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NASA NTRS2014

Science Accomplishments from a Decade of Aura OMI/MLS Tropospheric Ozone Measurements

Measurements of tropospheric ozone from combined Aura OMI and MLS instruments have yielded a large number of new and important science discoveries over the last decade. These discoveries have generated a much greater understanding of biomass burning, lightning NO, and stratosphere-troposphere exchange sources of tropospheric ozone, ENSO dynamics and photochemistry, intra-seasonal variability-Madden-Julian Oscillation including convective transport, radiative forcing, measuring ozone pollution from space, improvements to ozone retrieval algorithms, and evaluation of chemical-transport and chemistry-climate models. The OMI-MLS measurements have been instrumental in giving us better understanding of the dynamics and chemistry involving tropospheric ozone and the many drivers affecting the troposphere in general. This discussion will provide an overview focusing on our main science results.

ENSO↗

NASA NTRS2014

Reconciliation of Halogen-Induced Ozone Loss with the Total-Column Ozone Record

The observed depletion of the ozone layer from the 1980s onwards is attributed to halogen source gases emitted by human activities. However, the precision of this attribution is complicated by year-to-year variations in meteorology, that is, dynamical variability, and by changes in tropospheric ozone concentrations. As such, key aspects of the total-column ozone record, which combines changes in both tropospheric and stratospheric ozone, remain unexplained, such as the apparent absence of a decline in total-column ozone levels before 1980, and of any long-term decline in total-column ozone levels in the tropics. Here we use a chemistry-climate model to estimate changes in halogen-induced ozone loss between 1960 and 2010; the model is constrained by observed meteorology to remove the eects of dynamical variability, and driven by emissions of tropospheric ozone precursors to separate out changes in tropospheric ozone. We show that halogen-induced ozone loss closely followed stratospheric halogen loading over the studied period. Pronounced enhancements in ozone loss were apparent in both hemispheres following the volcanic eruptions of El Chichon and, in particular, Mount Pinatubo, which significantly enhanced stratospheric aerosol loads. We further show that approximately 40% of the long-term non-volcanic ozone loss occurred before 1980, and that long-term ozone loss also occurred in the tropical stratosphere. Finally, we show that halogeninduced ozone loss has declined by over 10% since stratospheric halogen loading peaked in the late 1990s, indicating that the recovery of the ozone layer is well underway.

Shepherd, T. G.↗

NASA NTRS2014

Global Distribution and Trends of Tropospheric Ozone: An Observation-Based Review

Tropospheric ozone plays a major role in Earth's atmospheric chemistry processes and also acts as an air pollutant and greenhouse gas. Due to its short lifetime, and dependence on sunlight and precursor emissions from natural and anthropogenic sources, tropospheric ozone's abundance is highly variable in space and time on seasonal, interannual and decadal time-scales. Recent, and sometimes rapid, changes in observed ozone mixing ratios and ozone precursor emissions inspired us to produce this up-to-date overview of tropospheric ozone's global distribution and trends. Much of the text is a synthesis of in situ and remotely sensed ozone observations reported in the peer-reviewed literature, but we also include some new and extended analyses using well-known and referenced datasets to draw connections between ozone trends and distributions in different regions of the world. In addition, we provide a brief evaluation of the accuracy of rural or remote surface ozone trends calculated by three state-of-the-science chemistry-climate models, the tools used by scientists to fill the gaps in our knowledge of global tropospheric ozone distribution and trends.

Mixing ratios↗

NASA NTRS2014

Assessing the Ability of Instantaneous Aircraft and Sonde Measurements to Characterize Climatological Means and Long-Term Trends in Tropospheric Composition

