Enhanced step coverage and reduced resistivity of a TaSiN layer may be achieved when a semiconductor device is manufactured by: forming an interlayer insulating layer on a semiconductor substrate, the interlayer insulating layer having a contact hole that partially exposes the substrate; depositing a TaN thin film on the interlayer insulating layer and in the contact hole using a reaction gas containing a Ta precursor and a nitrogen source gas; removing impurities from the TaN thin film; forming a TaSiN thin film by reacting the impurity-removed TaN thin film with a silicon source gas, and repeating the TaN-depositing, impurity-removing, and silicon source gas-reacting steps.