Readme for Documentation of Research Datasets Readme Creator: Kloß, Simon D. Readme Creation Date: 2026-10-21 ______________________________ Research Dataset Title: Data to Complex magnetism in a transition metal nitride DOI of Publication Data Collection Location: Institut Laue-Langevin (ILL), Grenoble, France; Ludwig-Maximilians-Universität München, Germany Version: 1.0 Version Changes: - Publisher: Open Data LMU, Universitätsbibliothek der Ludwig-Maximilians-Universität München Publisher Identifier: https://ror.org/05591te55 ______________________________ Dataset Creator 1: Werhahn, Dominik Creator 1 Affiliation: Ludwig-Maximilians-Universität München Contributor 1: Drötboom, Felix Contributor 1 Affiliation: Ludwig-Maximilians-Universität München Contributor 1 Type: Researcher Contributor 2: Steinberg, Simon Contributor 2 Affiliation: RWTH Aachen University Contributor 2 Type: Researcher Contributor 3: Attfield, J. Paul Contributor 3 Affiliation: University of Edinburgh, Centre for Science at Extreme Conditions Contributor 3 Type: Researcher Contributor 4: Ritter, Clemens Contributor 4 Affiliation: Institut Laue-Langevin, Grenoble Contributor 4 Type: DataCollector Contributor 5: Kloß, Simon D. Contributor 5 Affiliation: Ludwig-Maximilians-Universität München Contributor 5 Identifier: https://orcid.org/0000-0002-7188-5729 Contributor 5 Type: Principal Investigator ______________________________ Project Name: Complex magnetism in a transition metal nitride ______________________________ Abstract: This dataset contains powder X-ray diffraction, powder neutron diffraction and magnetization data of Ca2CoN2, a transition metal nitride with Co(II) in linear two-fold coordination. The compound was synthesized from Ca3N2, Co and NaN3 at 8 GPa and ca. 800 °C using a multianvil large-volume press and crystallizes in the Na2HgO2-type structure (tetragonal, space group I4/mmm, no. 139) with lattice parameters a = 3.57175(9) Å, c = 12.4127(6) Å and V = 158.35(1) Å3 at 295 K. Powder neutron diffraction (D20, ILL) shows an incommensurate double-k spin density wave below TN = 54 K with propagation vectors (k 0 0) and (0 k 0), k = 0.5665(1) at 5 K, and magnetic moments aligned along the c axis (maximum amplitude 5.00(3) µB at 5 K and 3.21(7) µB at 46 K). The magnetic susceptibility follows the Curie-Weiss law between 150 and 300 K (µeff = 5.04(1) µB, Weiss temperature Θ = −222.7(2) K) and shows a broad maximum at 62 K, indicating dominant antiferromagnetic exchange and magnetic frustration on the body-centred tetragonal lattice. Temperature-dependent powder X-ray diffraction between 50 and 950 °C documents the thermal expansion and the decomposition of the compound above ca. 600 °C. Magnetic Data Collection: Magnetization data were collected with the vibrating sample magnetometer option of a Quantum Design Physical Property Measurement System (PPMS). Temperature-dependent susceptibility (MVST) was measured in a field of 30 kOe (3 T) from 300 to 1.9 K and in a field of 100 Oe from 1.9 to 300 K. Field-dependent magnetization (MVSH) was measured at constant temperatures of 1.9 and 300 K in fields between -50 and +50 kOe. The sample was placed in a polyethylene capsule of known diamagnetic contribution. The files contain the uncorrected instrument data (moment in emu). Correction for Diamagnetic Contribution of Capsule: diamagnetic_correction = 0.000000148 - (0.00000000906 * Field) Powder X-ray Data Collection: Powder X-ray diffraction data were obtained on a Stoe StadiP diffractometer with monochromatized Mo-Kα1 radiation (Ge(111) monochromator) and a MYTHEN 1K Si-strip