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Success of Montreal Protocol Demonstrated by Comparing High-Quality UV Measurements with “World Avoided” Calculations from Two Chemistry-Climate Models
The Montreal protocol on Substances that Deplete the ozone Layer has been hailed as the most successful environmental treaty ever (https://www.unenvironment.org/news-and-stories/story/montreal-protocol-triumph-treaty). Yet, although our main concern about ozone depletion is the subsequent increase in harmful solar UV radiation at the earth’s surface, no studies to date have demonstrated its effectiveness in that regard. Here we use long-term UV Index (UVI) data derived from high-quality UV spectroradiometer measurements to demonstrate its success in curbing increases in UV radiation. Without this landmark agreement, UVi values would have increased at mid-latitude locations by approximately 20% between the early 1990s and today and would approximately quadruple at mid-latitudes by 2100. In contrast, an analysis of UVI data from multiple clean-air sites shows that maximum daily UVI values have remained essentially constant over the last ~20 years in all seasons, and may even have decreased slightly in the southern hemisphere, especially in Antarctica, where effects of ozone depletion were larger. Reconstructions of the UVi from total ozone data show evidence of increasing UVI levels in the 1980s, but unfortunately, there are no high-quality UV measurements available prior to the early 1990s to confirm these increases with direct observations.
File Specification for MERRA-2 Stratospheric Composition Reanalysis of Aura MLS (M2-SCREAM)
This document provides a brief description of the output collections from the MERRA-2 Stratospheric Composition Reanalysis of the Aura Microwave Limb Sounder (M2-SCREAM) produced at NASA’s Global Modeling and Assimilation Office. These data are generated by assimilating retrievals from the Microwave Limb Sounder (MLS) and the Ozone Monitoring Instrument (OMI) into the Global Earth Observing System (GEOS) Constituent Data Assimilation System (CoDAS) driven by meteorological fields from MERRA-2. M2-SCREAM assimilates hydrochloric acid (HCl), nitric acid (HNO3), stratospheric water vapor (H2O), nitrous oxide (N2O) and ozone with a system equipped with a version of the GEOS general circulation model and a stratospheric chemistry model, StratChem. Assimilated fields are provided globally at 0.5° by 0.625° resolution at three-hourly frequencies from 2004/09/01 to 2021. Assimilation uncertainties for each of the assimilated constituents are calculated from the CoDAS statistical output (Wargan et al., 2022) and provided as global full-resolution three-dimensional monthly files.
A Method for Estimating Global Subgrid‐Scale Orographic Gravity‐Wave Temperature Perturbations in Chemistry‐Climate Models
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Evaluation of the N 2 O Rate of Change to Understand the Stratospheric Brewer‐Dobson Circulation in a Chemistry‐Climate Model
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Intercomparison Between Surrogate, Explicit, and Full Treatments of VSL Bromine Chemistry Within the CAM‐Chem Chemistry‐Climate Model
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Atmospheric Chemistry Surrogate Modeling With Sparse Identification of Nonlinear Dynamics
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The Influences of Airmass Histories on Radical Species During POLARIS
The POLARIS mission focused on understanding the processes associated with the decrease of polar stratospheric ozone from spring to fall at high latitudes. This decrease is linked primarily to in situ photochemical destruction by reactive nitrogen species, NO and NO2, which also control other catalytic loss cycles. Steady state models have been used to test photochemistry and radical behavior but are not always adequate in simulating radical species observations. In some cases, air mass history can be important and trajectory models give an improved simulation of the radical species. Trajectory chemistry models, however, still consistently underestimate NO and NO2 abundances compared to measurements along the ER-2 flight track. The Goddard chemistry on trajectory model has been used to test updated rate constants for NO2 + OH, NO2 + O and OH + HNO3, key reactions that affect NO and NO2 abundances. We present comparisons between the modified Goddard chemistry on trajectory model, the JPL steady state model and observations from selected flights.
