Corrigendum to "First direct observation of the atmospheric CO2 year-to-year increase from space" published in Atmos. Chem. Phys., 7, 4249─4256, 2007

No abstract available

First direct observation of the atmospheric CO2 year-to-year increase from space

The reliable prediction of future atmospheric CO₂ concentrations and associated global climate change requires an adequate understanding of the CO₂ sources and sinks. The sparseness of the existing surface measurement network limits current knowledge about the global distribution of CO₂ surface fluxes. The retrieval of CO₂ total vertical columns from satellite observations is predicted to improve this situation. Such an application however requires very high accuracy and precision. We report on retrievals of the column-averaged CO₂ dry air mole fraction, denoted XCO₂, from the near-infrared nadir spectral radiance and solar irradiance measurements of the SCIAMACHY satellite instrument between 2003 and 2005. We focus on northern hemispheric large scale CO₂ features such as the CO₂ seasonal cycle and show - for the first time - that the atmospheric annual increase of CO₂ can be directly observed using satellite measurements of the CO₂ total column. The satellite retrievals are compared with global XCO₂ obtained from NOAA's CO₂ assimilation system CarbonTracker taking into account the spatio-temporal sampling and altitude sensitivity of the satellite data. We show that the measured CO₂ year-to-year increase agrees within about 1 ppm/year with CarbonTracker. We also show that the latitude dependent amplitude of the northern hemispheric CO₂ seasonal cycle agrees with CarbonTracker within about 2 ppm with the retrieved amplitude being systematically larger. The analysis demonstrates that it is possible using satellite measurements of the CO₂ total column to retrieve information on the atmospheric CO₂ on the level of a few parts per million

Trend in ice moistening the stratosphere – constraints from isotope data of water and methane

Water plays a major role in the chemistry and radiative budget of the stratosphere. Air enters the stratosphere predominantly in the tropics, where the very low temperatures around the tropopause constrain water vapour mixing ratios to a few parts per million. Observations of stratospheric water vapour show a large positive long-term trend, which can not be explained by change in tropopause temperatures. Trends in the partitioning between vapour and ice of water entering the stratosphere have been suggested to resolve this conundrum. We present measurements of stratospheric H_(2)O, HDO, CH_4 and CH_(3)D in the period 1991–2007 to evaluate this hypothesis. Because of fractionation processes during phase changes, the hydrogen isotopic composition of H_(2)O is a sensitive indicator of changes in the partitioning of vapour and ice. We find that the seasonal variations of H_(2)O are mirrored in the variation of the ratio of HDO to H_(2)O with a slope of the correlation consistent with water entering the stratosphere mainly as vapour. The variability in the fractionation over the entire observation period is well explained by variations in H_(2)O. The isotopic data allow concluding that the trend in ice arising from particulate water is no more than (0.01±0.13) ppmv/decade in the observation period. Our observations suggest that between 1991 and 2007 the contribution from changes in particulate water transported through the tropopause plays only a minor role in altering in the amount of water entering the stratosphere

The importance of transport model uncertainties for the estimation of CO2 sources and sinks using satellite measurements

This study presents a synthetic model intercomparison to investigate the importance of transport model errors for estimating the sources and sinks of CO2 using satellite measurements. The experiments were designed for testing the potential performance of the proposed CO2 lidar A-SCOPE, but also apply to other space borne missions that monitor total column CO2. The participating transport models IFS, LMDZ, TM3, and TM5 were run in forward and inverse mode using common a priori CO2 fluxes and initial concentrations. Forward simulations of column averaged CO2 (xCO2) mixing ratios vary between the models by s=0.5 ppm over the continents and s=0.27 ppm over the oceans. Despite the fact that the models agree on average on the sub-ppm level, these modest differences nevertheless lead to significant discrepancies in the inverted fluxes of 0.1 PgC/yr per 106 km2 over land and 0.03 PgC/yr per 106 km2 over the ocean. These transport model induced flux uncertainties exceed the target requirement that was formulated for the A-SCOPE mission of 0.02 PgC/yr per 106 km2, and could also limit the overall performance of other CO2 missions such as GOSAT. A variable, but overall encouraging agreement is found in comparison with FTS measurements at Park Falls, Darwin, Spitsbergen, and Bremen, although systematic differences are found exceeding the 0.5 ppm level. Because of this, our estimate of the impact of transport model uncerainty is likely to be conservative. It is concluded that to make use of the remote sensing technique for quantifying the sources and sinks of CO2 not only requires highly accurate satellite instruments, but also puts stringent requirements on the performance of atmospheric transport models. Improving the accuracy of these models should receive high priority, which calls for a closer collaboration between experts in atmospheric dynamics and tracer transpor

