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Daily NO<sub>2</sub> vertical column density (VCD) has been routinely measured by zenith sky spectroscopy at the subtropical station of Izaña (28° N, 16° W) since 1993 in the framework of the Network for the Detection of Atmospheric Composition Change (NDACC). Based on 14 years of data the first low latitude NO<sub>2</sub> VCD climatology has been established and the main characteristics from short timescales of one day to interannual variability are presented. Instrumental descriptions and different sources of errors are described in detail. The observed diurnal cycle follows that expected by gas-phase NO<sub>x</sub> chemistry, as can be shown by the good agreement with a vertically integrated chemical box model, and is modulated by solar radiation. The seasonal evolution departs from the phase of the hours of daylight, indicating the signature of upper stratospheric temperature changes. From the data record (1993–2006) no significant long-term trends in NO<sub>2</sub> VCD can be inferred. Comparison of the ground-based data sets with nadir-viewing satellite spectrometers shows excellent agreement for SCIAMACHY with differences between both datasets of 1.1%. GOME displays unrealistic features with the largest discrepancies during summer. The ground-based data are compared with long-term output of the SLIMCAT 3-D chemical transport model (CTM). The basic model, forced by ECMWF (ERA-40) analyses, captures the observed NO<sub>2</sub> annual cycle but significantly underestimates the spring/summer maximum (by 12% at sunset and up to 25% at sunrise). In a model run which uses assimilation of satellite CH<sub>4</sub> profiles to constrain the model long-lived tracers the agreement is significantly improved. This improvement in modelled column NO<sub>2</sub> is due to better modelled NO<sub>y</sub> profiles and points to transport errors in the ECMWF ERA-40 reanalyses.
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Subvisible cirrus (SVC) clouds are often observed within the tropical tropopause layer (TTL). Some studies suggest that SVC has a significant impact on the earth radiation budget. The Costa Rica Aura Validation Experiment (CR-AVE) sponsored by the National Aeronautics and Space Administration (NASA) took place near San Jose, Costa Rica from 14 January–15 February 2006. The NASA WB-57F sampled SVC in the TTL from −75°C to −90°C with an improved set of cloud particle probes. The first digital images of ice particles in the TTL are compared with replicator images of ice particles collected in 1973 by a WB-57F in the TTL. The newer measurements reveal larger particles, on the order of 100 μm compared with <50 μm from the earlier measurements, and also different particle shapes. The 1973 particles were mainly columnar and trigonal, whereas the newer measurements are quasi-spherical and hexagonal plates. The WB-57F also measured very high water vapor contents with some instruments, up to 4 ppmv, and aerosols with mixed organics and sulfates. It is unknown whether these ambient conditions were present in the 1973 studies, and whether such conditions have an influence on particle shape and the development of the large particles. A companion paper (Jensen et al., 2008) presents crystal growth calculations that suggest that the high water vapor measurements are required to grow ice particles to the observed sizes of 100 μm and larger.
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The implementation of processes related to chemistry into Earth System Models and their coupling within such systems requires the consistent description of the chemical species involved. We provide a tool (written in Fortran95) to structure and manage information about constituents, hereinafter referred to as tracers, namely the Modular Earth Submodel System (MESSy) generic (i.e., infrastructure) submodel TRACER. With TRACER it is possible to define a multitude of tracer sets, depending on the spatio-temporal representation (i.e., the grid structure) of the model. The required information about a specific chemical species is split into the static meta-information about the characteristics of the species, and its (generally in time and space variable) abundance in the corresponding representation. TRACER moreover includes two submodels. One is TRACER_FAMILY, an implementation of the tracer family concept. It distinguishes between two types: type-1 families are usually applied to handle strongly related tracers (e.g., fast equilibrating species) for a specific process (e.g., advection). In contrast to this, type-2 families are applied for tagging techniques. Tagging means the artificial decomposition of one or more species into parts, which are additionally labelled (e.g., by the region of their primary emission) and then processed as the species itself. The type-2 family concept is designed to conserve the linear relationship between the family and its members. The second submodel is TRACER_PDEF, which corrects and budgets numerical negative overshoots that arise in many process implementations due to the numerical limitations (e.g., rounding errors). The submodel therefore guarantees the positive definiteness of the tracers and stabilises the integration scheme. As a by-product, it further provides a global tracer mass diagnostic. Last but not least, we present the submodel PTRAC, which allows the definition of tracers via a Fortran95 namelist, as a complement to the standard tracer definition by application of the TRACER interface routines in the code. TRACER with its submodels and PTRAC can readily be applied to a variety of models without further requirements. The code and a documentation are included in the electronic supplement.
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We present a "nudged" version of the Met Office general circulation model, the Unified Model. We constrain this global climate model using ERA-40 re-analysis data with the aim of reproducing the observed "weather" over a year from September 1999. Quantitative assessments are made of its performance, focusing on dynamical aspects of nudging and demonstrating that the "weather" is well simulated.