Over four decades of measurements exist that sample the 3-D composition of reactive trace gases in the troposphere from approximately weekly ozone sondes, instrumentation on civil aircraft, and individual comprehensive aircraft field campaigns. An obstacle to using these data to evaluate coupled chemistry-climate models (CCMs)the models used to project future changes in atmospheric composition and climateis that exact space-time matching between model fields and observations cannot be done, as CCMs generate their own meteorology. Evaluation typically involves averaging over large spatiotemporal regions, which may not reflect a true average due to limited or biased sampling. This averaging approach generally loses information regarding specific processes. Here we aim to identify where discrete sampling may be indicative of long-term mean conditions, using the GEOS-Chem global chemical-transport model (CTM) driven by the MERRA reanalysis to reflect historical meteorology from 2003 to 2012 at 2o by 2.5o resolution. The model has been sampled at the time and location of every ozone sonde profile available from the Would Ozone and Ultraviolet Radiation Data Centre (WOUDC), along the flight tracks of the IAGOSMOZAICCARABIC civil aircraft campaigns, as well as those from over 20 individual field campaigns performed by NASA, NOAA, DOE, NSF, NERC (UK), and DLR (Germany) during the simulation period. Focusing on ozone, carbon monoxide and reactive nitrogen species, we assess where aggregates of the in situ data are representative of the decadal mean vertical, spatial and temporal distributions that would be appropriate for evaluating CCMs. Next, we identically sample a series of parallel sensitivity simulations in which individual emission sources (e.g., lightning, biogenic VOCs, wildfires, US anthropogenic) have been removed one by one, to assess where and when the aggregated observations may offer constraints on these processes within CCMs. Lastly, we show results of an additional 31-year simulation from 1980-2010 of GEOS-Chem driven by the MACCity emissions inventory and MERRA reanalysis at 4o by 5o. We sample the model at every WOUDC sonde and flight track from MOZAIC and NASA field campaigns to evaluate which aggregate observations are statistically reflective of long-term trends over the period.

Atmospheric composition↗

NASA NTRS2016

Silicon Chemistry in the Mesosphere and Lower Thermosphere

Silicon is one of the most abundant elements in cosmic dust, and meteoric ablation injects a significant amount of Si into the atmosphere above 80 km. In this study, a new model for silicon chemistry in the mesosphere lower thermosphere is described, based on recent laboratory kinetic studies of Si, SiO,SiO2, and S(exp +). Electronic structure calculations and statistical rate theory are used to show that the likely fate of SiO2 is a two-step hydration to silicic acid (Si(OH)4), which then polymerizes with metal oxides and hydroxides to form meteoric smoke particles. This chemistry is then incorporated into a whole atmosphere chemistry-climate model. The vertical profiles of Si+ and the Si(exp +)Fe(exp +) ratio are shown to be in good agreement with rocket-borne mass spectrometric measurements between 90 and 110 km. Si(exp +) has consistently been observed to be the major meteoric ion around 110 km; this implies that the relative injection rate of Si from meteoric ablation, compared to metals such as Fe and Mg, is significantly larger than expected based on the irrelative chondritic abundances. Finally, the global abundances of SiO and Si(OH)4 show clear evidence of the seasonal meteoric input function, which is much less pronounced in the case of other meteoric species.

Plane, John M. C.↗

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 NTRS2015

Future Changes in Major Stratospheric Warmings in CCMI Models

Major stratospheric warmings (MSWs) are one of the most important phenomena of wintertime Arctic stratospheric variability. They consist of a warming of the Arctic stratosphere and a deceleration of the polar night jet, triggered by an anomalously high injection of tropospheric wave activity into the stratosphere. Due to the relevance and the impact of MSWs on the tropospheric circulation, several model studies have investigated their potential responses to climate change. However, a wide range of results has been obtained, extending from a future increase in the frequency of MSWs to a decrease. These discrepancies might be explained by different factors such as a competition of radiative and dynamical contributors with opposite effects on the Arctic polar vortex, biases of models to reproduce the related processes, or the metric chosen for the identification of MSWs. In this study, future changes in wintertime Arctic stratospheric variability are examined in order to obtaina more precise picture of future changes in the occurrence of MSWs. In particular, transient REFC2 simulations of different CCMs involved in the Chemistry Climate Model Initiative (CCMI) are used. These simulations extend from 1960 to 2100 and include forcings by halogens and greenhouse gases following the specifications of the CCMI-REF-C2 scenario. Sea surface temperatures (SSTs) and sea-ice distributions are either prescribed from coupled climate model integrations or calculated internally in the case of fully coupled atmosphere-ocean CCMs. Potential changes in the frequency and main characteristics of MSWs in the future are investigated with special focus on the dependence of the results on the criterion for the identification of MSWs and the tropospheric forcing of these phenomena.

