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Abstract Complex oxide films stabilized by epitaxial growth can exhibit large populations of point defects which have important effects on their properties. The site occupancy of pulsed laser‐deposited epitaxial terbium iron garnet (TbIG) films with excess terbium (Tb) is analyzed, in which the terbium:iron (Tb:Fe)ratio is 0.86 compared to the stoichiometric value of 0.6. The magnetic properties of the TbIG are sensitive to site occupancy, exhibiting a higher compensation temperature (by 90 K) and a lower Curie temperature (by 40 K) than the bulk Tb₃Fe₅O₁₂garnet. Data derived from X‐ray core‐level spectroscopy, magnetometry, and molecular field coefficient modeling are consistent with occupancy of the dodecahedral sites by Tb³⁺, the octahedral sites by Fe³⁺, Tb³⁺and vacancies, and the tetrahedral sites by Fe³⁺and vacancies. Energy dispersive X‐ray spectroscopy in a scanning transmission electron microscope provides direct evidence of Tb_Feantisites. A small fraction of Fe²⁺is present, and oxygen vacancies are inferred to be present to maintain charge neutrality. Variation of the site occupancies provides a path to considerable manipulation of the magnetic properties of epitaxial iron garnet films and other complex oxides, which readily accommodate stoichiometries not found in their bulk counterparts. 

Abstract Films of polycrystalline terbium iron garnet (TbIG), cerium‐substituted TbIG (CeTbIG), and bismuth‐substituted TbIG (BiTbIG) are grown on Si substrates by pulsed laser deposition. The films grow under tensile strain due to thermal mismatch with the Si substrate, resulting in a dominant magnetoelastic anisotropy which, combined with shape anisotropy, leads to in‐plane magnetization. TbIG has a compensation temperature of 253 K which is reduced by substitution of Ce and Bi. The Faraday rotation at 1550 nm of the TbIG, Ce_0.36TbIG, and Bi_0.03TbIG films is 5400 ± 600° cm⁻¹, 4500 ± 100° cm^–1, and 6200 ± 300° cm⁻¹, respectively, while Ce_0.36TbIG and Bi_0.03TbIG exhibit lower optical absorption than TbIG, attributed to a reduction in Fe²⁺and Tb⁴⁺absorption pathways. The high Faraday rotation of the films, and in particular the high magneto‐optical figure of merit of the Bi_0.03TbIG of 720° dB⁻¹at 1550 nm, make these polycrystalline films valuable for applications in integrated photonics.