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| Open AccessProposed energy-metabolisms cannot explain the atmospheric chemistry of Venus
The metabolisms proposed for hypothetical life in the clouds of Venus cannot explain the planet’s atmospheric chemistry and thus a limit can be placed on the maximum allowed biomass.
- Sean Jordan
- , Oliver Shorttle
- & Paul B. Rimmer
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| Open AccessUnexpected response of nitrogen deposition to nitrogen oxide controls and implications for land carbon sink
Recent vigorous controls in anthropogenic nitrogen oxide emissions in China cannot result in proportionate decreases in regional atmospheric nitrogen deposition. Enhanced atmospheric oxidizing capacity offsets those reductions of precursor emissions.
- Mingxu Liu
- , Fang Shang
- & Tong Zhu
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| Open AccessAmazonian terrestrial water balance inferred from satellite-observed water vapor isotopes
The evolution of the Amazon forest is tightly coupled to its terrestrial water balance. Here, the authors show that forest biomass changes in the Amazon are a driver of the spatiotemporal variation of evapotranspiration, and such changes could have a larger impact on water availability in the dry regions (southern, eastern) of the Amazon.
- Mingjie Shi
- , John R. Worden
- & Joshua B. Fisher
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| Open AccessNew seasonal pattern of pollution emerges from changing North American wildfires
Growing emissions from Pacific Northwest wildfires have increased atmospheric carbon monoxide in August, raising questions about potential health impacts as the seasonal pattern of air quality changes for large regions of North America.
- Rebecca R. Buchholz
- , Mijeong Park
- & Sheryl Magzamen
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| Open AccessProjected climate-driven changes in pollen emission season length and magnitude over the continental United States
Atmospheric conditions affect the release of anemophilous pollen. Zhang et al. use a pollen emission model together with future climate data to simulate changes in pollen emission. The study shows that climate change driven pollen increase and seasonal changes may increase seasonal allergies
- Yingxiao Zhang
- & Allison L. Steiner
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| Open AccessUptake of N2O5 by aqueous aerosol unveiled using chemically accurate many-body potentials
The reactive uptake of N2O5 to aqueous aerosol is a major loss channel for nitrogen oxides in the troposphere. Here authors report a theoretical investigation on the N2O5 uptake into aqueous aerosol and determine the hydrolysis rates by numerically solving a molecularly detailed reaction–diffusion equation.
- Vinícius Wilian D. Cruzeiro
- , Mirza Galib
- & Andreas W. Götz
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| Open AccessAbrupt emissions reductions during COVID-19 contributed to record summer rainfall in China
In the summer of 2020, China experienced record rainfall and flooding. Here, the authors investigate the connection between the rainfall and the abrupt decrease in emissions due to Covid-19 and find that the emission decrease may have contributed to the rainfall.
- Yang Yang
- , Lili Ren
- & Zhen-Qiang Zhou
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Article
| Open AccessEvidence for the oxidation of Earth’s crust from the evolution of manganese minerals
The co-evolution of oxygenation of the Earth’s atmosphere and lithosphere is still poorly constrained. However, the oxidation state of manganese minerals reveals that the redox state of Earth’s crust responds to changes in atmospheric oxygen following a ~66 million-year time lag.
- Daniel R. Hummer
- , Joshua J. Golden
- & Robert M. Hazen
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| Open AccessPhotodissociation of particulate nitrate as a source of daytime tropospheric Cl2
This study unravels an important daytime Cl2 source in the extra-polar atmosphere and shows that photolysis of particle nitrate at high acidity produced unprecedented levels of Cl2, boosting the oxidative power and air pollutants like O3.
- Xiang Peng
- , Tao Wang
- & Jianmin Chen
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| Open AccessPhotochemistry of the pyruvate anion produces CO2, CO, CH3–, CH3, and a low energy electron
Pyruvic acid and its conjugate base, the pyruvate anion, are largely present in the atmosphere. Here the authors, using photoelectron imaging and quantum chemistry calculations, investigate the photochemistry of isolated pyruvate anions initiated by UVA radiation and report the formation of CO2, CO, and CH3− further decomposing into CH3 and a free electron.
