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At least 19 records

Improvement of Raman lidar algorithm for quantifying aerosol extinction

Aerosols are particles of different composition and origin and influence the formation of clouds which are important in atmospheric radiative balance. At the present there is high uncertainty on the effect of aerosols on climate and this is mainly due to the fact that aerosol presence in the atmosphere can be highly variable in space and time. Monitoring of the aerosols in the atmosphere is necessary to better understanding many of these uncertainties. A lidar (an instrument that uses light to detect the extent of atmospheric aerosol loading) can be particularly useful to monitor aerosols in the atmosphere since it is capable to record the scattered intensity as a function of altitude from molecules and aerosols. One lidar method (the Raman lidar) makes use of the different wavelength changes that occur when light interacts with the varying chemistry and structure of atmospheric aerosols. One quantity that is indicative of aerosol presence is the aerosol extinction which quantifies the amount of attenuation (removal of photons), due to scattering, that light undergoes when propagating in the atmosphere. It can be directly measured with a Raman lidar using the wavelength dependence of the received signal. In order to calculate aerosol extinction from Raman scattering data it is necessary to evaluate the rate of change (derivative) of a Raman signal with respect to altitude. Since derivatives are defined for continuous functions, they cannot be performed directly on the experimental data which are not continuous. The most popular technique to find the functional behavior of experimental data is the least-square fit. This procedure allows finding a polynomial function which better approximate the experimental data. The typical approach in the lidar community is to make an a priori assumption about the functional behavior of the data in order to calculate the derivative. It has been shown in previous work that the use of the chi-square technique to determine the most likely functional behavior of the data prior to actually calculating the derivative eliminates the need for making a priori assumptions. We note that the a priori choice of a model itself can lead to larger uncertainties as compared to the method that is validated here. In this manuscript, the chi-square technique that determines the most likely functional behavior is validated through numerical simulation and by application to a large body of Raman lidar measurements. In general, we show that the chi-square approach to evaluate aerosol extinction yields lower extinction uncertainty than the traditional technique. We also use the technique to study the feasibility of developing a general characterization of the extinction uncertainty that could permit the uncertainty in Raman lidar aerosol extinction measurements to be estimated accurately without the use of the chi-square technique.

Russo, Felicita↗

In Situ Measurement of Aerosol Extinction

Aerosols are important contributors to the radiative forcing in the atmosphere. Much of the uncertainty in our knowledge of climate forcing is due to uncertainties in the radiative forcing due to aerosols as illustrated in the IPCC reports of the last ten years. Improved measurement of aerosol optical properties, therefore, is critical to an improved understanding of atmospheric radiative forcing. Additionally, attempts to reconcile in situ and remote measurements of aerosol radiative properties have generally not been successful. This is due in part to the fact that it has been impossible to measure aerosol extinction in situ in the past. In this presentation we introduce a new instrument that employs the techniques used in cavity ringdown spectroscopy to measure the aerosol extinction and scattering coefficients in situ. A prototype instrument has been designed and tested in the lab and the field. It is capable of measuring aerosol extinction coefficient to 2x10(exp -6) per meter. This prototype instrument is described and results are presented.

Strawa, Anthony W.↗

Spectral Aerosol Extinction (SpEx): A New Instrument for In situ Ambient Aerosol Extinction Measurements Across the UV/Visible Wavelength Range

We introduce a new instrument for the measurement of in situ ambient aerosol extinction over the 300-700 nm wavelength range, the Spectral Aerosol Extinction (SpEx) instrument. This measurement capability is envisioned to complement existing in situ instrumentation, allowing for simultaneous measurement of the evolution of aerosol optical, chemical, and physical characteristics in the ambient environment. In this work, a detailed description of the instrument is provided along with characterization tests performed in the laboratory. Measured spectra of NO2 and polystyrene latex spheres agreed well with theoretical calculations. Good agreement was also found with simultaneous aerosol extinction measurements at 450, 530, and 630 nm using CAPS PMex instruments in a series of 22 tests including non-absorbing compounds, dusts, soot, and black and brown carbon analogs. SpEx can more accurately distinguish the presence of brown carbon from other absorbing aerosol due to its 300 nm lower wavelength limit compared to measurements limited to visible wavelengths. In addition, the spectra obtained by SpEx carry more information than can be conveyed by a simple power law fit that is typically defined by the use of Angstrom Exponents. Future improvements aim at lowering detection limits and ruggedizing the instrument for mobile operation.

