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Rajesh Kumar

Publications and source records attributed to Rajesh Kumar.

Decoupling in the Vertical Shape of HCHO During a Sea Breeze Event: the Effect on Trace Gas Satellite Retrievals and Column-to-Surface Translation

The effect of sea breeze circulation on stratification of the vertical formaldehyde (HCHO) concentration vertical profiles is explored using a regional atmospheric chemical transport model (CTM) for three synoptically stagnant days focused on the east coast of the U.S in June 2018. During this event, a significant thermal contrast between the Atlantic Ocean and the terrestrial regions (12–17 °C), observed by moderate resolution imaging spectroradiometer (MODIS) and well-captured by the WRF-CMAQ model (15–18 °C), is conducive to monsoon-like flow, perpendicular to the shorelines, carrying clean marine air masses over the land within a few hundreds of meters above the surface. In contrast, the westerly continental polluted air masses prevail in higher altitudes. These two conflicting flows result in atypical vertical shapes of HCHO concentrations increasing with altitude. This decoupling pattern is so pronounced that we observe total column HCHO negatively correlate with surface concentrations. Comparisons of an accredited global model, GEOS-CF, to surface wind measurements and MODIS skin temperature indicate its poor representation of the sea breeze timing and strength, resulting in GEOS-CF HCHO vertical shapes being drastically different from the WRF-CMAQ. Based on radiative transfer calculations, the differences in the vertical distribution of HCHO between the WRF-CMAQ and that of GEOS-CF in the first 3 km are sufficient to induce a 20–30% error in air mass factors (thus total vertical HCHO column abundances). Through an experiment involving converting HCHO total columns to surface mixing ratios, we demonstrate that GEOS-CF allocates noticeably more HCHO molecules (40–150%) to the surface layer due to the misrepresentation of the vertical shape of HCHO during the sea breeze event. It is known that a significant fraction of the human population lives in coastal areas prone to detrimental effects caused by air pollution, and elevated pollutant concentrations usually occur in synoptically stagnant atmospheric conditions when local circulation patterns come into play; accordingly, our experiments emphasize the importance of the effect a priori profiles can have on satellite-derived applications under such conditions. To ensure that the quantitative representation of satellite-based trace gas retrievals on a daily basis is trustworthy and useable for air quality applications, atmospheric models providing a priori profiles for satellite retrievals should be well-tuned to reproduce complex local circulation such as sea-land breezes.

sea breeze↗

Satellite Remote-Sensing Capability to Assess Tropospheric-Column Ratios of Formaldehyde and Nitrogen Dioxide: Case Study During the Long Island Sound Tropospheric Ozone Study 2018 (LISTOS 2018) Field Campaign