detector. The air-sensitive sample was measured in a glass capillary (0.5 mm outer diameter). Data cover 2θ = 2.000-60.275° in steps of 0.015°. Rietveld refinements were carried out with TOPAS Academic V6. Temperature-dependent powder X-ray diffraction data were collected on a Stoe StadiP diffractometer equipped with a graphite furnace and an image-plate position sensitive detector (Mo-Kα1 radiation). The sample was loaded in a quartz capillary (0.4 mm outer diameter) in a glovebox and measured under exclusion of atmosphere. Data were collected from 50 to 950 °C in steps of 20 °C (46 patterns, 2θ = 2.998-78.013° in steps of 0.015°). The three-digit number in the file name is the temperature in °C. Powder Neutron diffraction data collection: Data were collected on 13-14 June 2024 at the high-intensity two-axis powder diffractometer D20 of the Institut Laue-Langevin (experiment 5-21-1195, doi:10.5291/ILL-DATA.5-21-1195) with a take-off angle of 42° and a wavelength of 2.42 Å (as given in the file headers; ca. 2.4 Å in the manuscript). Long scans were recorded at 5 K (6 h), 46 K (1.25 h) and 100 K (1.25 h, 5 h and 6 h). The files named 5K-100K+20000 and 46K-100K+4167 are difference patterns I(5 K) - I(100 K) + 20000 and I(46 K) - I(100 K) + 4167, respectively (constant offsets added to keep intensities positive). The temperature-dependent data (folder T-dependence) are 33 short scans of 900 s each, recorded during a continuous heating ramp from 7 to 98 K (ramp 0.1 K per 20 s). The run number of the ILL is given in the file name together with the sample temperature from the file header. Each neutron file contains 2959 data points (2θ = 0.03-149.63° in steps of 0.05°) in three columns: 2θ (°), intensity and estimated standard deviation, preceded by a six-line ILL header. Rietveld refinements were carried out with FullProf; magnetic propagation vectors were determined with K-Search (FullProf suite). Keywords: nitride, transition metal nitride, Ca2CoN2, Na2HgO2-type, spin density wave, incommensurate magnetic structure, frustrated magnetism, body-centred tetragonal lattice, powder neutron diffraction, magnetic susceptibility, high-pressure synthesis, solid-state chemistry, Rietveld refinement. Data Collection Method: Synthesis via high-pressure high-temperature conditions (8 GPa, ca. 800 °C) in a multianvil large-volume press from Ca3N2 (22.5 wt-% excess), Co and NaN3 as nitrogen source/oxidant. Powder X-ray diffraction (laboratory, including temperature-dependent measurements),powder neutron diffraction (D20, ILL; 5-100 K), and magnetometry (PPMS-VSM, 1.9-300 K, up to 50 kOe). Further methods described in the associated publication (synchrotron powder diffraction at ESRF ID22, DFT calculations with VASP) are not part of this dataset. ______________________________ File List: (Run List is included in File Structure where needed) File Structure: top-level folder contains the powder X-ray pattern; subfolders PPMS, PND (with subfolder T-dependence) and HTXRD contain the magnetization, neutron and temperature-dependent X-ray data, respectively. Powder X-ray diffraction: Ca2CoN2_PXRD.xy Magnetization (PPMS-VSM); MVST = M vs. T, MVSH = M vs. H: PPMS/Ca2CoN2_MVSH_1_9K_5T.DAT PPMS/Ca2CoN2_MVSH_300K_5T.DAT PPMS/Ca2CoN2_MVST_100OE_1_9K-300K.DAT PPMS/Ca2CoN2_MVST_3T_300-1_9K.DAT Powder neutron diffraction, long scans (D20, 2.42 Å): PND/Ca2CoN2_100K_1_25h_2_42A.dat PND/Ca2CoN2_100K_5h_2_42A.dat PND/Ca2CoN2_100K_6h_2_42A.dat PND/Ca2CoN2_46K-100K+4167_1_25h_2_42A.dat PND/Ca2CoN2_46K_1_25h_2_42A.dat PND/Ca2CoN2_5K-100K+20000_6h_2_42A.dat PND/Ca2CoN2_5K_6h_2_42A.dat Powder