Civil Aircraft For Regular Investigation Research Articles

An optical particle size spectrometer for aircraft-borne measurements in IAGOS-CARIBIC

Abstract. The particle number size distribution is an important parameter to characterize the atmospheric aerosol and its influence on the Earth's climate. Here we describe a new optical particle size spectrometer (OPSS) for measurements of the accumulation mode particle number size distribution in the tropopause region on board a passenger aircraft (IAGOS-CARIBIC observatory: In-service Aircraft for a Global Observing System – Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container). A modified KS93 particle sensor from RION Co., Ltd., together with a new airflow system and a dedicated data acquisition system, is the key component of the CARIBIC OPSS. The instrument records individual particle pulse signal curves in the particle size range 130–1110 nm diameter (for a particle refractive index of 1.47-i0.006) together with a time stamp and thus allows the post-flight choice of the time resolution and the size distribution bin width. The CARIBIC OPSS has a 50 % particle detection diameter of 152 nm and a maximum asymptotic counting efficiency of 98 %. The instrument's measurement performance shows no pressure dependency and no particle coincidence for free tropospheric conditions. The size response function of the CARIBIC OPSS was obtained by a polystyrene latex calibration in combination with model calculations. Particle number size distributions measured with the new OPSS in the lowermost stratosphere agreed within a factor of 2 in concentration with balloon-borne measurements over western North America. Since June 2010 the CARIBIC OPSS is deployed once per month in the IAGOS-CARIBIC observatory.

Influence of volcanic eruptions on midlatitude upper tropospheric aerosol and consequences for cirrus clouds

AbstractThe influence of downwelling stratospheric sulfurous aerosol on the UT (upper troposphere) aerosol concentrations and on cirrus clouds is investigated using CARIBIC (Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container observations) (between 1999–2002 and 2005–2013) and the cirrus reflectance product from Moderate Resolution Imaging Spectroradiometer (MODIS). The initial period, 1999–2002, was volcanically quiescent after which the sulfurous aerosol in the LMS (lowermost stratosphere) (SLMS) became enhanced by several volcanic eruptions starting 2005. From 2005 to 2008 and in 2013, volcanic aerosol from several tropical eruptions increased SLMS. Due to consequent subsidence, the sulfur loading of the upper troposphere (SUT) was increased by a factor of 2.5 compared to background levels. Comparison of SLMS and SUT during the seasons March–July and August–November shows a close coupling of the UT and LMS. Finally, the relationship between SLMS and the cirrus cloud reflectance (CR) retrieved from MODIS spectrometer (on board the satellites Terra and Aqua) is studied. SLMS and CR show a strong anticorrelation, with a factor of 3.5 increase in SLMS and decrease of CR by 8 ± 2% over the period 2001–2011. We propose that the increase of SLMS due to volcanism has caused the coinciding cirrus CR decrease, which would be associated with a negative radiative forcing in the Northern Hemisphere midlatitudes.

Mercury Plumes in the Global Upper Troposphere Observed during Flights with the CARIBIC Observatory from May 2005 until June 2013

Tropospheric sections of flights with the CARIBIC (Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrumented Container) observatory from May 2005 until June 2013, are investigated for the occurrence of plumes with elevated Hg concentrations. Additional information on CO, CO2, CH4, NOy, O3, hydrocarbons, halocarbons, acetone and acetonitrile enable us to attribute the plumes to biomass burning, urban/industrial sources or a mixture of both. Altogether, 98 pollution plumes with elevated Hg concentrations and CO mixing ratios were encountered, and the Hg/CO emission ratios for 49 of them could be calculated. Most of the plumes were found over East Asia, in the African equatorial region, over South America and over Pakistan and India. The plumes encountered over equatorial Africa and over South America originate predominantly from biomass burning, as evidenced by the low Hg/CO emission ratios and elevated mixing ratios of acetonitrile, CH3Cl and particle concentrations. The backward trajectories point to the regions around the Rift Valley and the Amazon Basin, with its outskirts, as the source areas. The plumes encountered over East Asia and over Pakistan and India are predominantly of urban/industrial origin, sometimes mixed with products of biomass/biofuel burning. Backward trajectories point mostly to source areas in China and northern India. The Hg/CO2 and Hg/CH4 emission ratios for several plumes are also presented and discussed.

