Interactive chemistry in the Laboratoire de Météorologie Dynamique general circulation model: model description and impact analysis of biogenic hydrocarbons on tropospheric chemistry

We present a description and evaluation of LMDz-INCA, a global three-dimensional chemistry-climate model, pertaining to its recently developed NMHC version. In this substantially extended version of the model a comprehensive representation of the photochemistry of non-methane hydrocarbons (NMHC) and volatile organic compounds (VOC) from biogenic, anthropogenic, and biomass-burning sources has been included. The tropospheric annual mean methane (9.2 years) and methylchloroform (5.5 years) chemical lifetimes are well within the range of previous modelling studies and are in excellent agreement with estimates established by means of global observations. The model provides a reasonable simulation of the horizontal and vertical distribution and seasonal cycle of CO and key non-methane VOC, such as acetone, methanol, and formaldehyde as compared to observational data from several ground stations and aircraft campaigns. LMDz-INCA in the NMHC version reproduces tropospheric ozone concentrations fairly well throughout most of the troposphere. The model is applied in several sensitivity studies of the biosphere-atmosphere photochemical feedback. The impact of surface emissions of isoprene, acetone, and methanol is studied. These experiments show a substantial impact of isoprene on tropospheric ozone and carbon monoxide concentrations revealing an increase in surface O₃ and CO levels of up to 30 ppbv and 60 ppbv, respectively. Isoprene also appears to significantly impact the global OH distribution resulting in a decrease of the global mean tropospheric OH concentration by approximately 0.7×10⁵ molecules cm^-3 or roughly 8% and an increase in the global mean tropospheric methane lifetime by approximately seven months. A global mean ozone net radiative forcing due to the isoprene induced increase in the tropospheric ozone burden of 0.09 W m^-2 is found. The key role of isoprene photooxidation in the global tropospheric redistribution of NO_x is demonstrated. LMDz-INCA calculates an increase of PAN surface mixing ratios ranging from 75 to 750 pptv and 10 to 250 pptv during northern hemispheric summer and winter, respectively. Acetone and methanol are found to play a significant role in the upper troposphere/lower stratosphere (UT/LS) budget of peroxy radicals. Calculations with LMDz-INCA show an increase in HO_x concentrations region of 8 to 15% and 10 to 15% due to methanol and acetone biogenic surface emissions, respectively. The model has been used to estimate the global tropospheric CO budget. A global CO source of 3019 Tg CO yr^-1 is estimated. This source divides into a primary source of 1533 Tg CO yr^-1 and secondary source of 1489 Tg CO yr^-1 deriving from VOC photooxidation. Global VOC-to-CO conversion efficiencies of 90% for methane and between 20 and 45% for individual VOC are calculated by LMDz-INCA

INFERNO: a fire and emissions scheme for the UK Met Office's Unified Model

Warm and dry climatological conditions favour the occurrence of forest fires. These fires then become a significant emission source to the atmosphere. Despite this global importance, fires are a local phenomenon and are difficult to represent in a large-scale Earth System Model (ESM). To address this, the INteractive Fire and Emission algoRithm for Natural envirOnments (INFERNO) was developed. INFERNO follows a reduced complexity approach and is intended for decadal to centennial scale climate simulations and assessment models for policy making. Fuel flammability is simulated using temperature, relative humidity, fuel density as well as precipitation and soil moisture. Combining flammability with ignitions and vegetation, burnt area is diagnosed. Emissions of carbon and key species are estimated using the carbon scheme in the JULES land surface model. JULES also possesses fire index diagnostics which we document and compare with our fire scheme. Two meteorology datasets and three ignition modes are used to validate the model. INFERNO is shown to effectively diagnose global fire occurrence (R = 0.66) and emissions (R = 0.59) through an approach appropriate to the complexity of an ESM, although regional biases remain

Sensitivity of mid-19th century tropospheric ozone to atmospheric chemistry-vegetation interactions

