Redistribution of electronic charges in spin-Peierls state in
  (TMTTF)2AsF6 observed by 13C NMR

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Abstract

We report ^{13}C NMR spectra and nuclear spin lattice relaxation rate 1/T_1 for a quasi-one-dimensional quarter-filled organic material (TMTTF)_{2}AsF_{6}, which undergoes charge ordering (T_{{CO}} = 102 K) and spin-Peierls phase transitions (T_{{SP}} = 14 K). The ratio of two 1/T_1 for the charge accepting and donating TMTTF sites which grows from T_{CO} finally saturates in approaching T_{{SP}}, indicating one spin correlation function even in the charge ordered state. Below T_{{SP}}, however, the doubly split NMR lines from inequivalently charged molecules merge into one line, originated from the variation in charge densities. This shows that a rearrangement of the charge configuration occurs at T_{{SP}}.

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Competition and coexistence of bond and charge orders in (TMTTF)2AsF6

A. Baur, F. Zamborszky, B. Alavi … (2002)

(TMTTF)2AsF6 undergoes two phase transitions upon cooling from 300 K. At Tco=103 K a charge-ordering (CO) occurs, and at Tsp(B=9 T)=11 K the material undergoes a spin-Peierls (SP) transition. Within the intermediate, CO phase, the charge disproportionation ratio is found to be at least 3:1 from carbon-13 NMR 1/T1 measurements on spin-labeled samples. Above Tsp, up to about 3Tsp, 1/T1 is independent of temperature, indicative of low-dimensional magnetic correlations. With the application of about 0.15 GPa pressure, Tsp increases substantially, while Tco is rapidly suppressed, demonstrating that the two orders are competing. The experiments are compared to results obtained from calculations on the 1D extended Peierls-Hubbard model.

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Bond and charge density waves in the isotropic interacting two-dimensional quarter-filled band and the insulating state proximate to organic superconductivity

Rudolf Clay (2009)

We report two surprising results regarding the nature of the spatial broken symmetries in the two-dimensional (2D), quarter-filled band with strong electron-electron interactions. First, in direct contradiction to the predictions of one-electron theory, we find a coexisting ``bond-order and charge density wave'' (BCDW) insulating ground state in the 2D rectangular lattice for all anisotropies, including the isotropic limit. Second, we find that the BCDW further coexists with a spin-density wave (SDW) in the range of large anisotropy. Further, in contrast to the interacting half-filled band, in the interacting quarter-filled band there are two transitions: first, a similar singlet-to-AFM/SDW transition for large anisotropy and second, an AFM/SDW-to-singlet transition at smaller anisotropy. We discuss how these theoretical results apply to the insulating states that are proximate to the superconducting states of 2:1 cationic charge-transfer solids (CTS). An important consequence of this work is the suggestion that organic superconductivity is related to the proximate Coulomb-induced BCDW, with the SDW that coexists for large anisotropies being also a consequence of the BCDW, rather than the driver of superconductivity.