Biogenic nitric oxide emissions from soils: impact on NOx and ozone over West Africa during AMMA (African Monsoon Multidisciplinary Analysis) - Modelling study

Nitrogen oxide biogenic emissions from soils are driven by soil and environmental parameters. The relationship between these parameters and NO fluxes is highly non linear. A new algorithm, based on a neural network calculation, is used to reproduce the NO biogenic emissions linked to precipitations in the Sahel on the 6 August 2006 during the AMMA campaign. This algorithm has been coupled in the surface scheme of a coupled chemistry dynamics model (MesoNH Chemistry) to estimate the impact of the NO emissions on NOx and O3 formation in the lower troposphere for this particular episode. Four different simulations on the same domain and at the same period are compared: one with anthropogenic emissions only, one with soil NO emissions from a static inventory, at low time and space resolution, one with NO emissions from neural network, and one with NO from neural network plus lightning NOx. The influence of NOx from lightning is limited to the upper troposphere. The NO emission from soils calculated with neural network responds to changes in soil moisture giving enhanced emissions over the wetted soil, as observed by aircraft measurements after the passing of a convective system. The subsequent enhancement of NOx and ozone is limited to the lowest layers of the atmosphere in modelling, whereas measurements show higher concentrations above 1000 m. The neural network algorithm, applied in the Sahel region for one particular day of the wet season, allows an immediate response of fluxes to environmental parameters, unlike static emission inventories. Stewart et al (2008) is a companion paper to this one which looks at NOx and ozone concentrations in the boundary layer as measured on a research aircraft, examines how they vary with respect to the soil moisture, as indicated by surface temperature anomalies, and deduces NOx fluxes. In this current paper the model-derived results are compared to the observations and calculated fluxes presented by Stewart et al (2008).

Recent changes in solar outputs and the global mean surface temperature. III. Analysis of contributions to global mean air surface temperature rise

A multivariate fit to the variation in global mean surface air temperature anomaly over the past half century is presented. The fit procedure allows for the effect of response time on the waveform, amplitude and lag of each radiative forcing input, and each is allowed to have its own time constant. It is shown that the contribution of solar variability to the temperature trend since 1987 is small and downward; the best estimate is -1.3% and the 2sigma confidence level sets the uncertainty range of -0.7 to -1.9%. The result is the same if one quantifies the solar variation using galactic cosmic ray fluxes (for which the analysis can be extended back to 1953) or the most accurate total solar irradiance data composite. The rise in the global mean air surface temperatures is predominantly associated with a linear increase that represents the combined effects of changes in anthropogenic well-mixed greenhouse gases and aerosols, although, in recent decades, there is also a considerable contribution by a relative lack of major volcanic eruptions. The best estimate is that the anthropogenic factors contribute 75% of the rise since 1987, with an uncertainty range (set by the 2sigma confidence level using an AR(1) noise model) of 49–160%; thus, the uncertainty is large, but we can state that at least half of the temperature trend comes from the linear term and that this term could explain the entire rise. The results are consistent with the intergovernmental panel on climate change (IPCC) estimates of the changes in radiative forcing (given for 1961–1995) and are here combined with those estimates to find the response times, equilibrium climate sensitivities and pertinent heat capacities (i.e. the depth into the oceans to which a given radiative forcing variation penetrates) of the quasi-periodic (decadal-scale) input forcing variations. As shown by previous studies, the decadal-scale variations do not penetrate as deeply into the oceans as the longer term drifts and have shorter response times. Hence, conclusions about the response to century-scale forcing changes (and hence the associated equilibrium climate sensitivity and the temperature rise commitment) cannot be made from studies of the response to shorter period forcing changes.

