Radiative Transfer Model SCIATRAN Research Articles

Greenhouse gas retrievals for the CO2M mission using the FOCAL method: first performance estimates

Abstract. The Anthropogenic Carbon Dioxide Monitoring (CO2M) mission is a constellation of satellites currently planned to be launched in 2026. CO2M is planned to be a core component of a Monitoring and Verification Support (MVS) service capacity under development as part of the Copernicus Atmosphere Monitoring Service (CAMS). The CO2M radiance measurements will be used to retrieve column-averaged dry-air mole fractions of atmospheric carbon dioxide (XCO2), methane (XCH4) and total columns of nitrogen dioxide (NO2). Using appropriate inverse modelling, the atmospheric greenhouse gas (GHG) observations will be used to derive United Nations Framework Convention on Climate Change (UNFCCC) COP 21 Paris Agreement relevant information on GHG sources and sinks. This challenging application requires highly accurate XCO2 and XCH4 retrievals. Three different retrieval algorithms to derive XCO2 and XCH4 are currently under development for the operational processing system at EUMETSAT. One of these algorithms uses the heritage of the FOCAL (Fast atmOspheric traCe gAs retrievaL) method, which has already successfully been applied to measurements from other satellites. Here, we show recent results generated using the CO2M version of FOCAL, called FOCAL-CO2M. To assess the quality of the FOCAL-CO2M retrievals, a large set of representative simulated radiance spectra has been generated using the radiative transfer model SCIATRAN. These simulations consider the planned viewing geometry of the CO2 instrument and corresponding geophysical scene data (including different types of aerosols and varying surface properties), which were taken from model data for the year 2015. We consider instrument noise and systematic errors caused by the retrieval method but have not considered additional error sources due to, for example, instrumental issues, spectroscopy or meteorology. On the other hand, we have also not taken advantage in this study of CO2M's MAP (multi-angle polarimeter) instrument, which will provide additional information on aerosols and cirrus clouds. By application of the FOCAL retrieval to these simulated data, confidence is gained that the FOCAL method is able to fulfil the challenging requirements for systematic errors for the CO2M mission (spatio-temporal bias ≤ 0.5 ppm for XCO2 and ≤ 5 ppb for XCH4).

Revisiting the question “Why is the sky blue?”

Abstract. The common answer to the question “Why is the sky blue?” is usually Rayleigh scattering. In 1953 Edward Hulburt demonstrated that Rayleigh scattering accounts for 1/3 and ozone absorption for 2/3 of the blue colour of the zenith sky at sunset. In this study, an approach to quantify the contribution of ozone to the blue colour of the sky for different viewing geometries is implemented using the radiative transfer model SCIATRAN and the CIE (International Commission on Illumination) XYZ 1931 colour system. The influence of ozone on the blue colour of the sky is calculated for solar zenith angles of 10–90∘ and a wide range of viewing geometries. For small solar zenith angles, the influence of ozone on the blue colour of the sky is minor, as expected. However, the effect of ozone increases with increasing solar zenith angle. The calculations for the Sun at the horizon confirm Hulburt's estimation with remarkably good agreement. More stratospheric aerosols reduce the ozone contribution at and near the zenith for the Sun at the horizon. The exact contribution of ozone depends strongly on the assumed total ozone column. The calculations also show that the contribution of ozone increases with increasing viewing zenith angle and total ozone column. Variations in surface albedo as well as full treatment of polarised radiative transfer were found to have only minor effects on the contribution of ozone to the blue colour of the sky. Furthermore, with an observer at 10 km altitude an increase in the ozone influence can be seen.

Validation of EMI-2 Radiometric Performance with TROPOMI over Dome C Site in Antarctica

