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Air–sea fluxes of CO2 and CH4 from the Penlee Point Atmospheric Observatory on the south-west coast of the UK

We present air–sea fluxes of carbon dioxide (CO2), methane (CH4), momentum, and sensible heat measured by the eddy covariance method from the recently established Penlee Point Atmospheric Observatory (PPAO) on the south-west coast of the United Kingdom. Measurements from the south-westerly direction (open water sector) were made at three different sampling heights (approximately 15, 18, and 27 m above mean sea level, a.m.s.l.), each from a different period during 2014–2015. At sampling heights ≥  18 m a.m.s.l., measured fluxes of momentum and sensible heat demonstrate reasonable ( ≤  ±20 % in the mean) agreement with transfer rates over the open ocean. This confirms the suitability of PPAO for air–sea exchange measurements in shelf regions. Covariance air–sea CO2 fluxes demonstrate high temporal variability. Air-to-sea transport of CO2 declined from spring to summer in both years, coinciding with the breakdown of the spring phytoplankton bloom. We report, to the best of our knowledge, the first successful eddy covariance measurements of CH4 emissions from a marine environment. Higher sea-to-air CH4 fluxes were observed during rising tides (20 ± 3; 38 ± 3; 29 ± 6 µmole m−2 d−1 at 15, 18, 27 m a.m.s.l.) than during falling tides (14 ± 2; 22 ± 2; 21 ± 5 µmole m−2 d−1), consistent with an elevated CH4 source from an estuarine outflow driven by local tidal circulation. These fluxes are a few times higher than the predicted CH4 emissions over the open ocean and are significantly lower than estimates from other aquatic CH4 hotspots (e.g. polar regions, freshwater). Finally, we found the detection limit of the air–sea CH4 flux by eddy covariance to be 20 µmole m−2 d−1 over hourly timescales (4 µmole m−2 d−1 over 24 h).
Comprehensive tool for calculation of radiative fluxes: illustration of shortwave aerosol radiative effect sensitivities to the details in aerosol and underlying surface characteristics

The evaluation of aerosol radiative effect on broadband hemispherical solar flux is often performed using simplified spectral and directional scattering characteristics of atmospheric aerosol and underlying surface reflectance. In this study we present a rigorous yet fast computational tool that accurately accounts for detailed variability of both spectral and angular scattering properties of aerosol and surface reflectance in calculation of direct aerosol radiative effect. The tool is developed as part of the GRASP (Generalized Retrieval of Aerosol and Surface Properties) project. We use the tool to evaluate instantaneous and daily average radiative efficiencies (radiative effect per unit aerosol optical thickness) of several key atmospheric aerosol models over different surface types. We then examine the differences due to neglect of surface reflectance anisotropy, nonsphericity of aerosol particle shape and accounting only for aerosol angular scattering asymmetry instead of using full phase function. For example, it is shown that neglecting aerosol particle nonsphericity causes mainly overestimation of the aerosol cooling effect and that magnitude of this overestimate changes significantly as a function of solar zenith angle (SZA) if the asymmetry parameter is used instead of detailed phase function. It was also found that the nonspherical–spherical differences in the calculated aerosol radiative effect are not modified significantly if detailed BRDF (bidirectional reflectance distribution function) is used instead of Lambertian approximation of surface reflectance. Additionally, calculations show that usage of only angular scattering asymmetry, even for the case of spherical aerosols, modifies the dependence of instantaneous aerosol radiative effect on SZA. This effect can be canceled for daily average values, but only if sun reaches the zenith; otherwise a systematic bias remains. Since the daily average radiative effect is obtained by integration over a range of SZAs, the errors vary with latitude and season. In summary, the present analysis showed that use of simplified assumptions causes systematic biases, rather than random uncertainties, in calculation of both instantaneous and daily average aerosol radiative effect. Finally, we illustrate application of the rigorous aerosol radiative effect calculations performed as part of GRASP aerosol retrieval from real POLDER/PARASOL satellite observations.
Impact of buildings on surface solar radiation over urban Beijing

