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This dissertation encompasses three projects that quantify the emissions of greenhouse gases and air pollutants from human activities. In the first project, we use the aircraft-based mass balance (MB) approach to quantify the emission of CO2 from the Baltimore, MD-Washington, D.C. (Balt-Wash) area during winter 2015. Based on analysis of aircraft observations using the MB-based top-down approach, we estimate the emission of 1.9 ± 0.3 million metric tons (MtC) of CO2 due to the combustion of fossil fuels (FFCO2) from the Balt-Wash region February 2015. Our value is 14% lower than the 2.2 ± 0.3 MtC mean estimate of FFCO2 from four bottom-up inventories often used to drive climate policy. In the second project, we investigate the declines in the emissions of CO2 and CO from the Balt-Wash area during the COVID-19 pandemic. We estimate using the MB approach applied to aircraft data that the emission of CO2 and CO declined by 29–32% and by 27–37%, respectively, from February 2020 (prior to COVID-19 lockdowns) to April – May 2020 (in the midst of COVID-19 pandemic). We show that for February 2020, two bottom-up emission inventories (EDGARv50 and the state of Maryland inventory) underestimate CO2 emissions by 13–18%, whereas two bottom-up inventories (EDGARv50 and NEI2017) overestimate the emission of CO by 54–66%. We show that the major contributor to the overestimation of the emission of CO in the bottom-up inventory is due to the mobile (i.e., cars and trucks) sector. The third project examines the emissions of CO2 and NOx from the U.S. power sector. We quantify reductions in the emissions due to the following two factors: the direct impact of COVID-19; changes in the fuel-mix profile during 2015-2020 (i.e., switching from coal to natural gas). For the contiguous U.S., we estimate the impact of COVID-19 in April 2020 to be the decline of 18±4% on the emission of CO2 and 22± 5% on the emission of NOx. For the same month, we estimate the impact of the fuel-mix transition t