LiSn, the Most Lithium-Rich Binary Stannide: A Combined Experimental and Computational Study.

From reaction of excess lithium with tin, we isolate well-crystallized LiSn and solve the crystal structure from single-crystal X-ray diffraction data. The orthorhombic structure (space group ) features the same coordination polyhedra around tin and lithium as previously predicted by electronic structure calculations for this composition, however differently arranged. An extensive analysis, including thermodynamic integration using Langevin dynamics in combination with a machine-learning potential (moment tensor potential), is conducted to understand the thermodynamic stability of this LiSn structure observed in our experiments.