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Abstract: Total soil organic matter levels and humic acid formation processes in mountain calcimorphic soils from Sierra María-Los Vélez Natural Park (Almería, Southern Spain) were found to differ depending on soil use (pine and oak forests, and cleared areas either cultivated or affected by bush encroachment). Biogeochemical indicators such as the concentration of exchangeable cations, or the concentration of the different types of humic substances were neither influenced by the type of vegetation nor soil use. In fact, multidimensional scaling and multiple correlations suggest that soil carbon sequestration processes are controlled by small-scale topographical features and their impact on water holding capacity. From a qualitative viewpoint, there were two more or less defined sets of soils: one set consisted of soils with humic acids with marked aliphatic character, displayed intense 2920cm−1 infrared band, and had low optical density. The resolution-enhanced infrared spectra suggested typical lignin patterns and well-defined amide bands, which point to a selective preservation of comparatively young organic matter. This situation contrasts with that in other set of soils with low C levels (<20gkg−1) where humic acids with featureless infrared spectra showed high aromaticity and were associated with perylenequinonic chromophors of fungal origin: this is considered the consequence of overlapping biogeochemical mechanisms involving both microbial synthesis and condensation processes. The results from visible and infrared derivative spectroscopies suggest that the reliability of statistically assessing the biogeochemical performance of the different uses on the site studied in terms of the intensity of the prevailing humic acid formation mechanisms, i.e., accumulation of inherited macromolecular substances in the former set, vs. microbial synthesis including the condensation of precursors of low molecular weight substances in the latter. [Copyright &y& Elsevier]