Jordan, C. E.↗

Using Airborne High Spectral Resolution Lidar Data to Evaluate Combined Active Plus Passive Retrievals of Aerosol Extinction Profiles

Aerosol extinction profiles are derived from backscatter data by constraining the retrieval with column aerosol optical thickness (AOT), for example from coincident MODIS observations and without reliance on a priori assumptions about aerosol type or optical properties. The backscatter data were acquired with the NASA Langley High Spectral Resolution Lidar (HSRL). The HSRL also simultaneously measures extinction independently, thereby providing an ideal data set for evaluating the constrained retrieval of extinction from backscatter. We will show constrained extinction retrievals using various sources of column AOT, and examine comparisons with the HSRL extinction measurements and with a similar retrieval using data from the CALIOP lidar on the CALIPSO satellite.

Burton, S. P.↗

Wavelength dependence of aerosol extinction coefficient for stratospheric aerosols

A simple empirical formula for the wavelength dependence of the aerosol extinction coefficient is proposed. The relationship between the constants in the formula and the variable parameter in the aerosol size distribution is explicitly expressed. Good agreement is found between the extinction coefficients calculated from the proposed formula and that calculated from Mie theory. The proposed expression is shown to be better than the Angstroem formula commonly used by atmospheric scientists.

Yue, Glenn K.↗

Using Airborne High Spectral Resolution Lidar Data to Evaluate Combined Active Plus Passive Retrievals of Aerosol Extinction Profiles

We derive aerosol extinction profiles from airborne and space-based lidar backscatter signals by constraining the retrieval with column aerosol optical thickness (AOT), with no need to rely on assumptions about aerosol type or lidar ratio. The backscatter data were acquired by the NASA Langley Research Center airborne High Spectral Resolution Lidar (HSRL) and by the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument on the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite. The HSRL also simultaneously measures aerosol extinction coefficients independently using the high spectral resolution lidar technique, thereby providing an ideal data set for evaluating the retrieval. We retrieve aerosol extinction profiles from both HSRL and CALIOP attenuated backscatter data constrained with HSRL, Moderate-Resolution Imaging Spectroradiometer (MODIS), and Multiangle Imaging Spectroradiometer column AOT. The resulting profiles are compared with the aerosol extinction measured by HSRL. Retrievals are limited to cases where the column aerosol thickness is greater than 0.2 over land and 0.15 over water. In the case of large AOT, the results using the Aqua MODIS constraint over water are poorer than Aqua MODIS over land or Terra MODIS. The poorer results relate to an apparent bias in Aqua MODIS AOT over water observed in August 2007. This apparent bias is still under investigation. Finally, aerosol extinction coefficients are derived from CALIPSO backscatter data using AOT from Aqua MODIS for 28 profiles over land and 9 over water. They agree with coincident measurements by the airborne HSRL to within +/-0.016/km +/- 20% for at least two-thirds of land points and within +/-0.028/km +/- 20% for at least two-thirds of ocean points.

Burton, S. P.↗

Improvement of Stratospheric Aerosol Extinction Retrieval from OMPS/LP Using a New Aerosol Model

The Ozone Mapping and Profiler Suite Limb Profiler (OMPS/LP) has been flying on the Suomi National Polar-orbiting Partnership (S-NPP) satellite since October 2011. It is designed to produce ozone and aerosol vertical profiles at 2-kilometer vertical resolution over the entire sunlit globe. Aerosol extinction profiles are computed with Mie theory using radiances measured at 675 nanometers. The operational Version 1.0 (V1.0) aerosol extinction retrieval algorithm assumes a bimodal lognormal aerosol size distribution (ASD) whose parameters were derived by combining an in situ measurement of aerosol microphysics with the Stratospheric Aerosol and Gas Experiment (SAGE II) aerosol extinction climatology. Internal analysis indicates that this bimodal lognormal ASD does not sufficiently explain the spectral dependence of LP-measured radiances. In this paper we describe the derivation of an improved aerosol size distribution, designated Version 1.5 (V1.5), for the LP retrieval algorithm. The new ASD uses a gamma function distribution that is derived from Community Aerosol and Radiation Model for Atmospheres (CARMA)-calculated results. A cumulative distribution fit derived from the gamma function ASD gives better agreement with CARMA results at small particle radii than bimodal or unimodal functions. The new ASD also explains the spectral dependence of LP-measured radiances better than the V1.0 ASD. We find that the impact of our choice of ASD on the retrieved extinctions varies strongly with the underlying reflectivity of the scene. Initial comparisons with collocated extinction profiles retrieved at 676 nanometers from the SAGE III instrument on the International Space Station (ISS) show a significant improvement in agreement for the LP V1.5 retrievals. Zonal mean extinction profiles agree to within 10 percent between 19 and 29 kilometers, and regression fits of collocated samples show improved correlation and reduced scatter compared to the V1.0 product. This improved agreement will motivate development of more sophisticated ASDs from CARMA results that incorporate latitude, altitude and seasonal variations in aerosol properties.