(1) The Environmental Trace Gases Monitoring Instrument-2(EMI-2) is a high-quality spaceborne imaging spectrometer that launched in September 2021. To evaluate its radiometric calibration performance in-flight, the UV2 and VIS1 bands of EMI-2 were cross-calibrated by the corresponding bands (band3 and band4) of TROPOMI over the pseudo-invariant calibration site Dome C. (2) After angle limitation and cloud filtering of the Earth radiance data measured by EMI-2 and TROPOMI over Dome C, the top of atmosphere (TOA) reflectance time series were calculated. The spectral adjustment factors (SAF) were derived from the solar spectrum measured by the sensor to minimize the uncertainties caused by the different spectral response functions (SRF) of sensors. In addition, a correction method based on the radiative transfer model (RTM) SCIATRAN was used to suppress unaccounted angular dependence of atmospheric scattering. The radiation performance of EMI-2 is evaluated using the TOA reflectance ratio of EMI-2 and TROPOMI, combining the SAF correction and RTM-based correction methods. (3) It was shown that the time series trending of the TOA reflectance ratio between EMI-2 measurements and TROPOMI demonstrate flat characteristics and strong correlation. The mean reflectance ratios range from 0.998 to 1.09. The standard deviation of the reflection ratio is less than 3%. For 328 nm, 335 nm, 340 nm, 460 nm, and 490 nm, the mean values are close to one, and the relative radiometric bias estimated through EMI-2 and TROPOMI intercalibration is less than 3%, and for other wavelengths, the biases are less than 6%, except for 416 nm, which behaves higher than 7%. The cross-calibration results show that the radiometric calibration of EMI-2 is within the relative accuracy requirement.

SCIATRAN software package (V4.6): update and further development of aerosol, clouds, surface reflectance databases and models

Abstract. Since the initiation of development at the Institute of Environmental Physics (IUP), University of Bremen, in 1994, the radiative transfer model SCIATRAN (formerly GOMETRAN) has been continuously improved and new versions have been released (Rozanov et al., 1997, 2002, 2005, 2014, 2017). In the course of development, the SCIATRAN software package became capable of simulating radiative transfer processes through the Earth's atmosphere or coupled atmosphere–ocean system with a variety of approaches to treat the sphericity of the atmosphere (plane-parallel, pseudo-spherical, approximately spherical and full-spherical solutions) in both scalar and vector modes. Supported by a variety of built-in databases and parameterizations, these capabilities made SCIATRAN widely used for various remote-sensing applications related to the retrieval of atmospheric trace gases and characteristics of aerosols, clouds and surfaces. This paper presents an overview of the cloud, aerosol and surface (CAS) databases and models implemented in the SCIATRAN software package (V4.6) and provides some recommendations on their usage. The new implementations offer potential users a flexible interface to perform radiative transfer simulations: (1) accounting for multilayer liquid water, ice and mixed-phase clouds; (2) employing typical aerosol-type parameterizations (including vertical variability) used in the satellite and model communities as well as updated databases; (3) including various surface bidirectional reflectance distribution function (BRDF) and albedo models for land, vegetation, ocean, snow and melt ponds on sea ice. The most recent version of the radiative transfer model SCIATRAN is freely available at the website of the IUP, University of Bremen: http://www.iup.physik.uni-bremen.de/sciatran (last access: November 2022).

On the twilight phenomenon of the green band.

The twilight sky is usually characterized by the well-known reddish/orange colors close to the horizon and the blue colors above. However, in many cases, a green or greenish band forms between the blue and reddish parts of the sky, and it is essentially not documented in the literature. In this study, the green band phenomenon is simulated using the radiative transfer model SCIATRAN and subsequent color modeling based on the CIE color matching functions and chromaticity values. Different parameters and processes that have a potential influence are investigated. In addition, a possible contribution by airglow emissions is discussed. The simulations show that it requires just the right intensities in the blue, green, and long-wave spectral regions to produce a green color. The total ozone column has the comparatively largest influence. This study is, to the best of our knowledge, the first detailed investigation of the green band phenomenon.

On the colour of noctilucent clouds

Abstract. The high-latitude phenomenon of noctilucent clouds (NLCs) is characterised by a silvery-blue or pale blue colour. In this study, we employ the radiative transfer model SCIATRAN to simulate spectra of solar radiation scattered by NLCs for a ground-based observer and assuming spherical NLC particles. To determine the resulting colours of NLCs in an objective way, the CIE (International Commission on Illumination) colour-matching functions and chromaticity values are used. Different processes and parameters potentially affecting the colour of NLCs are investigated, i.e. the size of the NLC particles, the abundance of middle atmospheric O3 and the importance of multiply scattered solar radiation. We affirm previous research indicating that solar radiation absorption in the O3 Chappuis bands can have a significant effect on the colour of the NLCs. A new result of this study is that for sufficiently large NLC optical depths and for specific viewing geometries, O3 plays only a minor role for the blueish colour of NLCs. The simulations also show that the size of the NLC particles affects the colour of the clouds. Cloud particles of unrealistically large sizes can lead to a reddish colour. Furthermore, the simulations show that the contribution of multiple scattering to the total scattering is only of minor importance, providing additional justification for the earlier studies on this topic, which were all based on the single-scattering approximation.

