One of the least understood aspects in atmospheric chemistry is how urban emissions influence the formation of natural organic aerosols, which affect Earth’s energy budget. The Amazon rainforest, during its wet season, is one of the few remaining places on Earth where atmospheric chemistry transitions between preindustrial and urban-influenced conditions. Here, we integrate insights from several laboratory measurements and simulate the formation of secondary organic aerosols (SOA) in the Amazon using a high-resolution chemical transport model. Simulations show that emissions of nitrogen-oxides from Manaus, a city of ~2 million people, greatly enhance production of biogenic SOA by 60–200% on average with peak enhancements of 400%, through the increased oxidation of gas-phase organic carbon emitted by the forests. Simulated enhancements agree with aircraft measurements, and are much larger than those reported over other locations. The implication is that increasing anthropogenic emissions in the future might substantially enhance biogenic SOA in pristine locations like the Amazon.
11 September 2012 in Atmospheric Chemistry and Physics
An Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed during the Carbonaceous Aerosols and Radiative Effects Study (CARES) that took place in northern California in June 2010. We present results obtained at Cool (denoted as the T1 site of the project) in the foothills of the Sierra Nevada Mountains, where intense biogenic emissions are periodically mixed with urban outflow transported by daytime southwesterly winds from the Sacramento metropolitan area. During this study, the average mass loading of submicrometer particles (PM1) was 3.0 μg m−3, dominated by organics (80%) and sulfate (9.9%). The organic aerosol (OA) had a nominal formula of C1H1.38N0.004OM0.44, thus an average organic mass-to-carbon (OM/OC) ratio of 1.70. Two distinct oxygenated OA factors were identified via Positive matrix factorization (PMF) of the high-resolution mass spectra of organics. The more oxidized MO-OOA (O/C = 0.54) was interpreted as a surrogate for secondary OA (SOA) influenced by biogenic emissions whereas the less oxidized LO-OOA (O/C = 0.42) was found to represent SOA formed in photochemically processed urban emissions. LO-OOA correlated strongly with ozone and MO-OOA correlated well with two 1st generation isoprene oxidation products (methacrolein and methyl vinyl ketone), indicating that both SOAs were relatively fresh. A hydrocarbon like OA (HOA) factor was also identified, representing primary emissions mainly due to local traffic. On average, SOA (= MO-OOA + LO-OOA) accounted for 91% of the total OA mass and 72% of the PM1 mass observed at Cool. Twenty three periods of urban plumes from T0 (Sacramento) to T1 (Cool) were identified using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem). The average PM1 mass loading was considerably higher in urban plumes than in air masses dominated by biogenic SOA. The change in OA mass relative to CO (ΔOA/ΔCO) varied in the range of 5-196 μg m−3 ppm−1, reflecting large variability in SOA production. The highest ΔOA/ΔCO was reached when air masses were dominated by anthropogenic emissions in the presence of a high concentration of biogenic volatile organic compounds (BVOCs). This ratio, which was 97 μg m−3 ppm−1 on average, was much higher than when urban plumes arrived in a low BVOC environment (~36 μg m−3 ppm−1) or during other periods dominated by biogenic SOA (35 μg m−3 ppm−1). These results demonstrate that SOA formation is enhanced when anthropogenic emissions interact with biogenic precursors.
In this study, the authors incorporate an operational-like irrigation scheme into the Noah land surface model as part of the Weather Research and Forecasting Model (WRF). A series of simulations, with and without irrigation, is conducted over the Southern Great Plains (SGP) for an extremely dry (2006) and wet (2007) year. The results show that including irrigation reduces model bias in soil moisture and surface latent heat (LH) and sensible heat (SH) fluxes, especially during a dry year. Irrigation adds additional water to the surface, leading to changes in the planetary boundary layer. The increase in soil moisture leads to increases in the surface evapotranspiration and near-surface specific humidity but decreases in the SH and surface temperature. Those changes are local and occur during daytime. There is an irrigation-induced decrease in both the lifting condensation level (ZLCL) and mixed-layer depth. The decrease in ZLCL is larger than the decrease in mixed-layer depth, suggesting an increasing probability of shallow clouds. The simulated changes in precipitation induced by irrigation are highly variable in space, and the average precipitation over the SGP region only slightly increases. A high correlation is found among soil moisture, SH, and ZLCL. Larger values of soil moisture in the irrigated simulation due to irrigation in late spring and summer persist into the early fall, suggesting that irrigation-induced soil memory could last a few weeks to months. The results demonstrate the importance of irrigation parameterization for climate studies and improve the process-level understanding on the role of human activity in modulating land–air–cloud interactions.
