The influence of stratosphere‐to‐troposphere transport (STT) on surface ozone (O3) concentrations in the greater Los Angeles area during the CalNex and IONS‐2010 measurement campaigns has been ...investigated. Principal component analysis (PCA) of surface O3measurements from 41 sampling stations indicates that ∼13% of the variance in the maximum daily 8‐h average (MDA8) O3between May 10 and June 19, 2010 was associated with changes of 2–3 day duration linked to the passage of upper‐level troughs. Ozonesondes launched from Joshua Tree National Park and airborne lidar measurements show that these changes coincided with the appearance of stratospheric intrusions in the lower troposphere above southern California. The Lagrangian particle dispersion model FLEXPART reproduces most of these intrusions, and supports the conclusion from the PCA that significant transport of stratospheric air to the surface occurred on May 28–30. This intrusion led to a peak 1‐h O3 concentration of 88 ppbv at Joshua Tree National Monument near the ozonesonde launch site on May 28, and widespread entrainment of stratospheric air into the boundary layer increased the local background O3 over the entire area to ∼55 ppbv on May 29–30. This background was 10–15 ppbv higher than the baseline O3 in air transported ashore from the Pacific Ocean, and when combined with locally produced O3 led to several exceedances of the current National Ambient Air Quality Standard (NAAQS) on the following day.
Key Points
Stratosphere‐troposphere transport can influence surface ozone
Background ozone must be considered in urban areas
Transport cannot be neglected in air quality studies
A single-particle soot photometer (SP2) was flown on a NASA WB-57F high-altitude research aircraft in November 2004 from Houston, Texas. The SP2 uses laser-induced incandescence to detect individual ...black carbon (BC) particles in an air sample in the mass range of approx.3-300 fg (approx.0.15-0.7 microns volume equivalent diameter). Scattered light is used to size the remaining non-BC aerosols in the range of approx.0.17-0.7 microns diameter. We present profiles of both aerosol types from the boundary layer to the lower stratosphere from two midlatitude flights. Results for total aerosol amounts in the size range detected by the SP2 are in good agreement with typical particle spectrometer measurements in the same region. All ambient incandescing particles were identified as BC because their incandescence properties matched those of laboratory-generated BC aerosol. Approximately 40% of these BC particles showed evidence of internal mixing (e.g., coating). Throughout profiles between 5 and 18.7 km, BC particles were less than a few percent of total aerosol number, and black carbon aerosol (BCA) mass mixing ratio showed a constant gradient with altitude above 5 km. SP2 data was compared to results from the ECHAM4/MADE and LmDzT-INCA global aerosol models. The comparison will help resolve the important systematic differences in model aerosol processes that determine BCA loadings. Further intercomparisons of models and measurements as presented here will improve the accuracy of the radiative forcing contribution from BCA.
We describe a two-channel broadband cavity enhanced absorption spectrometer (BBCEAS) for aircraft measurements of glyoxal (CHOCHO), methylglyoxal (CH3COCHO), nitrous acid (HONO), nitrogen dioxide ...(NO2), and water (H2O). The instrument spans 361–389 and 438–468 nm, using two light-emitting diodes (LEDs) and a single grating spectrometer with a charge-coupled device (CCD) detector. Robust performance is achieved using a custom optical mounting system, high-power LEDs with electronic on/off modulation, high-reflectivity cavity mirrors, and materials that minimize analyte surface losses. We have successfully deployed this instrument during two aircraft and two ground-based field campaigns to date. The demonstrated precision (2σ) for retrievals of CHOCHO, HONO and NO2 are 34, 350, and 80 parts per trillion (pptv) in 5 s. The accuracy is 5.8, 9.0, and 5.0 %, limited mainly by the available absorption cross sections.
The Santa Ana winds of Southern California have long been associated with wildland fires that can adversely affect air quality and lead to loss of life and property. These katabatic winds are driven ...primarily by thermal gradients but can be exacerbated by northerly flow associated with upper level troughs passing through the western U.S. In this paper, we show that the fire danger associated with the passage of upper level troughs can be further increased by the formation of deep tropopause folds that transport extremely dry ozone‐rich air from the upper troposphere and lower stratosphere to the surface. Stratospheric intrusions can thus increase surface ozone both directly through transport and indirectly through their influence on wildland fires. We illustrate this situation with the example of the Springs Fire, which burned nearly 25,000 acres in Ventura County during May 2013.
