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We present a method for harmonized retrieval of integrated water vapor (IWV) from existing, long-term, measurement records at the ground-based mid-infrared solar FTIR spectrometry stations of the Network for the Detection of Atmospheric Composition Change (NDACC). Correlation of IWV from FTIR with radiosondes shows an ideal slope of 1.00(3). This optimum matching is achieved via tuning one FTIR retrieval parameter, i.e., the strength of a Tikhonov regularization constraining the derivative (with respect to height) of retrieved water profiles given in per cent difference relative to an a priori profile. All other FTIR-sonde correlation parameters (intercept=0.02(12) mm, bias=0.02(5) mm, standard deviation of coincident IWV differences (stdv)=0.27 mm, <i>R</i>=0.99) are comparable to or better than results for all other ground-based IWV sounding techniques given in the literature. An FTIR-FTIR side-by-side intercomparison reveals a strong exponential increase in stdv as a function of increasing temporal mismatch starting at Δ<i>t</i>≈1 min. This is due to atmospheric water vapor variability. Based on this result we derive an upper limit for the precision of the FTIR IWV retrieval for the smallest Δ<i>t</i>(=3.75 min) still giving a statistically sufficient sample (32 coincidences), i.e., precision(IWV<sub>FTIR</sub>)<0.05 mm (or 2.2% of the mean IWV). The bias of the IWV retrievals from the two different FTIR instruments is nearly negligible (0.02(1) mm). The optimized FTIR IWV retrieval is set up in the standard NDACC algorithm SFIT 2 without changes to the code. A concept for harmonized transfer of the retrieval between different stations deals with all relevant control parameters; it includes correction for differing spectral point spacings (via regularization strength), and final quality selection of the retrievals (excluding the highest residuals (measurement minus model), 5% of the total). <br><br> As first application examples long-term IWV data sets are retrieved from the FTIR records of the Zugspitze (47.4° N, 11.0° E, 2964 m a.s.l.) and Jungfraujoch (46.5° N, 8.0° E, 3580 m a.s.l.) NDACC sites. Station-trend analysis comprises a linear fit after subtracting an intra-annual model (3 Fourier components) and constructing an uncertainty interval [95% confidence] via bootstrap resampling. For the Zugspitze a significant trend of 0.79 [0.65, 0.92] mm/decade is found for the time interval [1996–2008], whereas for the Jungfraujoch no significant trend is found. This confirms recent findings that strong variations of IWV trends do occur above land on the local to regional scale (≈250 km) in spite of homogeneous surface temperature trends. This paper provides a basis for future exploitation of more than a dozen existing, multi-decadal FTIR measurement records around the globe for climate studies.
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OH reactivity is one of key indicators which reflect impacts of photochemical reactions in the atmosphere. An observation campaign has been conducted in the summer of 2007 at the heart of Tokyo metropolitan area to measure OH reactivity. The total OH reactivity measured directly by the laser-induced pump and probe technique was higher than the sum of the OH reactivity calculated from concentrations and reaction rate coefficients of individual species measured in this campaign. And then, three-dimensional air quality simulation has been conducted to evaluate the simulation performance on the total OH reactivity including "missing sinks", which correspond to the difference between the measured and calculated total OH reactivity. The simulated OH reactivity is significantly underestimated because the OH reactivity of volatile organic compounds (VOCs) and missing sinks are underestimated. When scaling factors are applied to input emissions and boundary concentrations, a good agreement is observed between the simulated and measured concentrations of VOCs. However, the simulated OH reactivity of missing sinks is still underestimated. Therefore, impacts of unidentified missing sinks are investigated through sensitivity analyses. In the cases that unknown secondary products are assumed to account for unidentified missing sinks, they tend to suppress formation of secondary aerosol components and enhance formation of ozone. In the cases that unidentified primary emitted species are assumed to account for unidentified missing sinks, a variety of impacts may be observed, which could serve as precursors of secondary organic aerosols (SOA) and significantly increase SOA formation. Missing sinks are considered to play an important role in the atmosphere over Tokyo metropolitan area.
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We evaluate black carbon (BC) model predictions from the AeroCom model intercomparison project by considering the diversity among year 2000 model simulations and comparing model predictions with available measurements. These model-measurement intercomparisons include BC surface and aircraft concentrations, aerosol absorption optical depth (AAOD) retrievals from AERONET and Ozone Monitoring Instrument (OMI) and BC column estimations based on AERONET. In regions other than Asia, most models are biased high compared to surface concentration measurements. However compared with (column) AAOD or BC burden retreivals, the models are generally biased low. The average ratio of model to retrieved AAOD is less than 0.7 in South American and 0.6 in African biomass burning regions; both of these regions lack surface concentration measurements. In Asia the average model to observed ratio is 0.7 for AAOD and 0.5 for BC surface concentrations. Compared with aircraft measurements over the Americas at latitudes between 0 and 50N, the average model is a factor of 8 larger than observed, and most models exceed the measured BC standard deviation in the mid to upper troposphere. At higher latitudes the average model to aircraft BC ratio is 0.4 and models underestimate the observed BC loading in the lower and middle troposphere associated with springtime Arctic haze. Low model bias for AAOD but overestimation of surface and upper atmospheric BC concentrations at lower latitudes suggests that most models are underestimating BC absorption and should improve estimates for refractive index, particle size, and optical effects of BC coating. Retrieval uncertainties and/or differences with model diagnostic treatment may also contribute to the model-measurement disparity. Largest AeroCom model diversity occurred in northern Eurasia and the remote Arctic, regions influenced by anthropogenic sources. Changing emissions, aging, removal, or optical properties within a single model generated a smaller change in model predictions than the range represented by the full set of AeroCom models. Upper tropospheric concentrations of BC mass from the aircraft measurements are suggested to provide a unique new benchmark to test scavenging and vertical dispersion of BC in global models.
