0000000001311335
AUTHOR
Sergej Molleker
Chemical analysis of refractory stratospheric aerosol particles collected within the arctic vortex and inside polar stratospheric clouds
Abstract. Stratospheric aerosol particles with diameters larger than about 10 nm were collected within the arctic vortex during two polar flight campaigns: RECONCILE in winter 2010 and ESSenCe in winter 2011. Impactors were installed on board the aircraft M-55 Geophysica, which was operated from Kiruna, Sweden. Flights were performed at a height of up to 21 km and some of the particle samples were taken within distinct polar stratospheric clouds (PSCs). The chemical composition, size and morphology of refractory particles were analyzed by scanning electron microscopy and energy-dispersive X-ray microanalysis. During ESSenCe no refractory particles with diameters above 500 nm were sampled. I…
The ACRIDICON-CHUVA campaign: Studying tropical deep convective clouds and precipitation over Amazonia using the new German research aircraft HALO
Abstract Between 1 September and 4 October 2014, a combined airborne and ground-based measurement campaign was conducted to study tropical deep convective clouds over the Brazilian Amazon rain forest. The new German research aircraft, High Altitude and Long Range Research Aircraft (HALO), a modified Gulfstream G550, and extensive ground-based instrumentation were deployed in and near Manaus (State of Amazonas). The campaign was part of the German–Brazilian Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems–Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (Global Precipitatio…
The realization of autonomous, aircraft-based, real-time aerosol mass spectrometry in the upper troposphere and lower stratosphere
Abstract. We report on the developments that enabled the field deployment of a fully-automated aerosol mass spectrometer, specially designed for high-altitude measurements on unpressurised aircraft. The merits of the two main categories of real-time aerosol mass spectrometry, i.e. (a) single particle laser desorption and ionization, and (b) continuous thermal desorption / electron impact ionization of aerosols, have been integrated into one compact apparatus with the aim to perform in-situ real-time analysis of aerosol chemical composition. The demonstrated instrument, named ERICA (European Research council Instrument for the Chemical composition of Aerosols), operated successfully aboard t…
Nitric acid trihydrate nucleation and denitrification in the Arctic stratosphere
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 n…
Application of an O-ring pinch device as a constant-pressure inlet (CPI) for airborne sampling
We present a novel and compact design of a constant-pressure inlet (CPI) developed for use in airborne aerosol mass spectrometry. In particular, the inlet system is optimized for aerodynamic lenses commonly used in aerosol mass spectrometers, in which efficient focusing of aerosol particles into a vacuum chamber requires a precisely controlled lens pressure, typically of a few hectopascals. The CPI device can also be used in condensation particle counters (CPCs), cloud condensation nucleus counters (CCNCs), and gas-phase sampling instruments across a wide range of altitudes and inlet pressures. The constant pressure is achieved by changing the inner diameter of a properly scaled O-ring that…
Aerosol concentrations determine the height of warm rain and ice initiation in convective clouds over the Amazon basin
Abstract. We have investigated how pollution aerosols affect the height above cloud base of rain and ice hydrometeor initiation and the subsequent vertical evolution of cloud droplet size and number concentrations in growing convective cumulus. For this purpose we used in-situ data of hydrometeor size distributions measured with instruments mounted on HALO (High Altitude and Long Range Research Aircraft) during the ACRIDICON-CHUVA campaign over the Amazon during September 2014. The results show that the height of rain initiation by collision and coalescence processes (Dr, in units of meters above cloud base) is linearly correlated with the number concentration of droplets (Nd in cm−3) nucle…
ML-CIRRUS: The Airborne Experiment on Natural Cirrus and Contrail Cirrus with the High-Altitude Long-Range Research Aircraft HALO
Abstract The Midlatitude Cirrus experiment (ML-CIRRUS) deployed the High Altitude and Long Range Research Aircraft (HALO) to obtain new insights into nucleation, life cycle, and climate impact of natural cirrus and aircraft-induced contrail cirrus. Direct observations of cirrus properties and their variability are still incomplete, currently limiting our understanding of the clouds’ impact on climate. Also, dynamical effects on clouds and feedbacks are not adequately represented in today’s weather prediction models. Here, we present the rationale, objectives, and selected scientific highlights of ML-CIRRUS using the G-550 aircraft of the German atmospheric science community. The first combi…
