A method of layer formation on a substrate with high aspect ratio features is disclosed. The layer is formed from a gas mixture comprising one or more process gases and one or more etch species. The one or more process gases react to deposit a material layer on the substrate. In conjunction with the material layer deposition, the etch species selectively remove portions of the deposited material layer adjacent to high aspect ratio feature openings, filling such features in a void-free and/or seam-free manner. The material layer may be deposited on the substrate using physical vapor deposition (PVD) and/or chemical vapor deposition (CVD) techniques.