Is there a quantifiable relationship between lightning and nitrate deposition in the subtropics?

Lightning is a significant natural source of nitrogen oxides (NOx). The high temperatures that occur in a lightning channel fix atmospheric N2, producing nitrogen monoxide (NO) that quickly forms NO2 (NOx = NO + NO2). Lightning-produced NOx (LNOx) dominates NOx concentrations in the upper troposphere, which affect tropospheric ozone and OH concentrations and in turn the oxidizing capacity of the atmosphere. The main sink for NOx in the atmosphere is formation of nitric acid (HNO3) and subsequent deposition of nitrate (NO3-). A widely accepted estimate for the global LNOx production rate is ~5±3 TgN/yr (uncertainty of 1-20 TgN/yr). The global source term for NOx is an estimated 50 TgN/yr. Global chemical transport model studies have found that LNOx contributes to NO3- deposition (wet+dry) that is nearly equal over both land and ocean, with the greatest deposition between 30°N and 30°S. Models also predict that lightning can be the dominant source of NO3- deposition in areas where industrial sources are limited. Is it possible that an empirical relationship exists between NO3- deposition and lightning? Using 10 years of deposition, lightning, and meteorological data, we investigate the relationship between lightning and NO3- in the subtropics and assess meteorological variables that contribute significantly to the distribution of LNOx and NO3-. For NO3- deposition, we use weekly, monthly, and event-based wet deposition data from 8 coastal sites in Florida, the US Virgin Islands, and Puerto Rico (NADP); satellite and ground-based lightning data in the same region is from TRMM and Unidata; meteorology is obtained from the NCEP/NCAR Reanalysis. We use multiple linear regression in an attempt to explain variance among historical NO3- data, lightning and meteorology. We expect certain meteorological variables—particularly those related to transport and deposition—to help illuminate a relation between lightning and NO3-. The relation between NOx emissions and NO3- deposition is unclear, as is the ability to constrain NO3- sources to any given location and decouple anthropogenic versus natural effects. Our investigation addresses such questions as: from daily and monthly rain data, can total, average, or extreme precipitation events explain temporal/spatial NO3- distribution? Using numerical weather models, can regional meteorology predict NO3- deposition related to LNOx? Moreover, could such a prediction distinguish between free troposphere and planetary boundary layer sources of NO3-? How much of NO3- deposition is due to local LNOx sources versus regional transport? Quantifying the relationship between lightning and NO3- will be useful in evaluating atmospheric chemistry models, and such results could provide insight in predicting lightning-influenced NO3- deposition under future climate change scenarios. Furthermore, elucidating LNOx's impact on NO3- would provide a means to better constrain natural and anthropogenic effects on the global N cycle.