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Retrieving high-resolution surface solar radiation with cloud parameters derived by combining MODIS and MTSAT data

Cloud parameters (cloud mask, effective particle radius, and liquid/ice water path) are the important inputs in estimating surface solar radiation (SSR). These parameters can be derived from MODIS with high accuracy, but their temporal resolution is too low to obtain high-temporal-resolution SSR retrievals. In order to obtain hourly cloud parameters, an artificial neural network (ANN) is applied in this study to directly construct a functional relationship between MODIS cloud products and Multifunctional Transport Satellite (MTSAT) geostationary satellite signals. In addition, an efficient parameterization model for SSR retrieval is introduced and, when driven with MODIS atmospheric and land products, its root mean square error (RMSE) is about 100 W m−2 for 44 Baseline Surface Radiation Network (BSRN) stations. Once the estimated cloud parameters and other information (such as aerosol, precipitable water, ozone) are input to the model, we can derive SSR at high spatiotemporal resolution. The retrieved SSR is first evaluated against hourly radiation data at three experimental stations in the Haihe River basin of China. The mean bias error (MBE) and RMSE in hourly SSR estimate are 12.0 W m−2 (or 3.5 %) and 98.5 W m−2 (or 28.9 %), respectively. The retrieved SSR is also evaluated against daily radiation data at 90 China Meteorological Administration (CMA) stations. The MBEs are 9.8 W m−2 (or 5.4 %); the RMSEs in daily and monthly mean SSR estimates are 34.2 W m−2 (or 19.1 %) and 22.1 W m−2 (or 12.3 %), respectively. The accuracy is comparable to or even higher than two other radiation products (GLASS and ISCCP-FD), and the present method is more computationally efficient and can produce hourly SSR data at a spatial resolution of 5 km.
Using statistical models to explore ensemble uncertainty in climate impact studies: the example of air pollution in Europe

Because of its sensitivity to unfavorable weather patterns, air pollution is sensitive to climate change so that, in the future, a climate penalty could jeopardize the expected efficiency of air pollution mitigation measures. A common method to assess the impact of climate on air quality consists in implementing chemistry-transport models forced by climate projections. However, the computing cost of such methods requires optimizing ensemble exploration techniques. By using a training data set from a deterministic projection of climate and air quality over Europe, we identified the main meteorological drivers of air quality for eight regions in Europe and developed statistical models that could be used to predict air pollutant concentrations. The evolution of the key climate variables driving either particulate or gaseous pollution allows selecting the members of the EuroCordex ensemble of regional climate projections that should be used in priority for future air quality projections (CanESM2/RCA4; CNRM-CM5-LR/RCA4 and CSIRO-Mk3-6-0/RCA4 and MPI-ESM-LR/CCLM following the EuroCordex terminology). After having tested the validity of the statistical model in predictive mode, we can provide ranges of uncertainty attributed to the spread of the regional climate projection ensemble by the end of the century (2071–2100) for the RCP8.5. In the three regions where the statistical model of the impact of climate change on PM2.5 offers satisfactory performances, we find a climate benefit (a decrease of PM2.5 concentrations under future climate) of −1.08 (±0.21), −1.03 (±0.32), −0.83 (±0.14) µg m−3, for respectively Eastern Europe, Mid-Europe and Northern Italy. In the British-Irish Isles, Scandinavia, France, the Iberian Peninsula and the Mediterranean, the statistical model is not considered skillful enough to draw any conclusion for PM2.5. In Eastern Europe, France, the Iberian Peninsula, Mid-Europe and Northern Italy, the statistical model of the impact of climate change on ozone was considered satisfactory and it confirms the climate penalty bearing upon ozone of 10.51 (±3.06), 11.70 (±3.63), 11.53 (±1.55), 9.86 (±4.41), 4.82 (±1.79) µg m−3, respectively. In the British-Irish Isles, Scandinavia and the Mediterranean, the skill of the statistical model was not considered robust enough to draw any conclusion for ozone pollution.
Oxygen isotope mass balance of atmospheric nitrate at Dome C, East Antarctica, during the OPALE campaign

