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Pyrite FeS2 has outstanding potential as an earth-abundant, low-cost, nontoxic photovoltaic, but underperforms dramatically in solar cells. While the full reasons for this are not clear, one certain factor is the inability to understand and control doping in FeS2. This is exemplified by the widely accepted but unexplained observation that unintentionally doped FeS2 single crystals are predominantly n type, whereas thin films are p type. Here we provide a potential resolution to this "doping puzzle," arrived at via Hall effect, thermopower, and resistivity measurements on a large set of FeS2 single crystals and films that span five orders of magnitude in mobility. The results reveal three main findings. First, in addition to crystals, the highest mobility thin films in this study are shown to be definitively n type, from both Hall effect and thermopower. Second, as mobility decreases an apparent crossover to p type occurs, first in thermopower, then in Hall measurements. This can be understood, however, in terms of the crossover from diffusive to hopping transport that is clearly reflected in resistivity. Third, universal behavior is found for both crystals and films, suggesting a common n dopant, possibly sulfur vacancies. We thus argue that n-type doping is facile in FeS2 films, that apparent p-type behavior in low mobility samples can be an artifact of hopping, and that the prevailing notion of predominantly p-type films must be revised. These conclusions have deep implications, both for interpretation of prior work on FeS2 solar cells and for the design of future studies.
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