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Rodriguez, Jose M.

Publications and source records attributed to Rodriguez, Jose M..

At least 19 records

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

Interpreting Space-Based Trends in Carbon Monoxide with Multiple Models

We use a series of chemical transport model and chemistry climate model simulations to investigate the observed negative trends in MOPITT CO over several regions of the world, and to examine the consistency of timedependent emission inventories with observations. We find that simulations driven by the MACCity inventory, used for the Chemistry Climate Modeling Initiative (CCMI), reproduce the negative trends in the CO column observed by MOPITT for 2000-2010 over the eastern United States and Europe. However, the simulations have positive trends over eastern China, in contrast to the negative trends observed by MOPITT. The model bias in CO, after applying MOPITT averaging kernels, contributes to the model-observation discrepancy in the trend over eastern China. This demonstrates that biases in a model's average concentrations can influence the interpretation of the temporal trend compared to satellite observations. The total ozone column plays a role in determining the simulated tropospheric CO trends. A large positive anomaly in the simulated total ozone column in 2010 leads to a negative anomaly in OH and hence a positive anomaly in CO, contributing to the positive trend in simulated CO. These results demonstrate that accurately simulating variability in the ozone column is important for simulating and interpreting trends in CO.

carbon monoxide

Changes in Global Tropospheric OH Expected as a Result of Climate Change Over the Last Several Decades

The oxidizing capacity of the troposphere is controlled primarily by the abundance of hydroxyl radical (OH). The global mean concentration of OH, [OH]_GLOBAL, inferred from measurements of methyl chloroform, has remained relatively constant during the past several decades, despite rising levels of CH4 that should have led to a steady decline. Here we examine other factors that may have affected [OH]_GLOBAL, such as the changing overhead burden of stratospheric O3 using observations from OMI, TOMS and SBUV; rising tropospheric H2O using observations from AIRS and reanalysis fields from MERRA; and widening of the climatological tropics using widening rate estimates from the literature and global OH fields from the GEOS Chemistry-Climate Model. Our analysis suggests these factors may have contributed a positive trend to [OH]_GLOBAL large enough to counter the decrease due to CH4.

Climate Change

Concentration Effects and Ion Properties Controlling the Fractionation of Halides during Aerosol Formation

During the aerosolization process at the sea surface, halides are incorporated into aerosol droplets, where they may play an important role in tropospheric ozone chemistry. Although this process may significantly contribute to the formation of reactive gas phase molecular halogens, little is known about the environmental factors that control how halides selectively accumulate at the air−water interface. In this study, the production of sea spray aerosol is simulated using electrospray ionization (ESI) of 100 nM equimolar solutions of NaCl, NaBr, NaI, NaNO2, NaNO3, NaClO4, and NaIO4. The microdroplets generated are analyzed by mass spectrometry to study the comparative enrichment of anions (f (Isub x-)) and their correlation with ion properties. Although no correlation exists between f (sub x-) and the limiting equivalent ionic conductivity, the correlation coefficient of the linear fit with the size of the anions R(sub x-), dehydration free-energy ΔGdehyd, and polarizability alpha, follows the order: (R(sub x-)(exp −2)) > (R(sub x-)(exp −1)) >(R(sub x-) > delta G(sub dehyd) > alpha. The same pure physical process is observed in H2O and D2O. The factor f (sub x-) does not change with pH (6.8−8.6), counterion (Li+, Na+, K+, and Cs+) substitution effects, or solvent polarity changes in methanol − and ethanol−water mixtures (0 <= xH2O <= 1). Sodium polysorbate 20 surfactant is used to modify the structure of the interface. Despite the observed enrichment of I− on the air−water interface of equimolar solutions, our results of seawater mimic samples agree with a model in which the interfacial composition is increasingly enriched in I− < Br− < Cl− over the oceanic boundary layer due to concentration effects in sea spray aerosol formation.