Chemistry-Climate Modeling↗

NASA NTRS2016

Chemistry Simulations Using MERRA-2 Reanalysis with the GMI CTM and Replay in Support of the Atmospheric Composition Community

Simulations using reanalyzed meteorological conditions have been long used to understand causes of atmospheric composition change over the recent past. Using the new Modern-Era Retrospective analysis for Research and Applications, version 2 (MERRA-2) meteorology, chemistry simulations are being conducted to create products covering 1980-2016 for the atmospheric composition community. These simulations use the Global Modeling Initiative (GMI) chemical mechanism in two different models: the GMI Chemical Transport Model (CTM) and the GEOS-5 model developed Replay mode. Replay mode means an integration of the GEOS-5 general circulation model that is incrementally adjusted each time step toward the MERRA-2 analysis. The GMI CTM is a 1 x 1.25 simulation and the MERRA-2 GMI Replay simulation uses the native MERRA-2 approximately horizontal resolution on the cubed sphere. The Replay simulations is driven by the online use of key MERRA-2 meteorological variables (i.e. U, V, T, and surface pressure) with all other variables calculated in response to those variables. A specialized set of transport diagnostics is included in both runs to better understand trace gas transport and changes over the recent past.

Chemistry-Climate Model↗

NASA NTRS2013

Impacts of Atmosphere-Ocean Coupling on Southern Hemisphere Climate Change

Climate in the Southern Hemisphere (SH) has undergone significant changes in recent decades. These changes are closely linked to the shift of the Southern Annular Mode (SAM) towards its positive polarity, which is driven primarily by Antarctic ozone depletion. There is growing evidence that Antarctic ozone depletion has significant impacts on Southern Ocean circulation change. However, it is poorly understood whether and how ocean feedback might impact the SAM and climate change in the SH atmosphere. This outstanding science question is investigated using the Goddard Earth Observing System Coupled Atmosphere-Ocean-Chemistry Climate Model(GEOS-AOCCM).We perform ensemble simulations of the recent past (1960-2010) with and without the interactive ocean. For simulations without the interactive ocean, we use sea surface temperatures and sea ice concentrations produced by the interactive ocean simulations. The differences between these two ensemble simulations quantify the effects of atmosphere-ocean coupling. We will investigate the impacts of atmosphere-ocean coupling on stratospheric processes such as Antarctic ozone depletion and Antarctic polar vortex breakup. We will address whether ocean feedback affects Rossby wave generation in the troposphere and wave propagation into the stratosphere. Another focuson this study is to assess how ocean feedback might affect the tropospheric SAM response to Antarctic ozone depletion

Chemistry-Climate Modeling↗

NASA NTRS2015

Impact of Stratospheric Ozone Zonal Asymmetries on the Tropospheric Circulation

The depletion and recovery of Antarctic ozone plays a major role in changes of Southern Hemisphere (SH) tropospheric climate. Recent studies indicate that the lack of polar ozone asymmetries in chemistry climate models (CCM) leads to a weaker and warmer Antarctic vortex, and smaller trends in the tropospheric mid-latitude jet and the surface pressure. However, the tropospheric response to ozone asymmetries is not well understood. In this study we report on a series of integrations of the Goddard Earth Observing System Chemistry Climate Model (GEOS CCM) to further examine the effect of zonal asymmetries on the state of the stratosphere and troposphere. Integrations with the full, interactive stratospheric chemistry are compared against identical simulations using the same CCM except that (1) the monthly mean zonal mean stratospheric ozone from first simulation is prescribed and (2) ozone is relaxed to the monthly mean zonal mean ozone on a three day time scale. To analyze the tropospheric response to ozone asymmetries, we examine trends and quantify the differences in temperatures, zonal wind and surface pressure among the integrations.

