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Steenrod, Stephen D.

Publications and source records attributed to Steenrod, Stephen D..

Cloud Impacts on Photochemistry: Building a Climatology of Photolysis Rates from the Atmospheric Tomography Mission

Measurements from actinic flux spectroradiometers on board the NASA DC-8 during the Atmospheric Tomography (ATom) mission provide an extensive set of statistics on how clouds alter photolysis rates (J values) throughout the remote Pacific and Atlantic Ocean basins. J values control tropospheric ozone and methane abundances, and thus clouds have been included for more than three decades in tropospheric chemistry modeling. ATom made four profiling circumnavigations of the troposphere capturing each of the seasons during 2016–2018. This work examines J values from the Pacific Ocean flights of the first deployment, but publishes the complete Atom-1 data set (29 July to 23 August 2016). We compare the observed J values (every 3 s along flight track) with those calculated by nine global chemistry– climate/transport models (globally gridded, hourly, for a mid-August day). To compare these disparate data sets, we build a commensurate statistical picture of the impact of clouds on J values using the ratio of J -cloudy (standard, sometimes cloudy conditions) to J -clear (artificially cleared of clouds). The range of modeled cloud effects is inconsistently large but they fall into two distinct classes: (1) models with large cloud effects showing mostly enhanced J values aloft and or diminished at the surface and (2) models with small effects having nearly clear-sky J values much of the time. The ATom-1 measurements generally favor large cloud effects but are not precise or robust enough to point out the best cloud-modeling approach. The models here have resolutions of 50–200 km and thus reduce the occurrence of clear sky when averaging over grid cells. In situ measurements also average scattered sunlight over a mixed cloud field, but only out to scales of tens of kilometers. A primary uncertainty remains in the role of clouds in chemistry, in particular, how models average over cloud fields, and how such averages can simulate measurements.

actinic flux spectroradiometers↗

Chemical Modeling of the Reactivity of Short-Lived Greenhouse Gases: A Model Inter-Comparison Prescribing a Well-Measured, Remote Troposphere

We develop a new protocol for merging in situ measurements with 3-D model simulations of atmospheric chemistry with the goal of integrating over the data to identify the most reactive air parcels in terms of tropospheric production and loss of the greenhouse gases ozone and methane. Presupposing that we can accurately measure atmospheric composition, we examine whether models constrained by such measurements agree on the chemical budgets for ozone and methane. In applying our technique to a synthetic data stream of 14,880 parcels along 180W, we are able to isolate the performance of the photochemical modules operating within their global chemistry-climate and chemistry-transport models, removing the effects of modules controlling tracer transport, emissions, and scavenging. Differences in reactivity across models are driven only by the chemical mechanism and the diurnal cycle of photolysis rates, which are driven in turn by temperature, water vapor, solar zenith angle, clouds, and possibly aerosols and overhead ozone, which are calculated in each model. We evaluate six global models and identify their differences and similarities in simulating the chemistry through a range of innovative diagnostics. All models agree that the more highly reactive parcels dominate the chemistry (e.g., the hottest 10% of parcels control 25-30% of the total reactivities), but do not fully agree on which parcels comprise the top 10%. Distinct differences in specific features occur, including the regions of maximum ozone production and methane loss, as well as in the relationship between photolysis and these reactivities. Unique, possibly aberrant, features are identified for each model, providing a benchmark for photochemical module development. Among the 6 models tested here, 3 are almost indistinguishable based on the inherent variability caused by clouds, and thus we identify 4, effectively distinct, chemical models. Based on this work, we suggest that water vapor differences in model simulations of past and future atmospheres may be a cause of the different evolution of tropospheric O3 and CH4, and lead to different chemistry-climate feedbacks across the models.

greenhouse gases↗

Investigation of Global Particulate Nitrate from the AeroCom Phase III Experiment

An assessment of global particulate nitrate and ammonium aerosol based on simulations from nine models participating in the Aerosol Comparisons between Observations and Models (AeroCom) phase III study is presented. A budget analysis was conducted to understand the typical magnitude, distribution, and diversity of the aerosols and their precursors among the models. To gain confidence regarding model performance, the model results were evaluated with various observations globally, including ground station measurements over North America, Europe, and east Asia for tracer concentrations and dry and wet depositions, as well as with aircraft measurements in the Northern Hemisphere mid-to-high latitudes for tracer vertical distributions. Given the unique chemical and physical features of the nitrate occurrence, we further investigated the similarity and differentiation among the models by examining (1) the pH-dependent NH3 wet deposition; (2) the nitrate formation via heterogeneous chemistry on the surface of dust and sea salt particles or thermodynamic equilibrium calculation including dust and sea salt ions; and (3) the nitrate coarse-mode fraction (i.e., coarse/total). It is found that HNO3, which is simulated explicitly based on full O3-HOx-NOx-aerosol chemistry by all models, differs by up to a factor of 9 among the models in its global tropospheric burden. This partially contributes to a large difference in NO3(-), whose atmospheric burden differs by up to a factor of 13. The atmospheric burdens of NH3 and NHC 4 differ by 17 and 4, respectively. Analyses at the process level show that the large diversity in atmospheric burdens of NO3(-), NH3, and NHC4(+) is also related to deposition processes. Wet deposition seems to be the dominant process in determining the diversity in NH3 and NHC 4 lifetimes. It is critical to correctly account for contributions of heterogeneous chemical production of nitrate on dust and sea salt, because this process overwhelmingly controls atmospheric nitrate production (typically greater than 80 %) and determines the coarse- and fine-mode distribution of nitrate aerosol.

