Monika Kopacz

Intercontinental source attribution of ozone pollution at western U.S. sites using an adjoint method

[1] We use the GEOS-Chem chemical transport model and its adjoint to quantify source contributions to ozone pollution at two adjacent sites on the U.S. west coast in spring 2006: Mt. Bachelor Observatory (MBO) at 2.7 km altitude and Trinidad Head (TH) at sea level. The adjoint computes the sensitivity of ozone concentrations at the receptor sites to ozone production rates at 2° x 2.5° resolution over the history of air parcels reaching the site. MBO experiences distinct Asian ozone pollution episodes; most of the ozone production in these episodes takes place over East Asia with maxima over northeast China and southern Japan, adding to a diffuse background production distributed over the extratropical northern hemisphere. TH shows the same Asian origins for ozone as MBO but no distinct Asian pollution episodes. We find that transpacific pollution plumes transported in the free troposphere are diluted by a factor of 3 when entrained into the boundary layer, explaining why these plumes are undetectable in U.S. surface air.

Spatially Refined Aerosol Direct Radiative Forcing Efficiencies

Global aerosol direct radiative forcing (DRF) is an important metric for assessing potential climate impacts of future emissions changes. However, the radiative consequences of emissions perturbations are not readily quantified nor well understood at the level of detail necessary to assess realistic policy options. To address this challenge, here we show how adjoint model sensitivities can be used to provide highly spatially resolved estimates of the DRF from emissions of black carbon (BC), primary organic carbon (OC), sulfur dioxide (SO(2)), and ammonia (NH(3)), using the example of emissions from each sector and country following multiple Representative Concentration Pathway (RCPs). The radiative forcing efficiencies of many individual emissions are found to differ considerably from regional or sectoral averages for NH(3), SO(2) from the power sector, and BC from domestic, industrial, transportation and biomass burning sources. Consequently, the amount of emissions controls required to attain a specific DRF varies at intracontinental scales by up to a factor of 4. These results thus demonstrate both a need and means for incorporating spatially refined aerosol DRF into analysis of future emissions scenario and design of air quality and climate change mitigation policies.

Exploring CO pollution episodes observed at Rishiri Island by chemical weather simulations and AIRS satellite measurements: long-range transport of burning plumes and implications for emissions inventories.

The summer of 2003 was an active forest fire season in Siberia. Several events of elevated carbon monoxide (CO) were observed at Rishiri Island in northern Japan during an intensive field campaign in September 2003. A simulation with a global chemistry-transport model is able to reproduce the general features of the baseline levels and variability in the observed CO, and a source attribution for CO in the model suggests that the contribution from North Asia dominated, accounting for approximately 50% on average, with contributions of 7% from North America and 8% from Europe and 30% from oxidation of hydrocarbons. With consideration of recent emission estimates for East Asian fossil fuel and Siberian biomass burning sources, the model captures the timing and magnitude of the CO enhancements in two pollution episodes well (17 and 24 September). However, it significantly underestimates the amplitude during another episode (11–13 September), requiring additional CO emissions for this event. Daily satellite images from AIRS reveal CO plumes transported from western Siberia toward northern Japan. These results suggest that CO emissions from biomass burning in western Siberia in 2003 are likely underestimated in the inventory and further highlight large uncertainties in estimating trace gas emissions from boreal fires.