Satellite retrievals of tropospheric-column formaldehyde (HCHO) and nitrogen dioxide (NO 2 ) are frequently used to investigate the sensitivity of ozone (O 3 ) production to emissions of nitrogen oxides and volatile organic carbon compounds. This study inter-compared the systematic biases and uncertainties in retrievals of NO 2 and HCHO, as well as resulting HCHO–NO 2 ratios (FNRs), from two commonly applied satellite sensors to investigate O 3 production sensitivities (Ozone Monitoring Instrument, OMI, and TROPOspheric Monitoring Instrument, TROPOMI) using airborne remote-sensing data taken during the Long Island Sound Tropospheric Ozone Study 2018 between 25 June and 6 September 2018. Compared to aircraft-based HCHO and NO 2 observations, the accuracy of OMI and TROPOMI were magnitude-dependent with high biases in clean environments and a tendency towards more accurate comparisons to even low biases in moderately polluted to polluted regions. OMI and TROPOMI NO 2 systematic biases were similar in magnitude (normalized median bias, NMB = 5 %–6 %; linear regression slope ≈ 0.5–0.6), with OMI having a high median bias and TROPOMI resulting in small low biases. Campaign-averaged uncertainties in the three satellite retrievals (NASA OMI; Quality Assurance for Essential Climate Variables, QA4ECV OMI; and TROPOMI) of NO 2 were generally similar, with TROPOMI retrievals having slightly less spread in the data compared to OMI. The three satellite products differed more when evaluating HCHO retrievals. Campaign-averaged tropospheric HCHO retrievals all had linear regression slopes ∼0.5 and NMBs of 39 %, 17 %, 13 %, and 23 % for NASA OMI, QA4ECV OMI, and TROPOMI at finer (0.05° x 0.05°) and coarser (0.15° x 0.15°) spatial resolution, respectively. Campaign-averaged uncertainty values (root mean square error, RMSE) in NASA and QA4ECV OMI HCHO retrievals were ~9.0 x 10 15 molecules cm –2 (∼ 50 %–55 % of mean column abundance), and the higher-spatial-resolution retrievals from TROPOMI resulted in RMSE values ∼30 % lower. Spatially averaging TROPOMI tropospheric-column HCHO, along with NO 2 and FNRs, to resolutions similar to the OMI reduced the uncertainty in these retrievals. Systematic biases in OMI and TROPOMI NO 2 and HCHO retrievals tended to cancel out, resulting in all three satellite products comparing well to observed FNRs. However, while satellite-derived FNRs had minimal campaign-averaged median biases, unresolved errors in the indicator species did not cancel out in FNR calculations, resulting in large RMSE values compared to observations. Uncertainties in HCHO retrievals were determined to drive the unresolved biases in FNR retrievals.

Matthew S. Johnson↗

Evaluation and Intercomparison of Wildfire Smoke Forecasts from Multiple Modeling Systems for the 2019 Williams Flats Fire

Wildfire smoke is one of the most significant concerns of human and environmental health, associated with its substantial impacts on air quality, weather, and climate. However, biomass burning emissions and smoke remain among the largest sources of uncertainties in air quality forecasts. In this study, we evaluate the smoke emissions and plume forecasts from 12 state-of-the-art air quality forecasting systems during the Williams Flats fire in Washington State, US, August 2019, which was intensively observed during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) field campaign. Model forecasts with lead times within 1 d are intercompared under the same framework based on observations from multiple platforms to reveal their performance regarding fire emissions, aerosol optical depth (AOD), surface PM2.5, plume injection, and surface PM2.5 to AOD ratio. The comparison of smoke organic carbon (OC) emissions suggests a large range of daily totals among the models, with a factor of 20 to 50. Limited representations of the diurnal patterns and day-to-day variations of emissions highlight the need to incorporate new methodologies to predict the temporal evolution and reduce uncertainty of smoke emission estimates. The evaluation of smoke AOD (sAOD) forecasts suggests overall underpredictions in both the magnitude and smoke plume area for nearly all models, although the high-resolution models have a better representation of the fine-scale structures of smoke plumes. The models driven by fire radiative power (FRP)-based fire emissions or assimilating satellite AOD data generally outperform the others. Additionally, limitations of the persistence assumption used when predicting smoke emissions are revealed by substantial underpredictions of sAOD on 8 August 2019, mainly over the transported smoke plumes, owing to the underestimated emissions on 7 August. In contrast, the surface smoke PM2.5 (sPM2.5) forecasts show both positive and negative overall biases for these models, with most members presenting more considerable diurnal variations of sPM2.5. Overpredictions of sPM2.5 are found for the models driven by FRP-based emissions during nighttime, suggesting the necessity to improve vertical emission allocation within and above the planetary boundary layer (PBL). Smoke injection heights are further evaluated using the NASA Langley Research Center's Differential Absorption High Spectral Resolution Lidar (DIAL-HSRL) data collected during the flight observations. As the fire became stronger over 3–8 August, the plume height became deeper, with a day-to-day range of about 2–9 km a.g.l. However, narrower ranges are found for all models, with a tendency of overpredicting the plume heights for the shallower injection transects and underpredicting for the days showing deeper injections. The misrepresented plume injection heights lead to inaccurate vertical plume allocations along the transects corresponding to transported smoke that is 1 d old. Discrepancies in model performance for surface PM2.5 and AOD are further suggested by the evaluation of their ratio, which cannot be compensated for by solely adjusting the smoke emissions but are more attributable to model representations of plume injections, besides other possible factors including the evolution of PBL depths and aerosol optical property assumptions. By consolidating multiple forecast systems, these results provide strategic insight on pathways to improve smoke forecasts.