Variations in the stable oxygen isotope composition of atmospheric nitrate act as novel tools for studying oxidative processes taking place in the troposphere. They provide both qualitative and quantitative constraints on the pathways determining the fate of atmospheric nitrogen oxides (NO + NO2 = NOx). The unique and distinctive 17O excess (Δ17O = δ17O − 0.52 × δ18O) of ozone, which is transferred to NOx via oxidation, is a particularly useful isotopic fingerprint in studies of NOx transformations. Constraining the propagation of 17O excess within the NOx cycle is critical in polar areas, where there exists the possibility of extending atmospheric investigations to the glacial–interglacial timescale using deep ice core records of nitrate. Here we present measurements of the comprehensive isotopic composition of atmospheric nitrate collected at Dome C (East Antarctic Plateau) during the austral summer of 2011/2012. Nitrate isotope analysis has been here combined for the first time with key precursors involved in nitrate production (NOx, O3, OH, HO2, RO2, etc.) and direct observations of the transferrable Δ17O of surface ozone, which was measured at Dome C throughout 2012 using our recently developed analytical approach. Assuming that nitrate is mainly produced in Antarctica in summer through the OH + NO2 pathway and using concurrent measurements of OH and NO2, we calculated a Δ17O signature for nitrate on the order of (21–22 ± 3) ‰. These values are lower than the measured values that ranged between 27 and 31 ‰. This discrepancy between expected and observed Δ17O(NO3−) values suggests the existence of an unknown process that contributes significantly to the atmospheric nitrate budget over this East Antarctic region. However, systematic errors or false isotopic balance transfer functions are not totally excluded.
A new source of methylglyoxal in the aqueous phase

Carbonyl compounds are ubiquitous in atmospheric multiphase system participating in gas, particle, and aqueous-phase chemistry. One important compound is methyl ethyl ketone (MEK), as it is detected in significant amounts in the gas phase as well as in cloud water, ice, and rain. Consequently, it can be expected that MEK influences the liquid-phase chemistry. Therefore, the oxidation of MEK and the formation of corresponding oxidation products were investigated in the aqueous phase. Several oxidation products were identified from the oxidation with OH radicals, including 2,3-butanedione, hydroxyacetone, and methylglyoxal. The molar yields were 29.5 % for 2,3-butanedione, 3.0 % for hydroxyacetone, and 9.5 % for methylglyoxal. Since methylglyoxal is often related to the formation of organics in the aqueous phase, MEK should be considered for the formation of aqueous secondary organic aerosol (aqSOA). Based on the experimentally obtained data, a reaction mechanism for the formation of methylglyoxal has been developed and evaluated with a model study. Besides known rate constants, the model contains measured photolysis rate constants for MEK (kp  =  5  ×  10−5 s−1), 2,3-butanedione (kp  =  9  ×  10−6 s−1), methylglyoxal (kp  =  3  ×  10−5 s−1), and hydroxyacetone (kp  =  2  ×  10−5 s−1). From the model predictions, a branching ratio of 60 /40 for primary/secondary H-atom abstraction at the MEK skeleton was found. This branching ratio reproduces the experiment results very well, especially the methylglyoxal formation, which showed excellent agreement. Overall, this study demonstrates MEK as a methylglyoxal precursor compound for the first time.
Properties of cloud condensation nuclei (CCN) in the trade wind marine boundary layer of the western North Atlantic

Cloud optical properties in the trade winds over the eastern Caribbean Sea have been shown to be sensitive to cloud condensation nuclei (CCN) concentrations. The objective of the current study was to investigate the CCN properties in the marine boundary layer (MBL) in the tropical western North Atlantic, in order to assess the respective roles of inorganic sulfate, organic species, long-range transported mineral dust and sea-salt particles. Measurements were carried out in June–July 2013, on the east coast of Barbados, and included CCN number concentrations, particle number size distributions and offline analysis of sampled particulate matter (PM) and sampled accumulation mode particles for an investigation of composition and mixing state with transmission electron microscopy (TEM) in combination with energy-dispersive X-ray spectroscopy (EDX). During most of the campaign, significant mass concentrations of long-range transported mineral dust was present in the PM, and influence from local island sources can be ruled out. The CCN and particle number concentrations were similar to what can be expected in pristine marine environments. The hygroscopicity parameter κ was inferred, and values in the range 0.2–0.5 were found during most of the campaign, with similar values for the Aitken and the accumulation mode. The accumulation mode particles studied with TEM were dominated by non-refractory material, and concentrations of mineral dust, sea salt and soot were too small to influence the CCN properties. It is highly likely that the CCN were dominated by a mixture of sulfate species and organic compounds.
Transport pathways from the Asian monsoon anticyclone to the stratosphere