Methyl chloride in the upper troposphere observed by the CARIBIC passenger aircraft observatory: Large‐scale distributions and Asian summer monsoon outflow

AbstractWe present spatial and temporal variations of methyl chloride (CH3Cl) in the upper troposphere (UT) observed mainly by the Civil Aircraft for Regular Investigation of the atmosphere Based on an Instrument Container (CARIBIC) passenger aircraft for the years 2005–2011. The CH3Cl mixing ratio in the UT over Europe was higher than that observed at a European surface baseline station throughout the year, indicative of a persistent positive vertical gradient at Northern Hemisphere midlatitudes. A series of flights over Africa and South Asia show that CH3Cl mixing ratios increase toward tropical latitudes, and the observed UT CH3Cl level over these two regions and the Atlantic was higher than that measured at remote surface sites. Strong emissions of CH3Cl in the tropics combined with meridional air transport through the UT may explain such vertical and latitudinal gradients. Comparisons with carbon monoxide (CO) data indicate that noncombustion sources in the tropics dominantly contribute to forming the latitudinal gradient of CH3Cl in the UT. We also observed elevated mixing ratios of CH3Cl and CO in air influenced by biomass burning in South America and Africa, and the enhancement ratios derived for CH3Cl to CO in those regions agree with previous observations. In contrast, correlations indicate a high CH3Cl to CO ratio of 2.9 ± 0.5 ppt ppb−1 in the Asian summer monsoon anticyclone and domestic biofuel emissions in South Asia are inferred to be responsible. We estimated the CH3Cl emission in South Asia to be 134 ± 23 Gg Cl yr−1, which is higher than a previous estimate due to the higher CH3Cl to CO ratio observed in this study.

Observations of the 2008 Kasatochi volcanic SO<sub>2</sub> plume by CARIBIC aircraft DOAS and the GOME-2 satellite

Abstract. The 2008 Kasatochi volcanic eruption emitted ≈1.5–2.5 Tg SO2 into the upper troposphere and lower stratosphere. Parts of the main volcanic plume (gases and particles) reached central Europe a week after the eruption and were detected there by the CARIBIC (Civil Aircraft for Regular investigation of the Atmosphere based on an Instrument Container) flying observatory. The plume was also observed by the GOME-2 satellite instrument, only a few hours after the CARIBIC aircraft had crossed the plume, thus giving a unique opportunity to compare results. Trajectories and local wind speeds are investigated in detail using the GOME-2 and CARIBIC observations for better comparison of the results from these two observational systems. A comparison of the satellite spatial pattern with the local observations of the wind speed and the trajectory model TRAJKS showed a slight discrepancy, which has to be considered for satellite validation. Hence, it appears that detailed analyses of wind speeds are required. Emitted and secondary particles, partly measured and sampled by the CARIBIC in situ instruments, affected the DOAS SO2 measurements, of both CARIBIC and GOME-2. Overall GOME-2 and the CARIBIC SO2 measurements agree very well. The major uncertainties remain the actual wind speed needed to properly correct for the advection of the plume between the different overpass times and effects of aerosols on DOAS retrievals. The good agreement can be seen as validation for both GOME-2 and CARIBIC DOAS observations.