- Connor J. Clarke
- , Jemma A. Gibbard
- & Basile F. E. Curchod
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| Open AccessA bimodal distribution of haze in Pluto’s atmosphere
Pluto’s haze is revealed to have two types of particles: small spherical organic haze particles and micron-size fluffy aggregates. The persistence of these two populations has important implications for haze formation and properties on icy worlds.
- Siteng Fan
- , Peter Gao
- & Yuk L. Yung
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| Open AccessSecondary organic aerosol association with cardiorespiratory disease mortality in the United States
Fine particle air pollution causes premature death, but the role of different fine particle components in mortality is not well characterized. Here, the authors show the secondary organic aerosol component of fine particle mass is associated with significant cardiorespiratory mortality in the U.S.
- Havala O. T. Pye
- , Cavin K. Ward-Caviness
- & Karl M. Seltzer
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| Open AccessRapid increase in dichloromethane emissions from China inferred through atmospheric observations
Dichloromethane (CH2Cl2) is an unregulated ozone depleting substance whose emissions have strongly increased in recent years. Here, the authors show that rising emissions of dichloromethane in China between 2011 and 2019 can explain much of this global increase.
- Minde An
- , Luke M. Western
- & Matthew Rigby
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| Open AccessOptical emissions associated with narrow bipolar events from thunderstorm clouds penetrating into the stratosphere
Strong thunderstorms can reach the lower stratosphere and produce cloud-top blue emissions, affecting the exchange of greenhouse gases between the troposphere and stratosphere. Here, the authors reveal the direct link of blue emissions with the radio signals of one sort of intra-cloud discharges called NBEs.
- Feifan Liu
- , Gaopeng Lu
- & Baoyou Zhu
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| Open AccessMitigation potential of global ammonia emissions and related health impacts in the trade network
Ammonia emissions from agricultural sources can cause severe health impacts. Here, the authors show that about 25% of global agricultural ammonia emissions in 2012 were related to international exported goods and caused 61 thousand PM2.5 related premature deaths, which points out large ammonia mitigation potential in international trade.
- Rong Ma
- , Ke Li
- & Jing Meng
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| Open AccessAerosol-boundary-layer-monsoon interactions amplify semi-direct effect of biomass smoke on low cloud formation in Southeast Asia
Biomass burning emissions have been shown to influence clouds in the Atlantic, but its influence in other regions is not well known. Here, the authors show that biomass burning aerosols increase the low-cloud cover over subtropical southeastern Asia by a similar magnitude than over the Atlantic.
- Ke Ding
- , Xin Huang
- & Meinrat O. Andreae
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| Open AccessAntarctic ozone hole modifies iodine geochemistry on the Antarctic Plateau
The Antarctic ozone hole has had far-reaching impacts, but effects on geochemical cycles in polar regions is still unknown. Iodine records from the interior of Antarctica provide evidence for human alteration of the natural geochemical cycle of this essential element.
- Andrea Spolaor
- , François Burgay
- & Alfonso Saiz-Lopez
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| Open AccessSignificance of the organic aerosol driven climate feedback in the boreal area
Vegetation emits organic vapors which can form aerosols in the atmosphere and influence cloud properties. Here, the authors show observational evidence that warmer temperatures lead to increased emissions of these aerosols in boreal forests which cause surface cooling, demonstrating a negative climate feedback mechanism.
- Taina Yli-Juuti
- , Tero Mielonen
- & Annele Virtanen
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| Open AccessDiel cycle of sea spray aerosol concentration
Sea spray aerosol (SSA) are an important way through which oceans can influence the atmosphere’s radiative properties. Here, the authors present measurements taken over a 42,000 km ship cruise in the Atlantic and Pacific Ocean and show that SSA number concentrations vary over a 24-hour cycle, possibly linked to surface water bubble-bursting dynamics.
- J. Michel Flores
- , Guillaume Bourdin
- & Ilan Koren
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| Open AccessCO2, nitrogen deposition and a discontinuous climate response drive water use efficiency in global forests
Water use efficiency is a key measure of plant responses to climate change. Here, the authors investigate its control by CO2, nitrogen deposition, and water availability using a global tree-ring dataset. They find an aridity threshold and quantify changes in control over the past 50 years.