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In this paper, we discuss scintillation time-spectra of the double star α Cru, which were measured by the GOMOS/Envisat photometer. The components of α Cru are not resolved by the angular field of view of the detector. The double structure of the light source reveals itself in the modulation of the observed scintillation spectra; this modulation is caused by anisotropic irregularities of the stratospheric air density. We present a qualitative and quantitative explanation of the properties of the double-star scintillation spectra. Possibilities of using double star scintillations for studying atmospheric air density irregularities are also discussed in the paper.
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We present an original multi-spectrum fitting procedure to retrieve volume mixing ratio (VMR) profiles of carbonyl fluoride (COF<sub>2</sub>) from ground-based high resolution Fourier transform infrared (FTIR) solar spectra. The multi-spectrum approach consists of simultaneously combining, during the retrievals, all spectra recorded consecutively during the same day and with the same resolution. Solar observations analyzed in this study with the SFIT-2 v3.91 fitting algorithm correspond to more than 2900 spectra recorded between January 2000 and December 2007 at high zenith angles, with a Fourier Transform Spectrometer operated at the high-altitude International Scientific Station of the Jungfraujoch (ISSJ, 46.5° N latitude, 8.0° E longitude, 3580 m altitude), Switzerland. The goal of the retrieval strategy described here is to provide information about the vertical distribution of carbonyl fluoride. The microwindows used are located in the ν<sub>4</sub> or in the ν<sub>4</sub> COF<sub>2</sub> infrared (IR) absorption bands. Averaging kernel and eigenvector analysis indicates that our FTIR retrieval is sensitive to COF<sub>2</sub> inversion between 17 and 30 km, with the major contribution to the retrieved information always coming from the measurement. Moreover, there was no significant bias between COF<sub>2</sub> partial columns, total columns or VMR profiles retrieved from the two bands. For each wavenumber region, a complete error budget including all identified sources has been carefully established. In addition, comparisons of FTIR COF<sub>2</sub> 17–30 km partial columns with KASIMA and SLIMCAT 3-D CTMs are also presented. If we do not notice any significant bias between FTIR and SLIMCAT time series, KASIMA COF<sub>2</sub> 17–30 km partial columns are lower of around 25%, probably due to incorrect lower boundary conditions. For each times series, linear trend estimation for the 2000–2007 time period as well as a seasonal variation study are also performed and critically discussed. For FTIR and KASIMA time series, very low COF<sub>2</sub> growth rates (0.4±0.2%/year and 0.3±0.2%/year, respectively) have been derived. However, the SLIMCAT data set gives a slight negative trend (−0.5±0.2%/year), probably ascribable to discontinuities in the meteorological data used by this model. We further demonstrate that all time series are able to reproduce the COF<sub>2</sub> seasonal cycle, which main seasonal characteristics deduced from each data set agree quite well.
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Large volcanic eruptions emit huge amounts of sulfur and fine ash into the stratosphere. These products cause an impact on radiative processes, temperature and wind patterns. In simulations with a General Circulation Model including detailed aerosol microphysics, the relation between the impact of sulfur and fine ash is determined for different eruption strengths and locations, one in the tropics and one in high Northern latitudes. Fine ash with effective radii between 1 μm and 15 μm has a lifetime of several days only. Nevertheless, the strong absorption of shortwave and long-wave radiation causes additional heating and cooling of ±20 K/day and impacts the evolution of the volcanic cloud. Depending on the location of the volcanic eruption, transport direction changes due to the presence of fine ash, vortices develop and temperature anomalies at ground increase. The results show substantial impact on the local scale but only minor impact on the evolution of sulfate in the stratosphere in the month after the simulated eruptions.
