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The climate-chemistry-aerosol-cloud-radiation feedbacks are important processes occurring in the atmosphere. Accurately simulating those feedbacks requires fully-coupled meteorology, climate, and chemistry models and presents significant challenges in terms of both scientific understanding and computational demand. This paper reviews the history and current status of the development and application of online-coupled meteorology and chemistry models, with a focus on five representative models developed in the US including GATOR-GCMOM, WRF/Chem, CAM3, MIRAGE, and Caltech unified GCM. These models represent the current status and/or the state-of-the science treatments of online-coupled models worldwide. Their major model features, typical applications, and physical/chemical treatments are compared with a focus on model treatments of aerosol and cloud microphysics and aerosol-cloud interactions. Aerosol feedbacks to planetary boundary layer meteorology and aerosol indirect effects are illustrated with case studies for some of these models. Future research needs for model development, improvement, application, as well as major challenges for online-coupled models are discussed.
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We measured the number concentrations of cloud condensation nuclei (CCN) and the size distributions of CCN/CN (CN: condensation nuclei) ratios at supersaturations (<i>SS</i>s) of 0.097, 0.27, 0.58, and 0.97% at Jeju Island, Korea during March-April 2005. We made simultaneous measurements of aerosol inorganic ions, water-soluble organic carbon (WSOC), organic carbon (OC), and elemental carbon (EC) in PM<sub>2.5</sub>. The CCN/CN ratios increased with increasing particle diameter, and the diameter at CCN/CN=0.5 was defined as <i>D</i><sub>50</sub>. <i>D</i><sub>50</sub> represents the activation dry diameter of atmospheric particles. The average <i>D</i><sub>50</sub> at <i>SS</i>=0.097% and 0.97% was 136±17 nm and 31±3 nm, respectively. The temporal variation of <i>D</i><sub>50</sub> at <i>SS</i>=0.097% was correlated with the mass fraction of water-soluble components (inorganic ions + WSOC), indicating that the temporal variation of CCN activity was mainly controlled by changes in the water-soluble components fraction. The critical dry diameter (<i>D</i><sub>crit</sub>), which is the threshold dry diameter for CCN activation, was calculated from the observed aerosol chemical compositions by Köhler theory for comparison with <i>D</i><sub>50</sub>. The <i>D</i><sub>50</sub> at <i>SS</i>=0.097% was correlated (<i>r</i><sup>2</sup>=0.48) with calculated <i>D</i><sub>crit</sub>, although <i>D</i><sub>crit</sub> was larger than <i>D</i><sub>50</sub> by 20–29% on average. The systematic difference between <i>D</i><sub>50</sub> and <i>D</i><sub>crit</sub> could be caused by the size dependence of the aerosol chemical compositions or surface tension lowering caused by the mixing of water-soluble organic compounds. This difference corresponds to a 27±14% uncertainty in the CCN number concentration estimated from the observed particle number size distribution.
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The LYRA instrument onboard ESA PROBA2 satellite will provide 6-hourly solar irradiance at the Lyman-alpha (121.6 nm) and the Herzberg continuum (~200–220 nm wavelength range). Because the nowcasting of the neutral and ionic state of the middle atmosphere requires the solar irradiance for the wide spectral range (120–680 nm) we have developed the statistical tool for the reconstruction of the full spectrum from the LYRA measurements. The accuracy of the reconstructed irradiance has been evaluated with 1-D transient radiative-convective model with neutral and ion chemistry using the daily solar spectral irradiance measured with SUSIM and SOLSTICE instruments onboard UARS satellite. We compared the results of transient 1-year long model simulations for 2000 driven by the observed and reconstructed solar irradiance and showed that the reconstruction of the full spectrum using linear regression equation based on the solar irradiance in two LYRA channels can be successfully used for nowcasting of the middle atmosphere. We have also identified conditions when the proposed approach does not yield spectral reconstruction with sufficient accuracy.
