This readme.txt file was updated on 2023-09-05 by Silu Guo Recommended citation for the data: Guo, Silu; Yun, Hwanhui; Nair, Sreejith; Jalan, Bharat; Mkhoyan, K. Andre. (2023). Supporting data for Mending Cracks Atom-by-atom in Rutile TiO2 with Electron Beam Radiolysis. Retrieved from the Data Repository for the University of Minnesota, https://doi.org/10.13020/ya9y-bp34 ------------------- GENERAL INFORMATION ------------------- Title of Dataset: Supporting Data for Mending Cracks Atom-by-atom in Rutile TiO2 with Electron Beam Radiolysis Author Information: Name: Silu Guo Institution: University of Minnesota Address: Email: guo00208@umn.edu ORCID: Name: Hwanhui Yun Institution: University of Minnesota Address: Email: yunxx133@umn.edu ORCID: Name: Sreejith Nair Institution: University of Minnesota Address: Email: nair0074@umn.edu ORCID: Name: Bharat Jalan Institution: University of Minnesota Address: Email: bjalan@umn.edu ORCID: Name: K. Andre Mkhoyan Institution: University of Minnesota Address: Email: mkhoyan@umn.edu ORCID: Principal Investigator Contact Information Name: K. Andre Mkhoyan Institution: University of Minnesota Address: Email: mkhoyan@umn.edu ORCID: Date of data collection (single date, range, approximate date): 2022-01-18 to 2023-07-13 Geographic location of data collection (where was data collected?): University of Minnesota Information about funding sources that supported the collection of the data: This work was supported primarily by the National Science Foundation (NSF) through the University of Minnesota MRSEC under Award No. DMR-2011401 (B.J. and K.A.M.) and partially through NSF Grant No. DMR-2309431 (K.A.M.). Parts of this work were carried out at the UMN Characterization Facility, supported in part by the NSF through the UMN MRSEC program. The authors acknowledge the Minnesota Supercomputing Institute (MSI) at the University of Minnesota for providing computational resources. Film growth was supported by the U.S. Department of Energy (DOE) through Grant No. DE-SC0020211 (B.J.). -------------------------- SHARING/ACCESS INFORMATION -------------------------- 1. Licenses/restrictions placed on the data: CC0 1.0 Universal 2. Links to publications that cite or use the data: Guo, S., Yun, H., Nair, S., Jalan, B. & Mkhoyan, K. A. Mending cracks atom-by-atom in rutile TiO2 with electron beam radiolysis. Nat Commun 14, 6005 (2023). https://doi.org/10.1038/s41467-023-41781-x 3. Links to other publicly accessible locations of the data: 4. Links/relationships to ancillary data sets: 5. Was data derived from another source? --------------------- DATA & FILE OVERVIEW --------------------- 1. File List for Main Text Figures Figure 1: A. Filename: Fig1_atomic intensity linescan.xlsx Short description: The files contains atomic intensity linescan vs position of the atomic columns in Figure 1b and Figure 1d. Figure 3: A. Filename: Fig_3a_EELS_9 spectra.xslx Short description: The file contains the 9 EELS spectra data exported from .dm3 (Gatan DigitalMicrograph Image Document 3) files corresponding to Figure 3a. B. Filename: Fig_3b_EELS_spectrum data.zip Short description: This zip folder includes 5 EELS spectra .xslx files needed to calculate and plot the pure bulk spectrum and pure surface spectrum in Figure 3b. C. Filename: Fig_3c_data.zip Short description: Composition of bulk and surface .xslx file and its platform function fitting .xslx file for each spectrum presented in Figure 3a. D. Filename: Fig_3d_data.zip Short description: 9 crack-region EELS spectra .xslx file for full range of Ti and O signal as well as 9 EELS spectra .xslx file for O signal range subtracting the background. Figure 4: A: Fig4d_EDX_statistics.zip Short description: This folder includes a brightrow_distance_distribution.xslx file and a darkrow_distance_distribution.xslx file, corresponding to the interstitial position distribution histogram plotted in Figure 4d. B: Fig4e_Fitted_crosssection Short description: This is a .xsls file for the radiolysis cross section fitting using experimental