Key Points
Synoptic flow associated with stratospheric intrusions can force Santa Ana winds
Descent of dry lower stratospheric air to the surface can foment wildfires
Stratospheric intrusions can indirectly increase ozone by exacerbating wildfires
The 2013 Las Vegas Ozone Study (LVOS) was conducted in the late spring and early summer of 2013 to assess the seasonal contribution of stratosphere-to-troposphere transport (STT) and long-range ...transport to surface ozone in Clark County, Nevada and determine if these processes directly contribute to exceedances of the National Ambient Air Quality Standard (NAAQS) in this area. Secondary goals included the characterization of local ozone production, regional transport from the Los Angeles Basin, and impacts from wildfires. The LVOS measurement campaign took place at a former U.S. Air Force radar station ∼45 km northwest of Las Vegas on Angel Peak (∼2.7 km above mean sea level, asl) in the Spring Mountains. The study consisted of two extended periods (May 19–June 4 and June 22–28, 2013) with near daily 5-min averaged lidar measurements of ozone and backscatter profiles from the surface to ∼2.5 km above ground level (∼5.2 km asl), and continuous in situ measurements (May 20–June 28) of O3, CO, (1-min) and meteorological parameters (5-min) at the surface. These activities were guided by forecasts and analyses from the FLEXPART (FLEXible PARTticle) dispersion model and the Real Time Air Quality Modeling System (RAQMS), and the NOAA Geophysical Research Laboratory (NOAA GFDL) AM3 chemistry-climate model. In this paper, we describe the LVOS measurements and present an overview of the results. The combined measurements and model analyses show that STT directly contributed to each of the three O3 exceedances that occurred in Clark County during LVOS, with contributions to 8-h surface concentrations in excess of 30 ppbv on each of these days. The analyses show that long-range transport from Asia made smaller contributions (<10 ppbv) to surface O3 during two of those exceedances. The contribution of regional wildfires to surface O3 during the three LVOS exceedance events was found to be negligible, but wildfires were found to be a major factor during exceedance events that occurred before and after the LVOS campaign. Our analyses also shows that ozone exceedances would have occurred on more than 50% of the days during the six-week LVOS campaign if the 8-h ozone NAAQS had been 65 ppbv instead of 75 ppbv.
•Stratosphere-to-troposphere transport (STT) significantly impacts surface O3 in the intermountain west.•STT can directly lead to exceedances of the 2008 ozone NAAQS during springtime.•STT influences background surface O3 more than long-range transport from Asia.•With a 65 ppbv standard, exceedances may be too frequent to treat as “exceptional events” in the intermountain west during springtime.
The contribution of stratosphere‐to‐troposphere transport to high surface ozone (O3) along the Colorado Front Range during spring of 1999 is examined using lidar and surface measurements. A deep ...tropopause fold brought ∼215 ppbv of O3 to within 1 km of the highest peaks in the Rocky Mountains on 6 May 1999. One‐minute average O3 mixing ratios exceeding 100 ppbv were subsequently measured at a surface site in Boulder, and daily maximum 8‐hour O3 concentrations greater or equal to the 2008 NAAQS O3 standard of 0.075 ppmv were recorded at 3 of 9 Front Range monitoring stations. Other springtime peaks in surface O3 are also shown to coincide with passage of upper level troughs and dry stable layers aloft. These results show that the stratospheric contribution to surface ozone is significant, and can lead to exceedance of the 2008 NAAQS O3 standards in a major U.S. metropolitan area.
A series of deep stratospheric intrusions in late May 2013 increased the daily maximum 8 h surface ozone (O3) concentrations to more than 70 parts per billion by volume (ppbv) at rural and urban ...surface monitors in California and Nevada. This influx of ozone‐rich lower stratospheric air and entrained Asian pollution persisted for more than 5 days and contributed to exceedances of the 2008 8 h national ambient air quality standard of 75 ppbv on 21 and 25 May in Clark County, NV. Exceedances would also have occurred on 22 and 23 May had the new standard of 70 ppbv been in effect. In this paper, we examine this episode using lidar measurements from a high‐elevation site on Angel Peak, NV, and surface measurements from NOAA, the Clark County, Nevada Department of Air Quality, the Environmental Protection Agency Air Quality System, and the Nevada Rural Ozone Initiative. These measurements, together with analyses from the National Centers for Environmental Prediction/North American Regional Reanalysis; NOAA Geophysical Fluid Dynamics Laboratory AM3 model; NOAA National Environmental Satellite, Data, and Information Service Real‐time Air Quality Modeling System; and FLEXPART models, show that the exceedances followed entrainment of ~20 to 40 ppbv of lower stratospheric ozone mingled with another 0 to 10 ppbv of ozone transported from Asia by the unusually deep convective boundary layers above the Mojave desert. Our analysis suggests that this vigorous mixing can affect both high and low elevations and help explain the springtime ozone maximum in the southwestern U.S.
