Browsing by Author "Pyle, John A."
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Item Open Access Diagnosing the radiative and chemical contributions to future changes in tropical column ozone with the UM-UKCA chemistry–climate model(2017-11-20) Keeble, James; Bednarz, Ewa M.; Banerjee, Antara; Abraham, N. Luke; Harris, Neil R. P.; Maycock, Amanda C.; Pyle, John A.Chemical and dynamical drivers of trends in tropical total-column ozone (TCO3) for the recent past and future periods are explored using the UM-UKCA (Unified Model HadGEM3-A (Hewitt et al., 2011) coupled with the United Kingdom Chemistry and Aerosol scheme) chemistry–climate model. A transient 1960–2100 simulation is analysed which follows the representative concentration pathway 6.0 (RCP6.0) emissions scenario for the future. Tropical averaged (10° S–10° N) TCO3 values decrease from the 1970s, reach a minimum around 2000 and return to their 1980 values around 2040, consistent with the use and emission of halogenated ozone-depleting substances (ODSs), and their later controls under the Montreal Protocol. However, when the ozone column is subdivided into three partial columns (PCO3) that cover the upper stratosphere (PCO3US), lower stratosphere (PCO3LS) and troposphere (PCO3T), significant differences in the temporal behaviour of the partial columns are seen. Modelled PCO3T values under the RCP6.0 emissions scenario increase from 1960 to 2000 before remaining approximately constant throughout the 21st century. PCO3LS values decrease rapidly from 1960 to 2000 and remain constant from 2000 to 2050, before gradually decreasing further from 2050 to 2100 and never returning to their 1980s values. In contrast, PCO3US values decrease from 1960 to 2000, before increasing rapidly throughout the 21st century and returning to 1980s values by ∼ 2020, and reach significantly higher values by 2100. Using a series of idealised UM-UKCA time-slice simulations with concentrations of well-mixed greenhouse gases (GHGs) and halogenated ODS species set to either year 2000 or 2100 levels, we examine the main processes that drive the PCO3 responses in the three regions and assess how these processes change under different emission scenarios. Finally, we present a simple, linearised model to describe the future evolution of tropical stratospheric column ozone values based on terms representing time-dependent abundances of GHG and halogenated ODS.Item Open Access Global modelling of the total OH reactivity: investigations on the “missing” OH sink and its atmospheric implications(European Geosciences Union (EGU) / Copernicus Publications, 2018-05-24) Ferracci, Valerio; Heimann, Ines; Abraham, N. Luke; Pyle, John A.; Archibald, Alexander T.The hydroxyl radical (OH) plays a crucial role in the chemistry of the atmosphere as it initiates the removal of most trace gases. A number of field campaigns have observed the presence of a “missing” OH sink in a variety of regions across the planet. A comparison of direct measurements of the OH loss frequency, also known as total OH reactivity (kOH), with the sum of individual known OH sinks (obtained via the simultaneous detection of species such as volatile organic compounds and nitrogen oxides) indicates that, in some cases, up to 80 % of kOH is unaccounted for. In this work, the UM-UKCA chemistry-climate model was used to investigate the wider implications of the missing reactivity on the oxidising capacity of the atmosphere. Simulations of the present-day atmosphere were performed and the model was evaluated against an array of field measurements to verify that the known OH sinks were reproduced well, with a resulting good agreement found for most species. Following this, an additional sink was introduced to simulate the missing OH reactivity as an emission of a hypothetical molecule, X, which undergoes rapid reaction with OH. The magnitude and spatial distribution of this sink were underpinned by observations of the missing reactivity. Model runs showed that the missing reactivity accounted for on average 6 % of the total OH loss flux at the surface and up to 50 % in regions where emissions of the additional sink were high. The lifetime of the hydroxyl radical was reduced by 3 % in the boundary layer, whilst tropospheric methane lifetime increased by 2 % when the additional OH sink was included. As no OH recycling was introduced following the initial oxidation of X, these results can be interpreted as an upper limit of the effects of the missing reactivity on the oxidising capacity of the troposphere. The UM-UKCA simulations also allowed us to establish the atmospheric implications of the newly characterised reactions of peroxy radicals (RO2) with OH. Whilst the effects of this chemistry on kOH were minor, the reaction of the simplest peroxy radical, CH3O2, with OH was found to be a major sink for CH3O2 and source of HO2 over remote regions at the surface and in the free troposphere. Inclusion of this reaction in the model increased tropospheric methane lifetime by up to 3 %, depending on its product branching. Simulations based on the latest kinetic and product information showed that this reaction cannot reconcile models with observations of atmospheric methanol, in contrast to recent suggestions.Item Open Access iDirac: a field-portable instrument for long-term autonomous measurements of isoprene and selected VOCs(European Geosciences Union, 2020-02-19) Bolas, Conor G.; Ferracci, Valerio; Robinson, Andrew D.; Mead, Mohammed Iqbal; Nadzir, Mohd Shahrul Mohd; Pyle, John A.; Jones, Roderic L.; Harris, Neil R. P.The iDirac is a new instrument to measure selected hydrocarbons in the remote atmosphere. A robust design is central to its specifications, with portability, power efficiency, low gas consumption and autonomy as the other driving factors in the instrument development. The iDirac is a dual-column isothermal oven gas chromatograph with photoionisation detection (GC-PID). The instrument is designed and built in-house. It features a modular design, with the novel use of open-source technology for accurate instrument control. Currently configured to measure biogenic isoprene, the system is suitable for a range of compounds. For isoprene measurements in the field, the instrument precision (relative standard deviation) is ±10 %, with a limit of detection down to 38 pmol mol−1 (or ppt). The instrument was first tested in the field in 2015 during a ground-based campaign, and has since shown itself suitable for deployment in a variety of environments and platforms. This paper describes the instrument design, operation and performance based on laboratory tests in a controlled environment as well as during deployments in forests in Malaysian Borneo and central England.