Incipient Dissolution of Emplaced Forsterite and Fayalite Records the Effects of Climate, Mineral Composition, and Crystallographic Orientation

Abstract

To investigate the effects of environment, composition, and crystal orientation on incipient surface alteration of forsterite and fayalite in a natural environment, polycrystalline forsterite and fayalite samples were emplaced in Mg/Fe-rich and Al-poor ultramafic soils under subarctic (Tablelands in Newfoundland, Canada; 3.9 ⁰C and ∼120 cm precipitation/year), Mediterranean (Klamath Mountains, California;≤12.8 ⁰C and ∼101-118 cm precipitation/year), and desert (Pickhandle Gulch, Nevada; ∼14.1 ⁰C and ∼14.4 cm/year) climates for one year. Incipient alteration after one year was examined using scanning electron microscopy, atomic force microscopy, electron backscatter diffraction, X-ray photoelectron spectroscopy, and visible and near-infrared reflectance spectroscopy.Alteration features on forsterite surfaces included flat-bottomed pits with steeply dipping walls likely developing on grain faces and representing surface retreat of individual grains and lining features likely developing along grain boundaries. Mg-leached surface layers formed under acidic to slightly alkaline conditions while Mg-enrichment was observed under alkaline conditions. Flat bottomed pit formation preferentially occurs on surfaces within 30° of perpendicular to the b-axis (on the [010] plane) of the olivine crystal lattice. Depth of flat-bottomed pits on forsterite surfaces follows the order Klamath Mountains > Tablelands >> Pickhandle Gulch, reflecting the importance of environmental conditions. Warm, wet, and relatively acidic conditions enhanced forsterite dissolution over cold, wet, and slightly alkaline conditions, with minimal alteration observed under hot but arid and alkaline conditions. Greater surface roughness on flat-bottomed pit floors on Klamath Mountain forsterite surfaces are consistent with less-saturated soil-pore water reaction conditions.In contrast, fayalite disks buried in the Klamath Mountains show no evidence for etch-pit formation despite the warm, wet, and slightly acidic conditions. Elevated Fe/Si ratios from X-ray photoelectron spectroscopy measurements and evidence of M-OH bonds in visual and near infrared spectra are consistent with formation of a Fe-enriched hydroxylated layer limiting fayalite surface area available for water-rock interaction and retarding fayalite dissolution during aqueous alteration under oxidizing conditions. These results differ from previous laboratory experiments that show enhanced dissolution of fayalite relative to forsterite, showing the effect of natural, oxic, unsaturated weathering zones. These results will be helpful for interpreting observations of this widely studied mineral, including from the planet Mars.