Modeling free convective gravitational effects in chemical vapor deposition
In this paper, a combined fluid-mechanics, mass-transport, and chemistry model describing CVD in an open-tube atmospheric-pressure flow reactor is developed. The model allows gas-phase reactions to proceed to equilibrium and accounts for finite reaction rates at the surface of the deposition substrate. This model is a useful intermediate step toward a model employing fully rate-limited chemistry. The model is used to predict the effects of free convection on flow patterns, temperature and species-concentration profiles, and local deposition rates for silicon deposited by silane pyrolysis. These results are discussed in terms of implications for CVD of silicon and other compounds, microgravity studies, and techniques for testing and validating the model.
A study of reacting free and ducted hydrogen/air jets
The mixing and reaction of a supersonic jet of hydrogen in coaxial free and ducted high temperature test gases were investigated. The importance of chemical kinetics on computed results, and the utilization of free-jet theoretical approaches to compute enclosed flow fields were studied. Measured pitot pressure profiles were correlated by use of a parabolic mixing analysis employing an eddy viscosity model. All computations, including free, ducted, reacting, and nonreacting cases, use the same value of the empirical constant in the viscosity model. Equilibrium and finite rate chemistry models were utilized. The finite rate assumption allowed prediction of observed ignition delay, but the equilibrium model gave the best correlations downstream from the ignition location. Ducted calculations were made with finite rate chemistry; correlations were, in general, as good as the free-jet results until problems with the boundary conditions were encountered.
Multi-model Mean Nitrogen and Sulfur Deposition from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP): Evaluation Historical and Projected Changes
We present multi-model global datasets of nitrogen and sulfate deposition covering time periods from 1850 to 2100, calculated within the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The computed deposition fluxes are compared to surface wet deposition and ice-core measurements. We use a new dataset of wet deposition for 2000-2002 based on critical assessment of the quality of existing regional network data. We show that for present-day (year 2000 ACCMIP time-slice), the ACCMIP results perform similarly to previously published multi-model assessments. For this time slice, we find a multi-model mean deposition of 50 Tg(N) yr1 from nitrogen oxide emissions, 60 Tg(N) yr1 from ammonia emissions, and 83 Tg(S) yr1 from sulfur emissions. The analysis of changes between 1980 and 2000 indicates significant differences between model and measurements over the United States but less so over Europe. This difference points towards misrepresentation of 1980 NH3 emissions over North America. Based on ice-core records, the 1850 deposition fluxes agree well with Greenland ice cores but the change between 1850 and 2000 seems to be overestimated in the Northern Hemisphere for both nitrogen and sulfur species. Using the Representative Concentration Pathways to define the projected climate and atmospheric chemistry related emissions and concentrations, we find large regional nitrogen deposition increases in 2100 in Latin America, Africa and parts of Asia under some of the scenarios considered. Increases in South Asia are especially large, and are seen in all scenarios, with 2100 values more than double 2000 in some scenarios and reaching 1300 mg(N) m2 yr1 averaged over regional to continental scale regions in RCP 2.6 and 8.5, 3050 larger than the values in any region currently (2000). The new ACCMIP deposition dataset provides novel, consistent and evaluated global gridded deposition fields for use in a wide range of climate and ecological studies.
