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Prior to the SOLVE deployment, we modified and ran a chemical transport model (CTM) to set up a stratospheric climatology for 1 September 1999. During and immediately following the SOLVE deployments, we ran the model in near-real-time and used these results in conjunction with SOLVE observations to draw conclusions about stratospheric transport.
Observations of constituents from satellite, aircraft and sondes can be utilized to develop diagnostics of various aspects of tropical transport. These include tropical mid-latitude isolation, the seasonal transport from the upper tropical troposphere to the mid-latitude lowermost stratosphere, the seasonal cycle of the tropical total ozone and its variability. These diagnostics will be applied to constituent fields from an off-line chemistry and transport model (CTM) driven by winds from two sources. These are the Finite Volume Community Climate Model (FV-CCM), a general circulation model that uses the NCAR CCM physics and the Lin and Rood dynamical core, and an assimilation system developed by the Data Assimilation Office at the Goddard Space Flight Center that uses the FV-CCM at its core. Signatures of the quasi-biennial oscillation present in the observations will be emphasized to understand differences between the two model transports and the transport inferred from the observations.
Recent development in chemistry transport models (CTM) and in data assimilation systems (DAS) indicate impressive predictive capability for the movement of airparcels and the chemistry that goes on within these. This project was aimed at exploring the use of this capability to achieve improved retrieval of geophysical parameters from remote sensing data. The specific goal was to improve retrieval of the CLAES CH4 data obtained during the active north high latitude dynamics event of 18 to 25 February 1992. The model capabilities would be used: (1) rather than climatology to improve on the first guess and the a-priori fields, and (2) to provide horizontal gradients to include in the retrieval forward model. The retrieval would be implemented with the first forward DAS prediction. The results would feed back to the DAS and a second DAS prediction for first guess, a-priori and gradients would feed to the retrieval. The process would repeat to convergence and then proceed to the next day.
Chemical transport models (CTMs) must conserve mass to be useful for applications involving assessment of the effect of various pollutants on the troposphere and stratosphere. Furthermore, calculations of the evolution of constituents such as SF6 are used to evaluate overall model transport, and interpretation of such simulations is clouded if mass conservation is not assured. For realistic simulations or predictions, it is crucial that constituents are not produced or lost by transport or other processes in the CTMs. Analysis of CO2 and SF6 experiments using a CTM shows that problems with mass conservation can seriously degrade the simulations. Failure to conserve mass results from inconsistency of the surface pressure tendency and the divergence of horizontal mass flux when the model is forced by assimilated meteorological data. We have developed an effective method to eliminate the inconsistency by modifying the divergent part of the wind field. The changes in the wind fields are quite small but the impact on mass conservation is large. Parameterizations of physical processes such as convection or turbulent transport can also affect mass conservation. The lack of conservation is small but accumulates when integrations are lengthy such as required for SF6. This lack of conservation is found using winds from either a GCM or from an assimilation system. A simple adjustment removes much of the inaccuracy in the convective parameterization. A CO2 simulation using assimilated winds from the most recent version of the Goddard Earth Observing System Data Assimilation System will be used to illustrate the impact of these transport improvements.
This report presents the Cryogenic Limb Array Etalon Spectrometer (CLAES) product improvement by use of the GSFC Data Assimilation System (DAS). The first task is to plug line of sight gradients derived from the CTM for 2/20/92 into the forward model of our retrieval software (RSW) in order to assess the impact on the retrieved quantities. The reporting period covers 12 May 2000 - 21 December 2000.
Since 1999 the DAO (Data Assimilation Office) at NASA Goddard has operationally assimilated ozone measurements in near real time. Currently, the assimilation system analyzes SBUV profile and total column measurements using an off line CTM with parameterized chemistry within the 3D-PSAS algorithm. During the last year the assimilation system was modified to either monitor or actively assimilate MLS (Microwave Limb Sounder) measurements in conjunction with the active assimilation of TOMS total column and SBUV profiles. It is expected that the active assimilation of MLS profiles will improve analysis results in two ways. First, there should be an improvement in the vertical resolution. Second, there should be an improvement in regions where SBUV measurements do not exist (such as in the polar night). A series of experiments using UARS (Upper Atmospheric Research Satellite) MLS data from December 1991 to March 1992 were run. In these experiments MLS data was either monitored in conjunction with active assimilation of the SBUV profile and TOMS total column measurements, or some combination of MLS, TOMS, and SBUV observations was actively assimilated. Monitoring of MLS data indicated that the MLS observations contain verifiable information that should improve the vertical structure of the analysis results, especially below the ozone peak and above the tropopause. The monitoring also substantiated the potential to improve the assimilation in the polar night. Active assimilation of MLS data does indeed improve the analysis results in these two ways, although the quality of the improvements is not uniform. This suggests that refinement of the specification of the error covariances might be needed to optimize the system. In addition it may be necessary to account for biases between the different sources of ozone information.