Macrocyclic amines as structure-directing agents for the synthesis of three-dimensional antimony-sulfide frameworks

A new family of antimony sulfides, incorporating the macrocyclic tetramine 1,4,8,11-tetraazacyclotetradecane ( cyclam), has been prepared by a hydrothermal method. [C10N4H26][Sb4S7] (1), [Ni(C10N4H24)][Sb4S7] (2), and [Co(C10N4H24)](x)[C10N4H26](1-x)[Sb4S7] (0.08 <= x <= 0.74) (3) have been characterized by single-crystal X-ray diffraction, elemental analysis, thermogravimetry, and analytical electron microscopy. All three materials possess the same novel three-dimensional Sb4S72- framework, constructed from layers of parallel arrays of Sb4S84- chains stacked at 90 to one another. In 1, doubly protonated macrocyclic cations reside in the channel structure of the antimonysulfide framework. In 2 and 3, the cyclam acts as a ligand, chelating the divalent transition- metal cation. Analytical and X-ray diffraction data indicate that the level of metal incorporation in 2 is effectively complete, whereas in 3, both metalated and nonmetalated forms of the macrocycle coexist within the structure.

U.K. HiGEM: Simulations of desert dust and biomass burning aerosols with a high-resolution atmospheric GCM

The atmospheric component of the United Kingdom’s new High-resolution Global Environmental Model (HiGEM) has been run with interactive aerosol schemes that include biomass burning and mineral dust. Dust emission, transport, and deposition are parameterized within the model using six particle size divisions, which are treated independently. The biomass is modeled in three nonindependent modes, and emissions are prescribed from an external dataset. The model is shown to produce realistic horizontal and vertical distributions of these aerosols for each season when compared with available satellite- and ground-based observations and with other models. Combined aerosol optical depths off the coast of North Africa exceed 0.5 both in boreal winter, when biomass is the main contributor, and also in summer, when the dust dominates. The model is capable of resolving smaller-scale features, such as dust storms emanating from the Bode´ le´ and Saharan regions of North Africa and the wintertime Bode´ le´ low-level jet. This is illustrated by February and July case studies, in which the diurnal cycles of model variables in relation to dust emission and transport are examined. The top-of-atmosphere annual mean radiative forcing of the dust is calculated and found to be globally quite small but locally very large, exceeding 20 W m22 over the Sahara, where inclusion of dust aerosol is shown to improve the model radiative balance. This work extends previous aerosol studies by combining complexity with increased global resolution and represents a step toward the next generation of models to investigate aerosol–climate interactions. 1. Introduction Accurate modeling of mineral dust is known to be important because of its radiative impact in both numerical weather prediction models (Milton et al. 2008; Haywood et

Transport impacts on atmosphere and climate: metrics

The transport sector emits a wide variety of gases and aerosols, with distinctly different characteristics which influence climate directly and indirectly via chemical and physical processes. Tools that allow these emissions to be placed on some kind of common scale in terms of their impact on climate have a number of possible uses such as: in agreements and emission trading schemes; when considering potential trade-offs between changes in emissions resulting from technological or operational developments; and/or for comparing the impact of different environmental impacts of transport activities. Many of the non-CO2 emissions from the transport sector are short-lived substances, not currently covered by the Kyoto Protocol. There are formidable difficulties in developing metrics and these are particularly acute for such short-lived species. One difficulty concerns the choice of an appropriate structure for the metric (which may depend on, for example, the design of any climate policy it is intended to serve) and the associated value judgements on the appropriate time periods to consider; these choices affect the perception of the relative importance of short- and long-lived species. A second difficulty is the quantification of input parameters (due to underlying uncertainty in atmospheric processes). In addition, for some transport-related emissions, the values of metrics (unlike the gases included in the Kyoto Protocol) depend on where and when the emissions are introduced into the atmosphere – both the regional distribution and, for aircraft, the distribution as a function of altitude, are important. In this assessment of such metrics, we present Global Warming Potentials (GWPs) as these have traditionally been used in the implementation of climate policy. We also present Global Temperature Change Potentials (GTPs) as an alternative metric, as this, or a similar metric may be more appropriate for use in some circumstances. We use radiative forcings and lifetimes from the literature to derive GWPs and GTPs for the main transport-related emissions, and discuss the uncertainties in these estimates. We find large variations in metric (GWP and GTP) values for NOx, mainly due to the dependence on location of emissions but also because of inter-model differences and differences in experimental design. For aerosols we give only global-mean values due to an inconsistent picture amongst available studies regarding regional dependence. The uncertainty in the presented metric values reflects the current state of understanding; the ranking of the various components with respect to our confidence in the given metric values is also given. While the focus is mostly on metrics for comparing the climate impact of emissions, many of the issues are equally relevant for stratospheric ozone depletion metrics, which are also discussed.