Chemistry-Climate Modeling↗

NASA NTRS2015

Using Satellite Observations of Cloud Vertical Distribution to Improve Global Model Estimates of Cloud Radiative Effect on Key Tropospheric Oxidants

Radiative effect of clouds is one of the major factors that affect tropospheric OH. Large differences in cloud distributions among current (chemistry-climate or chemical transport) models could contribute significantly to the wide model spread of tropospheric OH, which was reported by the ACCMIP activity (Voulgarakis et al., ACP 2013). CCCM, a 3-D cloud data product developed at NASA Langley and merged from multiple A-Train satellite observations, provides unprecedentedly strong constraints on the vertical distribution of clouds and therefore simulated effects of clouds on key tropospheric oxidants.

Liu, Hongyu↗

NASA NTRS2012

The Response of Tropospheric Ozone to ENSO in Observations and a Chemistry-Climate Simulation

The El Nino-Southern Oscillation (ENSO) is the dominant mode of tropical variability on interannual time scales. ENSO appears to extend its influence into the chemical composition of the tropical troposphere. Recent results have revealed an ENSO induced wave-l anomaly in observed tropical tropospheric column ozone. This results in a dipole over the western and eastern tropical Pacific, whereby differencing the two regions produces an ozone anomaly with an extremely high correlation to the Nino 3.4 Index. We have successfully reproduced this result using the Goddard Earth Observing System Version 5 (GEOS-5) general circulation model coupled to a comprehensive stratospheric and tropospheric chemical mechanism forced with observed sea surface temperatures over the past 25 years. An examination of the modeled ozone field reveals the vertical contributions of tropospheric ozone to the column over the western and eastern Pacific region. We will show targeted comparisons with observations from NASA's Aura satellite Microwave Limb Sounder (MLS), and the Tropospheric Emissions Spectrometer (TES) to provide insight into the vertical structure of ozone changes. The tropospheric ozone response to ENSO could be a useful chemistry-climate model evaluation tool and should be considered in future modeling assessments.

Oman, L. D.↗

NASA NTRS2002

Chemistry-Climate Interactions in the Goddard Institute for Space Studies General Circulation Model: New Insights into Modeling the Pre-Industrial Atmosphere - 2

We investigate the chemical (hydroxyl and ozone) and dynamical response to changing from present day to pre-industrial conditions in the Goddard Institute for Space Studies General Circulation Model (GISS GMC). We identify three main improvements not included by many other works. Firstly, our model includes interactive cloud calculations. Secondly we reduce sulfate aerosol which impacts NOx partitioning hence Ox distributions. Thirdly we reduce sea surface temperatures and increase ocean ice coverage which impact water vapor and ground albedo respectively. Changing the ocean data (hence water vapor and ozone) produces a potentially important feedback between the Hadley circulation and convective cloud cover. Our present day run (run 1, control run) global mean OH value was 9.8 x 10(exp 5) molecules/cc. For our best estimate of pre-industrial conditions run (run 2) which featured modified chemical emissions, sulfate aerosol and sea surface temperatures/ocean ice, this value changed to 10.2 x 10(exp 5) molecules/cc. Reducing only the chemical emissions to pre-industrial levels in run 1 (run 3) resulted in this value increasing to 10.6 x 10(exp 5) molecules/cc. Reducing the sulfate in run 3 to pre-industrial levels (run 4) resulted in a small increase in global mean OH (10.7 x 10(exp 5) molecules/cc). Changing the ocean data in run 4 to pre-industrial levels (run 5) led to a reduction in this value to 10.3 x 10(exp 5) molecules/cc. Mean tropospheric ozone burdens were 262, 181, 180, 180, and 182 Tg for runs 1-5 respectively.