Transport pathways of air originating in the upper-tropospheric Asian monsoon anticyclone are investigated based on three-dimensional trajectories. The Asian monsoon anticyclone emerges in response to persistent deep convection over India and southeast Asia in northern summer, and this convection is associated with rapid transport from the surface to the upper troposphere and possibly into the stratosphere. Here, we investigate the fate of air that originates within the upper-tropospheric anticyclone from the outflow of deep convection, using trajectories driven by ERA-interim reanalysis data. Calculations include isentropic estimates, plus fully three-dimensional results based on kinematic and diabatic transport calculations. Isentropic calculations show that air parcels are typically confined within the anticyclone for 10–20 days and spread over the tropical belt within a month of their initialization. However, only few parcels (3 % at 360 K, 8 % at 380 K) reach the extratropical stratosphere by isentropic transport. When considering vertical transport we find that 31 % or 48 % of the trajectories reach the stratosphere within 60 days when using vertical velocities or diabatic heating rates to calculate vertical transport, respectively. In both cases, most parcels that reach the stratosphere are transported upward within the anticyclone and enter the stratosphere in the tropics, typically 10–20 days after their initialization at 360 K. This suggests that trace gases, including pollutants, that are transported into the stratosphere via the Asian monsoon system are in a position to enter the tropical pipe and thus be transported into the deep stratosphere. Sensitivity calculations with respect to the initial altitude of the trajectories showed that air needs to be transported to levels of 360 K or above by deep convection to likely (≧ 50 %) reach the stratosphere through transport by the large-scale circulation.
Understanding cirrus ice crystal number variability for different heterogeneous ice nucleation spectra

Along with minimizing parameter uncertainty, understanding the cause of temporal and spatial variability of the nucleated ice crystal number, Ni, is key to improving the representation of cirrus clouds in climate models. To this end, sensitivities of Ni to input variables like aerosol number and diameter provide valuable information about nucleation regime and efficiency for a given model formulation. Here we use the adjoint model of the adjoint of a cirrus formation parameterization (Barahona and Nenes, 2009b) to understand Ni variability for various ice-nucleating particle (INP) spectra. Inputs are generated with the Community Atmosphere Model version 5, and simulations are done with a theoretically derived spectrum, an empirical lab-based spectrum and two field-based empirical spectra that differ in the nucleation threshold for black carbon particles and in the active site density for dust. The magnitude and sign of Ni sensitivity to insoluble aerosol number can be directly linked to nucleation regime and efficiency of various INP. The lab-based spectrum calculates much higher INP efficiencies than field-based ones, which reveals a disparity in aerosol surface properties. Ni sensitivity to temperature tends to be low, due to the compensating effects of temperature on INP spectrum parameters; this low temperature sensitivity regime has been experimentally reported before but never deconstructed as done here.
Nucleation and growth of sub-3 nm particles in the polluted urban atmosphere of a megacity in China

Particle size distribution down to 1.4 nm was measured in the urban atmosphere of Nanjing, China, in spring, summer, and winter during 2014–2015. Sub-3 nm particle event, which is equivalent to nucleation event, occurred on 42 out of total 90 observation days, but new particles could grow to cloud condensation nuclei (CCN)-active sizes on only 9 days. In summer, infrequent nucleation was limited by both unfavorable meteorological conditions (high temperature and relative humidity – RH) and reduced anthropogenic precursor availability due to strict emission control measures during the 2014 Youth Olympic Games in Nanjing. The limiting factors for nucleation in winter and spring were meteorological conditions (radiation, temperature, and RH) and condensation sink, but for the further growth of sub-3 nm particles to CCN-active sizes, anthropogenic precursors again became limiting factors. Nucleation events were strong in the polluted urban atmosphere. Initial J1.4 at the onset and peak J1.4 at the noontime could be up to 2.1 × 102 and 2.5 × 103 cm−3 s−1, respectively, during the eight nucleation events selected from different seasons. Time-dependent J1.4 usually showed good linear correlations with a sulfuric acid proxy for every single event (R2 = 0.56–0.86, excluding a day with significant nocturnal nucleation), but the correlation among all eight events deteriorated (R2 =  0.17) due to temperature or season change. We observed that new particle growth rate (GR) did not increase monotonically with particle size, but had a local maximum up to 25 nm h−1 between 1 and 3 nm. The existence of local maxima GR in sub-3 nm size range, though sensitive to measurement uncertainties, gives new insight into cluster dynamics in polluted environments. In this study such growth rate behavior was interpreted as the solvation effect of organic activating vapor in newly formed inorganic nuclei.
On the characteristics of aerosol indirect effect based on dynamic regimes in global climate models