The rugged surface of an urban area due to varying buildings can interact with solar beams and affect both the magnitude and spatiotemporal distribution of surface solar fluxes. Here we systematically examine the impact of buildings on downward surface solar fluxes over urban Beijing by using a 3-D radiation parameterization that accounts for 3-D building structures vs. the conventional plane-parallel scheme. We find that the resulting downward surface solar flux deviations between the 3-D and the plane-parallel schemes are generally ±1–10 W m−2 at 800 m grid resolution and within ±1 W m−2 at 4 km resolution. Pairs of positive–negative flux deviations on different sides of buildings are resolved at 800 m resolution, while they offset each other at 4 km resolution. Flux deviations from the unobstructed horizontal surface at 4 km resolution are positive around noon but negative in the early morning and late afternoon. The corresponding deviations at 800 m resolution, in contrast, show diurnal variations that are strongly dependent on the location of the grids relative to the buildings. Both the magnitude and spatiotemporal variations of flux deviations are largely dominated by the direct flux. Furthermore, we find that flux deviations can potentially be an order of magnitude larger by using a finer grid resolution. Atmospheric aerosols can reduce the magnitude of downward surface solar flux deviations by 10–65 %, while the surface albedo generally has a rather moderate impact on flux deviations. The results imply that the effect of buildings on downward surface solar fluxes may not be critically significant in mesoscale atmospheric models with a grid resolution of 4 km or coarser. However, the effect can play a crucial role in meso-urban atmospheric models as well as microscale urban dispersion models with resolutions of 1 m to 1 km.
The origin of midlatitude ice clouds and the resulting influence on their microphysical properties

The radiative role of ice clouds in the atmosphere is known to be important, but uncertainties remain concerning the magnitude and net effects. However, through measurements of the microphysical properties of cirrus clouds, we can better characterize them, which can ultimately allow for their radiative properties to be more accurately ascertained. Recently, two types of cirrus clouds differing by formation mechanism and microphysical properties have been classified – in situ and liquid origin cirrus. In this study, we present observational evidence to show that two distinct types of cirrus do exist. Airborne, in situ measurements of cloud ice water content (IWC), ice crystal concentration (Nice), and ice crystal size from the 2014 ML-CIRRUS campaign provide cloud samples that have been divided according to their origin type. The key features that set liquid origin cirrus apart from the in situ origin cirrus are higher frequencies of high IWC ( > 100 ppmv), higher Nice values, and larger ice crystals. A vertical distribution of Nice shows that the in situ origin cirrus clouds exhibit a median value of around 0.1 cm−3, while the liquid origin concentrations are slightly, but notably higher. The median sizes of the crystals contributing the most mass are less than 200 µm for in situ origin cirrus, with some of the largest crystals reaching 550 µm in size. The liquid origin cirrus, on the other hand, were observed to have median diameters greater than 200 µm, and crystals that were up to 750 µm. An examination of these characteristics in relation to each other and their relationship to temperature provides strong evidence that these differences arise from the dynamics and conditions in which the ice crystals formed. Additionally, the existence of these two groups in cirrus cloud populations may explain why a bimodal distribution in the IWC-temperature relationship has been observed. We hypothesize that the low IWC mode is the result of in situ origin cirrus and the high IWC mode is the result of liquid origin cirrus.
Wind speed response of marine non-precipitating stratocumulus clouds over a diurnal cycle in cloud-system resolving simulations

Observed and projected trends in large-scale wind speed over the oceans prompt the question: how do marine stratocumulus clouds and their radiative properties respond to changes in large-scale wind speed? Wind speed drives the surface fluxes of sensible heat, moisture, and momentum and thereby acts on cloud liquid water path (LWP) and cloud radiative properties. We present an investigation of the dynamical response of non-precipitating, overcast marine stratocumulus clouds to different wind speeds over the course of a diurnal cycle, all else equal. In cloud-system resolving simulations, we find that higher wind speed leads to faster boundary layer growth and stronger entrainment. The dynamical driver is enhanced buoyant production of turbulence kinetic energy (TKE) from latent heat release in cloud updrafts. LWP is enhanced during the night and in the morning at higher wind speed, and more strongly suppressed later in the day. Wind speed hence accentuates the diurnal LWP cycle by expanding the morning–afternoon contrast. The higher LWP at higher wind speed does not, however, enhance cloud top cooling because in clouds with LWP ⪆ 50 g m−2, longwave emissions are insensitive to LWP. This leads to the general conclusion that in sufficiently thick stratocumulus clouds, additional boundary layer growth and entrainment due to a boundary layer moistening arises by stronger production of TKE from latent heat release in cloud updrafts, rather than from enhanced longwave cooling. We find that large-scale wind modulates boundary layer decoupling. At nighttime and at low wind speed during daytime, it enhances decoupling in part by faster boundary layer growth and stronger entrainment and in part because shear from large-scale wind in the sub-cloud layer hinders vertical moisture transport between the surface and cloud base. With increasing wind speed, however, in decoupled daytime conditions, shear-driven circulation due to large-scale wind takes over from buoyancy-driven circulation in transporting moisture from the surface to cloud base and thereby reduces decoupling and helps maintain LWP. The total (shortwave + longwave) cloud radiative effect (CRE) responds to changes in LWP and cloud fraction, and higher wind speed translates to a stronger diurnally averaged total CRE. However, the sensitivity of the diurnally averaged total CRE to wind speed decreases with increasing wind speed.
Modeling lightning-NOx chemistry on a sub-grid scale in a global chemical transport model