iodine

Assessment of the Effects of High-Speed Aircraft in the Stratosphere: 1998

This report assesses the potential atmospheric impacts of a proposed fleet of high-speed civil transport (HSCT) aircraft. The purpose of the report is to assess the effects of HSCT's on atmospheric composition and climate in order to provide a scientific basis for making technical, commercial, and environmental policy decisions regarding the HSCT fleet. The work summarized here was carried out as part of NASA's Atmospheric Effects of Aviation Project (a component of the High-Speed Research Program) as well as other NASA, U.S., and international research programs. The principal focus is on change in stratospheric ozone concentrations. The impact on climate change is also a concern. The report describes progress in understanding atmospheric processes, the current state of understanding of HSCT emissions, numerical model predictions of HSCT impacts, the principal uncertainties in atmospheric predictions, and the associated sensitivities in predicted effects of HSCT'S.

Kawa, S. Randolph

Nitrogen Species in the Post-Pinatubo Stratosphere: Model Analysis Utilizing UARS Measurements

We present an analysis of the impact of heterogeneous chemistry on the partitioning of nitrogen species measured by the Upper Atmosphere Research Satellite (UARS) instruments. The UARS measurements utilized include N2O, HNO3, and ClONO2 from the cryogenic limb array etalon spectrometer (CLAES), version 7 (v.7), and temperature, methane, ozone, H2O, HCl, NO and NO2 from the halogen occultation experiment (HALOE), version 18. The analysis is carried out for the UARS data obtained between January 1992 and September 1994 in the 100- to 1-mbar (approx. 17-47 km) altitude range and over 10 deg latitude bins from 70 deg S to 70 deg N. The spatiotemporal evolution of aerosol surface area density (SAD) is adopted from analysis of the Stratospheric Aerosol and Gas Experiment (SAGE) II data. A diurnal steady state photochemical box model, constrained by the temperature, ozone, H2O, CH4, aerosol SAD, and columns of O2 and O3 above the point of interest, has been used as the main tool to analyze these data. Total inorganic nitrogen (NOY) is obtained by three different methods: (1) as a sum of the UARS-measured NO, NO2, HNO3, and ClONO2; (2) from the N2O-NOY correlation; and (3) from the CH4-NOY correlation. To validate our current understanding of stratospheric heterogeneous chemistry for post-Pinatubo conditions, the model-calculated monthly averaged NO(x)/NO(y) ratios and the NO, NO2, and HNO3 profiles are compared with the UARS-derived data. In general, the UARS-constrained box model captures the main features of nitrogen species partitioning in the post-Pinatubo years, such as recovery of NO(x) after the eruption, their seasonal variability and vertical profiles. However, the model underestimates the NO2 content, particularly in the 30- to 7-mbar (approx. 23-32 km) range. Comparisons of the calculated temporal behavior of the partial columns of NO2 and HNO3 and ground-based measurements at 45 deg S and 45 deg N are also presented. Our analysis indicates that ground-based and HALOE v.18 measurements of the NO2 vertical columns are consistent within the range of their uncertainties and are systematically higher (up to 50%) than the model results at midlatitudes in both hemispheres. Reasonable agreement is obtained for HNO3 columns at 45 deg S, suggesting some problems with nitrogen species partitioning in the model. Outstanding uncertainties are discussed.

Danilin, Michael Y.

Nitrogen Species in the Post-Pinatubo Stratosphere: Model Analysis Utilizing UARS Measurements

