JClOOCl over the ClOOCl formation rate constant krec. Here, we constrain the atmospherically effective JClOOCl independent of krec, using ClO measured in the same air masses before and directly after sunrise during an aircraft flight that was part of the RECONCILE field c aign in the winter 2010 from Kiruna, Sweden. Over sunrise, when the ClO/ClOOCl system comes out of thermal equilibrium and the influence of the ClO recombination reaction is negligible, the increase in ClO concentrations is significantly faster than expected from JClOOCl based on the absorption spectrum proposed by Pope et al. (2007), but does not warrant cross sections larger than recently published values by Papanastasiou et al. (2009). In particular, the existence of a significant ClOOCl absorption band longwards of 420 nm is not supported by our observations. The observed night-time ClO would not be consistent with a ClO/ClOOCl thermal equilibrium constant significantly higher than the one proposed by Plenge et al. (2005).
Publisher: Copernicus GmbH
Date: 04-01-2018
Publisher: Copernicus GmbH
Date: 04-01-2018
Abstract: Abstract. Secondary Organic Aerosol (SOA) particles have been found to be efficient ice nucleating particles under the cold conditions of (tropical) upper tropospheric cirrus clouds. Whether they also are efficient at initiating freezing at slightly warmer conditions as found in mixed phase clouds remains undetermined. Here, we study the ice nucleating ability of photo-chemically produced SOA particles with the combination of the Manchester Aerosol and Ice Cloud Chambers. Three SOA systems were tested resembling biogenic/anthropogenic particles and particles of different phase state. After the aerosol particles were formed, they were transferred into the cloud chamber where subsequent quasi-adiabatic cloud evacuations were performed. Additionally, the ice forming abilities of ammonium sulfate and kaolinite were investigated as a reference to test the experimental setup. Clouds were formed in the temperature range of −20 °C to −28.6 °C. Only the reference experiment using dust particles showed evidence of ice nucleation. No ice particles were observed in any other experiment. Thus, we conclude that SOA particles produced under the conditions of the reported experiments are not efficient ice nucleating particles starting at liquid saturation under mixed-phase cloud conditions.
Publisher: Copernicus GmbH
Date: 12-07-2022
Abstract: Abstract. The Fast Infrared Hygrometer (FIRH), employing open-path tunable diode laser absorption spectroscopy at the wavelengths near the 1364.6896 nm line, was adapted to perform contactless humidity measurements at the Turbulent Leipzig Aerosol Cloud Interaction Simulator (LACIS-T), a unique turbulent moist-air wind tunnel. The configuration of the setup allows for scanning from outside the walls of the wind tunnel and at various positions without the need for repeated optics adjustments. We identified three factors which significantly influence the measurement – self-broadening of the absorption line, interference in the glass windows and parasitic absorption in the ambient air outside the wind tunnel – and developed correction methods which satisfactorily account for these effects. The comparison between FIRH and a reference hygrometer (dew-point mirror MBW 973) indicated a good agreement within the expected errors across the wide range of water vapour concentration 1.0–6.1×1017 cm−3 (equivalent to dew-point temperature of −5.4 to +21 ∘C at the temperature of 23 ∘C). High temporal resolution (∼2 kHz) allowed for studying turbulent fluctuations in the course of intensive mixing of two air streams which had the same mean velocity but differed in temperature and humidity, also including the settings for which the mixture can be supersaturated. The obtained results contribute to improved understanding and interpretation of cloud formation studies conducted in LACIS-T by complementing the previous characterizations of turbulent velocity and temperature fields inside the wind tunnel.
Publisher: Copernicus GmbH
Date: 30-09-2010
Abstract: Abstract. Lineshaped contrails were detected with the research aircraft Falcon during the CONCERT – CONtrail and Cirrus ExpeRimenT – c aign in October/November 2008. The Falcon was equipped with a set of instruments to measure the particle size distribution, shape, extinction and chemical composition as well as trace gas mixing ratios of sulfur dioxide (SO2), reactive nitrogen and halogen species (NO, NOy, HNO3, HONO, HCl), ozone (O3) and carbon monoxide (CO). During 12 mission flights over Europe, numerous contrails, cirrus clouds and a volcanic aerosol layer were probed at altitudes between 8.5 and 11.6 km and at temperatures above 213 K. 22 contrails from 11 different aircraft were observed near and below ice saturation. The observed NO mixing ratios, ice crystal and soot number densities are compared to a process based contrail model. On 19 November 2008 the contrail from a CRJ-2 aircraft was penetrated in 10.1 km altitude at a temperature of 221 K. The contrail had mean ice crystal number densities of 125 cm−3 with effective radii reff of 2.6 μm. The presence of particles with r μm in the less than 2 min old contrail suggests that natural cirrus crystals were entrained in the contrail. Mean HONO/NO (HONO/NOy) ratios of 0.037 (0.024) and the fuel sulfur conversion efficiency to H2SO4 (εS↓) of 2.9 % observed in the CRJ-2 contrail are in the range of previous measurements in the gaseous aircraft exhaust. On 31 October 2010 aviation NO emissions could have contributed by more than 40% to the regional scale NO levels in the mid-latitude lowest stratosphere. The CONCERT observations help to better quantify the climate impact from contrails and will be used to investigate the chemical processing of trace gases on contrails.