The PI has undertaken a theoretical analysis of the existence and nature of compact tracer-tracer relationships of the kind observed in the stratosphere, augmented with three-dimensional model simulations of stratospheric tracers (the latter being an extension of modeling work the group did during the SOLVE experiment). This work achieves a rigorous theoretical basis for the existence and shape of these relationships, as well as a quantitative theory of their width and evolution, in terms of the joint tracer-tracer PDF distribution. A paper on this work is almost complete and will soon be submitted to Rev. Geophys. We have analyzed lower stratospheric water in simulations with an isentropic-coordinate version of the MATCH transport model which we recently helped to develop. The three-dimensional structure of lower stratospheric water, in particular, attracted our attention: dry air is, below about 400K potential temperature, localized in the regions of the west Pacific and equatorial South America. We have been analyzing air trajectories to determine how air passes through the tropopause cold trap. This work is now being completed, and a paper will be submitted to Geophys. Res. Lett. before the end of summer. We are continuing to perform experiments with the 'MATCH' CTM, in both sigma- and entropy-coordinate forms. We earlier found (in collaboration with Dr Natalie Mahowald, and as part of an NSF-funded project) that switching to isentropic coordinates made a substantial improvement to the simulation of the age of stratospheric air. We are now running experiments with near-tropopause sources in both versions of the model, to see if and to what extent the simulation of stratosphere-troposphere transport is dependent on the model coordinate. Personnel Research is supervised by the PI, Prof. Alan Plumb. Mr William Heres conducts the tracer modeling work and performs other modeling tasks. Two graduate students, Ms Irene Lee and Mr Michael Ring, have been participating in the research.
A general circulation model (GCM) relies on various physical parameterizations and provides a solution to the atmospheric equations of motion. A data assimilation system (DAS) combines information from observations with a GCM forecast and produces analyzed meteorological fields that represent the observed atmospheric state. An off-line chemistry and transport model (CTM) can use winds and temperatures from a either a GCM or a DAS. The latter application is in common usage for interpretation of observations from various platforms under the assumption that the DAS transport represents the actual atmospheric transport. Here we compare the transport produced by a DAS with that produced by the particular GCM that is combined with observations to produce the analyzed fields. We focus on transport in the tropics and middle latitudes by comparing the age-of-air inferred from observations of SF6 and CO2 with the age-of-air calculated using GCM fields and DAS fields. We also compare observations of ozone, total reactive nitrogen, and methane with results from the two simulations. These comparisons show that DAS fields produce rapid upward tropical transport and excessive mixing between the tropics and middle latitudes. The unrealistic transport produced by the DAS fields may be due to implicit forcing that is required by the assimilation process when there is bias between the GCM forecast and observations that are combined to produce the analyzed fields. For example, the GCM does not produce a quasi-biennial oscillation (QBO). The QBO is present in the analyzed fields because it is present in the observations, and systematic implicit forcing is required by the DAS. Any systematic bias between observations and the GCM forecast used to produce the DAS analysis is likely to corrupt the transport produced by the analyzed fields. Evaluation of transport in the lower tropical stratosphere in a global chemistry and transport model.