Analysis of vertical distribution differences of global stratospheric ozone based on weighted multiplication algebraic algorithm

Global climate change and the formation of the Antarctic ozone hole have prompted people to pay attention to the changes in atmospheric ozone content. The global continuous observation of ozone is achieved by retrieving the global total column concentration from nadir satellite data. In this work, the weighted multiplication algebraic algorithm is combined with the radiative transfer model SCIATRAN, by using the 2011 Chappuis-Wulf band SCIAMACHY limb radiation data to retrieve the stratospheric ozone profile between 15- and 40 km altitude, solving the ozone global stratified observation problems. In the ozone global stratification map, the whole process of the global transmission of ozone formed in low latitude regions to high latitude regions is observed, which is directly related to the Brewer-Dobson circulation. During the most severe period of the Antarctic ozone hole from September to October, the Antarctic polar vortex has an obvious hindering effect on ozone transmission, and the polar vortex has a “transparent wall” effect. On the one hand, it is difficult to transfer ozone from the equatorial region to the Antarctic region for replenishment. On the other hand, the retention of ozone-depleting substances over the Antarctic region leads to the acceleration of ozone depletion, and the combination of low replenishment and high depletion contributes to the Antarctic ozone hole. Compared with the global total column concentration of ozone, the observation of global ozone stratification is very valuable for scientific research and will promote the detailed study of the whole process of ozone formation, transmission, and consumption.

Modeling of inelastically scattered radiation: Rotational Raman scattering in the spherical Earth’s atmosphere

This study presents an approximative approach to solve the radiative transfer equation accounting for the rotational Raman scattering in a spherical atmosphere. The solution is obtained employing the method of characteristics in combination with the discrete-ordinates technique and the forward-adjoint perturbation theory. For a non-limb observational geometry, impact of the atmospheric sphericity on the filling-in of solar Fraunhofer lines is discussed. For a limb viewing geometry, the dependence of the filling-in on the surface elevation, surface albedo, and cloudiness below the instrument line of sight as well as the effect of the multiple scattering in the spatial domain is analyzed. A comparison of modeled and measured Ring spectra for a limb-viewing geometry is shown. The considered solution technique is implemented in the radiative transfer model SCIATRAN and is ready to use for atmospheric applications.

Simulated reflectance above snow constrained by airborne measurements of solar radiation: implications for the snow grain morphology in the Arctic

Abstract. Accurate knowledge of the reflectance from snow/ice-covered surfaces is of fundamental importance for the retrieval of snow parameters and atmospheric constituents from space-based and airborne observations. In this paper, we simulate the reflectance in a snow–atmosphere system, using the phenomenological radiative transfer model SCIATRAN, and compare the results with that of airborne measurements. To minimize the differences between measurements and simulation, we determine and employ the key atmospheric and surface parameters, such as snow grain morphologies (or habits). First, we report on a sensitivity study. This addresses the requirement for adequate a priori knowledge about snow models and ancillary information about the atmosphere. For this aim, we use the well-validated phenomenological radiative transfer model, SCIATRAN. Second, we present and apply a two-stage snow grain morphology (i.e., size and shape of ice crystals in the snow) retrieval algorithm. We then describe the use of this new retrieval for estimating the most representative snow model, using different types of snow morphologies, for the airborne observation conditions performed by NASA's Cloud Absorption Radiometer (CAR). Third, we present a comprehensive comparison of the simulated reflectance (using retrieved snow grain size and shape and independent atmospheric data) with that from airborne CAR measurements in the visible (0.670 µm) and near infrared (NIR; 0.870 and 1.6 µm) wavelength range. The results of this comparison are used to assess the quality and accuracy of the radiative transfer model in the simulation of the reflectance in a coupled snow–atmosphere system. Assuming that the snow layer consists of ice crystals with aggregates of eight column ice habit and having an effective radius of ∼99 µm, we find that, for a surface covered by old snow, the Pearson correlation coefficient, R, between measurements and simulations is 0.98 (R2∼0.96). For freshly fallen snow, assuming that the snow layer consists of the aggregate of five plates ice habit with an effective radius of ∼83 µm and having surface inhomogeneity, the correlation is ∼0.97 (R2∼0.94) in the infrared and 0.88 (R2∼0.77) in the visible wavelengths. The largest differences between simulated and measured values are observed in the glint area (i.e., in the angular regions of specular and near-specular reflection), with relative azimuth angles <±40∘ in the forward-scattering direction. The absolute difference between the modeled results and measurements in off-glint regions, with a viewing zenith angle of less than 50∘, is generally small ∼±0.025 and does not exceed ±0.05. These results will help to improve the calculation of snow surface reflectance and relevant assumptions in the snow–atmosphere system algorithms (e.g., aerosol optical thickness retrieval algorithms in the polar regions).

