Search Results
Aircraft-based observations of isoprene-epoxydiol-derived secondary organic aerosol (IEPOX-SOA) in the tropical upper troposphere over the Amazon region
2018, Schulz, Christiane, Schneider, Johannes, Amorim Holanda, Bruna, Appel, Oliver, Costa, Anja, de Sá, Suzane S., Dreiling, Volker, Fütterer, Daniel, Jurkat-Witschas, Tina, Klimach, Thomas, Knote, Christoph, Krämer, Martina, Martin, Scot T., Mertes, Stephan, Pöhlker, Mira L., Sauer, Daniel, Voigt, Christiane, Walser, Adrian, Weinzierl, Bernadett, Ziereis, Helmut, Zöger, Martin, Andreae, Meinrat O., Artaxo, Paulo, Machado, Luiz A. T., Pöschl, Ulrich, Wendisch, Manfred, Borrmann, Stephan
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.
Coupling aerosols to (cirrus) clouds in the global EMAC-MADE3 aerosol–climate model
2020, Righi, Mattia, Hendricks, Johannes, Lohmann, Ulrike, Beer, Christof Gerhard, Hahn, Valerian, Heinold, Bernd, Heller, Romy, Krämer, Martina, Ponater, Michael, Rolf, Christian, Tegen, Ina, Voigt, Christiane
A new cloud microphysical scheme including a detailed parameterization for aerosol-driven ice formation in cirrus clouds is implemented in the global ECHAM/MESSy Atmospheric Chemistry (EMAC) chemistry–climate model and coupled to the third generation of the Modal Aerosol Dynamics model for Europe adapted for global applications (MADE3) aerosol submodel. The new scheme is able to consistently simulate three regimes of stratiform clouds – liquid, mixed-, and ice-phase (cirrus) clouds – considering the activation of aerosol particles to form cloud droplets and the nucleation of ice crystals. In the cirrus regime, it allows for the competition between homogeneous and heterogeneous freezing for the available supersaturated water vapor, taking into account different types of ice-nucleating particles, whose specific ice-nucleating properties can be flexibly varied in the model setup. The new model configuration is tuned to find the optimal set of parameters that minimizes the model deviations with respect to observations. A detailed evaluation is also performed comparing the model results for standard cloud and radiation variables with a comprehensive set of observations from satellite retrievals and in situ measurements. The performance of EMAC-MADE3 in this new coupled configuration is in line with similar global coupled models and with other global aerosol models featuring ice cloud parameterizations. Some remaining discrepancies, namely a high positive bias in liquid water path in the Northern Hemisphere and overestimated (underestimated) cloud droplet number concentrations over the tropical oceans (in the extratropical regions), which are both a common problem in these kinds of models, need to be taken into account in future applications of the model. To further demonstrate the readiness of the new model system for application studies, an estimate of the anthropogenic aerosol effective radiative forcing (ERF) is provided, showing that EMAC-MADE3 simulates a relatively strong aerosol-induced cooling but within the range reported in the Intergovernmental Panel on Climate Change (IPCC) assessments.
Classification of Arctic, midlatitude and tropical clouds in the mixed-phase temperature regime
2017, Costa, Anja, Meyer, Jessica, Afchine, Armin, Luebke, Anna, Günther, Gebhard, Dorsey, James R., Gallagher, Martin W., Ehrlich, Andre, Wendisch, Manfred, Baumgardner, Darrel, Wex, Heike, Krämer, Martina
The degree of glaciation of mixed-phase clouds constitutes one of the largest uncertainties in climate prediction. In order to better understand cloud glaciation, cloud spectrometer observations are presented in this paper, which were made in the mixed-phase temperature regime between 0 and -38°C (273 to 235K), where cloud particles can either be frozen or liquid. The extensive data set covers four airborne field campaigns providing a total of 139000 1Hz data points (38.6h within clouds) over Arctic, midlatitude and tropical regions. We develop algorithms, combining the information on number concentration, size and asphericity of the observed cloud particles to classify four cloud types: liquid clouds, clouds in which liquid droplets and ice crystals coexist, fully glaciated clouds after the Wegener-Bergeron-Findeisen process and clouds where secondary ice formation occurred. We quantify the occurrence of these cloud groups depending on the geographical region and temperature and find that liquid clouds dominate our measurements during the Arctic spring, while clouds dominated by the Wegener-Bergeron-Findeisen process are most common in midlatitude spring. The coexistence of liquid water and ice crystals is found over the whole mixed-phase temperature range in tropical convective towers in the dry season. Secondary ice is found at midlatitudes at -5 to -10°C (268 to 263K) and at higher altitudes, i.e. lower temperatures in the tropics. The distribution of the cloud types with decreasing temperature is shown to be consistent with the theory of evolution of mixed-phase clouds. With this study, we aim to contribute to a large statistical database on cloud types in the mixed-phase temperature regime.