10 October 2014 in Atmospheric Measurement Techniques
We present measurements acquired by the world's first airborne 3 backscatter (β) + 2 extinction (α) High Spectral Resolution Lidar (HSRL-2). HSRL-2 measures particle backscatter coefficients at 355, 532, and 1064 nm, and particle extinction coefficients at 355 and 532 nm. The instrument has been developed by the NASA Langley Research Center. The instrument was operated during Phase 1 of the Department of Energy (DOE) Two-Column Aerosol Project (TCAP) in July 2012. We observed pollution outflow from the northeastern coast of the US out over the western Atlantic Ocean. Lidar ratios were 50–60 sr at 355 nm and 60–70 sr at 532 nm. Extinction-related Ångström exponents were on average 1.2–1.7, indicating comparably small particles. Our novel automated, unsupervised data inversion algorithm retrieved particle effective radii of approximately 0.2 μm, which is in agreement with the large Ångström exponents. We find good agreement with particle size parameters obtained from coincident in situ measurements carried out with the DOE Gulfstream-1 aircraft.
1 October 2015 in Bulletin of the American Meteorological Society
The Wind Forecast Improvement Project (WFIP) is a public–private research program, the goal of which is to improve the accuracy of short-term (0–6 h) wind power forecasts for the wind energy industry. WFIP was sponsored by the U.S. Department of Energy (DOE), with partners that included the National Oceanic and Atmospheric Administration (NOAA), private forecasting companies (WindLogics and AWS Truepower), DOE national laboratories, grid operators, and universities. WFIP employed two avenues for improving wind power forecasts: first, through the collection of special observations to be assimilated into forecast models and, second, by upgrading NWP forecast models and ensembles. The new observations were collected during concurrent year-long field campaigns in two high wind energy resource areas of the United States (the upper Great Plains and Texas) and included 12 wind profiling radars, 12 sodars, several lidars and surface flux stations, 184 instrumented tall towers, and over 400 nacelle anemometers. Results demonstrate that a substantial reduction (12%–5% for forecast hours 1–12) in power RMSE was achieved from the combination of improved numerical weather prediction models and assimilation of new observations, equivalent to the previous decade’s worth of improvements found for low-level winds in NOAA/National Weather Service (NWS) operational weather forecast models. Data-denial experiments run over select periods of time demonstrate that up to a 6% improvement came from the new observations. Ensemble forecasts developed by the private sector partners also produced significant improvements in power production and ramp prediction. Based on the success of WFIP, DOE is planning follow-on field programs.
The California Research at the Nexus of Air Quality and Climate Change (CalNex) and Carbonaceous Aerosol and Radiative Effects Study (CARES) field campaigns during May and June 2010 provided a data set appropriate for studying the structure of the atmospheric boundary layer (BL). The NASA Langley Research Center (LaRC) airborne high spectral resolution lidar (HSRL) was deployed to California onboard the NASA LaRC B-200 aircraft to aid in characterizing aerosol properties during these two field campaigns. Measurements of aerosol extinction (532 nm), backscatter (532 and 1064 nm), and depolarization (532 and 1064 nm) profiles during 31 flights, many in coordination with other research aircraft and ground sites, constitute a diverse data set for use in characterizing the spatial and temporal distribution of aerosols, as well as the depth and variability of the daytime mixed layer (ML) height. The paper describes the modified Haar wavelet covariance transform method used to derive the ML heights from HSRL backscatter profiles. HSRL ML heights are validated using ML heights derived from two radiosonde profile sites during CARES. Comparisons between ML heights from HSRL and a Vaisala ceilometer operated during CalNex were used to evaluate the representativeness of a fixed measurement over a larger region. In the Los Angeles basin, comparisons of ML heights derived from HSRL measurements and ML heights derived from the ceilometer result in a very good agreement (mean bias difference of 10 m and correlation coefficient of 0.89) up to 30 km away from the ceilometer site, but are essentially uncorrelated for larger distances, indicating that the spatial variability of the ML height is significant over these distances and not necessarily well captured by limited ground stations. The HSRL ML heights are also used to evaluate the performance in simulating the temporal and spatial variability of ML heights from the Weather Research and Forecasting Chemistry (WRF-Chem) community model. When compared to aerosol ML heights from HSRL, thermodynamic ML heights from WRF-Chem were underpredicted in the CalNex and CARES regions, shown by a bias difference value of −157 m and −29 m, respectively. Better agreement over the Central Valley than in mountainous regions suggests that some variability in the ML height is not well captured at the 4 km grid resolution of the model. A small but significant number of cases have poor agreement when WRF-Chem consistently overestimates the ML height in the late afternoon. Additional comparisons with WRF-Chem aerosol mixed layer heights show no significant improvement over thermodynamic ML heights, confirming that any differences between measurement and model are not due to the methodology of ML height determination.