Atmospheric chemistry and physics in the atmosphere of a developed megacity (London): an overview of the REPARTEE experiment and its conclusions

The REgents PARk and Tower Environmental Experiment (REPARTEE) comprised two campaigns in London in October 2006 and October/November 2007. The experiment design involved measurements at a heavily trafficked roadside site, two urban background sites and an elevated site at 160–190 m above ground on the BT Tower, supplemented in the second campaign by Doppler lidar measurements of atmospheric vertical structure. A wide range of measurements of airborne particle physical metrics and chemical composition were made as well as measurements of a considerable range of gas phase species and the fluxes of both particulate and gas phase substances. Significant findings include (a) demonstration of the evaporation of traffic-generated nanoparticles during both horizontal and vertical atmospheric transport; (b) generation of a large base of information on the fluxes of nanoparticles, accumulation mode particles and specific chemical components of the aerosol and a range of gas phase species, as well as the elucidation of key processes and comparison with emissions inventories; (c) quantification of vertical gradients in selected aerosol and trace gas species which has demonstrated the important role of regional transport in influencing concentrations of sulphate, nitrate and secondary organic compounds within the atmosphere of London; (d) generation of new data on the atmospheric structure and turbulence above London, including the estimation of mixed layer depths; (e) provision of new data on trace gas dispersion in the urban atmosphere through the release of purposeful tracers; (f) the determination of spatial differences in aerosol particle size distributions and their interpretation in terms of sources and physico-chemical transformations; (g) studies of the nocturnal oxidation of nitrogen oxides and of the diurnal behaviour of nitrate aerosol in the urban atmosphere, and (h) new information on the chemical composition and source apportionment of particulate matter size fractions in the atmosphere of London derived both from bulk chemical analysis and aerosol mass spectrometry with two instrument types.

Remarkable dynamics of nanoparticles in the urban atmosphere

Nanoparticles emitted from road traffic are the largest source of respiratory exposure for the general public living in urban areas. It has been suggested that adverse health effects of airborne particles may scale with airborne particle number, which if correct, focuses attention on the nanoparticle (less than 100 nm) size range which dominates the number count in urban areas. Urban measurements of particle size distributions have tended to show a broadly similar pattern dominated by a mode centred on 20–30 nm diameter emitted by diesel engine exhaust. In this paper we report the results of measurements of particle number concentration and size distribution made in a major London park as well as on the BT Tower, 160 m aloft. These measurements taken during the REPARTEE project (Regents Park and BT Tower experiment) show a remarkable shift in particle size distributions with major losses of the smallest particle class as particles are advected away from the traffic source. In the Park, the traffic related mode at 20–30 nm diameter is much reduced with a new mode at <10 nm. Size distribution measurements also revealed higher number concentrations of sub-50 nm particles at the BT Tower during days affected by higher turbulence as determined by Doppler Lidar measurements and are indicative of loss of nanoparticles from air aged during less turbulent conditions. These results are suggestive of nanoparticle loss by evaporation, rather than coagulation processes. The results have major implications for understanding the impacts of traffic-generated particulate matter on human health.

An overview on the urban boundary-layer atmosphere network in Helsinki

The Helsinki Urban Boundary-Layer Atmosphere Network (UrBAN: http://urban.fmi.fi) is a dedicated research-grade observational network where the physical processes in the atmosphere above the city are studied. Helsinki UrBAN is the most poleward intensive urban research observation network in the world and thus will allow studying some unique features such as strong seasonality. The network's key purpose is for the understanding of the physical processes in the urban boundary layer and associated fluxes of heat, momentum, moisture, and other gases. A further purpose is to secure a research-grade database, which can be used internationally to validate and develop numerical models of air quality and weather prediction. Scintillometers, a scanning Doppler lidar, ceilometers, a sodar, eddy-covariance stations, and radiometers are used. This equipment is supplemented by auxiliary measurements, which were primarily set up for general weather and/or air-quality mandatory purposes, such as vertical soundings and the operational Doppler radar network. Examples are presented as a testimony to the potential of the network for urban studies, such as (i) evidence of a stable boundary layer possibly coupled to an urban surface, (ii) the comparison of scintillometer data with sonic anemometry above an urban surface, (iii) the application of scanning lidar over a city, and (iv) combination of sodar and lidar to give a fuller range of sampling heights for boundary layer profiling.