Retrieval of aerosol optical thickness and surface parameters based on multi-spectral and multi-viewing space-borne measurements

We present a novel approach to derive Aerosol Optical Thickness (AOT) at 0.5 µm and the surface reflectance for five spectral channels at native spatial resolution from the measurements of the Polarization and Directionality of Earth’s Reflectances-3 (POLDER) instrument aboard the Polarization & Anisotropy of Reflectances for Atmospheric Sciences coupled with Observations from a Lidar (PARASOL) satellite. POLDER had multi-spectral and multi-viewing capabilities. This publication describes the first step in the design of a high-quality AOT and surface property retrieval algorithm, enabling the global evaluation of future missions providing multi-spectral and multi-viewing space-borne measurements. The developed retrieval approach is based on the radiative transfer and retrieval model SCIATRAN using an analytical linearized retrieval mode. The surface is parametrized according to the Ross-Li model and the aerosol typing was using prescribed types based on the approach by Levy et al. [26]. The minimization using SCIATRAN has been done by solving the quadratic programming problem which minimizes the considered system of equations (typically) based on linear constraints. In this study we constrained the retrieval so far only by assuming that the retrieved AOT at 0.5 µm is larger than 0.01 and smaller than 1.5. Until now, the retrieval is based only upon unpolarized POLDER data and shows promisingly weak dependence on a priori information.As a first validation, the retrieved AOT values have been compared with ground based measurements over Atmospheric Radiation Measurement Climate Research Facilities (ARM) in the Southern Great Plains (SGP). The SCIATRAN retrievals are mostly homogeneous and consistent in the region around the US ARM/SGP measurement stations. The retrieval results agree well with the ARM ground based measurements of AOT. The correlation coefficient was R=0.84and part of the remaining differences between ARM measurements and SCIATRAN retrievals can be attributed to unmasked clouds. Histogram based analysis of the AOT values showed reasonable distributions using SCIATRAN. Most distributions based on SCIATRAN AOT retrievals within a radius of 25 km around the stations are significantly broader than those derived from ARM measurements during 30 minutes but are well centered around the ARM AOT distributions.

A fast and accurate radiative transfer model for aerosol remote sensing

After several decades’ development of retrieval techniques in aerosol remote sensing, no fast and accurate analytical Radiative Transfer Model (RTM) has been developed and applied to create global aerosol products for non-polarimetric instruments such as Ocean and Land Colour Instrument/Sentinel-3 (OLCI/Sentinel-3) and Meteosat Second Generation/Spinning Enhanced Visible and Infrared Imager (MSG/SEVIRI). Global aerosol retrieval algorithms are typically based on a Look-Up–Table (LUT) technique, requiring high-performance computers. The current eXtensible Bremen Aerosol/cloud and surfacE parameters Retrieval (XBAER) algorithm also utilizes the LUT method. In order to have a near-real time retrieval and achieve a quick and accurate “FIRST-LOOK” aerosol product without high-demand of computing resource, we have developed a Fast and Accurate Semi-analytical Model of Atmosphere-surface Reflectance (FASMAR) for aerosol remote sensing. The FASMAR is developed based on a successive order of scattering technique. In FASMAR, the first three orders of scattering are calculated exactly. The contribution of higher orders of scattering is estimated using an extrapolation technique and an additional correction function. The evaluation of FASMAR has been performed by comparing with radiative transfer model SCIATRAN for all typical observation/illumination geometries, surface/aerosol conditions, and wavelengths 412, 550, 670, 870, 1600, 2100 nm used for aerosol remote sensing. The selected observation/illumination conditions are based on the observations from both geostationary satellite (e.g. MSG/SEVIRI) and polar-orbit satellite (e.g. OLCI/Sentinel-3). The percentage error of the top of atmosphere reflectance calculated by FASMAR is within ± 3% for typical polar-orbit/geostationary satellites’ observation/illumination geometries. The accuracy decreases for solar and viewing zenith angles larger than 70∘. However, even in such cases, the error is within the range ± 5%. The evaluation of model performance also shows that FASMAR can be used for all typical surfaces with albedo in the interval [0−1]and aerosol with optical thickness in the range [0.01−1].