Chemical and aerosol characterisation of the troposphere over West Africa during the monsoon period as part of AMMA

During June, July and August 2006 five aircraft took part in a campaign over West Africa to observe the aerosol content and chemical composition of the troposphere and lower stratosphere as part of the African Monsoon Multidisciplinary Analysis (AMMA) project. These are the first such measurements in this region during the monsoon period. In addition to providing an overview of the tropospheric composition, this paper provides a description of the measurement strategy (flights performed, instrumental payloads, wing-tip to wing-tip comparisons) and points to some of the important findings discussed in more detail in other papers in this special issue. The ozone data exhibits an "S" shaped vertical profile which appears to result from significant losses in the lower troposphere due to rapid deposition to forested areas and photochemical destruction in the moist monsoon air, and convective uplift of ozone-poor air to the upper troposphere. This profile is disturbed, particularly in the south of the region, by the intrusions in the lower and middle troposphere of air from the southern hemisphere impacted by biomass burning. Comparisons with longer term data sets suggest the impact of these intrusions on West Africa in 2006 was greater than in other recent wet seasons. There is evidence for net photochemical production of ozone in these biomass burning plumes as well as in urban plumes, in particular that from Lagos, convective outflow in the upper troposphere and in boundary layer air affected by nitrogen oxide emissions from recently wetted soils. This latter effect, along with enhanced deposition to the forested areas, contributes to a latitudinal gradient of ozone in the lower troposphere. Biogenic volatile organic compounds are also important in defining the composition both for the boundary layer and upper tropospheric convective outflow. Mineral dust was found to be the most abundant and ubiquitous aerosol type in the atmosphere over Western Africa. Data collected within AMMA indicate that injection of dust to altitudes favourable for long-range transport (i.e. in the upper Sahelian planetary boundary layer) can occur behind the leading edge of mesoscale convective system (MCS) cold-pools. Research within AMMA also provides the first estimates of secondary organic aerosols across the West African Sahel and have shown that organic mass loadings vary between 0 and 2 μg m−3 with a median concentration of 1.07 μg m−3. The vertical distribution of nucleation mode particle concentrations reveals that significant and fairly strong particle formation events did occur for a considerable fraction of measurement time above 8 km (and only there). Very low concentrations were observed in general in the fresh outflow of active MCSs, likely as the result of efficient wet removal of aerosol particles due to heavy precipitation inside the convective cells of the MCSs. This wet removal initially affects all particle size ranges as clearly shown by all measurements in the vicinity of MCSs.

Sensitivity of GCM tropical middle atmosphere variability and climate to ozone and parametrized gravity wave changes

This paper describes the impact of changing the current imposed ozone climatology upon the tropical Quasi-Biennial Oscillation (QBO) in a high top climate configuration of the Met Office U.K. general circulation model. The aim is to help distinguish between QBO changes in chemistry climate models that result from temperature-ozone feedbacks and those that might be forced by differences in climatology between previously fixed and newly interactive ozone distributions. Different representations of zonal mean ozone climatology under present-day conditions are taken to represent the level of change expected between acceptable model realizations of the global ozone distribution and thus indicate whether more detailed investigation of such climatology issues might be required when assessing ozone feedbacks. Tropical stratospheric ozone concentrations are enhanced relative to the control climatology between 20–30 km, reduced from 30–40 km and enhanced above, impacting the model profile of clear-sky radiative heating, in particular warming the tropical stratosphere between 15–35 km. The outcome is consistent with a localized equilibrium response in the tropical stratosphere that generates increased upwelling between 100 and 4 hPa, sufficient to account for a 12 month increase of modeled mean QBO period. This response has implications for analysis of the tropical circulation in models with interactive ozone chemistry because it highlights the possibility that plausible changes in the ozone climatology could have a sizable impact upon the tropical upwelling and QBO period that ought to be distinguished from other dynamical responses such as ozone-temperature feedbacks.