data plotted in Figure 4e. Supplementary Figures: Figure S1: A. Filename: FigS1_crack_images_angle_statistics Short description: The folder includes 12 different cracks images and a Origin file including all the measured wedge angles from the 12 cracks as plotted in Figure S1. Figure S5: A. Filename: FigS6_EELS_bulk_surface_10 spectra each.zip Short description: Two sets of raw EELS spectra taken from bulk region and surface region of rutile TiO2 to calculate the pure bulk and pure surface EELS spectra. The two calculated output spectra files are also included, an additional calculated pure surface file smoothed every ten 10 pixels is also included. Figure S6: A. Filename: FigS7_low_loss_EELS.zip Short description: This folder includes a Full_spectrum.xslx file, a TiO2_Substrate_zero_and_plasma.xslx file, a Gaussian_Fitted_Zero_peak.xslx file and a Lorentzian_Fitted_Plasmon_peak.xslx file that were used to plot Figure S7. Figure S7: A: Filename: FigS8_EELS_fit.zip Short description: The file contains two EELS spectra .xslx files and their corresponding compositional fitting data. Figure S8: A: Filename: FigS9__EELS_integrated_intensity_data.zip Short description: 10 bulk-region EELS spectra .xslx file for full range of Ti and O signal as well as 10 EELS spectra .xslx file for O signal range subtracting the background. Figure S11: A: Filename: FigS11_linscans.xlsx Short description: Atomic intensity linescan data for plot in Figure S11c. Figure S12: A: Filename: FigS12b.xlsx Short description: Electron dose vs electron energy data for stage1 and stage2 in Figure S12b. B: Filename: FigS12c_Fitted_crosssection.xlsx Short description: This is a .xsls file for the radiolysis cross section fitting using experimental data plotted in Figure S12c. Figure S14: A: Filename: FigS14_data.zip Short description: 4 .xslx files for the knock-on cross section curve in Figure S14. Figure S15: A: Filename: FigS15a_Time_per_octa_3voltages.xslx Short description: Calculated time vs electron doses curve plotted in Figure S15a B: Filename: FigS15b_Time_per_octa_3voltages_large_range.xslx Short description: Calculated time vs electron doses curve plotted in Figure S15b 2. Relationship between files: 3. Additional related data collected that was not included in the current data package: 4. Are there multiple versions of the dataset? Y/N -------------------------- METHODOLOGICAL INFORMATION -------------------------- 1. Description of methods used for collection/generation of data: The dataset including high angle annular dark field (HAADF) scanning transmission electron microscopy (STEM) images and electron energy loss spectra (EELS) were obtained on an aberration-corrected FEI Titan G2 60–300 (S)TEM microscope equipped with a CEOS DCOR probe corrector, a Schottky field emission gun, a monochromator, a super-X energy dispersive X-ray (EDX) spectrometer, and a Gatan Enfinium ER spectrometer. 2. Methods for processing the data: EELS data are stored in .dm3 format in Gatan DigitalMicrograph, EELS data background are subtracted using the background subtraction function in Gatan DigitalMicrograph and the spectrum intensities were exported to .xslx format in Microsoft Excel worksheet and plotted in Origin. 3. Instrument- or software-specific information needed to interpret the data: Image files in .tif format can be opened using any image software such as windows photo viewer, etc. EELS data in .xslx format can be opened by Microsoft Excel. 