Opinion: Coordinated Development of Emission Inventories for Climate Forcers and Air Pollutants

Emissions into the atmosphere of fine particulates, their precursors, and precursors to tropospheric ozone, not only impact human health and ecosystems, but also impact the climate by altering Earth’s radiative balance. Accurately quantifying these impacts across local to global scales, historically, and in future scenarios, requires emission inventories that are accurate, transparent, complete, comparable, and consistent. In an effort to better quantify the emissions and impacts of these pollutants, also called short-lived climate forcers (SLCFs), the Intergovernmental Panel on Climate Change (IPCC) is developing a new SLCF emissions methodology report. This report would supplement existing IPCC reporting guidance on greenhouse gas (GHG) emissions inventories, currently used by inventory compilers to fulfill national reporting requirements under the United Nations Framework Convention on Climate Change (UNFCCC) and new requirements of the Enhanced Transparency Framework (ETF) under the Paris Agreement starting in 2024. We review the relevant issues, including how air pollutant and GHG inventory activities have historically been structured, as well as potential benefits, challenges, and recommendations for coordinating GHG and air pollutant inventory efforts. We argue that while there are potential benefits to increasing coordination between air pollutant and GHG inventory development efforts, we also caution that there are differences in appropriate methodologies and applications that must jointly be considered.

Modelling SO₂ conversion into sulphates in the mid-troposphere with a 3D chemistry-transport model: the case of Mount Etna's eruption on April 12, 2012

Volcanic activity is an important source of atmospheric sulphur dioxide (SO2), which, after conversion into sulphuric acid, induces impacts on, among others, rain acidity, human health, meteorology and the radiative balance of the atmosphere. This work focuses on the conversion of SO2 into sulphates (, S(+VI)) in the mid-tropospheric volcanic plume emitted by the explosive eruption of Mount Etna (Italy) on Apr. 12, 2012, using the CHIMERE chemistry-transport model. Since volcanic plume location and composition depend on several often poorly constrained parameters, using a chemistry-transport model allows us to study the sensitivity of SO2 oxidation to multiple aspects such as volcanic water emissions, transition metal emissions, plume diffusion and plume altitude. Our results show that in the mid-troposphere, two pathways contribute to sulphate production, the oxidation of SO2 by OH in the gaseous phase (70 %), and the aqueous oxidation by O2 catalyzed by Mn2+ and Fe3+ ions (25 %). The oxidation in aqueous phase is the faster process, but in the mid-troposphere, liquid water is scarce, therefore the relative share of gaseous oxidation can be important. After one day in the mid-troposphere, about 0.5 % of the volcanic SO2 was converted to sulphates through the gaseous process. Because of the nonlinear dependency of the kinetics in the aqueous phase to the amount of volcanic water emitted and on the availability of transition metals in the aqueous phase, several experiments have been designed to determine the prominence of different parameters. Our simulations show that during the short time that liquid water remains in the plume, around 0.4 % of sulphates manage to quickly enter the liquid phase. Sensitivity tests regarding the advection scheme have shown that this scheme must be chosen wisely, as dispersion will impact both oxidation pathways explained above.

Global Climate Change by Wetland Greenhouse Gas Fluxes

Wetlands (WLs) in the landscapes are important for the GHGs production, ingesting, and exchange with the atmosphere. In this chapter, the authors illustrated how the WLs influence climate change, even though it is typical for determining the climatic role of WLs in the broader perspective. The conclusions might be wary based on the radiative balance as the radiative forcing since the 1750s or climatic roles are continuously changing in the wetlands. Degradation of WLs leads to reducing their functioning, and GHG fluxes might change and alter the climatic roles of the WLs. The chapter demonstrated that WL disturbances might cause global warming for a longer duration even though the WLs are restored or managed by replacing them with the mitigation WLs. Thus, activities that cause disturbance in the WLs leading to carbon oxidation in the soils should be avoided. Regulating the climate is an ecosystem service in the WLs; during the planning of the WLs, protection, restoration, and creation, environmental management should be considered.