Origin of aerosol particles in the mid-latitude and subtropical upper troposphere and lowermost stratosphere from cluster analysis of CARIBIC data

Abstract. The origin of aerosol particles in the upper troposphere and lowermost stratosphere over the Eurasian continent was investigated by applying cluster analysis methods to in situ measured data. Number concentrations of submicrometer aerosol particles and trace gas mixing ratios derived by the CARIBIC (Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container) measurement system on flights between Germany and South-East Asia were used for this analysis. Four cluster analysis methods were applied to a test data set and their capability of separating the data points into scientifically reasonable clusters was assessed. The best method was applied to seasonal data subsets for summer and winter resulting in five cluster or air mass types: stratosphere, tropopause, free troposphere, high clouds, and boundary layer influenced. Other source clusters, like aircraft emissions could not be resolved in the present data set with the used methods. While the cluster separation works satisfactory well for the summer data, in winter interpretation is more difficult, which is attributed to either different vertical transport pathways or different chemical lifetimes in both seasons. The geographical distribution of the clusters together with histograms for nucleation and Aitken mode particles within each cluster are presented. Aitken mode particle number concentrations show a clear vertical gradient with the lowest values in the lowermost stratosphere (750–2820 particles/cm3 STP, minimum of the two 25% – and maximum of the two 75%-percentiles of both seasons) and the highest values for the boundary-layer-influenced air (4290–22 760 particles/cm3 STP). Nucleation mode particles are also highest in the boundary-layer-influenced air (1260–29 500 particles/cm3 STP), but are lowest in the free troposphere (0–450 particles/cm3 STP). The given submicrometer particle number concentrations represent the first large-scale seasonal data sets for the upper troposphere and lowermost stratosphere over the Eurasian continent.

Gaseous mercury distribution in the upper troposphere and lower stratosphere observed onboard the CARIBIC passenger aircraft

Abstract. Total gaseous mercury (TGM) was measured onboard a passenger aircraft during monthly CARIBIC flights (Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrumented Container) made between May 2005 and March 2007 on the routes Frankfurt–São Paulo–Santiago de Chile and back and Frankfurt–Guangzhou–Manila and back. The data provide for the first time an insight into the seasonal distributions of TGM in the upper troposphere and lower stratosphere (UT/LS) of both hemispheres and demonstrate the importance of mercury emissions from biomass burning in the Southern Hemisphere. Numerous plumes were observed in the upper troposphere, the larger of which could be characterized in terms of Hg/CO emission ratios and their probable origins. During the flights to China TGM correlated with CO in the upper troposphere with a seasonally dependent slope reflecting the longer lifetime of elemental mercury when compared to that of CO. A pronounced depletion of TGM was always observed in the extratropical lowermost stratosphere. TGM concentrations there were found to decrease with the increasing concentrations of particles. Combined with the large concentrations of particle bond mercury in the stratosphere observed by others, this finding suggests either a direct conversion of TGM to particle bound mercury or an indirect conversion via a semivolatile bivalent mercury compound. Based on concurrent measurements of SF6 during two flights, the rate of this conversion is estimated to 0.4 ng m−3 yr−1. A zero TGM concentration was not observed during some 200 flight hours in the lowermost stratosphere suggesting an equilibrium between the gaseous and particulate mercury.

Chemical composition and morphology of individual aerosol particles from a CARIBIC flight at 10 km altitude between 50°N and 30°S

Analysis of individual particles by analytical electron microscopy as well as quantitative analysis using particle‐induced X‐ray emission (PIXE) and particle elastic scattering analysis (PESA) were carried out on samples collected from a flight at 10 km altitude between 50°N and 30°S as part of the Civil Aircraft for Regular Investigation of the atmosphere Based on an Instrument Container (CARIBIC) project (http://www.caribic-atmospheric.com). Particle morphology showed large variability with sampling latitude. Complicated branched structures dominated the large particles of the extratropical northern and southern hemisphere and the northern tropics. Particles in the tropics of the southern hemisphere were small in size and large in number concentration, whereas particles in or close to the intertropical convergence zone were few and small in size. Particles in the lowermost stratosphere were found to have similar structures but more branched than the ones found in the upper troposphere of the extratropics. Quantitative analysis revealed that the sulfur concentration varied by a factor of 50 in the nine samples analyzed in this study. The carbon‐to‐sulfur mass concentration ratio was lowest in the lowermost stratosphere (0.5) and highest in the tropics of the southern hemisphere (3.5). The elemental distribution of carbon and sulfur in individual particles was mapped by energy‐filtered transmission electron microscopy (EFTEM). Almost all particles analyzed contained a mixture of carbonaceous and sulfurous matter. Particles with satellites were found by EFTEM to contain both carbon and sulfur in the central particle, whereas in the satellite particles only carbonaceous material was detected.