Publisher: Copernicus GmbH
Date: 16-06-2011
Abstract: Abstract. In situ measurements of ice crystal size distributions in tropical upper troposphere/lower stratosphere (UT/LS) clouds were performed during the SCOUT-AMMA c aign over West Africa in August 2006. The cloud properties were measured with a Forward Scattering Spectrometer Probe (FSSP-100) and a Cloud Imaging Probe (CIP) operated aboard the Russian high altitude research aircraft M-55 Geophysica with the mission base in Ouagadougou, Burkina Faso. A total of 117 ice particle size distributions were obtained from the measurements in the vicinity of Mesoscale Convective Systems (MCS). Two to four modal lognormal size distributions were fitted to the average size distributions for different potential temperature bins. The measurements showed proportionately more large ice particles compared to former measurements above maritime regions. With the help of trace gas measurements of NO, NOy, CO2, CO, and O3 and satellite images, clouds in young and aged MCS outflow were identified. These events were observed at altitudes of 11.0 km to 14.2 km corresponding to potential temperature levels of 346 K to 356 K. In a young outflow from a developing MCS ice crystal number concentrations of up to (8.3 ± 1.6) cm−3 and rimed ice particles with maximum dimensions exceeding 1.5 mm were found. A maximum ice water content of 0.05 g m−3 was observed and an effective radius of about 90 μm. In contrast the aged outflow events were more diluted and showed a maximum number concentration of 0.03 cm−3, an ice water content of 2.3 × 10−4 g m−3, an effective radius of about 18 μm, while the largest particles had a maximum dimension of 61 μm. Close to the tropopause subvisual cirrus were encountered four times at altitudes of 15 km to 16.4 km. The mean ice particle number concentration of these encounters was 0.01 cm−3 with maximum particle sizes of 130 μm, and the mean ice water content was about 1.4 × 10−4 g m−3. All known in situ measurements of subvisual tropopause cirrus are compared and an exponential fit on the size distributions is established for modelling purposes. A comparison of aerosol to ice crystal number concentrations, in order to obtain an estimate on how many ice particles may result from activation of the present aerosol, yielded low ratios for the subvisual cirrus cases of roughly one cloud particle per 30 000 aerosol particles, while for the MCS outflow cases this resulted in a high ratio of one cloud particle per 300 aerosol particles.
Publisher: Copernicus GmbH
Date: 14-01-2015
DOI: 10.5194/ACPD-15-1041-2015
Abstract: Abstract. In this study we examine the simulated downward transport and mixing of stratospheric air into the upper tropical troposphere as observed on a research flight during the SCOUT-O3 c aign in connection to a deep convective system. We use the Advanced Research Weather and Research Forecasting (WRF-ARW) model with a horizontal resolution of 333 m to examine this downward transport. The simulation reproduces the deep convective system, its timing and overshooting altitudes reasonably well compared to radar and aircraft observations. Passive tracers initialised at pre-storm times indicate the downward transport of air from the stratosphere to the upper troposphere as well as upward transport from the boundary layer into the cloud anvils and overshooting tops. For ex le, a passive ozone tracer (i.e. a tracer not undergoing chemical processing) shows an enhancement in the upper troposphere of up to about 30 ppbv locally in the cloud, while the in situ measurements show an increase of 50 ppbv. However, the passive carbon monoxide tracer exhibits an increase, while the observations show a decrease of about 10 ppbv, indicative of an erroneous model representation of the transport processes in the tropical tropopause layer. Furthermore, it could point to insufficient entrainment and detrainment in the model. The simulation shows a general moistening of air in the lower stratosphere but it also exhibits local dehydration features. Here we use the model to explain the processes causing the transport and also expose areas of inconsistencies between the model and observations.
