scholarly journals Global atmospheric methane: budget, changes and dangers

2011 ◽  
Vol 369 (1943) ◽  
pp. 2058-2072 ◽  
Author(s):  
Edward J. Dlugokencky ◽  
Euan G. Nisbet ◽  
Rebecca Fisher ◽  
David Lowry
Keyword(s):  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
Emissions Trading ◽  
Mitigation Strategies ◽  
Anthropogenic Source ◽  
Atmospheric Methane ◽  
Emission Mitigation ◽  
Observation Network ◽  
Rate Of Increase ◽  
Isotopic Measurements

A factor of 2.5 increase in the global abundance of atmospheric methane (CH 4 ) since 1750 contributes 0.5 Wm −2 to total direct radiative forcing by long-lived greenhouse gases (2.77 Wm −2 in 2009), while its role in atmospheric chemistry adds another approximately 0.2 Wm −2 of indirect forcing. Since CH 4 has a relatively short lifetime and it is very close to a steady state, reductions in its emissions would quickly benefit climate. Sensible emission mitigation strategies require quantitative understanding of CH 4 ’s budget of emissions and sinks. Atmospheric observations of CH 4 abundance and its rate of increase, combined with an estimate of the CH 4 lifetime, constrain total global CH 4 emissions to between 500 and 600 Tg CH 4  yr −1 . While total global emissions are constrained reasonably well, estimates of emissions by source sector vary by up to a factor of 2. Current observation networks are suitable to constrain emissions at large scales (e.g. global) but not at the regional to national scales necessary to verify emission reductions under emissions trading schemes. Improved constraints on the global CH 4 budget and its break down of emissions by source sector and country will come from an enhanced observation network for CH 4 abundance and its isotopic composition ( δ 13 C, δ D (D= 2 H) and δ 14 C). Isotopic measurements are a valuable tool in distinguishing among various sources that contribute emissions to an air parcel, once fractionation by loss processes is accounted for. Isotopic measurements are especially useful at regional scales where signals are larger. Reducing emissions from many anthropogenic source sectors is cost-effective, but these gains may be cancelled, in part, by increasing emissions related to economic development in many parts of the world. An observation network that can quantitatively assess these changing emissions, both positive and negative, is required, especially in the context of emissions trading schemes.

scholarly journals Global sensitivity of aviation NO<sub>x</sub> effects to the HNO<sub>3</sub>-forming channel of the HO<sub>2</sub>+NO reaction

2012 ◽  
Vol 12 (9) ◽  
pp. 24287-24349
Author(s):  
K. Gottschaldt ◽  
C. Voigt ◽  
P. Jöckel ◽  
M. Righi ◽  
R. Deckert ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
Climate Model ◽  
Rate Coefficient ◽  
Climate Impact ◽  
Mitigation Strategies ◽  
Global Sensitivity ◽  
Mixing Ratios ◽  
Modelling Studies ◽  
The Impact

Abstract. The impact of a recently proposed HNO3-forming channel of the HO2+NO reaction (Butkovskaya et al., 2005, 2007) on atmospheric mixing ratios of ozone, methane and their precursors is assessed with a global stratosphere-troposphere chemistry-climate model. Previous modelling studies applied a rate coefficient that depends only on pressure and temperature. We additionally considered a possible enhancement of the reaction by humidity, as found by a laboratory study (Butkovskaya et al., 2009). This particularly reduces the oxidation capacity of the atmosphere, increasing methane lifetime significantly. The effects of aircraft NOx emissions on atmospheric chemistry are altered when considering the above reaction, resulting in a negative net radiative forcing relative to an atmosphere without aviation NOx. Uncertainties associated with the inclusion of the HO2+NO → HNO3 reaction and with its corresponding rate coefficient propagate a considerable additional uncertainty on estimates of the climate impact of aviation and on NOx-related mitigation strategies.

scholarly journals Influence of future air pollution mitigation strategies on total aerosol radiative forcing

