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NASA NTRS2005

Chemical Loss of Polar Ozone: Present Understanding and Remaining Uncertainties

Not long after the discovery of the Antarctic ozone hole, it was established that halogen compounds, supplied to the atmosphere mainly by anthropogenic activities, are the primary driver of polar ozone loss. We will briefly review the chemical mechanisms that cause polar ozone loss and the early evidence showing the key role played by anthropogenic halogens. Recently, stratospheric halogen loading has leveled off, due to adherence to the Montreal Protocol and its amendments that has essentially banned CFCs (chlorofluorocarbons) and other halocarbons. We will describe recent reports of the first stage of recovery of the Antarctic ozone hole (e.g., a statistically significant slowing of the downward trend), associated with the leveling off of stratospheric halogens. Despite this degree of understanding, we will discuss the tendency of photochemical models to underestimate the observed rate of polar ozone loss and a hypothesis that has recently been put forth that might resolve this discrepancy. Finally, we will briefly discuss chemical loss of Arctic ozone, which

climate change↗
NASA NTRS2011

Satellite Observations and Chemistry Climate Models - A Meandering Path Towards Better Predictions

Knowledge of the chemical and dynamical processes that control the stratospheric ozone layer has grown rapidly since the 1970s, when ideas that depletion of the ozone layer due to human activity were put forth. The concept of ozone depletion due to anthropogenic chlorine increase is simple; quantification of the effect is much more difficult. The future of stratospheric ozone is complicated because ozone is expected to increase for two reasons: the slow decrease in anthropogenic chlorine due to the Montreal Protocol and its amendments and stratospheric cooling caused by increases in carbon dioxide and other greenhouse gases. Prediction of future ozone levels requires three-dimensional models that represent physical, photochemical and radiative processes, i.e., chemistry climate models (CCMs). While laboratory kinetic and photochemical data are necessary inputs for a CCM, atmospheric measurements are needed both to reveal physical and chemical processes and for comparison with simulations to test the conceptual model that CCMs represent. Global measurements are available from various satellites including but not limited to the LIMS and TOMS instruments on Nimbus 7 (1979 - 1993), and various instruments on the Upper Atmosphere Research Satellite (1991 - 2005), Envisat (2002 - ongoing), Sci-Sat (2003 - ongoing) and Aura (2004 - ongoing). Every successful satellite instrument requires a physical concept for the measurement, knowledge of physical chemical properties of the molecules to be measured, and stellar engineering to design an instrument that will survive launch and operate for years with no opportunity for repair but providing enough information that trend information can be separated from any instrument change. The on-going challenge is to use observations to decrease uncertainty in prediction. This talk will focus on two applications. The first considers transport diagnostics and implications for prediction of the eventual demise of the Antarctic ozone hole. The second focuses on the upper stratosphere, where ozone is predicted to increase both due to chlorine decrease and due to temperature decrease expected as a result of increased concentrations Of CO2 and other greenhouse gases. Both applications show how diagnostics developed from global observations are being used to explain why the ozone response varies among CCM predictions for stratospheric ozone in the 21st century.

Douglass, Anne R.↗
NASA NTRS2010

The Unique OMI HCHO/NO2 Feature During the 2008 Beijing Summer Olympics: Implications for Ozone Production Sensitivity

