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Abstract In a series of 10-day campaigns in Ontario and Quebec, Canada, between 2005 and 2007, ozonesondes were launched twice daily in conjunction with continuous high-resolution wind-profiling radar measurements. Windprofilers can measure rapid changes in the height of the tropopause, and in some cases follow stratospheric intrusions. Observed stratospheric intrusions were studied with the aid of a Lagrangian particle dispersion model and the Canadian operational weather forecast system. Definite stratosphere-troposphere transport (STT) events occurred approximately every 2–3 days during the spring and summer campaigns, whereas during autumn and winter, the frequency was reduced to every 4–5 days. Although most events reached the lower troposphere, only three events appear to have significantly contributed to ozone amounts in the surface boundary layer. Detailed calculations find that STT, while highly variable, is responsible for an average, over the seven campaigns, of 3.1% of boundary layer ozone (1.2 ppb), but 13% (5.4 ppb) in the lower troposphere and 34% (22 ppb) in the middle and upper troposphere, where these layers are defined as 0–1 km, 1–3 km, and 3–8 km respectively. Estimates based on counting laminae in ozonesonde profiles, with judicious choices of ozone and relative humidity thresholds, compare moderately well, on average, with these values. The lamina detection algorithm is then applied to a large dataset from four summer ozonesonde campaigns at 18 North American sites between 2006 and 2011. The results show some site-to-site and year-to-year variability, but stratospheric ozone contributions average 4.6% (boundary layer), 15% (lower troposphere) and 26% (middle/upper troposphere). Calculations were also performed based on the TOST global 3D trajectory-mapped ozone data product. Maps of STT in the same three layers of the troposphere suggest that the STT ozone flux is greater over the North American continent than Europe, and much greater in winter and spring than in summer or fall. When averaged over all seasons, magnitudes over North America show similar ratios between levels to the previous calculations, but are overall 3–4 times smaller. This may be because of limitations (trajectory length and vertical resolution) to the current TOST-based calculation. Highlights • Wind-profiling radars measure rapid changes in tropopause height, follow intrusions • STT events every 2–3 days in spring/summer campaigns; every 4–5 days in fall/winters • STT flux estimates from RH laminae compare well with FLEXPART, but only on average • STT ozone flux is greater over North America than Europe [ABSTRACT FROM AUTHOR]

Vertical diffusion and mixing of tracers in the upper troposphere and lower stratosphere (UTLS) are not uniform, but primarily occur due to patches of turbulence that are intermittent in time and space. The effective diffusivity of regions of patchy turbulence is related to statistical parameters describing the morphology of turbulent events, such as lifetime, number, width, depth and local diffusivity (i.e., diffusivity within the turbulent patch) of the patches. While this has been recognized in the literature, the primary focus has been on well-mixed layers, with few exceptions. In such cases the local diffusivity is irrelevant, but this is not true for weakly and partially mixed layers. Here, we use both theory and numerical simulations to consider the impact of intermediate and weakly mixed layers, in addition to well-mixed layers. Previous approaches have considered only one dimension (vertical), and only a small number of layers (often one at each time step), and have examined mixing of constituents. We consider a two-dimensional case, with multiple layers (10 and more, up to hundreds and even thousands), having well-defined, non-infinite, lengths and depths. We then provide new formulas to describe cases involving well-mixed layers which supersede earlier expressions. In addition, we look in detail at layers that are not well mixed, and, as an interesting variation on previous models, our procedure is based on tracking the dispersion of individual particles, which is quite different to the earlier approaches which looked at mixing of constituents. We develop an expression which allows determination of the degree of mixing, and show that layers used in some previous models were in fact not well mixed and so produced erroneous results. We then develop a generalized model based on two dimensional random-walk theory employing Rayleigh distributions which allows us to develop a universal formula for diffusion rates for multiple two-dimensional layers with general degrees of mixing. We show that it is the largest, most vigorous and less common turbulent layers that make the major contribution to global diffusion. Finally, we make estimates of global-scale diffusion coefficients in the lower stratosphere and upper troposphere. For the lower stratosphere , κ eff ≈ 2x10 − 2 m 2 s − 1 , assuming no other processes contribute to large-scale diffusion. [ABSTRACT FROM AUTHOR]

Abstract: Longer-term (i.e., 20–40 years) tropospheric ozone (O3) time series obtained from surface and ozonesonde observations have been analyzed to assess possible changes with time through 2010. The time series have been selected to reflect relatively broad geographic regions and where possible minimize local scale influences, generally avoiding sites close to larger urban areas. Several approaches have been used to describe the changes with time, including application of a time series model, running 15-year trends, and changes in the distribution by month in the O3 mixing ratio. Changes have been investigated utilizing monthly averages, as well as exposure metrics that focus on specific parts of the distribution of hourly average concentrations (e.g., low-, mid-, and high-level concentration ranges). Many of the longer time series (∼30 years) in mid-latitudes of the Northern Hemisphere, including those in Japan, show a pattern of significant increase in the earlier portion of the record, with a flattening over the last 10–15 years. It is uncertain if the flattening of the O3 change over Japan reflects the impact of O3 transported from continental East Asia in light of reported O3 increases in China. In the Canadian Arctic, declines from the beginning of the ozonesonde record in 1980 have mostly rebounded with little overall change over the period of record. The limited data in the tropical Pacific suggest very little change over the entire record. In the southern hemisphere subtropics and mid-latitudes, the significant increase observed in the early part of the record has leveled off in the most recent decade. At the South Pole, a decline observed during the first half of the 35-year record has reversed, and O3 has recovered to levels similar to the beginning of the record. Our understanding of the causes of the longer-term changes is limited, although it appears that in the mid-latitudes of the northern hemisphere, controls on O3 precursors have likely been a factor in the leveling off or decline from earlier O3 increases. [Copyright &y& Elsevier]