Unprecedented tuning of the in-plane easy axis in (100) magnetite films grown by IR-PLD

Abstract

Magnetite (Fe3O4) is attracting much interest in the last years due to its robust ferrimagnetism down to nanometer thickness, good electrical conductivity and presumed half-metal character. In particular, Fe3O4 films are studied as ideal cases for the design of improved bulk magnets [1] and have been tentatively used in spin-valves and spin-LEDs. Fe3O4 presents a low-temperature metal-insulator transition, the Verwey transition (TV) which has also been proposed for spintronic applications. An open question is to what extent the preparation of Fe3O4 films can affect their detailed magnetic properties, such as the magnetic anisotropy axis. This information is required to efficiently apply Fe3O4 in technological multiphase magnets and spintronic applications [1]. Most of studies dealing with bulk and Fe3O4 thin film systems show room temperature (RT) in-plane <110> magnetic easy axis. By contrast, we show in this work the preparation of pure stoichiometric Fe3O4 thin films with RT easy axes along the in-plane <100> directions [2], i.e. rotated by 45º respect to previous studies. Fe3O4 films have been grown by ablation from a sintered hematite target using a nanosecond infrared (IR) laser at 1064 nm and a substrate temperature of 750 K [3]. Single crystal substrates of SrTiO3, MgAl2O4 and MgO have been used. The films were characterized using XRD, AFM, Raman and Mössbauer spectroscopies, vectorial magneto-optical Kerr effect microscopy (v-MOKE) and SQUID magnetometry. All films consisted of stoichiometric Fe3O4 and presented a Verwey transition at TV=115-118 K. RT in-plane hysteresis loops were measured by vectorial-MOKE as a function of the direction of the applied magnetic field in the 0º-360º range with an angular step of 5º. For all epitaxial films under study, the highest coercivity and remanence are found at 0º, 90º, 180º and 270º (i.e. <100> directions), thus orthogonal to each other, while the lowest coercivity values are found between them [Figures 1(a) and 1(b), respectively]. This results in a well-defined four-fold symmetry indicative of biaxial magnetic anisotropy [2]. In order to verify this result, ferromagnetic resonance (FMR) experiments have been carried out at 9.4 GHz frequency. The angular dependence of the in-plane resonance field at RT for the Fe3O4 layers proves that the easy axes are indeed the in-plane <100> directions (Fig. 2). Furthermore, spin-polarized low-energy electron microscopy (SPLEEM) has allowed imaging the individual magnetic domains at the surface of the films [2]. The magnetic domains present magnetization vectors along the in-plane ¿100¿ directions, while the domain walls are aligned with the in-plane ¿110¿ directions. The most probable cause for the observed magnetization easy-axis direction is the orientation of the anti-phase domain boundaries (APBs). It is known that depending on the orientation of the APBs, they can couple both ferromagnetically or antiferromagnetically the magnetite grains that lie across the boundary. We thus propose that the particular distribution and orientation of APBs that our growth conditions promote are responsible for the observed easy-axis directions of our films. Consequently, all angular studies here shown in addition to SPLEEM experiments demonstrate easy-axis orientation along in-plane <100> directions, i.e., differing from that of bulk magnetite or films prepared by other techniques, and thus demonstrating the possibility of tuning the easy axis orientation in Fe3O4 films.