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In the all-organic paramagnetic correlated metal ${\ensuremath{\beta}}^{\ensuremath{''}}\text{\ensuremath{-}}{(\text{BEDT}\text{\ensuremath{-}}\mathrm{TTF})}_{2}{\mathrm{SF}}_{5}{\mathrm{CH}}_{2}{\mathrm{CF}}_{2}{\mathrm{SO}}_{3}$ spin fluctuations can be ruled out as the glue to superconductivity below ${T}_{c}=5.5$ K. Instead, we demonstrate the coupling of charge degrees of freedom to the superconducting state, which occurs adjacent to a charge-ordered insulating phase. A comparison to isostructural ${\ensuremath{\beta}}^{\ensuremath{''}}\text{\ensuremath{-}}{(\mathrm{BEDT}\text{\ensuremath{-}}\mathrm{TTF})}_{2}{\mathrm{SF}}_{5}R{\mathrm{SO}}_{3}$ compounds reveals that superconductivity is suppressed when the system is tuned away from the insulator towards the metal; an enhanced charge imbalance, on the other hand, leads to an increase in ${T}_{c}$, suggesting an involvement of charge fluctuations. By locally probing the charge disproportionation through the superconducting transition, we discover slight modifications of the Fano coupling constant and intensity at ${T}_{c}$, indicating the effect of the paired electrons on the molecular vibrations.

Coexistence of charge order and superconductivity in β″−(BEDT−TTF)2SF5CH2CF2SO3