Aerosol–cloud interactions continue to constitute a major source of uncertainty for the estimate of climate radiative forcing. The variation of aerosol indirect effects (AIE) in climate models is investigated across different dynamical regimes, determined by monthly mean 500 hPa vertical pressure velocity (ω500), lower-tropospheric stability (LTS) and large-scale surface precipitation rate derived from several global climate models (GCMs), with a focus on liquid water path (LWP) response to cloud condensation nuclei (CCN) concentrations. The LWP sensitivity to aerosol perturbation within dynamic regimes is found to exhibit a large spread among these GCMs. It is in regimes of strong large-scale ascent (ω500  <  −25 hPa day−1) and low clouds (stratocumulus and trade wind cumulus) where the models differ most. Shortwave aerosol indirect forcing is also found to differ significantly among different regimes. Shortwave aerosol indirect forcing in ascending regimes is close to that in subsidence regimes, which indicates that regimes with strong large-scale ascent are as important as stratocumulus regimes in studying AIE. It is further shown that shortwave aerosol indirect forcing over regions with high monthly large-scale surface precipitation rate (> 0.1 mm day−1) contributes the most to the total aerosol indirect forcing (from 64 to nearly 100 %). Results show that the uncertainty in AIE is even larger within specific dynamical regimes compared to the uncertainty in its global mean values, pointing to the need to reduce the uncertainty in AIE in different dynamical regimes.
Detailed budget analysis of HONO in central London reveals a missing daytime source

Measurements of HONO were carried out at an urban background site near central London as part of the Clean air for London (ClearfLo) project in summer 2012. Data were collected from 22 July to 18 August 2014, with peak values of up to 1.8 ppbV at night and non-zero values of between 0.2 and 0.6 ppbV seen during the day. A wide range of other gas phase, aerosol, radiation, and meteorological measurements were made concurrently at the same site, allowing a detailed analysis of the chemistry to be carried out. The peak HONO/NOx ratio of 0.04 is seen at ∼  02:00 UTC, with the presence of a second, daytime, peak in HONO/NOx of similar magnitude to the night-time peak, suggesting a significant secondary daytime HONO source. A photostationary state calculation of HONO involving formation from the reaction of OH and NO and loss from photolysis, reaction with OH, and dry deposition shows a significant underestimation during the day, with calculated values being close to 0, compared to the measurement average of 0.4 ppbV at midday. The addition of further HONO sources from the literature, including dark conversion of NO2 on surfaces, direct emission, photolysis of ortho-substituted nitrophenols, the postulated formation from the reaction of HO2 ×  H2O with NO2, photolysis of adsorbed HNO3 on ground and aerosols, and HONO produced by photosensitized conversion of NO2 on the surface increases the daytime modelled HONO to 0.1 ppbV, still leaving a significant missing daytime source. The missing HONO is plotted against a series of parameters including NO2 and OH reactivity (used as a proxy for organic material), with little correlation seen. Much better correlation is observed with the product of these species with j(NO2), in particular NO2 and the product of NO2 with OH reactivity. This suggests the missing HONO source is in some way related to NO2 and also requires sunlight. Increasing the photosensitized surface conversion rate of NO2 by a factor of 10 to a mean daytime first-order loss of ∼ 6 × 10−5 s−1 (but which varies as a function of j(NO2)) closes the daytime HONO budget at all times (apart from the late afternoon), suggesting that urban surfaces may enhance this photosensitized source. The effect of the missing HONO to OH radical production is also investigated and it is shown that the model needs to be constrained to measured HONO in order to accurately reproduce the OH radical measurements.