- Mark A. Adams
- , Thomas N. Buckley
- & Tarryn L. Turnbull
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| Open AccessFire-derived phosphorus fertilization of African tropical forests
Nowhere is biomass burning more abundant than on the African continent, but the biogeochemical impacts on forests are poorly understood. Here the authors show that biomass burning leads to high phosphorus deposition in the Congo basin, which scales with forest age as a result of increasing canopy complexity.
- Marijn Bauters
- , Travis W. Drake
- & Pascal Boeckx
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| Open AccessThe underappreciated role of agricultural soil nitrogen oxide emissions in ozone pollution regulation in North China
Summertime ozone air pollution in North China remains severe. Here the authors find large biogenic emissions of nitrogen oxides in North China, mainly driven by fertilizer application, challenge the mitigation of ozone pollution by only reducing combustion induced ozone precursors’ emissions.
- Xiao Lu
- , Xingpei Ye
- & Yuanhang Zhang
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| Open AccessClimate change modulates the stratospheric volcanic sulfate aerosol lifecycle and radiative forcing from tropical eruptions
How climate change influences the lifecycle of stratospheric volcanic aerosols and the associated radiative forcing is unknown. Here, the authors present model experiments suggesting that climate change amplifies the forcing of large-magnitude tropical eruptions but reduces the forcing of moderate-magnitude tropical eruptions.
- Thomas J. Aubry
- , John Staunton-Sykes
- & Anja Schmidt
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| Open AccessThe Great Oxygenation Event as a consequence of ecological dynamics modulated by planetary change
The Great Oxygenation Event (GOE) 2.4 billion years ago is believed to have been critical for the evolution of complex life. Here, Olejarz et al. propose a model suggesting that competition between major bacterial groups could have triggered the GOE in a feedback loop with geophysical processes.
- Jason Olejarz
- , Yoh Iwasa
- & Martin A. Nowak
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| Open AccessClimate change favours large seasonal loss of Arctic ozone
Despite a ban on ozone depleting substances, ozone depletion during cold winters in the Arctic stratosphere has been increasing in recent decades. Here, the authors show conditions favourable for Arctic ozone depletion could worsen as a response of stratospheric temperature and water to continued release of greenhouse gases.
- Peter von der Gathen
- , Rigel Kivi
- & Markus Rex
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| Open AccessJoint inference of CFC lifetimes and banks suggests previously unidentified emissions
The production of chlorofluorocarbons (CFC) was phased-out under the Montreal, but renewed emissions of CFC-11 have been reported recently. Here, the authors present a joint analysis of multiple factors and find that emissions of CFC-11, but also CFC-12 and CFC-113 are higher than expected, indicating renewed emissions.
- Megan Lickley
- , Sarah Fletcher
- & Susan Solomon
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| Open AccessElectron donation of non-oxide supports boosts O2 activation on nano-platinum catalysts
Activation of O2 is a critical step in heterogeneous catalytic oxidation. Here, the authors adopt the concept of increased electron donors induced by nitrogen vacancy to develop an efficient strategy for preparing highly active and stable catalysts for molecular O2 activation.
- Tao Gan
- , Jingxiu Yang
- & Gang Liu
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| Open AccessSulfate formation is dominated by manganese-catalyzed oxidation of SO2 on aerosol surfaces during haze events
Sulfate aerosols are an important component of wintertime haze events in China, but their production mechanisms are not well known. Here, the authors show that transition metal-catalyzed oxidation of SO2 on aerosol surfaces could be the dominant sulfate formation pathway in Northern China.
- Weigang Wang
- , Mingyuan Liu
- & Maofa Ge
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| Open AccessPhotolytic radical persistence due to anoxia in viscous aerosol particles
Sunlight can change the composition of atmospheric aerosol particles, but the mechanisms through which this happens are not well known. Here, the authors show that fast radical reaction and slow diffusion near viscous organic particle surfaces can cause oxygen depletion, radical trapping and humidity dependent oxidation.
- Peter A. Alpert
- , Jing Dou
- & Markus Ammann
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| Open AccessMolecular mechanism for rapid autoxidation in α-pinene ozonolysis
Oxidation of volatile organic compounds leads to aerosol formation in the atmosphere, but the mechanism of some fast reactions is still unclear. The authors, using quantum chemical modelling and experiments, reveal that in key monoterpenes the cyclobutyl ring that would hinder the reactivity is broken in the early exothermic steps of the reaction.
