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Advection of Biomass Burning Aerosols towards the Southern Hemispheric Mid-Latitude Station of Punta Arenas as Observed with Multiwavelength Polarization Raman Lidar
In this paper, we present long-term observations of the multiwavelength Raman lidar PollyXT conducted in the framework of the DACAPO-PESO campaign. Regardless of the relatively clean atmosphere in the southern mid-latitude oceans region, we regularly observed events of long-range transported smoke, originating either from regional sources in South America or from Australia. Two case studies will be discussed, both identified as smoke events that occurred on 5 February 2019 and 11 March 2019. For the first case considered, the lofted smoke layer was located at an altitude between 1.0 and 4.2 km, and apart from the predominance of smoke particles, particle linear depolarization values indicated the presence of dust particles. Mean lidar ratio values at 355 and 532 nm were 49 ± 12 and 24 ± 18 sr respectively, while the mean particle linear depolarization was 7.6 ± 3.6% at 532 nm. The advection of smoke and dust particles above Punta Arenas affected significantly the available cloud condensation nuclei (CCN) and ice nucleating particles (INP) in the lower troposphere, and effectively triggered the ice crystal formation processes. Regarding the second case, the thin smoke layers were observed at altitudes 5.5–7.0, 9.0 and 11.0 km. The particle linear depolarization ratio at 532 nm increased rapidly with height, starting from 2% for the lowest two layers and increasing up to 9.5% for the highest layer, indicating the possible presence of non-spherical coated soot aggregates. INP activation was effectively facilitated. The long-term analysis of the one year of observations showed that tropospheric smoke advection over Punta Arenas occurred 16 times (lasting from 1 to 17 h), regularly distributed over the period and with high potential to influence cloud formation in the otherwise pristine environment of the region.
A new Lagrangian in-time particle simulation module (Itpas v1) for atmospheric particle dispersion
Trajectory models are intuitive tools for airflow studies. But in general, they are limited to non-turbulent, i.e. laminar flow, conditions. Therefore, trajectory models are not particularly suitable for investigating airflow within the turbulent atmospheric boundary layer. To overcome this, a common approach is handling the turbulent uncertainty as a random deviation from a mean path in order to create a statistic of possible solutions which envelops the mean path. This is well known as the Lagrangian particle dispersion model (LPDM). However, the decisive factor is the representation of turbulence in the model, for which widely used models such as FLEXPART and HYSPLIT use an approximation. A conceivable improvement could be the use of a turbulence parameterisation approach based on the turbulent kinetic energy (TKE) at high temporal resolution. Here, we elaborated this approach and developed the LPDM Itpas, which is coupled online to the German Weather Service's mesoscale weather forecast model COSMO. It benefits from the prognostically calculated TKE as well as from the high-frequency wind information. We demonstrate the model's applicability for a case study on agricultural particle emission in eastern Germany. The results obtained are discussed with regard to the model's ability to describe particle transport within a turbulent boundary layer. Ultimately, the simulations performed suggest that the newly introduced method based on prognostic TKE sufficiently represents the particle transport.
ICONGETM v1.0 – flexible NUOPC-driven two-way coupling via ESMF exchange grids between the unstructured-grid atmosphere model ICON and the structured-grid coastal ocean model GETM
Two-way model coupling is important for representing the mutual interactions and feedbacks between atmosphere and ocean dynamics. This work presents the development of the two-way coupled model system ICONGETM, consisting of the atmosphere model ICON and the ocean model GETM. ICONGETM is built on the latest NUOPC coupling software with flexible data exchange and conservative interpolation via ESMF exchange grids. With ICON providing a state-of-the-art kernel for numerical weather prediction on an unstructured mesh and GETM being an established coastal ocean model, ICONGETM is especially suited for high-resolution studies. For demonstration purposes the newly developed model system has been applied to a coastal upwelling scenario in the central Baltic Sea.