We present an analysis of the impact of heterogeneous chemistry on the partitioning of nitrogen species measured by the Upper Atmosphere Research Satellite (UARS) instruments. The UARS measurements utilized include N2O, HNO3, and ClONO2 from the cryogenic limb array etalon spectrometer (CLAES), version 7 (v.7), and temperature, methane, ozone, H2O, HCl, NO and NO2 from the halogen occultation experiment (HALOE), version 18. The analysis is carried out for the UARS data obtained between January 1992 and September 1994 in the 100-to 1-mbar (approx. 17-47 km) altitude range and over 10 degrees latitude bins from 70 S to 70 N. The spatiotemporal evolution of aerosol surface area density (SAD) is adopted from analysis of the Stratospheric Aerosol and Gas Experiment (SAGE) II data. A diurnal steady state photochemical box model, constrained by the temperature, ozone, H2O, CH4, aerosol SAD, and columns of O2 and O3 above the point of interest, has been used as the main tool to analyze these data. Total inorganic nitrogen (NOy) is obtained by three different methods: (1) as a sum of the UARS-measured NO, NO2, HNO3, and ClONO2; (2) from the N2O-NOy correlation, and (3) from the CH4-NOy correlation. To validate our current understanding of stratospheric heterogeneous chemistry for post-Pinatubo conditions, the model-calculated monthly averaged NOx/NOy ratios and the NO, NO2, and HNO3 profiles are compared with the UARS-derived data. In general, the UARS-constrained box model captures the main features of nitrogen species partitioning in the post-Pinatubo years, such as recovery of NOx after the eruption, their seasonal variability and vertical profiles. However, the model underestimates the NO2 content, particularly in the 30- to 7-mbar (approx.23-32 km) range. Comparisons of the calculated temporal behavior of the partial columns of NO2 and HNO3 and ground-based measurements at 45 S and 45 N are also presented. Our analysis indicates that ground-based and HALOE v.18 measurements of the NO2 vertical columns are consistent within the range of their uncertainties and are systematically higher (up to 50%) than the model results at midlatitudes in both hemispheres. Reasonable agreement is obtained for HNO3 columns at 45 S, suggesting some problems with nitrogen species partitioning in the model. Outstanding uncertainties are discussed.

Danilin, Michael Y.

Ozone Depletion Potential of CH3Br

The ozone depletion potential (ODP) of methyl bromide (CH3Br) can be determined by combining the model-calculated bromine efficiency factor (BEF) for CH3Br and its atmospheric lifetime. This paper examines how changes in several key kinetic data affect BEF. The key reactions highlighted in this study include the reaction of BrO + HO2, the absorption cross section of HOBr, the absorption cross section and the photolysis products of BrONO2, and the heterogeneous conversion of BrONO2 to HOBr and HNO3 on aerosol particles. By combining the calculated BEF with the latest estimate of 0.7 year for the atmospheric lifetime of CH3Br, the likely value of ODP for CH3Br is 0.39. The model-calculated concentration of HBr (approx. 0.3 pptv) in the lower stratosphere is substantially smaller than the reported measured value of about 1 pptv. Recent publications suggested models can reproduce the measured value if one assumes a yield for HBr from the reaction of BrO + OH or from the reaction of BrO + HO2. Although the evaluation concluded any substantial yield of HBr from BrO + HO2 is unlikely, for completeness, we calculate the effects of these assumed yields on BEF for CH3Br. Our calculations show that the effects are minimal: practically no impact for an assumed 1.3% yield of HBr from BrO + OH and 10% smaller for an assumed 0.6% yield from BrO + HO2.

Ko, Malcolm K. W.

Stratospheric Cooling and Arctic Ozone Recovery

We present sensitivity studies using the AER box model for an idealized parcel in the lower stratosphere at 70 deg N during winter/spring with different assumed stratospheric cooling and chlorine loadings. Our calculations show that stratospheric cooling could further deplete ozone via increased polar stratospheric cloud (PSC) formation and retard its expected recovery even with the projected chlorine loading decrease. We introduce the concept of chlorine-cooling equivalent and show that a 1 K cooling could provide the same local ozone depletion as an increase of chlorine by 0.4 - 0.7 ppbv for the scenarios considered. Thus, sustained stratospheric cooling could further reduce Arctic ozone content and delay the anticipated ozone recovery in the Northern Hemisphere even with the realization of the Montreal Protocol and its Amendments.

Danilin, Michael Y.

