Articles | Volume 16, issue 3
Atmos. Chem. Phys., 16, 1459–1477, 2016
Atmos. Chem. Phys., 16, 1459–1477, 2016

Research article 09 Feb 2016

Research article | 09 Feb 2016

Sensitivity of nitrate aerosols to ammonia emissions and to nitrate chemistry: implications for present and future nitrate optical depth

F. Paulot1,2, P. Ginoux1, W. F. Cooke1, L. J. Donner1, S. Fan1, M.-Y. Lin1,2, J. Mao1,2, V. Naik3, and L. W. Horowitz1 F. Paulot et al.
  • 1Geophysical Fluid Dynamics Laboratory, National Oceanic and Atmospheric Administration, Princeton, New Jersey, USA
  • 2Program in Atmospheric and Oceanic Sciences, Princeton University, New Jersey, USA
  • 3UCAR, National Oceanic and Atmospheric Administration, Princeton, New Jersey, USA

Abstract. We update and evaluate the treatment of nitrate aerosols in the Geophysical Fluid Dynamics Laboratory (GFDL) atmospheric model (AM3). Accounting for the radiative effects of nitrate aerosols generally improves the simulated aerosol optical depth, although nitrate concentrations at the surface are biased high. This bias can be reduced by increasing the deposition of nitrate to account for the near-surface volatilization of ammonium nitrate or by neglecting the heterogeneous production of nitric acid to account for the inhibition of N2O5 reactive uptake at high nitrate concentrations. Globally, uncertainties in these processes can impact the simulated nitrate optical depth by up to 25 %, much more than the impact of uncertainties in the seasonality of ammonia emissions (6 %) or in the uptake of nitric acid on dust (13 %). Our best estimate for fine nitrate optical depth at 550 nm in 2010 is 0.006 (0.005–0.008). In wintertime, nitrate aerosols are simulated to account for over 30 % of the aerosol optical depth over western Europe and North America. Simulated nitrate optical depth increases by less than 30 % (0.0061–0.010) in response to projected changes in anthropogenic emissions from 2010 to 2050 (e.g., −40 % for SO2 and +38 % for ammonia). This increase is primarily driven by greater concentrations of nitrate in the free troposphere, while surface nitrate concentrations decrease in the midlatitudes following lower concentrations of nitric acid. With the projected increase of ammonia emissions, we show that better constraints on the vertical distribution of ammonia (e.g., convective transport and biomass burning injection) and on the sources and sinks of nitric acid (e.g., heterogeneous reaction on dust) are needed to improve estimates of future nitrate optical depth.

Short summary
We characterize the sensitivity of NO3 optical depth (OD) to both the sources of its precursors (NH3 and HNO3) and to its surface sinks. Uncertainties in the heterogeneous chemistry of HNO3 and the near-surface volatilization of NH4NO3 can cause up to 25 % difference in the global NO3 OD. Simulated NO3 OD increases little (< 30 %) in response to changes in emissions (2010 to 2050). Better constraints on the tropical flux of NH3 into the free troposphere are needed to improve estimates of NO3 OD.
Final-revised paper