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During the European heat wave summer 2003 with predominant high pressure conditions we performed a detailed study of upper tropospheric humidity and ice particles which yielded striking results concerning the occurrence of ice supersaturated regions (ISSR), cirrus, and contrails. Our study is based on lidar observations and meteorological data obtained at Lindenberg/Germany (52.2° N, 14.1° E) as well as the analysis of the European centre for medium range weather forecast (ECMWF). Cirrus clouds were detected in 55% of the lidar profiles and a large fraction of them were subvisible (optical depth <0.03). Thin ice clouds were particularly ubiquitous in high pressure systems. The radiosonde data showed that the upper troposphere was very often supersaturated with respect to ice. Relating the radiosonde profiles to concurrent lidar observations reveals that the ISSRs almost always contained ice particles. Persistent contrails observed with a camera were frequently embedded in these thin or subvisible cirrus clouds. The ECMWF cloud parametrisation reproduces the observed cirrus clouds consistently and a close correlation between the ice water path in the model and the measured optical depth of cirrus is demonstrated.
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A new formulation for the turbulence dissipation rate ε occurring in meandering conditions has been presented. The derivation consists of a MacLaurin series expansion of a lateral dispersion parameter that represents cases in which turbulence and oscillatory movements associated to the meandering events coexist. The new formulation presents the identical physical premises contained in the classical and largely used one, but the new formulation derived from meandering situations is expressed in terms of the loop parameter <I>m</I> that controls the absolute value of the negative lobe in the meandering autocorrelation function. Therefore, the <I>m</I> magnitude regulates the turbulence dissipation rate. This dissipation rate decreases for cases in which turbulence and low frequency horizontal wind oscillations coexist and increases for a fully developed turbulence. Furthermore, a statistical comparison to observed concentration data shows that the alternative relation for the turbulent dissipation rate occurring in situations of meandering enhanced dispersion is suitable for applications in Lagrangian Stochastic dispersion models.
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Several short-lived pollutants known to impact Arctic climate may be contributing to the accelerated rates of warming observed in this region relative to the global annually averaged temperature increase. Here, we present a summary of the short-lived pollutants that impact Arctic climate including methane, tropospheric ozone, and tropospheric aerosols. For each pollutant, we provide a description of the major sources and the mechanism of forcing. We also provide the first seasonally averaged forcing and corresponding temperature response estimates focused specifically on the Arctic. The calculations indicate that the forcings due to black carbon, methane, and tropospheric ozone lead to a positive surface temperature response indicating the need to reduce emissions of these species within and outside the Arctic. Additional aerosol species may also lead to surface warming if the aerosol is coincident with thin, low lying clouds. We suggest strategies for reducing the warming based on current knowledge and discuss directions for future research to address the large remaining uncertainties.
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Volatile organic compound concentration ratios can be used as indicators of halogen chemistry that occurs during ozone depletion events in the Arctic during spring. Here we use a combination of modeling and measurements of [acetone]/[propanal] as an indicator of bromine chemistry, and [isobutane]/[n-butane] and [methyl ethyl ketone]/[n-butane] are used to study the extent of chlorine chemistry during four ozone depletion events during the Polar Sunrise Experiment of 1995. Using a 0-D photochemistry model in which the input of halogen atoms is controlled and varied, the approximate ratio of [Br]/[Cl] can be estimated for each ozone depletion event. It is concluded that there must be an additional source of propanal (likely from the snowpack) to correctly simulate the VOC chemistry of the Arctic, and further evidence that the ratio of Br atoms to Cl atoms can vary greatly during ozone depletion events is presented.
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In this study, we measure the extinction efficiency at 532 nm of absorbing aerosol particles coated with a non-absorbing solid and liquid organic shell with coating thickness varying between 5 and 100 nm using cavity ring down aerosol spectrometry. For this purpose, we use nigrosin, an organic black dye, as a model absorbing core and two non-absorbing organic substances as shells, glutaric acid (GA) and Di-Ethyl-Hexyl-Sebacate (DEHS). The measured behavior of the coated particles is consistent with Mie calculations of core-shell particles. Errors between measured and calculated values for nigrosin coated with GA and DEHS are between 0.5% and 10.5% and between 0.5% and 9%, respectively. However, it is evident that the calculations are in better agreement with the measured results for thinner coatings. Possible reasons for these discrepancies are discussed.
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Trace gas measurements of TOPSE and TRACE-P experiments and corresponding global GEOS-Chem model simulations are analyzed with the Positive Matrix Factorization (PMF) method for model evaluation purposes. Specially, we evaluate the model simulated contributions to O<sub>3</sub> variability from stratospheric transport, intercontinental transport, and production from urban/industry and biomass burning/biogenic sources. We select a suite of relatively long-lived tracers, including 7 chemicals (O<sub>3</sub>, NO<sub>y</sub>, PAN, CO, C<sub>3</sub>H<sub>8</sub>, CH<sub>3</sub>Cl, and <sup>7</sup>Be) and 1 dynamic tracer (potential temperature). The largest discrepancy is found in the stratospheric contribution to <sup>7</sup>Be. The model underestimates this contribution by a factor of 2–3, corresponding well to a reduction of <sup>7</sup>Be source by the same magnitude in the default setup of the standard GEOS-Chem model. In contrast, we find that the simulated O<sub>3</sub> contributions from stratospheric transport are in reasonable agreement with those derived from the measurements. However, the springtime increasing trend over North America derived from the measurements are largely underestimated in the model, indicating that the magnitude of simulated stratospheric O<sub>3</sub> source is reasonable but the temporal distribution needs improvement. The simulated O<sub>3</sub> contributions from long-range transport and production from urban/industry and biomass burning/biogenic emissions are also in reasonable agreement with those derived from the measurements, although significant discrepancies are found for some regions.
