Transport and Distribution of the Short-Lived Halocarbons in the Tropical Tropopause Layer in the Pacific Ocean: the Role of Convection

Abstract

This PhD thesis investigates the transport and distribution of short-lived halogenated organic substances in the tropical tropopause layer (TTL) in the Pacific Ocean. Short-lived halocarbons are one of the major groups of the ozone depleting substances as they provide a source for the active halogens which decrease ozone in the atmosphere. The TTL serves as the primary gateway of tropospheric air to enter the stratosphere. The air which enters the stratosphere is distributed all over the globe. Thus, the research on which tropospheric air masses go into the TTL, its structure and composition and the transport within is crucial.

This thesis uses the UK Meteorological Office Lagrangian particle dispersion model NAME to (i) support the flight planning activities and achieve the multi aircraft coordination in CAST, CONTRAST, ATTREX 2014 campaigns, and (ii) quantify the amount and distribution of short-lived halocarbons in the TTL, and explain differences in these vertical distributions and transport characteristics. The halocarbons of interest are methyl iodide (CH3I), bromoform (CHBr3) and dibromomethane (CH2Br2).

A new NAME procedure was developed and operated successfully to provide routine simulations and near real-time products suitable for guiding the CAST, CONTRAST and ATTREX aircraft in order to achieve their mission scientific objectives, and to make coordinated measurements.

NAME was used post-campaign to analyse distribution of short-lived halocarbons in the TTL, identify their source regions and transport timescales. A new approach is proposed to investigate the TTL composition in terms of the boundary layer air influence, and subsequently quantify CH3I, CHBr3 and CH2Br2 by estimating their boundary layer and background contribution. The sums of these modelled estimates are in good agreement with the ATTREX 2014 and 2013 CH3I, CHBr3 and CH2Br2 observations. The quantification of the contribution of short-lived bromocarbons to the active bromine in the TTL was achieved, and the results lie within the range of the recent literature studies.

The final focus of this thesis is on how well NAME represents the particle displacement via convection. Convection is the major transport pathway for the short-lived halocarbons to reach the TTL. The role of convection in transporting CH3I, CHBr3 and CH2Br2 to the TTL is assessed using the new convection scheme in NAME. A validation of the performance of this scheme is provided, showing that it yields improved and more realistic representation of the particle displacement via convection.