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These datasets contain experimental time-, polarization-, and angle-resolved photoemission spectroscopy (tr-ARPES) measurements of tin-sulfide (SnS), as well as corresponding theoretical simulations based on the time-dependent density functional theory (TDDFT). They support the findings reported in the publication: Fragkos et al., "Symmetry-Driven Floquet Engineering in Multivalley SnS" (2026). README.txt files are included, offering a detailed overview of the dataset contents. Additional metadata associated with each dataset are provided in separate metadata files. Acknowledgments This work is supported by the Cluster of Excellence 'CUI: Advanced Imaging of Matter' of the Deutsche Forschungsgemeinschaft (DFG) - EXC 2056 - project ID 39071599 and the European Research Council (ERC-2024-SyG- 101167294 ; UnMySt), We acknowledge support from the Max Planck-New York City Center for Non-Equilibrium Quantum Phenomena. The Flatiron Institute is a division of the Simons Foundation. We acknowledge the financial support of the IdEx University of Bordeaux/Grand Research Program "GPR LIGHT". This work is part of the ULTRAFAST and TORNADO projects of PEPR LUMA and was supported by the French National Research Agency, as a part of the France 2030 program, under grants ANR-23-EXLU-0002 and ANR-23-EXLU-0004. We acknowledge support from ERC Starting Grant ERC-2022-STG No. 101076639, the Marie Skłodowska-Curie Doctoral Networks TIMES No. 101118915 and SPARKLE No. 101169225, Quantum Matter Bordeaux, AAP CNRS Tremplin, AAP SMR from Université de Bordeaux, from the Italian Ministry of University and Research (MUR) under the PRIN 2022738 Grant No. 2022PX279E 003, and from the Next Generation EU Partenariato Esteso NQSTI-Spoke 2 (THENCE-740PE00000023) and MUR D.M. 737/2021 “Materials Manipulation with Light”. S.F. acknowledges funding from the European Union’s Horizon Europe research and innovation programme under the Marie Skłodowska-Curie 2024 Postdoctoral Fellowship No. 101198277 (TopQMat). The views and opinions expressed herein do not necessarily reflect those of the European Commission. Neither the European Union nor the granting authority can be held responsible for them.