We use an Earth-System model (HadGEM2-ES) to investigate the sensitivity of mid-19th century tropospheric ozone to vegetation distribution and atmospheric chemistry-vegetation interaction processes. We conduct model experiments to isolate the response of mid-19th century tropospheric ozone to vegetation cover changes between the 1860s and present-day and to CO2 induced changes in isoprene emissions and dry deposition over the same period. Changes in vegetation distribution and CO2 suppression of isoprene emissions between mid-19th century and present-day, lead to decreases in global isoprene emissions of 19% and 21% respectively. This results in increases in surface ozone over the continents of up to 2 ppbv and of 2-6 ppbv in the tropical upper troposphere. The effects of CO2 increases on suppression of isoprene emissions and suppression of dry deposition to vegetation are small compared with the effects of vegetation cover change. Assuming present-day climate in addition to present-day vegetation cover and atmospheric CO2 concentrations, leads to increases in surface ozone concentrations of up to 5 ppbv over the entire northern hemisphere (NH), and of up to 8 ppbv in the NH free troposphere, compared with a mid-19th century simulation. Ozone changes are dominated by: 1) the role of isoprene as an ozone sink in the low NOx mid-19th century at30 mosphere, and 2) the redistribution of NOx to remote regions and the free troposphere via PAN (peroxyacetyl nitrate) formed from isoprene oxidation. We estimate a tropospheric ozone radiative forcing of 0.264W m−2 and a sensitivity in ozone radiative forcing to mid-19th century to present-day vegetation cover change of -0.012W m−2

Studying the impact of biomass burning aerosol radiative and climate effects on the Amazon rainforest productivity with an Earth system model

Diffuse light conditions can increase the efficiency of photosynthesis and carbon uptake by vegetation canopies. The diffuse fraction of photosynthetically active radiation (PAR) can be affected by either a change in the atmospheric aerosol burden and/or a change in cloudiness. During the dry season, a hotspot of biomass burning on the edges of the Amazon rainforest emits a complex mixture of aerosols and their precursors and climate-active trace gases (e.g. CO2, CH4, NOx). This creates potential for significant interactions between chemistry, aerosol, cloud, radiation and the biosphere across the Amazon region. The combined effects of biomass burning on the terrestrial carbon cycle for the present day are potentially large, yet poorly quantified. Here, we quantify such effects using the Met Office Hadley Centre Earth system model HadGEM2-ES, which provides a fully coupled framework with interactive aerosol, radiative transfer, dynamic vegetation, atmospheric chemistry and biogenic volatile organic compound emission components. Results show that for present day, defined as year 2000 climate, the overall net impact of biomass burning aerosols is to increase net primary productivity (NPP) by +80 to +105 TgC yr−1, or 1.9 % to 2.7 %, over the central Amazon Basin on annual mean. For the first time we show that this enhancement is the net result of multiple competing effects: an increase in diffuse light which stimulates photosynthetic activity in the shaded part of the canopy (+65 to +110 TgC yr−1), a reduction in the total amount of radiation (−52 to −105 TgC yr−1) which reduces photosynthesis and feedback from climate adjustments in response to the aerosol forcing which increases the efficiency of biochemical processes (+67 to +100 TgC yr−1). These results illustrate that despite a modest direct aerosol effect (the sum of the first two counteracting mechanisms), the overall net impact of biomass burning aerosols on vegetation is sizeable when indirect climate feedbacks are considered. We demonstrate that capturing the net impact of aerosols on vegetation should be assessed considering the system-wide behaviour

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 (ΔCO/ΔNOx, 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

Transition between nuclear and quark-gluon descriptions of hadrons and light nuclei

We provide a perspective on studies aimed at observing the transition between hadronic and quark-gluonic descriptions of reactions involving light nuclei. We begin by summarizing the results for relatively simple reactions such as the pion form factor and the neutral pion transition form factor as well as that for the nucleon and end with exclusive photoreactions in our simplest nuclei. A particular focus will be on reactions involving the deuteron. It is noted that a firm understanding of these issues is essential for unraveling important structure information from processes such as deeply virtual Compton scattering as well as deeply virtual meson production. The connection to exotic phenomena such as color transparency will be discussed. A number of outstanding challenges will require new experiments at modern facilities on the horizon as well as further theoretical developments.Comment: 37 pages, 17 figures, submitted to Reports on Progress in Physic