AOD↗

The impact of Los Angeles Basin pollution and stratospheric intrusions on the surrounding San Gabriel Mountains as seen by surface measurements, lidar, and numerical models

In this work, the impact of Los Angeles Basin pollution transport and stratospheric intrusions on the surface ozone levels observed in the San Gabriel Mountains is investigated based on a combination of surface and lidar measurements as well as WRF-Chem (Weather Research and Forecasting with Chemistry) and WACCM (Whole Atmosphere Community Climate Model) runs. The number of days with observed surface ozone levels exceeding the National Ambient Air Quality Standards exhibit a clear seasonal pattern, with a maximum during summer, when models suggest a minimum influence of stratospheric intrusions and the largest impact from Los Angeles Basin pollution transport. Additionally, measured and modeled surface ozone and PM10 were analyzed as a function of season, time of the day, and wind direction. Measurements and models are in good qualitative agreement, with maximum surface ozone observed for southwest and west winds. For the prevailing summer wind direction, slightly south of the ozone maximum and corresponding to south-southwest winds, lower ozone levels were observed. Back trajectories suggest that this is associated with transport from the central Los Angeles Basin, where titration limits the amount of surface ozone. A quantitative comparison of the lidar profiles with WRF-Chem and WACCM models revealed good agreement near the surface, with models showing an increasing positive bias as function of altitude, reaching 75 % at 15 km above sea level. Finally, three selected case studies covering the different mechanisms affecting the near-surface ozone concentration over the San Gabriel Mountains, namely stratospheric intrusions and pollution transport, are analyzed based on surface and ozone lidar measurements, as well as co-located ceilometer measurements and models.

Impact↗

Air Pollution Trends Measured From Terra: CO and AOD Over Industrial, Fire-prone, and Background Regions

Following past studies to quantify decadal trends in global carbon monoxide (CO) using satellite observations, we update estimates and find a CO trend in column amounts of about −0.50 % per year between 2002 to 2018, which is a deceleration compared to analyses performed on shorter records that found −1 % per year. Aerosols are co-emitted with CO from both fires and anthropogenic sources but with a shorter lifetime than CO. A combined trend analysis of CO and aerosol optical depth (AOD) measurements from space helps to diagnose the drivers of regional differences in the CO trend. We use the long-term records of CO from the Measurements of Pollution in the Troposphere (MOPITT) and AOD from the Moderate Resolution Imaging Spectroradiometer (MODIS) instrument. Other satellite instruments measuring CO in the thermal infrared, AIRS, TES, IASI, and CrIS, show consistent hemispheric CO variability and corroborate results from the trend analysis performed with MOPITT CO. Trends are examined by hemisphere and in regions for 2002 to 2018, with uncertainties quantified. The CO and AOD records are split into two sub-periods (2002 to 2010 and 2010 to 2018) in order to assess trend changes over the 16 years. We focus on four major population centers: Northeast China, North India, Europe, and Eastern USA, as well as fire-prone regions in both hemispheres. In general, CO declines faster in the first half of the record compared to the second half, while AOD trends show more variability across regions. We find evidence of the atmospheric impact of air quality management policies. The large decline in CO found over Northeast China is initially associated with an improvement in combustion efficiency, with subsequent additional air quality improvements from 2010 onwards. Industrial regions with minimal emission control measures such as North India become more globally relevant as the global CO trend weakens. We also examine the CO trends in monthly percentile values to understand seasonal implications and find that local changes in biomass burning are sufficiently strong to counteract the global downward trend in atmospheric CO, particularly in late summer.

carbon monoxide↗

Toward Improving Short-Term Predictions of Fine Particulate Matter Over the United States Via Assimilation of Satellite Aerosol Optical Depth Retrievals