In preparation of the Beijing Summer Olympic and Paralympics Games, strict controls were imposed between July and September 2008 on motor vehicle traffic and industrial emissions to improve air quality for the competitors. We assessed chemical sensitivity of ozone production to these controls using Ozone Monitoring Instrument (OMI) column measurements of formaldehyde (HCHO) and nitrogen dioxide (NO2), where their ratio serves as a proxy for the sensitivity. During the emission controls, HCHO/NO2 increased and indicated a NOx-limited regime, in contrast to the same period in the preceding three years when the ratio indicates volatile organic carbon (VOC)-limited and mixed NOx-VOC-limited regimes. After the emission controls were lifted, observed NO2 and HCHO/NO2 returned to their previous values. The 2005-2008 OMI record shows that this transition in regimes was unique as ozone production in Beijing was rarely NOx-limited. OMI measured summertime increases in HCHO of around 13% in 2008 compared to prior years, the same time period during which MODIS vegetation indices increased. The OMI HCHO increase may be due to higher biogenic emissions of HCHO precursors, associated with Beijing's greening initiative for the Olympics. However, NO2 and HCHO were also found to be well-correlated during the summer months. This indicates an anthropogenic VOC contribution from vehicle emissions to OMI HCHO and is a plausible explanation for the relative HCHO minimum observed in August 2008, concurrent with a minimum in traffic emissions. We calculated positive trends in 2005-2008 OMI HCHO and NO2 of about +1 x 10(exp 14) Molec/ square M-2 and +3 x 10(exp 13) molec CM-2 per month, respectively. The positive trend in NO2 may be an indicator of increasing vehicular traffic since 2005, while the positive trend in HCHO may be due to a combined increase in anthropogenic and biogenic emissions since 2005.

Witte, J. C.↗
NASA NTRS2011

SO2 Emissions and Lifetimes: Estimates from Inverse Modeling Using In Situ and Global, Space-Based (SCIAMACHY and OMI) Observations

Top-down constraints on global sulfur dioxide (SO2) emissions are inferred through inverse modeling using SO2 column observations from two satellite instruments (SCIAMACHY and OMI). We first evaluated the S02 column observations with surface SO2 measurements by applying local scaling factors from a global chemical transport model (GEOS-Chem) to SO2 columns retrieved from the satellite instruments. The resulting annual mean surface SO2 mixing ratios for 2006 exhibit a significant spatial correlation (r=0.86, slope=0.91 for SCIAMACHY and r=0.80, slope = 0.79 for OMI) with coincident in situ measurements from monitoring networks throughout the United States and Canada. We evaluate the GEOS-Chem simulation of the SO2 lifetime with that inferred from in situ measurements to verity the applicability of GEOS-Chem for inversion of SO2 columns to emissions. The seasonal mean SO2 lifetime calculated with the GEOS-Chem model over the eastern United States is 13 h in summer and 48 h in winter, compared to lifetimes inferred from in situ measurements of 19 +/- 7 h in summer and 58 +/- 20 h in winter. We apply SO2 columns from SCIAMACHY and OMI to derive a top-down anthropogenic SO2 emission inventory over land by using the local GEOS-Chem relationship between SO2 columns and emissions. There is little seasonal variation in the top-down emissions (<15%) over most major industrial regions providing some confidence in the method. Our global estimate for annual land surface anthropogenic SO2 emissions (52.4 Tg S/yr from SCIAMACHY and 49.9 Tg S / yr from OMI) closely agrees with the bottom-up emissions (54.6 Tg S/yr) in the GEOS-Chem model and exhibits consistency in global distributions with the bottom-up emissions (r = 0.78 for SCIAMACHY, and r = 0.77 for OMI). However, there are significant regional differences.

Lee, Chulkyu↗
NASA NTRS2011

Lessons Learned from OMI Observations of Point Source SO2 Pollution

The Ozone Monitoring Instrument (OMI) on NASA Aura satellite makes global daily measurements of the total column of sulfur dioxide (SO2), a short-lived trace gas produced by fossil fuel combustion, smelting, and volcanoes. Although anthropogenic SO2 signals may not be detectable in a single OMI pixel, it is possible to see the source and determine its exact location by averaging a large number of individual measurements. We describe new techniques for spatial and temporal averaging that have been applied to the OMI SO2 data to determine the spatial distributions or "fingerprints" of SO2 burdens from top 100 pollution sources in North America. The technique requires averaging of several years of OMI daily measurements to observe SO2 pollution from typical anthropogenic sources. We found that the largest point sources of SO2 in the U.S. produce elevated SO2 values over a relatively small area - within 20-30 km radius. Therefore, one needs higher than OMI spatial resolution to monitor typical SO2 sources. TROPOMI instrument on the ESA Sentinel 5 precursor mission will have improved ground resolution (approximately 7 km at nadir), but is limited to once a day measurement. A pointable geostationary UVB spectrometer with variable spatial resolution and flexible sampling frequency could potentially achieve the goal of daily monitoring of SO2 point sources and resolve downwind plumes. This concept of taking the measurements at high frequency to enhance weak signals needs to be demonstrated with a GEOCAPE precursor mission before 2020, which will help formulating GEOCAPE measurement requirements.