2008 ◽  
Vol 8 (2) ◽  
pp. 5563-5627 ◽  
Author(s):  
S. Kloster ◽  
F. Dentener ◽  
J. Feichter ◽  
F. Raes ◽  
J. van Aardenne ◽  
...  
Keyword(s):  
Air Pollution ◽  
Radiative Forcing ◽  
Mitigation Strategies ◽  
Radiation Budget ◽  
Anthropogenic Source ◽  
Anthropogenic Aerosol ◽  
Aerosol Radiative Forcing ◽  
Aerosol Forcing ◽  
The Future ◽  
Aerosol Radiative

Abstract. We apply different aerosol and aerosol precursor emission scenarios reflecting possible future control strategies for air pollution in the ECHAM5-HAM model, and simulate the resulting effect on the Earth's radiation budget. We use two opposing future mitigation strategies for the year 2030: one in which emission reduction legislation decided in countries throughout the world are effectively implemented (current legislation; CLE 2030) and one in which all technical options for emission reductions are being implemented independent of their cost (maximum feasible reduction; MFR 2030). We consider the direct, semi-direct and indirect radiative effects of aerosols. The total anthropogenic aerosol radiative forcing defined as the difference in the top-of-the-atmosphere radiation between 2000 and pre-industrial times amounts to −2.05 W/m2. In the future this negative global annual mean aerosol radiative forcing will only slightly change (+0.02 W/m2) under the "current legislation" scenario. Regionally, the effects are much larger: e.g. over Eastern Europe radiative forcing would increase by +1.50 W/m2 because of successful aerosol reduction policies, whereas over South Asia it would decrease by −1.10 W/m2 because of further growth of emissions. A "maximum feasible reduction" of aerosols and their precursors would lead to an increase of the global annual mean aerosol radiative forcing by +1.13 W/m2. Hence, in the latter case, the present day negative anthropogenic aerosol forcing cloud be more than halved by 2030 because of aerosol reduction policies and climate change thereafter will be to a larger extend be controlled by greenhouse gas emissions. We combined these two opposing future mitigation strategies for a number of experiments focusing on different sectors and regions. In addition, we performed sensitivity studies to estimate the importance of future changes in oxidant concentrations and the importance of the aerosol microphysical coupling within the range of expected future changes. For changes in oxidant concentrations in the future within a realistic range, we do not find a significant effect for the global annual mean radiative aerosol forcing. In the extreme case of only abating SO2 or carbonaceous emissions to a maximum feasible extent, we find deviations from additivity for the radiative forcing over anthropogenic source regions up to 10% compared to an experiment abating both at the same time.

scholarly journals Regional and seasonal radiative forcing by perturbations to aerosol and ozone precursor emissions

2016 ◽  
Vol 16 (21) ◽  
pp. 13885-13910 ◽  
Author(s):  
Nicolas Bellouin ◽  
Laura Baker ◽  
Øivind Hodnebrog ◽  
Dirk Olivié ◽  
Ribu Cherian ◽  
...  
Keyword(s):  
Sulfur Dioxide ◽  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
General Circulation ◽  
Mitigation Strategies ◽  
Climate Mitigation ◽  
Radiative Forcings ◽  
Radiative Processes ◽  
Temperature And Precipitation ◽  
Near Term

Abstract. Predictions of temperature and precipitation responses to changes in the anthropogenic emissions of climate forcers require the quantification of the radiative forcing exerted by those changes. This task is particularly difficult for near-term climate forcers like aerosols, methane, and ozone precursors because their short atmospheric lifetimes cause regionally and temporally inhomogeneous radiative forcings. This study quantifies specific radiative forcing, defined as the radiative forcing per unit change in mass emitted, for eight near-term climate forcers as a function of their source regions and the season of emission by using dedicated simulations by four general circulation and chemistry-transport models. Although differences in the representation of atmospheric chemistry and radiative processes in different models impede the creation of a uniform dataset, four distinct findings can be highlighted. Firstly, specific radiative forcing for sulfur dioxide and organic carbon are stronger when aerosol–cloud interactions are taken into account. Secondly, there is a lack of agreement on the sign of the specific radiative forcing of volatile organic compound perturbations, suggesting they are better avoided in climate mitigation strategies. Thirdly, the strong seasonalities of the specific radiative forcing of most forcers allow strategies to minimise positive radiative forcing based on the timing of emissions. Finally, European and shipping emissions exert stronger aerosol specific radiative forcings compared to East Asia where the baseline is more polluted. This study can therefore form the basis for further refining climate mitigation options based on regional and seasonal controls on emissions. For example, reducing summertime emissions of black carbon and wintertime emissions of sulfur dioxide in the more polluted regions is a possible way to improve air quality without weakening the negative radiative forcing of aerosols.