Implementation of an ice crystal single-scattering property database in the radiative transfer model SCIATRAN

Ice crystal single-scattering properties (single-scattering albedo, extinction cross section, scattering matrix) determine the radiative transfer through ice clouds and snow layers. In the radiative transfer model SCIATRAN, only a limited range of particle sizes and shapes were available. Consequentially, and to achieve a much more realistic representation, a new database of nine ice crystals (droxtals, solid and hollow columns, aggregates of eight hexagonal solid columns, hexagonal plates, aggregates of five or 10 hexagonal plates, and solid and hollow bullet rosettes) with maximum dimensions from 2 to 10 000 µm has been implemented and tested. SCIATRAN now includes the relevant single-scattering albedo, extinction cross section, and scattering matrix. Additionally, the scattering matrix is expanded in generalized spherical functions based on a combination of trapezoidal and Gaussian quadrature. This implemented database in conjunction with a built in user-defined particle size distribution and an arbitrary habit ratio enable the radiative transfer through a variety of layers, composed of polydisperse ice particles having particular habit mixtures. A comparison of satellite measured snow surface reflectances with respective simulations demonstrates that assuming ice crystal habit mixtures rather than single-habits as snow crystals reduces significantly the differences between the model and satellite data from 8.5 % to 2 %.

Impact of the near-field effects on radiative transfer simulations of the bidirectional reflectance factor and albedo of a densely packed snow layer

Phenomenological radiative transfer models commonly assume that particles in media reside in each other’s far zone and, thus, are defined by their single-scattering properties. This so called far-field assumption becomes questionable for dense particulate snow layers since the location of the snow grains inside is close and in each other’s near zone. Electromagnetic interactions among the particles can occur, which potentially change their single-scattering properties. In this paper, the near-field effects in radiative transfer simulations of the snow surface bidirectional reflectance factor (BRF) and the albedo of a snow layer in the wavelength range of 300 - 2500 nm are investigated using the phenomenological radiative transfer model SCIATRAN. The snow layer is composed of densely packed snow grains of droxtal shape with a maximum dimension of 60 µm. The snow grain shape assumption is justified by the good agreement of the simulated top of atmosphere BRF with satellite measurements over a pure snow surface in Greenland. To evaluate the error of the far-field assumption, the single-scattering properties of the dense particulate snow layer has been modified according to the dense-medium light-scattering theory. By applying the far-field approximation, the BRF is overestimated by less than 0.039 % at forward-scattering angles and underestimated by less than 0.006 % at backscattering angles, respectively. The albedo of the dense particulate snow layer is overestimated by less than 0.012 %. In the considered case, the near-field effects on the snow surface BRF and the albedo of radiative transfer simulations appear negligibly small. Consequently, the simulation of snow surface BRF and albedo in the wavelength range of 300 - 2500 nm by phenomenological radiative transfer models under the far-field assumption is well justified.

Concept of small satellite UV/visible imaging spectrometer optimized for tropospheric NO2 measurements in air quality monitoring

Satellite observations at nadir can potentially facilitate a better understanding of the emissions and distribution of tropospheric nitrogen dioxide, NO2, which is a well-known pollutant. The identification of emissions requires adequate spatiotemporal resolution measurements of the total column amounts of NO2. The spatial resolution of previous and current observations is insufficient for the identification of NO2 hot-spots. Switching to a spatial resolution of ∼ 1 km × ∼ 1 km can improve the identification of local sources of NO2 and their emissions. To investigate the feasibility of observations with such a high spatial resolution, we simulated radiance spectra for different cases under varying parameters, such as area, season, satellite altitude, and surface reflectance by using the radiative transfer model SCIATRAN. We subsequently retrieved NO2 slant column densities (SCDs) using the differential optical absorption spectroscopy (DOAS) technique with several fit windows. For test cases associated with polluted conditions, we found that the conceptual nadir-observing instrument on a satellite at an altitude of ∼ 300 km involved the lowest retrieval errors for signal-to-noise ratios of around 1000 with accuracy better than the required 5% for tropospheric NO2 SCD and that the fit window of 425–497 nm met the scientific requirements for both surface reflectance cases.

