The CO2 tracer clock for the Tropical Tropopause Layer

Observations of CO2 were made in the upper troposphere and lower stratosphere in the deep tropics in order to determine the patterns of large-scale vertical transport and age of air in the Tropical Tropopause Layer (TTL). Flights aboard the NASA WB-57F aircraft over Central America and adjacent ocean areas took place in January and February, 2004 (Pre-AURA Validation Experiment, Pre-AVE) and 2006 (Costa Rice AVE, CR-AVE), and for the same flight dates of 2006, aboard the Proteus aircraft from the surface to 15 km over Darwin, Australia (Tropical Warm Pool International Cloud Experiment, TWP-ICE). The data demonstrate that the TTL is composed of two layers with distinctive features: (1) the lower TTL, 350-360 K (potential temperature(theta); approximately 12-14 km), is subject to inputs of convective outflows, as indicated by layers of variable CO2 concentrations, with air parcels of zero age distributed throughout the layer; (2) the upper TTL, from theta=similar to 360 K to similar to 390 K (14-18 km), ascends slowly and ages uniformly, as shown by a linear decline in CO2 mixing ratio tightly correlated with altitude, associated with increasing age. This division is confirmed by ensemble trajectory analysis. The CO2 concentration at the level of 360 K was 380.0(+/-0.2) ppmv, indistinguishable from surface site values in the Intertropical Convergence Zone (ITCZ) for the flight dates. Values declined with altitude to 379.2(+/-0.2) ppmv at 390 K, implying that air in the upper TTL monotonically ages while ascending. In combination with the winter slope of the CO2 seasonal cycle (+10.8+?-0.4 ppmv/yr), the vertical gradient of -0.78 (+/-0.09) ppmv gives a mean age of 26(+/-3) days for the air at 390 K and a mean ascent rate of 1.5(+/-0.3) mm s(-1). The TTL near 360 K in the Southern Hemisphere over Australia is very close in CO2 composition to the TTL in the Northern Hemisphere over Costa Rica, with strong contrasts emerging at lower altitudes (<360 K). Both Pre-AVE and CR-AVE CO2 observed unexpected input from deep convection over Amazonia deep into the TTL. The CO2 data confirm the operation of a highly accurate tracer clock in the TTL that provides a direct measure of the ascent rate of the TTL and of the age of air entering the stratosphere.