Krotkov, N.↗
NASA NTRS2011

Recent Rates of Forest Harvest and Conversion in North America

Incorporating ecological disturbance into biogeochemical models is critical for estimating current and future carbon stocks and fluxes. In particular, anthropogenic disturbances, such as forest conversion and wood harvest, strongly affect forest carbon dynamics within North America. This paper summarizes recent (2000.2008) rates of extraction, including both conversion and harvest, derived from national forest inventories for North America (the United States, Canada, and Mexico). During the 2000s, 6.1 million ha/yr were affected by harvest, another 1.0 million ha/yr were converted to other land uses through gross deforestation, and 0.4 million ha/yr were degraded. Thus about 1.0% of North America fs forests experienced some form of anthropogenic disturbance each year. However, due to harvest recovery, afforestation, and reforestation, the total forest area on the continent has been roughly stable during the decade. On average, about 110 m3 of roundwood volume was extracted per hectare harvested across the continent. Patterns of extraction vary among the three countries, with U.S. and Canadian activity dominated by partial and clear ]cut harvest, respectively, and activity in Mexico dominated by conversion (deforestation) for agriculture. Temporal trends in harvest and clearing may be affected by economic variables, technology, and forest policy decisions. While overall rates of extraction appear fairly stable in all three countries since the 1980s, harvest within the United States has shifted toward the southern United States and away from the Pacific Northwest.

Masek, Jeffrey G.↗
NASA NTRS2011

Biogeochemical Impact of Long-Range Transported Dust over Northern South China Sea

Transpacific transport and impact of Asian dust aerosols have been well documented (e.g., results from ACE-Asia and regional follow-on campaigns), but little is known about dust invasion to the South China Sea (SCS). On 19-21 March 2010, a fierce Asian dust storm affected large areas from the Gobi deserts to the West Pacific, including Taiwan and Hong Kong. As a pilot study of the 7-SEAS (Seven South East Asian Studies) in the northern SCS, detailed characteristics of long-range transported dust aerosols were first observed by a comprehensive set of ground-based instruments deployed at the Dongsha islands (20deg42'52" N, 116deg43'51" E). Aerosol measurements such as particle mass concentrations, size distribution, optical properties, hygroscopicity, and vertical profiles help illustrate the evolution of this dust outbreak. Our results indicate that these dust particles were mixed with anthropogenic and marine aerosols, and transported near the surface. Satellite assessment of biogeochemical impact of dust deposition into open oceans is hindered by our current inability in retrieving areal dust properties and ocean colors over an extensive period of time, particularly under the influence of cloudy conditions. In this paper, we analyze the changes of retrieved Chlorophyll-a (Chl-a) concentration over the northern SCS, considered as oligotophic waters in the spring, from long-term SeaWiFS measurements since 1997. Over the past decade, six long-range transported dust events are identified based on spatiotemporal evolutions of PM10 measurements from regional monitoring stations, with the aid of trajectory analysis. Multi-year composites of Chl-a imagery for dust event and non-dust background during March-April are applied to overcome insufficient retrievals of Chl-a due to cloudy environment. Due to anthropogenic modification within a shallow boundary layer off the densely populated and industrial southeast coast of China, the iron ion activation of deliquescent dust particles enhances the efficiency of fertilization for biological productivity. Compared to the West Pacific, the marine ecosystem in the northern SCS is much more susceptible to the biogeochemical impact of long-range transported Asian dust.