- Siddharth Iyer
- , Matti P. Rissanen
- & Theo Kurtén
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| Open AccessGreater fuel efficiency is potentially preferable to reducing NOx emissions for aviation’s climate impacts
The regulation of aircraft engine NOx emissions was introduced to improve local air quality and reduce NOx emissions at altitude. Here, the authors find that greater fuel efficiency of aircrafts, and therefore lower CO2 emissions, could be preferable to reducing NOx emissions in terms of the aviation industries future climate impacts.
- Agnieszka Skowron
- , David S. Lee
- & Bethan Owen
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| Open AccessStructures and reactivity of peroxy radicals and dimeric products revealed by online tandem mass spectrometry
Organic peroxy radicals play a pivotal role in producing highly oxygenated organic molecules but the formation mechanisms remain elusive. Here, the authors show in-situ characterization of peroxy radicals and dimer structures in the gas-phase, using online tandem mass spectrometry analyses.
- Sophie Tomaz
- , Dongyu Wang
- & Matthieu Riva
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| Open AccessBiomass burning aerosols in most climate models are too absorbing
Wildfires produce aerosols known to impact the climate, but the wider-reaching effects of this biomass burning are poorly constrained in models. Here the authors use a suite of observations from 12 campaigns around the globe to determine that the values used by most climate models overestimate the contribution of biomass burning aerosols.
- Hunter Brown
- , Xiaohong Liu
- & Duli Chand
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| Open AccessSulfur monoxide dimer chemistry as a possible source of polysulfur in the upper atmosphere of Venus
Photochemistry of sulfur species in the upper Venus atmosphere is not well understood and the identity of ultraviolet (UV) absorber(s) remain unknown. Here, the authors show that sulfur monoxide dimer chemistry is a possible source of polysulfur, which could be responsible for the UV absorption.
- Joseph P. Pinto
- , Jiazheng Li
- & Yuk L. Yung
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| Open AccessCarbonate-silicate cycle predictions of Earth-like planetary climates and testing the habitable zone concept
In the habitable zone concept, a planet’s carbon dioxide-water greenhouse maintains surface liquid water. Here, the authors estimate how many Earthlike exoplanets are needed to detect a relationship between stellar flux and the atmospheric carbon dioxide predicted by carbon cycle modeling.
- Owen R. Lehmer
- , David C. Catling
- & Joshua Krissansen-Totton
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| Open AccessA biogenic secondary organic aerosol source of cirrus ice nucleating particles
Ice nucleating particles impact the global climate by altering cloud formation and properties, but the sources of these emissions are not completely characterized. Here, the authors show that secondary organic aerosols formed from the oxidation of organic gases in the atmosphere can be a source of ice nucleating particles.
- Martin J. Wolf
- , Yue Zhang
- & Daniel J. Cziczo
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| Open AccessFrequent new particle formation over the high Arctic pack ice by enhanced iodine emissions
Which vapors are responsible for new particle formation in the Arctic is largely unknown. Here, the authors show that the formation of new particles at the central Arctic Ocean is mainly driven by iodic acid and that particles smaller than 30 nm in diameter can activate as cloud condensation nuclei.
- Andrea Baccarini
- , Linn Karlsson
- & Julia Schmale
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| Open AccessMethane emissions from natural gas vehicles in China
The methane emissions from natural gas vehicles (NGVs) are unclear. Here the authors report high methane emissions from heavy-duty NGVs, and by using a scenario analysis show that strictly implementing the upcoming China VI standard could reduce GHG emissions by 509 Mt CO2eq for 2020-2030.
- Da Pan
- , Lei Tao
- & Mark A. Zondlo
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| Open AccessPersisting volcanic ash particles impact stratospheric SO2 lifetime and aerosol optical properties
Volcanic ash is often neglected in climate simulations as it is assumed to have a short atmospheric lifetime. Here, the authors show a persistent super-micron ash layer after the Mt. Kelut eruption in 2014 that impacts the stratospheric sulfur burden and chemistry for over the first months after the eruption.