Submicrometer aerosol particle distributions in the upper troposphere over the mid-latitude North Atlantic—results from the third route of ‘CARIBIC’

Particle number and mass concentrations of submicrometer aerosol particles were determined for the upper troposphere over the mid-latitude North Atlantic within the Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container project (CARIBIC, http://www.caribic-atmospheric.com). Between May 2001 and April 2002, 22 flights from Germany to the Caribbean were conducted using an automated measurement container on a B767 passenger aircraft. Spatial and seasonal probability distributions for ultrafine and Aitken mode particles as well as mass concentrations of particulate sulphur in 8–12 km altitude are presented. High particle number concentrations (mostly 2500–15 000 particles cm-3 STP) are particularly found in summer over the western North Atlantic Ocean close to the North American continent. The distributions together with an analysis of particle source processes show that deep vertical transport is the dominant process leading to most of the events with high particle number concentrations (8000 particles cm-3 STP) for ultrafine particles as well as for Aitken mode particles. This study emphasizes the importance of deep vertical transport and cloud processing for the concentration of aerosol particles in the upper troposphere.

Civil Aircraft for the regular investigation of the atmosphere based on an instrumented container: The new CARIBIC system

Abstract. An airfreight container with automated instruments for measurement of atmospheric gases and trace compounds was operated on a monthly basis onboard a Boeing 767-300 ER of LTU International Airways during long-distance flights from 1997 to 2002 (CARIBIC, Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container, http://www.caribic-atmospheric.com). Subsequently a more advanced system has been developed, using a larger capacity container with additional equipment and an improved inlet system. CARIBIC phase #2 was implemented on a new long-range aircraft type Airbus A340-600 of the Lufthansa German Airlines (Star Alliance) in December 2004, creating a powerful flying observatory. The instrument package comprises detectors for the measurement of O3, total and gaseous H2O, NO and NOy, CO, CO2, O2, Hg, and number concentrations of sub-micrometer particles (>4 nm, >12 nm, and >18 nm diameter). Furthermore, an optical particle counter (OPC) and a proton transfer mass spectrometer (PTR-MS) are incorporated. Aerosol samples are collected for analysis of elemental composition and particle morphology after flight. Air samples are taken in glass containers for laboratory analyses of hydrocarbons, halocarbons and greenhouse gases (including isotopic composition of CO2) in several laboratories. Absorption tubes collect oxygenated volatile organic compounds. Three differential optical absorption spectrometers (DOAS) with their telescopes mounted in the inlet system measure atmospheric trace gases such as BrO, HONO, and NO2. A video camera mounted in the inlet provides information about clouds along the flight track. The flying observatory, its equipment and examples of measurement results are reported.

Design and Calibration of a Multi-Channel Aerosol Sampler for Tropopause Region Studies from the CARIBIC Platform

An aircraft-based, multi-channel aerosol sampler for studies of the upper troposphere and lowermost stratosphere from the CARIBIC (Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container) platform was designed and calibrated. The sampler operates with an impaction technique at a flow rate of 10.4 lpm and consists of sixteen sampling channels. Samples are collected in a time sequence. Each channel contains two sample types that are used for quantitative measurement of concentrations, using particle-induced X-ray emission (PIXE), and single particle analysis with electron microscopy. The minimum detection limits for PIXE analysis after 1.5 h sampling are, for example, 2.0, 0.14, and 0.02 ng/m3 STP (standard temperature and pressure) for sulfur, potassium, and nickel. Calibration included penetration studies of a cyclone arrangement used to define the upper size limit in the sampling to 2.0 μ m diameter and the collection efficiency of the impactor. Both components of the sampling system showed penetration and collection efficiency close to 100%, respectively, in the particle size range of interest. The impactor cut-off was found to be dependent on the ratio of the impactor upstream-to-downstream pressure for ratios well below the critical pressure drop (i.e., the pressure where the jet reaches sonic velocity) being 0.15 μ m and 0.08 μ m for ratios 0.41 and 0.2.