Tsay, Si-Chee↗
NASA NTRS2011

Global Distributions of Mineral Dust Properties from SeaWiFS and MODIS: From Sources to Sinks

The impact of natural and anthropogenic sources of mineral dust has gained increasing attention from scientific communities in recent years. Indeed, these airborne dust particles, once lifted over the source regions, can be transported out of the boundary layer into the free troposphere and can travel thousands of kilometers across the oceans resulting in important biogeochemical impacts on the ecosystem. Due to the relatively short lifetime (a few hours to about a week), the distributions of these mineral dust particles vary extensively in both space and time. Consequently, satellite observations are needed over both source and sink regions for continuous temporal and spatial sampling of aerosol properties. With the launch of SeaWiFS in 1997, Terra/MODIS in 1999, and Aqua/MODIS in 2002, high quality comprehensive aerosol climatology is becoming feasible for the first time. As a result of these unprecedented satellite data records, studies of the radiative and biogeochemical effects due to dust aerosols are now possible. In this study, we will show the comparisons of satellite retrieved aerosol optical thickness using Deep Blue algorithm with data from AERONET sunphotometers over desert and semi-desert regions as well as vegetated areas. Our results indicate reasonable agreements between these two. These new satellite products will allow scientists to determine quantitatively the aerosol properties near sources using high spatial resolution measurements from Sea WiFS and MODIS-like instruments. The multiyear satellite measurements since 1997 from Sea WiFS will be compared with those retrieved from MODIS and MISR, and will be utilized to investigate the interannual variability of source, pathway, and dust loading associated with the dust outbreaks over the entire globe. Finally, the trends observed over the last decade based upon the SeaWiFS time series in the amounts of tropospheric aerosols due to natural and anthropogenic sources (such as changes in the frequency of dust storms) will be discussed.

Hsu, N. Christina↗
NASA NTRS2011

East Asian Studies of Tropospheric Aerosols and their Impact on Regional Climate (EAST -AIRC): An overview

As the most populated region of the world, Asia is a major source of aerosols with potential large impact over vast downstream areas, Papers published in this special section describe the variety of aerosols observed in China and their effects and interactions with the regional climate as part of the East Asian Study of Tropospheric Aerosols and their Impact on Regional Climate (EAST-AIRC), The majority of the papers are based on analyses of observations made under three field projects, namely, the Atmospheric Radiation Measurements (ARM) Mobile Facility mission in China (AMF-China), the East Asian Study of Tropospheric Aerosols: An International Regional Experiment (EAST-AIRE), and the Atmospheric Aerosols of China and their Climate Effects (AACCE), The former two are U,S,-China collaborative projects, and the latter is a part of the China's National Basic Research program (or often referred to as "973 project"), Routine meteorological data of China are also employed in some studies, The wealth of general and speCIalized measurements lead to extensive and close-up investigations of the optical, physical, and chemical properties of anthropogenic, natural, and mixed aerosols; their sources, formation, and transport mechanisms; horizontal, vertical, and temporal variations; direct and indirect effects; and interactions with the East Asian monsoon system, Particular efforts are made to advance our understanding of the mixing and interaction between dust and anthropogenic pollutants during transport. Several modeling studies were carried out to simulate aerosol impact on radiation budget, temperature, precipitation, wind and atmospheric circulation, fog, etc, In addition, impacts of the Asian monsoon system on aerosol loading are also simulated.

Zhangqing, Li↗
NASA NTRS2012

The Geostationary Fourier Transform Spectrometer

The Geostationary Fourier Transform Spectrometer (GeoFTS) is an imaging spectrometer designed for a geostationary orbit (GEO) earth science mission to measure key atmospheric trace gases and process tracers related to climate change and human activity. GEO allows GeoFTS to continuously stare at a region of the earth for frequent sampling to capture the variability of biogenic fluxes and anthropogenic emissions from city to continental spatial scales and temporal scales from diurnal, synoptic, seasonal to interannual. The measurement strategy provides a process based understanding of the carbon cycle from contiguous maps of carbon dioxide (CO2), methane (CH4), carbon monoxide (CO), and chlorophyll fluorescence (CF) collected many times per day at high spatial resolution (~2.7kmx2.7km at nadir). The CO2/CH4/CO/CF measurement suite in the near infrared spectral region provides the information needed to disentangle natural and anthropogenic contributions to atmospheric carbon concentrations and to minimize uncertainties in the flow of carbon between the atmosphere and surface. The half meter cube size GeoFTS instrument is based on a Michelson interferometer design that uses all high TRL components in a modular configuration to reduce complexity and cost. It is self-contained and as independent of the spacecraft as possible with simple spacecraft interfaces, making it ideal to be a "hosted" payload on a commercial communications satellite mission. The hosted payload approach for measuring the major carbon-containing gases in the atmosphere from the geostationary vantage point will affordably advance the scientific understating of carbon cycle processes and climate change.

