Ionization in the atmosphere, comparison between measurements and simulations

A survey of the data on measured particle fluxes and the rate of ionization in the atmosphere is presented. Measurements as a function of altitude, time and cut-off rigidity are compared with simulations of particle production from cosmic rays. The simulations generally give a reasonable representation of the data. However, some discrepancies are found. The solar modulation of the particle fluxes is measured and found to be a factor 2.7$\pm$0.8 greater than that observed for muons alone near sea level.Comment: Accepted for publication in Astrophysics and Space Science Transactions. Typographical errors fixe

Results from the CERN pilot CLOUD experiment

During a 4-week run in October–November 2006, a pilot experiment was performed at the CERN Proton Synchrotron in preparation for the Cosmics Leaving OUtdoor Droplets (CLOUD) experiment, whose aim is to study the possible influence of cosmic rays on clouds. The purpose of the pilot experiment was firstly to carry out exploratory measurements of the effect of ionising particle radiation on aerosol formation from trace H2SO4 vapour and secondly to provide technical input for the CLOUD design. A total of 44 nucleation bursts were produced and recorded, with formation rates of particles above the 3 nm detection threshold of between 0.1 and 100 cm−3 s−1, and growth rates between 2 and 37 nm h−1. The corresponding H2SO4 concentrations were typically around 106 cm−3 or less. The experimentally-measured formation rates and H2SO4 concentrations are comparable to those found in the atmosphere, supporting the idea that sulphuric acid is involved in the nucleation of atmospheric aerosols. However, sulphuric acid alone is not able to explain the observed rapid growth rates, which suggests the presence of additional trace vapours in the aerosol chamber, whose identity is unknown. By analysing the charged fraction, a few of the aerosol bursts appear to have a contribution from ion-induced nucleation and ion-ion recombination to form neutral clusters. Some indications were also found for the accelerator beam timing and intensity to influence the aerosol particle formation rate at the highest experimental SO2 concentrations of 6 ppb, although none was found at lower concentrations. Overall, the exploratory measurements provide suggestive evidence for ion-induced nucleation or ion-ion recombination as sources of aerosol particles. However in order to quantify the conditions under which ion processes become significant, improvements are needed in controlling the experimental variables and in the reproducibility of the experiments. Finally, concerning technical aspects, the most important lessons for the CLOUD design include the stringent requirement of internal cleanliness of the aerosol chamber, as well as maintenance of extremely stable temperatures (variations below 0.1 _C)

New particle formation in the sulfuric acid-dimethylamine-water system: reevaluation of CLOUD chamber measurements and comparison to an aerosol nucleation and growth model

A recent CLOUD (Cosmics Leaving OUtdoor Droplets) chamber study showed that sulfuric acid and dimethylamine produce new aerosols very efficiently and yield particle formation rates that are compatible with boundary layer observations. These previously published new particle formation (NPF) rates are reanalyzed in the present study with an advanced method. The results show that the NPF rates at 1.7 nm are more than a factor of 10 faster than previously published due to earlier approximations in correcting particle measurements made at a larger detection threshold. The revised NPF rates agree almost perfectly with calculated rates from a kinetic aerosol model at different sizes (1.7 and 4.3 nm mobility diameter). In addition, modeled and measured size distributions show good agreement over a wide range of sizes (up to ca. 30 nm). Furthermore, the aerosol model is modified such that evaporation rates for some clusters can be taken into account; these evaporation rates were previously published from a flow tube study. Using this model, the findings from the present study and the flow tube experiment can be brought into good agreement for the high base-to-acid ratios (similar to 100) relevant for this study. This confirms that nucleation proceeds at rates that are compatible with collision-controlled (a.k.a. kinetically controlled) NPF for the conditions during the CLOUD7 experiment (278 K, 38% relative humidity, sulfuric acid concentration between 1 x 10(6) and 3 x 10(7) cm(-3), and dimethylamine mixing ratio of similar to 40 pptv, i.e., 1 x 10(9) cm(-3)).Peer reviewe

Causes and importance of new particle formation in the present-day and pre-industrial atmospheres

New particle formation has been estimated to produce around half of cloud-forming particles in the present-day atmosphere, via gas-to-particle conversion. Here we assess the importance of new particle formation (NPF) for both the present-day and the pre-industrial atmospheres. We use a global aerosol model with parametrisations of NPF from previously published CLOUD chamber experiments involving sulphuric acid, ammonia, organic molecules and ions. We find that NPF produces around 67% of cloud condensation nuclei at 0.2% supersaturation (CCN0.2%) at the level of low clouds in the pre-industrial atmosphere (estimated uncertainty range 45-84%) and 54% in the present day (estimated uncertainty range 38-66%). Concerning causes, we find that the importance of biogenic volatile organic compounds (BVOCs) in NPF and CCN formation is greater than previously thought. Removing BVOCs and hence all secondary organic aerosol from our model reduces low-cloud-level CCN concentrations at 0.2% supersaturation by 26% in the present-day atmosphere and 41% in the pre-industrial. Around three-quarters of this reduction is due to the tiny fraction of the oxidation products of BVOCs that have sufficiently low volatility to be involved in NPF and early growth. Furthermore, we estimate that 40% of pre-industrial CCN0.2% are formed via ion-induced NPF, compared with 27% in the present-day, although we caution that the ion-induced fraction of NPF involving BVOCs is poorly measured at present. Our model suggests that the effect of changes in cosmic ray intensity on CCN is small and unlikely to be comparable to the effect of large variations in natural primary aerosol emissions

