Abstract. We have used the Whole Atmosphere Community Climate Model (WACCM), with an updated treatment of loss processes, to determine the atmospheric lifetime of sulfur hexafluoride (SF 6 ). The model includes the following SF 6 removal processes: photolysis, electron attachment and reaction with mesospheric metal atoms. The Sodankylä Ion Chemistry (SIC) model is incorporated into the standard version of WACCM to produce a new version with a detailed D region ion chemistry with cluster ions and negative ions. This is used to determine a latitude-and altitudedependent scaling factor for the electron density in the standard WACCM in order to carry out multi-year SF 6 simulations. The model gives a mean SF 6 lifetime over an 11-year solar cycle (τ ) of 1278 years (with a range from 1120 to 1475 years), which is much shorter than the currently widely used value of 3200 years, due to the larger contribution (97.4 %) of the modelled electron density to the total atmospheric loss. The loss of SF 6 by reaction with mesospheric metal atoms (Na and K) is far too slow to affect the lifetime. We investigate how this shorter atmospheric lifetime impacts the use of SF 6 to derive stratospheric age of air. The age of air derived from this shorter lifetime SF 6 tracer is longer by 9 % in polar latitudes at 20 km compared to a passive SF 6 tracer. We also present laboratory measurements of the infrared spectrum of SF 6 and find good agreement with previous studies. We calculate the resulting radiative forcings and efficiencies to be, on average, very similar to those reported previously. Our values for the 20-, 100-and 500-year global warming potentials are 18 000, 23 800 and 31 300, respectively.
We present a path forward on a long-standing issue concerning the flux of small and slow meteoroids, which are believed to be the dominant portion of the incoming meteoric mass flux into the Earth's atmosphere. Such a flux, which is predicted by dynamical dust models of the Zodiacal Cloud, is not evident in ground-based radar observations. For decades this was attributed to the fact that the radars used for meteor observations lack the sensitivity to detect this population, due to the small amount of ionization produced by slow-velocity meteors. Such a hypothesis has been challenged by the introduction of meteor head echo (HE) observations with High Power and Large Aperture radars, in particular the Arecibo 430 MHz radar. Janches et al. developed a probabilistic approach to estimate the detectability of meteors by these radars and initially showed that, with the current knowledge of ablation and ionization, such particles should dominate the detected rates by one to two orders of magnitude compared to the actual observations. In this paper, we include results in our model from recently published laboratory measurements, which showed that (1) the ablation of Na is less intense covering a wider altitude range; and (2) the ionization probability, b ip , for Na atoms in the air is up to two orders of magnitude smaller for low speeds than originally believed. By applying these results and using a somewhat smaller size of the HE radar target we offer a solution that reconciles these observations with model predictions.
Silicon is one of the most abundant elements in cosmic dust, and meteoric ablation injects a significant amount of Si into the atmosphere above 80 km. In this study, a new model for silicon chemistry in the mesosphere/lower thermosphere is described, based on recent laboratory kinetic studies of Si, SiO, SiO2, and Si+. Electronic structure calculations and statistical rate theory are used to show that the likely fate of SiO2 is a two‐step hydration to silicic acid (Si(OH)4), which then polymerizes with metal oxides and hydroxides to form meteoric smoke particles. This chemistry is then incorporated into a whole atmosphere chemistry‐climate model. The vertical profiles of Si+ and the Si+/Fe+ ratio are shown to be in good agreement with rocket‐borne mass spectrometric measurements between 90 and 110 km. Si+ has consistently been observed to be the major meteoric ion around 110 km; this implies that the relative injection rate of Si from meteoric ablation, compared to metals such as Fe and Mg, is significantly larger than expected based on their relative chondritic abundances. Finally, the global abundances of SiO and Si(OH)4 show clear evidence of the seasonal meteoric input function, which is much less pronounced in the case of other meteoric species.
We present laboratory measurements of the phase functions and degree of linear polarization (DLP) curves of a selection of millimeter-sized cosmic dust analog particles. The set includes particles with similar sizes but diverse internal structure (compact and porous) and absorbing properties. The measured phase functions are found to be in all cases very different from those of micron-sized particles. They show a monotonic decrease with increasing phase angle from the back- to the side-scattering region, reaching a minimum at large phase angles before a steep increase of the forward peak. This is in stark contrast to the phase functions of micron-sized particles, which are rather flat at low and intermediate phase angles. The maximum of the DLP for millimeter-sized compact particles is shifted toward larger phase angles (∼130°) compared to that of micron-sized particles (∼90°). Porosity plays an important role in the measured DLP curves: the maximum significantly decreases for increasing porosity as a result of multiple scattering within the particle. Large porous particles with highly absorbing inclusions can reproduce both the OSIRIS/Rosetta phase functions and ground-based DLP observations of comet 67P/Churyumov–Gerasimenko.
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