Publisher: Copernicus GmbH
Date: 06-05-2009
Abstract: Abstract. A new airborne tandem measurement platform for cloud-radiation interaction studies is introduced in this paper. It consists of a Learjet 35A research aircraft and the AIRcraft TOwed Sensor Shuttle (AIRTOSS), which is an instrumented drag-body towed by the Learjet. Currently, the AIRTOSS is instrumented with a Cloud Imaging Probe (CIP) for measuring cloud microphysical properties and an Inertial Navigation System (INS) for measurements of flight attitudes. The cable dragging AIRTOSS can be as long as four kilometres. Thus, truly collocated measurements in two altitudes above, in, and below clouds can be obtained. Results from first test flights with Learjet and AIRTOSS are reported here. The flights were performed from Hohn Airport, Germany. Specific manoeuvres were flown to test the aerodynamic behaviour of the drag-body and to investigate the suitability of AIRTOSS for high-precision irradiance measurements which require a stable flight attitude of AIRTOSS. The flight attitude data show that AIRTOSS is sensitive to several flight manoeuvres such as turns, altitude and airspeed changes, and also to changes of towing cable length. The effects of these manoeuvres on the attitude angles of AIRTOSS have been quantified. Maximum roll angle deviations were observed during turns. Even small changes in heading can lead to high roll angles (one degree change in heading causes a change in roll angle of about eight degrees). The pitch angle varies during climb or e periods, extending or retracting of towing cable, acceleration or deceleration, and even when flying at too low or too high true airspeed depending on altitude. Values of pitch angle between −5° ( e) and 8° (climb and retracting towing cable) have been observed. While change in attitude is not problematic for cloud particle property measurements it is for radiation measurements. Here, the deviation from the horizontal should be no more than 3° to avoid large errors. When keeping the above mentioned flight parameters constant, sufficiently stable flight conditions can be maintained to perform high-quality irradiance measurements with AIRTOSS in future experiments. During this test c aign also observations of cloud microphysical data as for ex le droplet number concentrations and size distributions with the AIRTOSS in stratocumulus clouds were performed to prove the compliance with scientific needs. Simultaneous spectral cloud radiation measurements have been made. The measurements of internal operational data of AIRTOSS as well as the first atmospheric data demonstrate the suitability of this tandem platform for detailed cloud microphysics and radiation interaction studies.
Publisher: American Geophysical Union (AGU)
Date: 10-09-2010
DOI: 10.1029/2009JD013093
Publisher: Copernicus GmbH
Date: 18-09-2009
Abstract: Abstract. In-situ ice crystal size distribution measurements are presented within the tropical troposphere and lower stratosphere. The measurements were performed using a combination of a Forward Scattering Spectrometer Probe (FSSP-100) and a Cloud Imaging Probe (CIP), which were installed on the Russian high altitude research aircraft M55 "Geophysica" during the SCOUT-O3 c aign in Darwin, Australia. One of the objectives of the c aign was to characterise the Hector convective system, which appears on an almost daily basis during the pre-monsoon season over the Tiwi Islands, north of Darwin. In total 90 encounters with ice clouds, between 10 and 19 km altitude were selected from the dataset and were analysed. Six of these encounters were observed in the lower stratosphere, up to 1.4 km above the local tropopause. Concurrent lidar measurements on board "Geophysica" indicate that these ice clouds were a result of overshooting convection. Large ice crystals, with a maximum dimension up to 400 μm, were observed in the stratosphere. The stratospheric ice clouds included an ice water content ranging from 7.7×10−5 to 8.5×10−4 g m−3 and were observed at ambient relative humidities (with respect to ice) between 75 and 157%. Three modal lognormal size distributions were fitted to the average size distributions for different potential temperature intervals, showing that the shape of the size distribution of the stratospheric ice clouds are similar to those observed in the upper troposphere. In the tropical troposphere the effective radius of the ice cloud particles decreases from 100 μm at about 10 km altitude, to 3 μm at the tropopause, while the ice water content decreases from 0.04 to 10−5 g m−3. No clear trend in the number concentration was observed with altitude, due to the thin and inhomogeneous characteristics of the observed cirrus clouds. The ice water content calculated from the observed ice crystal size distribution is compared to the ice water content derived from two hygrometer instruments. This independent measurement of the ice water content agrees within the combined uncertainty of the instruments for ice water contents exceeding 3×10−4g m−3. Stratospheric residence times, calculated based on gravitational settling, and evaporation rates show that the ice crystals observed in the stratosphere over the Hector storm system had a high potential of humidifying the stratosphere locally. Utilizing total aerosol number concentration measurements from a four channel condensation particle counter during two separate c aigns, it can be shown that the fraction of ice particles to the number of aerosol particles remaining ranges from 1:300 to 1:30 000 for tropical upper tropospheric ice clouds with ambient temperatures below −75°C.
