Spontaneous formation of nanostructures during pulsed laser deposition of epitaxial half-Heusler TiNiSn on MgO(001) Robert W.H. Webster,1* John E. Halpin,1 Srinivas R. Popuri,2 Jan-Willem G. Bos,2 Donald A. MacLaren.1** 1 SUPA, School of Physics and Astronomy, University of Glasgow, G12 8QQ, United Kingdom 2 Institute of Chemical Sciences and Centre for Advanced Energy Storage and Recovery, School of Engineering and Physical Sciences, Heriot-Watt University, Edinburgh EH14 4AS, United Kingdom *Email: rwebster@physics.org **Email: dmaclaren@physics.org Understanding the filenames --------------------------- All data-files included have been named to easily relate data to the figures they contribute to. The filename can be broken down into "Figure#_SampleDetails_DataType.extension" Atomic Force Microscopy data (Figure 1) --------------------------------------- The raw AFM data are Veeco nanoscope files which can be read by the free-to-use Gwyddion software (http://www.gwyddion.net/). Reflection High-Energy Electron Diffraction data (Figures 1 & 2) ---------------------------------------------------------------- The original RHEED patterns which contribute to figures 1 & 2 are provided as images in the TIFF format. X-ray Diffraction data (Figure 3) --------------------------------- XRD data are provided in the csv file '.csv' with a header including the relevant metadata. Transmission Electron Microscopy (Figures 4 through 9) ------------------------------------------------------ Raw data is recorded in Gatan's Digital Micrograph file format (details at the time of writing are advertised at: http://www.gatan.com/products/tem-analysis/gatan-microscopy-suite-software. This file format is readable by open source software package HyperSpy (http://hyperspy.org/). All data was acquired using a JEOL ARMcFEG instrument at 200kV, equipped with a Gatan Quantum electron spectrometer for EELS measurements. Spectrum imaging is performed by first collecting a dark field 'survey image' then acquiring data within a sub-region indicated within the survey image. For the datasets used here, two EELS spectra (low-loss and core loss) are recorded; the file names generally indicate the nature of each subset of the data. Note that metadata within the DM3 files may not be accurate, particularly user-inputted details of the sample and 'session info.' STEM data are generally collected using a 40 micron condenser aperture with 'spot size 4,6 or 8' JEOL ARM configuration and a camera length of 20mm. Processing of EELS data uses methods similar to those presented in references 34-36 of the manuscript.