This is the dataset for the publication on 'Advanced Materials Interfaces' with publication DOI: 10.1002/admi.202201340. The dataset contains the raw trARPES experimental data and the normalized magnetic x-ray diffraction amplitude dynamics (published in https://doi.org/10.1038/s42005-020-00407-0) of GdRh2Si2. - 'trARPES_T_20K_static_MX_cube.nxs' contains a cube of trARPES intensity along the MX cut of the surface Brillouin zone presented in Figure 1-b. - 'trARPES_T_20K_fl_(number).nxs' series contain temporal evolution of raw trARPES intensity measured at sample temperature of 20 K with pump fluence of (number) mJ/cm^2. Figure 2 a-d, 3, 4, 5 b-d, B1, C1 used these trARPES intensity evolution. - 'trARPES_T_150K_fl_(number).nxs' series contain temporal evolution of raw trARPES intensity measured at sample temperature of 150 K (above T_N) with pump fluence of (number) mJ/cm^2. Figure A1 used these trARPES intensity evolution. - 'trRXD_T_20K_fl_(number).txt' series contain temporal evolution of AF order parameter of GdRh2Si2 measured at sample temperature of 20 K with pump fluence of (number) mJ/cm^2. Figure 2-e, 4, 5 used these trRXD amplitude evolution.

We thank the Helmholtz-Zentrum Berlin f ̈ur Materialien und Energie for the allocation of synchrotronradiation beamtime. The experimental support of the staff at beamlines UE56/1 (HZB), X11MA (SLS), and PM3 (HZB) is gratefully acknowledged. This work received funding from the Deutsche Forschungsgemeinscahft (DFG, German Research Foundation) within the Emmy Noether program (Grant No. RE 3977/1), within the Transregio TRR 227 - 328545488 Ultrafast Spin Dynamics (Projects A03, A08, and A09), within TRR 288 - 422213477 (Project A03), SFB1143 (No. 247310070) and within Grant No. 282 KR3831/5-1. Funding was also received from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (Grant Agreement Number ERC-2015-CoG-682843). We also thank support from the Spanish Ministry of Science and Innovation, project PID2020-116093RB-C44, funded by MCIN/ AEI/10.13039/501100011033.

{"references": ["Windsor, Y.W., Ernst, A., Kummer, K. et al. Deterministic control of an antiferromagnetic spin arrangement using ultrafast optical excitation. Commun Phys 3, 139 (2020). https://doi.org/10.1038/s42005-020-00407-0"]}