High-pressure
solid-state synthesis advances boost discoveries
of new materials and unusual phenomena but endures stringent recipe
conditions, poor yield, and high cost. A methodological approach for
accelerated and precisely high-pressure synthesis is therefore highly
desired. Here, we take the exotic double-perovskite-related nonmagnetic
Li2
B
+4
B′+6O6 as an example to show the pipeline of data-mining,
high-throughput calculations, experimental realization, and chemical
interception of metastable phases. A total of 140 compounds in 7 polymorph
categories were initially screened by the convex hull, which left
∼50% candidates in chemical space on the phase diagram of pressure-dependent
polymorph evolution. Li2TiWO6 and Li2TiTeO6 were singled out for experimental testing according
to the predicted map of crystal structure, function, and synthesis
parameters. Computation on surface energy effect and interfacial chemical
strain suggested that the as-made high-pressure R3-Li2TiTeO6 polymorph cannot be intercepted
below a critical nanoscale but can be stabilized in heterojunction
film on a selected compressive substrate at ambient pressure. The
developed methodology is expected to accelerate the big-data-driven
discovery of generic chemical formula-based new materials beyond perovskites
by high-pressure synthesis and shed light on the large-scale stabilization
of metastable phases under mild conditions.