atmospheric trace gases↗
NASA NTRS2013

Carbon Dioxide: Surprising Effects on Decision Making and Neurocognitive Performance

The occupants of modern submarines and the International Space Station (ISS) have much in common as far as their air quality is concerned. Air is polluted by materials offgassing, use of utility compounds, leaks of systems chemicals, and anthropogenic sources. The primary anthropogenic compound of concern to submariners and astronauts has been carbon dioxide (CO2). NASA and the US Navy rely on the National Research Council Committee on Toxicology (NRC-COT) to help formulate exposure levels to CO2 that are thought to be safe for exposures of 3-6 months. NASA calls its limits Spacecraft Maximum Allowable Concentrations (SMACs). Years of experience aboard the ISS and a recent publication on deficits in decision making in ground-based subjects exposed briefly to 0.25% CO2 suggest that exposure levels that have been presumed acceptable to preserve health and performance need to be reevaluated. The current CO2 exposure limits for 3-6 months set by NASA and the UK Navy are 0.7%, and the limit for US submariners is 0.5%, although the NRC-COT recommended a 90-day level of 0.8% as safe a few years ago. NASA has set a 1000-day SMAC at 0.5% for exploration-class missions. Anecdotal experience with ISS operations approaching the current 180-day SMAC of 0.7% suggest that this limit is too high. Temporarily, NASA has limited exposures to 0.5% until further peer-reviewed data become available. In the meantime, a study published last year in the journal Environmental Health Perspectives (Satish U, et al. 2012) demonstrated that complexdecision- making performance is somewhat affected at 0.1% CO2 and becomes "dysfunctional" for at least half of the 9 indices of performance at concentrations approaching 0.25% CO2. The investigators used the Strategic Management Simulation (SMS) method of testing for decisionmaking ability, and the results were so surprising to the investigators that they declared that their findings need to be independently confirmed. NASA has responded to the findings on decision making by developing a study to either confirm or refute the published results. In addition, other neurocognitive tests that have been and will be used aboard the ISS will be part of the ground-based study. Further evaluations during the exposures will include ocular and cardiovascular effects of CO2 exposure. In addition, the 1- carbon genetics of the test subjects will be evaluated to determine if any individual subjects are unusually susceptible to CO2 exposure because of genetic factors. Our plan is to extend the published study from Satish by employing a wider series of CO2 exposures to include concentrations of 0.06, 0.12, 0.25, and 0.50%. We believe that our findings will be of keen interest to submariners and to those designing "tight" buildings.

James, John T.↗
NASA NTRS2012

Climate Impacts of Ice Nucleation

Several different ice nucleation parameterizations in two different General Circulation Models (GCMs) are used to understand the effects of ice nucleation on the mean climate state, and the Aerosol Indirect Effects (AIE) of cirrus clouds on climate. Simulations have a range of ice microphysical states that are consistent with the spread of observations, but many simulations have higher present-day ice crystal number concentrations than in-situ observations. These different states result from different parameterizations of ice cloud nucleation processes, and feature different balances of homogeneous and heterogeneous nucleation. Black carbon aerosols have a small (0.06 Wm(exp-2) and not statistically significant AIE when included as ice nuclei, for nucleation efficiencies within the range of laboratory measurements. Indirect effects of anthropogenic aerosols on cirrus clouds occur as a consequence of increasing anthropogenic sulfur emissions with different mechanisms important in different models. In one model this is due to increases in homogeneous nucleation fraction, and in the other due to increases in heterogeneous nucleation with coated dust. The magnitude of the effect is the same however. The resulting ice AIE does not seem strongly dependent on the balance between homogeneous and heterogeneous ice nucleation. Regional effects can reach several Wm2. Indirect effects are slightly larger for those states with less homogeneous nucleation and lower ice number concentration in the base state. The total ice AIE is estimated at 0.27 +/- 0.10 Wm(exp-2) (1 sigma uncertainty). This represents a 20% offset of the simulated total shortwave AIE for ice and liquid clouds of 1.6 Wm(sup-2).