Towards understanding the variability in biospheric CO2 fluxes:Using FTIR spectrometry and a chemical transport model to investigate the sources and sinks of carbonyl sulfide and its link to CO2

Understanding carbon dioxide (CO2) biospheric processes is of great importance because the terrestrial exchange drives the seasonal and interannual variability of CO2 in the atmosphere. Atmospheric inversions based on CO2 concentration measurements alone can only determine net biosphere fluxes, but not differentiate between photosynthesis (uptake) and respiration (production). Carbonyl sulfide (OCS) could provide an important additional constraint: it is also taken up by plants during photosynthesis but not emitted during respiration, and therefore is a potential means to differentiate between these processes. Solar absorption Fourier Transform InfraRed (FTIR) spectrometry allows for the retrievals of the atmospheric concentrations of both CO2 and OCS from measured solar absorption spectra. Here, we investigate co-located and quasi-simultaneous FTIR measurements of OCS and CO2 performed at five selected sites located in the Northern Hemisphere. These measurements are compared to simulations of OCS and CO2 using a chemical transport model (GEOS-Chem). The coupled biospheric fluxes of OCS and CO2 from the simple biosphere model (SiB) are used in the study. The CO2 simulation with SiB fluxes agrees with the measurements well, while the OCS simulation reproduced a weaker drawdown than FTIR measurements at selected sites, and a smaller latitudinal gradient in the Northern Hemisphere during growing season when comparing with HIPPO (HIAPER Pole-to-Pole Observations) data spanning both hemispheres. An offset in the timing of the seasonal cycle minimum between SiB simulation and measurements is also seen. Using OCS as a photosynthesis proxy can help to understand how the biospheric processes are reproduced in models and to further understand the carbon cycle in the real world

Remote sensing of CO2 and CH4 using solar absorption spectrometry with a low resolution spectrometer

Throughout the last few years solar absorption Fourier Transform Spectrometry (FTS) has been further developed to measure the total columns of CO2 and CH4. The observations are performed at high spectral resolution, typically at 0.02 cm(-1). The precision currently achieved is generally better than 0.25%. However, these high resolution instruments are quite large and need a dedicated room or container for installation. We performed these observations using a smaller commercial interferometer at its maximum possible resolution of 0.11 cm(-1). The measurements have been performed at Bremen and have been compared to observations using our high resolution instrument also situated at the same location. The high resolution instrument has been successfully operated as part of the Total Carbon Column Observing Network (TCCON). The precision of the low resolution instrument is 0.32% for XCO2 and 0.46% for XCH4. A comparison of the measurements of both instruments yields an average deviation in the retrieved daily means of 0.2% for CO2. For CH4 an average bias between the instruments of 0.47% was observed. For test cases, spectra recorded by the high resolution instrument have been truncated to the resolution of 0.11 cm(-1). This study gives an offset of 0.03% for CO2 and 0.26% for CH4. These results indicate that for CH4 more than 50% of the difference between the instruments results from the resolution dependent retrieval. We tentatively assign the offset to an incorrect a-priori concentration profile or the effect of interfering gases, which may not be treated correctly

Rapid meridional transport of tropical airmasses to the Arctic during the major stratospheric warming in January 2003

International audienceWe present observations of unusually high values of ozone and N2O in the middle stratosphere that were observed by the airborne submillimeter radiometer ASUR in the Arctic. The observations took place in the meteorological situation of a major stratospheric warming that occurred in mid-January 2003 and was dominated by a wave 2 event. On 23 January 2003 the observed N2O and O3 mixing ratios around 69° N in the middle stratosphere reached maximum values of ~190 ppb and ~10 ppm, respectively. The similarities of these N2O profiles in a potential temperature range between 800 and 1200 K with N2O observations around 20° N on 1 March 2003 by the same instrument suggest that the observed Arctic airmasses were transported from the tropics quasi-isentropically. This is confirmed by 5-day back trajectory calculations which indicate that the airmasses between about 800 and 1000 K had been located around 20° N 3?5 days prior to the measurement in the Arctic. Calculations with a linearized ozone chemistry model along calculated as well as idealized trajectories, initialized with the low-latitude ASUR ozone measurements, give reasonable agreement with the Arctic ozone measurement by ASUR. PV distributions suggest that these airmasses did not stay confined in the Arctic region which makes it unlikely that this dynamical situation lead to the formation of dynamically caused pockets of low ozone