4. Standards and calibration information, if appropriate: Not applicable 5. Environmental/experimental conditions: STEM characterization experiments are done under high vacuum in the microscope 6. Describe any quality-assurance procedures performed on the data: Not applicable 7. People involved with sample collection, processing, analysis and/or submission: Silu Guo ------------------------------ DATA-SPECIFIC INFORMATION For: ------------------------------ Fig1_atomic intensity linescan.xlsx: 1. Number of variables:4 2. Number of columns: 6 3. Missing data codes: Not applicable Code/symbol Definition Code/symbol Definition 4. Variable List: pixel position, intensity in b, intensity in d1, intensity in d2 A. Name: pixel position Description: Columns 1, 3, 5 are pixel position where the atomic intensity is taken Value label: pixel position B. Name: intensity in b, intensity in d1, intensity in d2 Description: Columns 2, 4, 6 are intensity in b, intensity in d1, intensity in d2 Value label: intensity in b, intensity in d1, intensity in d2 Fig_3a_EELS_9 spectra.xslx, Fig3d_EELS_Surface_Oxygen_9_spectra_background_subtracted.xlsx, Fig_3d_EELS_Surface_full range_9 spectra.xlsx: 1. Number of variables:9 2. Number of columns: 9 3. Missing data codes: Not applicable Code/symbol Definition Code/symbol Definition 4. Variable List: Spectrum 1 intensity (arbitrary unit), Spectrum 2 intensity (arbitrary unit), Spectrum 3 intensity (arbitrary unit), Spectrum 4 intensity (arbitrary unit), Spectrum 5 intensity (arbitrary unit), Spectrum 6 intensity (arbitrary unit), Spectrum 7 intensity (arbitrary unit), Spectrum 8 intensity (arbitrary unit), Spectrum 9 intensity (arbitrary unit) A. Name: Spectrum 1-9 intensity (arbitrary unit) Description: Columns 1-9 are EELS Ti-L23 signal intensity from spectrum no.1 to no.9, correspondingly Value label: Spectrum 1-9 intensity (arbitrary unit) Fig3b_Calculated_pure_bulk_spectrum.csv, Fig3b_Calculated_pure_surface_spectrum.csv, Fig_3b_Calculated_pure_surface_spectrum_smooth.csv, Calculated_pure_bulk_spectrum.csv, Calculated_pure_surface_spectrum.csv, Calculated_pure_surface_spectrum_smooth.csv,Full_spectrum.csv, Gaussian_Fitted_Zero_peak.csv, Lorentzian_Fitted_Plasmon_peak.csv, TiO2_Substrate_zero_and_plasmon.csv: 1. Number of variables:2 2. Number of columns: 2 3. Missing data codes: Not applicable Code/symbol Definition Code/symbol Definition 4. Variable List: Spectrum Energy loss (eV), Spectrum intensity (arbitrary unit) A. Name: Spectrum Energy loss (eV) Description: Columns 1 is EELS spectrum energy loss Value label: Spectrum Energy loss (eV) B. Name: Spectrum intensity (arbitrary unit) Description: Columns 2 is EELS spectrum intensity in arbitrary unit Value label: Spectrum intensity (arbitrary unit) Fig3b_EELS_bulk_10_spectra.xlsx, Fig3b_EELS_surface_10 spectra.xlsx, EELS_substrate_10_scans.xlsx, EELS_substrate_O_background_subtraction_10_scans.xlsx: 1. Number of variables:10 2. Number of columns: 10 3. Missing data codes: Not applicable Code/symbol Definition Code/symbol Definition 4. Variable List: Spectrum 1 intensity (arbitrary unit), Spectrum 2 intensity (arbitrary unit), Spectrum 3 intensity (arbitrary unit), Spectrum 4 intensity (arbitrary unit), Spectrum 5 intensity (arbitrary unit), Spectrum 6 intensity (arbitrary unit), Spectrum 7 intensity (arbitrary unit), Spectrum 8 intensity (arbitrary unit), Spectrum 9 intensity (arbitrary unit), Spectrum 10 intensity (arbitrary unit), Averaged Pixel Spectrum intensity from previous 10 columns (arbitrary unit) A. Name: Spectrum 1-10 intensity (arbitrary unit) and Averaged Pixel Spectrum intensity from previous 10 columns (arbitrary unit) Description: Columns 1-10 are EELS Ti-L23 signal intensity from spectrum no.1 to no.10, and column 11 is the averaged pixel spectrum intensity from the first 10 columns Value label: Spectrum 1-10 intensity (arbitrary unit), Averaged Pixel Spectrum intensity from previous 10 columns (arbitrary unit) Composition_trend.csv: 1. Number of variables:2 2. Number of columns: 2 3. Missing data codes: Not applicable Code/symbol Definition Code/symbol Definition 4. Variable List: Spectrum number, Concentration of surface Ti A. Name: Spectrum number Description: Columns 1 is the spectrum number from 1 to 9 Value label: Spectrum number B. Name: Concentration of surface Ti Description: Columns 2 is Concentration of surface Ti Value label: Concentration of surface Ti Composition_w_fit.csv: 1. Number of variables:2 2. Number of columns: 2 3. Missing data codes: Not applicable Code/symbol Definition Code/symbol Definition 4. Variable List: Range from spectrum 