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Prognostic equations for the rain mass mixing ratio and the rain drop number concentration are introduced into the large-scale cloud microphysics parameterization of the ECHAM5 general circulation model (ECHAM5-PROG). To this end, a rain flux from one level to the next with the appropriate fall speed is introduced. This maintains rain water in the atmosphere to be available for the next time step. Rain formation in ECHAM5-PROG is, therefore, less dependent on the autoconversion rate than the standard ECHAM5 but shifts the emphasis towards the accretion rates in accordance with observations. ECHAM5-PROG is tested and evaluated with Single Column Model (SCM) simulations for two cases: the marine stratocumulus study EPIC (October 2001) and the continental mid-latitude ARM Cloud IOP (shallow frontal cloud case – March 2000). In case of heavy precipitation events, the prognostic equations for rain hardly affect the amount and timing of precipitation at the surface in different SCM simulations because heavy rain depends mainly on the large-scale forcing. In case of thin, drizzling clouds (i.e., stratocumulus), surface precipitation is sensitive to the number of sub-time steps used in the prognostic rain scheme. Cloud microphysical quantities, such as cloud liquid and rain water within the atmosphere, are sensitive to the number of sub-time steps in both considered cases. This results from the decreasing autoconversion rate and increasing accretion rate.
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We interpret a suite of satellite, aircraft, and ground-based measurements over the North Pacific Ocean and western North America during April–May 2006 as part of the Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign to understand the implications of long-range transport of East Asian emissions to North America. The Canadian component of INTEX-B included 33 vertical profiles from a Cessna 207 aircraft equipped with an aerosol mass spectrometer. Long-range transport of organic aerosols was insignificant, contrary to expectations. Measured sulfate plumes in the free troposphere over British Columbia exceeded 2 μg/m<sup>3</sup>. We update the global anthropogenic emission inventory in a chemical transport model (GEOS-Chem) and use it to interpret the observations. Aerosol Optical Depth (AOD) retrieved from two satellite instruments (MISR and MODIS) for 2000–2006 are analyzed with GEOS-Chem to estimate an annual growth in Chinese sulfur emissions of 6.2% and 9.6%, respectively. Analysis of aircraft sulfate measurements from the NASA DC-8 over the central Pacific, the NSF C-130 over the east Pacific and the Cessna over British Columbia indicates most Asian sulfate over the ocean is in the lower free troposphere (800–600 hPa), with a decrease in pressure toward land due to orographic effects. We calculate that 56% of the measured sulfate between 500–900 hPa over British Columbia is due to East Asian sources. We find evidence of a 72–85% increase in the relative contribution of East Asian sulfate to the total burden in spring off the northwest coast of the United States since 1985. Campaign-average simulations indicate anthropogenic East Asian sulfur emissions increase mean springtime sulfate in Western Canada at the surface by 0.31 μg/m<sup>3</sup> (~30%) and account for 50% of the overall regional sulfate burden between 1 and 5 km. Mean measured daily surface sulfate concentrations taken in the Vancouver area increase by 0.32 μg/m<sup>3</sup> per 10% increase in the simulated fraction of Asian sulfate, and suggest current East Asian emissions episodically degrade local air quality by more than 1.5 μg/m<sup>3</sup>.
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An Ensemble Kalman Filter (EnKF) data assimilation system was developed for a regional dust transport model. This paper applied the EnKF method to investigate modeling of severe dust storm episodes occurring in March 2002 over China based on surface observations of dust concentrations to explore the impact of the EnKF data assimilation systems on forecast improvement. A series of sensitivity experiments using our system demonstrates the ability of the advanced EnKF assimilation method using surface observed PM<sub>10</sub> in North China to correct initial conditions, which leads to improved forecasts of dust storms. However, large errors in the forecast may arise from model errors (uncertainties in meteorological fields, dust emissions, dry deposition velocity, etc.). This result illustrates that the EnKF requires identification and correction model errors during the assimilation procedure in order to significantly improve forecasts. Results also show that the EnKF should use a large inflation parameter to obtain better model performance and forecast potential. Furthermore, the ensemble perturbations generated at the initial time should include enough ensemble spreads to represent the background error after several assimilation cycles.
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Long-term measurements of erythemally weighted UV irradiance (Q<sub><i>er</i></sub>) have been analyzed for the 1999–2006 period as well as UV variability according to a reconstruction model since 1968. The estimates of different atmospheric parameters effects, including NO<sub>2</sub> content, on Q<sub><i>er</i></sub> have been obtained on seasonal and interannual scales. It has been shown that NO<sub>2</sub> content in conditions of large megalopolis provides average Q<sub><i>er</i></sub> decrease of about 1.5–2%. The seasonal variations of the observed UV indices are discussed from the point of view of the impact on health. Using the reconstruction model we showed a distinct growth in Q<sub><i>er</i></sub> since 1980 due to changes in total ozone (+2.5% per decade), effective cloud amount transmission (+2.1% per decade) and aerosol loading (+1.1% per decade). However, there is no change in Q<sub><i>er</i></sub> over the longer 1968–2006 period due to significant decrease in effective cloud amount transmission (−11% per decade) in 1968–1980.
