This dataset contains the information on our recent body of work on the study of magneto-ionic properties in structure/composition-engineered ternary nitrides and all the relevant data files. Magneto-ionics, an emerging approach to manipulate magnetism that relies on voltage-driven ion motion, holds the promise to boost energy efficiency in information technologies such as spintronic devices or future non-von Neumann computing architectures. For this purpose, stability, reversibility, endurance, and ion motion rates need to be synergistically optimized. Among various ions, nitrogen has demonstrated superior magneto-ionic performance compared to classical species such as oxygen or lithium. Here, we show that ternary Co1−xFexN compound exhibits an unprecedented nitrogen magneto-ionic response. Partial substitution of Co by Fe in binary CoN is shown to be favorable in terms of generated magnetization, cyclability and ion motion rates. Specifically, the Co0.35Fe0.65N films exhibit an induced saturation magnetization of 1500 emu cm–3, a magneto-ionic rate of 35.5 emu cm–3 s–1 and endurance exceeding 103 cycles. These values significantly surpass those of other existing nitride and oxide systems. This improvement can be attributed to the larger saturation magnetization of Co0.35Fe0.65 compared to individual Co and Fe, the nature and size of structural defects in as-grown films of different composition, and the dissimilar formation energies of Fe and Co with N in the various developed crystallographic structures.

METHODOLOGICAL INFORMATION

1. Description of methods used for collection-generation of data: Various experimental tools were employed in this line of work, such as magnetron sputter for the materials growth, magnetometry for magneto-electric study, transmission electron microscopy for structural study, and positron annihilation spectroscopy for defect inspections.

2. Methods for processing the data: The data files can be processed using Origin software, PowerPoint, and DigitalMicrograph.

3. Instrument- or software- specific information needed to interpret the data: For the magnetometry data, any antiferromagnetic signals were subtracted using the VSM software in our lab. The format of this dataset was converted into an open format that can be processed using Origin software.

4. Instruments, calibration and standards information: The VSM magnetometer was calibrated using a standard nickel pallet provided by the company (Micro Sense, LOT, Quantum Design). Magnetization data is shown in the paper as magnetic moment divided by the effective volume of the films.

5. Environmental or experimental conditions: The measurements were conducted in ambient conditions.

6. Quality-assurance procedures performed on the data: The results were carefully analyzed and interpreted. Peer review process of the corresponding scientific article by experts in this field has been done, and its imminent publication in Journal of Materiomics is expected.