1 to spectrum 9, Platform fitting of the concentration trend A. Name: Spectrum number Description: Columns 1 is range from spectrum 1 to spectrum 9 Value label: Range from spectrum 1 to spectrum 9 B. Name: Platform fitting of the concentration trend Description: Columns 2 is Platform fitting of the concentration trend Value label: Platform fitting of the concentration trend brightrow_distance_distribution.xslx and darkrow_distance_distribution.xslx: 1. Number of variables:1 2. Number of columns: 1 3. Missing data codes: Not applicable Code/symbol Definition Code/symbol Definition 4. Variable List: Distance of interstitial Ti atoms from its nearest atomic column (in Å) A. Name: Distance of interstitial Ti atoms from its nearest atomic column (in Å) Description: Columns 1 is the Distance of interstitial Ti atoms from its nearest atomic column (in Å) Value label: Distance of interstitial Ti atoms from its nearest atomic column (in Å) Fig4e_Fitted_crosssection.csv and Fig12c_Fitted_crosssection.csv: 1. Number of variables:2 2. Number of columns: 2 3. Missing data codes: Not applicable Code/symbol Definition Code/symbol Definition 4. Variable List: Electron energy (eV), Fitted radiolysis cross section (10^-8 nm^2) A. Name: Spectrum number Description: Columns 1 is Electron energy (eV) Value label: Electron energy (eV) B. Name: Fitted radiolysis cross section (10^-8 nm^2) Description: Columns 2 is Fitted radiolysis cross section (10^-8 nm^2) Value label: Fitted radiolysis cross section (10^-8 nm^2) Spectrum1_fit_Ib_Is.csv, Spectrum5_fit_Ib_Is.csv: 1. Number of variables:3 2. Number of columns:3 3. Missing data codes: Not applicable Code/symbol Definition Code/symbol Definition 4. Variable List: Spectrum Energy loss (eV), Experimental spectrum intensity (arbitrary unit), Fitted spectrum intensity (arbitrary unit) A. Name: Spectrum Energy loss (eV) Description: Columns 1 is EELS spectrum energy loss Value label: Spectrum Energy loss (eV) B. Name: Experimental spectrum intensity (arbitrary unit) Description: Columns 2 is Experimental spectrum intensity (arbitrary unit) Value label: Experimental spectrum intensity (arbitrary unit) C. Name: Fitted spectrum intensity (arbitrary unit) Description: Columns 3 is Fitted spectrum intensity (arbitrary unit) Value label: Fitted spectrum intensity (arbitrary unit) FigS11_linscans.xlsx: 1. Number of variables:10 2. Number of columns:10 3. Missing data codes: Not applicable Code/symbol Definition Code/symbol Definition 4. Variable List: Pixel position, bright row intensity-1, bright row intensity-2, bright row intensity-3, bright row intensity-4, bright row intensity-5, dim row intensity-1, dim row intensity-2, dim row intensity-3, dim row intensity-4 A. Name: Pixel position Description: Columns 1 is Pixel position for the linescan Value label: Pixel position B. Name: bright row intensity-1 to bright row intensity-5 Description: Columns 2-6 are bright row intensity-1 to bright row intensity-5, correspondingly Value label: bright row intensity-1 to bright row intensity-5 C. Name: dim row intensity-1 to dim row intensity-4 Description: Columns 7-10 are dim row intensity-1 to dim row intensity-4, correspondingly Value label: dim row intensity-1 to dim row intensity-4 FigS12b.xlsx: 1. Number of variables:3 2. Number of columns:3 3. Missing data codes: Not applicable Code/symbol Definition Code/symbol Definition 4. Variable List: Electron energy (keV), Stage 1 doses (e*Å^-2), Stage 2 doses (e*Å^-2) A. Name: Electron energy (keV) Description: Columns 1 is EELS spectrum energy loss Value label: Spectrum Energy loss (eV) B. Name: Stage 1 doses (e*Å^-2) Description: Columns 2 is Stage 1 doses (e*Å^-2) Value label: Stage 1 doses (e*Å^-2) C. Name: Stage 2 doses (e*Å^-2) Description: Columns 3 is Stage 2 doses (e*Å^-2) Value label: Stage 2 doses (e*Å^-2) Oxygen_26eV_Radiolysis_and_KnockOn.csv, Oxygen_39eV_Radiolysis_and_KnockOn.csv, Titanium_39eV_Radiolysis_and_KnockOn.csv, Titanium_47eV_Radiolysis_and_KnockOn.csv: 1. Number of variables:3 2. Number of columns:3 