Abstract
We report the synthesis of bulk, highly oriented, crystalline 4H hexagonal silicon (4H-Si), through a metastable phase transformation upon heating the single-crystalline Si_{24} allotrope. Remarkably, the resulting 4H-Si crystallites exhibit an orientation relationship with the Si_{24} crystals, indicating a structural relationship between the two phases. Optical absorption measurements reveal that 4H-Si exhibits an indirect band gap near 1.2eV, in agreement with first principles calculations. The metastable crystalline transition pathway provides a novel route to access bulk crystalline 4H-Si in contrast to previous transformation paths that yield only nanocrystalline-disordered materials.
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