Comparison of results from several AOGCMs for global and regional sea-level change 1900-2100

Sea-level rise is an important aspect of climate change because of its impact on society and ecosystems. Here we present an intercomparison of results from ten coupled atmosphere-ocean general circulation models (AOGCMs) for sea-level changes simulated for the twentieth century and projected to occur during the twenty first century in experiments following scenario IS92a for greenhouse gases and sulphate aerosols. The model results suggest that the rate of sea-level rise due to thermal expansion of sea water has increased during the twentieth century, but the small set of tide gauges with long records might not be adequate to detect this acceleration. The rate of sea-level rise due to thermal expansion continues to increase throughout the twenty first century, and the projected total is consequently larger than in the twentieth century; for 1990-2090 it amounts to 0.20-0.37 in. This wide range results from systematic uncertainty in modelling of climate change and of heat uptake by the ocean. The AOGCMs agree that sea-level rise is expected to be geographically non-uniform, with some regions experiencing as much as twice the global average, and others practically zero, but they do not agree about the geographical pattern. The lack of agreement indicates that we cannot currently have confidence in projections of local sea- level changes, and reveals a need for detailed analysis and intercomparison in order to understand and reduce the disagreements.

The role of atmosphere feedbacks during ENSO in the CMIP3 models. Part II: using AMIP runs to understand the heat flux feedback mechanisms

Several studies using ocean–atmosphere general circulation models (GCMs) suggest that the atmospheric component plays a dominant role in the modelled El Niño-Southern Oscillation (ENSO). To help elucidate these findings, the two main atmosphere feedbacks relevant to ENSO, the Bjerknes positive feedback (μ) and the heat flux negative feedback (α), are here analysed in nine AMIP runs of the CMIP3 multimodel dataset. We find that these models generally have improved feedbacks compared to the coupled runs which were analysed in part I of this study. The Bjerknes feedback, μ, is increased in most AMIP runs compared to the coupled run counterparts, and exhibits both positive and negative biases with respect to ERA40. As in the coupled runs, the shortwave and latent heat flux feedbacks are the two dominant components of α in the AMIP runs. We investigate the mechanisms behind these two important feedbacks, in particular focusing on the strong 1997–1998 El Niño. Biases in the shortwave flux feedback, α SW, are the main source of model uncertainty in α. Most models do not successfully represent the negative αSW in the East Pacific, primarily due to an overly strong low-cloud positive feedback in the far eastern Pacific. Biases in the cloud response to dynamical changes dominate the modelled α SW biases, though errors in the large-scale circulation response to sea surface temperature (SST) forcing also play a role. Analysis of the cloud radiative forcing in the East Pacific reveals model biases in low cloud amount and optical thickness which may affect α SW. We further show that the negative latent heat flux feedback, α LH, exhibits less diversity than α SW and is primarily driven by variations in the near-surface specific humidity difference. However, biases in both the near-surface wind speed and humidity response to SST forcing can explain the inter-model αLH differences.

Determining the contribution of volcanic ash and boundary layer aerosol in backscatter lidar returns: a three‐component atmosphere approach

