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Tin monosulfide (SnS) is a naturally p-type semiconductor with a layeredcrystal structure, but no reliable n-type SnS has been obtained by conventionalaliovalent ion substitution. In this work, carrier polarity conversion ton-type was achieved by isovalent ion substitution for polycrystalline SnS thinfilms on glass substrates. Substituting Pb2+ for Sn2+ converted the majoritycarrier from hole to electron, and the free electron density ranged from 1012to 1015 cm-3 with the largest electron mobility of 7.0 cm2/(Vs). The n-typeconduction was confirmed further by the position of the Fermi level (EF) basedon photoemission spectroscopy and electrical characteristics of pnheterojunctions. Density functional theory calculations reveal that the Pbsubstitution invokes a geometrical size effect that enlarges the interlayerdistance and subsequently reduces the formation energies of Sn and Pbinterstitials, which work as electron donors.

n-type conversion of SnS by isovalent ion substitution: Geometrical doping as a new doping route