Modeling the spin-Peierls transition of spin-$1/2$ chains with correlated states: $J_1-J_2$ model, CuGeO$_3$ and TTF-CuS$_4$C$_4$(CF$_3$)$_4$

Abstract: The spin-Peierls transition at $T_{SP}$ of spin-$1/2$ chains with isotropic exchange interactions has previously been modeled as correlated for $T > T_{SP}$ and mean field for $T < T_{SP}$. We use correlated states throughout in the $J_1-J_2$ model with antiferromagnetic exchange $J_1$ and $J_2 = \alpha J_1$ between first and second neighbors, respectively, and variable frustration $0 \leq \alpha \leq 0.50$. The thermodynamic limit is reached at high $T$ by exact diagonalization of short chains and at low $T$ by density matrix renormalization group calculations of progressively longer chains. In contrast to mean field results, correlated states of 1D models with linear spin-phonon coupling and a harmonic adiabatic lattice provide an internally consistent description in which the parameter $T_{SP}$ yields both the stiffness and the lattice dimerization $\delta(T)$. The relation between $T_{SP}$ and $\Delta(\delta,\alpha)$, the $T = 0$ gap induced by dimerization, depends strongly on $\alpha$ and deviates from the BCS gap relation that holds in uncorrelated spin chains. Correlated states account quantitatively for the magnetic susceptibility of TTF-CuS$4$C$_4$(CF$_3$)$_4$ crystals ($J_1 = 79$ K, $\alpha = 0$, $T{SP} = 12$ K) and CuGeO$3$ crystals ($J_1 = 160$ K, $\alpha = 0.35$, $T{SP} = 14$ K). The same parameters describe the specific heat anomaly of CuGeO$_3$ and inelastic neutron scattering. Modeling the spin-Peierls transition with correlated states exploits the fact that $\delta(0)$ limits the range of spin correlations at $T = 0$ while $T > 0$ limits the range at $\delta= 0$.