As a result of photochemistry, some relationship between the stratospheric age-of-air and the amount of tracer contained within an air sample is expected. The existence of such a relationship allows inferences about transport history to be made from observations of chemical tracers. This paper lays down the conceptual foundations for the relationship between age and tracer amount, developed within a Lagrangian framework. In general, the photochemical loss depends not only on the age of the parcel but also on its path. We show that under the "average path approximation" that the path variations are less important than parcel age. The average path approximation then allows us to develop a formal relationship between the age spectrum and the tracer spectrum. Using the relation between the tracer and age spectra, tracer-tracer correlations can be interpreted as resulting from mixing which connects parts of the single path photochemistry curve, which is formed purely from the action of photochemistry on an irreducible parcel. This geometric interpretation of mixing gives rise to constraints on trace gas correlations, and explains why some observations are do not fall on rapid mixing curves. This effect is seen in the ATMOS observations. Schoeberl, M. R. and Sparling, L. and Dessler, A. and Jackman, C. H. and Fleming, E. L. Goddard Space Flight Center ...

As a result of photochemistry, some relationship between the stratospheric age-of-air and the amount of tracer contained within an air sample is expected. The existence of such a relationship allows inferences about transport history to be made from observations of chemical tracers. This paper lays down the conceptual foundations for the relationship between age and tracer amount, developed within a Lagrangian framework. In general, the photochemical loss depends not only on the age of the parcel but also on its path. We show that under the "average path approximation" that the path variations are less important than parcel age. The average path approximation then allows us to develop a formal relationship between the age spectrum and the tracer spectrum. Using the relation between the tracer and age spectra, tracer-tracer correlations can be interpreted as resulting from mixing which connects parts of the single path photochemistry curve, which is formed purely from the action of photochemistry on an irreducible parcel. This geometric interpretation of mixing gives rise to constraints on trace gas correlations, and explains why some observations are do not fall on rapid mixing curves. This effect is seen in the ATMOS observations.

Published by the American Geophysical Union as part of the Geophysical Monograph Series, Volume 200. Trajectory-based (“Lagrangian”) atmospheric transport and dispersion modeling has gained in popularity and sophistication over the previous several decades. It is common practice now for researchers around the world to apply Lagrangian models to a wide spectrum of issues. Lagrangian Modeling of the Atmosphere is a comprehensive volume that includes sections on Lagrangian modeling theory, model applications, and tests against observations. Published by the American Geophysical Union as part of the Geophysical Monograph Series. Comprehensive coverage of trajectory-based atmospheric dispersion modeling Important overview of a widely used modeling tool Sections look at modeling theory, application of models, and tests against observations

Stratosphere-troposphere exchange processes are responsible for controlling the distribution of chemically and radiatively important trace gases in the upper troposphere and lower stratosphere. Extensive characterization of exchange processes is critical to the development of our understanding and prediction of the climate system. This study examines the occurrence and dynamical and chemical characteristics related to two primary stratosphere-troposphere exchange processes: Rossby wavebreaking and moist convection. Intrusions of air from the tropical upper troposphere into the extratropical stratosphere above the subtropical jet via Rossby wavebreaking potentially have a significant impact on the composition of the lowermost stratosphere (the stratospheric part of the "middleworld"). We first present an analysis of tropospheric intrusion events observed in aircraft observations using kinematic and chemical diagnostics. The transport processes operating during each event are discussed using high-resolution model analyses and backward trajectory calculations. In situ chemical observations of the tropospheric intrusions are used to estimate the mixing timescales of the observed intrusions through use of a simple box model and trace species with different photo-chemical lifetimes. We estimate that the timescale for an intrusion to mix with the background stratospheric air is 5 to 6 days. Detailed analysis of small-scale features with tropospheric characteristics observed in the stratosphere suggests frequent irreversible transport associated with tropospheric intrusions. We also present a 30-year climatology (1981-2010) of anticyclonically and cyclonically sheared Rossby wave-breaking events along the boundary of the tropics in the 350-500 K potential temperature range from ECMWF ERA-Interim reanalyses. Lagrangian transport analyses show poleward transport at altitudes below and above the 370-390 K layer. Poleward transport at lower levels is in disagreement with previous studies and is shown to be largely dependent on the choice of tropical boundary. In addition, transport analyses reveal three modes of transport for anticyclonic wavebreaking events near the tropical tropopause (380 K): poleward, equatorward, and bidirectional. These transport modes are associated with distinct characteristics in the geometry of the mean flow. Stratospheric intrusions (tropopause folds) are known to be major contributors to stratosphere-troposphere exchange. The specific mixing processes that lead to irreversible exchange between stratospheric intrusions and the surrounding troposphere, however, are not entirely understood. This study presents direct observations of moist convection penetrating into stratospheric intrusions. The characteristics of convective injection are shown by using in situ aircraft measurements, radar reflectivities, and model analyses. Convective injection is observed at altitudes up to 5 km above the bottom of a stratospheric intrusion. Aircraft measurements show that convective injection in stratospheric intrusions can be uniquely identified by coincident observations of water vapor greater than about 100 ppmv and ozone greater than about 125 ppbv. Trajectory analyses show that convective injection can impact transport in both directions: from troposphere to stratosphere and from stratosphere to troposphere. We present a conceptual model of the synoptic meteorological conditions conducive to convective injection in stratospheric intrusions. In particular, convective injection is found to be associated with a "split front" where the upper-level frontal boundary outruns the surface cold front.