Ab initio equation-of-motion coupled cluster singles and doubles calculations have been carried out oil a variety of 2:1 FH:NH3 complexes (FbHb:FaHa:NH3) to investigate the effects of structural changes on one and two-bond spin-spin Coupling constants across F-a-H-a-N and F-b-H-b-F-a hydrogen bonds and to provide insight into experimentally measured coupling constants for 2:1 FH:collidine (2:1 FH:2,4,6-trimethylpyridine) complexes. Coupling constants have been computed for 2:1 FH:NH3 equilibrium structures and proton-transferred perpendicular and open structures at 2:1 FH:NH3. FH:pyridine, and FH:collidine geometries. (2h)J(Fa-N), and (1)J(Ha-N) and (1h)J(ha-N) exhibit expected dependencies on distances, angles, and the nature of the nitrogen base. In contrast, one- and two-bond coupling constants associated with the F-b-H-b-F-a, hydrogen bond, particularly (2h)J(Fb-Fa) vary significantly depending on the F-F distance, the orientation of the hydrogen-bonded pair, and (2h)J(Fb-Fa), the nature of the complex (HF dimer versus the anion FHF-). The structure of the 2:1 FH:collidine complex proposed on the basis of experimentally measured coupling constants is supported by the computed coupling constants. This study of the structures of open proton-transferred 2:1 FH:NH3, FH:pyridine, and FH:collidine complexes and the coupling constants computed for 2:1 FH:NH3 complexes at these geometries provides insight into the role of the solvent in enhancing proton transfer across both N-H-a-F-a and F-b-H-b-F-a hydrogen bonds.