Characteristics and origin of lowermost stratospheric aerosol at northern midlatitudes under volcanically quiescent conditions based on CARIBIC observations

Characteristics and origin of the aerosol in the lowermost stratosphere at northern midlatitudes were studied using measurements from a passenger aircraft (Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container, or CARIBIC). Aerosol samples were collected during 60 intercontinental flights during 1999–2002 and analyzed for elemental composition with particle‐induced X‐ray emission (PIXE). Concurrent measurements of trace gases were used to interpret the aerosol measurements. It was found that particulate sulfur concentration increased steadily in the potential vorticity (PV) region of 2–7 PVU, whereas particulate potassium and iron showed no such dependence. The variability in concentration of the latter two elements was mainly connected with season, similar to their variation in the upper troposphere, whereas PV dominated the particulate sulfur variability. An ozone‐based model was developed to quantitatively determine the mixing of stratospheric and tropospheric air masses. A significant dependence on PV was found, and the stratospheric fraction of the air peaked during spring. It was found that the particulate sulfur concentration was strongly dependent on the origin of the air masses. The concentration increased by a factor of 3 over the lowermost stratosphere. A discontinuity in the concentration over the tropopause indicated particle formation from sulfur dioxide transported across the tropopause. The concentration at the top of the lowermost stratosphere was used to estimate that the particulate sulfur production in the stratosphere is 0.066 Tg S/yr with approximately half of the amount transported across the top of the lowermost stratosphere originating in carbonyl sulfide.

Meridional distributions of aerosol particle number concentrations in the upper troposphere and lower stratosphere obtained by Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container (CARIBIC) flights

Number concentrations of submicrometer aerosol particles at altitudes of 8.5–11.3 km were measured along a single flight route between Germany (∼50°N, ∼10°E) and the Indic (∼5°N, ∼80°E) over 3 years using a commercial aircraft platform (project Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container (CARIBIC)). During 41 intercontinental flights (∼380 flight hours), more than one million individual particle concentration measurements were made, yielding a comprehensive and unique aerosol data set. Using these data, the first meridional and seasonal probability distributions for ultrafine particles and for Aitken mode plus accumulation mode particles in the upper troposphere (UT) and lower stratosphere (LS) were derived. High particle number concentrations were observed in summer at tropical latitudes over the Arabian Sea and at midlatitudes over Europe, in contrast to lower values in the subtropics over the Middle East. This distribution primarily reflects the vertical transport pattern of the atmosphere. In winter, number concentrations were generally lower. The Intertropical Convergence Zone (ITCZ) was identified as a region of pronounced particle formation, but particle nucleation also occurred in the upper troposphere at midlatitudes. At tropical latitudes, convective transport and photochemistry appear to be the main driving forces for particle formation in the free troposphere. Consistent with these observations, integral length scales calculated from the aerosol data ranged from 6 to 12 km. Compared to particle concentrations in the midlatitudinal upper troposphere, those in the lowermost stratosphere were lower in winter, but equal or higher in summer. This seasonality is likely caused by stronger in‐mixing of upper tropospheric air in summer.

Two Automated Ozone Analyzers for Use on Civil Aircraft Operating in the Tropopause Region

Abstract Within the CARIBIC (Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container) project, deployment of an automated container with analytical equipment for the observation of atmospheric trace gases and aerosols in the tropopause region allows a systematic collection of relevant data at comparatively low costs. Two ozone analyzers for simultaneous operation in the CARIBIC container during long-distance flights were developed for high-altitude measurements. Typical cruising altitudes during long-distance flights of about 10 000 km are in the range of 10–12 km. The design and characteristics of the two instruments, a fast-response ozone sensor, OSCAR (Ozone Sensor CARIBIC), based on a dry chemiluminescence technique; and a modified UV absorption ozone analyzer, OMCAL (Ozone Monitor Calibrator), are described. While OSCAR with a time resolution of 10 Hz can measure changes in ozone concentration at cruising altitudes on a horizontal scale of about 30 m, OMCAL with a ...

