Short-term methane emissions from two dairy farms in California estimated by different measurement techniques and US Environmental Protection Agency inventory methodology: A case study

Atmospheric top-down measurements have attributed up to twice the methane (CH4) emissions of bottom-up (BU) inventories to dairy production. We explored this discrepancy by estimating CH4 emissions of two dairy facilities in California with U.S. Environmental Protection Agency (USEPA) methodology, which is used for BU inventories, and three independent measurement techniques: 1) open-path measurements with inverse dispersion modeling (hereafter “open-path”); 2) vehicle measurements with tracer flux ratio method; and 3) aircraft measurements with closed-path method. All three techniques estimated whole farm CH4 emissions during one week in the summer of 2016. In addition, open-path also estimated whole farm CH4 emissions during two months in the winter of 2017. The objectives of the present study were: 1) to compare the different techniques to measure whole farm CH4 emissions from dairies, 2) to estimate CH4 emissions from animal housing and liquid manure storage, and compare them to USEPA inventory estimates, and 3) to compare CH4 emissions between the two dairies. Whole farm CH4 estimates were similar among measurement techniques. No seasonality was detected for CH4 emissions from animal housing, but CH4 emissions from liquid manure storage were three to six times greater during the summer than during the winter. Open-path estimates for liquid manure storage emissions were similar to monthly USEPA estimates during the summer but not during the winter, and neither open-path estimates from summer nor winter were similar to the annual USEPA estimate. Thus, CH4 emissions need to be measured throughout the year to evaluate annual inventories. Methane yields from housing and liquid manure storage were used to compare emissions between the farms. While CH4 yields from animal housing were similar (on average 20.9 g CH4/kg dry matter intake), CH4 yields from liquid manure storage at one dairy were 1.7 and 3.5 times greater than at the other dairy during summer (234 vs. 137 g CH4/kg volatile solids [VS]) and winter (78 vs. 22 g CH4/kg VS), respectively. This greater CH4 yield was attributed to the greater proportion of manure stored in liquid form, which suggests that the promotion of manure management practices that reduce the amount of manure solids stored in liquid form, such as manure separators, could significantly reduce CH4 emissions from dairies. These results demonstrate that multiple techniques for monitoring emissions on these farms were comparable

The California baseline ozone transport study (CABOTS)

Ozone is one of the six criteria pollutants identified by the U.S. Clean Air Act Amendment of 1970 as particularly harmful to human health. Concentrations have decreased markedly across the United States over the past 50 years in response to regulatory efforts, but continuing research on its deleterious effects have spurred further reductions in the legal threshold. The South Coast and San Joaquin Valley Air Basins of California remain the only two extreme ozone nonattainment areas in the United States. Further reductions of ozone in the West are complicated by significant background concentrations whose relative importance increases as domestic anthropogenic contributions decline and the national standards continue to be lowered. These background concentrations derive largely from uncontrollable sources including stratospheric intrusions, wildfires, and intercontinental transport. Taken together the exogenous sources complicate regulatory strategies and necessitate a much more precise understanding of the timing and magnitude of their contributions to regional air pollution. The California Baseline Ozone Transport Study was a field campaign coordinated across Northern and Central California during spring and summer 2016 aimed at observing daily variations in the ozone columns crossing the North American coastline, as well as the modification of the ozone layering downwind across the mountainous topography of California to better understand the impacts of background ozone on surface air quality in complex terrain

Pacific Atmospheric Sulfur Experiment (PASE): dynamics and chemistry of the south Pacific tropical trade wind regime