BOREAS – a new MAX-DOAS profile retrieval algorithm for aerosols and trace gases

Abstract. We present a new MAX-DOAS profiling algorithm for aerosols and trace gases, BOREAS, which utilizes an iterative solution method including Tikhonov regularization and the optimal estimation technique. The aerosol profile retrieval is based on a novel approach in which the absorption depth of O4 is directly used in order to retrieve extinction coefficient profiles instead of the commonly used perturbation theory method. The retrieval of trace gases is done with the frequently used optimal estimation method but significant improvements are presented on how to deal with wrongly weighted a priori constraints and for scenarios in which the a priori profile is inaccurate. Performance tests are separated into two parts. First, we address the general sensitivity of the retrieval to the example of synthetic data calculated with the radiative transfer model SCIATRAN. In the second part of the study, we demonstrate BOREAS profiling accuracy by validating the results with the help of ancillary measurements carried out during the CINDI-2 campaign in Cabauw, the Netherlands, in 2016. The synthetic sensitivity tests indicate that the regularization between measurement and a priori constraints is insufficient when knowledge of the true state of the atmosphere is poor. We demonstrate a priori pre-scaling and extensive regularization tests as a tool for the optimization of retrieved profiles. The comparison of retrieval results with in situ, ceilometer, NO2 lidar, sonde and long-path DOAS measurements during the CINDI-2 campaign always shows high correlations with coefficients greater than 0.75. The largest differences can be found in the morning hours, when the planetary boundary layer is not yet fully developed and the concentration of trace gases and aerosol, as a result of a low night-time boundary layer having formed, is focused in a shallow, near-surface layer.

Comparison of SO2 column retrievals from BRD and DOAS algorithms

Atmospheric SO2 has a significant impact on the urban environment and global climate. Band Residual Difference Algorithm (BRD) and Differential Optical Absorption Spectroscopy (DOAS) were used respectively by NASA and ESA science team to derive SO2 columns from satellite observations, but there are few studies on the comparison and validation of BRD and DOAS SO2 retrievals under the same observation conditions. In this study, the radiative transfer model SCIATRAN was firstly used to validate the accuracies of BRD and DOAS SO2 retrievals, and analyse the uncertainty of SO2 retrieval caused by band selection, O3 absorption, aerosol, surface reflectance, solar and viewing zenith angle. Finally, BRD and DOAS algorithms were applied to the same radiances from satellite observations, and comparisons of BRD and DOAS SO2 retrievals were conducted over volcanic eruption and North China. Results show that, for the case with low SO2 columns, BRD SO2 retrievals have higher retrieval accuracy than DOAS, but typical seasonal variation with high SO2 column in winter and low in summer can be more clearly discernible in DOAS SO2 retrievals than BRD from satellite observations. For the case with high SO2 columns, the differences between BRD (310.8–314.4 nm) and DOAS (315–327 nm) retrievals are large, and the value and accuracy of BRD (310.8–314.4 nm) SO2 retrievals are lower than those of DOAS (315–327 nm) retrievals. Compared with the SO2 inputs in forward model, both BRD (310.8–314.4 nm) and DOAS (315–327 nm) SO2 retrievals are underestimated for the case with high SO2 columns. The selection of wavelength range can significantly affect the accuracy of SO2 retrieval. The error of BRD SO2 retrieval from 310.8–314.4 nm is lower than other bands in the ultraviolet spectral region (306–327 nm). The increase of wavelength in the ultraviolet spectral region 306–330 nm can reduce the underestimation of DOAS SO2 retrievals in the case of high SO2 column, but slight overestimation of SO2 retrieval is found from the 315–327 nm range in the case of low SO2 column. The values of BRD and DOAS SO2 retrieval decrease with atmospheric O3 column and aerosol optical depth increasing, but increase with surface reflectance increasing. Large solar zenith angle and viewing zenith angle can introduce more errors to the BRD and DOAS SO2 retrievals. This study is important for the improvement of retrieval algorithm and the application of SO2 products from satellite observations.

