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Wildfire smoke, Arctic haze, and aerosol effects on mixed-phase and cirrus clouds over the North Pole region during MOSAiC: an introduction
2021, Engelmann, Ronny, Ansmann, Albert, Ohneiser, Kevin, Griesche, Hannes, Radenz, Martin, Hofer, Julian, Althausen, Dietrich, Dahlke, Sandro, Maturilli, Marion, Veselovskii, Igor, Jimenez, Cristofer, Wiesen, Robert, Baars, Holger, Bühl, Johannes, Gebauer, Henriette, Haarig, Moritz, Seifert, Patric, Wandinger, Ulla, Macke, Andreas
An advanced multiwavelength polarization Raman lidar was operated aboard the icebreaker Polarstern during the MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition to continuously monitor aerosol and cloud layers in the central Arctic up to 30gkm height. The expedition lasted from September 2019 to October 2020 and measurements were mostly taken between 85 and 88.5ggN. The lidar was integrated into a complex remote-sensing infrastructure aboard the Polarstern. In this article, novel lidar techniques, innovative concepts to study aerosol-cloud interaction in the Arctic, and unique MOSAiC findings will be presented. The highlight of the lidar measurements was the detection of a 10gkm deep wildfire smoke layer over the North Pole region between 7-8gkm and 17-18gkm height with an aerosol optical thickness (AOT) at 532gnm of around 0.1 (in October-November 2019) and 0.05 from December to March. The dual-wavelength Raman lidar technique allowed us to unambiguously identify smoke as the dominating aerosol type in the aerosol layer in the upper troposphere and lower stratosphere (UTLS). An additional contribution to the 532gnm AOT by volcanic sulfate aerosol (Raikoke eruption) was estimated to always be lower than 15g%. The optical and microphysical properties of the UTLS smoke layer are presented in an accompanying paper . This smoke event offered the unique opportunity to study the influence of organic aerosol particles (serving as ice-nucleating particles, INPs) on cirrus formation in the upper troposphere. An example of a closure study is presented to explain our concept of investigating aerosol-cloud interaction in this field. The smoke particles were obviously able to control the evolution of the cirrus system and caused low ice crystal number concentration. After the discussion of two typical Arctic haze events, we present a case study of the evolution of a long-lasting mixed-phase cloud layer embedded in Arctic haze in the free troposphere. The recently introduced dual-field-of-view polarization lidar technique was applied, for the first time, to mixed-phase cloud observations in order to determine the microphysical properties of the water droplets. The mixed-phase cloud closure experiment (based on combined lidar and radar observations) indicated that the observed aerosol levels controlled the number concentrations of nucleated droplets and ice crystals.
Sun photometer retrievals of Saharan dust properties over Barbados during SALTRACE
2019, Toledano, Carlos, Torres, BenjamÃn, Velasco-Merino, Cristian, Althausen, Dietrich, Groß, Silke, Wiegner, Matthias, Weinzierl, Bernadett, Gasteiger, Josef, Ansmann, Albert, González, Ramiro, Mateos, David, Farrel, David, Müller, Thomas, Haarig, Moritz, Cachorro, Victoria E.
The Saharan Aerosol Long-Range Transport and Aerosol-Cloud-Interaction Experiment (SALTRACE) was devoted to the investigation of Saharan dust properties over the Caribbean. The campaign took place in June-July 2013. A wide set of ground-based and airborne aerosol instrumentation was deployed at the island of Barbados for a comprehensive experiment. Several sun photometers performed measurements during this campaign: two AERONET (Aerosol Robotic Network) Cimel sun photometers and the Sun and Sky Automatic Radiometer (SSARA). The sun photometers were co-located with the ground-based multi-wavelength lidars BERTHA (Backscatter Extinction lidar Ratio Temperature Humidity profiling Apparatus) and POLIS (Portable Lidar System). Aerosol properties derived from direct sun and sky radiance observations are analyzed, and a comparison with the co-located lidar and in situ data is provided. The time series of aerosol optical depth (AOD) allows identifying successive dust events with short periods in between in which the marine background conditions were observed. The moderate aerosol optical depth in the range of 0.3 to 0.6 was found during the dust periods. The sun photometer infrared channel at the 1640nm wavelength was used in the retrieval to investigate possible improvements to aerosol size retrievals, and it was expected to have a larger sensitivity to coarse particles. The comparison between column (aerosol optical depth) and surface (dust concentration) data demonstrates the connection between the Saharan Air Layer and the boundary layer in the Caribbean region, as is shown by the synchronized detection of the successive dust events in both datasets. However the differences of size distributions derived from sun photometer data and in situ observations reveal the difficulties in carrying out a column closure study. © 2019 All rights reserved.
