This PDF file includes:

• Supplementary Materials and Methods
• scheme S1. Synthesis of BPP34C10DAM from BPP34C10DA.
• fig. S1. Schematic representation of the fabrication procedure to form graphene field-effect transistor arrays.
• fig. S2. Optical microscopic images of graphene devices with different magnification.
• fig. S3. Characterization of an indented nanogap array.
• fig. S4. Solid-state electrical characterization.
• fig. S5. Reproducibility and differential conductance spectra.
• fig. S6. Schematic processes used to fabricate molecular devices.
• fig. S7. Control experiments using a partially cleaved graphene ribbon device.
• fig. S8. Control experiments using an OPEDAM-connected device.
• figs. S9 to S12. Real-time measurements of host-guest dynamics in SMJs at the device-liquid interface.
• fig. S13. Thermodynamic analyses of SMJ devices.
• fig. S14. ¹H NMR titration.
• fig. S15. Thermodynamic analyses of SMJ devices.
• figs. S16 to S19. Host-guest kinetics analysis.
• fig. S20. Host-guest kinetics analysis.
• fig. S21. Geometric optimizations of BPP34C10 and MV²⁺⊂BPP34C10 complexes.
• tables S1 to S6. Binding constants.
• table S7. Chemical shifts for 1H NMR titrations in CD₃SOCD₃.
• table S8. Chemical shifts for 1H NMR titrations in D₂O.
• tables S9 to S14. Dissociation (k_d) and association (k_a) rate constants.

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