Showing papers by "Prasad S. Kasibhatla published in 2018"

Global impact of nitrate photolysis in sea-salt aerosol on NO x , OH, and O 3 in the marine boundary layer

Abstract: . Recent field studies have suggested that sea-salt particulate nitrate (NITs) photolysis may act as a significant local source of nitrogen oxides (NOx) over oceans. We present a study of the global impact of this process on oxidant concentrations in the marine boundary layer (MBL) using the GEOS-Chem model, after first updating the model to better simulate observed gas–particle phase partitioning of nitrate in the marine boundary layer. Model comparisons with long-term measurements of NOx from the Cape Verde Atmospheric Observatory (CVAO) in the eastern tropical North Atlantic provide support for an in situ source of NOx from NITs photolysis, with NITs photolysis coefficients about 25–50 times larger than corresponding HNO3 photolysis coefficients. Short-term measurements of nitrous acid (HONO) at this location show a clear daytime peak, with average peak mixing ratios ranging from 3 to 6 pptv. The model reproduces the general shape of the diurnal HONO profile only when NITs photolysis is included, but the magnitude of the daytime peak mixing ratio is under-predicted. This under-prediction is somewhat reduced if HONO yields from NITs photolysis are assumed to be close to unity. The combined NOx and HONO analysis suggests that the upper limit of the ratio of NITs : HNO3 photolysis coefficients is about 100. The largest simulated relative impact of NITs photolysis is in the tropical and subtropical marine boundary layer, with peak local enhancements ranging from factors of 5 to 20 for NOx, 1.2 to 1.6 for OH, and 1.1 to 1.3 for ozone. Since the spatial extent of the sea-salt aerosol (SSA) impact is limited, global impacts on NOx, ozone, and OH mass burdens are small ( ∼ 1–3 %). We also present preliminary analysis showing that particulate nitrate photolysis in accumulation-mode aerosols (predominantly over continental regions) could lead to ppbv-level increases in ozone in the continental boundary layer. Our results highlight the need for more comprehensive long-term measurements of NOx, and related species like HONO and sea-salt particulate nitrate, to better constrain the impact of particulate nitrate photolysis on marine boundary layer oxidant chemistry. Further field and laboratory studies on particulate nitrate photolysis in other aerosol types are also needed to better understand the impact of this process on continental boundary layer oxidant chemistry.

A review of land-based greenhouse gas flux estimates in Indonesia

Abstract: This study examines underlying reasons for differences among land-based greenhouse gas flux estimates in Indonesia, where six national inventories reported average emissions of between 0.4 and 1.1 Gt CO2e yr−1 over the 2000–2012 period. The large range among estimates is only somewhat smaller than Indonesia's GHG mitigation commitment. To determine the reasons for these differences, we compared input data and estimation methods, including the definitions and assumptions used for setting accounting boundaries, including emitting activities, incorporating fluxes from various carbon pools, and handling legacy fluxes. We also tested the sensitivity of methodological differences by generating our own reference emissions estimate and iteratively modifying individual components of the inventory. We found that the largest changes stem from the inclusion of legacy GHG emissions due to peat drainage (which increased emissions by at least +94% compared to the reference), methane emissions due to peat fires (+35%), and GHG emissions from belowground biomass and necromass carbon pools (+61%), modifications to assumptions of the mass of fuel burnt in peat fire events (+88%), and accounting for regrowth following a deforestation event (−31%). These differences cumulatively explain more than half of the observed difference among inventory estimates. Understanding the various approaches to emissions estimation, and how these influence the magnitude of component GHG fluxes, is an important first step towards reconciling GHG inventories. The Indonesian government's success in achieving its mitigation goal will depend on its ability to measure progress and evaluate the effectiveness of abatement actions, for which reliable harmonized greenhouse gas inventories are an essential foundation.