Fluxes of Atmospheric Greenhouse-Gases in Maryland (FLAGG-MD): Emissions of Carbon Dioxide in the Baltimore, MD-Washington, D.C. area.

To study emissions of CO2 in the Baltimore, MD-Washington, D.C. (Balt-Wash) area, an aircraft campaign was conducted in February 2015, as part of the FLAGG-MD (Fluxes of Atmospheric Greenhouse-Gases in Maryland) project. During the campaign, elevated mole fractions of CO2 were observed downwind of the urban center and local power plants. Upwind flight data and HYSPLIT (Hybrid Single Particle Lagrangian Integrated Trajectory) model analyses help account for the impact of emissions outside the Balt-Wash area. The accuracy, precision, and sensitivity of CO2 emissions estimates based on the mass balance approach were assessed for both power plants and cities. Our estimates of CO2 emissions from two local power plants agree well with their CEMS (Continuous Emissions Monitoring Systems) records. For the 16 power plant plumes captured by the aircraft, the mean percentage difference of CO2 emissions was -0.3 %. For the Balt-Wash area as a whole, the 1σ CO2 emission rate uncertainty for any individual aircraft-based mass balance approach experiment was ±38 %. Treating the mass balance experiments, which were repeated seven times within nine days, as individual quantifications of the Balt-Wash CO2 emissions, the estimation uncertainty was ±16 % (standard error of the mean at 95% CL). Our aircraft-based estimate was compared to various bottom-up fossil fuel CO2 (FFCO2) emission inventories. Based on the FLAGG-MD aircraft observations, we estimate 1.9±0.3 MtC of FFCO2 from the Balt-Wash area during the month of February 2015. The mean estimate of FFCO2 from the four bottom-up models was 2.2±0.3 MtC.

Increased atmospheric ammonia over the world's major agricultural areas detected from space.

This study provides evidence of substantial increases in atmospheric ammonia (NH3) concentrations (14-year) over several of the worlds major agricultural regions, using recently available retrievals from the Atmospheric Infrared Sounder (AIRS) aboard NASA's Aqua satellite. The main sources of atmospheric NH3 are farming and animal husbandry involving reactive nitrogen ultimately derived from fertilizer use; rates of emission are also sensitive to climate change. Significant increasing trends are seen over the US (2.61% yr-1), the European Union (EU) (1.83% yr-1), and China (2.27% yr-1). Over the EU, the trend results from decreased scavenging by acid aerosols. Over the US, the increase results from a combination of decreased chemical loss and increased soil temperatures. Over China, decreased chemical loss, increasing temperatures, and increased fertilizer use all play a role. Over South Asia, increased NH3 emissions are masked by increased SO2 and NOx emissions, leading to increased aerosol loading and adverse health effects.

The Indian Ocean experiment: widespread air pollution from South and Southeast Asia.

The Indian Ocean Experiment (INDOEX) was an international, multiplatform field campaign to measure long-range transport of air pollution from South and Southeast Asia toward the Indian Ocean during the dry monsoon season in January to March 1999. Surprisingly high pollution levels were observed over the entire northern Indian Ocean toward the Intertropical Convergence Zone at about 6 degrees S. We show that agricultural burning and especially biofuel use enhance carbon monoxide concentrations. Fossil fuel combustion and biomass burning cause a high aerosol loading. The growing pollution in this region gives rise to extensive air quality degradation with local, regional, and global implications, including a reduction of the oxidizing power of the atmosphere.

A photothermal interferometer for gas-phase ammonia detection.

Detection of gas-phase ammonia is particularly challenging because ambient ammonia concentrations may be less than 1 ppb (molecules of NH(3) per 10(9) molecules of air), ammonia sticks to many materials commonly used to sample air, and particles containing ammonium may interfere with gas-phase measurements. We have built a new and sensitive photothermal interferometer to detect gas-phase ammonia in situ, under typical atmospheric conditions. Ammonia molecules in sampled air absorb infrared radiation from a CO(2) laser at 9.22 µm, with consequent collisional heating, expansion, and refractive index change. This change in refractive index is detected as a phase shift in one arm of a homodyne interferometer. Measurements of vibrational and electrical noise in the interferometer correlate to an instrumental lower limit of detection of 6.6 ppt ammonia in 1 s. The CO(2) laser output is modulated at 1.2 kHz, and the ac signal from the interferometer is measured with a lock-in amplifier. The detector is zeroed by sampling through a H(3)PO(4)-coated denuder tube and is calibrated by dynamic dilution of two permeation tube outputs and by standard addition. Signal gain is insensitive to CO(2) or H(2)O in the sample, and the signal is linear over 5 orders of magnitude. The instrument 2σ precision is 31 ppt when the signal is integrated for 100 s and 250 ppt with a 1-s integration time. The windowless sample cell and inlet is fabricated entirely of glass to minimize sample loss and hysteresis. The instrument response time is demonstrated to be about 1 s.