Climatological and radiative properties of midlatitude cirrus clouds derived by automatic evaluation of lidar measurements
2016, Kienast-Sjögren, Erika, Rolf, Christian, Seifert, Patric, Krieger, Ulrich K., Luo, Bei P., Krämer, Martina, Peter, Thomas
Cirrus, i.e., high, thin clouds that are fully glaciated, play an important role in the Earth's radiation budget as they interact with both long- and shortwave radiation and affect the water vapor budget of the upper troposphere and stratosphere. Here, we present a climatology of midlatitude cirrus clouds measured with the same type of ground-based lidar at three midlatitude research stations: at the Swiss high alpine Jungfraujoch station (3580 m a.s.l.), in Zürich (Switzerland, 510 m a.s.l.), and in Jülich (Germany, 100 m a.s.l.). The analysis is based on 13 000 h of measurements from 2010 to 2014. To automatically evaluate this extensive data set, we have developed the Fast LIdar Cirrus Algorithm (FLICA), which combines a pixel-based cloud-detection scheme with the classic lidar evaluation techniques. We find mean cirrus optical depths of 0.12 on Jungfraujoch and of 0.14 and 0.17 in Zürich and Jülich, respectively. Above Jungfraujoch, subvisible cirrus clouds (τ < 0.03) have been observed during 6 % of the observation time, whereas above Zürich and Jülich fewer clouds of that type were observed. Cirrus have been observed up to altitudes of 14.4 km a.s.l. above Jungfraujoch, whereas they have only been observed to about 1 km lower at the other stations. These features highlight the advantage of the high-altitude station Jungfraujoch, which is often in the free troposphere above the polluted boundary layer, thus enabling lidar measurements of thinner and higher clouds. In addition, the measurements suggest a change in cloud morphology at Jungfraujoch above ∼ 13 km, possibly because high particle number densities form in the observed cirrus clouds, when many ice crystals nucleate in the high supersaturations following rapid uplifts in lee waves above mountainous terrain. The retrieved optical properties are used as input for a radiative transfer model to estimate the net cloud radiative forcing, CRFNET, for the analyzed cirrus clouds. All cirrus detected here have a positive CRFNET. This confirms that these thin, high cirrus have a warming effect on the Earth's climate, whereas cooling clouds typically have cloud edges too low in altitude to satisfy the FLICA criterion of temperatures below −38 °C. We find CRFNET = 0.9 W m−2 for Jungfraujoch and 1.0 W m−2 (1.7 W m−2) for Zürich (Jülich). Further, we calculate that subvisible cirrus (τ < 0.03) contribute about 5 %, thin cirrus (0.03 < τ < 0.3) about 45 %, and opaque cirrus (0.3 < τ) about 50 % of the total cirrus radiative forcing.
Aerosol characteristics and particle production in the upper troposphere over the Amazon Basin
2018, Andreae, Meinrat O., Afchine, Armin, Albrecht, Rachel, Holanda, Bruna Amorim, Artaxo, Paulo, Barbosa, Henrique M. J., Borrmann, Stephan, Cecchini, Micael A., Costa, Anja, Dollner, Maximilian, Fütterer, Daniel, Järvinen, Emma, Jurkat, Tina, Klimach, Thomas, Konemann, Tobias, Knote, Christoph, Krämer, Martina, Krisna, Trismono, Machado, Luiz A. T., Mertes, Stephan, Minikin, Andreas, Pöhlker, Christopher, Pöhlker, Mira L., Pöschl, Ulrich, Rosenfeld, Daniel, Sauer, Daniel, Schlager, Hans, Schnaiter, Martin, Schneider, Johannes, Schulz, Christiane, Spanu, Antonio, Sperling, Vinicius B., Voigt, Christiane, Walser, Adrian, Wang, Jian, Weinzierl, Bernadett, Wendisch, Manfred, Ziereis, Helmut
Airborne observations over the Amazon Basin showed high aerosol particle concentrations in the upper troposphere (UT) between 8 and 15ĝ€km altitude, with number densities (normalized to standard temperature and pressure) often exceeding those in the planetary boundary layer (PBL) by 1 or 2 orders of magnitude. The measurements were made during the German–Brazilian cooperative aircraft campaign ACRIDICON–CHUVA, where ACRIDICON stands for Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems
and CHUVA is the acronym for Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (global precipitation measurement)
, on the German High Altitude and Long Range Research Aircraft (HALO). The campaign took place in September–October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with atmospheric trace gases, aerosol particles, and atmospheric radiation.
Aerosol enhancements were observed consistently on all flights during which the UT was probed, using several aerosol metrics, including condensation nuclei (CN) and cloud condensation nuclei (CCN) number concentrations and chemical species mass concentrations. The UT particles differed sharply in their chemical composition and size distribution from those in the PBL, ruling out convective transport of combustion-derived particles from the boundary layer (BL) as a source. The air in the immediate outflow of deep convective clouds was depleted of aerosol particles, whereas strongly enhanced number concentrations of small particles (< 90ĝ€nm diameter) were found in UT regions that had experienced outflow from deep convection in the preceding 5–72ĝ€h. We also found elevated concentrations of larger (> 90ĝ€nm) particles in the UT, which consisted mostly of organic matter and nitrate and were very effective CCN.
Our findings suggest a conceptual model, where production of new aerosol particles takes place in the continental UT from biogenic volatile organic material brought up by deep convection and converted to condensable species in the UT. Subsequently, downward mixing and transport of upper tropospheric aerosol can be a source of particles to the PBL, where they increase in size by the condensation of biogenic volatile organic compound (BVOC) oxidation products. This may be an important source of aerosol particles for the Amazonian PBL, where aerosol nucleation and new particle formation have not been observed. We propose that this may have been the dominant process supplying secondary aerosol particles in the pristine atmosphere, making clouds the dominant control of both removal and production of atmospheric particles.