Tuning Charge Order in (TMTTF)2X by Partial Anion Substitution

Abstract

In the quasi-one-dimensional (TMTTF)2X compounds with effectively quarter-filled bands, electronic charge order is stabilized from the delicate interplay of Coulomb repulsion and electronic bandwidth. The correlation strength is commonly tuned by physical pressure or chemical substitution with stoichiometric ratios of anions and cations. Here, we investigate the charge-ordered state through partial substitution of the anions in (TMTTF)2[AsF6]1−x[SbF6]x with x≈0.3, determined from the intensity of infrared vibrations, which is sufficient to suppress the spin-Peierls state. Our dc transport experiments reveal a transition temperature TCO = 120 K and charge gap ΔCO=430 K between the values of the two parent compounds (TMTTF)2AsF6 and (TMTTF)2SbF6. Upon plotting the two parameters for different (TMTTF)2X, we find a universal relationship between TCO and ΔCO yielding that the energy gap vanishes for transition temperatures TCO≤60 K. While these quantities indicate that the macroscopic correlation strength is continuously tuned, our vibrational spectroscopy results probing the local charge disproportionation suggest that 2δ is modulated on a microscopic level.