During the NASA Cirrus Regional Study of Tropical Anvils and Cirrus Layers-Florida Area Cirrus Experiment (CRYSTAL-FACE) enhanced mixing ratios of nitric oxide were measured in the anvils of thunderstorms and in clear air downwind of storm systems on flights of a Wl3-57F high-altitude aircraft. Mixing ratios greater than l0 - 20 times background were readily observed over distances of 25-120 km due to lightning activity. In many of the Florida storms deposition of NO occurred up to near the tropopause but major deposition usually occurred 1 - 2 km below the tropopause, or mostly within the visible anvil volume formed prior to storm decay. Observations from two storms of very different anvil size and electrical activity allowed estimates of the total mass of NO, vented to the middle and upper troposphere. Using the cloud-to ground (CG) flash accumulations from the National Lightning Detection Network, climatological intra-cloud (IC) to CG ratios, and assuming that CG and IC flashes were of equivalent efficiency for NO production, the ranges of production per flash for a moderate-sized and a large storm were (0.51 - 1.0) x l0(exp 26) and (2.3 - 3.1) x 10(exp 26) molecules NO/flash, respectively. Using the recently determined average global flash rate of 44 8, a gross extrapolation of these two storms to represent possible global annual production rates yield 1.6 - 3.2 and 7.3 - 9.9 Tg(N)/yr, respectively. If the more usual assumption is made that IC efficiency is l/l0th that of CG activity, the ranges of production for the moderate-sized and large storm were (1.3 - 2.7) x l0(exp 26) and (6.0 - 8.1) x l0(exp 26) molecules NO/CG flash, respectively. The estimates from the large storm may be high because there is indirect evidence that the IC/CG ratio was larger than would be derived from climatology. These two storms and others studied did not have flash rates that scaled as approx. H(sup 5) where H is the cloud top altitude. The observed CG flash accumulations and NO(x) mass production estimate for the month of July over the Florida area were compared with a representative 3D global Chemistry-Transport Model (CTMJ that uses the Price et al. lightning parameterization. For two land grid points representing the Florida peninsula the model compared well with the observations: CG flash rates were low by only a factor of approx. 2. When the model grid points included the coastal regions of Florida the flash accumulations were lower than observed by a factor of 3.4 - 4.6. It is recommended that models using the Price et al. parameterization allow any global coastal grid point to maintain the land rather than the marine flash rate parameterization. The convection in this CTM underestimated the actual cloud top heights over Florida by 1 - 2 km and thus the total lightning flash rates and the altitude range of reactive nitrogen deposition. Broad scale (20 - 120 km) median mixing ratios of NO within anvils over Florida were significantly larger than in storms previously investigated over Colorado and New Mexico.
Our work has two primary scientific goals, the interannual variability (IAV) of stratospheric ozone and the hydrological cycle of the upper troposphere and lower stratosphere. Our efforts are aimed at integrating new information obtained by spacecraft and aircraft measurements to achieve a better understanding of the chemical and dynamical processes that are needed for realistic evaluations of human impact on the global environment. A primary motivation for studying the ozone layer is to separate the anthropogenic perturbations of the ozone layer from natural variability. Using the recently available merged ozone data (MOD), we have carried out an empirical orthogonal function EOF) study of the temporal and spatial patterns of the IAV of total column ozone in the tropics. The outstanding problem about water in the stratosphere is its secular increase in the last few decades. The Caltech/PL multi-dimensional chemical transport model (CTM) photochemical model is used to simulate the processes that control the water vapor and its isotopic composition in the stratosphere. Datasets we will use for comparison with model results include those obtained by the Total Ozone Mapping Spectrometer (TOMS), the Solar Backscatter Ultraviolet (SBUV and SBUV/2), Stratosphere Aerosol and Gas Experiment (SAGE I and II), the Halogen Occultation Experiment (HALOE), the Atmospheric Trace Molecular Spectroscopy (ATMOS) and those soon to be obtained by the Cirrus Regional Study of Tropical Anvils and Cirrus Layers Florida Area Cirrus Experiment (CRYSTAL-FACE) mission. The focus of the investigations is the exchange between the stratosphere and the troposphere, and between the troposphere and the biosphere.
The UC Irvine project for Trace-P (PI: Prather) is a collaboration with Frontier-Japan (Wild and Akimoto) and U. Oslo (Sundet and Isaksen) to make high-resolution global T63 CTM simulations of trace gases and the oxidant budgets for the Trace-P period. Research at FRS and Oslo is not funded by GTE/TRACE-P. Completed control runs for the Trace-P period at T63L40 resolution using the standard emissions with the two related, but independent CTMs at Frontier-UCI and at U. Oslo. Preliminary diagnosis of the impact of Asian emissions on ozone and oxidant budgets is completed. A series of sensitivity runs is beginning to analyze where uncertainty in emissions is related to better simulation of the Trace-P observations.