Ozone Mapping Profiler Suite Limb Profiler (OMPS/L↗

Airborne HSRL Assessment of CALIOP Aerosol Extinction Retrievals Constrained by Column AOD

Current operational CALIOP aerosol extinction profile retrievals usually rely on accurately specifying the relationship between aerosol extinction and backscattering (i.e. lidar ratio). Uncertainties in the assigned lidar ratios are typically the largest source of systematic error (~30-50%) in the CALIOP retrievals of aerosol extinction, backscatter, and aerosol optical depth. Alternatively, column aerosol optical depth (AOD) can be used to solve the lidar equation and obtain column-equivalent lidar ratios and retrieve aerosol extinction profiles from the CALIOP attenuated backscatter profiles. These derived lidar ratios correspond to the aerosols in the altitude range from 0-7 km. We derive column-equivalent aerosol lidar ratios and aerosol extinction profiles from CALIOP attenuated backscatter profiles constrained using co-located column AODs provided by several instruments/techniques: Synergized Optical Depth of Aerosols (SODA), Ocean-Derived Column Optical Depths (ODCOD), MODIS (dark target), MODIS (Multi-Angle Implementation of Atmospheric Correction-MAIAC), and PARASOL (Generalized Retrieval of Aerosol and Surface Properties-GRASP). These various retrievals of AOD and the column-average aerosol lidar ratios and aerosol extinction profiles derived from CALIOP using these AOD constraints are evaluated using the extensive record of coincident and co-located airborne HSRL measurements of AOD, aerosol lidar ratio, and aerosol extinction profiles acquired during more than 140 HSRL underflights of CALIPSO since 2006. The HSRL technique allows for the independent measurement of extinction and backscatter without the need for external constraints or assumptions regarding the lidar ratios. Initial comparisons with these coincident HSRL aerosol extinction profiles show that the CALIOP aerosol extinction profiles retrieved using these various AOD constraints are generally in better agreement with the HSRL measurements than aerosol extinction profiles from the operational techniques. The quality of agreement depends on the accuracy and magnitude of the AOD constraint. We present these comparisons of AOD, column aerosol lidar ratio, and aerosol extinction profiles for each of the AOD constraints described above.

lidar↗

Inter-Comparison of ILAS-II Version 1.4 Aerosol Extinction Coefficient at 780 nm with SAGE II, SAGE III, and POAM III Aerosol Data

The Improved Limb Atmospheric Spectrometer (ILAS) II on board the Advanced Earth Observing Satellite (ADEOS) II observed stratospheric aerosol in visible/near-infrared/infrared spectra over high latitudes in the Northern and Southern Hemispheres. Observations were taken intermittently from January to March, and continuously from April through October, 2003. We assessed the data quality of ILAS-II version 1.4 aerosol extinction coefficients at 780 nm from comparisons with the Stratospheric Aerosol and Gas Experiment (SAGE) II, SAGE III, and the Polar Ozone and Aerosol Measurement (POAM) III aerosol data. At heights below 20 km in the Northern Hemisphere, aerosol extinction coefficients from ILAS-II agreed with those from SAGE II and SAGE III within 10%, and with those from POAM III within 15%. From 20 to 26 km, ILAS-II aerosol extinction coefficients were smaller than extinction coefficients from the other sensors; differences between ILAS-II and SAGE II ranged from 10% at 20 km to 34% at 26 km. ILAS-II aerosol extinction coefficients from 20 to 25 km in February over the Southern Hemisphere had a negative bias (12-66%) relative to SAGE II aerosol data. The bias increased with increasing altitude. Comparisons between ILAS-II and POAM III aerosol extinction coefficients from January to May in the Southern Hemisphere (defined as the non-Polar Stratospheric Cloud (PSC) season ) yielded qualitatively similar results. From June to October (defined as the PSC season ), aerosol extinction coefficients from ILAS-II were smaller than those from POAM III above 17 km, as in the case of the non-PSC season; however, ILAS-II and POAM III aerosol data were within 15% of each other from 12 to 17 km.

