Methods for depositing silicon on a semiconductor or metallic surface include cycling dosing of silane and chlorosilane precursors at a temperature between 50° C. and 300° C., and continuing cycling between three and twenty three cycles until the deposition self-limits via termination of surface sites with Si—H groups. Methods of layer formation include depositing a chlorosilane onto a substrate to form a first layer, wherein the substrate is selected from the group consisting of InxGa1-xAs, InxGa1-xSb, InxGa1-xN, SiGe, and Ge, wherein X is between 0.1 and 0.99. The methods may include pulsing a silane to form a silicon monolayer and cycling dosing of the chlorosilane and the silane. Layered compositions include a first layer selected from the group consisting of InxGa1-xAs, InxGa1-xSb, InxGa1-xN, SiGe, and Ge, wherein X is between 0.1 and 0.99, and a second layer, wherein the second layer comprises Si—H and Si—OH.