Real world and tropical cyclone world. Part I: high-resolution climate model verification

Recent global climate models with sufficient resolution and physics offer a promising approach for simulating real-world tropical cyclone (TC) statistics and their changing relationship with climate. In the first part of this study, we examine the performance of a high-resolution (;40-km horizontal grid) global climate model, the atmospheric component of the Australian Community Climate and Earth System Simulator (ACCESS) based on the Met Office Unified Model (UM8.5) Global Atmosphere (GA6.0). The atmospheric model is forced with observed sea surface temperature, and 20 years of integrations (1990–2009) are analyzed for evaluating the simulated TC statistics compared with observations. The model reproduces the observed climatology, geographical distribution, and interhemispheric asymmetry of global TC formation rates reasonably well. The annual cycle of regional TC formation rates over most basins is also well captured. However, there are some regional biases in the geographical distribution of TC formation rates. To identify the sources of these biases, a suite of model-simulated large-scale climate conditions that critically modulate TC formation rates are further evaluated, including the assessment of a multivariate genesis potential index. Results indicate that the model TC genesis biases correspond well to the inherent biases in the simulated large-scale climatic states, although the relative effects on TC genesis of some variables differs between basins. This highlights the model’s mean-state dependency in simulating accurate TC formation rates

Acid-yield measurements of the gas-phase ozonolysis of ethene as a function of humidity using Chemical Ionisation Mass Spectrometry (CIMS)

Gas-phase ethene ozonolysis experiments were conducted at room temperature to determine formic acid yields as a function of relative humidity (RH) using the integrated EXTreme RAnge chamber-Chemical Ionisation Mass Spectrometry technique, employing a CH<sub>3</sub>I ionisation scheme. RHs studied were <1, 11, 21, 27, 30 % and formic acid yields of (0.07±0.01) and (0.41±0.07) were determined at <1 % RH and 30 % RH respectively, showing a strong water dependence. It has been possible to estimate the ratio of the rate coefficient for the reaction of the Criegee biradical, CH<sub>2</sub>OO with water compared with decomposition. This analysis suggests that the rate of reaction with water ranges between 1×10<sup>−12</sup>–1×10<sup>−15</sup> cm<sup>3</sup> molecule<sup>−1</sup> s<sup>−1</sup> and will therefore dominate its loss with respect to bimolecular processes in the atmosphere. Global model integrations suggest that this reaction between CH<sub>2</sub>OO and water may dominate the production of HC(O)OH in the atmosphere

WRF-Chem model predictions of the regional impacts of N2O5 heterogeneous processes on night-time chemistry over north-western Europe

Abstract. Chemical modelling studies have been conducted over north-western Europe in summer conditions, showing that night-time dinitrogen pentoxide (N2O5) heterogeneous reactive uptake is important regionally in modulating particulate nitrate and has a~modest influence on oxidative chemistry. Results from Weather Research and Forecasting model with Chemistry (WRF-Chem) model simulations, run with a detailed volatile organic compound (VOC) gas-phase chemistry scheme and the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) sectional aerosol scheme, were compared with a series of airborne gas and particulate measurements made over the UK in July 2010. Modelled mixing ratios of key gas-phase species were reasonably accurate (correlations with measurements of 0.7–0.9 for NO2 and O3). However modelled loadings of particulate species were less accurate (correlation with measurements for particulate sulfate and ammonium were between 0.0 and 0.6). Sulfate mass loadings were particularly low (modelled means of 0.5–0.7 μg kg−1air, compared with measurements of 1.0–1.5 μg kg−1air). Two flights from the campaign were used as test cases – one with low relative humidity (RH) (60–70%), the other with high RH (80–90%). N2O5 heterogeneous chemistry was found to not be important in the low-RH test case; but in the high-RH test case it had a strong effect and significantly improved the agreement between modelled and measured NO3 and N2O5. When the model failed to capture atmospheric RH correctly, the modelled NO3 and N2O5 mixing ratios for these flights differed significantly from the measurements. This demonstrates that, for regional modelling which involves heterogeneous processes, it is essential to capture the ambient temperature and water vapour profiles. The night-time NO3 oxidation of VOCs across the whole region was found to be 100–300 times slower than the daytime OH oxidation of these compounds. The difference in contribution was less for alkenes (× 80) and comparable for dimethylsulfide (DMS). However the suppression of NO3 mixing ratios across the domain by N2O5 heterogeneous chemistry has only a very slight, negative, influence on this oxidative capacity. The influence on regional particulate nitrate mass loadings is stronger. Night-time N2O5 heterogeneous chemistry maintains the production of particulate nitrate within polluted regions: when this process is taken into consideration, the daytime peak (for the 95th percentile) of PM10 nitrate mass loadings remains around 5.6 μg kg−1air, but the night-time minimum increases from 3.5 to 4.6 μg kg−1air. The sustaining of higher particulate mass loadings through the night by this process improves model skill at matching measured aerosol nitrate diurnal cycles and will negatively impact on regional air quality, requiring this process to be included in regional models. This work was supported by the NERC RONOCO project NE/F004656/1. S. Archer-Nicholls was supported by a NERC quota studentship.This is the final version of the article. It first appeared at http://www.atmos-chem-phys.net/15/1385/2015/acp-15-1385-2015.pd

