Ba0.6Sr0.4TiO3 films were deposited by pulsed laser deposition on orthorhombic REScO3(110) (RE = Dy, Gd) single-crystal substrates. Films were investigated for their growth mode, crystalline quality, and strain states. Substrates were treated prior to growth to produce atomically flat surfaces having wide terraces (approximate to 200 nm) and clear unit-cell-high steps. Atomic force microscopy and reflection high-energy electron diffraction indicated that the films grew epitaxially in a two-dimensional (213) layer-by-layer mode. X-ray diffraction showed that all films (200 ran thick and less) were coherently/orthorhombically strained to the substrate according to the epitaxial relationship: (001)(film)parallel to(110)(substrates), [100]film parallel to[001]substrate (and [010](film)parallel to[1 (1) over bar0](substrate)). (002) rocking curves were 17 and 20 arcsec wide for films grown on RE = Dy and Gd, respectively. These films have rocking curve widths and dislocation densities that are several orders of magnitude lower than a film grown on SrTiO3 (001). (c) 2007 Elsevier B.V. All rights reserved.