Estimates of free-tropospheric NO<sub>2</sub> and HCHO mixing ratios derived from high-altitude mountain MAX-DOAS observations at midlatitudes and in the tropics

Abstract. In this study, mixing ratios of NO2 (XNO2) and HCHO (XHCHO) in the free troposphere are derived from two multi-axis differential optical absorption spectroscopy (MAX-DOAS) data sets collected at Zugspitze (2650 m a.s.l., Germany) and Pico Espejo (4765 m a.s.l., Venezuela). The estimation of NO2 and HCHO mixing ratios is based on the modified geometrical approach, which assumes a single-scattering geometry and a scattering point altitude close to the instrument altitude. Firstly, the horizontal optical path length (hOPL) is obtained from O4 differential slant column densities (DSCDs) in the horizontal (0°) and vertical (90°) viewing directions. Secondly, XNO2 and XHCHO are estimated from the NO2 and HCHO DSCDs at the 0° and 90° viewing directions and averaged along the obtained hOPLs. As the MAX-DOAS instrument was performing measurements in the ultraviolet region, wavelength ranges of 346–372 and 338–357 nm are selected for the DOAS analysis to retrieve NO2 and HCHO DSCDs, respectively. In order to compare the measured O4 DSCDs and moreover to perform some sensitivity tests, the radiative transfer model SCIATRAN with adapted altitude settings for mountainous terrain is operated to simulate synthetic spectra, on which the DOAS analysis is also applied. The overall agreement between measured and synthetic O4 DSCDs is better for the higher Pico Espejo station than for Zugspitze. Further sensitivity analysis shows that a change in surface albedo (from 0.05 to 0.7) can influence the O4 DSCDs, with a larger absolute difference observed for the horizontal viewing direction. Consequently, the hOPL can vary by about 5 % throughout the season, for example when winter snow cover fully disappears in summer. Typical values of hOPLs during clear-sky conditions are 19 km (14 km) at Zugspitze and 34 km (26.5 km) at Pico Espejo when using the 346–372 (338–357 nm) fitting window. The estimated monthly values of XNO2 (XHCHO), averaged over these hOPLs during clear-sky conditions, are in the range of 60–100 ppt (500–950 ppt) at Zugspitze and 8.5–15.5 ppt (255–385 ppt) at Pico Espejo. Interestingly, multi-year-averaged monthly means of XNO2 and XHCHO increase towards the end of the dry season at the Pico Espejo site, suggesting that both trace gases are frequently lifted above the boundary layer as a result of South American biomass burning.

Global cloud top height retrieval using SCIAMACHY limb spectra: model studies and first results

Abstract. Cloud top heights (CTHs) are retrieved for the period 1 January 2003 to 7 April 2012 using height-resolved limb spectra measured with the SCanning Imaging Absorption SpectroMeter for Atmospheric CHartographY (SCIAMACHY) on board ENVISAT (ENVIronmental SATellite). In this study, we present the retrieval code SCODA (SCIAMACHY cloud detection algorithm) based on a colour index method and test the accuracy of the retrieved CTHs in comparison to other methods. Sensitivity studies using the radiative transfer model SCIATRAN show that the method is capable of detecting cloud tops down to about 5 km and very thin cirrus clouds up to the tropopause. Volcanic particles can be detected that occasionally reach the lower stratosphere. Upper tropospheric ice clouds are observable for a nadir cloud optical thickness (COT) ≥ 0.01, which is in the subvisual range. This detection sensitivity decreases towards the lowermost troposphere. The COT detection limit for a water cloud top height of 5 km is roughly 0.1. This value is much lower than thresholds reported for passive cloud detection methods in nadir-viewing direction. Low clouds at 2 to 3 km can only be retrieved under very clean atmospheric conditions, as light scattering of aerosol particles interferes with the cloud particle scattering. We compare co-located SCIAMACHY limb and nadir cloud parameters that are retrieved with the Semi-Analytical CloUd Retrieval Algorithm (SACURA). Only opaque clouds (τN,c > 5) are detected with the nadir passive retrieval technique in the UV–visible and infrared wavelength ranges. Thus, due to the frequent occurrence of thin clouds and subvisual cirrus clouds in the tropics, larger CTH deviations are detected between both viewing geometries. Zonal mean CTH differences can be as high as 4 km in the tropics. The agreement in global cloud fields is sufficiently good. However, the land–sea contrast, as seen in nadir cloud occurrence frequency distributions, is not observed in limb geometry. Co-located cloud top height measurements of the limb-viewing Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on ENVISAT are compared for the period from January 2008 to March 2012. The global CTH agreement of about 1 km is observed, which is smaller than the vertical field of view of both instruments. Lower stratospheric aerosols from volcanic eruptions occasionally interfere with the cloud retrieval and inhibit the detection of tropospheric clouds. The aerosol impact on cloud retrievals was studied for the volcanoes Kasatochi (August 2008), Sarychev Peak (June 2009), and Nabro (June 2011). Long-lasting aerosol scattering is detected after these events in the Northern Hemisphere for heights above 12.5 km in tropical and polar latitudes. Aerosol top heights up to about 22 km are found in 2009 and the enhanced lower stratospheric aerosol layer persisted for about 7 months. In August 2009 about 82 % of the lower stratosphere between 30 and 70° N was filled with scattering particles and nearly 50 % in October 2008.