Multi-Model Mean Nitrogen and Sulfur Deposition from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP): Evaluation of Historical and Projected Future Changes
We present multi-model global datasets of nitrogen and sulfate deposition covering time periods from 1850 to 2100, calculated within the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The computed deposition fluxes are compared to surface wet deposition and ice core measurements.We use a new dataset of wet deposition for 2000-2002 based on critical assessment of the quality of existing regional network data. We show that for present day (year 2000 ACCMIP time slice), the ACCMIP results perform similarly to previously published multi-model assessments. For this time slice, we find a multimodel mean deposition of approximately 50 Tg(N) yr−1 from nitrogen oxide emissions, 60 Tg(N) yr−1 from ammonia emissions, and 83 Tg(S) yr−1 from sulfur emissions. The analysis of changes between 1980 and 2000 indicates significant differences between model and measurements over the United States but less so over Europe. This difference points towards a potential misrepresentation of 1980 NH3 emissions over North America. Based on ice core records, the 1850 deposition fluxes agree well with Greenland ice cores, but the change between 1850 and 2000 seems to be overestimated in the Northern Hemisphere for both nitrogen and sulfur species. Using the Representative Concentration Pathways (RCPs) to define the projected climate and atmospheric chemistry related emissions and concentrations, we find large regional nitrogen deposition increases in 2100 in Latin America, Africa and parts of Asia under some of the scenarios considered. Increases in South Asia are especially large, and are seen in all scenarios, with 2100 values more than double their 2000 counterpart in some scenarios and reaching >1300 mg(N)m−2 yr−1 averaged over regional to continental-scale regions in RCP 2.6 and 8.5, 30-50% larger than the values in any region currently (circa 2000). However, sulfur deposition rates in 2100 are in all regions lower than in 2000 in all the RCPs. The new ACCMIP multimodel deposition dataset provides state-of-the-science, consistent and evaluated time slice (spanning 1850-2100) global gridded deposition fields for use in a wide range of climate and ecological studies.
GMI-IPS: Processing & Visualization Software Used in ATom DC-8 Aircraft Studies
NASA's Atmospheric Tomography Mission (ATom) deployed in each of the four seasons during 2016-2018, the DC-8 aircraft in order to establish global-scale datasets intended to improve the representation of chemically reactive gases in global atmospheric chemistry models (ACMs). The Global Modeling Initiative (GMI) executed simulations for each ATom flight using the GMI Chemistry Transport Model (GMI-CTM) to provide species concentrations of chemical gases along the DC-8 flight transects. To solve the problem of translating the GMI-CTM simulation data to the unique spatial resolutions of each ATom flight, the GMI ICARTT Processing Software (GMI-IPS) was developed.The GMI-IPS is written in Python and provides data processing, flight extraction, and visualization support for aircraft research projects using ICARTT format, which is a standard format for airborne instrument data. Additionally, the GMI-IPS interpolates global gridded model data from Hierarchical Data Format (HDF) to ICARTT compatible flight transects. Software classes for instruments and collections provided by the ATom DC-8 aircraft such as MER10, MMS, etc. are derived from a common base class. Other functionality provided by the GMI-IPS are: deriving missing flight entries along a transect, reading ICARTT entries from file, and providing Python data structures for storing flight and model information, and more.The GMI-IPS is GIT source controlled, has approximately 30,000 lines of code, and supports parallelization across data collections. It delivered GMI-CTM data for more than forty distinct DC-8 aircraft flights that took place under ATom. The output ICARTT files adhere to format standard V1.1, and pass the scan utility provided by NASA LaRC Airborne Science Data for Atmospheric Composition. This presentation will include a software and methods overview, and results from ATom, including assessments using the GMI-CTM showing how well observations from ATom flight transects represent a broader region.
Analysis of turbulent free jet hydrogen-air diffusion flames with finite chemical reaction rates
The nonequilibrium flow field resulting from the turbulent mixing and combustion of a supersonic axisymmetric hydrogen jet in a supersonic parallel coflowing air stream is analyzed. Effective turbulent transport properties are determined using the (K-epsilon) model. The finite-rate chemistry model considers eight reactions between six chemical species, H, O, H2O, OH, O2, and H2. The governing set of nonlinear partial differential equations is solved by an implicit finite-difference procedure. Radial distributions are obtained at two downstream locations of variables such as turbulent kinetic energy, turbulent dissipation rate, turbulent scale length, and viscosity. The results show that these variables attain peak values at the axis of symmetry. Computed distributions of velocity, temperature, and mass fraction are also given. A direct analytical approach to account for the effect of species concentration fluctuations on the mean production rate of species (the phenomenon of unmixedness) is also presented. However, the use of the method does not seem justified in view of the excessive computer time required to solve the resulting system of equations.