Max-Planck-Institut for Solid State Research
Using 63Cu NMR, we establish that the enhancement of spin order by a magnetic field H in YBa2Cu3O6.45 arises from a competition with superconductivity because the effect occurs for H perpendicular, but not parallel, to the CuO2 planes, and it persists up to field values comparable to Hc2. We also find that the spin-freezing has a glassy nature and that the frozen state onsets at a temperature which is independent of the magnitude of H. These results, together with the presence of a competing charge-ordering instability at nearby doping levels, are strikingly parallel to those previously obtained in La-214. This suggests a universal interpretation of magnetic field effects in underdoped cuprates where the enhancement of spin order by the field may not be the primary phenomenon but rather a byproduct of the competition between superconductivity and charge order. Low-energy spin fluctuations are manifested up to relatively high temperatures where they partially mask the signature of the pseudogap in 1/T1 data of planar Cu sites.
A central difficulty of state-specific Multi-Reference Coupled Cluster (MR-CC) formalisms concerns the definition of the amplitudes of the single and double excitation operators appearing in the exponential wave operator. If the reference space is a complete active space (CAS) the number of these amplitudes is larger than the number of singly and doubly excited determinants on which one may project the eigenequation, and one must impose additional conditions. The present work first defines a state-specific reference-independent operator T~^m\hat{\tilde{T}}^m which acting on the CAS component of the wave function Ψ0m|\Psi_0^m \rangle maximizes the overlap between (1+T~^m)Ψ0m(1+\hat{\tilde{T}}^m)|\Psi_0^m \rangle and the eigenvector of the CAS-SD CI matrix ΨCASSDm|\Psi_{\rm CAS-SD}^m \rangle. This operator may be used to generate approximate coefficients of the Triples and Quadruples, and a dressing of the CAS-SD CI matrix, according to the intermediate Hamiltonian formalism. The process may be iterated to convergence. As a refinement towards a strict Coupled Cluster formalism, one may exploit reference-independent amplitudes provided by (1+T~^m)Ψ0m(1+\hat{\tilde{T}}^m)|\Psi_0^m \rangle to define a reference-dependent operator T^m\hat{T}^m by fitting the eigenvector of the (dressed) CAS-SD CI matrix. The two variants, which are internally uncontracted, give rather similar results. The new MR-CC version has been tested on the ground state potential energy curves of 6 molecules (up to triple-bond breaking) and a two excited states. The non-parallelism error with respect to the Full-CI curves is of the order of 1 mEhE_{\rm h}.
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