Comparison between the ESFT and LBL simulation with enhanced SCIATRAN of orbital CO2 retrieval for High-resolution Satellite

The enhanced radiative transfer model SCIATRAN completes the simulation from the single point to the orbital data. There are 69 points locating at a global scale. The ESFT and LBL modes are implemented in the enhanced SCIATRAN for Medium-resolution Satellite (SCIAMACHY) and High-resolution Satellite simulations. A comparison of their spectra, accuracy and speed has been undertaken. For SCIAMACHY, the relative errors of O2 A-band (755–775nm) and WCO2 band (1560–1680nm) for ESFT and LBL (same sampling) are far less than 1%. The speed of ESFT mode is about 1.17 times faster than LBL mode for O2 A-band, about 5.24 times faster for WCO2 band. For High-resolution Satellite, the relative errors of O2 A-band and CO2 bands for ESFT and LBL are much less than 1%, and the speed increases to about 1.09 times for O2 A-band (759–769nm) than LBL mode, about 3.83 times for WCO2 band (1568–1583nm) than LBL mode. But the speed of LBL mode increases to about 47.55 times for SCO2 band (2043–2058nm) than ESFT mode. This study provides a theoretical guide for the subsequent inversion of CO2 column concentration for High-resolution Satellite.

Global retrieval of marine and terrestrial chlorophyll fluorescence at its red peak using hyperspectral top of atmosphere radiance measurements: Feasibility study and first results

Chlorophyll fluorescence is directly linked to the physiology of phytoplankton or plants. Here, we present a new satellite remote sensing approach to retrieve chlorophyll fluorescence at its red peak (~685nm) by using measurements from the hyperspectral instruments SCanning Imaging Absorption SpectroMeter for Atmospheric CHartographY (SCIAMACHY) and Global Ozone Monitoring Experiment-2 (GOME-2). This method, which is based on the Differential Optical Absorption Spectroscopy (DOAS) technique, was used to exploit narrow spectral structures resulting from the filling-in of the Fraunhofer Fe I line, which originates from fluorescence. The reference spectra for chlorophyll fluorescence were calculated by the coupled ocean–atmosphere radiative transfer model SCIATRAN. We compared our results on marine chlorophyll fluorescence observations with the MODIS Terra normalized Fluorescence Line Height (nFLH) product for the average of years 2003–2011 and year 2009. Our method also enables the retrieval of chlorophyll fluorescence above land vegetation scenes. The results for the fluorescence observed above terrestrial vegetation for July and December 2009 were compared to MODIS Enhanced Vegetation Index (EVI). The comparisons show good spatial agreement between different retrievals providing evidence for the good performance of our algorithm. The method presented is generic and can be applied to other hyperspectral instruments in the future. Having established the retrieval technique, extensive studies of chlorophyll fluorescence will improve global knowledge on physiology and photosynthetic efficiency, in both the marine and terrestrial realms, and its dependence on environmental factors.