We report on the preparation and characterization of epitaxial thin films of the double-perovskite Sr 2 CrWO 6 by Pulsed Laser Deposition (PLD). On substrates with low lattice mismatch like SrTiO 3 , epitaxial Sr 2 CrWO 6 films with high crystalline quality can be grown in a molecular layer-by-layer growth mode. Due to the similar ionic radii of Cr and W, these elements show no sublattice order. Nevertheless, the measured Curie temperature is well above 400 K. Due to the reducing growth atmosphere required for double perovskites, the SrTiO 3 substrate surface undergoes an insulator-metal transition impeding the separation of thin film and substrate electric transport properties. [5]. Thin films of the well studied system Sr 2 FeMoO 6 have been fabricated by pulsed-laser deposition (PLD) at relatively high temperatures of about 900 • C [6]. However, epitaxial growth was found to be complicated and difficult to control. There are indications that high structural quality of films grown on SrTiO 3 is associated with semiconducting behavior [7,8]. Here, we report on the epitaxial growth of Sr 2 CrWO 6 . Due to the good lattice match, epitaxial films of this material can be grown on SrTiO 3 substrates in a molecular layer-by-layer growth mode resulting in high crystalline quality.Sr 2 CrWO 6 thin films were deposited from stoichiometric targets [5] on atomically flat, HF etched and annealed (001) SrTiO 3 substrates by PLD using a 248 nm KrF excimer laser [9]. Fig. 1 shows the RHEED (Reflection High Energy Electron Diffraction) [10] intensity oscillations of the (0, 0) diffraction spot recorded during the PLD growth of a c-axis oriented Sr 2 CrWO 6 film. The molecular layer-bylayer or Frank-van der Merwe growth mode [11] is achieved for a substrate temperature of 740 • C, an argon pressure of 2 × 10 −4 Torr, a laser repetition rate of 2 Hz, and a laser energy density on the target of 1.2 J/cm 2 . RHEED was performed with 15 keV electrons at an incident angle of about 2 • . To obtain the number of RHEED oscillations per unit cell, the film thickness has been determined precisely by X-ray reflectometry (Fig. 4) and then divided by the number of observed RHEED oscillations. The derived molecular layer or block thickness corresponds to half a unit cell (c/2 = 4.004Å). Note that the intensity oscillations of the (0,0) and (0,1) spot are out of phase, since for the (0,1) spot the electrons reflected from different growth planes interfere constructively (in-Bragg condition). In this case no RHEED oscillations are expected. The fact that we do observe RHEED oscillations is caused by multiple and diffuse, incoherent scattering which results in an * Electronic address: Boris.Philipp@wmi.badw.de increasing (decreasing) intensity with increasing (decreasing) step density [12,13]. Figure 2 shows an in situ AFM picture of a 42 nm thick film. Clearly, a terrace structure due to the nonvanishing substrate miscut with about 4Å high steps corresponding to half a unit cell of Sr 2 CrWO 6 can be seen. The AFM analysis shows that Sr 2 CrW...