The slowly evolving background state of the atmosphere

The theory of wave–mean flow interaction requires a partition of the atmospheric flow into a notional background state and perturbations to it. Here, a background state, known as the Modified Lagrangian Mean (MLM), is defined as the zonally symmetric state obtained by requiring that every potential vorticity (PV) contour lying within an isentropic layer encloses the same mass and circulation as in the full flow. For adiabatic and frictionless flow, these two integral properties are time-invariant and the MLM state is a steady solution of the primitive equations. The time dependence in the adiabatic flow is put into the perturbations, which can be described by a wave-activity conservation law that is exact even at large amplitude. Furthermore, the effects of non-conservative processes on wave activity can be calculated from the conservation law. A new method to calculate the MLM state is introduced, where the position of the lower boundary is obtained as part of the solution. The results are illustrated using Northern Hemisphere ERA-Interim data. The MLM state evolves slowly, implying that the net non-conservative effects are weak. Although ‘adiabatic eddy fluxes’ cannot affect the MLM state, the effects of Rossby-wave breaking, PV filamentation and subsequent dissipation result in sharpening of the polar vortex edge and meridional shifts in the MLM zonal flow, both at tropopause level and on the winter stratospheric vortex. The rate of downward migration of wave activity during stratospheric sudden warmings is shown to be given by the vertical scale associated with polar vortex tilt divided by the time-scale for wave dissipation estimated from the wave-activity conservation law. Aspects of troposphere–stratosphere interaction are discussed. The new framework is suitable to examine the climate and its interactions with disturbances, such as midlatitude storm tracks, and makes a clean partition between adiabatic and non-conservative processes.

Quantifying the role of biosphere-atmosphere feedbacks in climate change: coupled model simulation for 6000 years B.P. and comparison with palaeodata for northern Eurasia and northern Africa

The LMD AGCM was iteratively coupled to the global BIOME1 model in order to explore the role of vegetation-climate interactions in response to mid-Holocene (6000 y BP) orbital forcing. The sea-surface temperature and sea-ice distribution used were present-day and CO2 concentration was pre-industrial. The land surface was initially prescribed with present-day vegetation. Initial climate “anomalies” (differences between AGCM results for 6000 y BP and control) were used to drive BIOME1; the simulated vegetation was provided to a further AGCM run, and so on. Results after five iterations were compared to the initial results in order to identify vegetation feedbacks. These were centred on regions showing strong initial responses. The orbitally induced high-latitude summer warming, and the intensification and extension of Northern Hemisphere tropical monsoons, were both amplified by vegetation feedbacks. Vegetation feedbacks were smaller than the initial orbital effects for most regions and seasons, but in West Africa the summer precipitation increase more than doubled in response to changes in vegetation. In the last iteration, global tundra area was reduced by 25% and the southern limit of the Sahara desert was shifted 2.5 °N north (to 18 °N) relative to today. These results were compared with 6000 y BP observational data recording forest-tundra boundary changes in northern Eurasia and savana-desert boundary changes in northern Africa. Although the inclusion of vegetation feedbacks improved the qualitative agreement between the model results and the data, the simulated changes were still insufficient, perhaps due to the lack of ocean-surface feedbacks.

Freshwater transport in the coupled ocean-atmosphere system: a passive ocean

Conservation of water demands that meridional ocean and atmosphere freshwater transports (FWT) are of equal magnitude but opposite in direction. This suggests that the atmospheric FWT and its associated latent heat (LH) transport could be thought of as a \textquotedblleft coupled ocean/atmosphere mode\textquotedblright. But what is the true nature of this coupling? Is the ocean passive or active? Here we analyze a series of simulations with a coupled ocean-atmosphere-sea ice model employing highly idealized geometries but with markedly different coupled climates and patterns of ocean circulation. Exploiting streamfunctions in specific humidity coordinates for the atmosphere and salt coordinates for the ocean to represent FWT in their respective medium, we find that atmospheric FWT/LH transport is essentially independent of the ocean state. Ocean circulation and salinity distribution adjust to achieve a return freshwater pathway demanded of them by the atmosphere. So, although ocean and atmosphere FWTs are indeed coupled by mass conservation, the ocean is a passive component acting as a reservoir of freshwater.

