Atmospheric aerosols exert an important influence on climate through their effects on stratiform cloud albedo and lifetime and the invigoration of convective storms. Model calculations suggest that almost half of the global cloud condensation nuclei in the atmospheric boundary layer may originate from the nucleation of aerosols from trace condensable vapours, although the sensitivity of the number of cloud condensation nuclei to changes of nucleation rate may be small. Despite extensive research, fundamental questions remain about the nucleation rate of sulphuric acid particles and the mechanisms responsible, including the roles of galactic cosmic rays and other chemical species such as ammonia. Here we present the first results from the CLOUD experiment at CERN. We find that atmospherically relevant ammonia mixing ratios of 100 parts per trillion by volume, or less, increase the nucleation rate of sulphuric acid particles more than 100–1,000-fold. Time-resolved molecular measurements reveal that nucleation proceeds by a base-stabilization mechanism involving the stepwise accretion of ammonia molecules. Ions increase the nucleation rate by an additional factor of between two and more than ten at ground-level galactic-cosmic-ray intensities, provided that the nucleation rate lies below the limiting ion-pair production rate. We find that ion-induced binary nucleation of H_(2)SO_(4)–H_(2)O can occur in the mid-troposphere but is negligible in the boundary layer. However, even with the large enhancements in rate due to ammonia and ions, atmospheric concentrations of ammonia and sulphuric acid are insufficient to account for observed boundary-layer nucleation.

/pdf/role-of-sulphuric-acid-ammonia-and-galactic-cosmic-rays-in-3k8is82upm.pdf

Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleation

The development of this
review article has evolved from work carried out by an international
team of the International Space Science Institute (ISSI),
Bern, Switzerland, and from work carried out under the auspices
of Scientific Committee on Solar Terrestrial Physics (SCOSTEP)
Climate and Weather of the Sun‐Earth System (CAWSES‐1).
The support of ISSI in providing workshop and meeting facilities
is acknowledged, especially support from Y. Calisesi and V. Manno.
SCOSTEP is acknowledged for kindly providing financial assistance
to allow the paper to be published under an open access
policy. L.J.G. was supported by the UK Natural Environment
Research Council (NERC) through their National Centre for Atmospheric
Research (NCAS) Climate program. K.M. was supported
by a Marie Curie International Outgoing Fellowship within the
6th European Community Framework Programme. J.L. acknowledges
support by the EU/FP7 program Assessing Climate Impacts
on the Quantity and Quality of Water (ACQWA, 212250) and from
the DFG Project Precipitation in the Past Millennium in Europe
(PRIME) within the Priority Program INTERDYNAMIK. L.H.
acknowledges support from the U.S. NASA Living With a Star
program. G.M. acknowledges support from the Office of Science
(BER), U.S. Department of Energy, Cooperative Agreement
DE‐FC02‐97ER62402, and the National Science Foundation. We
also wish to thank Karin Labitzke and Markus Kunze for supplying
an updated Figure 13, Andrew Heaps for technical support, and
Paul Dickinson for editorial support. Part of the research was
carried out under the SPP CAWSES funded by GFG. J.B. was
financially supported by NCCR Climate–Swiss Climate Research.

/pdf/solar-influences-on-climate-48ynhy9kuz.pdf

Solar influences on climate

Nucleation and Growth of Nanoparticles in the Atmosphere Renyi Zhang,* Alexei Khalizov, Lin Wang, Min Hu, and Wen Xu Department of Atmospheric Sciences andDepartment of Chemistry, Center for Atmospheric Chemistry and Environment, Texas A&M University, College Station, Texas 77843, United States Department of Environmental Science & Engineering and Institute of Global Environment Change Research, Fudan University, Shanghai 200433, China State Key Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing, 100871, China

Nucleation and Growth of Nanoparticles in the Atmosphere

About half of present-day cloud condensation nuclei originate from atmospheric nucleation, frequently appearing as a burst of new particles near midday. Atmospheric observations show that the growth rate of new particles often accelerates when the diameter of the particles is between one and ten nanometres. In this critical size range, new particles are most likely to be lost by coagulation with pre-existing particles, thereby failing to form new cloud condensation nuclei that are typically 50 to 100 nanometres across. Sulfuric acid vapour is often involved in nucleation but is too scarce to explain most subsequent growth, leaving organic vapours as the most plausible alternative, at least in the planetary boundary layer. Although recent studies predict that low-volatility organic vapours contribute during initial growth, direct evidence has been lacking. The accelerating growth may result from increased photolytic production of condensable organic species in the afternoon, and the presence of a possible Kelvin (curvature) effect, which inhibits organic vapour condensation on the smallest particles (the nano-Kohler theory), has so far remained ambiguous. Here we present experiments performed in a large chamber under atmospheric conditions that investigate the role of organic vapours in the initial growth of nucleated organic particles in the absence of inorganic acids and bases such as sulfuric acid or ammonia and amines, respectively. Using data from the same set of experiments, it has been shown that organic vapours alone can drive nucleation. We focus on the growth of nucleated particles and find that the organic vapours that drive initial growth have extremely low volatilities (saturation concentration less than 10(-4.5) micrograms per cubic metre). As the particles increase in size and the Kelvin barrier falls, subsequent growth is primarily due to more abundant organic vapours of slightly higher volatility (saturation concentrations of 10(-4.5) to 10(-0.5) micrograms per cubic metre). We present a particle growth model that quantitatively reproduces our measurements. Furthermore, we implement a parameterization of the first steps of growth in a global aerosol model and find that concentrations of atmospheric cloud concentration nuclei can change substantially in response, that is, by up to 50 per cent in comparison with previously assumed growth rate parameterizations.