Publisher: Copernicus GmbH
Date: 13-05-2014
DOI: 10.5194/ACPD-14-12071-2014
Abstract: Abstract. In January 2010 and December 2011 synoptic scale PSC fields were probed during seven flights of the high altitude research aircraft M-55 Geophysica within the RECONCILE (Reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interaction.) and the ESSenCe (ESSenCe: ESA Sounder C aign) projects. Particle size distributions in a diameter range between 0.46 μm and 40 μm were recorded simultaneously by up to four different optical in situ instruments. Three of these particle instruments are based on the detection of forward scattered light by single particles. The fourth instrument is a grey scale optical array imaging probe. Optical particle diameters of up to 35 μm were detected with particle number densities and total particle volumes exceeding previous Arctic measurements. Also, gas phase and particle bound NOy were measured, as well as water vapor concentrations, and other variables. Two remote sensing particle instruments, the Miniature Aerosol Lidar (MAL) and the backscatter sonde (MAS, Multiwavelenght Aerosol Scatterometer) showed the synoptic scale of the encountered PSCs. The particle mode below 2 μm in size diameter has been identified as supercooled ternary solution droplets (STS). The PSC particles in the size range above 2 μm in diameter are considered to consist of nitric acid hydrates or ice, and the particles' high HNO3 content was confirmed by the NOy instrument. Assuming a particle composition of nitric acid trihydrate (NAT), the optically measured size distributions result in particle-phase HNO3 mixing ratios exceeding available stratospheric values. In particular, with respect to the denitrification by sedimentation of large HNO3-contaning particles, generally considered as NAT, our new measurements raise questions concerning composition, shape and nucleation pathways. Measurement uncertainties are discussed concerning probable overestimations of measured particle sizes and volumes. We hypothesize that either a strong asphericity or the particle composition (e.g. water-ice coated with NAT) could explain our observations.
Publisher: Copernicus GmbH
Date: 12-01-2011
Abstract: Abstract. Airborne in-situ observations of ClO in the tropics were made during the TROCCINOX (Aracatuba, Brazil, February 2005) and SCOUT-O3 (Darwin, Australia, November/December 2005) field c aigns. While during most flights significant amounts of ClO (≈10–20 parts per trillion, ppt) were present only in aged stratospheric air, instances of enhanced ClO mixing ratios of up to 40 ppt – significantly exceeding those expected from gas phase chemistry – were observed in air masses of a more tropospheric character. Most of these observations are associated with low temperatures or with the presence of cirrus clouds (often both), suggesting that cirrus ice particles and/or liquid aerosol at low temperatures may promote significant heterogeneous chlorine activation in the tropical upper troposphere lower stratosphere (UTLS). In two case studies, particularly high levels of ClO observed were reproduced by chemistry simulations only under the assumption that significant denoxification had occurred in the observed air. However, to reproduce the ClO observations in these simulations, O3 mixing ratios higher than observed had to be assumed, and at least for one of these flights, a significant denoxification is in contrast to the observed NO levels, suggesting that the coupling of chlorine and nitrogen compounds in the tropical UTLS may not be completely understood.
Publisher: Copernicus GmbH
Date: 14-10-2014
DOI: 10.5194/ACP-14-10785-2014
Abstract: Abstract. In January 2010 and December 2011, synoptic-scale polar stratospheric cloud (PSC) fields were probed during seven flights of the high-altitude research aircraft M-55 Geophysica within the RECONCILE (Reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interaction) and the ESSenCe (ESSenCe: ESA Sounder C aign) projects. Particle size distributions in a diameter range between 0.46 and 40μm were recorded by four different optical in situ instruments. Three of these particle instruments are based on the detection of forward-scattered light by single particles. The fourth instrument is a grayscale optical array imaging probe. Optical particle diameters of up to 35μm were detected with particle number densities and total particle volumes exceeding previous Arctic measurements. Also, gas-phase and particle-bound NOy was measured, as well as water vapor concentrations. The optical characteristics of the clouds were measured by the remote sensing lidar MAL (Miniature Aerosol Lidar) and by the in situ backscatter sonde MAS (Multiwavelength Aerosol Scatterometer), showing the synoptic scale of the encountered PSCs. The particle mode below 2μm in size diameter has been identified as supercooled ternary solution (STS) droplets. The PSC particles in the size range above 2μm in diameter are considered to consist of nitric acid hydrates, and the particles' high HNO3 content was confirmed by the NOy instrument. Assuming a particle composition of nitric acid trihydrate (NAT), the optically measured size distributions result in particle-phase HNO3 mixing ratios exceeding available stratospheric values. Therefore the measurement uncertainties concerning probable overestimations of measured particle sizes and volumes are discussed in detail. We hypothesize that either a strong asphericity or an alternate particle composition (e.g., water ice coated with NAT) could explain our observations. In particular, with respect to the denitrification by sedimentation of large HNO3-containing particles, generally considered to be NAT, our new measurements raise questions concerning composition, shape and nucleation pathways. Answering these would improve the numerical simulation of PSC microphysical processes like cloud particle formation, growth and denitrification, which is necessary for better predictions of future polar ozone losses, especially under changing global climate conditions. Generally, it seems that the occurrence of large NAT particles – sometimes termed "NAT rocks" – are a regular feature of synoptic-scale PSCs in the Arctic.