A coupled cloud physics–radiation parameterization of the bulk optical properties of cirrus and its impact on the Met Office unified model global atmosphere 5.0 configuration

A new coupled cloud physics–radiation parameterization of the bulk optical properties of ice clouds is presented. The parameterization is consistent with assumptions in the cloud physics scheme regarding particle size distributions (PSDs) and mass–dimensional relationships. The parameterization is based on a weighted ice crystal habit mixture model, and its bulk optical properties are parameterized as simple functions of wavelength and ice water content (IWC). This approach directly couples IWC to the bulk optical properties, negating the need for diagnosed variables, such as the ice crystal effective dimension. The parameterization is implemented into the Met Office Unified Model Global Atmosphere 5.0 (GA5) configuration. The GA5 configuration is used to simulate the annual 20-yr shortwave (SW) and longwave (LW) fluxes at the top of the atmosphere (TOA), as well as the temperature structure of the atmosphere, under various microphysical assumptions. The coupled parameterization is directly compared against the current operational radiation parameterization, while maintaining the same cloud physics assumptions. In this experiment, the impacts of the two parameterizations on the SW and LW radiative effects at TOA are also investigated and compared against observations. The 20-yr simulations are compared against the latest observations of the atmospheric temperature and radiative fluxes at TOA. The comparisons demonstrate that the choice of PSD and the assumed ice crystal shape distribution are as important as each other. Moreover, the consistent radiation parameterization removes a long-standing tropical troposphere cold temperature bias but slightly warms the southern midlatitudes by about 0.5 K.

The Met Office Unified Model Global Atmosphere 3.0/3.1 and JULES Global Land 3.0/3.1 configurations

We describe Global Atmosphere 3.0 (GA3.0): a configuration of the Met Office Unified Model (MetUM) developed for use across climate research and weather prediction activities. GA3.0 has been formulated by converging the development paths of the Met Office's weather and climate global atmospheric model components such that wherever possible, atmospheric processes are modelled or parametrized seamlessly across spatial resolutions and timescales. This unified development process will provide the Met Office and its collaborators with regular releases of a configuration that has been evaluated, and can hence be applied, over a variety of modelling régimes. We also describe Global Land 3.0 (GL3.0): a configuration of the JULES community land surface model developed for use with GA3.0.

Further considerations of cosmic ray modulation of infra-red radiation in the atmosphere

Understanding effects of ionisation in the lower atmosphere is a new interdisciplinary area, crossing the traditionally distinct scientific boundaries between astro-particle and atmospheric physics and also requiring understanding of both heliospheric and magnetospheric influences on cosmic rays. Following the paper of Erlykin et al. (2014) we develop further the interpretation of our observed changes in long-wave (LW) radiation, Aplin and Lockwood (2013) by taking account of both cosmic ray ionisation yields and atmospheric radiative transfer. To demonstrate this, we show that the thermal structure of the whole atmosphere needs to be considered along with the vertical profile of ionisation. Allowing for, in particular, ionisation by all components of a cosmic ray shower and not just by the muons, reveals that the effect we have detected is certainly not inconsistent with laboratory observations of the LW absorption cross section. The analysis presented here, although very different from that of Erlykin et al., does come to the same conclusion that the events detected by AL were not caused by individual cosmic ray primaries – not because it is impossible on energetic grounds, but because events of the required energy are too infrequent for the 12 h_1 rate at which they were seen by the AL experiment. The present paper numerically models the effect of three different scenario changes to the primary GCR spectrum which all reproduce the required magnitude of the effect observed by AL. However, they cannot solely explain the observed delay in the peak effect which, if confirmed, would appear to open up a whole new and interesting area in the study of water oligomers and their effects on LW radiation. We argue that a technical artefact in the AL experiment is highly unlikely and that our initial observations merit both a wide-ranging follow-up experiment and more rigorous, self-consistent, three-dimensional radiative transfer modelling

Exploring strategies for coupled 4D-Var data assimilation using an idealised atmosphere-ocean model