This study develops a new approach to improve simulations of the particulate matter of aerodynamic diameter smaller than 2.5μm (PM2.5) in the Community Multiscale Air Quality (CMAQ) model via assimilation of Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol optical depth(AOD) retrievals using the Grid point Statistical Interpolation (GSI) system. In contrast to previous studies that only consider errors due to transport, our computation of the background error covariance matrix incorporates uncertainties in anthropogenic emissions. To understand the impact of this approach, three experiments (one background and two assimilations) are performed over the contiguous United States(CONUS) from 15 July to 14 August 2014. The background CMAQ experiment significantly underestimates both the MODIS AOD and surface PM2.5levels. MODIS AOD assimilation pushes both the CMAQ AOD and surface PM2.5distributions toward the observed distributions, but CMAQ still underestimates the observations. Averaged over CONUS, the two assimilation experiments with and without including the anthropogenic emission uncertainties improve the correlation coefficient between the model and independent observations of PM2.5 by ~67% and ~48%, respectively, and reduces the mean bias by ~38% and~10%, respectively. The assimilation improves the model performance everywhere over CONUS, except the New York and Wisconsin, where CMAQ overestimates the observed PM2.5during nighttime after assimilation likely because of overcorrection of aerosol mass concentrations by the AOD assimilation. Future work should incorporate uncertainties in other processes (biomass burning and biogenic emissions, deposition, chemistry, transport, and boundary conditions) to further enhance the value of assimilating spaceborne AOD retrievals.

Assimilation↗

How Well Satellite Remote Sensing Can Inform Surface Level Ozone Production Sensitivity to Precursor Trace Gas Emissions?

Surface-level ozone (O3) pollution mitigation strategies rely on a clear understanding of the atmospheric chemical processes involving O3, NOx (nitric oxide (NO) + nitrogen dioxide (NO2)) and volatile organic compounds (VOCs). A robust spatiotemporal classification of O3 photochemical regimes with relative chemical sensitivity of local O3 formation to emission reductions of NOx (NOx-limited regime) versus VOCs (radical-limited regime) is required to design anthropogenic emission reduction policies in order to improve surface air quality. Numerous studies found that the ratio of satellite-retrieved Vertical Column Densities (VCDs) of formaldehyde (HCHO) to NO2 can diagnose O3 production sensitivity. However, uncertainty still remains about the accuracy of such estimates using satellite-based retrievals. This study conducts an investigation to identify how well satellite data can inform surface-level O3 sensitivity by validating satellite-based estimates against aircraft-based retrievals taken during the Long Island Sound Tropospheric Ozone Study (LISTOS-2018) and Ozone Water-Land Environmental Transition Study (OWLETS-2) field campaigns. For this study, we use HCHO and NO2 retrievals from the Ozone Monitoring Instrument (OMI) onboard the Aura satellite, and high spatiotemporal resolution TROPOspheric Monitoring Instrument (TROPOMI) onboard the Sentinel-5 Precursor (S5P) satellite. The Community Multiscale Air Quality (CMAQ) modelling system is used to provide trace gas vertical profiles to recalculate air mass factor for deriving consistent satellite-based VCDs. To demonstrate the ability of satellites to diagnose O3 production regimes, we validate satellite-derived O3 sensitivity regimes, along with the OMI and TROPOMI products applied, using HCHO and NO2 retrievals from the aircraft-based instruments: Geostationary Trace gas and Aerosol Sensor Optimization (GeoTASO) spectrometer and Geostationary Coastal and Air Pollution Events Airborne Simulator (GCAS) instruments deployed during the LISTOS-2018 and OWLETS-2 campaigns. The results of this work will advance our fundamental knowledge of the spatiotemporal evolution of the complex O3-NOx-VOC chemistry, and will advance our understanding about the quality of remote-sensing, suborbital, and satellite data for accurately observing surface-level O3 production sensitivity.

