A TROPOMI- and GLM-Based Estimate of NOx Production by Lightning over the U.S.

Lightning produces NO because the extreme temperatures (>20000 K) in lightning channels dissociate molecular O2 and molecular N2, which then combine to form NOx which quickly reacts with O3 to form NO2. Lightning is responsible for 10-15% of NOx emissions globally. This is 2 8 Tg N a-1 [Schumann and Huntrieser, 2007] or 100 to 400 mol per flash. Much of the uncertainty stems from limited knowledge of lightning NOx production per flash (LNOx PE) or per unit flash length. Most LNOx is injected into mid- and upper-troposphere where away from deep convection its lifetime is longer relative to lower troposphere NOx. NOx in this region enhances the concentrations of upper tropospheric NOy, OH, and O3 and contributes to positive radiative forcing by O3 and negative forcing by CH4. We have previously used OMI NO2 to obtain estimates of LNOx production per flash over the Gulf of Mexico (Pickering et al., 2016, JGR), in convective events during NASAs TC4 field program (Bucsela et al., 2010, JGR), and over broad regions of the tropics (Allen et al., 2019, JGR) and midlatitudes (Bucsela et al., 2019, JGR). In the latter studies, we obtained PE values of 170 100 mol flash and 180 100 mol flash, respectively

Investigating the impact of coupling HARMONIE-WINS50 (cy43) meteorology to LOTOS-EUROS (v2.2.002) on a simulation of NO2 concentrations over the Netherlands

Meteorological fields calculated by numerical weather prediction (NWP) models drive offline chemical transport models (CTMs) to solve the transport, chemical reactions, and atmospheric interaction over the geographical domain of interest. HARMONIE (HIRLAM ALADIN Research on Mesoscale Operational NWP in Euromed) is a state-of-the-art non-hydrostatic NWP community model used at several European weather agencies to forecast weather at the local and/or regional scale. In this work, the HARMONIE WINS50 (cycle 43 cy43) reanalysis dataset at a resolution of 0.025° × 0.025° covering an area surrounding the North Sea for the years 2019–2021 was coupled offline to the LOTOS-EUROS (LOng-Term Ozone Simulation-EURopean Operational Smog model, v2.2.002) CTM. The impact of using either meteorological fields from HARMONIE or from ECMWF on LOTOS-EUROS simulations of NO2 has been evaluated against ground-level observations and TROPOMI tropospheric NO2 vertical columns. Furthermore, the difference between crucial meteorological input parameters such as the boundary layer height and the vertical diffusion coefficient between the hydrostatic ECMWF and non-hydrostatic HARMONIE data has been studied, and the vertical profiles of temperature, humidity, and wind are evaluated against meteorological observations at Cabauw in The Netherlands. The results of these first evaluations of the LOTOS-EUROS model performance in both configurations are used to investigate current uncertainties in air quality forecasting in relation to driving meteorological parameters and to assess the potential for improvements in forecasting pollution episodes at high resolutions based on the HARMONIE NWP model.</p

Hubbard model versus t-J model: The one-particle spectrum

The origin of the apparent discrepancies between the one-particle spectra of the Hubbard and t-J models is revealed: Wavefunction corrections, in addition to the three-site terms, should supplement the bare t-J. In this way a quantitative agreement between the two models is obtained, even for the intermediate-$U$ values appropriate for the high-Tc cuprate superconductors. Numerical results for clusters of up to 20 sites are presented. The momentum dependence of the observed intensities in the photoemission spectra of Sr2CuO2Cl2 are well described by this complete strong-coupling approach.Comment: 4 two-column RevTeX pages, including 4 Postscript figures. Uses epsf. Accepted for publication in Physical Review B, Rapid Communicatio

Intercomparison of SCIAMACHY and OMI Tropospheric NO2 Columns: Observing the Diurnal Evolution of Chemistry and Emissions from Space

Concurrent (August 2006) measurements of tropospheric NO2 columns from OMI aboard Aura (1330 local overpass time) and SCIAMACHY aboard Envisat (1000 local overpass time) offer an opportunity to examine the consistency between the two instruments under tropospheric background conditions and the effect of different observing times. For scenes with tropospheric NO2 columns <5.0 × 1015 molecules cm−2, SCIAMACHY and OMI agree within 1.0–2.0 × 1015 molecules cm−2, consistent with the detection limits of both instruments. We find evidence for a low bias of 0.2 × 1015 molecules cm−2 in OMI observations over remote oceans. Over the fossil fuel source regions at northern midlatitudes, we find that SCIAMACHY observes up to 40% higher NO2 at 1000 local time (LT) than OMI at 1330 LT. Over biomass burning regions in the tropics, SCIAMACHY observes up to 40% lower NO2 columns than OMI. These differences are present in the spectral fitting of the data (slant column) and are augmented in the fossil fuel regions and dampened in the tropical biomass burning regions by the expected increase in air mass factor as the mixing depth rises from 1000 to 1330 LT. Using a global 3-D chemical transport model (GEOS-Chem), we show that the 1000–1330 LT decrease in tropospheric NO2 column over fossil fuel source regions can be explained by photochemical loss, dampened by the diurnal cycle of anthropogenic emissions that has a broad daytime maximum. The observed 1000–1330 LT NO2 column increase over tropical biomass burning regions points to a sharp midday peak in emissions and is consistent with a diurnal cycle of emissions derived from geostationary satellite fire counts.Earth and Planetary SciencesEngineering and Applied Science

Top-Down NOx Emissions of European Cities Based on the Downwind Plume of Modelled and Space-Borne Tropospheric NO2 Columns