The unprecedented 2017–2018 stratospheric smoke event: decay phase and aerosol properties observed with the EARLINET
2019, Baars, Holger, Ansmann, Albert, Ohneiser, Kevin, Haarig, Moritz, Engelmann, Ronny, Althausen, Dietrich, Hanssen, Ingrid, Gausa, Michael, Pietruczuk, Aleksander, Szkop, Artur, Stachlewska, Iwona S., Wang, Dongxiang, Reichardt, Jens, Skupin, Annett, Mattis, Ina, Trickl, Thomas, Vogelmann, Hannes, Navas-Guzmán, Francisco, Haefele, Alexander, Acheson, Karen, Ruth, Albert A., Tatarov, Boyan, Müller, Detlef, Hu, Qiaoyun, Podvin, Thierry, Goloub, Philippe, Veselovskii, Igor, Pietras, Christophe, Haeffelin, Martial, Fréville, Patrick, Sicard, Michaël, Comerón, Adolfo, GarcÃa, Alfonso Javier Fernández, Molero Menéndez, Francisco, Córdoba-Jabonero, Carmen, Guerrero-Rascado, Juan Luis, Alados-Arboledas, Lucas, Bortoli, Daniele, Costa, Maria João, Dionisi, Davide, Liberti, Gian Luigi, Wang, Xuan, Sannino, Alessia, Papagiannopoulos, Nikolaos, Boselli, Antonella, Mona, Lucia, D’Amico, Guiseppe, Romano, Salvatore, Perrone, Maria Rita, Belegante, Livio, Nicolae, Doina, Grigorov, Ivan, Gialitaki, Anna, Amiridis, Vassilis, Soupiona, Ourania, Papayannis, Alexandros, Mamouri, Rodanthi-Elisaveth, Nisantzi, Argyro, Heese, Birgit, Hofer, Julian, Schechner, Yoav Y., Wandinger, Ulla, Pappalardo, Gelsomina
Six months of stratospheric aerosol observations with the European Aerosol Research Lidar Network (EARLINET) from August 2017 to January 2018 are presented. The decay phase of an unprecedented, record-breaking stratospheric perturbation caused by wildfire smoke is reported and discussed in terms of geometrical, optical, and microphysical aerosol properties. Enormous amounts of smoke were injected into the upper troposphere and lower stratosphere over fire areas in western Canada on 12 August 2017 during strong thunderstorm–pyrocumulonimbus activity. The stratospheric fire plumes spread over the entire Northern Hemisphere in the following weeks and months. Twenty-eight European lidar stations from northern Norway to southern Portugal and the eastern Mediterranean monitored the strong stratospheric perturbation on a continental scale. The main smoke layer (over central, western, southern, and eastern Europe) was found at heights between 15 and 20 km since September 2017 (about 2 weeks after entering the stratosphere). Thin layers of smoke were detected at heights of up to 22–23 km. The stratospheric aerosol optical thickness at 532 nm decreased from values > 0.25 on 21–23 August 2017 to 0.005–0.03 until 5–10 September and was mainly 0.003–0.004 from October to December 2017 and thus was still significantly above the stratospheric background (0.001–0.002). Stratospheric particle extinction coefficients (532 nm) were as high as 50–200 Mm−1 until the beginning of September and on the order of 1 Mm−1 (0.5–5 Mm−1) from October 2017 until the end of January 2018. The corresponding layer mean particle mass concentration was on the order of 0.05–0.5 µg m−3 over these months. Soot particles (light-absorbing carbonaceous particles) are efficient ice-nucleating particles (INPs) at upper tropospheric (cirrus) temperatures and available to influence cirrus formation when entering the tropopause from above. We estimated INP concentrations of 50–500 L−1 until the first days in September and afterwards 5–50 L−1 until the end of the year 2017 in the lower stratosphere for typical cirrus formation temperatures of −55 ∘C and an ice supersaturation level of 1.15. The measured profiles of the particle linear depolarization ratio indicated a predominance of nonspherical smoke particles. The 532 nm depolarization ratio decreased slowly with time in the main smoke layer from values of 0.15–0.25 (August–September) to values of 0.05–0.10 (October–November) and < 0.05 (December–January). The decrease of the depolarization ratio is consistent with aging of the smoke particles, growing of a coating around the solid black carbon core (aggregates), and thus change of the shape towards a spherical form. We found ascending aerosol layer features over the most southern European stations, especially over the eastern Mediterranean at 32–35∘ N, that ascended from heights of about 18–19 to 22–23 km from the beginning of October to the beginning of December 2017 (about 2 km per month). We discuss several transport and lifting mechanisms that may have had an impact on the found aerosol layering structures.
