Insulator-like behavior coexisting with metallic electronic structure in strained FeSe thin films grown by molecular beam epitaxy

Abstract: This paper reports that ~10-nm-thick FeSe thin films exhibit insulator-like behavior in terms of the temperature dependence of their electrical resistivity even though bulk FeSe has a metallic electronic structure that has been confirmed by photoemission spectroscopy and first-principles calculations. This apparent contradiction is explained by potential barriers formed in the conduction band. Very thin FeSe epitaxial films with various [Fe]/[Se] were fabricated by molecular beam epitaxy and classified into two groups with respect to lattice strain and electrical properties. Lattice parameter a increased and lattice parameter c decreased with increasing [Fe]/[Se] up to 1.1 and then a levelled off and c began to decrease at higher [Fe]/[Se]. Consequently, the FeSe films had the most strained lattice when [Fe]/[Se] was 1.1, but these films had the best quality with respect to crystallinity and surface flatness. All the FeSe films with [Fe]/[Se] of 0.8-1.9 exhibited insulator-like behavior, but the temperature dependences of their electrical resistivities exhibited different activation energies Ea between the Se-rich and Fe-rich regions; i.e., Ea were small (a few meV) up to [Fe]/[Se]=1.1 but jumped up to ~25 meV at higher [Fe]/[Se]. The film with [Fe]/[Se]=1.1 had the smallest Ea of 1.1 meV and exhibited an insulator-superconducting transition at 35 K with zero resistance under gate bias. The large Ea of the Fe-rich films was attributed to the unusual lattice strain with tensile in-plane and relaxed out-of-plane strains. The large Ea of films with [Fe]/[Se]>1.1 resulted in low mobility with a high potential barrier of ~50 meV in the conduction band for percolation carrier conduction compared with that of the [Fe]/[Se]=1.1 film (~17 meV). Therefore, the Fe-rich films exhibited remarkable insulator-like behavior similar to a semiconductor despite their metallic electronic structure.