Aerosol elemental concentrations in the tropopause region from intercontinental flights with the Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container (CARIBIC) platform

This study with the Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container (CARIBIC) platform investigates the aerosol elemental concentrations at 9–11 km altitude in the northern hemisphere. Measurements from 31 intercontinental flights over a 2‐year period between Germany and Sri Lanka/Maldives in the Indian Ocean are presented. Aerosol samples were collected with an impaction technique and were analyzed for the concentration of 18 elements using particle‐induced X‐ray emission (PIXE). Additional measurements of particle number concentrations, ozone and carbon monoxide concentrations, and meteorological modeling were included in the interpretation of the aerosol elemental concentrations. Particulate sulphur was found to be by far the most abundant element. Its upper tropospheric concentration increased, on average, by a factor of 2 from the tropics to midlatitudes, with another factor 2 higher concentrations in the lowermost stratosphere over midlatitudes. Correlation patterns and source profiles suggest contributions from crustal sources and biomass burning, but not from meteor ablation. Coinciding latitudinal gradients in particulate sulphur concentrations and emissions suggest that fossil fuel combustion is an important source of the aerosol in the upper troposphere and lowermost stratosphere. The measurements indicate aerosol transport along isentropic surfaces across the tropopause into the lowermost stratosphere. As a result of the prolonged residence time, ageing via oxidation of sulphur dioxide in the lowermost stratosphere was found to be a likely high‐altitude, strong source that, along with downward transport of stratospheric air, could explain the vertical gradient of particulate sulphur mass concentration around the extratropical tropopause.

Budgets of O3 and CO in the upper troposphere: CARIBIC passenger aircraft results 1997–2001

In situ measurements of ozone (O3) and carbon monoxide (CO) were conducted using a passenger aircraft during 47 flights (November 1997 to April 2001) between Germany and the Indian Ocean region at 10–11 km altitude, project Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container (CARIBIC). Here, emphasis is on a better understanding of the budgets of O3 and CO in the middle and upper northern hemispheric (NH) troposphere. Latitudinal and seasonal variations of the mean values and the local variability of O3 and CO are assessed. CO is moreover applied as tracer of polluted (surface) air, that is, as a measure of O3 precursors. This enables us to assign positive or negative O3–CO correlations and their slopes α = dO3/dCO to O3 produced by photochemistry or to O3 imported from the stratosphere. In the tropics, photochemical O3 production clearly dominates all year round, with mean O3–CO slopes of 0.45–0.53 in spring/summer and 0.20–0.27 in autumn/winter. Over the Arabian Sea and the Middle East, high annual net O3 production rates in the troposphere of 17.6 × 1010 O3 molecules cm−2 s−1 are estimated. In the extratropics, the well‐documented springtime O3 maximum emerged in the CARIBIC data set. Stratospheric O3 influx and photochemical O3 production contribute equally to this spring maximum. In summer, photochemical O3 formation clearly dominates, in winter, per contra, stratospheric O3 influx clearly dominates. In the extratropics, CO shows a sine seasonal variation between ∼81 ppbv in September and ∼111 ppbv in March, being delayed by ∼5 weeks compared to ground‐based background monitoring stations. In the tropics, however, no significant seasonal variations of CO were observed, mainly because of occasional high CO periods such as those associated with the 1997 Indonesian forest fires or the outflow of the Intertropical Convergence Zone, which pumps in summer immense amounts of pollutants emitted in South Asia (India, Bangladesh, Indochina) to the 10–11 km altitude range surveyed during CARIBIC.