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Chipperfield, M. P.

Publications and source records attributed to Chipperfield, M. P..

13 records
All sourcesNASA NTRSDOE OSTI
NASA NTRS2014

Resolving the Strange Behavior of Extraterrestrial Potassium in the Upper Atmosphere

It has been known since the 1960s that the layers of Na and K atoms, which occur between 80 and 105km in the Earth's atmosphere as a result of meteoric ablation, exhibit completely different seasonal behavior. In the extratropics Na varies annually, with a pronounced wintertime maximum and summertime minimum. However, K varies semiannually with a small summertime maximum and minima at the equinoxes. This contrasting behavior has never been satisfactorily explained. Here we use a combination of electronic structure and chemical kinetic rate theory to determine two key differences in the chemistries of K and Na. First, the neutralization of K+ ions is only favored at low temperatures during summer. Second, cycling between K and its major neutral reservoir KHCO3 is essentially temperature independent. A whole atmosphere model incorporating this new chemistry, together with a meteor input function, now correctly predicts the seasonal behavior of the K layer.

Earth atmosphere↗
NASA NTRS2014

Multimodel Estimates of Atmospheric Lifetimes of Long-lived Ozone-Depleting Substances: Present and Future

We have diagnosed the lifetimes of long-lived source gases emitted at the surface and removed in the stratosphere using six three-dimensional chemistry-climate models and a two-dimensional model. The models all used the same standard photochemical data. We investigate the effect of different definitions of lifetimes, including running the models with both mixing ratio (MBC) and flux (FBC) boundary conditions. Within the same model, the lifetimes diagnosed by different methods agree very well. Using FBCs versus MBCs leads to a different tracer burden as the implied lifetime contained in the MBC value does not necessarily match a model's own calculated lifetime. In general, there are much larger differences in the lifetimes calculated by different models, the main causes of which are variations in the modeled rates of ascent and horizontal mixing in the tropical midlower stratosphere. The model runs have been used to compute instantaneous and steady state lifetimes. For chlorofluorocarbons (CFCs) their atmospheric distribution was far from steady state in their growth phase through to the 1980s, and the diagnosed instantaneous lifetime is accordingly much longer. Following the cessation of emissions, the resulting decay of CFCs is much closer to steady state. For 2100 conditions the model circulation speeds generally increase, but a thicker ozone layer due to recovery and climate change reduces photolysis rates. These effects compensate so the net impact on modeled lifetimes is small. For future assessments of stratospheric ozone, use of FBCs would allow a consistent balance between rate of CFC removal and model circulation rate

CFC↗
NASA NTRS2014

Multimodel Estimates of Atmospheric Lifetimes of Long-Lived Ozone-Depleting Substances: Present and Future

We have diagnosed the lifetimes of long-lived source gases emitted at the surface and removed in the stratosphere using six three-dimensional chemistry-climate models and a two-dimensional model. The models all used the same standard photochemical data. We investigate the effect of different definitions of lifetimes, including running the models with both mixing ratio (MBC) and flux (FBC) boundary conditions. Within the same model, the lifetimes diagnosed by different methods agree very well. Using FBCs versus MBCs leads to a different tracer burden as the implied lifetime contained in theMBC value does not necessarilymatch a model's own calculated lifetime. In general, there are much larger differences in the lifetimes calculated by different models, the main causes of which are variations in the modeled rates of ascent and horizontal mixing in the tropical midlower stratosphere. The model runs have been used to compute instantaneous and steady state lifetimes. For chlorofluorocarbons (CFCs) their atmospheric distribution was far from steady state in their growth phase through to the 1980s, and the diagnosed instantaneous lifetime is accordingly much longer. Following the cessation of emissions, the resulting decay of CFCs is much closer to steady state. For 2100 conditions the model circulation speeds generally increase, but a thicker ozone layer due to recovery and climate change reduces photolysis rates. These effects compensate so the net impact on modeled lifetimes is small. For future assessments of stratospheric ozone, use of FBCs would allow a consistent balance between rate of CFC removal and model circulation rate.

