Abstract. In this work, we examined the interaction of ions and neutral particles during atmospheric new particle formation (NPF) events. The analysis is based on simultaneous field measurements of atmospheric ions and total particles using a neutral cluster and air ion spectrometer (NAIS) across the diameter range 2-25 nm. The Waldstein research site is located in a spruce forest in NE Bavaria, Southern Germany, known for enhanced radon concentrations, presumably leading to elevated ionization rates. Our observations show that the occurrence of the ion nucleation mode preceded that of the total particle nucleation mode during all analyzed NPF events. The time difference between the appearance of 2 nm ions and 2 nm total particles was typically about 20 to 30 min. A cross correlation analysis showed a rapid decrease of the time difference between the ion and total modes during the growth process. Eventually, this time delay vanished when both ions and total particles did grow to larger diameters. Considering the growth rates of ions and total particles separately, total particles exhibited enhanced growth rates at diameters below 15 nm. This observation cannot be explained by condensation or coagulation, because these processes would act more efficiently on charged particles compared to neutral particles. To explain our observations, we propose a mechanism including recombination and attachment of continuously present cluster ions with the ion nucleation mode and the neutral nucleation mode, respectively.

Microphysical measurements of orographic fog were performed above a montane cloud forest in northeastern Taiwan (Chilan mountain site). The measured parameters include droplet size distribution (DSD), absolute humidity (AH), relative humidity (RH), air temperature, wind speed and direction, visibility, and solar short wave radiation. The scope of this work was to study the short term variations of DSD, temperature, and RH, with a temporal resolution of 3 Hz. The results show that orographic fog is randomly composed of various air volumes that are intrinsically rather homogeneous, but exhibit clear differences between each other with respect to their size, RH, LWC, and DSD. Three general types of air volumes have been identified via the recorded DSD. A statistical analysis of the characteristics of these volumes yielded large variabilities in persistence, RH, and LWC. Further, the data revealed an inverse relation between RH and LWC. In principle, this finding can be explained by the condensational growth theory for droplets containing soluble or insoluble material. Droplets with greater diameters can exist at lower ambient RH than smaller ones. However, condensational growth alone is not capable to explain the large observed differences in DSD and RH because the respective growth speeds are too slow to explain the observed phenomena. Other mechanisms play key roles as well. Possible processes leading to the large observed differences in RH and DSD include turbulence induced collision and coalescence, and heterogeneous mixing. More analyses including fog droplet chemistry and dynamic microphysical modeling are required to further study these processes. To our knowledge, this is the first experimental field observation of the anti-correlation between RH and LWC in fog.

Abstract. New particle formation is a frequent phenomenon in the atmosphere and of major significance for the Earth's climate and human health. To date the mechanisms leading to the nucleation of particles as well as to aerosol growth are not completely understood. A lack of appropriate measurement equipment for online analysis of the chemical composition of freshly nucleated particles is one major limitation. We have developed a Chemical Analyzer for Charged Ultrafine Particles (CAChUP) capable of analyzing particles with diameters below 30 nm. A bulk of size-separated particles is collected electrostatically on a metal filament, resistively desorbed and subsequently analyzed for its molecular composition in a time of flight mass spectrometer. We report on technical details as well as characterization experiments performed with the CAChUP. Our instrument was tested in the laboratory for its detection performance as well as for its collection and desorption capabilities. The manual application of defined masses of camphene (C10H16) to the desorption filament resulted in a detection limit between 0.5 and 5 ng, and showed a linear response of the mass spectrometer. Flow tube experiments of 25 nm diameter secondary organic aerosol from ozonolysis of alpha-pinene also showed a linear relation between collection time and the mass spectrometer's signal intensity. The resulting mass spectra from the collection experiments are in good agreement with published work on particles generated by the ozonolysis of alpha-pinene. A sensitivity study shows that the current setup of CAChUP is ready for laboratory measurements and for the observation of new particle formation events in the field.

Abstract. In this work, we examined the interaction of ions and neutral particles during atmospheric new particle formation (NPF) events. The analysis is based on simultaneous field measurements of atmospheric ions and total particles using a neutral cluster and air ion spectrometer (NAIS) across the diameter range 2–25 nm. The "Waldstein" research site is located in a spruce forest in NE Bavaria, Southern Germany, known for enhanced radon concentrations, presumably leading to elevated ionization rates. Our observations show that the occurrence of the ion nucleation mode preceded that of the total particle nucleation mode during all analysed NPF events. The time difference between the appearance of 2 nm ions and 2 nm total particles was typically about 20 to 30 min. A cross correlation analysis showed a rapid decrease of the time difference between the ion and total modes during the growth process. Eventually, this time delay vanished when both ions and total particles did grow to larger diameters. Considering the growth rates of ions and total particles separately, total particles exhibited enhanced growth rates at diameters below 15 nm. This observation cannot be explained by condensation or coagulation, because these processes would act more efficiently on charged particles compared to neutral particles. To explain our observations, we propose a mechanism including recombination and attachment of continuously present cluster ions with the ion nucleation mode and the neutral nucleation mode, respectively.

New particle formation is a frequent phenomenon in the atmosphere and of major significance for the earth's climate and human health. To date the mechanisms leading to the nucleation of particles as well as to aerosol growth are not completely understood. A lack of appropriate measurement equipment for online analysis of the chemical composition of freshly nucleated particles is one major limitation. We have developed a Chemical Analyzer for Charged Ultrafine Particles (CAChUP) capable of analyzing particles with diameters below 30 nm. A bulk of size separated particles is collected electrostatically on a metal filament, resistively desorbed and consequently analyzed for its molecular composition in a time of flight mass spectrometer. We report of technical details as well as characterization experiments performed with the CAChUP. Our instrument was tested in the laboratory for its detection performance as well as for its collection and desorption capabilities. The manual application of known masses of camphene (C₁₀H₁₆) to the desorption filament resulted in a detection limit between 0.5 and 5 ng, and showed a linear response of the mass spectrometer. Flow tube experiments of 25 nm diameter secondary organic aerosol from ozonolysis of alpha-pinene also showed a linear relation between collection time and the mass spectrometer's signal intensity. The resulting mass spectra from the collection experiments are in good agreement with published work on particles generated by the ozonolysis of alpha-pinene. A sensitivity study shows that the current setup of CAChUP is ready for laboratory measurements and for the observation of new particle formation events in the field