High-Field Specific-Heat and Susceptibility Measurements: Relevance to the Spin-Peierls Phase Diagram and the Validity of a Soliton Picture

We discuss recent high-field specific-heat measurements on the spin-Peierls compound tetrathiafulvalinium bis-cis-(1,2-perfluoromethylethylene-1-2-dithiolato)–gold [TTF-BDT(Au)]. An ordering anomaly can clearly be detected which defines a high-field phase boundary, despite some extraneous structure in the data apparently reflecting experimental limitations. The high-field phase boundary is in good quantitative agreement with the theory of Cross and Fisher. Further, the specific-heat data are in good agreement with earlier ac susceptibility data, the reliability of which as indicators of a phase transition has been somewhat open to doubt because pronounced relaxation effects in the high-field regime result in striking differences between χac and χdc. Some observations are made concerning the extent of hysteresis associated with the phase boundary between dimerized and high-field phases. Finally, the extensive experimental data are employed in several tests to determine the applicability of recent soliton theories

Field-Dependent Differential Susceptibility Studies on Tetrathiafulvalene-AuS\u3csub\u3e4\u3c/sub\u3eC\u3csub\u3e4\u3c/sub\u3e(CF\u3csub\u3e3\u3c/sub\u3e)\u3csub\u3e4\u3c/sub\u3e: Universal Aspects of the Spin-Peierls Phase Diagram

An applied magnetic field is known to produce novel effects in the phase behavior of magnetoelastic spin-Peierls systems. Hence we report measurements of the differential susceptibility (χ) and magnetization (M) in fields up to 40 kOe (4 T) on the spin-Peierls compound tetrathiafulvalene (TTF)-AuS4C4(CF3)4 in the temperature region (1.1K \u3c- T \u3c- 4.2K). This range of field and temperature encompasses an interesting phase region, including the zero-field spin-Peierls transition temperature Tc(0)=2.03 K. The measurements of the differential (ac) susceptibility provide a more sensitive probe of the transition behavior than magnetization measurements. The first definitive evidence for significant deviations from mean-field critical behavior appear in these measurements, and the appropriate criteria for determining the precise location of the transitions are thus provided by the thermodynamic theory of λ transitions. Using the new criteria, qualitative and even quantitative agreement is obtained with current theories of the field dependence of spin-Peierls transitions. A novel contour plot of χac in the H − T plane is shown to be useful for the delineation of the global phase-transition behavior. An investigation of the role of relaxation effects in χac relative to the nature of the phase boundaries is conducted. A major feature is the observation of a striking degree of universality in the phase behavior of three spin-Peierls systems TTF-AuS4C4(CF3)4, TTF-AuS4C4(CF3)4, and methylethylmorpholinium di-tetracyanoquinodimethane [MEM-(TCNQ)2]. hese universal features are preserved through considerable differences in lattice structure and a variation in Tc(0) of a factor of 10

Spin-Peierls transitions in magnetic donor-acceptor compounds of tetrathiafulvalene (TTF) with bisdithiolene metal complexes

The spin-Peierls transition is considered as a progressive spin-lattice dimerization occurring below a transition temperature in a system of one-dimensional antiferromagnetic Heisenberg chains. In the simplest theories, the transition is second order and the ground state is a singlet with a magnetic gap. The historical origins and theoretical development of the concept are examined. Magnetic susceptibility and EPR measurements on the π-donor-acceptor compounds TTF·MS4C4(CF3)4 (M=Cu, Au; TTF is tetrathiafulvalene) are reported. These compounds exhibit clearly the characteristics of the spin-Peierls transition in reasonably good agreement with a mean-field theory. The susceptibility of each compound has a broad maximum near 50 K, while the transitions occur at 12 and 2.1 K for M=Cu and Au, respectively. EPR linewidth observations over a broad temperature range are examined. Areas for further experimental and theoretical work are indicated, and a critical comparison is made of related observations on other materials

Observation of a Spin-Peierls Transition in a Heisenberg Antiferromagnetic Linear-Chain System

Magnetic-susceptibility and EPR measurements are reported which provide the first unambiguous evidence for a spin-Peierls transition in a system of linear one-dimensional antiferromagnetic Heisenberg chains. The material studied is TTFCuS4C4(CF3)4 (TFF stands for tetrathiafulvalinium). At 12 K, the spin-lattice system undergoes a second-order phase transition to a singlet ground state

Thermal and magnetic study of exchange in the quasi-1-D molecular compound, TTF⋅PtS\u3csub\u3e4\u3c/sub\u3eC\u3csub\u3e4\u3c/sub\u3e(CF\u3csub\u3e3\u3c/sub\u3e)\u3csub\u3e4\u3c/sub\u3e

Single crystalmagnetic susceptibility results from 2.5 K to 270 K and specific heat results from 3 K to 16 K are reported for TTF⋅PtS4C4(CF3)4, (TTF=tetrathiafulvalene). The combined results are analyzed using a simple model which ignores differences between the two types of S=1/2 spin carriers and involves a system of ferromagnetic chains treated ’’exactly’’, with interchain antiferromagnetic interaction evaluated in a mean field approximation. Above an apparent ordering transition at 8 K, the susceptibility is well described by the model irrespective of whether the ferromagnetic exchange is Heisenberg, Ising or intermediate to these. The magnetic contribution to the specific heat is obtained using earlier results for the isostructural Au compound. Comparison with specific heat calculations for the Heisenberg, Ising and intermediate cases successfully narrows the ambiguity to an intermediate anisotropic exchange close to the Heisenberg limit