- Yunqian Zhu
- , Owen B. Toon
- & Sarah Woods
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| Open AccessA gas-to-particle conversion mechanism helps to explain atmospheric particle formation through clustering of iodine oxides
“How iodine-bearing molecules contribute to atmospheric aerosol formation is not well understood. Here, the authors provide a new gas-to-particle conversion mechanism and show that clustering of iodine oxides is an essential component of this process while previously proposed iodic acid does not play a large role.”
- Juan Carlos Gómez Martín
- , Thomas R. Lewis
- & Alfonso Saiz-Lopez
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Article
| Open AccessExposure to air pollution and scarlet fever resurgence in China: a six-year surveillance study
The reason for a re-emergence of scarlet fever in China remains unclear. Here the authors show that the number of scarlet fever cases surged in 2011 peaking in 2018, this correlates with an increase in NO2 and O3 but does not necessarily imply causation.
- Yonghong Liu
- , Hui Ding
- & Shelan Liu
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Article
| Open AccessA scalable method for preparing Cu electrocatalysts that convert CO2 into C2+ products
Selective reduction of carbon dioxide to high-value products is key for advancing carbon capture and utilization technologies. Here the authors prepare a copper catalyst for electrocatalytic conversion of carbon dioxide to C2+ products with enhanced selectivity that is attributed to a high density of surface defects.
- Taehee Kim
- & G. Tayhas R. Palmore
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Article
| Open AccessNon-natural ruthenium isotope ratios of the undeclared 2017 atmospheric release consistent with civilian nuclear activities
A cloud of enhanced ruthenium concentrations has been observed over Europe in 2017, but no country has acknowledged responsibility for this nuclear release. Here, the authors show that the stable isotopic composition of ruthenium emitted from nuclear fuel reprocessing during the 2017 event is consistent with the isotopic signature of civilian Russian nuclear reactor fuel.
- Timo Hopp
- , Dorian Zok
- & Georg Steinhauser
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Article
| Open AccessFast sulfate formation from oxidation of SO2 by NO2 and HONO observed in Beijing haze
How sulfur dioxide emitted through coal combustion is oxidized to sulfate particles during winter haze pollution events has been the subject of debate. Here, the authors show that rapid oxidation takes place by nitrogen dioxide and nitrous acid, producing nitrous oxide together with sulfate.
- Junfeng Wang
- , Jingyi Li
- & Daniel J. Jacob
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Article
| Open AccessQuantifying contributions of chlorofluorocarbon banks to emissions and impacts on the ozone layer and climate
Following international agreements, the use of chlorofluorocarbons in production is supposed to be phased out. Here, the authors present a new estimate of these products already in use and their emissions and show that they are larger than expected and that not recovering these banks leads to a substantial delay in the polar ozone hole recovery.
- Megan Lickley
- , Susan Solomon
- & Kane Stone
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Article
| Open AccessThe Red Sea Deep Water is a potent source of atmospheric ethane and propane
The Middle East is known to emit large amounts of non-methane hydrocarbon pollutants to the atmosphere, but the sources are poorly characterized. Here the authors discover a new source—deep water in the Red Sea—and calculate that its emissions exceed rates of several high gas-production countries.
- E. Bourtsoukidis
- , A. Pozzer
- & J. Williams
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| Open AccessIncrease in global emissions of HFC-23 despite near-total expected reductions
International agreements have been implemented to reduce emissions of hydrofluorocarbons (HFCs) to reduce their radiative forcing. Even though reported HFC-23 emissions are at a historical low, observations indicate that emissions have actually increased over recent years to higher levels than previously.
- K. M. Stanley
- , D. Say
- & M. Rigby
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Article
| Open AccessDelay in recovery of the Antarctic ozone hole from unexpected CFC-11 emissions
The Antarctic ozone hole is decreasing in size due to policies implemented following the Montreal Protocol. Here, model simulations show that if recently discovered increase in unreported CFC-11 emissions continue, they could delay the recovery of the ozone hole by well over a decade.
- S. S. Dhomse
- , W. Feng
- & M. P. Chipperfield
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| Open AccessKey drivers of cloud response to surface-active organics
Aerosol-cloud interactions are a large source of uncertainty in radiative forcing estimates. Here, the authors show that the radiative effects of clouds are influenced by a combination of aerosol particle distribution, environmental conditions and atmosphere dynamics.
- S. J. Lowe
- , D. G. Partridge
- & I. Riipinen