Search

The present work describes the implementation of the state of the art Cloud- J v7.3 photolysis rate calculation code in the EMEP MSC-W chemistry-transport model. Cloud- J calculates photolysis rates and accounts for cloud and aerosol optical properties at model run time, replacing the old system based on tabulated values. The performance of Cloud- J is evaluated against aerial photolysis rate observations made over the Pacific Ocean and against surface observations from three measurement sites in Europe. Numerical experiments are performed to investigate the sensitivity of the calculated photolysis rates to the spatial and temporal model resolution, input meteorology model, simulated ozone column, and cloud effect parameterization. These experiments indicate that the calculated photolysis rates are most sensitive to the choice of input meteorology model and cloud effect parameterization while also showing that surface ozone photolysis rates can vary by up to 20 % due to daily variations in total ozone column. Further analysis investigates the impact of Cloud- J on the oxidizing capacity of the troposphere, aerosol–photolysis interactions, and surface air quality predictions. Results find that the annual mean mass-weighted tropospheric hydroxyl concentration is increased by 26 %, while the photolytic impact of aerosols is mostly limited to large tropical biomass-burning regions. Overall, Cloud- J represents a major improvement over the tabulated system, leading to improved model performance for predicting carbon monoxide and daily maximum ozone surface concentrations. [ABSTRACT FROM AUTHOR]

Ground-based high resolution observations of downward longwave irradiance (DLI), surface air temperature, water vapour surface partial pressure and column amount, zenith sky infrared (IR) radiance in the atmospheric window, and all-sky camera images are regularly obtained at the Thule High Arctic Atmospheric Observatory (THAAO, 76.5°N, 68.8°W), North-West Greenland. The datasets for the years 2017 and 2018 have been used to assess the performance of different empirical formulas to infer clear sky DLI. An algorithm to identify clear sky observations has been developed, based on value, variability, and persistence of zenith sky IR radiance. Seventeen different formulas to estimate DLI have been tested against the THAAO dataset, using the originally determined coefficients. The formulas which combine information on total column water vapour and surface air temperature appear to perform better than others, with a mean bias with respect to the measured DLI smaller than 1 W/m² and a root mean squared error (RMSE) around 6 W/m². Some formulas, specifically developed for the Arctic, are found to produce poor statistical results; this is attributed partly to limitations in the originally used dataset, which does not cover a whole year, or is relative to very specific conditions (i.e., the ice sheet). The bias displays a significant improvement when the coefficients of the different formulas are calculated using the THAAO dataset. The presence of two full years of data allows the investigation of the inter-annual variability, and the use of different years for the determination of the coefficients and the evaluation of results. The smallest values of the bias and RMSE reach 0.1 W/m² and 5 W/m², respectively. Overall, best results are found for formulas which use both surface parameters and total water vapour column, and have been developed from global datasets. Conversely, formulas which express the atmospheric emissivity as a linear function of the logarithm of the column integrated water vapour appear to poorly reproduce the observations at THAAO. [ABSTRACT FROM AUTHOR]

The Arctic climate is influenced by the interaction of shortwave (SW) and longwave (LW) radiation with the atmosphere and the surface. The comprehensive evolution of the Surface Radiative Fluxes (SRF) on different time scales is of paramount importance to understanding the complex mechanisms governing the Arctic climate. However, only a few sites located in the Arctic region provide long-term time series of SRF allowing for capturing the seasonality of atmospheric and surface parameters and carrying out validation of satellite products and/or reanalyses. This paper presents the daily and monthly SRF record collected at the Thule High Arctic Atmospheric Observatory (THAAO, 76.5° N, 68.8° W), in North-Western Greenland. The downwelling components of the SW (DSI) and the LW (DLI) irradiances have been measured at THAAO since 2009, while the collection of the upwelling SW (USI) and LW (ULI) irradiance was started in 2016, together with additional measurements, such as e.g., meteorological parameters and column water vapour. The datasets of DSI (Meloni et al., 2022a; https://doi.org/10.13127/thaao/dsi), USI (Meloni et al., 2022b; https://doi.org/10.13127/thaao/usi), DLI (Meloni et al., 2022c; https://doi.org/10.13127/thaao/dli), ULI (Meloni et al., 2022d; https://doi.org/10.13127/thaao/uli), and near surface air temperature (Muscari et al., 2018; https://doi.org/10.13127/thaao/met), can be accessed through the THAAO web site (https://www.thuleatmos-it.it/data). DSI is absent (solar zenith angle=90°) from 29 October to 13 February, assuming maxima in June (monthly mean of 277.0 Wm-2), when it is about half of the total incoming irradiance. The USI maximum occurs in May (132.4 Wm-2) due to the combination of moderately high DSI values and high albedo. The shortwave surface albedo (A) assumes an average of 0.16 during summer, when the surface is free of snow. Differently, during months of snow-covered surface, when solar radiation allows estimating A, its values are greater than 0.6. A large interannual variability is observed in May and September, months characterized by rapidly changing surface conditions, which appear to be linked with air temperature anomalies. DLI and ULI maxima occur in July and August, and minima in February and March. ULI is always larger than DLI and shows a wider annual cycle. ULI is well described by a fourth-order polynomial fit to the air temperature (R²>0.99 for monthly data and R²>0.97 for daily data). The surface radiation budget (SRB) is positive from April to August, when absorption of solar radiation exceeds the infrared net cooling, with a maximum value of 153.2 Wm-2 in June. From November to February, during the polar night, the LW net flux varies between -34.5 and -43.0 Wm-2. In March and September, the negative LW net flux overcomes the positive SW contribution, producing a negative SRB. THAAO measurements show clear evidence of the influence of several regional weather/climate events, which appear strongly linked with SRF anomalies. These anomalies are found for example during summer 2012, when a large ice melting event took place over Greenland, and during winter 2019-2020, extraordinarily cold in the Arctic region. [ABSTRACT FROM AUTHOR]