Publisher: Copernicus GmbH
Date: 16-09-2013
Abstract: Abstract. The international research project RECONCILE has addressed central questions regarding polar ozone depletion, with the objective to quantify some of the most relevant yet still uncertain physical and chemical processes and thereby improve prognostic modelling capabilities to realistically predict the response of the ozone layer to climate change. This overview paper outlines the scope and the general approach of RECONCILE, and it provides a summary of observations and modelling in 2010 and 2011 that have generated an in many respects unprecedented dataset to study processes in the Arctic winter stratosphere. Principally, it summarises important outcomes of RECONCILE including (i) better constraints and enhanced consistency on the set of parameters governing catalytic ozone destruction cycles, (ii) a better understanding of the role of cold binary aerosols in heterogeneous chlorine activation, (iii) an improved scheme of polar stratospheric cloud (PSC) processes that includes heterogeneous nucleation of nitric acid trihydrate (NAT) and ice on non-volatile background aerosol leading to better model parameterisations with respect to denitrification, and (iv) long transient simulations with a chemistry-climate model (CCM) updated based on the results of RECONCILE that better reproduce past ozone trends in Antarctica and are deemed to produce more reliable predictions of future ozone trends. The process studies and the global simulations conducted in RECONCILE show that in the Arctic, ozone depletion uncertainties in the chemical and microphysical processes are now clearly smaller than the sensitivity to dynamic variability.
Publisher: Copernicus GmbH
Date: 23-09-2016
DOI: 10.5194/ACP-16-11883-2016
Abstract: Abstract. Aerosols of the volcanic degassing plumes from Mt. Etna and Mt. Stromboli were probed with in situ instruments on board the Deutsches Zentrum für Luft- und Raumfahrt research aircraft Falcon during the contrail, volcano, and cirrus experiment CONCERT in September 2011. Aerosol properties were analyzed using angular-scattering intensities and particle size distributions measured simultaneously with the Polar Nephelometer and the Forward Scattering Spectrometer probes (FSSP series 100 and 300), respectively. Aerosols of degassing plumes are characterized by low values of the asymmetry parameter (between 0.6 and 0.75) the effective diameter was within the range of 1.5–2.8 µm and the maximal diameter was lower than 20 µm. A principal component analysis applied to the Polar Nephelometer data indicates that scattering features of volcanic aerosols of different crater origins are clearly distinctive from angular-scattering intensities of cirrus and contrails. Retrievals of aerosol properties revealed that the particles were "optically spherical" and the estimated values of the real part of the refractive index are within the interval from 1.35 to 1.38. The interpretation of these results leads to the conclusion that the degassing plume aerosols were porous with air voids. Our estimates suggest that aerosol particles contained about 18 to 35 % of air voids in terms of the total volume.
Publisher: Copernicus GmbH
Date: 12-06-2015
Abstract: Abstract. In this study we examine the simulated downward transport and mixing of stratospheric air into the upper tropical troposphere as observed on a research flight during the SCOUT-O3 c aign in connection with a deep convective system. We use the Advanced Research Weather and Research Forecasting (WRF-ARW) model with a horizontal resolution of 333 m to examine this downward transport. The simulation reproduces the deep convective system, its timing and overshooting altitudes reasonably well compared to radar and aircraft observations. Passive tracers initialised at pre-storm times indicate the downward transport of air from the stratosphere to the upper troposphere as well as upward transport from the boundary layer into the cloud anvils and overshooting tops. For ex le, a passive ozone tracer (i.e. a tracer not undergoing chemical processing) shows an enhancement in the upper troposphere of up to about 30 ppbv locally in the cloud, while the in situ measurements show an increase of 50 ppbv. However, the passive carbon monoxide tracer exhibits an increase, while the observations show a decrease of about 10 ppbv, indicative of an erroneous model representation of the transport processes in the tropical tropopause layer. Furthermore, it could point to insufficient entrainment and detrainment in the model. The simulation shows a general moistening of air in the lower stratosphere, but it also exhibits local dehydration features. Here we use the model to explain the processes causing the transport and also expose areas of inconsistencies between the model and observations.