CH3CCl3↗
NASA NTRS2013

Evaluating Global Emission Inventories of Biogenic Bromocarbons

Emissions of halogenated very short-lived substances (VSLS) are poorly constrained. However, their inclusion in global models is required to simulate a realistic inorganic bromine (Bry) loading in both the troposphere, where bromine chemistry perturbs global oxidizing capacity, and in the stratosphere, where it is a major sink for ozone (O3). We have performed simulations using a 3-D chemical transport model (CTM) including three top-down and a single bottom-up derived emission inventory of the major brominated VSLS bromoform (CHBr3) and dibromomethane (CH2Br2). We perform the first concerted evaluation of these inventories, comparing both the magnitude and spatial distribution of emissions. For a quantitative evaluation of each inventory, model output is compared with independent long-term observations at National Oceanic and Atmospheric Administration (NOAA) ground-based stations and with aircraft observations made during the NSF (National Science Foundation) HIAPER Pole-to-Pole Observations (HIPPO) project. For CHBr3, the mean absolute deviation between model and surface observation ranges from 0.22 (38 %) to 0.78 (115 %) parts per trillion (ppt) in the tropics, depending on emission inventory. For CH2Br2, the range is 0.17 (24 %) to 1.25 (167 %) ppt. We also use aircraft observations made during the 2011 Stratospheric Ozone: Halogen Impacts in a Varying Atmosphere (SHIVA) campaign, in the tropical western Pacific. Here, the performance of the various inventories also varies significantly, but overall the CTM is able to reproduce observed CHBr3 well in the free troposphere using an inventory based on observed sea-to-air fluxes. Finally, we identify the range of uncertainty associated with these VSLS emission inventories on stratospheric bromine loading due to VSLS (Br(VSLS/y)). Our simulations show Br(VSLS/y) ranges from approximately 4.0 to 8.0 ppt depending on the inventory. We report an optimized estimate at the lower end of this range (approximately 4 ppt) based on combining the CHBr3 and CH2Br2 inventories which give best agreement with the compilation of observations in the tropics.

bromocarbons↗
NASA NTRS2010

Multimodel Assessment of the Factors Driving Stratospheric Ozone Evolution over the 21st Century

The evolution of stratospheric ozone from 1960 to 2100 is examined in simulations from 14 chemistry-climate models, driven by prescribed levels of halogens and greenhouse gases. There is general agreement among the models that total column ozone reached a minimum around year 2000 at all latitudes, projected to be followed by an increase over the first half of the 21st century. In the second half of the 21st century, ozone is projected to continue increasing, level off, or even decrease depending on the latitude. Separation into partial columns above and below 20 hPa reveals that these latitudinal differences are almost completely caused by differences in the model projections of ozone in the lower stratosphere. At all latitudes, upper stratospheric ozone increases throughout the 21st century and is projected to return to 1960 levels well before the end of the century, although there is a spread among models in the dates that ozone returns to specific historical values. We find decreasing halogens and declining upper atmospheric temperatures, driven by increasing greenhouse gases, contribute almost equally to increases in upper stratospheric ozone. In the tropical lower stratosphere, an increase in upwelling causes a steady decrease in ozone through the 21st century, and total column ozone does not return to 1960 levels in most of the models. In contrast, lower stratospheric and total column ozone in middle and high latitudes increases during the 21st century, returning to 1960 levels well before the end of the century in most models.

Oman, L. D.↗
NASA NTRS2010

Quantifying Uncertainty in Projections of Stratospheric Ozone Over the 21st Century

Future stratospheric ozone concentrations will be determined both by changes in the concentration of ozone depleting substances (ODSs) and by changes in stratospheric and tropospheric climate, including those caused by changes in anthropogenic greenhouse gases (GHGs). Since future economic development pathways and resultant emissions of GHGs are uncertain, anthropogenic climate change could be a significant source of uncertainty for future projections of stratospheric ozone. In this pilot study, using an ensemble of opportunity of chemistry-climate model (CCM) simulations, the contribution of scenario uncertainty from different plausible emissions pathways for 10 ODSs and GHGs to future ozone projections is quantified relative to the contribution from model uncertainty and internal variability of the chemistry-climate system. For both the global, annual mean ozone concentration and for ozone in specific geographical regions, differences between CCMs are the dominant source of uncertainty for the first two-thirds of the 21 st century, up-to and after the time when ozone concentrations 15 return to 1980 values. In the last third of the 21st century, dependent upon the set of greenhouse gas scenarios used, scenario uncertainty can be the dominant contributor. This result suggests that investment in chemistry-climate modelling is likely to continue to refine projections of stratospheric ozone and estimates of the return of stratospheric ozone concentrations to pre-1980 levels.