Comparing calculated microphysical properties of tropical convective clouds at cloud base with measurements during the ACRIDICON-CHUVA campaign
Abstract. Reliable aircraft measurements of cloud microphysical properties are essential for understanding liquid convective cloud formation. In September 2014, the properties of convective clouds were measured with a Cloud Combination Probe (CCP), a Cloud and Aerosol Spectrometer (CAS-DPOL), and a cloud condensation nuclei (CCN) counter on board the HALO (High Altitude and Long Range Research Aircraft) aircraft during the ACRIDICON-CHUVA campaign over the Amazon region. An intercomparison of the cloud drop size distributions (DSDs) and the cloud water content derived from the different instruments generally shows good agreement within the instrumental uncertainties. The objective of this s…
Sensitivities of Amazonian clouds to aerosols and updraft speed
Abstract. The effects of aerosol particles and updraft speed on warm-phase cloud microphysical properties are studied in the Amazon region as part of the ACRIDICON-CHUVA experiment. Here we expand the sensitivity analysis usually found in the literature by concomitantly considering cloud evolution, putting the sensitivity quantifications into perspective in relation to in-cloud processing, and by considering the effects on droplet size distribution (DSD) shape. Our in situ aircraft measurements over the Amazon Basin cover a wide range of particle concentration and thermodynamic conditions, from the pristine regions over coastal and forested areas to the southern Amazon, which is highly poll…
Comparing parameterized versus measured microphysical properties of tropical convective cloud bases during the ACRIDICON–CHUVA campaign
The objective of this study is to validate parameterizations that were recently developed for satellite retrievals of cloud condensation nuclei supersaturation spectra, NCCN(S), at cloud base alongside more traditional parameterizations connecting NCCN(S) with cloud base updrafts and drop concentrations. This was based on the HALO aircraft measurements during the ACRIDICON–CHUVA campaign over the Amazon region, which took place in September 2014. The properties of convective clouds were measured with a cloud combination probe (CCP), a cloud and aerosol spectrometer (CAS-DPOL), and a CCN counter onboard the HALO aircraft. An intercomparison of the cloud drop size distributions (DSDs) and the…
Aircraft-based observation of meteoric material in lower-stratospheric aerosol particles between 15 and 68° N
We analyse aerosol particle composition measurements from five research missions between 2014 and 2018 to assess the meridional extent of particles containing meteoric material in the upper troposphere and lower stratosphere (UTLS). Measurements from the Jungfraujoch mountaintop site and a low-altitude aircraft mission show that meteoric material is also present within middle- and lower-tropospheric aerosol but within only a very small proportion of particles. For both the UTLS campaigns and the lower- and mid-troposphere observations, the measurements were conducted with single-particle laser ablation mass spectrometers with bipolar-ion detection, which enabled us to measure the chemical c…
Chemical analysis of the Asian tropopause aerosol layer (ATAL) with emphasis on secondary aerosol particles using aircraft-based in situ aerosol mass spectrometry
Abstract. Aircraft-borne in situ measurements of the chemical aerosol composition were conducted in the Asian tropopause aerosol layer (ATAL) over the Indian subcontinent in the summer of 2017, covering particle sizes below ∼3 µm. We have implemented a recently developed aerosol mass spectrometer, which adopts the laser desorption technique as well as the thermal desorption method for quantitative bulk information (i.e., a modified Aerodyne AMS), aboard the high-altitude research aircraft M-55 Geophysica. The instrument was deployed in July and August 2017 during the StratoClim EU campaign (Stratospheric and upper tropospheric processes for better Climate predictions) over Nepal, India, Ban…
The challenge of simulating the sensitivity of the Amazonian clouds microstructure to cloud condensation nuclei number concentrations
The realistic representation of cloud-aerosol interactions is of primary importance for accurate climate model projections. The investigation of these interactions in strongly contrasting clean and polluted atmospheric conditions in the Amazon area has been one of the motivations for several field observations, including the airborne Aerosol, Cloud, Precipitation, and Radiation Interactions and DynamIcs of CONvective cloud systems – Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (Global Precipitation Measurement) (ACRIDICON-CHUVA) campaign based in Manaus, Brazil in September 2014. In this work we combine in situ …
Arctic low-level boundary layer clouds: in situ measurements and simulations of mono- and bimodal supercooled droplet size distributions at the top layer of liquid phase clouds
