Alex J. DeCaria

A cloud‐scale model study of lightning‐generated NO x in an individual thunderstorm during STERAO‐A

Understanding lightning NOx (NO 1 NO2) production on the cloud scale is key for developing better parameterizations of lightning NOx for use in regional and global chemical transport models. This paper attempts to further the understanding of lightning NOx production on the cloud scale using a cloud model simulation of an observed thunderstorm. Objectives are (1) to infer from the model simulations and in situ measurements the relative production rates of NOx by cloud-to-ground (CG) and intracloud (IC) lightning for the storm; (2) to assess the relative contributions in the storm anvil of convective transport of NOx from the boundary layer and NOx production by lightning; and (3) to simulate the effects of the lightning-generated NOx on subsequent photochemical ozone production. We use a two-dimensional cloud model that includes a parameterized source of lightning-generated NOx to study the production and advection of NOx associated with a developing northeast Colorado thunderstorm observed on July 12, 1996, during the Stratosphere-Troposphere Experiment—Radiation, Aerosols, Ozone (STERAO-A) field campaign. Model results are compared with the sum of NO measurements taken by aircraft and photostationary state estimates of NO2 in and around the anvil of the thunderstorm. The results show that IC lightning was the dominant source of NOx in this thunderstorm. We estimate from our simulations that the NOx production per CG flash (PCG) was of the order of 200 to 500 mol flash 21 .N O x production per IC flash (PIC) appeared to be half or more of that for a CG flash, a higher ratio of P IC/PCG than is commonly assumed. The results also indicate that the majority of NOx (greater than 80%) in the anvil region of this storm resulted from lightning as opposed to transport from the boundary layer. The effect of the lightning NOx on subsequent photochemical ozone production was assessed using a column chemical model initialized with values of NOx ,O 3, and hydrocarbons taken from a horizontally averaged vertical profile through the anvil of the simulated storm. The lightning NOx increased simulated ozone production rates by a maximum of over 7 ppbv d 21 in the upper troposphere downwind of this storm.

Trace gas transport and scavenging in PEM‐Tropics B South Pacific Convergence Zone convection

Analysis of chemical transport on Flight 10 of the 1999 Pacific Exploratory Mission (PEM) Tropics B mission clarifies the role of the South Pacific Convergence Zone (SPCZ) in establishing ozone and other trace gas distributions in the southwestern tropical Pacific. The SPCZ is found to be a barrier to mixing in the lower troposphere but a mechanism for convective mixing of tropical boundary layer air from northeast of the SPCZ with upper tropospheric air arriving from the west. A two-dimensional cloud-resolving model is used to quantify three critical processes in global and regional transport: convective mixing, lightning NOx production, and wet scavenging of soluble species. Very low NO and O3 tropical boundary layer air from the northeastern side of the SPCZ entered the convective updrafts and was transported to the upper troposphere where it mixed with subtropical upper tropospheric air containing much larger NO and O3 mixing ratios that had arrived from Australia. Aircraft observations show that very little NO appears to have been produced by electrical discharges within the SPCZ convection. We estimate that at least 90% of the HNO3 and H2O2 that would have been in upper tropospheric cloud outflow had been removed during transport through the cloud. Lesser percentages are estimated for less soluble species (e.g., <50% for CH3OOH). Net ozone production rates were decreased in the upper troposphere by ∼60% due to the upward transport and outflow of low-NO boundary layer air. However, this outflow mixed with much higher NO air parcels on the southwest edge of the cloud, and the mixture ultimately possessed a net ozone production potential intermediate between those of the air masses on either side of the SPCZ.