This dataset includes the original data used to draft the manuscript for the publication "Room-Temperature Solid-State Nitrogen-Based Magneto-Ionics in CoxMn1−xN Films" (DOI: 10.1002/adfm.202404487). The data includes the magnetic response of CoMnN layers with varying Co composition, as well as the temperature dependence of the Co0.55Mn0.45N layer, which had the highest magneto-ionic response. Additionally, the structural XRD and HRTEM characterization of the samples is also provided for all compositions, and specifically for the Co0.55Mn0.45N after electrically actuating it. Composition studies to check how the nitrogen evolved after the electric actuation on the Co0.55Mn0.45N is also provided in the form of EELS mappings and line scans, as well as positron lifetime studies. Finally, the oxidation state of the Co and Mn comprised in the Co0.55Mn0.45N layer was studied by synchrotron polarized XAS tecniques, before and after electric actuation, with a temperature dependence, the data of which is also supplied in the dataset. The origin of the magnetic changes after the electric actuation are succesfully correlated to the structural and chemical evolution of the sample, resulting in a new pathway for low-energy spintronic devices.

METHODOLOGICAL INFORMATION

1. Description of methods used for collection-generation of data: Various experimental tools were employed in this line of work, such as reactive magnetron sputtering for the material growth, magnetometry for magneto-electric study at room temperature (VSM) and low temperatures (SQUID), transmission electron microscopy for structural and elemental study, and positron annihilation spectroscopy for defect inspections, polarized absorption spectroscopy for magnetic and valence fine resolution.

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 diamagnetic background was subtracted using the VSM software in our lab, or a specific homemade code. 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 at ambient pressure. Temperature ranged from room temperature to liquid helium temperature depending on the experiment. Structural analysis were always conducted at 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 the field has been approved, and its imminent publication in Advanced Functional Materials is expected.