scholarly journals 100 Years of Progress in Cloud Physics, Aerosols, and Aerosol Chemistry Research

2019 ◽  
Vol 59 ◽  
pp. 11.1-11.72 ◽  
Author(s):  
Sonia M. Kreidenweis ◽  
Markus Petters ◽  
Ulrike Lohmann
Keyword(s):  
Radiative Forcing ◽  
Cloud Microphysics ◽  
Climate System ◽  
Mitigation Strategies ◽  
Climate Projections ◽  
Weather Modification ◽  
Theoretical Understanding ◽  
Aerosol Cloud ◽  
Chemistry Research ◽  
Aerosol Cloud Interactions

Abstract This chapter reviews the history of the discovery of cloud nuclei and their impacts on cloud microphysics and the climate system. Pioneers including John Aitken, Sir John Mason, Hilding Köhler, Christian Junge, Sean Twomey, and Kenneth Whitby laid the foundations of the field. Through their contributions and those of many others, rapid progress has been made in the last 100 years in understanding the sources, evolution, and composition of the atmospheric aerosol, the interactions of particles with atmospheric water vapor, and cloud microphysical processes. Major breakthroughs in measurement capabilities and in theoretical understanding have elucidated the characteristics of cloud condensation nuclei and ice nucleating particles and the role these play in shaping cloud microphysical properties and the formation of precipitation. Despite these advances, not all their impacts on cloud formation and evolution have been resolved. The resulting radiative forcing on the climate system due to aerosol–cloud interactions remains an unacceptably large uncertainty in future climate projections. Process-level understanding of aerosol–cloud interactions remains insufficient to support technological mitigation strategies such as intentional weather modification or geoengineering to accelerating Earth-system-wide changes in temperature and weather patterns.

scholarly journals Investigation of water adsorption and hygroscopicity of atmospherically relevant particles using a commercial vapor sorption analyzer

2017 ◽  
Vol 10 (10) ◽  
pp. 3821-3832 ◽  
Author(s):  
Wenjun Gu ◽  
Yongjie Li ◽  
Jianxi Zhu ◽  
Xiaohong Jia ◽  
Qinhao Lin ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
Water Adsorption ◽  
Theoretical Data ◽  
Atmospheric Particles ◽  
Relative Mass ◽  
Nonspherical Particles ◽  
Vapor Sorption ◽  
Hygroscopic Growth ◽  
Dry Conditions

Abstract. Water adsorption and hygroscopicity are among the most important physicochemical properties of aerosol particles, largely determining their impacts on atmospheric chemistry, radiative forcing, and climate. Measurements of water adsorption and hygroscopicity of nonspherical particles under subsaturated conditions are nontrivial because many widely used techniques require the assumption of particle sphericity. In this work we describe a method to directly quantify water adsorption and mass hygroscopic growth of atmospheric particles for temperature in the range of 5–30 °C, using a commercial vapor sorption analyzer. A detailed description of instrumental configuration and experimental procedures, including relative humidity (RH) calibration, is provided first. It is then demonstrated that for (NH4)2SO4 and NaCl, deliquescence relative humidities and mass hygroscopic growth factors measured using this method show good agreements with experimental and/or theoretical data from literature. To illustrate its ability to measure water uptake by particles with low hygroscopicity, we used this instrument to investigate water adsorption by CaSO4 ⋅ 2H2O as a function of RH at 25 °C. The mass hygroscopic growth factor of CaSO4 ⋅ 2H2O at 95 % RH, relative to that under dry conditions (RH  < 1 %), was determined to be (0.450±0.004) % (1σ). In addition, it is shown that this instrument can reliably measure a relative mass change of 0.025 %. Overall, we have demonstrated that this commercial instrument provides a simple, sensitive, and robust method to investigate water adsorption and hygroscopicity of atmospheric particles.