A study of the link between cosmic rays and clouds with a cloud chamber at the CERN PS

Recent satellite data have revealed a surprising correlation between galactic cosmic ray (GCR) intensity and the fraction of the Earth covered by clouds. If this correlation were to be established by a causal mechanism, it could provide a crucial step in understanding the long-sought mechanism connecting solar and climate variability. The Earth's climate seems to be remarkably sensitive to solar activity, but variations of the Sun's electromagnetic radiation appear to be too small to account for the observed climate variability. However, since the GCR intensity is strongly modulated by the solar wind, a GCR-cloud link may provide a sufficient amplifying mechanism. Moreover if this connection were to be confirmed, it could have profound consequences for our understanding of the solar contributions to the current global warming. The CLOUD (Cosmics Leaving OUtdoor Droplets) project proposes to test experimentally the existence a link between cosmic rays and cloud formation, and to understand the microphysical mechanism. CLOUD plans to perform detailed laboratory measurements in a particle beam at CERN, where all the parameters can be precisely controlled and measured. The beam will pass through an expansion cloud chamber and a reactor chamber where the atmosphere is to be duplicated by moist air charged with selected aerosols and trace condensable vapours. An array of external detectors and mass spectrometers is used to analyse the physical and chemical characteristics of the aerosols and trace gases during beam exposure. Where beam effects are found, the experiment will seek to evaluate their significance in the atmosphere by incorporating them into aerosol and cloud models.Recent satellite data have revealed a surprising correlation between galactic cosmic ray (GCR) intensity and the fraction of the Earth covered by clouds. If this correlation were to be established by a causal mechanism, it could provide a crucial step in understanding the long-sought mechanism connecting solar and climate variability. The Earth's climate seems to be remarkably sensitive to solar activity, but variations of the Sun's electromagnetic radiation appear to be too small to account for the observed climate variability. However, since the GCR intensity is strongly modulated by the solar wind, a GCR-cloud link may provide a sufficient amplifying mechanism. Moreover if this connection were to be confirmed, it could have profound consequences for our understanding of the solar contributions to the current global warming. The CLOUD (Cosmics Leaving OUtdoor Droplets) project proposes to test experimentally the existence a link between cosmic rays and cloud formation, and to understand the microphysical mechanism. CLOUD plans to perform detailed laboratory measurements in a particle beam at CERN, where all the parameters can be precisely controlled and measured. The beam will pass through an expansion cloud chamber and a reactor chamber where the atmosphere is to be duplicated by moist air charged with selected aerosols and trace condensable vapours. An array of external detectors and mass spectrometers is used to analyse the physical and chemical characteristics of the aerosols and trace gases during beam exposure. Where beam effects are found, the experiment will seek to evaluate their significance in the atmosphere by incorporating them into aerosol and cloud models

Experimental investigation of ion-ion recombination under atmospheric conditions

We present the results of laboratory measurements of the ion–ion recombination coefficient at different temperatures, relative humidities and concentrations of ozone and sulfur dioxide. The experiments were carried out using the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at CERN, the walls of which are made of conductive material, making it possible to measure small ions. We produced ions in the chamber using a 3.5 GeV c−1 beam of positively charged pions (π+) generated by the CERN Proton Synchrotron (PS). When the PS was switched off, galactic cosmic rays were the only ionization source in the chamber. The range of the ion production rate varied from 2 to 100 cm−3 s−1, covering the typical range of ionization throughout the troposphere. The temperature ranged from −55 to 20 °C, the relative humidity (RH) from 0 to 70 %, the SO2 concentration from 0 to 40 ppb, and the ozone concentration from 200 to 700 ppb. The best agreement of the retrieved ion–ion recombination coefficient with the commonly used literature value of 1.6 × 10−6 cm3 s−1 was found at a temperature of 5 °C and a RH of 40 % (1.5 ± 0.6) × 10−6 cm3 s−1. At 20 °C and 40 % RH, the retrieved ion–ion recombination coefficient was instead (2.3 ± 0.7) × 10−6 cm3 s−1. We observed no dependency of the ion–ion recombination coefficient on ozone concentration and a weak variation with sulfur dioxide concentration. However, we observed a more than fourfold increase in the ion–ion recombination coefficient with decreasing temperature. We compared our results with three different models and found an overall agreement for temperatures above 0 °C, but a disagreement at lower temperatures. We observed a strong increase in the recombination coefficient for decreasing relative humidities, which has not been reported previously

Addendum to the CLOUD proposal

This report is the first of two addenda to the CLOUD proposal at CERN (physics/0104048), which aims to test experimentally the existence a link between cosmic rays and cloud formation, and to understand the microphysical mechanism. The document provides further details on the detector design, scientific motivation and experimental programme

CLOUD: an atmospheric research facility at CERN

This report is the second of two addenda to the CLOUD proposal at CERN (physics/0104048), which aims to test experimentally the existence a link between cosmic rays and cloud formation, and to understand the microphysical mechanism. The document places CLOUD in the framework of a CERN facility for atmospheric research, and provides further details on the particle beam requirements