Global modelling studies of hydrogen and its isotopomers using STOCHEM-CRI:Likely radiative forcing consequences of a future hydrogen economy

A global chemistry-transport model has been employed to describe the global sources and sinks of hydrogen (H2) and its isotopomer (HD). The model is able to satisfactorily describe the observed tropospheric distributions of H2 and HD and deliver budgets and turnovers which agree with literature studies. We than go on to quantify the methane and ozone responses to emission pulses of hydrogen and their likely radiative forcing consequences. These radiative forcing consequences have been expressed on a 1 Tg basis and integrated over a hundred-year time horizon. When compared to the consequences of a 1 Tg emission pulse of carbon dioxide, 1 Tg of hydrogen causes 5 ± 1 times as much time-integrated radiative forcing over a hundred-year time horizon. That is to say, hydrogen has a global warming potential (GWP) of 5 ± 1 over a hundred-year time horizon. The global warming consequences of a hydrogen-based low-carbon energy system therefore depend critically on the hydrogen leakage rate. If the leakage of hydrogen from all stages in the production, distribution, storage and utilisation of hydrogen is efficiently curtailed, then hydrogen-based energy systems appear to be an attractive proposition in providing a future replacement for fossil-fuel based energy systems

The Common Representative Intermediates Mechanism Version 2 in the United Kingdom Chemistry and Aerosols Model

Funder: Met Office and the Natural Environment Research CouncilFunder: ESA Climate Change InitiativeAbstract: We document the implementation of the Common Representative Intermediates Mechanism version 2, reduction 5 into the United Kingdom Chemistry and Aerosol model (UKCA) version 10.9. The mechanism is merged with the stratospheric chemistry already used by the StratTrop mechanism, as used in UKCA and the UK Earth System Model, to create a new CRI‐Strat mechanism. CRI‐Strat simulates a more comprehensive treatment of non‐methane volatile organic compounds (NMVOCs) and provides traceability with the Master Chemical Mechanism. In total, CRI‐Strat simulates the chemistry of 233 species competing in 613 reactions (compared to 87 species and 305 reactions in the existing StratTrop mechanism). However, while more than twice as complex than StratTrop, the new mechanism is only 75% more computationally expensive. CRI‐Strat is evaluated against an array of in situ and remote sensing observations and simulations using the StratTrop mechanism in the UKCA model. It is found to increase production of ozone near the surface, leading to higher ozone concentrations compared to surface observations. However, ozone loss is also greater in CRI‐Strat, leading to less ozone away from emission sources and a similar tropospheric ozone burden compared to StratTrop. CRI‐Strat also produces more carbon monoxide than StratTrop, particularly downwind of biogenic VOC emission sources, but has lower burdens of nitrogen oxides as more is converted into reservoir species. The changes to tropospheric ozone and nitrogen budgets are sensitive to the treatment of NMVOC emissions, highlighting the need to reduce uncertainty in these emissions to improve representation of tropospheric chemical composition

Constraining regional greenhouse gas emissions using geostationary concentration measurements: a theoretical study

Abstract. We investigate the ability of column-integrated trace gas measurements from a geostationary satellite to constrain surface fluxes at regional scale. The proposed GEOCARB instrument measures CO2, CO and CH4 at a maximum resolution of 3 km east–west × 2.7 km north–south. Precisions are 3 ppm for CO2, 10 ppb for CO and 18 ppb for CH4. Sampling frequency is flexible. Here we sample a region at the location of Shanghai every 2 daylight hours for 6 days in June. We test the observing system by calculating the posterior uncertainty covariance of fluxes. We are able to constrain urban emissions at 3 km resolution including an isolated power plant. The CO measurement plays the strongest role; without it our effective resolution falls to 5 km. Methane fluxes are similarly well estimated at 5 km resolution. Estimating the errors for a full year suggests such an instrument would be a useful tool for both science and policy applications

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