Pollutant transport during a regional O3-episode in the mid-Atlantic states.

Ozone (O3) concentrations in the Baltimore-Washington (B-W) metropolitan area frequently exceed the National Ambient Air Quality Standard (NAAQS) in the summer months. The most extreme O3 events occur in multi-day high O3 episodes. These events can be regional in scale, with O3 concentrations exceeding the NAAQS at numerous locations along the eastern U.S. seaboard, and are typically associated with slow-moving or stagnant high pressure systems. In the B-W region, the most extreme events typically occur with surface high pressure overhead or just west of the region and an upper air high-pressure area (ridge) to the west or northwest. Besides providing conditions conductive to local O3 production (subsidence and strong low-level inversions, weak horizontal winds, little cloud cover), this weather pattern may also result in transport of O3 and its precursors from heavily industrialized areas west and north of the B-W region. In this paper, observations and back trajectories made during the severe regional O3 event of July 12-15, 1995, are used to confirm the hypothesis that significant regional-scale transport of O3 and its precursors occur during extreme O3 events of the standard type in the B-W area.

The impact of aerosols on solar ultraviolet radiation and photochemical smog.

Photochemical smog, or ground-level ozone, has been the most recalcitrant of air pollution problems, but reductions in emissions of sulfur and hydrocarbons may yield unanticipated benefits in air quality. While sulfate and some organic aerosol particles scatter solar radiation back into space and can cool Earth's surface, they also change the actinic flux of ultraviolet (UV) radiation. Observations and numerical models show that UV-scattering particles in the boundary layer accelerate photochemical reactions and smog production, but UV-absorbing aerosols such as mineral dust and soot inhibit smog production. Results could have major implications for the control of air pollution.

Thunderstorms: an important mechanism in the transport of air pollutants.

Acid deposition and photochemical smog are urban air pollution problems, and they remain localized as long as the sulfur, nitrogen, and hydrocarbon pollutants are confined to the lower troposphere (below about 1-kilometer altitude) where they are short-lived. If, however, the contaminants are rapidly transported to the upper troposphere, then their atmospheric residence times grow and their range of influence expands dramatically. Although this vertical transport ameliorates some of the effects of acid rain by diluting atmospheric acids, it exacerbates global tropospheric ozone production by redistributing the necessary nitrogen catalysts. Results of recent computer simulations suggest that thunderstorms are one means of rapid vertical transport. To test this hypothesis, several research aircraft near a midwestern thunderstrom measured carbon monoxide, hydrocarbons, ozone, and reactive nitrogen compounds. Their concentrations were much greater in the outflow region of the storm, up to 11 kilometers in altitude, than in surrounding air. Trace gas measurements can thus be used to track the motion of air in and around a cloud. Thunderstorms may transform local air pollution problems into regional or global atmospheric chemistry problems.

Qualitative and quantitative flow visualization technique using ozone.

We have developed a new flow-visualization technique based on the absorption of ultraviolet light by ozone. Ozone is an excellent tracer, because as a gas it has the same effective physical properties as air. Ozone strongly absorbs the principal line (253.7 nm) of a mercury lamp, varepsilon=310 (atm cm)(-1), where I/Io=exp(-varepsiloncl) such that when an ozone-traced flow passes between a mercury lamp and a fluorescent screen, a sharp, shadow-like image of the ozone tracer is cast on the screen. Quantitative photometry can be carried out by replacing the screen with ultraviolet detectors that yield the path-integrated column density of ozone in the flow. High-speed quantitative point monitoring (10 Hz at 10 ppb O3) is possible with capillary probes and chemiluminescent analysis.