Search

Nitrous oxide (N2O) is a potent long-lived greenhouse gas (GHG) and the strongest current emissions of global anthropogenic stratospheric ozone depletion weighted by its ozone depletion potential. In California, N2O is the third largest contributor to the state's anthropogenic GHG emission inventory, though no study has quantified its statewide annual emissions through top-down inverse modeling. Here we present the first annual (2013–2014) statewide top-down estimates of anthropogenic N2O emissions. Utilizing continuous N2O observations from six sites across California in a hierarchical Bayesian inversion, we estimate that annual anthropogenic emissions are 1.5–2.5 times (at 95% confidence) the state inventory (41 Gg N2O in 2014). Without mitigation, this estimate represents 4–7% of total GHG emissions assuming that other reported GHG emissions are reasonably correct. This suggests that control of N2O could be an important component in meeting California's emission reduction goals of 40% and 80% below 1990 levels of the total GHG emissions (in CO2 equivalent) by 2030 and 2050, respectively. Our seasonality analysis suggests that emissions are similar across seasons within posterior uncertainties. Future work is needed to provide source attribution for subregions and further characterization of seasonal variability.

We present an analysis of methane (CH4) emissions using atmospheric observations from 36 thirteen sites in California during June 2013 – May 2014. A hierarchical Bayesian inversion 37 method is used to estimate CH4 emissions for spatial regions (0.3° pixels for major regions) by 38 comparing measured CH4 mixing ratios with transport model (WRF-STILT) predictions based 39 on seasonally varying California-specific CH4 prior emission models. The transport model is 40 assessed using a combination of meteorological and carbon monoxide (CO) measurements 41 coupled with the gridded California Air Resources Board (CARB) carbon monoxide (CO) 42 emission inventory. Hierarchical Bayesian inversion suggests that state annual anthropogenic 43 CH4 emissions are 2.42 ± 0.49 Tg CH4/yr (at 95% confidence, including transport bias 44 uncertainty), higher (1.2 - 1.8 times) than the CARB current inventory (1.64 Tg CH4/yr in 2013). 45 We note that the estimated CH4 emissions drop to 1.0 - 1.6 times the CARB inventory if we 46 correct for the 10% median CH4 emissions assuming the bias in CO analysis is applicable to 47 CH4. The CH4 emissions from the Central Valley and urban regions (San Francisco Bay and 48 South Coast Air Basins) account for ~58% and 26% of the total posterior emissions, 49 respectively. This study suggests that the livestock sector is likely the major contributor to the 50 state total CH4 emissions, in agreement with CARB’s inventory. Attribution to source sectors for 51 sub-regions of California using additional trace gas species would further improve the 52 quantification of California’s CH4 emissions and mitigation efforts towards the California Global 53 Warming Solutions Act of 2006 (AB-32).

The yields of stabilized Criegee intermediates (sCIs), both CH2OO and CH3CHOO, produced from ozonolysis of propene at low pressures (7–16 Torr) were measured indirectly using cavity ringdown spectroscopy (CRDS) and chemical titration with an excess amount of sulfur dioxide (SO2). The method of monitoring the consumption of SO2 as a scavenger and the production of secondary formaldehyde (HCHO) allows characterization of the total sCI and the stabilized CH2OO yields at low pressure and in a short residence time. Both the total sCI and the stabilized CH2OO yields in the propene ozonolysis were found to decrease with decreasing pressure. By extrapolating the 7–16 Torr measurements to the zero-pressure limit, the nascent yield of the total sCIs was determined to be 25 ± 2%. The ranges of nascent yields of stabilized CH2OO and stabilized CH3CHOO were estimated to be 20–25% and 0–5%, respectively. The branching ratios of the stabilized and high-energy CH2OO* and CH3CHOO* were also determined. [ABSTRACT FROM AUTHOR]

The yields of stabilized Criegee intermediates (sCIs), both CH 2 OO and CH 3 CHOO, produced from ozonolysis of propene at low pressures (7-16 Torr) were measured indirectly using cavity ringdown spectroscopy (CRDS) and chemical titration with an excess amount of sulfur dioxide (SO 2 ). The method of monitoring the consumption of SO 2 as a scavenger and the production of secondary formaldehyde (HCHO) allows characterization of the total sCI and the stabilized CH 2 OO yields at low pressure and in a short residence time. Both the total sCI and the stabilized CH 2 OO yields in the propene ozonolysis were found to decrease with decreasing pressure. By extrapolating the 7-16 Torr measurements to the zero-pressure limit, the nascent yield of the total sCIs was determined to be 25 ± 2%. The ranges of nascent yields of stabilized CH 2 OO and stabilized CH 3 CHOO were estimated to be 20-25% and 0-5%, respectively. The branching ratios of the stabilized and high-energy CH 2 OO* and CH 3 CHOO* were also determined.