Satellite↗

Quantifying the benefits of improved satellite remote-sensing observations for inverse modeling of NOx and NMVOC emissions

This study aims to demonstrate the benefits of using novel high spatiotemporal retrieval products from newer satellites for top-down emission estimates of nitrogen oxides (NO x ) and non-methane volatile organic compounds (NMVOCs) for the summer of 2019 over the contiguous United States. Recent satellite retrievals have not only advanced spatiotemporal resolution but also greatly reduced error and uncertainty due to reduced noise in the retrievals compared to spaceborne sensors launched in the past. We applied inverse modeling techniques using tropospheric nitrogen dioxide (NO 2 ) and formaldehyde (H-CHO) column retrieval products from the Ozone Monitoring Instrument (OMI) and TROPOspheric Monitoring Instrument (TROPOMI) in conjunction with the Weather Research Forecast and Community Multiscale Air Quality Modeling system (WRF-CMAQ). In order to provide a better representation of background chemical composition and avoid misalignment of emission adjustment, we applied monthly scaling factors for ozone (O 3 ) and CO boundary concentrations in addition to the inclusion of lightning and aviation emissions. Satellite-constrained NO x and NMVOCs posterior emissions showed a mitigated discrepancy between observed and modeled columns. The improvement in the model performance was greater when using TROPOMI, primarily benefiting from reduced errors/biases of the satellite retrievals that enabled us to explore corresponding changes in O 3 concentrations and production sensitivity regimes using the ratio of H-CHO and NO 2 .

remote sensing↗

Improved Assessment of Recent Trends in NOx and VOC Emissions and Ozone Production Sensitivity Regimes Using Satellite Data

This presentation highlights results from a NASA Aura Science Team and Atmospheric Composition Modeling and Analysis Program (ACMAP) project which study the capability to observe and model trends in ozone (O3) production regimes using spaceborne sensors. Ultraviolet– visible (UV–Vis) tropospheric column satellite retrievals of formaldehyde (HCHO) (a proxy for volatile organic compound [VOC] reactivity) and nitrogen dioxide (NO2) (a proxy for nitrogen oxides [NOx]) are frequently used to investigate the sensitivity of O3 production to emissions of NOx and VOCs. There are challenges that come from using satellite-derived ratios of HCHO and NO2 (FNR) to study O3 production sensitivity with the largest uncertainties associated with specific spaceborne sensor’s retrieval biases and errors. This study quantifies the differences and improvements in satellite retrievals of O3 production sensitivity regimes using FNRs when moving from legacy polar orbiting satellites such as the Ozone Monitoring Instrument (OMI) onboard NASA’s Aura satellite and Ozone Mapping and Profiler Suite Nadir Mapper (OMPS-NM) onboard the NASA/NOAA Suomi-NPP platform to newer, higher spatiotemporal resolution satellite sensors TROPOspheric Monitoring Instrument (TROPOMI) and eventually the recently launched NASA geostationary sensor Tropospheric Emissions: Monitoring of Pollution (TEMPO). Furthermore, we investigate how using retrievals of NO2 and HCHO from these different satellites to constrain model predictions impacts the ability to accurately simulate O3 chemistry including chemical production regimes. To this end, we have conducted inverse model simulations, using the WRF-CMAQ-DDM data assimilation system at 12 km × 12 km, to constrain emissions of NOx and VOCs over the contiguous United States (CONUS) when assimilating OMI and TROPOMI retrievals of NO2 and HCHO. Two advantages of this are that we a) account for each satellite’s errors/biases in the emission estimation and b) update the prior profile to ensure that only radiance information is used for optimizing the emissions. This presentation will demonstrate: a) the varying accuracy of different satellite retrieved FNRs and ability to capture known sub-annual emission trends (e.g., seasonal, weekend/weekday) and emission anomalies during the COVID-19 lockdown of 2020, b) the differences and improvements in top-down emission estimates of NOx and VOCs when constrained by newer satellite sensors compared to legacy systems, and c) multi-sensor optimized emission estimates of summer-time NOx and VOCs between 2019-2021.

Data↗