Constraining atmospheric ammonia emissions through new observations with an open-path, laser-based sensor

Abstract

As the third most abundant nitrogen species in the atmosphere, ammonia (NH3) is a key component of the global nitrogen cycle. Since the industrial revolution, humans have more than doubled the emissions of NH3 to the atmosphere by industrial nitrogen fixation, revolutionizing agricultural practices, and burning fossil fuels. NH3 is a major precursor to fine particulate matter (PM2.5), which has adverse impacts on air quality and human health. The direct and indirect aerosol radiative forcings currently constitute the largest uncertainties for future climate change predictions. Gas and particle phase NH3 eventually deposits back to the Earth's surface as reactive nitrogen, leading to the exceedance of ecosystem critical loads and perturbation of ecosystem productivity. Large uncertainties still remain in estimating the magnitude and spatiotemporal patterns of NH3 emissions from all sources and over a range of scales. These uncertainties in emissions also propagate to the deposition of reactive nitrogen. To improve our understanding of NH3 emissions, observational constraints are needed from local to global scales. The first part of this thesis is to provide quality-controlled, reliable NH3 measurements in the field using an open-path, quantum cascade laser-based NH3 sensor. As the second and third part of my research, NH3 emissions were quantified from a cattle feedlot using eddy covariance (EC) flux measurements, and the similarities between NH3 turbulent fluxes and those of other scalars (temperature, water vapor, and CO2) were investigated. The fourth part involves applying a mobile laboratory equipped with the open-path NH3 sensor and other important chemical/meteorological measurements to quantify fleet-integrated NH3 emissions from on-road vehicles. In the fifth part, the on-road measurements were extended to multiple major urban areas in both the US and China in the context of five observation campaigns. The results significantly improved current urban NH3 emission estimates. Finally, NH3 observations from the TES instrument on NASA Aura satellite were validated with mobile measurements and aircraft observations. Improved validations will help to constrain NH3 emissions at continental to global scales. Ultimately, these efforts will improve the understanding of NH3 emissions from all scales, with implications on the global nitrogen cycle and atmospheric chemistry-climate interactions.