The Pacific Atmospheric Sulfur Experiment (PASE) was a comprehensive airborne study of the chemistry and dynamics of the tropical trade wind regime (TWR) east of the island of Kiritibati (Christmas Island, 157º, 20′ W, 2º 52′ N). Christmas Island is located due south of Hawaii. Geographically it is in the northern hemisphere yet it is 6–12º south of the intertropical convergence zone (ITCZ) which places it in the southern hemisphere meteorologically. Christmas Island trade winds in August and September are from east south east at 3–15 ms−1. Clouds, if present, are fair weather cumulus located in the middle layer of the TWR which is frequently labeled the buffer layer (BuL). PASE provided clear support for the idea that small particles (80 nm) were subsiding into the tropical trade wind regime (TWR) where sulfur chemistry transformed them to larger particles. Sulfur chemistry promoted the growth of some of these particles until they were large enough to activate to cloud drops. This process, promoted by sulfur chemistry, can produce a cooling effect due to the increase in cloud droplet density and changes in cloud droplet size. These increases in particle size observed in PASE promote additional cooling due to direct scattering from the aerosol. These potential impacts on the radiation balance in the TWR are enhanced by the high solar irradiance and ocean albedo of the TWR. Finally because of the large area involved there is a large factional impact on earth’s radiation budget. The TWR region near Christmas Island appears to be similar to the TWR that persists in August and September, from southwest of the Galapagos to at least Christmas Island. Transport in the TWR between the Galapagos and Christmas involves very little precipitation which could have removed the aerosol thus explaining at least in part the high concentrations of CCN (≈300 at 0.5% supersaturation) observed in PASE. As expected the chemistry of sulfur in the trade winds was found to be initiated by the emission of DMS into the convective boundary layer (BL, the lowest of three layers). However, the efficiency with which this DMS is converted to SO2 has been brought into further question by this study. This unusual result has come about as result of our using two totally different approaches for addressing this long standing question. In the first approach, based on accepted kinetic rate constants and detailed steps for the oxidation of DMS reflecting detailed laboratory studies, a DMS to SO2 conversion efficiency of 60–73% was determined. This range of values lies well within the uncertainties of previous studies. However, using a completely different approach, involving a budget analysis, a conversion value of 100% was estimated. The latter value, to be consistent with all other sulfur studies, requires the existence of a completely independent sulfur source which would emit into the atmosphere at a source strength approximately half that measured for DMS under tropical Pacific conditions. At this time, however, there is no credible scientific observation that identifies what this source might be. Thus, the current study has opened for future scientific investigation the major question: is there yet another major tropical marine source of sulfur? Of equal importance, then, is the related question, is our global sulfur budget significantly in error due to the existence of an unknown marine source of sulfur? Pivotal to both questions may be gaining greater insight about the intermediate DMS oxidation species, DMSO, for which rather unusual measurements have been reported in previous marine sulfur studies. The 3 pptv bromine deficit observed in PASE must be lost over the lifetime of the aerosol which is a few days. This observation suggests that the primary BrO production rate is very small. However, considering the uncertainties in these observations and the possible importance of secondary production of bromine radicals through aerosol surface reactions, to completely rule out the importance of bromine chemistry under tropical conditions at this time cannot be justified. This point has been brought into focus from prior work that even at levels of 1 pptv, the effect of BrO oxidation on DMS can still be quite significant. Thus, as in the case of DMS conversion to SO2, future studies will be needed. In the latter case there will need to be a specific focus on halogen chemistry. Such studies clearly must involve specific measurements of radical species such as BrO

The BLLAST field experiment: Boundary-Layer late afternoon and sunset turbulence

Due to the major role of the sun in heating the earth's surface, the atmospheric planetary boundary layer over land is inherently marked by a diurnal cycle. The afternoon transition, the period of the day that connects the daytime dry convective boundary layer to the night-time stable boundary layer, still has a number of unanswered scientific questions. This phase of the diurnal cycle is challenging from both modelling and observational perspectives: it is transitory, most of the forcings are small or null and the turbulence regime changes from fully convective, close to homogeneous and isotropic, toward a more heterogeneous and intermittent state. These issues motivated the BLLAST (Boundary-Layer Late Afternoon and Sunset Turbulence) field campaign that was conducted from 14 June to 8 July 2011 in southern France, in an area of complex and heterogeneous terrain. A wide range of instrumented platforms including full-size aircraft, remotely piloted aircraft systems, remote-sensing instruments, radiosoundings, tethered balloons, surface flux stations and various meteorological towers were deployed over different surface types. The boundary layer, from the earth's surface to the free troposphere, was probed during the entire day, with a focus and intense observation periods that were conducted from midday until sunset. The BLLAST field campaign also provided an opportunity to test innovative measurement systems, such as new miniaturized sensors, and a new technique for frequent radiosoundings of the low troposphere. Twelve fair weather days displaying various meteorological conditions were extensively documented during the field experiment. The boundary-layer growth varied from one day to another depending on many contributions including stability, advection, subsidence, the state of the previous day's residual layer, as well as local, meso- or synoptic scale conditions. Ground-based measurements combined with tethered-balloon and airborne observations captured the turbulence decay from the surface throughout the whole boundary layer and documented the evolution of the turbulence characteristic length scales during the transition period. Closely integrated with the field experiment, numerical studies are now underway with a complete hierarchy of models to support the data interpretation and improve the model representations.publishedVersio