Abstract. Aircraft borne optical in situ size distribution measurements were performed within Arctic boundary layer clouds with a special emphasis on the cloud top layer during the VERtical Distribution of Ice in Arctic clouds (VERDI) campaign in April and May 2012. An instrumented Basler BT-67 research aircraft operated out of Inuvik over the Mackenzie River delta and the Beaufort Sea in the Northwest Territories of Canada. Besides the cloud particle and hydrometeor size spectrometers the aircraft was equipped with instrumentation for aerosol, radiation and other parameters. Inside the cloud, droplet size distributions with monomodal shapes were observed for predominantly liquid-phase Arct…
Chemical analysis of the Asian Tropopause Aerosol Layer (ATAL) with emphasis on secondary aerosol particles using aircraft based in situ aerosol mass spectrometry
Abstract. Aircraft borne in-situ measurements of the chemical aerosol composition were conducted in the Asian Tropopause Aerosol layer (ATAL) over the Indian subcontinent in summer 2017 covering particle sizes below 3 µm. We have implemented a recently developed aerosol mass spectrometer, which adopts the laser desorption technique as well as the thermal desorption method for quantitative bulk information (i.e. a modified Aerodyne AMS), aboard the high altitude research aircraft M-55 Geophysica. The instrument was deployed in July and August 2017 during the StratoClim EU campaign (Stratospheric and upper tropospheric processes for better climate predictions) over Nepal, India, Bangladesh, a…
Application of an O-ring pinch device as a constant pressure inlet (CPI) for airborne sampling
Abstract. We present a novel and compact design of a constant pressure inlet (CPI) developed for use in airborne aerosol mass spectrometry. In particular the inlet system is optimized for aerodynamic lenses commonly used in aerosol mass spectrometers, where efficient focusing of aerosol particles into a vacuum chamber requires a precisely controlled lens pressure, typically of a few hPa. The CPI device can also be used in gas phase sampling instruments in a large range of altitude and inlet pressure. The constant pressure is achieved by changing the inner diameter of a properly scaled O-ring that acts as a critical orifice. The CPI control keeps air pressure and thereby mass flow rate (≈ 0.…
Aircraft-based observation of meteoric material in lower stratospheric aerosol particles between 15 and 68° N
Abstract. In this paper we analyze aerosol particle composition measurements from five research missions conducted between 2014 and 2018 sampling the upper troposphere and lower stratosphere (UTLS), to assess the meridional extent of particles containing meteoric material. Additional data sets from a ground based study and from a low altitude aircraft mission are used to confirm the existence of meteoric material in lower tropospheric particles. Single particle laser ablation techniques with bipolar ion detection were used to measure the chemical composition of particles in a size range of approximately 150 nm to 3 μm. The five UTLS aircraft missions cover a latitude range from 15 to 68° N,…
Further evidence for CCN aerosol concentrations determining the height of warm rain and ice initiation in convective clouds over the Amazon basin
We have investigated how aerosols affect the height above cloud base of rain and ice hydrometeor initiation and the subsequent vertical evolution of cloud droplet size and number concentrations in growing convective cumulus. For this purpose we used in situ data of hydrometeor size distributions measured with instruments mounted on HALO aircraft during the ACRIDICON–CHUVA campaign over the Amazon during September 2014. The results show that the height of rain initiation by collision and coalescence processes (Dr, in units of meters above cloud base) is linearly correlated with the number concentration of droplets (Nd in cm−3) nucleated at cloud base (Dr ≈ 5 ⋅ Nd). Additional cloud processes…
Design, characterization, and first field deployment of a novel aircraft-based aerosol mass spectrometer combining the laser ablation and flash vaporization techniques
In this paper, we present the design, development, and characteristics of the novel aerosol mass spectrometer ERICA (ERC Instrument for Chemical composition of Aerosols; ERC – European Research Council) and selected results from the first airborne field deployment. The instrument combines two well-established methods of real-time in situ measurements of fine particle chemical composition. The first method is the laser desorption and ionization technique, or laser ablation technique, for single-particle mass spectrometry (here with a frequency-quadrupled Nd:YAG laser at λ = 266 nm). The second method is a combination of thermal particle desorption, also called flash vaporization, and electro…
The realization of autonomous, aircraft-based, real-time aerosol mass spectrometry in the upper troposphere and lower stratosphere (dataset)
