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- ItemSolar cycle response and long-term trends in the mesospheric metal layers(Hoboken, NJ : Wiley, 2016) Dawkins, E.C.M.; Plane, J.M.C.; Chipperfield, M.P.; Feng, W.; Marsh, D.R.; Höffner, J.; Janches, D.The meteoric metal layers (Na, Fe, and K)—which form as a result of the ablation of incoming meteors—act as unique tracers for chemical and dynamical processes that occur within the upper mesosphere/lower thermosphere region. In this work, we examine whether these metal layers are sensitive indicators of decadal long-term changes within the upper atmosphere. Output from a whole-atmosphere climate model is used to assess the response of the Na, K, and Fe layers across a 50 year period (1955–2005). At short timescales, the K layer has previously been shown to exhibit a very different seasonal behavior compared to the other metals. Here we show that this unusual behavior is also exhibited at longer timescales (both the ~11 year solar cycle and 50 year periods), where K displays a much more pronounced response to atmospheric temperature changes than either Na or Fe. The contrasting solar cycle behavior of the K and Na layers predicted by the model is confirmed using satellite and lidar observations for the period 2004–2013.
- ItemResolving the strange behavior of extraterrestrial potassium in the upper atmosphere(Hoboken, NJ : Wiley, 2014) Plane, J.M.C.; Feng, W.; Dawkins, E.; Chipperfield, M.P.; Höffner, J.; Janches, D.; Marsh, D.R.It has been known since the 1960s that the layers of Na and K atoms, which occur between 80 and 105 km in the Earth's atmosphere as a result of meteoric ablation, exhibit completely different seasonal behavior. In the extratropics Na varies annually, with a pronounced wintertime maximum and summertime minimum. However, K varies semiannually with a small summertime maximum and minima at the equinoxes. This contrasting behavior has never been satisfactorily explained. Here we use a combination of electronic structure and chemical kinetic rate theory to determine two key differences in the chemistries of K and Na. First, the neutralization of K+ ions is only favored at low temperatures during summer. Second, cycling between K and its major neutral reservoir KHCO3 is essentially temperature independent. A whole atmosphere model incorporating this new chemistry, together with a meteor input function, now correctly predicts the seasonal behavior of the K layer.
- ItemA study of the dissociative recombination of CaO+ with electrons: Implications for Ca chemistry in the upper atmosphere(Hoboken, NJ : Wiley, 2016) Bones, D.L.; Gerding, M.; Höffner, J.; Gómez Martín, Juan Carlos; Plane, J.M.C.The dissociative recombination of CaO+ ions with electrons has been studied in a flowing afterglow reactor. CaO+ was generated by the pulsed laser ablation of a Ca target, followed by entrainment in an Ar+ ion/electron plasma. A kinetic model describing the gas-phase chemistry and diffusion to the reactor walls was fitted to the experimental data, yielding a rate coefficient of (3.0 ± 1.0) × 10−7 cm3 molecule−1 s−1 at 295 K. This result has two atmospheric implications. First, the surprising observation that the Ca+/Fe+ ratio is ~8 times larger than Ca/Fe between 90 and 100 km in the atmosphere can now be explained quantitatively by the known ion-molecule chemistry of these two metals. Second, the rate of neutralization of Ca+ ions in a descending sporadic E layer is fast enough to explain the often explosive growth of sporadic neutral Ca layers.