The dataset contains 44 molecular dynamic trajectories for the interaction of chlorine trifluoride with a monohydrogenated silicon surface, obtained using the CASTEP computer code. Output is provided in the form of *.md and .castep files produced by the code. The former contains position, velocity, and force data, which may be visualised using commonly available software, such as the Jmol code. The latter contains human-readable data concerning electronic spin during each trajectory, together with sufficient information about computational parameters to enable replication of the calculations. Also provided are results of single-point calculations (.den_fmt and .castep formats) that were used to extract information on atom-resolved charge and spin at specific times during the simulations. Results of geometry optimisation calculations (.geom and *.castep formats) are also included, which were used to obtain adsorption heats following-on from the end of each dynamic simulation.

For more information see also the ReadMe file.