Forest emissions of biogenic volatile organic compounds (BVOCs), such as isoprene and other terpenes, play a role in the production of tropospheric ozone and aerosols. In a northern Michigan forest, the direct measurement of total OH reactivity, which is the inverse of the OH lifetime, was significantly greater than expected. The difference between measured and expected OH reactivity, called the missing OH reactivity, increased with temperature, as did emission rates for terpenes and other BVOCs. These measurements are consistent with the hypothesis that unknown reactive BVOCs, perhaps terpenes, provide the missing OH reactivity.

The measurement of OH reactivity, the inverse of the OH lifetime, provides a powerful tool to investigate atmospheric photochemistry. A new airborne OH reactivity instrument was designed and deployed for the first time on the NASA DC-8 aircraft during the second phase of Intercontinental Chemical Transport Experiment-B (INTEX-B) campaign, which was focused on the Asian pollution outflow over Pacific Ocean and was based in Hawaii and Alaska. The OH reactivity was measured by adding OH, generated by photolyzing water vapor with 185 nm UV light in a moveable wand, to the flow of ambient air in a flow tube and measuring the OH signal with laser induced fluorescence. As the wand was pulled back away from the OH detector, the OH signal decay was recorded; the slope of −Δln(signal)/Δ time was the OH reactivity. The overall absolute uncertainty at the 2σ confidence levels is about 1 s⁻¹ at low altitudes (for decay about 6 s⁻¹), and 0.7 s⁻¹ at high altitudes (for decay about 2 s⁻¹). From the median vertical profile obtained in the second phase of INTEX-B, the measured OH reactivity (4.0±1.0 s⁻¹) is higher than the OH reactivity calculated from assuming that OH was in steady state (3.3±0.8 s⁻¹), and even higher than the OH reactivity that was calculated from the total measurements of all OH reactants (1.6±0.4 s⁻¹). Model calculations show that the missing OH reactivity is consistent with the over-predicted OH and under-predicted HCHO in the boundary layer and lower troposphere. The over-predicted OH and under-predicted HCHO suggest that the missing OH sinks are most likely related to some highly reactive VOCs that have HCHO as an oxidation product.

Severe haze is a major public health concern in China and India. Both countries rely heavily on coal for energy, and sulfur dioxide (SO₂) emitted from coal-fired power plants and industry is a major pollutant contributing to their air quality problems. Timely, accurate information on SO₂ sources is a required input to air quality models for pollution prediction and mitigation. However, such information has been difficult to obtain for these two countries, as fast-paced changes in economy and environmental regulations have often led to unforeseen emission changes. Here we use satellite observations to show that China and India are on opposite trajectories for sulfurous pollution. Since 2007, emissions in China have declined by 75% while those in India have increased by 50%. With these changes, India is now surpassing China as the world’s largest emitter of anthropogenic SO₂. This finding, not predicted by emission scenarios, suggests effective SO₂ control in China and lack thereof in India. Despite this, haze remains severe in China, indicating the importance of reducing emissions of other pollutants. In India, ~33 million people now live in areas with substantial SO₂ pollution. Continued growth in emissions will adversely affect more people and further exacerbate morbidity and mortality.

We use observations from the April 2008 NASA ARCTAS aircraft campaign to the North American Arctic, interpreted with a global 3-D chemical transport model (GEOS-Chem), to better understand the sources and cycling of hydrogen oxide radicals (HO_x≡H+OH+peroxy radicals) and their reservoirs (HO_y≡HO_x+peroxides) in the springtime Arctic atmosphere. We find that a standard gas-phase chemical mechanism overestimates the observed HO₂ and H₂O₂ concentrations. Computation of HO_x and HO_y gas-phase chemical budgets on the basis of the aircraft observations also indicates a large missing sink for both. We hypothesize that this could reflect HO₂ uptake by aerosols, favored by low temperatures and relatively high aerosol loadings, through a mechanism that does not produce H₂O₂. We implemented such an uptake of HO₂ by aerosol in the model using a standard reactive uptake coefficient parameterization with γ(HO₂) values ranging from 0.02 at 275 K to 0.5 at 220 K. This successfully reproduces the concentrations and vertical distributions of the different HO_x species and HO_y reservoirs. HO₂ uptake by aerosol is then a major HO_x and HO_y sink, decreasing mean OH and HO₂ concentrations in the Arctic troposphere by 32% and 31% respectively. Better rate and product data for HO₂ uptake by aerosol are needed to understand this role of aerosols in limiting the oxidizing power of the Arctic atmosphere.