For the first time, a plume-in-grid approach is implemented in a chemical transport model (CTM) to parameterize the effects of the nonlinear reactions occurring within high concentrated NOx plumes from lightning NOx emissions (LNOx) in the upper troposphere. It is characterized by a set of parameters including the plume lifetime, the effective reaction rate constant related to NOx–O3 chemical interactions, and the fractions of NOx conversion into HNO3 within the plume. Parameter estimates were made using the Dynamical Simple Model of Atmospheric Chemical Complexity (DSMACC) box model, simple plume dispersion simulations, and the 3-D Meso-NH (non-hydrostatic mesoscale atmospheric model). In order to assess the impact of the LNOx plume approach on the NOx and O3 distributions on a large scale, simulations for the year 2006 were performed using the GEOS-Chem global model with a horizontal resolution of 2° × 2.5°. The implementation of the LNOx parameterization implies an NOx and O3 decrease on a large scale over the region characterized by a strong lightning activity (up to 25 and 8 %, respectively, over central Africa in July) and a relative increase downwind of LNOx emissions (up to 18 and 2 % for NOx and O3, respectively, in July). The calculated variability in NOx and O3 mixing ratios around the mean value according to the known uncertainties in the parameter estimates is at a maximum over continental tropical regions with ΔNOx [−33.1, +29.7] ppt and ΔO3 [−1.56, +2.16] ppb, in January, and ΔNOx [−14.3, +21] ppt and ΔO3 [−1.18, +1.93] ppb, in July, mainly depending on the determination of the diffusion properties of the atmosphere and the initial NO mixing ratio injected by lightning. This approach allows us (i) to reproduce a more realistic lightning NOx chemistry leading to better NOx and O3 distributions on the large scale and (ii) to focus on other improvements to reduce remaining uncertainties from processes related to NOx chemistry in CTM.
Marine boundary layer structure as observed by A-train satellites

The marine boundary layer (MBL) structure is important to the marine low cloud processes, and the exchange of heat, momentum, and moisture between oceans and the low atmosphere. This study examines the MBL structure over the eastern Pacific region and further explores the controlling factors of MBL structure over the global oceans with a new 4-year satellite-based data set. The MBL top (boundary layer height, BLH) and the mixing layer height (MLH) were identified using the MBL aerosol lidar backscattering from the CALIPSO (Cloud–Aerosol Lidar and Infrared Pathfinder Satellite Observations). Results showed that the MBL is generally decoupled with MLH ∕ BLH ratio ranging from ∼  0.5 to ∼  0.8 over the eastern Pacific Ocean region. The MBL decoupling magnitude is mainly controlled by estimated inversion strength (EIS), which in turn controls the cloud top entrainment process. The systematic differences between drizzling and non-drizzling stratocumulus tops also show dependence on EIS. This may be related to the meso-scale circulations or gravity wave in the MBL. Further analysis indicates that the MBL shows a similar decoupled structure for clear-sky and cumulus-cloud-topped conditions, but is better mixed under stratiform cloud breakup and overcast conditions.
Atmospheric changes caused by galactic cosmic rays over the period 1960–2010

The Specified Dynamics version of the Whole Atmosphere Community Climate Model (SD-WACCM) and the Goddard Space Flight Center two-dimensional (GSFC 2-D) models are used to investigate the effect of galactic cosmic rays (GCRs) on the atmosphere over the 1960–2010 time period. The Nowcast of Atmospheric Ionizing Radiation for Aviation Safety (NAIRAS) computation of the GCR-caused ionization rates are used in these simulations. GCR-caused maximum NOx increases of 4–15 % are computed in the Southern polar troposphere with associated ozone increases of 1–2 %. NOx increases of ∼ 1–6 % are calculated for the lower stratosphere with associated ozone decreases of 0.2–1 %. The primary impact of GCRs on ozone was due to their production of NOx. The impact of GCRs varies with the atmospheric chlorine loading, sulfate aerosol loading, and solar cycle variation. Because of the interference between the NOx and ClOx ozone loss cycles (e.g., the ClO + NO2+ M  →  ClONO2+ M reaction) and the change in the importance of ClOx in the ozone budget, GCRs cause larger atmospheric impacts with less chlorine loading. GCRs also cause larger atmospheric impacts with less sulfate aerosol loading and for years closer to solar minimum. GCR-caused decreases of annual average global total ozone (AAGTO) were computed to be 0.2 % or less with GCR-caused column ozone increases between 1000 and 100 hPa of 0.08 % or less and GCR-caused column ozone decreases between 100 and 1 hPa of 0.23 % or less. Although these computed ozone impacts are small, GCRs provide a natural influence on ozone and need to be quantified over long time periods. This result serves as a lower limit because of the use of the ionization model NAIRAS/HZETRN which underestimates the ion production by neglecting electromagnetic and muon branches of the cosmic ray induced cascade. This will be corrected in future works.
Simulating the SOA formation of isoprene from partitioning and aerosol phase reactions in the presence of inorganics