Top-down estimates of surface NOX emissions were derived for 23 European cities based on the downwind plume decay of tropospheric nitrogen dioxide (NO2) columns from the LOTOS-EUROS (Long Term Ozone Simulation-European Ozone Simulation) chemistry transport model (CTM) and from Ozone Monitoring Instrument (OMI) satellite retrievals, averaged for the summertime period (April-September) during 2013. Here we show that the top-down NOX emissions derived from LOTOS-EUROS for European urban areas agree well with the bottom-up NOX emissions from the MACC-III inventory data (R(exp 2) = 0.88) driving the CTM demonstrating the potential of this method. OMI top-down NOX emissions over the 23 European cities are generally lower compared with the MACC-III emissions and their correlation is slightly lower (R(exp 2) = 0.79). The uncertainty on the derived NO2 lifetimes and NOX emissions are on average ~55% for OMI and ~63% for LOTOS-EUROS data. The downwind NO2 plume method applied on both LOTOS-EUROS and OMI tropospheric NO2 columns allows to estimate NOX emissions from urban areas, demonstrating that this is a useful method for real-time updates of urban NOX emissions with reasonable accuracy

Impact of synthetic space-borne NO2 observations from the Sentinel-4 and Sentinel-5P missions on tropospheric NO2 analyses

We present an Observing System Simulation Experiment (OSSE) dedicated to the evaluation of the added value of the Sentinel-4 and Sentinel-5P missions for tropospheric nitrogen dioxide (NO2). Sentinel-4 is a geostationary (GEO) mission covering the European continent, providing observations with high temporal resolution (hourly). Sentinel-5P is a low Earth orbit (LEO) mission providing daily observations with a global coverage. The OSSE experiment has been carefully designed, with separate models for the simulation of observations and for the assimilation experiments and with conservative estimates of the total observation uncertainties. In the experiment we simulate Sentinel-4 and Sentinel-5P tropospheric NO2 columns and surface ozone concentrations at 7 by 7 km resolution over Europe for two 3-month summer and winter periods. The synthetic observations are based on a nature run (NR) from a chemistry transport model (MOCAGE) and error estimates using instrument characteristics. We assimilate the simulated observations into a chemistry transport model (LOTOS-EUROS) independent of the NR to evaluate their impact on modelled NO2 tropospheric columns and surface concentrations. The results are compared to an operational system where only ground-based ozone observations are ingested. Both instruments have an added value to analysed NO2 columns and surface values, reflected in decreased biases and improved correlations. The Sentinel-4 NO2 observations with hourly temporal resolution benefit modelled NO2 analyses throughout the entire day where the daily Sentinel-5P NO2 observations have a slightly lower impact that lasts up to 3–6 h after overpass. The evaluated benefits may be even higher in reality as the applied error estimates were shown to be higher than actual errors in the now operational Sentinel-5P NO2 products. We show that an accurate representation of the NO2 profile is crucial for the benefit of the column observations on surface values. The results support the need for having a combination of GEO and LEO missions for NO2 analyses in view of the complementary benefits of hourly temporal resolution (GEO, Sentinel-4) and global coverage (LEO, Sentinel-5P)

New observations of NO2 in the upper troposphere from TROPOMI

Nitrogen oxides (NOx≡NO+NO2) in the NOx-limited upper troposphere (UT) are long-lived and so have a large influence on the oxidizing capacity of the troposphere and formation of the greenhouse gas ozone. Models misrepresent NOx in the UT, and observations to address deficiencies in models are sparse. Here we obtain a year of near-global seasonal mean mixing ratios of NO2 in the UT (450–180 hPa) at 1∘×1∘ by applying cloud-slicing to partial columns of NO2 from TROPOMI. This follows refinement of the cloud-slicing algorithm with synthetic partial columns from the GEOS-Chem chemical transport model. TROPOMI, prior to cloud-slicing, is corrected for a 13 % underestimate in stratospheric NO2 variance and a 50 % overestimate in free-tropospheric NO2 determined by comparison to Pandora total columns at high-altitude free-tropospheric sites at Mauna Loa, Izaña, and Altzomoni and MAX-DOAS and Pandora tropospheric columns at Izaña. Two cloud-sliced seasonal mean UT NO2 products for June 2019 to May 2020 are retrieved from corrected TROPOMI total columns using distinct TROPOMI cloud products that assume clouds are reflective boundaries (FRESCO-S) or water droplet layers (ROCINN-CAL). TROPOMI UT NO2 typically ranges from 20–30 pptv over remote oceans to >80 pptv over locations with intense seasonal lightning. Spatial coverage is mostly in the tropics and subtropics with FRESCO-S and extends to the midlatitudes and polar regions with ROCINN-CAL, due to its greater abundance of optically thick clouds and wider cloud-top altitude range. TROPOMI UT NO2 seasonal means are spatially consistent (R=0.6–0.8) with an existing coarser spatial resolution (5∘ latitude × 8∘ longitude) UT NO2 product from the Ozone Monitoring Instrument (OMI). UT NO2 from TROPOMI is 12–26 pptv more than that from OMI due to increase in NO2 with altitude from the OMI pressure ceiling (280 hPa) to that for TROPOMI (180 hPa), but possibly also due to altitude differences in TROPOMI and OMI cloud products and NO2 retrieval algorithms. The TROPOMI UT NO2 product offers potential to evaluate and improve representation of UT NOx in models and supplement aircraft observations that are sporadic and susceptible to large biases in the UT.This research has been supported by the European Research Council under the European Union’s Horizon 2020 research and innovation programme (through the Starting Grant awarded to Eloise A. Marais, UpTrop (grant no. 851854))