Saitoh, Naoko↗

Vertical distribution of aerosol extinction cross section and inference of aerosol imaginary index in the troposphere by lidar technique

The paper reports on vertical profiles of aerosol extinction and backscatter in the troposphere which were obtained from multi zenith angle lidar measurements. It is reported that a direct slant path solution was found to be not possible due to horizontal inhomogeneity of the atmosphere. Attention is given to the use of a regression analysis with respect to zenith angle for a layer integration of the angle dependent lidar equation in order to determine the optical thickness and aerosol extinction-to-backscatter ratio for defined atmospheric layers and the subsequent evaluation of cross-section profiles.

Spinhirne, J. D.↗

Airborne Cavity Ring-Down Measurement of Aerosol Extinction and Scattering During the Aerosol IOP

Large uncertainties in the effects of aerosols on climate require improved in-situ measurements of extinction coefficient and single-scattering albedo. This paper describes preliminary results from Cadenza, a new continuous wave cavity ring-down (CW-CRD) instrument designed to address these uncertainties. Cadenza measures the aerosol extinction coefficient for 675 nm and 1550 nm light, and simultaneously measures the scattering coefficient at 675 nm. In the past year Cadenza was deployed in the Asian Dust Above Monterey (ADAM) and DOE Aerosol Intensive Operating Period (IOP) field projects. During these flights Cadenza produced measurements of aerosol extinction in the range from 0.2 to 300 Mm-1 with an estimated precision of 0.1 Min-1 for 1550 nm light and 0.2 Mm-1 for 675 nm light. Cadenza data from the ADAM and Aerosol IOP missions compared favorably with data from the other instruments aboard the CIRPAS Twin Otter aircraft and participating in those projects.= We present comparisons between the Cadenza measurements and those friom a TSI nephelometer, Particle Soot Absorption Photometer (PSAP), and the AATS 14 sun-photometer. Measurements of the optical properties of smoke and dust plumes sampled during these campaigns are presented and estimates of heating rates due to these plumes are made.

Strawa, A. W.↗

Aerosol extinction measurements with CO2-lidar

With the aim to develop a model for infrared extinction due to aerosols in slant paths in the lower atmosphere we perform measurements with a CO2-lidar. Earlier measurements with a transmissometer along horizontal paths have been used to develop relations between aerosol extinction and meteorological parameters. With the lidar measurements we hope to develop corresponding relations for altitude profiles of the aerosol extinction in the infrared. An important application is prediction of detection range for infrared imaging systems.

Hagard, Arne↗

Toward a Combined SAGE II-HALOE Aerosol Climatology: An Evaluation of HALOE Version 19 Stratospheric Aerosol Extinction Coefficient Observations

Herein, the Halogen Occultation Experiment (HALOE) aerosol extinction coefficient data is evaluated in the low aerosol loading period after 1996 as the first necessary step in a process that will eventually allow the production of a combined HALOE/SAGE II (Stratospheric Aerosol and Gas Experiment) aerosol climatology of derived aerosol products including surface area density. Based on these analyses, it is demonstrated that HALOE's 3.46 microns is of good quality above 19 km and suitable for scientific applications above that altitude. However, it is increasingly suspect at lower altitudes and should not be used below 17 km under any circumstances after 1996. The 3.40 microns is biased by about 10% throughout the lower stratosphere due to the failure to clear NO2 but otherwise appears to be a high quality product down to 15 km. The 2.45 and 5.26 micron aerosol extinction coefficient measurements are clearly biased and should not be used for scientific applications after the most intense parts of the Pinatubo period. Many of the issues in the aerosol data appear to be related to either the failure to clear some interfering gas species or doing so poorly. For instance, it is clear that the 3.40micronaerosol extinction coefficient measurements can be improved through the inclusion of an NO2 correction and could, in fact, end up as the highest quality overall HALOE aerosol extinction coefficient measurement. It also appears that the 2.45 and 5.26 micron channels may be improved by updating the Upper Atmosphere Pilot Database which is used as a resource for the removal of gas species otherwise not available from direct HALOE measurements. Finally, a simple model to demonstrate the promise of mixed visible/infrared aerosol extinction coefficient ensembles for the retrieval of bulk aerosol properties demonstrates that a combined HALOE/SAGE II aerosol climatology is feasible and may represent a substantial improvement over independently derived data sets.

