Science Advances

Supplementary Materials

This PDF file includes:

  • Section S1. AFM images of prepared (001) STO substrates
  • Section S2. Details of the DFT-constrained fitting of specular reflectivity curves
  • Section S3. Calculated specular reflectivity curves of model STO (001) surfaces
  • Section S4. Calculated specular reflectivity curves of model thin-film structures
  • Section S5. Details of the SXRD characterization of the bare (001) substrates
  • Section S6. Details of the SXRD characterization of the surface structures after the T/L and L/T deposition sequences
  • Section S7. Details of the SXRD characterization of the surface structure after 1-ML LaO deposition
  • Section S8. Determining the optimal weighting between the experimental data and DFT-derived structures
  • Section S9. Determining the fraction of the coherent sum for the T/L and L/T reflectivity data
  • Section S10. Fit parameters for the diffuse scattering component after deposition of the initial LaO and TiO2 MLs
  • Section S11. Ex situ AFM images taken after the T/L and L/T depositions
  • Fig. S1. Surface morphologies of (001)-oriented STO substrates prepared using the etch-and-anneal method described in (2) by AFM.
  • Fig. S2. Calculated specular reflectivity curves of single-layer SrO (1 × 1-S) and TiO2 (1 × 1-T) surface terminations and TiO2 DL (1 × 1-TT) surface termination.
  • Fig. S3. Calculated specular reflectivity curves of several TiO2 DL STO (001) surface reconstructions under 15.0-keV NR conditions and 16.1-keV R conditions for absorption at the Sr K-edge.
  • Fig. S4. DFT-derived structures of possible layer sequences after deposition of LaO (L) and/or TiO2 (T) ML(s) on a TiO2 DL–terminated STO (001) surface and their calculated specular reflectivity curves.
  • Fig. S5. Fitted specular reflectivity curves taken after the LaO ML deposition in the T/L deposition sequence, in which the surface is modeled as a mixture of TLTL, TTL, TL, and TT model structures.
  • Fig. S6. Construction of a Pareto frontier to determine the optimal weighting between the experimental data and DFT-derived structures.
  • Fig. S7. Determination of the fraction of the coherent sum in fitting the specular reflectivity data for the T/L and L/T structures.
  • Fig. S8. Ex situ AFM images taken after the T/L and L/T deposition sequences.
  • Table S1. Measures of the deviations of the fitted atomic positions from the DFT-derived minimum-energy positions (zrms and Edist) and the goodness of fit (χ2) for the bare (001) STO substrates modeled using the RT13 and RT2 reconstructions.
  • Table S2. Measures of the deviations of the fitted atomic positions from the DFT-derived minimum-energy positions (zrms and Edist) and the goodness of fit (χ2) for the surfaces resulting after the T/L and L/T deposition sequences, modeled using the TLTT and TLT model structures.
  • Table S3. Measures of the deviations of the fitted atomic positions from the DFT-derived minimum-energy positions (zrms and Edist) and the goodness of fit (χ2) for the final structures modeled as mixtures of the TLTL, TTL, TL, and TT surface structures.
  • Table S4. Fit parameters for the diffuse scattering component after depositing the initial LaO and TiO2 MLs on each (001) STO substrate (STO #1 and STO #2).
  • References (5761)

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