1Division of Engineering and Applied Sciences, California Institute of Technology, Pasadena, California, USA
2Department of Mechanical Engineering, University of Colorado, Boulder, Colorado, USA
3Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, California, USA
*now at: Harvard University Center for the Environment, Harvard University, Cambridge, Massachusetts, USA
Received: 20 Jul 2011 – Published in Atmos. Chem. Phys. Discuss.: 13 Sep 2011
Abstract. Tropical tropospheric ozone affects Earth's radiative forcing and the oxidative capacity of the atmosphere. Considerable work has been devoted to the study of the processes controlling its budget. Yet, large discrepancies between simulated and observed tropical tropospheric ozone remain. Here, we characterize some of the mechanisms by which the photochemistry of isoprene impacts the budget of tropical ozone. At the regional scale, we use forward sensitivity simulation to explore the sensitivity to the representation of isoprene nitrates. We find that isoprene nitrates can account for up to 70% of the local NOx = NO+NO2 sink. The resulting modulation of ozone can be well characterized by their net modulation of NOx. We use adjoint sensitivity simulations to demonstrate that the oxidation of isoprene can affect ozone outside of continental regions through the transport of NOx over near-shore regions (e.g., South Atlantic) and the oxidation of isoprene outside of the boundary layer far from its emissions regions. The latter mechanism is promoted by the simulated low boundary-layer oxidative conditions. In our simulation, ~20% of the isoprene is oxidized above the boundary layer in the tropics. Changes in the interplay between regional and global effect are discussed in light of the forecasted increase in anthropogenic emissions in tropical regions.
Revised: 22 Dec 2011 – Accepted: 13 Jan 2012 – Published: 02 Feb 2012
Paulot, F., Henze, D. K., and Wennberg, P. O.: Impact of the isoprene photochemical cascade on tropical ozone, Atmos. Chem. Phys., 12, 1307-1325, doi:10.5194/acp-12-1307-2012, 2012.