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.

Rational design of technologically important exotic perovskites is hampered by the insufficient geometrical descriptors and costly and extremely high-pressure synthesis, while the big-data driven compositional identification and precise prediction entangles full understanding of the possible polymorphs and complicated multidimensional calculations of the chemical and thermodynamic parameter space. Here we present a rapid systematic data-mining-driven approach to design exotic perovskites in a high-throughput and discovery speed of the A2BB’O6 family as exemplified in A3TeO6. The magnetoelectric polar magnet Co3TeO6, which is theoretically recognized and experimentally realized at 5 GPa from the six possible polymorphs, undergoes two magnetic transitions at 24 and 58 K and exhibits helical spin structure accompanied by magnetoelastic and magnetoelectric coupling. We expect the applied approach will accelerate the systematic and rapid discovery of new exotic perovskites in a high-throughput manner and can be extended to arbitrary applications in other families.

The rational design of multifunctional inorganic pigments relies on the manipulation of ionic valence and local surroundings of a chromophore in structurally and chemically habitable hosts. To date, the development of environmentally benign and intense violet/purple pigments is still a challenge. Here we report a family of A 3−x Mn x TeO 6 and A 3−2x Mn x Li x TeO 6 (A = Zn, Mg; x = 0.01−0.15) pigments colored by site-selective Mn 2+ O 4 yellow and Mn 3+ O 5−6 violet chromophores. Zn 2.9 Mn 0.1 TeO 6 is intense bright yellow, comparable with commercial BiVO 4 , and has better near-infrared reflectivity (∼89%) in comparison to commercial TiO 2 . The codoped Li + "activator" generates holes and chargebalanced Mn 3+ (Mn 3+ O 5−6 ), realizing a color transformation from yellow to the bright violet pigments of A 3−2x Mn x Li x TeO 6 . The most vivid Mg 2.8 Mn 0.1 Li 0.1 TeO 6 is probably the best violet pigment known to date, exhibits excellent chemical and thermodynamic stability, and demonstrates pressure-dependent stability up to 5−7 GPa, before a (reversible) phase transition to pink. Theoretical calculations revealed the correlation between site-preference occupancy and chromophore motifs and predicted a wide color gamut of pigments in Zn 3 TeO 6 -hosted 3d transition-metal ions other than manganese.

High-pressure heaters in large volume presses must reconcile potentially contradictory properties, and the whole highpressure and high-temperature (HPHT) community has been engaged for years to seek a better heater. LaCrO 3 (LCO)-based ceramic heaters have been widely applied in multianvil apparatus; however, their performance is far from satisfactory, motivating further research on the chemical optimization strategy and corresponding thermochemical mechanism. Here, we adopted a chemical-screening strategy and manufactured tubular heaters using the electrically, chemically, and mechanically optimized Sr− Cu codoped La 0.9 Sr 0.1 Cr 0.8 Cu 0.2 O 3−δ (LSCCuO-9182). HPHT examinations of cylindrical LSCCuO-9182 heaters on Walker-type multianvil apparatuses demonstrated a small temperature gradient, robust thermochemical stability, and excellent compatibility with high-pressure assemblies below 2273 K and 10 GPa. Thermochemical mechanism analysis revealed that the temperature limitation of the LSCCuO-9182 heater was related to the autoredox process of the Cu dopant and Cr and the exchanging ionic migration of Cu and Mg between the LSCCuO-9182 heater and the MgO sleeve. Our combinatorial strategy coupled with thermochemical mechanism analysis makes the prioritization of contradictory objectives more rational, yields reliable LCO heaters, and sheds light on further improvement of the temperature limitation and thermochemical stability.

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