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Erythemaly weighted UV and total UV-A irradiance measured at the ALOMAR (Arctic Lidar Observatory for Middle Atmosphere Research; 69° N, 16° E) in June 2007 by two Kipp & Zonen UV broadband meters type, UV-S-EA-T, are examined. One unit is mounted on rotating vertical plane and the other is permanently fixed horizontally. The UV broadband meters measure simultaneously to compare UV irradiances on vertical and horizontal planes. The entire range of such relative exposure variations during clear-sky and overcast conditions over ALOMAR in the period March–June 2007 is examined using STAR and Radonic1 model (developed at the Meteorological Institute, University of Munich) for various action spectra: erythema, UV-A, and vitamin D<sub>3</sub>. The model and observations support that the daily means of relative exposures are quite stable, i.e., vary within the range 0.4–0.6 with the mean around 0.5 when the averaged intra-day, day-to-day, and seasonal changes of the relative erythemal exposures are considered. It seems that multiplication of the daily mean dose from a broadband meter placed horizontally by the factor of 0.5 gives reasonable estimation of the daily mean exposure on a vertically oriented receiver randomly oriented towards the Sun. The model studies during clear-sky conditions show that the extreme value and daily variability of relative exposure are the highest for UV-A, next for erythemal UV, then for vitamin D<sub>3</sub> weighed UV irradiance. The minima of relative exposure (~0.20–0.30) are almost the same for all weighting functions. The comparison of model simulations and measurements suggests that specific cloud configuration could lead to significant enhancement of UV exposure of rotating receiver.
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Recent aircraft studies showed that new particle formation (NPF) is very active in the free troposphere. And, these observations lead to a new question: when does NPF <i>not</i> occur? Here, we provide case studies to show how different meteorological parameters affect NPF in the upper troposphere, using the aerosol size distributions measured at latitudes from 18° N–52° N and altitudes up to 14 km during the NSF/NCAR GV Progressive Science Missions. About 95% of the total samples showed the NPF feature with median number concentrations of particles with diameters from 4 to 9 nm (<i>N</i><sub>4–9</sub>), 288±199 cm<sup>−3</sup>, and the total particle number concentrations with diameters from 4 to 2000 nm (<i>N</i><sub>4–2000</sub>), 500±259 cm<sup>−3</sup>. Surface areas were in general very low in the free troposphere, 1.58±0.87 μm<sup>2</sup> cm<sup>−3</sup>, which in part explains the high frequency of NPF measured in this region, but there was no distinctive difference in surface area for the NPF and non-NPF cases. Our case studies show that rather airmass history is more important for nucleation in this region. Weak- or non-events did not display uplifting of airmasses. On the other hand, strong NPF events were usually associated with uplifting of airmasses, although there were also NPF cases in which uplift did not occur, consistent with the previous observations (Young et al., 2007). NPF tends to easily occur in the free troposphere because of low surface areas and low temperatures (Carslaw and Kärcher, 2006), but because of the low aerosol precursors in this region, vertical motion (that can bring higher concentrations of aerosol precursors from low altitude source regions to higher altitudes) can play a critical role. Latitude dependence of new particles also shows higher particle concentrations in the midlatitude and subtropics tropopause region than in the tropics, consistent with Hermann et al. (2003).
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Non-linear maximum a posteriori (MAP) estimates of atmospheric profiles from the Tropospheric Emission Spectrometer (TES) contains a priori information that may vary geographically, which is a confounding factor in the analysis and physical interpretation of an ensemble of profiles. One mitigation strategy is to transform profile estimates to a common prior using a linear operation thereby facilitating the interpretation of profile variability. However, this operation is dependent on the assumption of not worse than moderate non-linearity near the solution of the non-linear estimate. The robustness of this assumption is tested by comparing atmospheric retrievals from the Tropospheric Emission Spectrometer processed with a uniform prior with those processed with a variable prior and converted to a uniform prior following the non-linear retrieval. Linearly converting the prior following a non-linear retrieval is shown to have a minor effect on the results as compared to a non-linear retrieval using a uniform prior when compared to the expected total error, with less than 10% of the change in the prior ending up as unbiased fluctuations in the profile estimate results.
