ConspectusThe application of high pressure adds an additional dimension to chemical phase space, opening up an unexplored expanse bearing tremendous potential for discovery. Our continuing mission is to explore this new frontier, to seek out new intermetallic compounds and new solid-state bonding. Simple binary elemental systems, in particular those composed of pairs of elements that do not form compounds under ambient pressures, can yield novel crystalline phases under compression. Thus, high-pressure synthesis can provide access to solid-state compounds that cannot be formed with traditional thermodynamic methods. An emerging approach for the rapid exploration of composition–pressure–temperature phase space is the use of hand-held high-pressure devices known as diamond anvil cells (DACs). These devices were originally developed by geologists as a way to study minerals under conditions relevant to the earth’s interior, but they possess a host of capabilities that make them ideal for high-pressure solid-s...