neutron diffraction, temperature-dependent short scans (D20, 2.42 Å; Ca2CoN2_Tdep_run__2_42A.dat): PND/T-dependence/Ca2CoN2_Tdep_run257258_7K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257259_9K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257260_12K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257261_14K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257262_16K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257263_18K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257264_21K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257265_23K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257266_25K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257267_27K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257268_29K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257269_32K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257270_34K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257271_36K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257272_38K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257273_41K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257274_43K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257275_45K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257276_47K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257277_49K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257278_52K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257279_54K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257280_56K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257281_58K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257282_63K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257283_67K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257284_72K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257285_76K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257286_80K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257287_85K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257288_89K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257289_94K_2_42A.dat PND/T-dependence/Ca2CoN2_Tdep_run257290_98K_2_42A.dat Temperature-dependent powder X-ray diffraction (number = temperature in °C): HTXRD/Ca2CoN2_HTXRD_050.xy HTXRD/Ca2CoN2_HTXRD_070.xy HTXRD/Ca2CoN2_HTXRD_090.xy HTXRD/Ca2CoN2_HTXRD_110.xy HTXRD/Ca2CoN2_HTXRD_130.xy HTXRD/Ca2CoN2_HTXRD_150.xy HTXRD/Ca2CoN2_HTXRD_170.xy HTXRD/Ca2CoN2_HTXRD_190.xy HTXRD/Ca2CoN2_HTXRD_210.xy HTXRD/Ca2CoN2_HTXRD_230.xy HTXRD/Ca2CoN2_HTXRD_250.xy HTXRD/Ca2CoN2_HTXRD_270.xy HTXRD/Ca2CoN2_HTXRD_290.xy HTXRD/Ca2CoN2_HTXRD_310.xy HTXRD/Ca2CoN2_HTXRD_330.xy HTXRD/Ca2CoN2_HTXRD_350.xy HTXRD/Ca2CoN2_HTXRD_370.xy HTXRD/Ca2CoN2_HTXRD_390.xy HTXRD/Ca2CoN2_HTXRD_410.xy HTXRD/Ca2CoN2_HTXRD_430.xy HTXRD/Ca2CoN2_HTXRD_450.xy HTXRD/Ca2CoN2_HTXRD_470.xy HTXRD/Ca2CoN2_HTXRD_490.xy HTXRD/Ca2CoN2_HTXRD_510.xy HTXRD/Ca2CoN2_HTXRD_530.xy HTXRD/Ca2CoN2_HTXRD_550.xy HTXRD/Ca2CoN2_HTXRD_570.xy HTXRD/Ca2CoN2_HTXRD_590.xy HTXRD/Ca2CoN2_HTXRD_610.xy HTXRD/Ca2CoN2_HTXRD_630.xy HTXRD/Ca2CoN2_HTXRD_650.xy HTXRD/Ca2CoN2_HTXRD_670.xy HTXRD/Ca2CoN2_HTXRD_690.xy HTXRD/Ca2CoN2_HTXRD_710.xy HTXRD/Ca2CoN2_HTXRD_730.xy HTXRD/Ca2CoN2_HTXRD_750.xy HTXRD/Ca2CoN2_HTXRD_770.xy HTXRD/Ca2CoN2_HTXRD_790.xy HTXRD/Ca2CoN2_HTXRD_810.xy HTXRD/Ca2CoN2_HTXRD_830.xy HTXRD/Ca2CoN2_HTXRD_850.xy HTXRD/Ca2CoN2_HTXRD_870.xy HTXRD/Ca2CoN2_HTXRD_890.xy HTXRD/Ca2CoN2_HTXRD_910.xy HTXRD/Ca2CoN2_HTXRD_930.xy HTXRD/Ca2CoN2_HTXRD_950.xy File Formats: .DAT (Quantum Design PPMS-VSM, comma-separated text with header), .dat (ILL D20 ASCII), .xy (two-column text: 2θ in °, intensity)