Gettelman, Andrew↗
NASA NTRS2009

Monitoring Exchange of CO2 - A KISS Workshop Report 2009

The problem and context: Can top-down estimates of carbon dioxide (CO2) fluxes resolve the anthropogenic emissions of China, India, the United States, and the European Union with an accuracy of +/-10% or better?The workshop "Monitoring Exchange of Carbon Dioxide" was convened at the Keck Institute for Space Studies in Pasadena, California in February 2010 to address this question. The Workshop brought together an international, interdisciplinary group of 24 experts in carbon cycle science, remote sensing, emissions inventory estimation, and inverse modeling. The participants reviewed the potential of space-based and sub-orbital observational and modeling approaches to monitor anthropogenic CO2 emissions in the presence of much larger natural fluxes from the exchange of CO2 between the land, atmosphere, and ocean. This particular challenge was motivated in part by the NRC Report "Verifying Greenhouse Gas Emissions" [Pacala et al., 2010]. This workshop report includes several recommendations for improvements to observing strategies and modeling frameworks for optimal and cost-effective monitoring of carbon exchange

Greenhouse Gas Emissions↗
NASA NTRS2012

Tropospheric Bromine Chemistry: Implications for Present and Pre-industrial Ozone and Mercury

We present a new model for the global tropospheric chemistry of inorganic bromine (Bry) coupled to oxidant-aerosol chemistry in the GEOS-Chem chemical transport model (CTM). Sources of tropospheric Bry include debromination of sea-salt aerosol, photolysis and oxidation of short-lived bromocarbons, and transport from the stratosphere. Comparison to a GOME-2 satellite climatology of tropospheric BrO columns shows that the model can reproduce the observed increase of BrO with latitude, the northern mid-latitudes maximum in winter, and the Arctic maximum in spring. This successful simulation is contingent on the HOBr + HBr reaction taking place in aqueous aerosols and ice clouds. Bromine chemistry in the model decreases tropospheric ozone mixing ratios by <1-8 nmol/mol (6.5% globally), with the largest effects in the northern extratropics in spring. The global mean tropospheric OH concentration decreases by 4 %. Inclusion of bromine chemistry improves the ability of global models (GEOS-Chem and p-TOMCAT) to simulate observed 19th-century ozone and its seasonality. Bromine effects on tropospheric ozone are comparable in the present-day and pre-industrial atmospheres so that estimates of anthropogenic radiative forcing are minimally affected. Br atom concentrations are 40% higher in the pre-industrial atmosphere due to lower ozone, which would decrease by a factor of 2 the atmospheric lifetime of elemental mercury against oxidation by Br. This suggests that historical anthropogenic mercury emissions may have mostly deposited to northern mid-latitudes, enriching the corresponding surface reservoirs. The persistent rise in background surface ozone at northern mid-latitudes during the past decades could possibly contribute to the observations of elevated mercury in subsurface waters of the North Atlantic.