Publisher: Wiley
Date: 2008
DOI: 10.1002/QJ.205
Publisher: Copernicus GmbH
Date: 29-09-2011
Abstract: Abstract. New particle formation (NPF), which generates nucleation mode aerosol, was observed in the tropical Upper Troposphere (UT) and Tropical Tropopause Layer (TTL) by in situ airborne measurements over South America (January–March 2005), Australia (November–December 2005), West Africa (August 2006) and Central America (2004–2007). Particularly intense NPF was found at the bottom of the TTL. Measurements with a set of condensation particle counters (CPCs) with different dp50 (50% lower size detection efficiency diameter or "cut-off diameter") were conducted on board the M-55 Geophysica in the altitude range of 12.0–20.5 km and on board the DLR Falcon-20 at up to 11.5 km altitude. On board the NASA WB-57F size distributions were measured over Central America in the 4 to 1000 nm diameter range with a system of nucleation mode aerosol spectrometers. Nucleation mode particle concentrations (NNM) were derived from these measurements which allow for identifying many NPF events with NNM in the range of thousands of particles per cm3. Over Australia and West Africa, we identified NPF in the outflow of tropical convection, in particular of a Mesoscale Convective System (MCS). Newly formed particles with NNM 1000 cm−3 were found to coexist with ice cloud particles (dp 2 μm) as long as cloud particle concentrations remained below 2 cm−3. The occurrence of NPF within the upper troposphere and the TTL was generally confined within 340 K to 380 K potential temperature, but NPF was of particular strength between 350 K and 370 K (i.e. ~1–4 km below the cold point tropopause). Analyses of the aerosol volatility (at 250 °C) show that in the TTL on average 75–90% of the particles were volatile, compared to typically only 50% in the extra-tropical UT, indicative for the particles to mainly consist of H2SO4-H2O and possibly organic compounds. Along two flight segments over Central and South America (24 February 2005 and 7 August 2006, at 12.5 km altitude) in cloud free air, above thin cirrus, particularly high NNM were observed. Recent lifting had influenced the probed air masses, and NNM reached up to 16 000 particles cm−3 (ambient concentration). A sensitivity study using an aerosol model, which includes neutral and ion induced nucleation processes, simulates NNM in reasonable agreement with the in situ observations of clear-air NPF. Based on new, stringent multi-CPC criteria, our measurements corroborate the hypothesis that the tropical UT and the TTL are regions supplying freshly nucleated particles. Our findings narrow the altitude of the main source region to the bottom TTL, i.e. to the level of main tropical convection outflow, and, by means of measurements of carbon monoxide, they indicate the importance of anthropogenic emissions in NPF. After growth and/or coalescence the nucleation mode particles may act as cloud condensation nuclei in the tropical UT, or, upon ascent into the stratosphere, contribute to maintain the stratospheric background aerosol.
Publisher: Copernicus GmbH
Date: 11-12-2014
DOI: 10.5194/ACP-14-13223-2014
Abstract: Abstract. The case study presented here focuses on the life cycle of clouds in the anvil region of a tropical deep convective system. During the SCOUT-O3 c aign from Darwin, Northern Australia, the Hector storm system has been probed by the Geophysica high-altitude aircraft. Clouds were observed by in situ particle probes, a backscatter sonde, and a miniature lidar. Additionally, aerosol number concentrations have been measured. On 30 November 2005 a double flight took place and Hector was probed throughout its life cycle in its developing, mature, and dissipating stage. The two flights were four hours apart and focused on the anvil region of Hector in altitudes between 10.5 and 18.8 km (i.e. above 350 K potential temperature). Trajectory calculations, satellite imagery, and ozone measurements have been used to ensure that the same cloud air masses have been probed in both flights. The size distributions derived from the measurements show a change not only with increasing altitude but also with the evolution of Hector. Clearly different cloud to aerosol particle ratios as well as varying ice crystal morphology have been found for the different development stages of Hector, indicating different freezing mechanisms. The development phase exhibits the smallest ice particles (up to 300 μm) with a rather uniform morphology. This is indicative for rapid glaciation during Hector's development. Sizes of ice crystals are largest in the mature stage (larger than 1.6 mm) and even exceed those of some continental tropical deep convective clouds, also in their number concentrations. The backscatter properties and particle images show a change in ice crystal shape from the developing phase to rimed and aggregated particles in the mature and dissipating stages the specific shape of particles in the developing phase cannot be distinguished from the measurements. Although optically thin, the clouds in the dissipating stage have a large vertical extent (roughly 6 km) and persist for at least 6 h. Thus, the anvils of these high-reaching deep convective clouds have a high potential for affecting the tropical tropopause layer by modifying the humidity and radiative budget, as well as for providing favourable conditions for subvisible cirrus formation. The involved processes may also influence the amount of water vapour that ultimately reaches the stratosphere in the tropics.