Thomason, L. W.↗

The Ozone Mapping and Profiler Suite (OMPS) Limb Profiler (LP) Version 1 Aerosol Extinction Retrieval Algorithm: Theoretical Basis

The theoretical basis of the Ozone Mapping and Profiler Suite (OMPS) Limb Profiler (LP) Version 1 aerosol extinction retrieval algorithm is presented. The algorithm uses an assumed bimodal lognormal aerosol size distribution to retrieve aerosol extinction profiles at 675 nm from OMPS LP radiance measurements. A first-guess aerosol extinction profile is updated by iteration using the Chahine nonlinear relaxation method, based on comparisons between the measured radiance profile at 675 nm and the radiance profile calculated by the Gauss Seidel limb-scattering (GSLS) radiative transfer model for a spherical-shell atmosphere. This algorithm is discussed in the context of previous limb-scattering aerosol extinction retrieval algorithms, and the most significant error sources are enumerated. The retrieval algorithm is limited primarily by uncertainty about the aerosol phase function. Horizontal variations in aerosol extinction, which violate the spherical-shell atmosphere assumed in the version 1 algorithm, may also limit the quality of the retrieved aerosol extinction profiles significantly.

Loughman, Robert↗

Raman Lidar Measurements of Aerosol Extinction and Backscattering: Derivation of Aerosol Real Refractive Index, Single-Scattering Albedo, and Humidification Factor using Raman Lidar and Aircraft Size Distribution - Report 2

Aerosol backscattering and extinction profiles measured by the NASA Goddard Space Flight Center Scanning Raman Lidar (SRL) during the remote cloud sensing (RCS) intensive operations period (IOP) at the Department of Energy Atmospheric Radiation Measurement (ARM) southern Great Plains (SGP) site during two nights in April 1994 are discussed. These profiles are shown to be consistent with the simultaneous aerosol size distribution measurements made by a PCASP (Passive Cavity Aerosol Spectrometer Probe) optical particle counter flown on the University of North Dakota Citation aircraft. We describe a technique which uses both lidar and PCASP measurements to derive the dependence of particle size on relative humidity, the aerosol real refractive index n, and estimate the effective single-scattering albedo Omega(sub 0). Values of n ranged between 1.4-1.5 (dry) and 1.37-1.47 (wet); Omega(sub 0) varied between 0.7 and 1.0. The single-scattering albedo derived from this technique is sensitive to the manner in which absorbing particles are represented in the aerosol mixture; representing the absorbing particles as an internal mixture rather than the external mixture assumed here results in generally higher values of Omega(sub 0). The lidar measurements indicate that the change in particle size with relative humidity as measured by the PCASP can be represented in the form discussed by Hattel with the exponent gamma = 0.3 + or - 0.05. The variations in aerosol optical and physical characteristics captured in the lidar and aircraft size distribution measurements are discussed in the context of the meteorological conditions observed during the experiment.

Ferrare, R. A.↗

Measurements of Stratospheric Pinatubo Aerosol Extinction Profiles by a Raman Lidar

The Raman lidar has been used for remote measurements of water vapor, ozone and atmospheric temperature in the lower troposphere because the Raman cross section is three orders smaller than the Rayleigh cross section. We estimated the extinction coefficients of the Pinatubo volcanic aerosol in the stratosphere using a Raman lidar. If the precise aerosol extinction coefficients are derived, the backscatter coefficient of a Mie scattering lidar will be more accurately estimated. The Raman lidar has performed to measure density profiles of some species using Raman scattering. Here we used a frequency-doubled Nd:YAG laser for transmitter and received nitrogen vibrational Q-branch Raman scattering signal. Ansmann et al. (1990) derived tropospherical aerosol extinction profiles with a Raman lidar. We think that this method can apply to dense stratospheric aerosols such as Pinatubo volcanic aerosols. As dense aerosols are now accumulated in the stratosphere by Pinatubo volcanic eruption, the error of Ramen lidar signal regarding the fluctuation of air density can be ignored.

Abo, Makoto↗

Antarctic springtime measurements of ozone, nitrogen dioxide, and aerosol extinction by SAM II, SAGE, and SAGE II

Simultaneous vertical profiles of O3, NO2, and aerosol extinction obtained with the Stratospheric Aerosol Measurement II, Stratospheric Aerosol and Gas Experiment (SAGE), and SAGE II satellite instruments across the southern polar vortex show that significant differences exist at all altitudes. Both gaseous species display lower concentrations within the vortex over measurement altitudes ranging from the tropopause to 60 km and 20 to 40 km for O3 and NO2, respectively. Aerosol extinction above 15-18 km and total aerosol stratospheric column are also lower inside the vortex than outside. Total column amounts of O3 and NO2 are found to be strongly coupled to spatial location within the vortex, with minimum total values located around the vortex center. Vertical profiles selected to emphasize the observed difference across the circumpolar vortex are presented for October 13, 1981, and October 13, 1985, near 70 and 68 deg S latitude, respectively.