Charlton-Perez, A. J.↗
NASA NTRS2010

Multi-Model Assessment of the Factors Driving Stratospheric Ozone Evolution Over the 21st Century

The evolution of stratospheric ozone from 1960 to 2100 is examined in simulations from fourteen chemistry-climate models. There is general agreement among the models at the broadest levels, showing column ozone decreasing at all latitudes from 1960 to around 2000, then increasing at all latitudes over the first half of the 21st century, and latitudinal variations in the rate of increase and date of return to historical values. In the second half of the century, ozone is projected to continue increasing, level off or even decrease depending on the latitude, resulting in variable dates of return to historical values at latitudes where column ozone has declined below those levels. Separation into partial column above and below 20 hPa reveals that these latitudinal differences are almost completely due to differences in the lower stratosphere. At all latitudes, upper stratospheric ozone increases throughout the 21st century and returns to 1960 levels before the end of the century, although there is a spread among the models in dates that ozone returns to historical values. Using multiple linear regression, we find decreasing halogens and increasing greenhouse gases contribute almost equally to increases in the upper stratospheric ozone. In the tropical lower stratosphere an increase in tropical upwelling causes a steady decrease in ozone through the 21st century, and total column ozone does not return to 1960 levels in all models. In contrast, lower stratospheric and total column ozone in middle and high latitudes increases during the 21st century and returns to 1960 levels.

Oman, L. D.↗
NASA NTRS2010

Using Transport Diagnostics to Understand Chemistry Climate Model Ozone Simulations

We demonstrate how observations of N2O and mean age in the tropical and midlatitude lower stratosphere (LS) can be used to identify realistic transport in models. The results are applied to 15 Chemistry Climate Models (CCMs) participating in the 2010 WMO assessment. Comparison of the observed and simulated N2O/mean age relationship identifies models with fast or slow circulations and reveals details of model ascent and tropical isolation. The use of this process-oriented N2O/mean age diagnostic identifies models with compensating transport deficiencies that produce fortuitous agreement with mean age. We compare the diagnosed model transport behavior with a model's ability to produce realistic LS O3 profiles in the tropics and midlatitudes. Models with the greatest tropical transport problems show the poorest agreement with observations. Models with the most realistic LS transport agree more closely with LS observations and each other. We incorporate the results of the chemistry evaluations in the SPARC CCMVal Report (2010) to explain the range of CCM predictions for the return-to-1980 dates for global (60 S-60 N) and Antarctic column ozone. Later (earlier) Antarctic return dates are generally correlated to higher (lower) vortex Cl(sub y) levels in the LS, and vortex Cl(sub y) is generally correlated with the model's circulation although model Cl(sub y) chemistry or Cl(sub y) conservation can have a significant effect. In both regions, models that have good LS transport produce a smaller range of predictions for the return-to-1980 ozone values. This study suggests that the current range of predicted return dates is unnecessarily large due to identifiable model transport deficiencies.

Strahan, S. E.↗
NASA NTRS2002

Particle Events as a Possible Source of Large Ozone Loss during Magnetic Polarity Transitions

The energy deposition in the mesosphere and stratosphere during large extraterrestrial charged particle precipitation events has been known for some time to contribute to ozone losses due to the formation of potential ozone destroying species like NO(sub x), and HO(sub x). These impacts have been measured and can be reproduced with chemistry models fairly well. In the recent past, however, even the impact of the largest solar proton events on the total amount of ozone has been small compared to the dynamical variability of ozone, and to the anthropogenic induced impacts like the Antarctic 'ozone hole'. This is due to the shielding effect of the magnetic field. However, there is evidence that the earth's magnetic field may approach a reversal. This could lead to a decrease of magnetic field strength to less than 25% of its usual value over a period of several centuries . We show that with realistic estimates of very large solar proton events, scenarios similar to the Antarctic ozone hole of the 1990s may occur during a magnetic polarity transition.

vonKoenig, M.↗
NASA NTRS1996

Chlorine Deactivation in the Lower Stratospheric Polar Regions during late Winter: Results from UARS