A solution of the lidar equation is discussed, that permits combining backscatter and depolarization measurements to quantitatively distinguish two different aerosol types with different depolarization properties. The method has been successfully applied to simultaneous observations of volcanic ash and boundary layer aerosol obtained in Exeter, United Kingdom, on 16 and 18 April 2010, permitting the contribution of the two aerosols to be quantified separately. First a subset of the atmospheric profiles is used where the two aerosol types belong to clearly distinguished layers, for the purpose of characterizing the ash in terms of lidar ratio and depolarization. These quantities are then used in a three‐component atmosphere solution scheme of the lidar equation applied to the full data set, in order to compute the optical properties of both aerosol types separately. On 16 April a thin ash layer, 100–400 m deep, is observed (average and maximum estimated ash optical depth: 0.11 and 0.2); it descends from ∼2800 to ∼1400 m altitude over a 6‐hour period. On 18 April a double ash layer, ∼400 m deep, is observed just above the morning boundary layer (average and maximum estimated ash optical depth: 0.19 and 0.27). In the afternoon the ash is entrained into the boundary layer, and the latter reaches a depth of ∼1800 m (average and maximum estimated ash optical depth: 0.1 and 0.15). An additional ash layer, with a very small optical depth, was observed on 18 April at an altitude of 3500–4000 m. By converting the lidar optical measurements using estimates of volcanic ash specific extinction, derived from other works, the observations seem to suggest approximate peak ash concentrations of ∼1500 and ∼1000 mg/m3,respectively, on the two observations dates.

Observed changes in top-of-the-atmosphere radiation and upper-ocean heating consistent within uncertainty

Global climate change results from a small yet persistent imbalance between the amount of sunlight absorbed by Earth and the thermal radiation emitted back to space. An apparent inconsistency has been diagnosed between interannual variations in the net radiation imbalance inferred from satellite measurements and upper-ocean heating rate from in situ measurements, and this inconsistency has been interpreted as ‘missing energy’ in the system. Here we present a revised analysis of net radiation at the top of the atmosphere from satellite data, and we estimate ocean heat content, based on three independent sources. We find that the difference between the heat balance at the top of the atmosphere and upper-ocean heat content change is not statistically significant when accounting for observational uncertainties in ocean measurements, given transitions in instrumentation and sampling. Furthermore, variability in Earth’s energy imbalance relating to El Niño-Southern Oscillation is found to be consistent within observational uncertainties among the satellite measurements, a reanalysis model simulation and one of the ocean heat content records. We combine satellite data with ocean measurements to depths of 1,800 m, and show that between January 2001 and December 2010, Earth has been steadily accumulating energy at a rate of 0.50±0.43 Wm−2 (uncertainties at the 90% confidence level). We conclude that energy storage is continuing to increase in the sub-surface ocean.

Relaxing the Tropics to an ‘observed’ state: analysis using a simple baroclinic model

The technique of relaxation of the tropical atmosphere towards an analysis in a month-season forecast model has previously been successfully exploited in a number of contexts. Here it is shown that when tropical relaxation is used to investigate the possible origin of the observed anomalies in June–July 2007, a simple dynamical model is able to reproduce the observed component of the pattern of anomalies given by an ensemble of ECMWF forecast runs. Following this result, the simple model is used for a range of experiments on time-scales of relaxation, variables and regions relaxed based on a control model run with equatorial heating in a zonal flow. A theory based on scale analysis for the large-scale tropics is used to interpret the results. Typical relationships between scales are determined from the basic equations, and for a specified diabatic heating a chain of deductions for determining the dependent variables is derived. Different critical time-scales are found for tropical relaxation of different dependent variables to be effective. Vorticity has the longest critical time-scale, typically 1.2 days. For temperature and divergence, the time-scales are 10 hours and 3 hours, respectively. However not all the tropical fields, in particular the vertical motion, are reproduced correctly by the model unless divergence is heavily damped. To obtain the correct extra-tropical fields, it is crucial to have the correct rotational flow in the subtropics to initiate the Rossby wave propagation from there. It is sufficient to relax vorticity or temperature on a time-scale comparable or less than their critical time-scales to obtain this. However if the divergent advection of vorticity is important in the Rossby Wave Source then strong relaxation of divergence is required to accurately represent the tropical forcing of Rossby waves.