Constraints for the photolysis rate and the equilibrium constant of ClO-dimer from airborne and balloon-borne measurements of chlorine compounds

We analyze measurements of ClO across the terminator taken by the Airborne Submillimeter Radiometer (ASUR) in the activated vortices of the Arctic winters of 1995/1996, 1996/1997, and 1999/2000 to evaluate the plausibility of various determinations of the ClO-dimer photolysis cross section and the rate constant controlling the thermal equilibrium between ClO-dimer and ClO. We use measured ClO during sunlit conditions to estimate total active chlorine (ClOx). As the measurements suggest nearly full chlorine activation in winter 1999/2000, we compare ClOx estimates based on various photolysis frequencies of ClO-dimer with total available inorganic chlorine (Cly), estimated from an N2O-Cly correlation established by a balloon-borne MkIV interferometer measurement. Only ClO-dimer cross sections leading to the fastest photolysis frequencies in the literature (including the latest evaluation by the Jet Propulsion Laboratory) give ClOx mixing ratios that overlap with the estimated range of available Cly. Slower photolysis rates lead to ClOx values that are higher than available Cly. We use the ClOx calculated from sunlit ClO measurements to estimate ClO in darkness based on different equilibrium constants, and compare it with ASUR ClO measurements before sunrise at high solar zenith angles. Calculations with equilibrium constants published in recent evaluations of the Jet Propulsion Laboratory give good agreement with observed ClO mixing ratios. Equilibrium constants leading to a higher ClO/ClOx ratio in darkness yield ClO values that tend to exceed observed abundances. Perturbing the rates for the ClO + BrO reaction in a manner that increases OClO formation and decreases BrCl formation leads to lower ClO values calculated for twilight conditions after sunset, resulting in better agreement with ASUR measurements

Atmospheric greenhouse gases retrieved from SCIAMACHY: comparison to ground-based FTS measurements and model results

SCIAMACHY onboard ENVISAT (launched in 2002) enables the retrieval of global long-term column-averaged dry air mole fractions of the two most important anthropogenic greenhouse gases carbon dioxide and methane (denoted XCO_2 and XCH_4). In order to assess the quality of the greenhouse gas data obtained with the recently introduced v2 of the scientific retrieval algorithm WFM-DOAS, we present validations with ground-based Fourier Transform Spectrometer (FTS) measurements and comparisons with model results at eight Total Carbon Column Observing Network (TCCON) sites providing realistic error estimates of the satellite data. Such validation is a prerequisite to assess the suitability of data sets for their use in inverse modelling. It is shown that there are generally no significant differences between the carbon dioxide annual increases of SCIAMACHY and the assimilation system CarbonTracker (2.00 ± 0.16 ppm yr^(−1) compared to 1.94 ± 0.03 ppm yr−1 on global average). The XCO_2 seasonal cycle amplitudes derived from SCIAMACHY are typically larger than those from TCCON which are in turn larger than those from CarbonTracker. The absolute values of the northern hemispheric TCCON seasonal cycle amplitudes are closer to SCIAMACHY than to CarbonTracker and the corresponding differences are not significant when compared with SCIAMACHY, whereas they can be significant for a subset of the analysed TCCON sites when compared with CarbonTracker. At Darwin we find discrepancies of the seasonal cycle derived from SCIAMACHY compared to the other data sets which can probably be ascribed to occurrences of undetected thin clouds. Based on the comparison with the reference data, we conclude that the carbon dioxide data set can be characterised by a regional relative precision (mean standard deviation of the differences) of about 2.2 ppm and a relative accuracy (standard deviation of the mean differences) of 1.1–1.2 ppm for monthly average composites within a radius of 500 km. For methane, prior to November 2005, the regional relative precision amounts to 12 ppb and the relative accuracy is about 3 ppb for monthly composite averages within the same radius. The loss of some spectral detector pixels results in a degradation of performance thereafter in the spectral range currently used for the methane column retrieval. This leads to larger scatter and lower XCH_4 values are retrieved in the tropics for the subsequent time period degrading the relative accuracy. As a result, the overall relative precision is estimated to be 17 ppb and the relative accuracy is in the range of about 10–20 ppb for monthly averages within a radius of 500 km. The derived estimates show that the SCIAMACHY XCH_4 data set before November 2005 is suitable for regional source/sink determination and regional-scale flux uncertainty reduction via inverse modelling worldwide. In addition, the XCO2 monthly data potentially provide valuable information in continental regions, where there is sparse sampling by surface flask measurements