bromine↗
NASA NTRS2014

Initial Results from the Kwajalein Micrometeorite Collections

Micrometeorites are constantly arriving at the Earth's surface, however, they are quickly diluted by the natural and anthropogenic back-ground dust. The successful collection of micromete-orites requires either the employment of a separation technique (e.g. using magnets to separate metal-bearing micrometeorites from deepsea sediments [e.g. 1,2] and dissolved pre-historic limestones and salts [e.g. 3,4]), or an approach that limits contamination by terrestrial dust (e.g. collecting from ice, snow and well water in polar regions - locations where the terrestrial dust flux is so low that micrometeorites repre-sent the major dust component [e.g. 5-7]). We have recently set up a micrometeorite collection station on Kwajalein Island in the Republic of the Marshall Is-lands in the Pacific Ocean, using high volume air samplers to collect particles directly from the atmosphere. Collecting at this location exploits the considerably reduced anthropogenic background; Kwajalein is >1000 miles from the nearest continent and for much of the year, trade winds blow from the northeast at 15 to 20 knots providing a continuous stream of oceanic aerosol for sampling. By collecting directly from the atmosphere, the terrestrial age of the particles, and hence weathering they experience, is minimal. We therefore anticipate that the Kwajalein col-lection may include particles that are highly susceptible to weathering and either not preserved well or not found at all in other collections. In addition, this collection method allows for particle arrival times to be constrained so that collections can be timed to correlate with celestial events (e.g. meteor showers). Here we describe the collections and their preparation and report on the initial results.

Wozniakiewicz, P. J.↗
NASA NTRS2013

Preindustrial to Present-Day Changes in Tropospheric Hydroxyl Radical and Methane Lifetime from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

We have analysed time-slice simulations from 17 global models, participating in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), to explore changes in present-day (2000) hydroxyl radical (OH) concentration and methane (CH4) lifetime relative to preindustrial times (1850) and to 1980. A comparison of modeled and observation-derived methane and methyl chloroform lifetimes suggests that the present-day global multi-model mean OH concentration is overestimated by 5 to 10% but is within the range of uncertainties. The models consistently simulate higher OH concentrations in the Northern Hemisphere (NH) compared with the Southern Hemisphere (SH) for the present-day (2000; inter-hemispheric ratios of 1.13 to 1.42), in contrast to observation-based approaches which generally indicate higher OH in the SH although uncertainties are large. Evaluation of simulated carbon monoxide (CO) concentrations, the primary sink for OH, against ground-based and satellite observations suggests low biases in the NH that may contribute to the high north–south OH asymmetry in the models. The models vary widely in their regional distribution of present-day OH concentrations (up to 34%). Despite large regional changes, the multi-model global mean (mass-weighted) OH concentration changes little over the past 150 yr, due to concurrent increases in factors that enhance OH (humidity, tropospheric ozone, nitrogen oxide (NOx) emissions, and UV radiation due to decreases in stratospheric ozone), compensated by increases in OH sinks (methane abundance, carbon monoxide and non-methane volatile organic carbon (NMVOC) emissions). The large inter-model diversity in the sign and magnitude of preindustrial to present-day OH changes (ranging from a decrease of 12.7% to an increase of 14.6%) indicate that uncertainty remains in our understanding of the long-term trends in OH and methane lifetime. We show that this diversity is largely explained by the different ratio of the change in global mean tropospheric CO and NOx burdens (Delta CO/Delta NOx, approximately represents changes in OH sinks versus changes in OH sources) in the models, pointing to a need for better constraints on natural precursor emissions and on the chemical mechanisms in the current generation of chemistry-climate models. For the 1980 to 2000 period, we find that climate warming and a slight increase in mean OH (3.5 +/- 2.2%) leads to a 4.3 +/- 1.9% decrease in the methane lifetime. Analysing sensitivity simulations performed by 10 models, we find that preindustrial to present-day climate change decreased the methane lifetime by about four months, representing a negative feedback on the climate system. Further, we analysed attribution experiments performed by a subset of models relative to 2000 conditions with only one precursor at a time set to 1860 levels. We find that global mean OH increased by 46.4 +/- 12.2% in response to preindustrial to present-day anthropogenic NOx emission increases, and decreased by 17.3 +/-2.3%, 7.6 +/- 1.5%, and 3.1 +/- 3.0% due to methane burden, and anthropogenic CO, and NMVOC emissions increases, respectively.