Arctic fog chemistry induces the unexpected growth of Aitken mode particles to CCN-active particles

<p>New particle formation (NPF) and early growth are efficient processes producing high concentrations of cloud condensation nuclei (CCNs) precursors in the Arctic marine boundary layer (AMBL). However, due to short lifetime and lack of condensable vapors, newly formed particles do often not grow beyond 50 nm and cause low CCN particle concentrations in the AMBL. Thus, even the smallest amount of Aitken mode particle growth is capable to significantly increase the CCN budget. However, the growth mechanism of Aitken-mode particles from NPF into CCN range in the Arctic is still rather unclear and was therefore investigated during the cruise campaign PASCAL in 2017.</p> <p>During PASCAL, aerosol particles measurements were performed and an unexpected rapid growth of Aitken mode particles was observed right after fog episodes. Combined field data analyses and detailed multiphase chemistry box model simulations with the CAPRAM mechanism were performed to study the underlying processes. Resulting, a new mechanism is proposed explaining how particles with d < 50 nm are able to grow into CCN size range in the Arctic without requiring high water vapor supersaturation (SS). The investigations demonstrated that the rapid post-fog particle growth of Aitken mode is related to chemical processes within the Arctic fog. The redistribution of semi-volatile acidic (e.g., methanesulfonic acid) and basic (e.g., ammonia) compounds from processed CCN-active particles to smaller CCN-inactive particles can cause a rapid particle growth of Aitken mode particles after fog evaporation enabling them to grow towards CCN size. Comparisons of the model results with Berner impactor measurements supports the proposed growth mechanism.</p> <p>Overall, this study provided new insights on how the increasing frequency of NPF and fog-related particle processing can increase in the number of CCNs and cloud droplets leading to an increased albedo of Arctic clouds and thus affect the radiative balance in the Arctic. Since fogs will occur more frequently in the Arctic as a result of climate change, this growth mechanism and a deeper knowledge on its feedbacks can be essential to understand Arctic warming.</p>

An experimental study of the reactivity of terpinolene and β-caryophyllene with the nitrate radical

Biogenic volatile organic compounds (BVOCs) are subject to an intense emission by forests and crops into the atmosphere. They can rapidly react with the nitrate radical (NO3) during nighttime to form number of functionalized products. Among them, organic nitrates (ON) have been shown to behave as reservoirs of reactive nitrogen and consequently influence the ozone budget and secondary organic aerosols (SOA) which are known to have a direct and indirect effect on the radiative balance, and thus on climate. Nevertheless, BVOCs + NO3 reactions remain poorly understood. Thus, the primary purpose of the follow-up study is to furnish new kinetic and mechanistic data for one monoterpenes (C10H16), terpinolene, and one sesquiterpene (C15H24), β-caryophyllene, using simulation chamber experiments. These two compounds have been chosen in order to fill the lack of experimental data. Rate constants have been measured using both relative and absolute methods. They have been measured to be (5.5 ± 3.8) × 10−11 and (1.7 ± 1.4) × 10−11 cm3 molecule−1 s−1 for terpinolene and β-caryophyllene respectively. Mechanistic studies have also been conducted in order to identify and quantify the main reaction products. Total organic nitrates and SOA yields have been determined. Both terpenes appear to be major ON precursors both in gas and particle phase with formation yields of 69 % for terpinolene and 79 % for β-caryophyllene respectively. They also are major SOA precursor, with maximum SOA yields of around 60 % for both of the compounds. In order to support these observations, chemical analyses of the gas phase products were performed at the molecular scale using PTR-TOF-MS and FTIR. Detected products allowed proposing chemical mechanisms and providing explanations through peroxy and alkoxy reaction pathways.

Spectropolarimetry as a tool for understanding the diversity of planetary atmospheres

The polarization state of starlight reflected by a planetary atmosphere uniquely reveals coverage, particle size, and composition of aerosols as well as changing cloud patterns. It is not possible to obtain a comparable level of detail from flux-only observations. It is therefore a powerful tool to better understand the crucial role played by clouds and aerosols in the chemistry, dynamics, and radiative balance of a planet. Furthermore, polarization observations can probe the atmosphere of planets independently of the orbital geometry (hence it applies to both transiting and non-transiting exoplanets). A high-resolution spectropolarimeter with a broad wavelength coverage, particularly if attached to a large space telescope, would enable simultaneous study of the polarimetric planetary properties of the continuum and to look for and characterize the polarimetric signal due to scattering from single molecules, providing detailed information about the composition and vertical structure of the atmosphere.