scholarly journals Sensitivity of black carbon concentrations and climate impact to aging and scavenging

2016 ◽  
Author(s):  
Marianne T. Lund ◽  
Terje K. Berntsen ◽  
Bjørn H. Samset
Keyword(s):  
Nitric Acid ◽  
Black Carbon ◽  
Radiative Forcing ◽  
Mitigation Strategies ◽  
The Arctic ◽  
Climate Mitigation ◽  
Vertical Profiles ◽  
The Impact ◽  
Model Measurement ◽  
Global Mean

Abstract. Despite recent improvements, significant uncertainties in global modeling of black carbon (BC) aerosols persist, posing important challenges for the design and evaluation of effective climate mitigation strategies targeted at BC emission reductions. Here we investigate the sensitivity of BC concentrations in the chemistry-transport model OsloCTM2 with the microphysical aerosol parameterization M7 (OsloCTM2-M7) to parameters controlling aerosol aging and scavenging. We focus on Arctic surface concentrations and remote region BC vertical profiles, and introduce a novel treatment of condensation of nitric acid on BC. The OsloCTM2-M7 underestimates annual averaged BC surface concentrations, with a mean normalized bias of −0.55. The seasonal cycle and magnitude of Arctic BC surface concentrations is improved compared to previous OsloCTM2 studies, but model-measurement discrepancies during spring remain. High-altitude BC over the Pacific is overestimated compared with measurements from the HIPPO campaigns. We find that a shorter global BC lifetime improves the agreement with HIPPO, in line with other recent studies. Several processes can achieve this, including allowing for convective scavenging of hydrophobic BC and reducing the amount of soluble material required for aging. Simultaneously, the concentrations in the Arctic are reduced, resulting in poorer agreement with measurements in part of the region. A first step towards inclusion of aging by nitrate in OsloCTM2-M7 is made by allowing for condensation of nitric acid on BC. This results in a faster aging and reduced lifetime, and in turn to a better agreement with the HIPPO measurements. On the other hand, model-measurement discrepancies in the Arctic are exacerbated. Work to further improve this parameterization is needed. The impact on global mean radiative forcing (RF) and surface temperature response (TS) in our experiments is estimated. Compared to the baseline, decreases in global mean direct RF on the order of 10–30 % of the total pre-industrial to present BC direct RF is estimated for the experiments that result in the largest changes in BC concentrations. We show that globally tuning parameters related to BC aging and scavenging can improve the representation of BC vertical profiles in the OsloCTM2-M7 compared with observations. Our results also show that such improvements can result from changes in several processes and often depend on assumptions about uncertain parameters such as the BC ice nucleating efficiency and the change in hygroscopicity with aging. It is also important to be aware of potential tradeoffs in model performance between different regions. Other important sources of uncertainty, particularly for Arctic BC, such as model resolution has not been investigated here. Our results underline the importance of more observations and experimental data to improve process understanding and thus further constrain models.

scholarly journals Impact of uncertainties in inorganic chemical rate constants on tropospheric composition and ozone radiative forcing

2017 ◽  
Author(s):  
Ben Newsome ◽  
Mat Evans
Keyword(s):  
Rate Constant ◽  
Atmospheric Chemistry ◽  
Rate Constants ◽  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
Transport Model ◽  
Surface Ozone ◽  
Photolysis Rates ◽  
The Impact ◽  
Chemical Rate