Dataset accompanying the journal article titled "The realization of autonomous, aircraft-based, real-time aerosol mass spectrometry in the upper troposphere and lower stratosphere". Preprint: doi.org/10.5194/egusphere-2022-33
Chemical analysis of the Asian tropopause aerosol layer (ATAL) with emphasis on secondary aerosol particles using aircraft-based in situ aerosol mass spectrometry
Aircraft-borne in situ measurements of the chemical aerosol composition were conducted in the Asian tropopause aerosol layer (ATAL) over the Indian subcontinent in the summer of 2017, covering particle sizes below ∼3 µm. We have implemented a recently developed aerosol mass spectrometer, which adopts the laser desorption technique as well as the thermal desorption method for quantitative bulk information (i.e., a modified Aerodyne AMS), aboard the high-altitude research aircraft M-55 Geophysica. The instrument was deployed in July and August 2017 during the StratoClim EU campaign (Stratospheric and upper tropospheric processes for better Climate predictions) over Nepal, India, Bangladesh, a…
Application of an O-ring pinch device as a constant-pressure inlet (CPI) for airborne sampling
We present a novel and compact design of a constant-pressure inlet (CPI) developed for use in airborne aerosol mass spectrometry. In particular, the inlet system is optimized for aerodynamic lenses commonly used in aerosol mass spectrometers, in which efficient focusing of aerosol particles into a vacuum chamber requires a precisely controlled lens pressure, typically of a few hectopascals. The CPI device can also be used in condensation particle counters (CPCs), cloud condensation nucleus counters (CCNCs), and gas-phase sampling instruments across a wide range of altitudes and inlet pressures. The constant pressure is achieved by changing the inner diameter of a properly scaled O-ring that…
Chemical analysis of the Asian Tropopause Aerosol Layer (ATAL) with emphasis on secondary aerosol particles using aircraft based in situ aerosol mass spectrometry
Aircraft borne in-situ measurements of the chemical aerosol composition were conducted in the Asian Tropopause Aerosol layer (ATAL) over the Indian subcontinent in summer 2017 covering particle sizes below 3 µm. We have implemented a recently developed aerosol mass spectrometer, which adopts the laser desorption technique as well as the thermal desorption method for quantitative bulk information (i.e. a modified Aerodyne AMS), aboard the high altitude research aircraft M-55 Geophysica. The instrument was deployed in July and August 2017 during the StratoClim EU campaign (Stratospheric and upper tropospheric processes for better climate predictions) over Nepal, India, Bangladesh, and t…
The realization of autonomous, aircraft-based, real-time aerosol mass spectrometry in the upper troposphere and lower stratosphere
We report on the developments that enabled the field deployment of a fully automated aerosol mass spectrometer, especially designed for high-altitude measurements on unpressurized aircraft. The merits of the two main categories of real-time aerosol mass spectrometry, i.e. (a) single-particle laser desorption and ionization and (b) continuous thermal desorption and electron impact ionization of aerosols, have been integrated into one compact apparatus with the aim to perform in situ real-time analysis of aerosol chemical composition. The demonstrated instrument, named the ERICA (European Research Council Instrument for Chemical composition of Aerosols), operated successfully aboard the high-…
Application of an O-ring pinch device as a constant pressure inlet (CPI) for airborne sampling
We present a novel and compact design of a constant pressure inlet (CPI) developed for use in airborne aerosol mass spectrometry. In particular the inlet system is optimized for aerodynamic lenses commonly used in aerosol mass spectrometers, where efficient focusing of aerosol particles into a vacuum chamber requires a precisely controlled lens pressure, typically of a few hPa. The CPI device can also be used in gas phase sampling instruments in a large range of altitude and inlet pressure. The constant pressure is achieved by changing the inner diameter of a properly scaled O-ring that acts as a critical orifice. The CPI control keeps air pressure and thereby mass flow rate (≈&thinsp…
Aircraft-based observation of meteoric material in lower stratospheric aerosol particles between 15 and 68° N
In this paper we analyze aerosol particle composition measurements from five research missions conducted between 2014 and 2018 sampling the upper troposphere and lower stratosphere (UTLS), to assess the meridional extent of particles containing meteoric material. Additional data sets from a ground based study and from a low altitude aircraft mission are used to confirm the existence of meteoric material in lower tropospheric particles. Single particle laser ablation techniques with bipolar ion detection were used to measure the chemical composition of particles in a size range of approximately 150 nm to 3 μm. The five UTLS aircraft missions cover a latitude range from 15 to 68…