The barocaloric effect is a promising means of achieving solid-state refrigeration. For this reason, the recent discovery that the coordination framework TPrA[Mn(dca)3] has a “giant” barocaloric coefficient is both scientifically exciting and potentially technologically exploitable. Exploiting this effect will require a detailed understanding of its origin at the atomic scale; yet so far, neither the structure nor the dynamics of this material have been determined under pressure. Here we begin to resolve this situation by proposing a diffraction study on GEM, using a gas cell to investigate the effect of small pressure increments on the structure. Our results will be important in their own right, but will also form the basis of a proposal for EPSRC funding to study these materials’ dynamics via subsequent neutron spectroscopy experiments.