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We carry out density functional theory calculation to enhance the Rashba spinsplitting (RSS) of BiTeI by modifying the interlayer interaction. It is shownthat RSS increases as the Te layer approaches to adjacent Bi layer or the Ilayer recedes from the Bi layer. Our results indicate that the RSS can besensitively increased by introducing a vacancy on the Te site to make effectiveBi-Te distance shorter. It is also found that the difference of Te p orbitalcharacter between two spin-split bands increases when the RSS is developedalong crystal momentum, which supports asymmetric interlayer interaction in thespin-split bands. Our work suggests that the modification of interlayerinteraction is an effective approach in the modeling of the RSS in BiTeI andother layered materials.

Enhancement of Giant Rashba Splitting in BiTeI under Asymmetric Interlayer Interaction