Pressure - temperature phase diagram of CrSiTe3

van der Waals solids are well known to host remarkable phase diagrams with competing phases, unusual energy transfer processes, and elusive states of matter. Among this class of materials, chalcogenides have emerged as the most flexible and relevant platforms for unraveling charge-structure-function relationships. In order to explore the properties of complex chalcogenides under external stimuli, we measured the far infrared spectroscopic response of CrSiTe3 under extreme pressure-temperature conditions. Analysis of the 368 cm−1 Si-Te stretching mode and the manner in which it is screened by the closure of the indirect gap reveals that the insulator-metal transition takes place immediately after the structural phase transition - once the mixed phase aspect of the lattice distortion is resolved. At the same time, the two-phase region associated with the structural transition widens with decreasing temperature, and the slope of the insulator-metal transition under pressure is consistent with increasing entropy. These trends completely revise the character of the temperature-pressure phase diagram as well as the relationship between the structural and insulator-metal transitions, leading to a critical nexus of activity that may hide a quantum critical point and allow superconductivity to emerge.