Structure of the Western Tibetan Vortex inconsistent with a thermally-direct circulation

The Western Tibetan Vortex (WTV) is a large-scale circulation pattern identified from year-to-year circulation variability, which was used to understand the causal mechanisms for slowdown of the glacier melting over the western Tibetan Plateau (TP). A recent argument has suggested the WTV is the set of wind field anomalies resulting from variability in near-surface air temperatures over the western TP (above 1500 m), which, in turn, is likely driven by the surface net radiation. This study thereby evaluates the above putative thermal-direct mechanism. By conducting numerical sensitivity experiments using a global atmospheric circulation model, SAMIL, we find a WTV-like structure cannot be generated from a surface thermal forcing imposed on the western TP. A thermally-direct circulation generated by the surface or near surface heating is expect to cause upward motions and a baroclinic structure above it. In contrast, downward motions and a quasi-barotropic are observed in the vertical structure of the WTV. Besides, we find variability of the surface net radiation (sum of the surface shortwave and longwave net radiation) over the western TP can be traced back to the WTV variability based on ERA5 data. The anticyclonic (cyclonic) WTV reduces (increases) the cloudiness through the anomalous downward (upward) motions, causes more (less) input shortwave net radiation and thereby more (less) surface net radiations, resulting in the warmer (cooler) surface and near-surface air temperature over the western TP. The argument is constructive in encouraging examination of the radiative balance processes that complements previous studies.

Transport of Water Vapor from Tropical Cyclones to the Upper Troposphere

This paper investigates the influence of tropical cyclones on water vapor concentrations in the upper atmosphere above these storms. We use independent data sets of tropical storm intensity, water vapor and lightning activity to investigate this relationship. Water vapor in the upper troposphere is a key greenhouse gas, with direct impacts on surface temperatures. Both the amount and altitude of water vapor impact the radiative balance and the greenhouse effect of the atmosphere. The water vapor enters the upper troposphere through deep convective storms, often associated with lightning activity. The intensity of the lightning activity represents the intensity of the convection in these storms, and hence the amount of water vapor transported aloft. In this paper, we investigate the role of tropical cyclones on the contribution of water vapor to the upper atmosphere moistening. Tropical cyclones are the largest most intense storms on Earth and can last for up to two weeks at a time. There is also evidence that the intensity of tropical cyclones is increasing, and will continue to increase, due to global warming. In this study we find that the maximum moistening of the upper atmosphere occurs at the 200 hPa level (~12 km altitude), with a lag of 1–2 days after the maximum sustained winds in the tropical cyclone. While the water vapor peaks after the maximum of the storm intensity, the lightning activity peaks before the maximum intensity of the storms, as shown previously. We show here that the absolute amount of water vapor in the upper troposphere above tropical storms increases linearly with the intensity of the storms. For every 10 hPa decrease in the minimum pressure of tropical storms, the specific humidity increases around 0.2 g/kg at the 200 hPa level.

Universal calculation method for optical reflection characteristics of dihedral reflector with lambert surfaces as per radiative balance method

Object and purpose of research. This paper discusses the ways to improve current calculation method for reflection parameters during remote laser detection and ranging by means of a dihedral reflector with Lambert surfaces equal to reflection coefficients of each surface as per the generalized method of radiative balance. The study also discusses the evolution of optical methods and analytical research tools in this domain, as well as laser signature calculation for various ships and other structures. Materials and methods. Analytical calculation methods, software, calculation methods for remote laser detection and ranging taking into account optical parameters and reflection coefficient of dihedral reflectors used to calculate laser signature of ship structures. Main results. Improved efficiency and accuracy of calculation methods for laser detection and ranging with respect to dihedral reflectors for surface ships. Conclusion. Calculation methods of remote laser detection and ranging suggested in this paper offer additional capabilities in lidar signature measurements of ships and other structures.