/pdf/the-role-of-low-volatility-organic-compounds-in-initial-3d5sajbwi1.pdf

The role of low-volatility organic compounds in initial particle growth in the atmosphere

. Improving observations of ocean heat content show that Earth is absorbing more energy from the Sun than it is radiating to space as heat, even during the recent solar minimum. The inferred planetary energy imbalance, 0.58 ± 0.15 W m −2 during the 6-yr period 2005–2010, confirms the dominant role of the human-made greenhouse effect in driving global climate change. Observed surface temperature change and ocean heat gain together constrain the net climate forcing and ocean mixing rates. We conclude that most climate models mix heat too efficiently into the deep ocean and as a result underestimate the negative forcing by human-made aerosols. Aerosol climate forcing today is inferred to be −1.6 ± 0.3 W m −2 , implying substantial aerosol indirect climate forcing via cloud changes. Continued failure to quantify the specific origins of this large forcing is untenable, as knowledge of changing aerosol effects is needed to understand future climate change. We conclude that recent slowdown of ocean heat uptake was caused by a delayed rebound effect from Mount Pinatubo aerosols and a deep prolonged solar minimum. Observed sea level rise during the Argo float era is readily accounted for by ice melt and ocean thermal expansion, but the ascendency of ice melt leads us to anticipate acceleration of the rate of sea level rise this decade.

/pdf/earth-s-energy-imbalance-and-implications-1on3qao1gw.pdf

Earth's energy imbalance and implications

[1]Close passages of coronal mass ejections from the sun are signaled at the Earth's surface by Forbush decreases in cosmic ray counts. We find that low clouds contain less liquid water following Forbush decreases, and for the most influential events the liquid water in the oceanic atmosphere can diminish by as much as 7%. Cloud water content as gauged by the Special Sensor Microwave/Imager (SSM/I) reaches a minimum ≈7days after the Forbush minimum in cosmic rays, and so does the fraction of low clouds seen by the Moderate Resolution Imaging Spectroradiometer (MODIS) and in the International Satellite Cloud Climate Project (ISCCP). Parallel observations by the aerosol robotic network AERONET reveal falls in the relative abundance of fine aerosol particles which, in normal circumstances, could have evolved into cloud condensation nuclei. Thus a link between the sun, cosmic rays, aerosols, and liquid-water clouds appears to exist on a global scale.

/pdf/cosmic-ray-decreases-affect-atmospheric-aerosols-and-clouds-y6w3dvnw8c.pdf

Cosmic ray decreases affect atmospheric aerosols and clouds

Aerosol nucleation has been studied experimentally in purified, atmospheric air, containing trace amounts of water vapor, ozone, and sulfur dioxide. The results are compared with model calculations. It is found that an increase in ionization by a factor of 10 increases the production rate of stable clusters by a factor of ∼3, probably due to ion-induced nucleation.

Evidence for the role of ions in aerosol nucleation.

. In order to elucidate the effect of galactic cosmic rays on cloud formation, we investigate the optical response of marine aerosols to Forbush decreases – abrupt decreases in galactic cosmic rays – by means of modeling. We vary the nucleation rate of new aerosols, in a sectional coagulation and condensation model, according to changes in ionization by the Forbush decrease. From the resulting size distribution we then calculate the aerosol optical thickness and Angstrom exponent, for the wavelength pairs 350, 450 nm and 550, 900 nm. In the cases where the output parameters from the model seem to compare best with atmospheric observations we observe, for the shorter wavelength pair, a change in Angstrom exponent, following the Forbush Decrease, of −6 to +3%. In some cases we also observe a delay in the change of Angstrom exponent, compared to the maximum of the Forbush decrease, which is caused by different sensitivities of the probing wavelengths to changes in aerosol number concentration and size. For the long wavelengths these changes are generally smaller. The types and magnitude of change is investigated for a suite of nucleation rates, condensable gas production rates, and aerosol loss rates. Furthermore we compare the model output with observations of 5 of the largest Forbush decreases after year 2000. For the 350, 450 nm pair we use AERONET data and find a comparable change in signal while the Angstrom Exponent is lower in the model than in the data, due to AERONET being mainly sampled over land. For 550, 900 nm we compare with both AERONET and MODIS and find little to no response in both model and observations. In summary our study shows that the optical properties of aerosols show a distinct response to Forbush Decreases, assuming that the nucleation of fresh aerosols is driven by ions. Shorter wavelengths seem more favorable for observing these effects and great care should be taken when analyzing observations, in order to avoid the signal being drowned out by noise.

/pdf/model-of-optical-response-of-marine-aerosols-to-forbush-b3wzdrb43d.pdf

Model of optical response of marine aerosols to Forbush decreases

(03/11/2019) The Mean Sea Surface DTU10mss Comparison With Gps And Tide Gauges Satellite altimetry and the Global Position System (GPS) are conveniently given in the same reference frame and can therefore be used to construct a vertical reference surface for offshore navigation. Here a new Mean Sea Surface DTU10MSS is presented with a vertical accuracy better than 10 cm in most areas of the world confirmed by extensive comparison with GPS leveled tide gauges around Britain and Norway. It is proposed that this model is used as a global vertical reference. This paper briefly outlines the update of the previous DTU model to DTU10MSS and presents comparisons on GPS positions measured at the ship relative to the sea surface model.

The Mean Sea Surface DTU10mss - Comparison With Gps And Tide Gauges

/pdf/influence-of-cosmic-radiation-on-aerosol-and-cloud-formation-sdhgluxtpv.pdf

Influence of cosmic radiation on aerosol and cloud formation over short time periods

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