European Geosciences Union, Atmospheric Chemistry and Physics, 20(18), p. 14799-14811, 2018
Meteoric ablation produces layers of metal atoms in the mesosphere and lower thermosphere (MLT). It has been known for more than 30 years that the Ca atom layer is depleted by over 2 orders of magnitude compared with Na, despite these elements having essentially the same elemental abundance in chondritic meteorites. In contrast, the Ca + ion abundance is depleted by less than a factor of 10. To explain these observations, a large data-base of neutral and ion-molecule reaction kinetics of Ca species, measured over the past decade, was incorporated into the Whole Atmosphere Community Climate Model (WACCM). A new meteoric input function for Ca and Na, derived using a chemical ablation model that has been tested experimentally with a Meteoric Ablation Simulator, shows that Ca experiences significant differential ablation, by almost 1 order of magnitude, with respect to Na. WACCM-Ca simulates the seasonal Ca layer satisfactorily when compared with lidar observations, but tends to overestimate Ca + measurements made by rocket mass spectrometry and lidar. A key finding is that CaOH and CaCO 3 are very stable reservoir species because they are involved in essentially closed reaction cycles with O 2 and O. This has been demonstrated experimentally for CaOH, and in this study for CaCO 3 using electronic structure and statistical rate theory. Most of the neutral Ca is therefore locked in these reservoirs, enabling rapid loss through polymerization into meteoric smoke particles and explaining the extreme depletion of Ca.