The atmospheric effects of stratospheric aircraft: A fourth program report

This document presents the fourth report from the Atmospheric Effects of Stratospheric Aircraft (AESA) component of NASA's High-Speed Research Program (HSRP). Market and technology considerations continue to provide an impetus for high-speed civil transport research. A recent AESA interim assessment report and a review of that report have shown that considerable uncertainty still exists about the possible impact of aircraft on the atmosphere. The AESA has been designed to develop the body of scientific knowledge necessary for the evaluation of the impact of stratospheric aircraft on the atmosphere. The first Program report presented the basic objectives and plans for AESA. This fourth report comes after the interim assessment and sets forth directions for the 1995 assessment at the end of AESA Phase 1. It also sets forth the goals and directions for AESA Phase 2, as reported at the 1994 Atmospheric Effects of Aviation Project (AEAP) annual meeting held in June. The focus of the Phase 2 effort is to obtain the best possible closure on the outstanding problems identified in the interim assessment and NASA/NRC review. Topics discussed in this report include how high-speed civil transports (HSCT) might affect stratospheric ozone, emissions scenarios and databases to assess potential atmospheric effects from HSCT's, calculated results from 2-D zonal mean models using emissions data, engine trace constituent measurements.

Stolarski, Richard S.

Effect of lightning on the concentration of odd nitrogen species in the lower stratosphere: An update

Revised model estimates of the effect of lightning on the lower stratospheric NOy are presented. Several changes in the Atmospheric and Environmental Research Incorporated model were made since the last evaluation of the impact of lightning. Improvements were made in the model circulation and location of tropopause in the tropics, which is now calculated from the National Meteorological Center temperature data. Changes in model circulation reduced the mass flux from the troposphere to the tropical stratosphere. The calculated mass fluxes are found to agree better with some recent estimates. The circulation changes also reduced the advective mass flux from the tropical lower stratosphere to the midlatitudes. The change in circulation and the change in the tropopause height lead to increases in the calculated concentration of N2O, O3 and NOy in the tropical lower stratosphere. The effect of lightning is to increase the calculated concentration of NOy around 64 mbar by a factor of 2, compared to a factor of 10 enhancement in the previous calculations. Comparison with the Stratosphere Troposphere Exchange Project 1987 data indicates that the inclusion of a lightning source brings the model results in closer agreement with the observations.

Kotamarthi, V. R.

Ozone response to enhanced heterogeneous processing after the eruption of Mt. Pinatubo

Increases in aerosol loading after the Pinatubo eruption are expected to cause additional ozone depletion. Even though aerosol loadings were highest in the winter of 1991-1992, recent analyses of satellite and ground-based ozone measurements indicate that ozone levels in the winter of 1992-1993 are the lowest recorded in recent years, raising the question of the mechanisms responsible for such behavior. We have incorporated aerosol surface areas derived from the Stratospheric Aerosol and Gas Experiment II (SAGE-II) measurements into our two-dimensional model. Inclusion of heterogeneous chemsitry on these enhanced aerosol surfaces yields maximum ozone reductions during the winter of 1992-1993 in the Northern Hemisphere, consistent with those derived from observations. This delayed behavior is due to the combination of the non-linear nature of the impact of heterogeneous reactions as a function of aerosol surface area, and the long time constants for ozone in the lower stratosphere. If heterogeneous mechanisms are primarily responsible for the low 1992-1993 ozone levels, we expect ozone concentrations to start recovering in 1994.

Rodriguez, Jose M.

Effects on stratospheric ozone from high-speed civil transport: Sensitivity to stratospheric aerosol loading

The potential impact of high-speed civil transport (HSCT) aircraft emissions on stratospheric ozone and the sensitivity of these results to changes in aerosol loading are examined with a two-dimensional model. With aerosols fixed at background levels, calculated ozone changes due to HSCT aircraft emissions range from negligible up to 4-6% depletions in column zone at northern high latitudes. The magnitude of the ozone change depends mainly on the NO(x) increase due to aircraft emissions, which depends on fleet size, cruise altitude, and engine design. The partitioning of the odd nitrogen species in the lower stratosphere among NO, NO2, N2O5, is strongly dependent on the concentration of sulfuric acid aerosol particles, and thus the sensitivity of O3 to NO(x) emissions changes when the stratospheric aerosol loading changes. Aerosol concentrations 4 times greater than background levels have not been unusual in the last 2 decades. Our model results show that a factor of 4 increase in aerosol loading would significantly reduce the calculated ozone depletion due to HSCT emissions. Because of the neutral variabiltiy of stratospheric aerosols, the possible impact of HSCT emissions on ozone must be viewed as a range of possible results.