Grenfell, J. Lee↗

NASA NTRS2012

Modeling and Observations of the Response of Tropical Tropospheric Ozone to ENSO

The El Nino-Southern Oscillation (ENSO) is the dominant mode of tropical variability on interannual time scales. ENSO appears to extend its influence into the chemical composition of the tropical troposphere, Recent results have revealed an ENSO induced wave-1 anomaly in observed tropical tropospheric column ozone, This results in a dipole over the western and eastern tropical Pacific, whereby differencing the two regions produces an ozone anomaly with an extremely high correlation to the Nino 3.4 Index. We have successfully reproduced this result using the Goddard Earth Observing System Version 5 (GEOS-5) general circulation model coupled to a comprehensive stratospheric and tropospheric chemical mechanism forced with observed sea surface temperatures over the past 25 years, An examination of the modeled ozone field reveals the vertical contributions of tropospheric ozone to the column over the western and eastern Pacific region, We will show targeted comparisons with SHADOZ ozonesondes over these regions to provide insight into the vertical structure. Also, comparisons with NASA's Aura satellite Microwave Limb Sounder (MLS) and Tropospheric Emissions Spectrometer (TES) instruments and other appropriate data sets will be shown. In addition, the water vapor response to ENSO will be compared to help illuminate its role relative to dynamics in impacting ozone concentrations. These results indicate that the tropospheric ozone response to ENSO is potentially a very useful chemistry-climate diagnostic and should be considered in future modeling assessments.

Oman, L. D.↗

NASA NTRS2012

The Response of Lower Atmospheric Ozone to ENSO in Aura Measurements and a Chemistry-Climate Simulation

The El Nino-Southern Oscillation (ENSO) is the dominant mode of tropical variability on interannual time scales. ENSO appears to extend its influence into the chemical composition of the tropical troposphere. Recent work has revealed an ENSO-induced wave-1 anomaly in observed tropical tropospheric column ozone. This results in a dipole over the western and eastern tropical Pacific, whereby differencing the two regions produces an ozone anomaly with an extremely high correlation to the Nino 3.4 Index. We have successfully reproduced this feature using the Goddard Earth Observing System Version 5 (GEOS-5) general circulation model coupled to a comprehensive stratospheric and tropospheric chemical mechanism forced with observed sea surface temperatures over the past 25 years. An examination of the modeled ozone field reveals the vertical contributions of tropospheric ozone to the column over the western and eastern Pacific region. We will show composition sensitivity in observations from NASA s Aura satellite Microwave Limb Sounder (MLS) and the Tropospheric Emissions Spectrometer (TES) and a simulation to provide insight into the vertical structure of these ENSO-induced ozone changes. The ozone changes due to the Quasi-Biennial Oscillation (QBO) in the extra-polar upper troposphere and lower stratosphere in MLS measurements will also be discussed.

Oman, L. D.↗

NASA NTRS2007

Clouds in GEOS-5

The GEOS-5 atmospheric model is being developed as a weather-and-climate capable model. It must perform well in assimilation mode as well as in weather and climate simulations and forecasts and in coupled chemistry-climate simulations. In developing GEOS-5, attention has focused on the representation of moist processes. The moist physics package uses a single phase prognostic condensate and a prognostic cloud fraction. Two separate cloud types are distinguished by their source: "anvil" cloud originates in detraining convection, and large-scale cloud originates in a PDF-based condensation calculation. Ice and liquid phases for each cloud type are considered. Once created, condensate and fraction from the anvil and statistical cloud types experience the same loss processes: evaporation of condensate and fraction, auto-conversion of liquid or mixed phase condensate, sedimentation of frozen condensate, and accretion of condensate by falling precipitation. The convective parameterization scheme is the Relaxed Arakawa-Schubert, or RAS, scheme. Satellite data are used to evaluate the performance of the moist physics packages and help in their tuning. In addition, analysis of and comparisons to cloud-resolving models such as the Goddard Cumulus Ensemble model are used to help improve the PDFs used in the moist physics. The presentation will show some of our evaluations including precipitation diagnostics.