Combined measurements of diffuse-to-global radiation ratio and global spectral irradiances in the UV are used to derive cosine-corrected UV irradiances and aerosol optical depth (AOD). The diffuse-to-global radiation ratio is used first in the cosine correction of the global irradiance, then to calculate absolutely calibrated direct irradiances. The Beer--Lambert law is applied to derive the UVAOD using independent measurements of the extraterrestrial solar flux. The AOD can be derived with an uncertainty of about 0.03 at 60[degrees] solar zenith angle. The method was applied to measurements obtained with two UV multi-filter rotating shadowband radiometers (UV-MFRSRs) and a MK III Brewer spectrophotometer on the Island of Lampedusa in the Central Mediterranean during two periods of 2002 and 2004. The derived AOD at 318 and 332 nm was compared with UV AOD measured at 318, 320, and 368 nm with different techniques. The retrieved AOD, combining MFRSR and Brewer measurements, is in good agreement with the optical depth derived with the other methods. OCIS codes: 010.1110, 010.5620, 120.0280, 120.6200.

This paper presents the results on simultaneous high time resolution measurements of biogenic aerosol (methane sulfonic acid-MSA, non-sea salt sulfate nssSO42-) with its gaseous precursor dimethylsulfide (DMS) performed at the Italian coastal base Mario Zucchelli Station (MZS) in Terra Nova Bay (MZS) during two summer campaigns (2018-2019 and 2019-2020). The study provides information on marine biological activity in the nearby polynya in the Ross Sea and on the influence of biogenic and atmospheric processes on biogenic aerosol formation. Data on atmospheric DMS concentration are scarce especially in Antarctica. The DMS-maximum at MZS occurs in December, one month earlier than at other Antarctic stations. The maximum of DMS concentration is connected with the phytoplanktonic senescent phase following the bloom of Phaeocystis antarctica that occurs in the polynya when sea ice opens up. The second plankton bloom occurs in January and, despite the high Dimethylsulfopropionate (DMSP) concentration in sea water, atmospheric DMS remains low probably due to its fast biological turnover in sea water in this period. The intensity and timing of the DMS evolution during the two years suggests that only the portion of the polynya close to the sampling site produces a discernible effect on the measured DMS. The closeness to the DMS source area, and the occurrence of air masses containing DMS and freshly formed oxidation products allow to study the kinetic of biogenic aerosol formation and the reliable derivation of the branch ratio between MSA and nssSO42- from DMS oxidation that is estimated to be 0.84 ±0.06. Conversely, for aged airmasses with low DMS content, an enrichment of nssSO42- with respect to MSA, due to the presence of background concentration of nssSO42-from volcanic origin (Erebus) or from long range transport, takes place. Therefore, the aged air mass presents an MSA/ nssSO42- ratio lower than in newly formed biogenic aerosol. By considering the sum of MSA and biogenic nssSO42-, we estimate that the mean contribution of biogenic particulate matter to PM10 is 17%, with a maximum of 56%. The high contribution of biogenic aerosol to the total PM10 mass in summer in this area highlights the dominant role of the polynya on biogenic aerosol formation. Finally, due to the regional and year-to year variability of DMS and related biogenic aerosol formation, we stress the need of long-term measurements of atmospheric DMS and biogenic aerosol along the Antarctic coast and in the Southern Ocean. [ABSTRACT FROM AUTHOR]

With a Brewer spectrophotometer, an estimation of total ozone is made from relative measurements of. direct-sun ultraviolet radiation at six wavelengths from 300 to 320 nm. During normal operations, one of six neutral-density filters is selected automatically to maintain the detector in its linear response range. On the basis of these standard direct-sun observations, estimates of aerosol optical depth can be derived, provided that a calibration of the relative measurements is available for each neutral-density filter. To obtain the calibration, we implemented a routine to measure direct-sun signals with a fixed neutral-density filter and applied the Langley method to the measured photon counts. Results show that if a sufficiently large number of cloud-free mornings or afternoons is available, a reliable calibration can be achieved even at sea-level sites that are characterized by large aerosol variability. The derived aerosol optical depths appear consistent with those measured independently by a multifilter rotating shadow-band radiometer. Existing relatively long-term series of direct-sun ozone measurements by Brewer instruments may be used for retrieval of aerosol optical depth. OCIS codes: 010.1110, 280.0280.