Weisenstein, Debra K.

Role of heterogeneous conversion of N2O5 on sulphate aerosols in global ozone losses

The reaction rate of N2O5 on sulphate aerosols is included in a model to predict global ozone loss and the column abundances of atmospheric gases. Because the reaction of N2O5 and the aerosols can take place in the stratospheric sulphate aerosol layer, it is included in the 2D model so that the results can be compared to abundances derived from satellite data and ground-based measurements. The N2O5/sulphate reaction is the only heterogeneous reaction in the model, in which aerosol loading is assumed to be constant and only diurnal values are examined. The decadal ozone trends resulting from calculations based on the model are found to be closer to the observed values. An important conclusion is that measurements of OH, ClO, HNO3, NO, and NO2 in the region of about 14-25 km are needed to examine significant changes in their abundances resulting from the inclusion of the N2O5/sulphate aerosol reaction.

Rodriguez, Jose M.

Effects of engine emissions from high-speed civil transport aircraft: A two-dimensional modeling study, part 1

The AER two-dimensional chemistry-transport model is used to study the effect on stratospheric ozone (O3) from operations of supersonic and subsonic aircraft. The study is based on six emission scenarios provided to AER. The study showed that: (1) the O3 response is dominated by the portion of the emitted nitrogen compounds that is entrained in the stratosphere; (2) the entrainment is a sensitive function of the altitude at which the material is injected; (3) the O3 removal efficiency of the emitted material depends on the concentrations of trace gases in the background atmosphere; and (4) evaluation of the impact of fleet operations in the future atmosphere must take into account the expected changes in trace gas concentrations from other activities. Areas for model improvements in future studies are also discussed.

Ko, Malcolm K. W.

Effects of engine emissions from high-speed civil transport aircraft: A two-dimensional modeling study, part 2

The AER two-dimensional chemistry-transport model is used to study the effect of supersonic and subsonic aircraft operation in the 2010 atmosphere on stratospheric ozone (O3). The results show that: (1) the calculated O3 response is smaller in the 2010 atmosphere compared to previous calculations performed in the 1980 atmosphere; (2) with the emissions provided, the calculated decrease in O3 column is less than 1 percent; and (3) the effect of model grid resolution on O3 response is small provided that the physics is not modified.

Ko, Malcolm K. W.

PEM-West trajectory climatology and photochemical model sensitivity study prepared using retrospective meteorological data

Trajectory and photochemical model calculations based on retrospective meteorological data for the operations areas of the NASA Pacific Exploratory Mission (PEM)-West mission are summarized. The trajectory climatology discussed here is intended to provide guidance for flight planning and initial data interpretation during the field phase of the expedition by indicating the most probable path air parcels are likely to take to reach various points in the area. The photochemical model calculations which are discussed indicate the sensitivity of the chemical environment to various initial chemical concentrations and to conditions along the trajectory. In the post-expedition analysis these calculations will be used to provide a climatological context for the meteorological conditions which are encountered in the field.

Merrill, John T.

Impact of biomass burning on tropospheric CO and OH - A two-dimensional study

Results are presented from a 2D model of the troposphere and stratosphere which allows the derivation of a budget for CO, as well as the assessment of contributions from different sources in maintaining observed CO concentrations. Attention is given to the results of a time-dependent calculation which evaluates the impact of present-day biomass burning on CO, OH, and CH4, as well as the time constants for the system to respond to changes in the biomass source.

Rodriguez, Jose M.