First triple-wavelength lidar observations of depolarization and extinction-to-backscatter ratios of Saharan dus
2022, Haarig, Moritz, Ansmann, Albert, Engelmann, Ronny, Baars, Holger, Toledano, Carlos, Torres, Benjamin, Althausen, Dietrich, Radenz, Martin, Wandinger, Ulla
Two layers of Saharan dust observed over Leipzig, Germany, in February and March 2021 were used to provide the first-ever lidar measurements of the dust lidar ratio (extinction-to-backscatter ratio) and linear depolarization ratio at all three classical lidar wavelengths (355, 532 and 1064gnm). The pure-dust conditions during the first event exhibit lidar ratios of 47g±g8, 50g±g5 and 69g±g14gsr and particle linear depolarization ratios of 0.242g±g0.024, 0.299g±g0.018 and 0.206g±g0.010 at wavelengths of 355, 532 and 1064gnm, respectively. The second, slightly polluted-dust case shows a similar spectral behavior of the lidar and depolarization ratio with values of the lidar ratio of 49g±g4, 46g±g5 and 57g±g9gsr and the depolarization ratio of 0.174g±g0.041, 0.298g±g0.016 and 0.242g±g0.007 at 355, 532 and 1064gnm, respectively. The results were compared with Aerosol Robotic Network (AERONET) version 3 (v3) inversion solutions and the Generalized Retrieval of Aerosol and Surface Properties (GRASP) at six and seven wavelengths. Both retrieval schemes make use of a spheroid shape model for mineral dust. The spectral slope of the lidar ratio from 532 to 1064gnm could be well reproduced by the AERONET and GRASP retrieval schemes. Higher lidar ratios in the UV were retrieved by AERONET and GRASP. The enhancement was probably caused by the influence of fine-mode pollution particles in the boundary layer which are included in the columnar photometer measurements. Significant differences between the measured and retrieved wavelength dependence of the particle linear depolarization ratio were found. The potential sources for these uncertainties are discussed.
1064nm rotational Raman lidar for particle extinction and lidar-ratio profiling: Cirrus case study
2016, Haarig, Moritz, Engelmann, Ronny, Ansmann, Albert, Veselovskii, Igor, Whiteman, David N., Althausen, Dietrich
For the first time, vertical profiles of the 1064 nm particle extinction coefficient obtained from Raman lidar observations at 1058 nm (nitrogen and oxygen rotational Raman backscatter) are presented. We applied the new technique in the framework of test measurements and performed several cirrus observations of particle backscatter and extinction coefficients, and corresponding extinction-to-backscatter ratios at the wavelengths of 355, 532, and 1064 nm. The cirrus backscatter coefficients were found to be equal for all three wavelengths keeping the retrieval uncertainties in mind. The multiple-scattering-corrected cirrus extinction coefficients at 355 nm were on average about 20–30 % lower than the ones for 532 and 1064 nm. The cirrus-mean extinction-to-backscatter ratio (lidar ratio) was 31 ± 5 sr (355 nm), 36 ± 5 sr (532 nm), and 38 ± 5 sr (1064 nm) in this single study. We further discussed the requirements needed to obtain aerosol extinction profiles in the lower troposphere at 1064 nm with good accuracy (20 % relative uncertainty) and appropriate temporal and vertical resolution.
Profiles of cloud condensation nuclei, dust mass concentration, and ice-nucleating-particle-relevant aerosol properties in the Saharan Air Layer over Barbados from polarization lidar and airborne in situ measurements
2019, Haarig, Moritz, Walser, Adrian, Ansmann, Albert, Dollner, Maximilian, Althausen, Dietrich, Sauer, Daniel, Farrell, David, Weinzierl, Bernadett
The present study aims to evaluate lidar retrievals of cloud-relevant aerosol properties by using polarization lidar and coincident airborne in situ measurements in the Saharan Air Layer (SAL) over the Barbados region. Vertical profiles of the number concentration of cloud condensation nuclei (CCN), large particles (diameter d > 500 nm), surface area, mass, and ice-nucleating particle (INP) concentration are derived from the lidar measurements and compared with CCN concentrations and the INP-relevant aerosol properties measured in situ with aircraft. The measurements were performed in the framework of the Saharan Aerosol Longrange Transport and Aerosol-Cloud-Interaction Experiment (SALTRACE) in summer 2013. The CCN number concentrations derived from lidar observations were up to a factor of 2 higher than the ones measured in situ aboard the research aircraft Falcon. Possible reasons for the difference are discussed. The number concentration of particles with a dry radius of more than 250 nm and the surface-area concentration obtained from the lidar observations and used as input for the INP parameterizations agreed well (< 30 %-50 % deviation) with the aircraft measurements. In a pronounced lofted dust layer during summer (10 July 2013), the lidar retrieval yielded 100-300 CCN per cubic centimeter at 0.2 % water supersaturation and 10-200 INPs per liter at-25?C. Excellent agreement was also obtained in the comparison of mass concentration profiles. During the SALTRACE winter campaign (March 2014), the dust layer from Africa was mixed with smoke particles which dominated the CCN number concentration. This example highlights the unique lidar potential to separate smoke and dust contributions to the CCN reservoir and thus to identify the sensitive role of smoke in trade wind cumuli developments over the tropical Atlantic during the winter season. © 2017 Georg Thieme Verlag. All rights reserved.