The Influence of Foreign vs North American Emissions on Surface Ozone in the US

As part of the Hemispheric Transport of Air Pollution (HTAP; www.htap.org) project, we analyze results from 16 global and hemispheric chemical transport models and compare these to Clean Air Status and Trends Network (CASTNet) observations in the United States (US) for 2001. Using the policy-relevant maximum daily 8-h ozone (MDA8 O3) statistic, the multi-model ensemble represents the observations well (mean r2=0.57, ensemble bias=+4.1 ppbv for all regions and all seasons) despite a wide range in the individual model results. Correlations are strongest in the NorthEastern US during spring and fall (r2=0.68); and weakest in the Midwestern US in summer (r2=0.46). However, large positive mean biases exist during summer for all Eastern US regions, ranging from 10¿20 ppbv, and a smaller negative bias is present in the Western US during spring (3 ppbv). In most all other regions and seasons, the biases of the model ensemble simulations are 5 ppbv. Sensitivity simulations in which anthropogenic O3-precursor emissions (NOx+NMVOC+CO+aerosols) were decreased by 20% in each of four source regions: East Asia (EA), South Asia (SA), Europe (EU) and North America (NA) show that the greatest response of MDA8 O3 to the summed foreign emissions reductions occurs during spring in the West (0.9 ppbv reduction due to 20% reductions from EA+SA+EU). East Asia is the largest contributor to MDA8 O3 at all ranges of the O3 distribution for most regions (typically 0.45 ppbv). The exception is in the NorthEastern US where European emissions reductions had the greatest impact on MDA8 O3, particularly in the middle of the MDA8 O3 distribution (response of 0.35 ppbv between 35¿55 ppbv). In all regions and seasons, however, O3-precursor emissions reductions of 20% in the NA source region decrease MDA8 O3 the most by a factor of 2 to nearly 10 relative to foreign emissions reductions. The O3 response to anthropogenic NA emissions is greatest in the Eastern US during summer at the high end of the O3 distribution (5-6 ppbv for 20% reductions). While the impact of foreign emissions on surface O3 in the US is not negligible and is of increasing concern given the growth in emissions upwind of the US - domestic emissions reductions remain a farmore effective means of decreasing MDA8 O3 values, particularly those above 75 ppb(the current US standard).JRC.H.2-Air and Climat

The Fire Modeling Intercomparison Project (FireMIP), phase 1: experimental and analytical protocols

The important role of fire in regulating vegetation community composition and contributions to emissions of greenhouse gases and aerosols make it a critical component of dynamic global vegetation models and Earth system models. Over two decades of development, a wide variety of model structures and mechanisms have been designed and incorporated into global fire models, which have been linked to different vegetation models. However, there has not yet been a systematic examination of how these different strategies contribute to model performance. Here we describe the structure of the first phase of the Fire Model Intercomparison Project (FireMIP), which for the first time seeks to systematically compare a number of models. By combining a standardized set of input data and model experiments with a rigorous comparison of model outputs to each other and to observations, we will improve the understanding of what drives vegetation fire, how it can best be simulated, and what new or improved observational data could allow better constraints on model behavior. Here we introduce the fire models used in the first phase of FireMIP, the simulation protocols applied, and the benchmarking system used to evaluate the models

A regional nuclear conflict would compromise global food security

A limited nuclear war between India and Pakistan could ignite fires large enough to emit more than 5 Tg of soot into the stratosphere. Climate model simulations have shown severe resulting climate perturbations with declines in global mean temperature by 1.8 °C and precipitation by 8%, for at least 5 y. Here we evaluate impacts for the global food system. Six harmonized state-of-the-art crop models show that global caloric production from maize, wheat, rice, and soybean falls by 13 (±1)%, 11 (±8)%, 3 (±5)%, and 17 (±2)% over 5 y. Total single-year losses of 12 (±4)% quadruple the largest observed historical anomaly and exceed impacts caused by historic droughts and volcanic eruptions. Colder temperatures drive losses more than changes in precipitation and solar radiation, leading to strongest impacts in temperate regions poleward of 30°N, including the United States, Europe, and China for 10 to 15 y. Integrated food trade network analyses show that domestic reserves and global trade can largely buffer the production anomaly in the first year. Persistent multiyear losses, however, would constrain domestic food availability and propagate to the Global South, especially to food-insecure countries. By year 5, maize and wheat availability would decrease by 13% globally and by more than 20% in 71 countries with a cumulative population of 1.3 billion people. In view of increasing instability in South Asia, this study shows that a regional conflict using <1% of the worldwide nuclear arsenal could have adverse consequences for global food security unmatched in modern history