Plain Language Summary
Ozone (O3) is formed high in the upper atmosphere when ultraviolet (UV) rays from the sun break the bond in molecular oxygen (O2). This so‐called "good" ozone protects plants and animals at the ground from the damaging effects of these UV rays. Ozone is also formed in the lower atmosphere through reactions between nitrogen oxides (NOx) and volatile organic compounds (VOCs) of natural and human origin. This "bad" ozone can damage the sensitive tissues of plants and animals. The U.S. Clean Air Act (CAA) established standards designed to keep the ozone in the air we breathe at healthy levels by regulating NOx and VOC precursors emitted by human activities. The standard is revised periodically as new data on the health effects of ozone become available, and the current standard is close to the normal background levels found in some parts of the U.S. during springtime. This means that the concentrations can sometimes exceed the standard when storms bring "good" ozone from the upper atmosphere down to the ground where it becomes "bad" ozone. We take a look at this process and discuss why it is more likely to happen in the Southwest than in other parts of the U.S.
Key Points
The deep convective boundary layers of the Southwestern U.S. increase entrainment of stratospheric air and transported pollution
Stratospheric intrusions contribute to the springtime surface ozone maximum in the Southwestern U.S.
Stratospheric intrusions can cause exceedances of the National Ambient Air Quality Standard for ozone in the Southwestern U.S.
We describe an instrument for simultaneous measurements of glyoxal (CHOCHO) and nitrogen dioxide (NO2) using cavity enhanced absorption spectroscopy with a broadband light source. The output of a ...Xenon arc lamp is coupled into a 1 m optical cavity, and the spectrum of light exiting the cavity is recorded by a grating spectrometer with a charge-coupled device (CCD) array detector. The mirror reflectivity and effective path lengths are determined from the known Rayleigh scattering of He and dry zero air (N2+O2). Least-squares fitting, using published reference spectra, allow the simultaneous retrieval of CHOCHO, NO2, O4, and H2O in the 441 to 469 nm spectral range. For a 1-min sampling time, the precision (±1σ) on signal for measurements of CHOCHO and NO2 is 29 pptv and 20 pptv, respectively. We directly compare measurements made with the incoherent broadband cavity enhanced absorption spectrometer with those from cavity ringdown instruments detecting CHOCHO and NO2 at 404 and 532 nm, respectively, and find linear agreement over a wide range of concentrations. The instrument has been tested in the laboratory with both synthetic and real air samples, and the demonstrated sensitivity and specificity suggest a strong potential for field measurements of both CHOCHO and NO2.
The California Research at the Nexus of Air Quality and Climate Change (CalNex) field study was conducted throughout California in May, June, and July of 2010. The study was organized to address ...issues simultaneously relevant to atmospheric pollution and climate change, including (1) emission inventory assessment, (2) atmospheric transport and dispersion, (3) atmospheric chemical processing, and (4) cloud‐aerosol interactions and aerosol radiative effects. Measurements from networks of ground sites, a research ship, tall towers, balloon‐borne ozonesondes, multiple aircraft, and satellites provided in situ and remotely sensed data on trace pollutant and greenhouse gas concentrations, aerosol chemical composition and microphysical properties, cloud microphysics, and meteorological parameters. This overview report provides operational information for the variety of sites, platforms, and measurements, their joint deployment strategy, and summarizes findings that have resulted from the collaborative analyses of the CalNex field study. Climate‐relevant findings from CalNex include that leakage from natural gas infrastructure may account for the excess of observed methane over emission estimates in Los Angeles. Air‐quality relevant findings include the following: mobile fleet VOC significantly declines, and NOx emissions continue to have an impact on ozone in the Los Angeles basin; the relative contributions of diesel and gasoline emission to secondary organic aerosol are not fully understood; and nighttime NO3 chemistry contributes significantly to secondary organic aerosol mass in the San Joaquin Valley. Findings simultaneously relevant to climate and air quality include the following: marine vessel emissions changes due to fuel sulfur and speed controls result in a net warming effect but have substantial positive impacts on local air quality.
Key Points
An overview of the multi‐platform, multi‐agency CalNex field study in 2010
A synthesis of CalNex research to date
Emphasis on policy‐relevant conclusions linking climate and air quality issues
We have observed lower nitrogen dioxide (NO2) and ozone (O3) during a hot weekend (summer 2010) from aircraft over the entire South Coast Air Basin (SoCAB). Surface concentrations of NO2, O3, and ...temperature from 1996 to 2014 corroborate that this lower O3 on weekends is increasingly likely in recent years. While higher surface O3 on the weekends (weekend ozone effect, WO3E) remains widespread, the spatial extent and the trend in the probability of WO3E occurrences (PWO3E) have decreased significantly compared to a decade ago. This decrease is mostly the result of lower O3 on hot weekends in recent years. PWO3E is lowest in the eastern SoCAB. The major decrease happened during the 2008 economic recession, after which PWO3E has stabilized at a 15–25% lower level throughout most of the basin. Future NOx reductions are likely to be increasingly effective at reducing O3 pollution initially under hot conditions in the coming decade.
Key Points
The probability and area in the SoCAB affected by higher weekend O3 have decreased
The recent economic recession expedited this decrease
Future NOx regulations will be increasingly effective at reducing O3 on hot weekends
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