Spectroscopic Indications of Tunnel Barrier Charging as the Switching Mechanism in Memristive Devices B Arndt, F Borgatti, F Offi, M Phillips, P Parreira, T Meiners, S Menzel, K Skaja, G Panaccione, D MacLaren*, R Waser, and R Dittmann Adv. Funct. Mater. 2017, 1702282 doi: 10.1002/adfm.201702282 * Contact E-mail: Donald.MacLaren@glasgow.ac.uk Raw data files, typically 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). Data were acquired using a JEOL ARMcFEG instrument operated at 200kV, using a Gatan Quantum electron spectrometer for EELS measurements, typically collected using the spectrum imaging methodology (see manuscript for details). 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) and dark field images from two detectors ('Gatan DF' and 'Gatan HAADF') 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 7,8 or 9' JEOL ARM configuration and a camera length of 20mm. (S)TEM and EELS data used to compile figs 4, 5 and S5 are provided here. The data derive from a larger set of scans and images that were used to check for consistency and reproducibility but which are not included here. Figure 4 All graphs were created using the spectrum imaging dataset with the file prefix N3_03. See manuscript for details on data processing. Figure 5 (a) Datasets N3_01, N3_04 (both set 'On' to low resistance state), N2_04, and N2_05 (both 'off' and high resistance state. (b) Datasets N2_05 and N3_04 (LRS,HRS, respectively) (c) Datasets N2_04 and N3_03 (LRS,HRS, respectively) (d) Datasets N2_05 and N3_02 (LRS,HRS, respectively) Files N2_0001.dm3 - N2_0003.dm3 provide some low-magnification overviews of the lamella produced for TEM/STEM imaging. The file N3_03_SI Survey Image.dm3 was also used for fig. S5; the inset to that figure was produced using the fast fourier transform algorithm within Digital Micrograph.