The global aerosol-climate model echam6.3-ham2.3 -Part 1: Aerosol evaluation
We introduce and evaluate aerosol simulations with the global aerosol-climate model ECHAM6.3-HAM2.3, which is the aerosol component of the fully coupled aerosol-chemistry-climate model ECHAM-HAMMOZ. Both the host atmospheric climate model ECHAM6.3 and the aerosol model HAM2.3 were updated from previous versions. The updated version of the HAM aerosol model contains improved parameterizations of aerosol processes such as cloud activation, as well as updated emission fields for anthropogenic aerosol species and modifications in the online computation of sea salt and mineral dust aerosol emissions. Aerosol results from nudged and free-running simulations for the 10-year period 2003 to 2012 are compared to various measurements of aerosol properties. While there are regional deviations between the model and observations, the model performs well overall in terms of aerosol optical thickness, but may underestimate coarse-mode aerosol concentrations to some extent so that the modeled particles are smaller than indicated by the observations. Sulfate aerosol measurements in the US and Europe are reproduced well by the model, while carbonaceous aerosol species are biased low. Both mineral dust and sea salt aerosol concentrations are improved compared to previous versions of ECHAM-HAM. The evaluation of the simulated aerosol distributions serves as a basis for the suitability of the model for simulating aerosol-climate interactions in a changing climate.
A protocol for quantifying mono- and polysaccharides in seawater and related saline matrices by electro-dialysis (ED) – combined with HPAEC-PAD
An optimized method is presented to determine dissolved free (DFCHO) and dissolved combined carbohydrates (DCCHO) in saline matrices, such as oceanic seawater, Arctic ice core samples or brine using a combination of a desalination with electro-dialysis (ED) and high-performance anion exchange chromatography coupled to pulsed amperometric detection (HPAEC-PAD). Free neutral sugars, such as glucose and galactose, were found with 95 %–98 % recovery rates. Free amino sugars and free uronic acids were strongly depleted during ED at pH=8, but an adjustment of the pH could result in higher recoveries (58 %–59 % for amino sugars at pH=11; 45 %–49 % for uronic acids at pH=1.5). The applicability of this method for the analysis of DCCHO was evaluated with standard solutions and seawater samples compared with another established desalination method using membrane dialysis. DFCHO in field samples from different regions on Earth ranged between 11 and 118 nM and DCCHO between 260 and 1410 nM. This novel method has the potential to contribute to a better understanding of biogeochemical processes in the oceans and sea–air transfer processes of organic matter into the atmosphere in future studies.
On the application and grid-size sensitivity of the urban dispersion model CAIRDIO v2.0 under real city weather conditions
There is a gap between the need for city-wide air-quality simulations considering the intra-urban variability and mircoscale dispersion features and the computational capacities that conventional urban microscale models require. This gap can be bridged by targeting model applications on the gray zone situated between the mesoscale and large-eddy scale. The urban dispersion model CAIRDIO is a new contribution to the class of computational-fluid dynamics models operating in this scale range. It uses a diffuse-obstacle boundary method to represent buildings as physical obstacles at gray-zone resolutions in the order of tens of meters. The main objective of this approach is to find an acceptable compromise between computationally inexpensive grid sizes for spatially comprehensive applications and the required accuracy in the description of building and boundary-layer effects. In this paper, CAIRDIO is applied on the simulation of black carbon and particulate matter dispersion for an entire mid-size city using a uniform horizontal grid spacing of 40gm. For model evaluation, measurements from five operational air monitoring stations representative for the urban background and high-traffic roads are used. The comparison also includes the mesoscale host simulation, which provides the boundary conditions. The measurements show a dominant influence of the mixing layer evolution at background sites, and therefore both the mesoscale and large-eddy simulation (LES) results are in good agreement with the observed air pollution levels. In contrast, at the high-traffic sites the proximity to emissions and the interactions with the building environment lead to a significantly amplified diurnal variability in pollutant concentrations. These urban road conditions can only be reasonably well represented by CAIRDIO while the meosocale simulation indiscriminately reproduces a typical urban-background profile, resulting in a large positive model bias. Remaining model discrepancies are further addressed by a grid-spacing sensitivity study using offline-nested refined domains. The results show that modeled peak concentrations within street canyons can be further improved by decreasing the horizontal grid spacing down to 10gm, but not beyond. Obviously, the default grid spacing of 40gm is too coarse to represent the specific environment within narrow street canyons. The accuracy gains from the grid refinements are still only modest compared to the remaining model error, which to a large extent can be attributed to uncertainties in the emissions. Finally, the study shows that the proposed gray-scale modeling is a promising downscaling approach for urban air-quality applications. The results, however, also show that aspects other than the actual resolution of flow patterns and numerical effects can determine the simulations at the urban microscale.