Ammonium aerosol based on simulations↗

Causes of Interannual Variability over the Southern Hemispheric Tropospheric Ozone Maximum

We examine the relative contribution of processes controlling the interannual variability (IAV) of tropospheric ozone over four sub-regions of the southern hemispheric tropospheric ozone maximum (SHTOM) over a 20-year period. Our study is based on hindcast simulations from the National Aeronautics and Space Administration Global Modeling Initiative chemistry transport model (NASA GMI-CTM) of tropospheric and stratospheric chemistry, driven by assimilated Modern Era Retrospective Analysis for Research and Applications (MERRA) meteorological fields. Our analysis shows that over SHTOM region, the IAV of the stratospheric contribution is the most important factor driving the IAV of upper tropospheric ozone (270 hectopascals), where ozone has a strong radiative effect. Over the South Atlantic region, the contribution from surface emissions to the IAV of ozone exceeds that from stratospheric input at and below 430 hectopascals. Over the South Indian Ocean, the IAV of stratospheric ozone makes the largest contribution to the IAV of ozone with little or no influence from surface emissions at 270 and 430 hectopascals in austral winter. Over the tropical South Atlantic region, the contribution from IAV of stratospheric input dominates in austral winter at 270 hectopascals and drops to less than half but is still significant at 430 hectopascals. Emission contributions are not significant at these two levels. The IAV of lightning over this region also contributes to the IAV of ozone in September and December. Over the tropical southeastern Pacific, the contribution of the IAV of stratospheric input is significant at 270 and 430 hectopascals in austral winter, and emissions have little influence.

Global Modeling Initiative chemistry transport mod↗

Quantifying the Causes of Differences in Tropospheric OH Within Global Models

The hydroxyl radical (OH) is the primary daytime oxidant in the troposphere and provides the main loss mechanism for many pollutants and greenhouse gases, including methane (CH4). Global mean tropospheric OH differs by as much as 80% among various global models, for reasons that are not well understood. We use neural networks (NNs), trained using archived output from eight chemical transport models (CTMs) that participated in the Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate, Chemistry, Aerosols and Transport Model Intercomparison Project (POLMIP), to quantify the factors responsible for differences in tropospheric OH and resulting CH4 lifetime (Tau CH4) between these models. Annual average Tau CH4, for loss by OH only, ranges from 8.0 to 11.6 years for the eight POLMIP CTMs. The factors driving these differences were quantified by inputting 3-D chemical fields from one CTM into the trained NN of another CTM. Across all CTMs, the largest mean differences in Tau CH4 (Delta Tau CH4) result from variations in chemical mechanisms (Delta Tau CH4 = 0.46 years), the photolysis frequency (J) of O3 yields O(D-1) (0.31 years), local O3 (0.30 years), and CO (0.23 years). The Delta Tau CH4 due to CTM differences in NO(x) (NO + NO2) is relatively low (0.17 years), although large regional variation in OH between the CTMs is attributed to NO(x). Differences in isoprene and J(NO2) have negligible overall effect on globally averaged tropospheric OH, although the extent of OH variations due to each factor depends on the model being examined. This study demonstrates that NNs can serve as a useful tool for quantifying why tropospheric OH varies between global models, provided that essential chemical fields are archived.

