Abstract
The ablation of phosphorus from interplanetary dust particles entering
the Earth’s atmosphere is a potentially significant source of this key
bio-element. In this study, the atmospheric chemistry of phosphorus is
explored by developing a reaction network of possible routes from PO,
the major ablation product in the upper mesosphere/lower thermosphere
region, to the stable reservoirs H3PO3
and H3PO4 that become incorporated into
meteoric smoke particles as metal phosphites and phosphates,
respectively. The network is constructed with reactions whose kinetics
have been measured experimentally, together with reactions where
theoretical rate coefficients are estimated using a combination of
electronic structure theory calculations and a
Rice-Ramsperger-Kassel-Markus master equation treatment. The network is
then incorporated into a global chemistry-climate model, together with a
phosphorus meteoric input function. The estimated global mean P
deposition flux, in the form of sub-micron sized meteoric smoke
particles, is 1 × 10-8 g m-2
yr-1, with a maximum of ~5 ×
10-8 g m-2 yr-1
over the northern Rockies, Himalayas and southern Andes. The estimated
fraction of ablated phosphorus forming bio-available metal phosphites is
11%, which results from the very large concentrations of O and H
compared to OH in the upper mesosphere. A layer of OPO is predicted to
occur at 90 km with a peak of concentration of ~50
cm-3; this is the counterpart of the well-known layers
of meteoric metals such as Na and Fe, and may be observable
spectroscopically.