Single crystals of MAPI were grown from γ-butyrolactone (GBL) by the temperature-rising method with procedures similar to previous works (36). The binary precursors, PbI2 (5 N; Sigma-Aldrich) and methylammonium iodide (Sigma-Aldrich), were mixed with a stochiometric ratio of 1:1 in GBL solvent at 60° to 70°C to form a 1.4 M solution. To facilitate the growth of single crystals, the as-prepared solution was then gradually heated to 100°–110°C. Once single crystals had nucleated, the solution temperature was kept constant to promote the continuous growth of large crystals. The as-grown single crystals were harvested after a period of several hours, yielding a cubic centimeter–sized single crystal with large and flat facets suitable for THz spectroscopy.

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