Recovery from enhanced chlorine conditions in the lower stratospheric polar regions of both hemispheres is investigated using data from the Upper Atmosphere Research Satellite (UARS). Microwave Limb Sounder (MLS) measurements of ClO within the polar vortices are used to infer ClO(sub x) (ClO + 2Cl202) abundances that are then correlated with simultaneous Cryogenic Limb Array Etalon Spectrometer (CLAES) measurements of ClON02 and Halogen Occultation Experiment (HALOE) measurements of HCl obtained starting within 5 days of the end of the MLS and CLAES high-latitude observing periods in each hemisphere. Time series of vortex-averaged mixing ratios are calculated on two potential temperature surfaces (585 K and 465 K) in the lower stratosphere for approximately month-long intervals during late winter: August 17 - September 17, 1992, in the southern hemisphere and February 12 - March 16, 1993, in the northern hemisphere. The observed mixing ratios are adjusted for the effects of vertical transport using diabatic vertical velocities estimated from CLAES tracer data. In the northern hemisphere, the decrease in ClO, is balanced on both surfaces by an increase in ClON02- In the southern hemisphere, continuing polar stratospheric cloud activity prevents ClO from undergoing sustained decline until about September 3. In contrast to the northern hemisphere, there is no significant chemical change in vortex-averaged ClON02 at 465 K, and there is an apparent decrease in ClON02 at 585 K, even after the enhanced ClO abundances have started to recede. Results from the SLIMCAT chemical transport model initialized with UARS data and run with OH + ClO yields HCl + 02 as an 8% channel suggest that the primary recovery product in the south during this time period is not ClON02, but HCl. HALOE HCl mixing ratios are extrapolated back to the time of the MLS and CLAES data. At 585 K, the chlorine budget can be made to balance by extrapolating HCl back to a value of 0.6 parts per billion by volume (ppbv) at the beginning of the study period; at 465 K, the contribution from extrapolated HCl is not sufficient to offset the loss in ClOx, and there is a slight imbalance between the decrease in reactive chlorine and the change in chlorine reservoirs. The difficulty in closing the chlorine budget in the southern hemisphere may arise from complications caused by ongoing activation, incomplete photochemical assumptions, and/or inadequate data quality.

Santee, M. L.↗
NASA NTRS1994

A two-dimensional model study of the QBO signal in SAGE II NO2 and O3

Calculations of the quasi biennial oscillation (QBO) signal in Stratospheric Aerosol and Gas Experiment (SAGE) II O3 and NO2 data between 1984 and 1991 are presented and have been investigated by using a two-dimensional model. The isentropic 2D model is a fully interactive radiative-dynamical-chemical model in which the eddy fluxes of chemical species are calculated in a consistent manner. The QBO in the model has been forced by relaxing the equatorial zonal wind toward the observations at Singapore allowing the comparison of the model with observations from specific years. The model reproduces the observed vertical structure of the equatorial ozone anomaly with the well-known transition from dynamical to photochemical control at around 28km. The model also reproduces the observed vertical structure of the SAGE II observed NO2 anomaly. The model studies have shown that it is the QBO modulation of NO2 which the main cause of QBO signal in O3 above 30 km. The model also reproduces the observed latitudinal structure of the QBO signals in O3 and NO2. Due to the differing horizontal distribution of O3 and NO(y) the ozone signal shows a distinct phase change in the subtropics whereas the NO2 anomaly gives a broader signal.

Chipperfield, M. P.↗
NASA NTRS1988

Modelling the Antarctic lower stratosphere

Results form modeling studies of the Antarctic lower stratosphere which have attempted to simulate the large springtime ozone losses and corresponding changes in other trace constituents are given. These studies were carried out in a photochemical box model, a one-dimensional model without transport and in a two-dimensional photochemical-dynamical-radiation model. The photochemical studies have investigated inter alia the sensitivity of ozone to inclusion in the model of heterogeneous chemistry, and to the inclusion of the ClO dimer. When both of these are incorporated in the model, ozone depletions resembling whose found in Halley Bay in 1987 (J.C. Farman, Nature, 329, 1987) can be reproduced. The temporal variations (both diurnal and during the August to October period) of a number of important tracers including HCl, ClONO2, OClO and BrO are discussed. The two-dimensional study concentrated on the difficulty of establishing in the model the dynamical preconditioning of the lower polar stratosphere - low temperatures, low N2O, etc., high ClOx. Calculations are presented to show: (1) the depletion of ozone during the springtime season, (2) the effect of large ozone losses on lower latitudes, and (3) the longer term (multi-year) variations of ozone in Antarctica, assuming realistic increases in the atmospheric halogen burden.

Chipperfield, M. P.↗