Operational forecasting centres are currently developing data assimilation systems for coupled atmosphere-ocean models. Strongly coupled assimilation, in which a single assimilation system is applied to a coupled model, presents significant technical and scientific challenges. Hence weakly coupled assimilation systems are being developed as a first step, in which the coupled model is used to compare the current state estimate with observations, but corrections to the atmosphere and ocean initial conditions are then calculated independently. In this paper we provide a comprehensive description of the different coupled assimilation methodologies in the context of four dimensional variational assimilation (4D-Var) and use an idealised framework to assess the expected benefits of moving towards coupled data assimilation. We implement an incremental 4D-Var system within an idealised single column atmosphere-ocean model. The system has the capability to run both strongly and weakly coupled assimilations as well as uncoupled atmosphere or ocean only assimilations, thus allowing a systematic comparison of the different strategies for treating the coupled data assimilation problem. We present results from a series of identical twin experiments devised to investigate the behaviour and sensitivities of the different approaches. Overall, our study demonstrates the potential benefits that may be expected from coupled data assimilation. When compared to uncoupled initialisation, coupled assimilation is able to produce more balanced initial analysis fields, thus reducing initialisation shock and its impact on the subsequent forecast. Single observation experiments demonstrate how coupled assimilation systems are able to pass information between the atmosphere and ocean and therefore use near-surface data to greater effect. We show that much of this benefit may also be gained from a weakly coupled assimilation system, but that this can be sensitive to the parameters used in the assimilation.

Origin and impact of initialisation shocks in coupled atmosphere-ocean forecasts

Current methods for initialising coupled atmosphere-ocean forecasts often rely on the use of separate atmosphere and ocean analyses, the combination of which can leave the coupled system imbalanced at the beginning of the forecast, potentially accelerating the development of errors. Using a series of experiments with the European Centre for Medium-range Weather Forecasts coupled system, the magnitude and extent of these so-called initialisation shocks is quantified, and their impact on forecast skill measured. It is found that forecasts initialised by separate ocean and atmospheric analyses do exhibit initialisation shocks in lower atmospheric temperature, when compared to forecasts initialised using a coupled data assimilation method. These shocks result in as much as a doubling of root-mean-square error on the first day of the forecast in some regions, and in increases that are sustained for the duration of the 10-day forecasts performed here. However, the impacts of this choice of initialisation on forecast skill, assessed using independent datasets, were found to be negligible, at least over the limited period studied. Larger initialisation shocks are found to follow a change in either the atmospheric or ocean model component between the analysis and forecast phases: changes in the ocean component can lead to sea surface temperature shocks of more than 0.5K in some equatorial regions during the first day of the forecast. Implications for the development of coupled forecast systems, particularly with respect to coupled data assimilation methods, are discussed.

Energetic particle influence on the Earth's atmosphere

This manuscript gives an up-to-date and comprehensive overview of the effects of energetic particle precipitation (EPP) onto the whole atmosphere, from the lower thermosphere/mesosphere through the stratosphere and troposphere, to the surface. The paper summarizes the different sources and energies of particles, principally galactic cosmic rays (GCRs), solar energetic particles (SEPs) and energetic electron precipitation (EEP). All the proposed mechanisms by which EPP can affect the atmosphere are discussed, including chemical changes in the upper atmosphere and lower thermosphere, chemistry-dynamics feedbacks, the global electric circuit and cloud formation. The role of energetic particles in Earth’s atmosphere is a multi-disciplinary problem that requires expertise from a range of scientific backgrounds. To assist with this synergy, summary tables are provided, which are intended to evaluate the level of current knowledge of the effects of energetic particles on processes in the entire atmosphere.

Atmosphere-ocean coupled processes in the Madden-Julian oscillation

The Madden-Julian oscillation (MJO) is a convectively coupled 30-70 day (intraseasonal) tropical atmospheric mode that drives variations in global weather, but which is poorly simulated in most atmospheric general circulation models. Over the past two decades, field campaigns and modeling experiments have suggested that tropical atmosphere-ocean interactions may sustain or amplify the pattern of enhanced and suppressed atmospheric convection that defines the MJO, and encourage its eastward propagation through the Indian and Pacific Oceans. New observations collected during the past decade have advanced our understand of the ocean response to atmospheric MJO forcing and the resulting intraseasonal sea surface temperature (SST) fluctuations. Numerous modeling studies have revealed a considerable impact of the mean state on MJO ocean-atmosphere coupled processes, as well as the importance of resolving the diurnal cycle of atmosphere--upper-ocean interactions. New diagnostic methods provide insight to atmospheric variability and physical processes associated with the MJO, but offer limited insight on the role of ocean feedbacks. Consequently, uncertainty remains concerning the role of the ocean in MJO theory. Our understanding of how atmosphere-ocean coupled processes affect the MJO can be improved by collecting observations in poorly sampled regions of MJO activity, assessing oceanic and atmospheric drivers of surface fluxes, improving the representation of upper-ocean mixing in coupled-model simulations, designing model experiments that minimize mean-state differences, and developing diagnostic tools to evaluate the nature and role of coupled ocean-atmosphere processes over the MJO cycle.

