Discovery of chalcogenides structures and compositions using mixed fluxes.

Advancements in many modern technologies rely on the continuous need for materials discovery. However, the design of synthesis routes leading to new and targeted solid-state materials requires understanding of reactivity patterns1-3. Advances in synthesis science are necessary to increase efficiency and accelerate materials discovery4-10. We present a highly effective methodology for the rational discovery of materials using high-temperature solutions or fluxes having tunable solubility. This methodology facilitates product selection by projecting the free-energy landscape into real synthetic variables: temperature and flux ratio. We demonstrate the effectiveness of this technique by synthesizing compounds in the chalcogenide system of A(Ba)-Cu-Q(O) (Q = S or Se; A = Na, K or Rb) using mixed AOH/AX (A = Li, Na, K or Rb; X = Cl or I) fluxes. We present 30 unreported compounds or compositions, including more than ten unique structural types, by systematically varying the temperature and flux ratios without requiring changing the proportions of starting materials. Also, we found that the structural dimensionality of the compounds decreases with increasing reactant solubility and temperature. This methodology serves as an effective general strategy for the rational discovery of inorganic solids.

Ingrained: An Automated Framework for Fusing Atomic-Scale Image Simulations into Experiments.

To fully leverage the power of image simulation to corroborate and explain patterns and structures in atomic resolution microscopy, an initial correspondence between the simulation and experimental image must be established at the outset of further high accuracy simulations or calculations. Furthermore, if simulation is to be used in context of highly automated processes or high-throughput optimization, the process of finding this correspondence itself must be automated. In this work, "ingrained," an open-source automation framework which solves for this correspondence and fuses atomic resolution image simulations into the experimental images to which they correspond, is introduced. Herein, the overall "ingrained" workflow, focusing on its application to interface structure approximations, and the development of an experimentally rationalized forward model for scanning tunneling microscopy simulation are described.

Synthesis of borophane polymorphs through hydrogenation of borophene.

Synthetic two-dimensional polymorphs of boron, or borophene, have attracted attention because of their anisotropic metallicity, correlated-electron phenomena, and diverse superlattice structures. Although borophene heterostructures have been realized, ordered chemical modification of borophene has not yet been reported. Here, we synthesize "borophane" polymorphs by hydrogenating borophene with atomic hydrogen in ultrahigh vacuum. Through atomic-scale imaging, spectroscopy, and first-principles calculations, the most prevalent borophane polymorph is shown to possess a combination of two-center-two-electron boron-hydrogen and three-center-two-electron boron-hydrogen-boron bonds. Borophane polymorphs are metallic with modified local work functions and can be reversibly returned to pristine borophene through thermal desorption of hydrogen. Hydrogenation also provides chemical passivation because borophane reduces oxidation rates by more than two orders of magnitude after ambient exposure.