Abstract. Chemical rate constants determine the composition of the atmosphere and how this composition has changed over time. They are central to our understanding of climate change and air quality degradation. Atmospheric chemistry models, whether online or offline, box, regional or global use these rate constants. Expert panels synthesise laboratory measurements, making recommendations for the rate constants that should be used. This results in very similar or identical rate constants being used by all models. The inherent uncertainties in these recommendations are, in general, therefore ignored. We explore the impact of these uncertainties on the composition of the troposphere using the GEOS-Chem chemistry transport model. Based on the JPL and IUPAC evaluations we assess 50 mainly inorganic rate constants and 10 photolysis rates, through simulations where we increase the rate of the reactions to the 1σ upper value recommended by the expert panels. We assess the impact on 4 standard metrics: annual mean tropospheric ozone burden, surface ozone and tropospheric OH concentrations, and tropospheric methane lifetime. Uncertainty in the rate constants for NO2 + OH    M →  HNO3, OH + CH4 → CH3O2 + H2O and O3 + NO → NO2 + O2 are the three largest source of uncertainty in these metrics. We investigate two methods of assessing these uncertainties, addition in quadrature and a Monte Carlo approach, and conclude they give similar outcomes. Combining the uncertainties across the 60 reactions, gives overall uncertainties on the annual mean tropospheric ozone burden, surface ozone and tropospheric OH concentrations, and tropospheric methane lifetime of 11, 12, 17 and 17 % respectively. These are larger than the spread between models in recent model inter-comparisons. Remote regions such as the tropics, poles, and upper troposphere are most uncertain. This chemical uncertainty is sufficiently large to suggest that rate constant uncertainty should be considered when model results disagree with measurement. Calculations for the pre-industrial allow a tropospheric ozone radiative forcing to be calculated of 0.412 ± 0.062 Wm−2. This uncertainty (15 %) is comparable to the inter-model spread in ozone radiative forcing found in previous model-model inter-comparison studies where the rate constants used in the models are all identical or very similar. Thus the uncertainty of tropospheric ozone radiative forcing should expanded to include this additional source of uncertainty. These rate constant uncertainties are significant and suggest that refinement of supposedly well known chemical rate constants should be considered alongside other improvements to enhance our understanding of atmospheric processes.

scholarly journals High-resolution glacial and deglacial record of atmospheric methane by continuous-flow and laser spectrometer analysis along the NEEM ice core

2013 ◽  
Vol 9 (6) ◽  
pp. 2579-2593 ◽  
Author(s):  
J. Chappellaz ◽  
C. Stowasser ◽  
T. Blunier ◽  
D. Baslev-Clausen ◽  
E. J. Brook ◽  
...  
Keyword(s):  
High Resolution ◽  
Continuous Flow ◽  
Ice Core ◽  
Rate Of Change ◽  
Atmospheric Methane ◽  
Data Set ◽  
Rate Of Increase ◽  
Concentration Changes ◽  
Cross Dating ◽  
Laser Spectroscopic

Abstract. The Greenland NEEM (North Greenland Eemian Ice Drilling) operation in 2010 provided the first opportunity to combine trace-gas measurements by laser spectroscopic instruments and continuous-flow analysis along a freshly drilled ice core in a field-based setting. We present the resulting atmospheric methane (CH4) record covering the time period from 107.7 to 9.5 ka b2k (thousand years before 2000 AD). Companion discrete CH4 measurements are required to transfer the laser spectroscopic data from a relative to an absolute scale. However, even on a relative scale, the high-resolution CH4 data set significantly improves our knowledge of past atmospheric methane concentration changes. New significant sub-millennial-scale features appear during interstadials and stadials, generally associated with similar changes in water isotopic ratios of the ice, a proxy for local temperature. In addition to the midpoint of Dansgaard–Oeschger (D/O) CH4 transitions usually used for cross-dating, sharp definition of the start and end of these events brings precise depth markers (with ±20 cm uncertainty) for further cross-dating with other palaeo- or ice core records, e.g. speleothems. The method also provides an estimate of CH4 rates of change. The onsets of D/O events in the methane signal show a more rapid rate of change than their endings. The rate of CH4 increase associated with the onsets of D/O events progressively declines from 1.7 to 0.6 ppbv yr−1 in the course of marine isotope stage 3. The largest observed rate of increase takes place at the onset of D/O event #21 and reaches 2.5 ppbv yr−1.