Publisher: Copernicus GmbH
Date: 17-03-2022
DOI: 10.5194/AMT-2022-79
Abstract: Abstract. The Fast Infrared Hygrometer (FIRH), employing open-path tunable diode laser absorption spectroscopy at the wavelengths near 1364.6896 nm line, was adapted to perform contactless humidity measurements at the Turbulent Leipzig Aerosol Cloud Interaction Simulator (LACIS-T), a unique turbulent moist-air wind tunnel. The configuration of the setup allows for scanning at various positions without the need for repeated optics adjustments. We identified three factors which significantly influence the measurement – self-broadening of the absorption line, interference in the glass windows and parasitic absorption in the ambient air outside the tunnel – and developed correction methods which satisfactorily account for these effects. The comparison between FIRH and a reference hygrometer (dew-point mirror MBW 973) indicated a good agreement within the expected errors across the wide range of water vapor concentration 1.0 . . . 6.1 cm−3 (equivalent to dew-point temperature of −5.4 . . . + 21 °C at the temperature of 23 °C). High temporal resolution (∼2 kHz) allowed for studying turbulent fluctuations in the course of intensive mixing of two air streams which had the same mean velocity but differed in temperature and humidity, including also the settings for which the mixture can be supersaturated. The obtained results complement the previous characterizations of turbulent velocity and temperature fields in LACIS-T. The variance of water vapor concentration exhibits a maximum in the center of the mixing zone which coincides with the steepest gradient.
Publisher: Copernicus GmbH
Date: 12-05-2014
DOI: 10.5194/ACPD-14-11815-2014
Abstract: Abstract. The case study presented here focusses on the life cycle of clouds in a tropical deep convective system. During the SCOUT-O3 c aign from Darwin, Northern Australia, the Hector storm system has been probed by the Geophysica high altitude aircraft. Clouds were observed by in situ particle probes, a backscatter sonde, and a miniature lidar. Additionally, aerosol number concentrations have been measured. On 30 November 2005 a double flight took place and Hector was probed throughout its life cycle in its developing, mature, and dissipating stage. The two flights were four hours apart and focussed on the anvil region of Hector in altitudes between 10.5 km and 18.8 km (i.e. above 350 K potential temperature). Trajectory calculations and ozone measurements have been used to identify that the same cloud air masses have been probed in both flights. The size distributions derived from the measurements not only show a change with increasing altitude but also with the evolution of Hector. Clearly different aerosol to cloud particle ratios as well as varying ice crystal morphology have been found for the different development stages of Hector, indicating a change in freezing mechanisms. The development phase exhibits the smallest ice particles (up to 300 μm) with a rather uniform morphology. This is indicative for rapid glaciation during Hector's development. Sizes of ice crystals are largest in the mature stage (larger 1.6 mm) and even exceed those of some continental tropical deep convective clouds, also in their number concentrations. The backscatter properties and particle images show a change from frozen droplets in the developing phase to rimed and aggregated particles. The clouds in the dissipating stage have a large vertical extend (roughly 6 km) though optically thin and persist for at least 6 h. This poses a high potential for affecting the tropical tropopause layer background conditions regarding humidity, e.g. through facilitating subvisible cirrus formation, and with this the amount of water vapour that is transported into the stratosphere.
Publisher: Copernicus GmbH
Date: 05-07-2018
Abstract: Abstract. Secondary organic aerosol (SOA) particles have been found to be efficient ice-nucleating particles under the cold conditions of (tropical) upper-tropospheric cirrus clouds. Whether they also are efficient at initiating freezing under slightly warmer conditions as found in mixed-phase clouds remains undetermined. Here, we study the ice-nucleating ability of photochemically produced SOA particles with the combination of the Manchester Aerosol Chamber and Manchester Ice Cloud Chamber. Three SOA systems were tested resembling biogenic and anthropogenic particles as well as particles of different phase state. These are namely α-pinene, heptadecane, and 1,3,5-trimethylbenzene. After the aerosol particles were formed, they were transferred into the cloud chamber, where subsequent quasi-adiabatic cloud activation experiments were performed. Additionally, the ice-forming abilities of ammonium sulfate and kaolinite were investigated as a reference to test the experimental setup. Clouds were formed in the temperature range of −20 to −28.6 ∘C. Only the reference experiment using dust particles showed evidence of ice nucleation. No ice particles were observed in any other experiment. Thus, we conclude that SOA particles produced under the conditions of the reported experiments are not efficient ice-nucleating particles starting at liquid saturation under mixed-phase cloud conditions.