The impacts of wildfires on ozone production and boundary layer dynamics in California's Central Valley

We investigate the role of wildfire smoke on ozone photochemical production (P(O3)) and atmospheric boundary layer (ABL) dynamics in California's Central Valley during June-September from 2016 to 2020. Wildfire events are identified by the Hazard Mapping System (HMS) and the Hybrid Single Particle Lagrangian Integrated Trajectory Model (HYSPLIT). Air quality and meteorological data are analyzed from 10 monitoring sites operated by the California Air Resources Board (CARB) across the Central Valley. On average, wildfires were found to influence air quality in the Central Valley on about 20% of the total summer days of the study. During wildfire-influenced periods, maximum daily 8h averaged (MDA8) O3 was enhanced by about 5.5ppb or 10% of the median MDA8 (once corrected for the slightly warmer temperatures) over the entire valley. Overall, nearly half of the total exceedances of the National Ambient Air Quality Standards (NAAQS) where MDA8 O3>70ppb occur under the influence of wildfires, and approximately 10% of those were in exceedance by 5ppb or less indicating circumstances that would have been in compliance with the NAAQS were it not for wildfire emissions. The photochemical ozone production rate calculated from the modified Leighton relationship was also found to be higher by 50% on average compared with non-fire periods despite the average diminution of j(NO2) by1/47% due to the shading effect of the wildfire smoke plumes. Surface heat flux measurements from two AmeriFlux sites in the northern San Joaquin Valley show midday surface buoyancy fluxes decrease by 30% on average when influenced by wildfire smoke. Similarly, afternoon peak ABL heights measured from a radio acoustic sounding system (RASS) located in Visalia in the southern San Joaquin Valley were found to decrease on average by 80m (1/415%) with a concomitant reduction of downwelling shortwave radiation of 54Wm-2, consistent with past observations of the dependence of boundary layer heights on insolation

Satellite NO2 trends reveal pervasive impacts of wildfire and soil emissions across California landscapes

Nitrogen dioxide (NO2) plays a pivotal role in the production of secondary pollutants, most importantly ozone (O3) and particulate matter. Regulatory controls have greatly reduced NO2 in cities, where most of the surface monitoring occurs, but the change in rural environments is less certain. Here, we present summertime (June-September) spatio-temporal patterns of NO2 concentrations using satellite and ground observations across California from 2009-2020, quantifying the differences in NO2 trends for five distinct land cover classes: urban, forests, croplands, scrublands (shrublands, savannas, and grasslands), and barren (minimally vegetated) lands. Over urban environments, NO2 columns exhibited continued but weakening downward trends (−3.7 ± 0.3%a−1), which agree fairly well with contemporaneous trends estimated from the surface air quality network (−4.5 ± 0.5%a−1). In rural (i.e., non-urban) parts of the state, however, secular trends are insignificant (0.0-0.4 ± 0.4%a−1) or in the case of remote forests are rapidly on the rise (+4.2 ± 1.2%a−1). Sorting the NO2 columns by air temperature and soil moisture reveals relationships that are commensurate with extant parameterizations but do indicate a stronger temperature dependence. We further find that rapidly rising temperatures and, to a lesser extent, decreasing precipitation in response to climate change are acting to increase soil NO x emissions, explaining about one-third of the observed NO2 rise in non-urban regions across California. Finally, we show that these trends, or their absence, can be attributed predominantly to the dramatic rise in wildfire frequency, especially since the turn of the 21st century