Science Advances

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• fig. S1. Schematic illustration of the deposition system.
  
• fig. S2. Sequential gas-phase reaction of MoS₂ on Si wafers.
  
• fig. S3. Influence of t_p of MoCl₅ on the uniform growth zone.
  
• fig. S4. Elemental and structural analyses of thin MoS₂ films.
  
• fig. S5. Elemental analysis of annealed CMS layers.
  
• fig. S6. High-resolution XPS spectra of the annealed CMS layers in Mo (3d), S (2p), Cu (2p), and Cl (2p) regions.
  
• fig. S7. Raman spectra of MoS₂ (300 cycles) grown on Au.
  
• fig. S8. The Mott-Schottky measurement of MoS₂ on an Au/Si substrate.
  
• fig. S9. The Hall effect measurements of MoS₂ on 500-nm-thick SiO2/Si.
  
• fig. S10. Arrhenius plot of the resistivity from Hall effect measurements on ALD-grown MoS2/SiO2 (500 nm)/Si.
  
• fig. S11. SEM images of the as-grown CMS layers.
  
• fig. S12. Thickness dependence of ALD films and Mo contents as a function of position.
  
• fig. S13. HER activities from the CMS samples with thickness gradient.
  
• fig. S14. Schematic illustration of the structural evolution of BLHJs upon annealing.
  
• fig. S15. Low-magnification TEM micrograph of our CMS layers upon annealing (500°C for ~1 hour under N₂ flow) to give an overview of the structures that consist of layered MoS₂ and the superstructures of Chevrel clusters (marked by yellow and blue arrows, respectively).
  
• fig. S16. XRD patterns of our CMS on Cu subjected to different thermal treatments.
  
• fig. S17. EDX elemental analysis of our TiO₂/CMS/Cu structures.
  
• fig. S18. EDX line scan results for the TiO₂/CMS/Cu structures.
  
• fig. S19. Detailed elemental maps of our CMS layers shown in Fig. 1E (main text), indicative of the origin of local variations in the detected elements.
  
• fig. S20. HR-TEM image of annealed CMS to give an overview of the local surface termination.
  
• fig. S21. Schematic of our three–electrode cell used for HER experiments.
  
• fig. S22. Surface morphology of TiO₂-coated annealed CMS.
  
• fig. S23. Estimation of electrochemically active surface area of our CMS material by double-layer capacitance measurements.
  
• fig. S24. XPS analyses of CMS materials to check possible contamination of noble metals.
  
• fig. S25. Stability against scanning of the present CMS system (10,000 times).
  
• fig. S26. XPS analyses of TiO₂/CMS after stability tests.
  
• fig. S27. Reproducibility tests in the electrocatalytic performance of CMS and NMS materials.
  
• fig. S28. Electrochemical analysis and HER of the CMS layers with a non-Pt counter electrode (that is, graphite).
  
• fig. S29. UPS spectra.
  
• fig. S30. Optical absorption of amorphous TiO₂ grown on quartz glass.
  
• fig. S31. Energy band diagrams and the corresponding circuit models of various structures.
  
• fig. S32. HER measurements of our 40-nm-thick TiO₂ with different control samples.
  
• fig. S33. KPFM study of our CMS on Cu.
  
• fig. S34. Local transport study of our annealed CMS/Cu samples.
  
• fig. S35. Comparison between our CMS/TiO₂ and various HER materials (32) in the electrocatalytic performance.
  
• fig. S36. TEM image of the NMS layer as prepared to give an overview of the structures that densely consist of layered MoS₂.
  
• fig. S37. ALD cycle–dependent HER performance of annealed CMS.
  
• fig. S38. HR-TEM image of a CMS layer annealed at 700°C.
  
• fig. S39. Linear sweep voltammetry of the CMS layers annealed at different temperatures.
  
• table S1. Summary of the catalytic performance of various materials for the hydrogen evolution reaction, reported in the literature.
  
• Reference (48)

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