Regionally coupled atmosphere-ocean-sea ice-marine biogeochemistry model ROM: 1. Description and validation

The general circulation models used to simulate global climate typically feature resolution too coarse to reproduce many smaller-scale processes, which are crucial to determining the regional responses to climate change. A novel approach to downscale climate change scenarios is presented which includes the interactions between the North Atlantic Ocean and the European shelves as well as their impact on the North Atlantic and European climate. The goal of this paper is to introduce the global ocean-regional atmosphere coupling concept and to show the potential benefits of this model system to simulate present-day climate. A global ocean-sea ice-marine biogeochemistry model (MPIOM/HAMOCC) with regionally high horizontal resolution is coupled to an atmospheric regional model (REMO) and global terrestrial hydrology model (HD) via the OASIS coupler. Moreover, results obtained with ROM using NCEP/NCAR reanalysis and ECHAM5/MPIOM CMIP3 historical simulations as boundary conditions are presented and discussed for the North Atlantic and North European region. The validation of all the model components, i.e., ocean, atmosphere, terrestrial hydrology, and ocean biogeochemistry is performed and discussed. The careful and detailed validation of ROM provides evidence that the proposed model system improves the simulation of many aspects of the regional climate, remarkably the ocean, even though some biases persist in other model components, thus leaving potential for future improvement. We conclude that ROM is a powerful tool to estimate possible impacts of climate change on the regional scale.

Current model capabilities for simulating black carbon and sulfate concentrations in the Arctic atmosphere: a multi-model evaluation using a comprehensive measurement data set

The concentrations of sulfate, black carbon (BC) and other aerosols in the Arctic are characterized by high values in late winter and spring (so-called Arctic Haze) and low values in summer. Models have long been struggling to capture this seasonality and especially the high concentrations associated with Arctic Haze. In this study, we evaluate sulfate and BC concentrations from eleven different models driven with the same emission inventory against a comprehensive pan-Arctic measurement data set over a time period of 2 years (2008–2009). The set of models consisted of one Lagrangian particle dispersion model, four chemistry transport models (CTMs), one atmospheric chemistry-weather forecast model and five chemistry climate models (CCMs), of which two were nudged to meteorological analyses and three were running freely. The measurement data set consisted of surface measurements of equivalent BC (eBC) from five stations (Alert, Barrow, Pallas, Tiksi and Zeppelin), elemental carbon (EC) from Station Nord and Alert and aircraft measurements of refractory BC (rBC) from six different campaigns. We find that the models generally captured the measured eBC or rBC and sulfate concentrations quite well, compared to previous comparisons. However, the aerosol seasonality at the surface is still too weak in most models. Concentrations of eBC and sulfate averaged over three surface sites are underestimated in winter/spring in all but one model (model means for January–March underestimated by 59 and 37 % for BC and sulfate, respectively), whereas concentrations in summer are overestimated in the model mean (by 88 and 44 % for July–September), but with overestimates as well as underestimates present in individual models. The most pronounced eBC underestimates, not included in the above multi-site average, are found for the station Tiksi in Siberia where the measured annual mean eBC concentration is 3 times higher than the average annual mean for all other stations. This suggests an underestimate of BC sources in Russia in the emission inventory used. Based on the campaign data, biomass burning was identified as another cause of the modeling problems. For sulfate, very large differences were found in the model ensemble, with an apparent anti-correlation between modeled surface concentrations and total atmospheric columns. There is a strong correlation between observed sulfate and eBC concentrations with consistent sulfate/eBC slopes found for all Arctic stations, indicating that the sources contributing to sulfate and BC are similar throughout the Arctic and that the aerosols are internally mixed and undergo similar removal. However, only three models reproduced this finding, whereas sulfate and BC are weakly correlated in the other models. Overall, no class of models (e.g., CTMs, CCMs) performed better than the others and differences are independent of model resolution.