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During the Arctic Study of Tropospheric Aerosol, Clouds and Radiation (ASTAR) in March and April 2007, measurements obtained at the AWIPEV Arctic Research Base in Ny-Ålesund, Spitsbergen at 78.9° N, 11.9° E (operated by the Alfred Wegener Institute for Polar and Marine Research – AWI and the Institut polaire français Paul-Emile Victor – IPEV), supported the airborne campaign. This included lidar data from the Koldewey Aerosol Raman Lidar (KARL) and the Micro Pulse Lidar (MPL), located in the atmospheric observatory as well as photometer data and the daily launched radiosonde. The MPL features nearly continuous measurements; the KARL was switched on whenever weather conditions allowed observations (145 h in 61 days). From 1 March to 30 April, 71 meteorological balloon soundings were performed and compared with the concurrent MPL measurements; photometer measurements are available from 18 March. For the KARL data, a statistical overview of particle detection based on their optical properties backscatter ratio and volume depolarization can be given. The altitudes of the occurrence of the named features (subvisible and visible ice and water as well as mixed-phase clouds, aerosol layers) as well as their dependence on different air mass origins are analyzed. Although the spring 2007 was characterized by rather clean conditions, diverse case studies of cloud and aerosol occurrence during March and April 2007 are presented in more detail, including temporal development and main optical properties as depolarization, backscatter and extinction coefficients. Links between air mass origins and optical properties can be presumed but need further evidence.
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This comment focuses on the statistical limitations of a model grading, as applied by D. Waugh and V. Eyring (2008) (WE08). The grade <i>g</i> is calculated for a specific diagnostic, which basically relates the difference of means of model and observational data to the standard deviation in the observational dataset. We performed Monte Carlo simulations, which show that this method has the potential to lead to large 95%-confidence intervals for the grade. Moreover, the difference between two model grades often has to be very large to become statistically significant. Since the confidence intervals were not considered in detail for all diagnostics, the grading in WE08 cannot be interpreted, without further analysis. The results of the statistical tests performed in WE08 agree with our findings. However, most of those tests are based on special cases, which implicitely assume that observations are available without any errors and that the interannual variability of the observational data and the model data are equal. Without these assumptions, the 95%-confidence intervals become even larger. Hence, the case, where we assumed perfect observations (ignored errors), provides a good estimate for an upper boundary of the threshold, below that a grade becomes statistically significant. Examples have shown that the 95%-confidence interval may even span the whole grading interval [0, 1]. Without considering confidence intervals, the grades presented in WE08 do not allow to decide whether a model result significantly deviates from reality. Neither in WE08 nor in our comment it is pointed out, which of the grades presented in WE08 inhibits such kind of significant deviation. However, our analysis of the grading method demonstrates the unacceptably high potential for these grades to be insignificant. This implies that the grades given by WE08 can not be interpreted by the reader. We further show that the inclusion of confidence intervals into the grading approach is necessary, since otherwise even a perfect model may get a low grade.
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Rapid Asian economic development might engender secondary impacts of atmospheric aerosol particles over the western Pacific after conversion of gaseous pollutants such as SO<sub>2</sub>. To elucidate changes in aerosol concentrations in leeward areas undergoing remarkable industrialization, the number-size distributions of submicrometer (0.3–1.0 μm) aerosols were measured at Murododaira (36.6° N, 137.6° E, 2450 m a.s.l.) on the western flank of Mount Tateyama in central Japan during January 1999–February 2009. Nighttime data obtained from 2400 to 0500 were used to analyze free-tropospheric aerosol concentration. Monthly average volume concentrations were calculated for months with >50% daily data coverage. Volume concentrations of submicrometer aerosols were high in spring to early summer and low in winter. Significant increasing trends at 95% confidence levels were found for volume concentrations in winter–spring. Simulated monthly anthropogenic aerosol concentrations at Mt. Tateyama from results of regional aerosol modeling with emission inventory up to 2005 showed seasonal variation and winter–spring increasing trends similar to those of observed aerosol concentration. According to the model analyses, the contribution of anthropogenic aerosol concentrations derived from China was high during winter–spring (60–80% of total anthropogenic aerosols at Mt. Tateyama). This accords with the increasing trend observed for winter–spring. Because SO<sub>4</sub><sup>2−</sup> is the dominant component of total anthropogenic aerosols, these results suggest that increasing anthropogenic emissions, especially for SO<sub>2</sub>, in China, engender enhancement of submicrometer-diameter aerosols over Japan during winter–spring.
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A strengthening of the equatorward temperature gradient in the upper troposphere/lower stratosphere (UTLS), at subtropics and midlatitudes, is consistently reproduced in several modelling studies of the atmospheric response to the increase of greenhouse gas radiative forcing. Some of those studies suggest an increase of the baroclinicity in the UTLS region because of the enhanced meridional temperature gradient. <br><br> This study presents observational evidence of an increase of the baroclinic wave components of UTLS circulation (UTLS wave baroclinicity), during the second half of the 20th century. The evidence is given by significant positive trends in the energy of baroclinic normal modes of the NCEP/NCAR reanalysis, and significant positive trends in the UTLS eddy available potential energy of the NCEP/NCAR, ERA-40, NCEP-2 and JRA-25 reanalyses. Significant positive trends in the frequency of double tropopause events in radiosonde data are also interpreted as a manifestation of an increase of the UTLS wave baroclinicity.