Triple-wavelength depolarization-ratio profiling of Saharan dust over Barbados during SALTRACE in 2013 and 2014
2017, Haarig, Moritz, Ansmann, Albert, Althausen, Dietrich, Klepel, André, Groß, Silke, Freudenthaler, Volker, Toledano, Carlos, Mamouri, Rodanthi-Elisavet, Farrell, David A., Prescod, Damien A., Marinou, Eleni, Burton, Sharon P., Gasteiger, Josef, Engelmann, Ronny, Baars, Holger
Triple-wavelength polarization lidar measurements in Saharan dust layers were performed at Barbados (13.1°N, 59.6°W), 5000-8000km west of the Saharan dust sources, in the framework of the Saharan Aerosol Long-range Transport and Aerosol-Cloud-Interaction Experiment (SALTRACE-1, June-July 2013, SALTRACE-3, June-July 2014). Three case studies are discussed. High quality was achieved by comparing the dust linear depolarization ratio profiles measured at 355, 532, and 1064nm with respective dual-wavelength (355, 532nm) depolarization ratio profiles measured with a reference lidar. A unique case of long-range transported dust over more than 12000km is presented. Saharan dust plumes crossing Barbados were measured with an airborne triple-wavelength polarization lidar over Missouri in the midwestern United States 7 days later. Similar dust optical properties and depolarization features were observed over both sites indicating almost unchanged dust properties within this 1 week of travel from the Caribbean to the United States. The main results of the triple-wavelength polarization lidar observations in the Caribbean in the summer seasons of 2013 and 2014 are summarized. On average, the particle linear depolarization ratios for aged Saharan dust were found to be 0.252±0.030 at 355nm, 0.280±0.020 at 532nm, and 0.225±0.022 at 1064nm after approximately 1 week of transport over the tropical Atlantic. Based on published simulation studies we present an attempt to explain the spectral features of the depolarization ratio of irregularly shaped mineral dust particles, and conclude that most of the irregularly shaped coarse-mode dust particles (particles with diameters > 1μm) have sizes around 1.5-2μm. The SALTRACE results are also set into the context of the SAMUM-1 (Morocco, 2006) and SAMUM-2 (Cabo Verde, 2008) depolarization ratio studies. Again, only minor changes in the dust depolarization characteristics were observed on the way from the Saharan dust sources towards the Caribbean.
Dry versus wet marine particle optical properties: RH dependence of depolarization ratio, backscatter, and extinction from multiwavelength lidar measurements during SALTRACE
2017, Haarig, Moritz, Ansmann, Albert, Gasteiger, Josef, Kandler, Konrad, Althausen, Dietrich, Baars, Holger, Radenz, Martin, Farrell, David A.
Triple-wavelength lidar observations of the depolarization ratio and the backscatter coefficient of marine aerosol as a function of relative humidity (RH) are presented with a 5min time resolution. The measurements were performed at Barbados (13°N, 59°W) during the Saharan Aerosol Long-range Transport and Aerosol-Cloud interaction Experiment (SALTRACE) winter campaign in February 2014. The phase transition from spherical sea salt particles to cubic-like sea salt crystals was observed with a polarization lidar. The radiosonde and water-vapor Raman lidar observations show a drop in RH below 50% in the marine aerosol layer simultaneously with a strong increase in particle linear depolarization ratio, which reaches values up to 0.12±0.08 (at 355nm), 0.15±0.03 (at 532nm), and 0.10±0.01 (at 1064nm). The lidar ratio (extinction-to-backscatter ratio) increased from 19 and 23sr for spherical sea salt particles to 27 and 25sr (at 355 and 532nm, respectively) for cubic-like particle ensembles. Furthermore the scattering enhancement due to hygroscopic growth of the marine aerosol particles under atmospheric conditions was measured. Extinction enhancement factors from 40 to 80% RH of 1.94±0.94 at 355nm, 3.70±1.14 at 532nm, and 5.37±1.66 at 1064nm were found. The enhanced depolarization ratios and lidar ratios were compared to modeling studies of cubic sea salt particles.