Net mass flux from the stratosphere to the troposphere can be computed from the heating rate along the 380K isentropic surface and the time rate of change of the mass of the lowermost stratosphere (the region between the tropopause and the 380K isentrope). Given this net mass flux and the cross tropopause diabatic mass flux, the residual adiabatic mass flux across the tropopause can also be estimated. These fluxes have been computed using meteorological fields from a free-running general circulation model (FVGCM) and two assimilation data sets, FVDAS, and UKMO. The data sets tend to agree that the annual average net mass flux for the Northern Hemisphere is about 1P10 kg/s. There is less agreement on the southern Hemisphere flux that might be half as large. For all three data sets, the adiabatic mass flux is computed to be from the upper troposphere into the lowermost stratosphere. This flux will dilute air entering from higher stratospheric altitudes. The mass fluxes are convolved with ozone mixing ratios from the Goddard 3D CTM (which uses the FVGCM) to estimate the cross-tropopause transport of ozone. A relatively large adiabatic flux of tropospheric ozone from the tropical upper troposphere into the extratropical lowermost stratosphere dilutes the stratospheric air in the lowermost stratosphere. Thus, a significant fraction of any measured ozone STE may not be ozone produced in the higher Stratosphere. The results also illustrate that the annual cycle of ozone concentration in the lowermost stratosphere has as much of a role as the transport in the seasonal ozone flux cycle. This implies that a simplified calculation of ozone STE mass from air mass and a mean ozone mixing ratio may have a large uncertainty.
We have produced a profile merged ozone data set (MOD) based on the SBUV/SBUV2 series of nadir-viewing satellite backscatter instruments, covering the period from November 1978 - December 2003. In 2004, data from the Nimbus 7 SBUV and NOAA 9, ll, and 16 SBUV/2 instruments were reprocessed using the Version 8 (V8) algorithm and most recent calibrations. More recently, data from the Nimbus 4 BUT instrument, which was operational from 1970 - 1977, were also reprocessed using the V8 algorithm. As part of the V8 profile calibration, the Nimbus 7 and NOAA 9 (1993-1997 only) instrument calibrations have been adjusted to match the NOAA 11 calibration, which was established based on comparisons with SSBUV shuttle flight data. Differences between NOAA 11, Nimbus 7 and NOAA 9 profile zonal means are within plus or minus 5% at all levels when averaged over the respective periods of data overlap. NOAA 16 SBUV/2 data have insufficient overlap with NOAA 11, so its calibration is based on pre-flight information. Mean differences over 4 months of overlap are within plus or minus 7%. Given the level of agreement between the data sets, we simply average the ozone values during periods of instrument overlap to produce the MOD profile data set. Initial comparisons of coincident matches of N4 BUV and Arosa Umkehr data show mean differences of 0.5 (0.5)% at 30km; 7.5 (0.5)% at 35 km; and 11 (0.7)% at 40 km, where the number in parentheses is the standard error of the mean. In this study, we use the MOD profile data set (1978-2003) to estimate the change in profile ozone due to changing stratospheric chlorine levels. We use a standard linear regression model with proxies for the seasonal cycle, solar cycle, QBO, and ozone trend. To account for the non-linearity of stratospheric chlorine levels since the late 1990s, we use a time series of Effective Chlorine, defined as the global average of Chlorine + 50 * Bromine at 1 hPa, as the trend proxy. The Effective Chlorine data are taken from the 3-D Goddard CTM. We will show the latest trend results using this statistical model. In addition, the Nimbus 4 BUV data offer an opportunity to test the physical properties of our statistical model. From ground-based comparisons we will establish an uncertainty range for the Nimbus 4 data. We then extrapolate our statistical model fit backwards in time and compare to the Nimbus 4 data. We compare the characteristics of the residual, defined as the difference between the data and statistical regression fit, during the Nimbus 4 time period and the 1978-2003 period over which the statistical model coefficients were estimated, and present these results.
We have developed a technique to diagnose the stratospheric age spectrum and estimate the mean age of air using the distributions of at least four constituents with different photochemical lifetimes. We demonstrate that the technique works using a 3D CTM and then apply the technique to UMS CLAES January 1993 observations of CFC11, CFC12, CH4 and N2O. Our results are generally in agreement with mean age of air estimates from the chemical model and from observations of SF6 and CO2; however, the mean age estimates show an intrusion of very young tropical air into the mid-latitude stratosphere. This feature is consistent with mixing of high N20 air out of the tropics during the westerly phase of the QBO.