Surface Measurements and Models↗

An Observationally Constrained Evaluation of the Oxidative Capacity in the Tropical Western Pacific Troposphere

Hydroxyl radical (OH) is the main daytime oxidant in the troposphere and determines the atmospheric lifetimes of many compounds. We use aircraft measurements of O3, H2O, NO, and other species from the Convective Transport of Active Species in the Tropics (CONTRAST) field campaign, which occurred in the tropical western Pacific (TWP) during January-February 2014, to constrain a photochemical box model and estimate concentrations of OH throughout the troposphere. We find that tropospheric column OH (OHCOL) inferred from CONTRAST observations is 12 to 40% higher than found in chemical transport models (CTMs), including CAM-chem-SD run with 2014 meteorology as well as eight models that participated in POLMIP (2008 meteorology). Part of this discrepancy is due to a clear-sky sampling bias that affects CONTRAST observations; accounting for this bias and also for a small difference in chemical mechanism results in our empirically based value of OHCOL being 0 to 20% larger than found within global models. While these global models simulate observed O3 reasonably well, they underestimate NOx (NO +NO2) by a factor of 2, resulting in OHCOL approx.30% lower than box model simulations constrained by observed NO. Underestimations by CTMs of observed CH3CHO throughout the troposphere and of HCHO in the upper troposphere further contribute to differences between our constrained estimates of OH and those calculated by CTMs. Finally, our calculations do not support the prior suggestion of the existence of a tropospheric OH minimum in the TWP, because during January-February 2014 observed levels of O3 and NO were considerably larger than previously reported values in the TWP.

Hydroxyl radical↗

Comparisons of Observations with Results from 3D Simulations and Implications for Predictions of Ozone Recovery

Although chemistry and transport models (CTMs) include the same basic elements (photo- chemical mechanism and solver, photolysis scheme, meteorological fields, numerical transport scheme), they produce different results for the future recovery of stratospheric ozone as chlorofluorcarbons decrease. Three simulations will be contrasted: the Global Modeling Initiative (GMI) CTM driven by a single year\'s winds from a general circulation model; the GMI CTM driven by a single year\'s winds from a data assimilation system; the NASA GSFC CTM driven by a winds from a multi-year GCM simulation. CTM results for ozone and other constituents will be compared with each other and with observations from ground-based and satellite platforms to address the following: Does the simulated ozone tendency and its latitude, altitude and seasonal dependence match that derived from observations? Does the balance from analysis of observations? Does the balance among photochemical processes match that expected from observations? Can the differences in prediction for ozone recovery be anticipated from these comparisons?

Douglass, Anne R.↗

The minor stratospheric warming of January 1989 - Results from STRATAN, a stratospheric-tropospheric data assimilation system

Using a stratospheric-tropospheric data assimilation system, referred to as STRATAN, a minor sudden stratospheric warming that occurred in January 1989 is investigated. The event had a maximum influence on the stratospheric circulation near 2 hPa. The zonal mean circulation reversed briefly in the polar region as the temperature increased 34 K in 3 days. The cause of the warming is shown to be the rapid development and subsequent movement of a warm anomaly, which initially developed in the midlatitudes. The development of the warm anomaly is caused by adiabatic descent, and the dissipation by radiative cooling. A brief comparison with the NMC analysis and temperature sounding data is also presented.

Steenrod, Stephen D.↗

A method of calculating the total flow from a given sea surface topography

Using a simple dynamical model of a wind-driven ocean circulation of the Stommel type, and an analytical basis developed to objectively analyze the sea surface height residuals from an altimeter and, in the process, to determine the total flow instead of just the near surface geostrophic component associated with the given sea surface topography. The method is based on first deriving the solution to the forced problem for a given wind stress required to develop a hypothetical true or perfect data field and to establishing the basis for the objective analysis. The stream function and the surface height field for the forced problem are developed in terms of certain characteristic functions with the same expansion coefficients for both fields. These characteristic functions are simply the solutions for a homogeneous elliptic equation for the stream function and the solutions of an inhomogeneous balance equation for the height field. For the objective analysis, using a sample of randomly selected height values from the true data field, the height field characteristic functions are used to fit the given topography in a least squares sense. The resulting expansion coefficients then permit the synthesis of the total flow field via the stream function characteristic modes and the solution is perfectly well behaved even along the equator. The method of solution is easily adaptable to realistic ocean basis by straight forward numerical methods. The analytical basis of the theory and the results for an ideal rectangular basin on a beta plane are described.

Rao, Desiraju B.↗

Tidal estimation in the Atlantic and Indian Oceans, 3 deg x 3 deg solution

An estimation technique was developed to extrapolate tidal amplitudes and phases over entire ocean basins using existing gauge data and the altimetric measurements provided by satellite oceanography. The technique was previously tested. Some results obtained by using a 3 deg by 3 deg grid are presented. The functions used in the interpolation are the eigenfunctions of the velocity (Proudman functions) which are computed numerically from a knowledge of the basin's bottom topography, the horizontal plan form and the necessary boundary conditions. These functions are characteristic of the particular basin. The gravitational normal modes of the basin are computed as part of the investigation; they are used to obtain the theoretical forced solutions for the tidal constituents. The latter can provide the simulated data for the testing of the method and serve as a guide in choosing the most energetic functions for the interpolation.

Sanchez, Braulio V.↗