nitrogen oxides↗
NASA NTRS2014

Climate Sensitivity in the Anthropocene

Climate sensitivity in its most basic form is defined as the equilibrium change in global surface temperature that occurs in response to a climate forcing, or externally imposed perturbation of the planetary energy balance. Within this general definition, several specific forms of climate sensitivity exist that differ in terms of the types of climate feedbacks they include. Based on evidence from Earth's history, we suggest here that the relevant form of climate sensitivity in the Anthropocene (e.g. from which to base future greenhouse gas (GHG) stabilization targets) is the Earth system sensitivity including fast feedbacks from changes in water vapour, natural aerosols, clouds and sea ice, slower surface albedo feedbacks from changes in continental ice sheets and vegetation, and climate-GHG feedbacks from changes in natural (land and ocean) carbon sinks. Traditionally, only fast feedbacks have been considered (with the other feedbacks either ignored or treated as forcing), which has led to estimates of the climate sensitivity for doubled CO2 concentrations of about 3 C. The 2×CO2 Earth system sensitivity is higher than this, being approx. 4-6 C if the ice sheet/vegetation albedo feedback is included in addition to the fast feedbacks, and higher still if climate-GHG feedbacks are also included. The inclusion of climate-GHG feedbacks due to changes in the natural carbon sinks has the advantage of more directly linking anthropogenic GHG emissions with the ensuing global temperature increase, thus providing a truer indication of the climate sensitivity to human perturbations. The Earth system climate sensitivity is difficult to quantify due to the lack of palaeo-analogues for the present-day anthropogenic forcing, and the fact that ice sheet and climate-GHG feedbacks have yet to become globally significant in the Anthropocene. Furthermore, current models are unable to adequately simulate the physics of ice sheet decay and certain aspects of the natural carbon and nitrogen cycles. Obtaining quantitative estimates of the Earth system sensitivity is therefore a high priority for future work.

Anthropocene↗
NASA NTRS2013

Tropospheric Ozone Changes, Radiative Forcing and Attribution to Emissions in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

Ozone (O3) from 17 atmospheric chemistry models taking part in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) has been used to calculate tropospheric ozone radiative forcings (RFs). All models applied a common set of anthropogenic emissions, which are better constrained for the present-day than the past. Future anthropogenic emissions follow the four Representative Concentration Pathway (RCP) scenarios, which define a relatively narrow range of possible air pollution emissions. We calculate a value for the pre-industrial (1750) to present-day (2010) tropospheric ozone RF of 410 mW m−2. The model range of pre-industrial to present-day changes in O3 produces a spread (+/-1 standard deviation) in RFs of +/-17%. Three different radiation schemes were used - we find differences in RFs between schemes (for the same ozone fields) of +/-10 percent. Applying two different tropopause definitions gives differences in RFs of +/-3 percent. Given additional (unquantified) uncertainties associated with emissions, climate-chemistry interactions and land-use change, we estimate an overall uncertainty of +/-30 percent for the tropospheric ozone RF. Experiments carried out by a subset of six models attribute tropospheric ozone RF to increased emissions of methane (44+/-12 percent), nitrogen oxides (31 +/- 9 percent), carbon monoxide (15 +/- 3 percent) and non-methane volatile organic compounds (9 +/- 2 percent); earlier studies attributed more of the tropospheric ozone RF to methane and less to nitrogen oxides. Normalising RFs to changes in tropospheric column ozone, we find a global mean normalised RF of 42 mW m(−2) DU(−1), a value similar to previous work. Using normalised RFs and future tropospheric column ozone projections we calculate future tropospheric ozone RFs (mW m(−2); relative to 1750) for the four future scenarios (RCP2.6, RCP4.5, RCP6.0 and RCP8.5) of 350, 420, 370 and 460 (in 2030), and 200, 300, 280 and 600 (in 2100). Models show some coherent responses of ozone to climate change: decreases in the tropical lower troposphere, associated with increases in water vapour; and increases in the sub-tropical to mid-latitude upper troposphere, associated with increases in lightning and stratosphere-to-troposphere transport. Climate change has relatively small impacts on global mean tropospheric ozone RF.

climate change↗