2013, Feng, Wuhu, Marsh, Daniel R., Chipperfield, Martyn P., Janches, Diego, Höffner, Josef, Yi, Fan, Plane, John M.C.

The first global model of meteoric iron in the atmosphere (WACCM-Fe) has been developed by combining three components: the Whole Atmosphere Community Climate Model (WACCM), a description of the neutral and ion-molecule chemistry of iron in the mesosphere and lower thermosphere (MLT), and a treatment of the injection of meteoric constituents into the atmosphere. The iron chemistry treats seven neutral and four ionized iron containing species with 30 neutral and ion-molecule reactions. The meteoric input function (MIF), which describes the injection of Fe as a function of height, latitude, and day, is precalculated from an astronomical model coupled to a chemical meteoric ablation model (CABMOD). This newly developed WACCM-Fe model has been evaluated against a number of available ground-based lidar observations and performs well in simulating the mesospheric atomic Fe layer. The model reproduces the strong positive correlation of temperature and Fe density around the Fe layer peak and the large anticorrelation around 100 km. The diurnal tide has a significant effect in the middle of the layer, and the model also captures well the observed seasonal variations. However, the model overestimates the peak Fe+concentration compared with the limited rocket-borne mass spectrometer data available, although good agreement on the ion layer underside can be obtained by adjusting the rate coefficients for dissociative recombination of Fe-molecular ions with electrons. Sensitivity experiments with the same chemistry in a 1-D model are used to highlight significant remaining uncertainties in reaction rate coefficients, and to explore the dependence of the total Fe abundance on the MIF and rate of vertical transport.

2016, Fytterer, T., Bender, S., Berger, U., Nieder, H., Sinnhuber, M., Wissing, J.M.

The 3-D global chemistry and transport model (3dCTM) was used to investigate NO, OH, and O3 from January 2002 to May 2010 between 60 km and 133 km. Their daytime and nighttime mean zonal means (55°–75° geomagnetic latitude) were analyzed with respect to short-term variations associated with particle precipitation. The corresponding ionization rates were derived from the 3-D atmospheric ionization module Osnabrück (AIMOS), which is based on particle flux measurements. The trace gas variations with respect to their background were investigated by using a superposed epoch analysis. The 27 day signature associated with particle precipitation is found in NO, while it is only indicated in OH and O3 during winter. A varying solar spectrum associated with the 11 year solar cycle causes modifications of this signal up to 10%, while the main patterns are conserved. Published observations show a clear 27 day signal, qualitatively agreeing with the model results at altitudes >70 km except for O3 in Northern Hemisphere winter. Further differences occur with respect to the magnitude of the trace gas variations, primarily attributed to the different trace gas background and dynamical variations of the background atmosphere. Absolute OH variations are overestimated by the 3dCTM during winter, while the opposite is true for O3. These differences might originate from an unknown offset in AIMOS, incorrect chemical reaction rates, a different background of H2O and O3, and the model dynamics. However, their nonlinear relationship and their altitude of largest response are qualitatively captured in Southern Hemisphere winter.

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.

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.

2015, Feng W., Höffner J., Marsh D.R., Chipperfield M.P., Dawkins E.C.M., Viehl T.P., Plane J.M.C.

Measurements of the diurnal cycle of potassium (K) atoms between 80 and 110 km have been made during October (for the years 2004–2011) using a Doppler lidar at Kühlungsborn, Germany (54.1°N, 11.7°E). A pronounced diurnal variation is observed in the K number density, which is explored by using a detailed description of the neutral and ionized chemistry of K in a three-dimensional chemistry climate model. The model captures both the amplitude and phase of the diurnal and semidiurnal variability of the layer, although the peak diurnal amplitude around 90 km is overestimated. The model shows that the total potassium density (≈ K + K+ + KHCO3) exhibits little diurnal variation at each altitude, and the diurnal variations are largely driven by photochemical conversion between these reservoir species. In contrast, tidally driven vertical transport has a small effect at this midlatitude location, and diurnal fluctuations in temperature are of little significance because they are small and the chemistry of K is relatively temperature independent.

2017-4-18, Lieberman, R.S., Riggin, D.M., Nguyen, V., Palo, S.E., Siskind, D.E., Mitchell, N.J., Stober, G., Wilhelm, S., Livesey, N.J.

We examine wave components in a high-altitude forecast-assimilation system that arise from nonlinear interaction between the diurnal tide and the westward traveling quasi 2 day wave. The process yields a westward traveling “sum” wave with zonal wave number 4 and a period of 16 h, and an eastward traveling “difference” wave with zonal wave number 2 and a period of 2 days. While the eastward 2 day wave has been reported in satellite temperatures, the westward 16 h wave lies outside the Nyquist limits of resolution of twice daily local time satellite sampling. Hourly output from a high-altitude forecast-assimilation model is used to diagnose the nonlinear quadriad. A steady state primitive equation model forced by tide-2 day wave advection is used to intepret the nonlinear wave products. The westward 16 h wave maximizes in the midlatitude winter mesosphere and behaves like an inertia-gravity wave. The nonlinearly generated component of the eastward 2 day wave maximizes at high latitudes in the lower thermosphere, and only weakly penetrates to low latitudes. The 16 h and the eastward 2 day waves are of comparable amplitude and alias to the same apparent frequency when viewed from a satellite perspective.

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.