Bacmeister, Julio↗

NASA NTRS2001

Chemistry-Climate Interactions in the GISS GCM: Tropospheric Chemistry Model Description and Evaluation - Part 1

A tropospheric chemistry module has been developed for use within the Goddard Institute for Space Studies (GISS) general circulation model (GCM) to study interactions between chemistry and climate change. The model uses a simplified chemistry scheme based on CO-NOx-CH4 chemistry, and also includes a parameterization for emissions of isoprene, the most important non-methane hydrocarbon. The model reproduces present day annual cycles and mean distributions of key trace gases fairly well, based on extensive comparisons with available observations. Examining the simulated change between present day and pre-industrial conditions, we find that the model has a similar response to that seen in other simulations. It shows a 45% increase in the global tropospheric ozone burden, within the 25% - 57% range seen in other studies. Annual average zonal mean ozone increases by more than 125% at Northern Hemisphere middle latitudes near the surface. Comparison of model runs that allow the calculated ozone to interact with the GCM's radiation and meteorology with those that do not shows only minor differences for ozone. The common usage of ozone fields that are not calculated interactively seems to be adequate to simulate both the present day and the pre-industrial ozone distributions. However, use of coupled chemistry does alter the change in tropospheric oxidation capacity, enlarging the overall decrease in OH concentrations from the pre-industrial to the present by about 10% (-5.3% global annual average in uncoupled mode, -5.9% in coupled mode). This indicates that there may be systematic biases in the simulation of the pre-industrial to present day decrease in the oxidation capacity of the troposphere (though a 10% difference is well within the total uncertainty). Global annual average radiative forcing from pre-industrial to present day ozone change is 0.32 W/sq m. The forcing seems to be increased by about 10% when the chemistry is coupled to the GCM. Forcing values greater than 0.8 W/sq m are seen over large areas of the United States, Southern Europe, North Africa, the Middle East, Central Asia, and the Arctic. Radiative forcing is greater than 1.5 W/sq m over parts of these areas during Northern summer Though there are local differences, the radiative forcing is overall in good agreement with the results of other modeling studies in both its magnitude and spatial distribution, demonstrating that the simplified chemistry is adequate for climate studies.

Shindell, Drew T.↗

NASA NTRS2012

The Role of Lightning in Controlling Interannual Variability of Tropical Tropospheric Ozone and OH and its Implications for Climate

Nitrogen oxides (NO(x) = NO + NO2) produced by lightning make a major contribution to the production of the dominant tropospheric oxidants (OH and ozone). These oxidants control the lifetime of many trace gases including long-lived greenhouse gases, and control the source-receptor relationship of inter-hemispheric pollutant transport. Lightning is affected by meteorological variability, and therefore represents a potentially important tropospheric chemistry-climate feedback. Understanding how interannual variability (IAV) in lightning affects IAV in ozone and OH in the recent past is important if we are to predict how oxidant levels may change in a future warmer climate. However, lightning parameterizations for chemical transport models (CTMs) show low skill in reproducing even climatological distributions of flash rates from the Lightning Imaging Sensor (LIS) and the Optical Transient Detector (OTD) satellite instruments. We present an optimized regional scaling algorithm for CTMs that enables sufficient sampling of spatiotemporally sparse satellite lightning data from LIS to constrain the spatial, seasonal, and interannual variability of tropical lightning. We construct a monthly time series of lightning flash rates for 1998-2010 and 35degS-35degN, and find a correlation of IAV in total tropical lightning with El Nino. We use the IAV-constraint to drive a 9-year hindcast (1998-2006) of the GEOS-Chem 3D chemical transport model, and find the increased IAV in LNO(x) drives increased IAV in ozone and OH, improving the model fs ability to simulate both. Although lightning contributes more than any other emission source to IAV in ozone, we find ozone more sensitive to meteorology, particularly convective transport. However, we find IAV in OH to be highly sensitive to lightning NO(x), and the constraint improves the ability of the model to capture the temporal behavior of OH anomalies inferred from observations of methyl chloroform and other gases. The sensitivity of OH is explained using photochemical reaction rates which show a "magnification" effect of the initial lightning NO perturbation on OH primary production, HO(x) recycling, and OH loss frequencies. This influence on OH may represent a negative feedback, if lightning increases in a warming world..

Murray, Lee T.↗