Mccormick, M. P.↗

Aircraft Measurements of BrO, IO, Glyoxal, NO2, H2O, O2-O2 and Aerosol Extinction Profiles in the Tropics: Comparison with Aircraft-/Ship-Based in Situ and Lidar Measurements

Tropospheric chemistry of halogens and organic carbon over tropical oceans modifies ozone and atmospheric aerosols, yet atmospheric models remain largely untested for lack of vertically resolved measurements of bromine monoxide (BrO), iodine monoxide (IO) and small oxygenated hydrocarbons like glyoxal (CHOCHO) in the tropical troposphere. BrO, IO, glyoxal, nitrogen dioxide (NO2), water vapor (H2O) and O2-O2 collision complexes (O4/ were measured by the University of Colorado Airborne Multi-AXis Differential Optical Absorption Spectroscopy (CU AMAXDOAS) instrument, aerosol extinction by high spectral resolution lidar (HSRL), in situ aerosol size distributions by an ultra high sensitivity aerosol spectrometer (UHSAS) and in situ H2O by vertical-cavity surface-emitting laser (VCSEL) hygrometer. Data are presented from two research flights (RF12, RF17) aboard the National Science Foundation/ National Center for Atmospheric Research Gulfstream V aircraft over the tropical Eastern Pacific Ocean (tEPO) as part of the "Tropical Ocean tRoposphere Exchange of Reactive halogens and Oxygenated hydrocarbons" (TORERO) project (January/February 2012). We assess the accuracy of O4 slant column density (SCD) measurements in the presence and absence of aerosols. Our O4-inferred aerosol extinction profiles at 477 nm agree within 6% with HSRL in the boundary layer and closely resemble the renormalized profile shape of Mie calculations constrained by UHSAS at low (sub-Rayleigh) aerosol extinction in the free troposphere. CU AMAX-DOAS provides a flexible choice of geometry, which we exploit to minimize the SCD in the reference spectrum (SCDREF, maximize signal-to-noise ratio) and to test the robustness of BrO, IO and glyoxal differential SCDs. The RF12 case study was conducted in pristine marine and free tropospheric air. The RF17 case study was conducted above the NOAA RV Ka'imimoana (TORERO cruise, KA-12-01) and provides independent validation data from ship-based in situ cavity-enhanced DOAS and MAX-DOAS. Inside the marine boundary layer (MBL) no BrO was detected (smaller than 0.5 pptv), and 0.2-0.55 pptv IO and 32-36 pptv glyoxal were observed. The near-surface concentrations agree within 30% (IO) and 10% (glyoxal) between ship and air-craft. The BrO concentration strongly increased with altitude to 3.0 pptv at 14.5 km (RF12, 9.1 to 8.6 deg N; 101.2 to 97.4 deg W). At 14.5 km, 5-10 pptv NO2 agree with model predictions and demonstrate good control over separating tropospheric from stratospheric absorbers (NO2 and BrO). Our profile retrievals have 12-20 degrees of freedom (DoF) and up to 500m vertical resolution. The tropospheric BrO vertical column density (VCD) was 1.5 x 10(exp 13) molec cm(exp -2) (RF12) and at least 0.5 x 10(exp 13) molec cm(exp -2) (RF17, 0- 10 km, lower limit). Tropospheric IO VCDs correspond to 2.1 x 10(exp 12) molec cm(exp -2) (RF12) and 2.5 x 10(exp 12) molec cm(exp -2) (RF17) and glyoxal VCDs of 2.6 x 10(exp 14) molec cm(exp -2) (RF12) and 2.7 x 10(exp 14) molec cm(exp -2) (RF17). Surprisingly, essentially all BrO as well as the dominant IO and glyoxal VCD fraction was located above 2 km (IO: 58 plus or minus 5 %, 0.1-0.2 pptv; glyoxal: 52 plus or minus 5 %, 3-20 pptv). To our knowledge there are no previous vertically resolved measurements of BrO and glyoxal from aircraft in the tropical free troposphere. The atmospheric implications are briefly discussed. Future studies are necessary to better understand the sources and impacts of free tropospheric halogens and oxygenated hydrocarbons on tropospheric ozone, aerosols, mercury oxidation and the oxidation capacity of the atmosphere.

Volkamer, R.↗