3. Missing data codes: Not applicable Code/symbol Definition Code/symbol Definition 4. Variable List: Electron energy (J), Radiolysis cross section (10^-8 nm^2), Knock-on cross section (10^-8 nm^2) A. Name: Electron energy (J) Description: Columns 1 is EELS spectrum energy loss Value label: Spectrum Energy loss (J) B. Name: Radiolysis cross section (10^-8 nm^2) Description: Columns 2 is Radiolysis cross section (10^-8 nm^2) Value label: Radiolysis cross section (10^-8 nm^2) C. Name: Knock-on cross section (10^-8 nm^2) Description: Columns 3 is Knock-on cross section (10^-8 nm^2) Value label: Knock-on cross section (10^-8 nm^2) FigS15_Time_per_octa_3voltages.csv, FigS15b_Time_per_octa_3voltages_large_range.xslx: 1. Number of variables:4 2. Number of columns:4 3. Missing data codes: Not applicable Code/symbol Definition Code/symbol Definition 4. Variable List: Dose rate (*10^6*e*Å^-2*s^-1), Octahedron flip time under 80 keV, Octahedron flip time under 200 keV, Octahedron flip time under 300 keV A. Name: Dose rate (*10^6*e*Å^-2*s^-1) Description: Columns 1 is Dose rate (*10^6*e*Å^-2*s^-1) Value label: Dose rate (*10^6*e*Å^-2*s^-1) B. Name: Octahedron flip time under 80 keV Description: Columns 2 is Octahedron flip time under 80 keV Value label: Octahedron flip time under 80 keV C. Name: Octahedron flip time under 200 keV Description: Columns 3 is Octahedron flip time under 200 keV Value label: Octahedron flip time under 200 keV D. Name: Octahedron flip time under 300 keV Description: Columns 4 is Octahedron flip time under 300 keV Value label: Octahedron flip time under 300 keV -------------------------- Data Tree ------------------------- | Fig12c_Fitted_crosssection.csv | Fig1_atomic intensity linescan.xlsx | Fig3b_EELS spectrum data.zip | \---3b | Fig3b_Calculated_pure_bulk_spectrum.csv | Fig3b_Calculated_pure_surface_spectrum.csv | Fig3b_EELS_bulk_10_spectra.xlsx | Fig3b_EELS_surface_10 spectra.xlsx | Fig_3b_Calculated_pure_surface_spectrum_smooth.csv | | Fig3c_data.zip | \---3c | Composition_trend.csv | Composition_w_fit.csv | | Fig3d_data.zip | \---3d | Fig3d_EELS_Surface_Oxygen_9_spectra_background_subtracted.xlsx | Fig_3d_EELS_Surface_full range_9 spectra.xlsx | | Fig4d_statistics.zip | \---4d | brightrow_distance_distribution.xslx | darkrow_distance_distribution.xslx: | | Fig4e_Fitted_crosssection.csv | FigS11_linscans.xlsx | FigS12b.xlsx | FigS14_data.zip | \---Supplementary Figure 1 Data | Oxygen_26eV_Radiolysis_and_KnockOn.csv | Oxygen_39eV_Radiolysis_and_KnockOn.csv | Titanium_39eV_Radiolysis_and_KnockOn.csv | Titanium_47eV_Radiolysis_and_KnockOn.csv | | FigS15_Time_per_octa_3voltages.csv | FigS15b_Time_per_octa_3voltages_large_range.xslx | FigS1_crack_images_angle_statistics.zip | \---Supplementary Figure 1 Data | 10cracks_statistics.opju | 11.06.17 Scanning Acquire.tif | 11.53.21filtered.tif | 14.12.17 Scanning Acquire.tif | 14.15.02 Scanning Acquire.tif | 14.37.52 Scanning Acquire-2-Acquire HAADF.tif | 15.36.10 Scanning Acquire-2-Acquire HAADF.tif | 15.36.54 Scanning Acquire-2-Acquire HAADF.tif | 16.42.31 Scanning Acquire.tif | 18.42.04 Scanning Acquire.tif | 20.06.58 Scanning Acquire-2-Acquire HAADF.tif | 20.49.17 Scanning Acquire-2-Acquire HAADF.tif | 21.49.39 Scanning Acquire-2-Acquire HAADF.tif | | FigS5_EELS_bulk_surface_10 spectra each.zip | \---Supplementary Figure 5 Data | Calculated_pure_bulk_spectrum.csv | Calculated_pure_surface_spectrum.csv | Calculated_pure_surface_spectrum_smooth.csv | EELS_substrate_10_scans.xlsx | EELS_surface_10scans.xlsx | | FigS6_low_loss_EELS.zip | \---Supplementary Figure 6 Data | Full_spectrum.csv | Gaussian_Fitted_Zero_peak.csv | Lorentzian_Fitted_Plasmon_peak.csv | TiO2_Substrate_zero_and_plasmon.csv | | FigS7_EELS_fit.zip | \---Supplementary Figure 7 Data | Spectrum1_fit_Ib_Is.csv | Spectrum5_fit_Ib_Is.csv | FigS8_EELS_integrated_intensity_data.zip | \---Supplementary Figure 8 Data | EELS_substrate_10_scans.xlsx | EELS_substrate_O_background_subtraction_10_scans.xlsx | Fig_3a_EELS_9 spectra.xlsx | README_Guo_Silu_072223.txt