scholarly journals Sensitivity of aerosol radiative effects to different mixing assumptions in the AEROPT 1.0 submodel of the EMAC atmospheric-chemistry–climate model

2014 ◽  
Vol 7 (5) ◽  
pp. 2503-2516 ◽  
Author(s):  
K. Klingmüller ◽  
B. Steil ◽  
C. Brühl ◽  
H. Tost ◽  
J. Lelieveld
Keyword(s):  
Optical Properties ◽  
Radiative Transfer ◽  
Black Carbon ◽  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
Climate Model ◽  
Mixing Rule ◽  
Aerosol Optical Properties ◽  
Internal Mixing ◽  
Aerosol Radiative

Abstract. The modelling of aerosol radiative forcing is a major cause of uncertainty in the assessment of global and regional atmospheric energy budgets and climate change. One reason is the strong dependence of the aerosol optical properties on the mixing state of aerosol components, such as absorbing black carbon and, predominantly scattering sulfates. Using a new column version of the aerosol optical properties and radiative-transfer code of the ECHAM/MESSy atmospheric-chemistry–climate model (EMAC), we study the radiative transfer applying various mixing states. The aerosol optics code builds on the AEROPT (AERosol OPTical properties) submodel, which assumes homogeneous internal mixing utilising the volume average refractive index mixing rule. We have extended the submodel to additionally account for external mixing, partial external mixing and multilayered particles. Furthermore, we have implemented the volume average dielectric constant and Maxwell Garnett mixing rule. We performed regional case studies considering columns over China, India and Africa, corroborating much stronger absorption by internal than external mixtures. Well-mixed aerosol is a good approximation for particles with a black-carbon core, whereas particles with black carbon at the surface absorb significantly less. Based on a model simulation for the year 2005, we calculate that the global aerosol direct radiative forcing for homogeneous internal mixing differs from that for external mixing by about 0.5 W m−2.

scholarly journals A new radiation infrastructure for the Modular Earth Submodel System (MESSy, based on version 2.51)

2016 ◽  
Author(s):  
Simone Dietmüller ◽  
Patrick Jöckel ◽  
Holger Tost ◽  
Markus Kunze ◽  
Cathrin Gellhorn ◽  
...  
Keyword(s):  
Optical Properties ◽  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
General Circulation ◽  
Circulation Model ◽  
Shortwave Radiation ◽  
Aerosol Optical Properties ◽  
On Line ◽  
User Friendly ◽  
Radiation Scheme

Abstract. The Modular Earth Submodel System (MESSy) provides an interface to couple submodels to a basemodel via a highly flexible data management facility (Jöckel et al., 2010). In the present paper we present the four new radiation related submodels RAD, AEROPT, CLOUDOPT and ORBIT. The submodel RAD (with shortwave radiation scheme RAD_FUBRAD) simulates the radiative transfer, the submodel AEROPT calculates the aerosol optical properties, the submodel CLOUDOPT calculates the cloud optical properties, and the submodel ORBIT is responsible for Earth orbit calculations. These submodels are coupled via the standard MESSy infrastructure and are largely based on the original radiation scheme of the general circulation model ECHAM5, however, expanded with additional features. These features comprise, among others, user-friendly and flexibly controllable (by namelists) on-line radiative forcing calculations by multiple diagnostic calls of the radiation routines. With this, it is now possible to calculate radiative forcing (instantaneous as well as stratosphere adjusted) of various greenhouse gases simultaneously in only one simulation, as well as the radiative forcing of cloud perturbations. Examples of on-line radiative forcing calculations in the ECHAM/MESSy Atmospheric Chemistry (EMAC) model are presented.

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