The secondary organic aerosol (SOA) produced by the photooxidation of isoprene with and without inorganic seed is simulated using the Unified Partitioning Aerosol Phase Reaction (UNIPAR) model. Recent work has found the SOA formation of isoprene to be sensitive to both aerosol acidity ([H+], mol L−1) and aerosol liquid water content (LWC) with the presence of either leading to significant aerosol phase organic mass generation and large growth in SOA yields (YSOA). Classical partitioning models alone are insufficient to predict isoprene SOA formation due to the high volatility of photooxidation products and sensitivity of their mass yields to variations in inorganic aerosol composition. UNIPAR utilizes the chemical structures provided by a near-explicit chemical mechanism to estimate the thermodynamic properties of the gas phase products, which are lumped based on their calculated vapor pressure (eight groups) and aerosol phase reactivity (six groups). UNIPAR then determines the SOA formation of each lumping group from both partitioning and aerosol phase reactions (oligomerization, acid-catalyzed reactions and organosulfate formation) assuming a single homogeneously mixed organic–inorganic phase as a function of inorganic composition and VOC ∕ NOx (VOC – volatile organic compound). The model is validated using isoprene photooxidation experiments performed in the dual, outdoor University of Florida Atmospheric PHotochemical Outdoor Reactor (UF APHOR) chambers. UNIPAR is able to predict the experimental SOA formation of isoprene without seed, with H2SO4 seed gradually titrated by ammonia, and with the acidic seed generated by SO2 oxidation. Oligomeric mass is predicted to account for more than 65 % of the total organic mass formed in all cases and over 85 % in the presence of strongly acidic seed. The model is run to determine the sensitivity of YSOA to [H+], LWC and VOC ∕ NOx, and it is determined that the SOA formation of isoprene is most strongly related to [H+] but is dynamically related to all three parameters. For VOC ∕ NOx  >  10, with increasing NOx both experimental and simulated YSOA increase and are found to be more sensitive to [H+] and LWC. For atmospherically relevant conditions, YSOA is found to be more than 150 % higher in partially titrated acidic seeds (NH4HSO4) than in effloresced inorganics or in isoprene only.
Effects of aerosols on clear-sky solar radiation in the ALADIN-HIRLAM NWP system

The direct shortwave radiative effect of aerosols under clear-sky conditions in the Aire Limitee Adaptation dynamique Developpement InterNational – High Resolution Limited Area Model (ALADIN-HIRLAM) numerical weather prediction system was investigated using three shortwave radiation schemes in diagnostic single-column experiments: the Integrated Forecast System (IFS), acraneb2 and the hlradia radiation schemes. The multi-band IFS scheme was formerly used operationally by the European Centre for Medium Range Weather Forecasts (ECMWF) whereas hlradia and acraneb2 are broadband schemes. The former is a new version of the HIRLAM radiation scheme while acraneb2 is the radiation scheme in the ALARO-1 physics package. The aim was to evaluate the strengths and weaknesses of the numerical weather prediction (NWP) system regarding aerosols and to prepare it for use of real-time aerosol information. The experiments were run with particular focus on the August 2010 Russian wildfire case. Each of the three radiation schemes accurately (within ±4 % at midday) simulates the direct shortwave aerosol effect when observed aerosol optical properties are used. When the aerosols were excluded from the simulations, errors of more than +15 % in global shortwave irradiance were found at midday, with the error reduced to +10 % when standard climatological aerosols were used. An error of −11 % was seen at midday if only observed aerosol optical depths at 550 nm, and not observation-based spectral dependence of aerosol optical depth, single scattering albedos and asymmetry factors, were included in the simulations. This demonstrates the importance of using the correct aerosol optical properties. The dependency of the direct radiative effect of aerosols on relative humidity was tested and shown to be within ±6 % in this case. By modifying the assumptions about the shape of the IFS climatological vertical aerosol profile, the inherent uncertainties associated with assuming fixed vertical profiles were investigated. The shortwave heating rates in the boundary layer changed by up to a factor of 2 in response to the aerosol vertical distribution without changing the total aerosol optical depth. Finally, we tested the radiative transfer approximations used in the three radiation schemes for typical aerosol optical properties compared to the accurate DISORT model. These approximations are found to be accurate to within ±13 % even for large aerosol loads.