Computationally driven experimental discovery of the CeIr${}_4$In compound

We present a combined experimental and computational methodology for the discovery of new materials. Density functional theory (DFT) formation energy calculations allow us to predict the stability of various hypothetical structures. We demonstrate this approach by computationally predicting the Ce-Ir-In ternary phase diagram. We predict previously unknown compounds CeIr${}_4$In and Ce${}_2$Ir${}_2$In to be stable. Subsequently, we successfully synthesize CeIr${}_4$In and characterize it by x-ray diffraction. Magnetization and heat capacity measurements of CeIr${}_4$In are reported. The correct prediction and discovery of CeIr${}_4$In validates this approach for discovering new materials.

Figure 1

Predicted Ce-Ir-In phase diagram. This top-down view of the convex hull of various calculated Ce-Ir-In phases illustrates which are stable at zero temperature. The phases at corners of each facet represent stable compounds. Additionally, some metastable phases found in this work are also plotted according to their compositions. Compounds are numbered following their order in Table .

Figure 2

X-ray powder diffraction of CeIr${}_4$In. Tick marks indicate the expected peak positions based on the MgCu${}_4$Sn structure type. The difference between the experimental (bottom) and calculated (middle) spectrum is shown in the top spectrum. The inset displays the crystal structure of CeIr${}_4$In with Ir forming a network of cornersharing tetrahedra and Ce and In occupying tetrahedral voids.

Figure 3

Magnetic susceptibility of CeIr${}_4$In versus temperature. Upper left inset displays the specific heat of CeIr${}_4$In versus temperature and the lower right inset shows the magnetization as a function of magnetic field at 2 K.