Publisher: Copernicus GmbH
Date: 06-03-2014
DOI: 10.5194/ACPD-14-5893-2014
Abstract: Abstract. Vertical redistribution of HNO3 through condensation, sedimentation and evaporation of large HNO3-containing particles inside polar stratospheric clouds (PSCs) plays an important role in the chemistry of the Arctic winter stratosphere. In situ observations by the particle probe FSSP-100 during the RECONCILE c aign indicate unexpected large potential NAT (nitric acid trihydrate) particles inside PSCs. The observations can hardly be explained assuming particles with compact morphology and spherical shape due to limited growing time at temperatures below the existence temperature of NAT (TNAT). Utilizing simulations by the CLaMS and measurements by the airborne Fourier transform infrared spectrometer MIPAS-STR we study the impact of reduced settling velocities of NAT particles on vertical HNO3 redistribution. Reduced settling velocities are expected for spherical NAT particles with low mass density or aspheric NAT particles that might explain the maximum sizes of the particles observed in situ. The results of our study support the hypothesis that denitrification is produced by significantly aspheric (i.e. columnar) compact NAT particles which are characterised by reduced settling velocities.
Publisher: Copernicus GmbH
Date: 31-03-2016
DOI: 10.5194/ACP-2016-183
Abstract: Abstract. Aerosols of the volcanic degassing plumes from Mt. Etna and Mt. Stromboli were probed with in situ instruments on board the Deutsches Zentrum für Luft- und Raumfahrt research aircraft Falcon during the contrail, volcano, and cirrus experiment CONCERT in September 2011. Aerosol properties were analyzed using angular scattering intensities and particle size distributions simultaneously measured with the Polar Nephelometer and the Forward Scattering Spectrometer probes (FSSP series 100 and 300), respectively. Aerosols of degassing plumes are characterized by low values of the asymmetry parameter (between 0.6 and 0.75) the effective diameter was within the range of 1.5–2.8 µm and the maximal diameter was lower than 20 µm. A principal component analysis applied to the Polar Nephelometer data indicates that scattering features of volcanic aerosols of different crater origins are clearly distinctive from angular scattering intensities of cirrus and contrails. Retrievals of aerosol properties revealed that the particles were "optically spherical" and the estimated values of the real part of the refractive index are within the interval from 1.35 to 1.38. The interpretation of these results leads to the conclusion that the degassing-plumes aerosols were porous with air voids. Our estimates suggest that aerosol particles contained about 18 to 35 % of air voids in terms of the total volume.
Publisher: Copernicus GmbH
Date: 17-03-2011
Abstract: Abstract. An FSSP-100 Optical Particle Counter designed to count and size particles in the micron range and a backscattersonde that measures in-situ particle optical properties such as backscatter and depolarization ratio, are part of the payload of the high altitude research aircraft M55 Geophysica. This aircraft was deployed in tropical field c aigns in Bauru, Brasil (TROCCINOX, 2004) Darwin, Australia (SCOUT-Darwin, 2005) and Ouagadougou, Burkina Faso (SCOUT-AMMA, 2006). In those occasions, measurements of particle size distributions and optical properties within cirrus cloud were performed. Scope of the present work is to assess and discuss the consistency between the particle volume backscatter coefficient observed by the backscattersonde and the same parameter retrieved by optical scattering theory applied to particle size distributions as measured by the FSSP-100. In addition, empirical relationships linking the optical properties measured in-situ by the backscattersonde, which generally can be obtained by remote sensing techniques (LIDAR), and microphysical bulk properties like total particle number, surface and volume density will be presented and discussed.
Publisher: Copernicus GmbH
Date: 29-01-2014
Abstract: Abstract. Nitric acid trihydrate (NAT) particles in the polar stratosphere have been shown to be responsible for vertical redistribution of reactive nitrogen (NOy). Recent observations by Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP) aboard the CALIPSO satellite have been explained in terms of heterogeneous nucleation of NAT on foreign nuclei, revealing this to be an important formation pathway for the NAT particles. In state of the art global- or regional-scale models, heterogeneous NAT nucleation is currently simulated in a very coarse manner using a constant, saturation-independent nucleation rate. Here we present first simulations for the Arctic winter 2009/2010 applying a new saturation-dependent parametrisation of heterogeneous NAT nucleation rates within the Chemical Lagrangian Model of the Stratosphere (CLaMS). The simulation shows good agreement of chemical trace species with in situ and remote sensing observations. The simulated polar stratospheric cloud (PSC) optical properties agree much better with CALIOP observations than those simulated with a constant nucleation rate model. A comparison of the simulated particle size distributions with observations made using the Forward Scattering Spectrometer Probe (FSSP) aboard the high altitude research aircraft Geophysica, shows that the model reproduces the observed size distribution, except for the very largest particles above 15 μm diameter. The vertical NOy redistribution caused by the sedimentation of the NAT particles, in particular the denitrification and nitrification signals observed by the ACE-FTS satellite instrument and the in situ SIOUX instrument aboard the Geophysica, are reproduced by the improved model, and a small improvement with respect to the constant nucleation rate model is found.
Location: United Kingdom of Great Britain and Northern Ireland
Start Date: 2019
End Date: 2021
Funder: European Commission
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