Inter-hemispheric mesospheric coupling in a comprehensive middle atmosphere model

Observations of noctilucent clouds have revealed a surprising coupling between the winter stratosphere and the summer polar mesopause region. In spite of the great distance involved, this inter-hemispheric link has been suggested to be the principal reason for both the year-to-year variability and the hemispheric differences in the frequency of occurrence of these high-altitude clouds. In this study, we investigate the dynamical influence of the winter stratosphere on the summer mesosphere using simulations from the vertically extended version of the Canadian Middle Atmosphere Model (CMAM). We find that for both Northern and Southern Hemispheres, variability in the summer polar mesopause region from one year to another can be traced back to the planetary-wave flux entering the winter stratosphere. The teleconnection pattern is the same for both positive and negative wave-flux anomalies. Using a composite analysis to isolate the events, it is argued that the mechanism for interhemispheric coupling is a feedback between summer mesosphere gravity-wave drag (GWD) and zonal wind, which is induced by an anomaly in mesospheric cross-equatorial flow, the latter arising from the anomaly in winter hemisphere GWD induced by the anomaly in stratospheric conditions.

The role of atmosphere feedbacks during ENSO in the CMIP3 models. Part III: the shortwave flux feedback

Previous studies using coupled general circulation models (GCMs) suggest that the atmosphere model plays a dominant role in the modeled El Nin ̃ o–Southern Oscillation (ENSO), and that intermodel differences in the thermodynamical damping of sea surface temperatures (SSTs) are a dominant contributor to the ENSO amplitude diversity. This study presents a detailed analysis of the shortwave flux feedback (aSW) in 12 Coupled Model Intercomparison Project phase 3 (CMIP3) simulations, motivated by findings that aSW is the primary contributor to model thermodynamical damping errors. A ‘‘feedback decomposition method,’’ developed to elucidate the aSW biases, shows that all models un- derestimate the dynamical atmospheric response to SSTs in the eastern equatorial Pacific, leading to un- derestimated aSW values. Biases in the cloud response to dynamics and the shortwave interception by clouds also contribute to errors in aSW. Changes in the aSW feedback between the coupled and corresponding atmosphere-only simulations are related to changes in the mean dynamics. A large nonlinearity is found in the observed and modeled SW flux feedback, hidden when linearly cal- culating aSW. In the observations, two physical mechanisms are proposed to explain this nonlinearity: 1) a weaker subsidence response to cold SST anomalies than the ascent response to warm SST anomalies and 2) a nonlinear high-level cloud cover response to SST. The shortwave flux feedback nonlinearity tends to be underestimated by the models, linked to an underestimated nonlinearity in the dynamical response to SST. The process-based methodology presented in this study may help to correct model ENSO atmospheric biases, ultimately leading to an improved simulation of ENSO in GCMs.

Summertime stratospheric processes at northern mid-latitudes: comparisons between MANTRA balloon measurements and the Canadian Middle Atmosphere Model

In this paper we report on a study conducted using the Middle Atmospheric Nitrogen TRend Assessment (MANTRA) balloon measurements of stratospheric constituents and temperature and the Canadian Middle Atmosphere Model (CMAM). Three different kinds of data are used to assess the inter-consistency of the combined dataset: single profiles of long-lived species from MANTRA 1998, sparse climatologies from the ozonesonde measurements during the four MANTRA campaigns and from HALOE satellite measurements, and the CMAM climatology. In doing so, we evaluate the ability of the model to reproduce the measured fields and to thereby test our ability to describe mid-latitude summertime stratospheric processes. The MANTRA campaigns were conducted at Vanscoy, Saskatchewan, Canada (52◦ N, 107◦ W)in late August and early September of 1998, 2000, 2002 and 2004. During late summer at mid-latitudes, the stratosphere is close to photochemical control, providing an ideal scenario for the study reported here. From this analysis we find that: (1) reducing the value for the vertical diffusion coefficient in CMAM to a more physically reasonable value results in the model better reproducing the measured profiles of long-lived species; (2) the existence of compact correlations among the constituents, as expected from independent measurements in the literature and from models, confirms the self-consistency of the MANTRA measurements; and (3) the 1998 measurements show structures in the chemical species profiles that can be associated with transport, adding to the growing evidence that the summertime stratosphere can be much more disturbed than anticipated. The mechanisms responsible for such disturbances need to be understood in order to assess the representativeness of the measurements and to isolate longterm trends.