Global aerosol mass and optical thickness (AOT) simulated by two aerosol models (GOCART and GMI-UMich) are evaluated and the strengths and shortcomings of the model approaches are investigated. These two offline CTM models are driven by the same meteorological fields (NASA GEOS-4), use the same dynamic transport algorithm, and have the same spatial resolution. However, they differ partially in emission, dry/wet deposition, and chemistry. The simulated aerosol masses are evaluated by the surface long-term measurements and short-term field campaigns (ACE-Asia and TRACE-P). AOT are calculated using modeled aerosol mass but externally mixed for GOCART and partially internally mixed for GMI-Mich. These AOT are evaluated using satellite observations from MODIS and MISR and ground measurements from AERONET. Our work demonstrates that there are significant differences in simulated aerosol mass and AOT by the two approaches. Further investigation will be performed to evaluate each mechanism which induces the differences quantitatively by implementing GOCART-like emission, deposition, and chemistry into GMI framework.
Long-term changes in greenhouse gases, primarily carbon dioxide, are expected to lead to a warming of the troposphere and a cooling of the stratosphere. We examine the cooling of the stratosphere and compare the contributions greenhouse gases and ozone change for the decades between 1980 and 2000. We use 150 years of simulation done with our coupled chemistry/climate model (GEOS 4 GCM with GSFC CTM chemistry) to calculate temperatures and constituents fiom,1950 through 2100. The contributions of greenhouse gases and ozone to temperature change are separated by a time-series analysis using a linear trend term throughout the period to represent the effects of greenhouse gases and an equivalent effective stratospheric chlorine (EESC) term to represent the effects of ozone change. The temperature changes over the 150 years of the simulation are dominated by the changes in greenhouse gases. Over the relatively short period (approx. 20 years) of ozone decline between 1980 and 2000 changes in ozone are competitive with changes in greenhouse gases. The changes in temperature induced by the ozone change are comparable to, but smaller than, those of greenhouse gases in the upper stratosphere (1-3 hPa) at mid latitudes. The ozone term dominates the temperature change near both poles with a negative temperature change below about 3-5 hPa and a positive change above. At mid latitudes in the upper stratosphere and mesosphere (above about 1 hPa) and in the middle stratosphere (3 to 70 ma), the greenhouse has term dominates. From about 70 hPa down to the tropopause at mid latitudes, cooling due to ozone changes is the largest influence on temperature. Over the 150 years of the simulation, the change in greenhouse gases is the most important contributor to temperature change. Ozone caused a perturbation that is expected to reverse over the coming decades. We show a model simulation of the expected temperature change over the next two decades (2006-2026). The simulation shows a crossover between lower atmospheric heating and upper atmospheric cooling that is located at about 90 hPa in the tropics and 30-40 hPa in the polar regions. This results from the combination of continuing increases in greehouse gases and recovery from ozone depletion.
We have used a three-dimensional chemistry and transport model (CTM), developed under the Global Modeling Initiative (GMI), to carry out two simulations of the composition of the stratosphere under changing halogen loading for 1995 through 2030. The two simulations differ only in that one uses meteorological fields from a general circulation model while the other uses meteorological fields from a data assimilation system. A single year's winds and temperatures are repeated for each 36-year simulation. We compare results from these two simulations with an extensive collection of data from satellite and ground-based measurements for 1993-2000. Comparisons of simulated fields with observations of radical and reservoir species for some of the major ozone-destroying compounds are of similar quality for both simulations. Differences in the upper stratosphere, caused by transport of total reactive nitrogen and methane, impact the balance among the ozone loss processes and the sensitivity of the two simulations to the change in composition.
Two approximations to convective transport have been implemented in an offline chemistry transport model (CTM) to explore the impact on calculated atmospheric CO2 distributions. GlobalCO2 in the year 2000 is simulated using theCTM driven by assimilated meteorological fields from the NASA s Goddard Earth Observation System Data Assimilation System, Version 4 (GEOS-4). The model simulates atmospheric CO2 by adopting the same CO2 emission inventory and dynamical modules as described in Kawa et al. (convective transport scheme denoted as Conv1). Conv1 approximates the convective transport by using the bulk convective mass fluxes to redistribute trace gases. The alternate approximation, Conv2, partitions fluxes into updraft and downdraft, as well as into entrainment and detrainment, and has potential to yield a more realistic simulation of vertical redistribution through deep convection. Replacing Conv1 by Conv2 results in an overestimate of CO2 over biospheric sink regions. The largest discrepancies result in a CO2 difference of about 7.8 ppm in the July NH boreal forest, which is about 30% of the CO2 seasonality for that area. These differences are compared to those produced by emission scenario variations constrained by the framework of Intergovernmental Panel on Climate Change (IPCC) to account for possible land use change and residual terrestrial CO2 sink. It is shown that the overestimated CO2 driven by Conv2 can be offset by introducing these supplemental emissions.