temperature. In contrast to the selenium analogs TMTSF which are one-dimensional metals, the sulfur salts are semiconductors with localized spins on the TMTTF dimers. Taking into account the thermal expansion of the crystals at high temperature (TϾ20 K) the ESR intensity of all sulfur compounds can be described as a spin-1/2 antiferromagnetic Heisenberg chain with exchange constants 420рJ р500 K. Although the TMTSF compounds are one-dimensional organic metals down to 10 K, the temperature dependence of the spin susceptibility can also be described within the framework of the Hubbard model in the limit of strong Coulomb repulsion with JϷ1400 K. By modeling (TMTTF) 2 ClO 4 as an alternating spin chain, the change of the alternation parameter at the first-order phase transition (T AO ϭ72.5 K) indicates a tetramerization of the chain. (TMTTF) 2 PF 6 undergoes a spin-Peierls transition at T SP ϭ19 K which can be well described by Bulaevskii's model with a singlet-triplet gap ⌬ (0)ϭ32.3 K. We find evidence of antiferromagnetic fluctuations at temperatures well above the magnetic ordering in (TMTTF) 2 Br, (TMTSF) 2 PF 6 , and (TMTSF) 2 AsF 6 which follow the critical behavior expected for three-dimensional ordering. (TMTTF) 2 PF 6 and (TMTTF) 2 Br show one-dimensional lattice fluctuations.