Characterization of localized hole states in Pr_(1+x)Ba_(2-x)Cu_(3)O_(6+y) by nuclear magnetic resonance

TL;DR

This study uses NMR and NQR to analyze charge distribution and localized hole states in Pr_{1+x}Ba_{2-x}Cu_{3}O_{6+y} crystals, revealing the localization of holes in CuO2 planes and the presence of two Pr-states affecting magnetic properties.

Contribution

It provides a detailed NMR-based characterization of hole localization and Pr-states in Pr-based cuprates, integrating experimental data with neutron scattering results.

Findings

Holes are localized in CuO2-plane O 2p - pi-orbitals.

Pr-resonance is assigned to Pr at RE-sites.

Two Pr-states are identified with different magnetic properties.

Abstract

We investigated the charge distribution in Pr_{1+x}Ba_{2-x}Cu_3O_{6+y}-crystals at liquid-He temperature by means of ^{63,65}Cu- and ^{141}Pr-NMR and NQR. The electric field gradients determined for the different oxygen coordinations of Cu(1) on the chains confirm the model that the hole states are localized in the O 2p - pi-orbitals of the CuO_(2)-planes. The intensity and line-shape analysis of the Cu(1)- and Pr-resonances in the oxygen doping series (x approx 0, y=0..1) and in the Pr/Ba solid-solution series (at y=1) allows us to assign the Pr-resonance to Pr at RE-sites. Therefore, we can investigate the charge distribution in the CuO_(2)-Pr-CuO_(2)-layers by crystal field analysis of the Pr-signal. To consistently describe our results with neutron scattering data we propose that two Pr-states are present in the RE-layer, and ascribe them to Pr with and one without a hole localized in the oxygen coordination shell. NMR detects only the former, with a virtually nonmagnetic singlet ground state, while space-integral techniques are dominated by the latter, due to a quasi-doublet ground state and antiferromagnetism of its Pr-moments at low temperature.