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Register a new userToward the Mott state with Magnetic Cluster Formation in Heavily Cu-Doped NaFe$_{1-x}$Cu$_{x}$As
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Recent neutron scattering measurements indicate that NaFe$_{1-x}$Cu$_{x}$As forms an antiferromagnetic stripe phase near $xapprox 0.5$ in a Mott insulating state. This copper concentration is well in excess of that required for superconductivity, $x < 0.04$. We have investigated the development of magnetism in this compound using $^{23}$Na nuclear magnetic resonance (NMR) spectra and spin-lattice relaxation measurements performed on single crystals ($x$ = 0.13, 0.18, 0.24, and 0.39). We find multiple inequivalent Na sites, each of which is associated with a different number of nearest neighbor Fe sites occupied by a Cu dopant. We show that the distribution of Cu substituted for Fe is random in-plane for low concentrations ($x = 0.13$ and 0.18), but deviates from this with increasing Cu doping. As is characteristic of many pnictide compounds, there is a spin pseudo gap that increases in magnitude with dopant concentration. This is correlated with a corresponding increase in orbital NMR frequency shift indicating a change in valence from Cu$^{2+}$ to a Cu$^{1+}$ state as $x$ exceeds 0.18, concomitant with the change of Fe$^{2+}$ to Fe$^{3+}$ resulting in the formation of magnetic clusters. However, for $xleq 0.39$ there is no evidence of long-range static magnetic order.
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Neutron scattering measurements have demonstrated that the heavily Cu-doped NaFe$_{1-x}$Cu$_{x}$As compound behaves like a Mott insulator exhibiting both real space Fe-Cu stripes, as well as antiferromagnetism below a Neel temperature for $xlesssim 0.5$. We have investigated evolution of structural and magnetic ordering using $^{23}$Na and $^{75}$As NMR for single crystals ($x$ = 0.39 and 0.48), confirming antiferromagnetism in the form of magnetic stripes. We show that end-chain defects in these stripes are the principal source of magnetic disorder and are responsible for cluster spin-glass transitions in both compounds, in the latter case coexistent with antiferromagnetism. Aided by our numerical simulation of the $^{75}$As spectra, we show that a staggered magnetization at the Fe sites is induced by non-magnetic Cu dopants.
A central question in a large class of strongly correlated electron systems, including heavy fermion compounds and iron pnictides, is the identification of different phases and their origins. It has been shown that the antiferromagnetic (AFM) phase in some heavy fermion compounds is induced by Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction between localized moments, and that the competition between this interaction and Kondo effect is responsible for quantum criticality. However, conclusive experimental evidence of the RKKY interaction in pnictides is lacking. Here, using high resolution $^{23}$Na NMR measurements on lightly Cu-doped metallic single crystals of NaFeCuAs ~($x approx 0.01$) and numerical simulation, we show direct evidence of the RKKY interaction in this pnictide system. Aided by computer simulation, we identify the $^{23}$Na NMR satellite resonances with the RKKY oscillations of spin polarization at Fe sites. Our NMR results indicate coexistence of local and itinerant magnetism in lightly Cu-doped NaFeCuAs.
Heavily doped Ba$_{1-x}$K$_{x}$Mn$_{2}$As$_{2}$ ($x$=0.19 and 0.26) single crystals were successfully grown, and investigated by the measurements of resistivity and anisotropic magnetic susceptibility. In contrast to the antiferromagnetic insulating ground state of the undoped BaMn$_{2}$As$_{2}$, the K-doped crystals show metallic conduction with weak ferromagnetism below $sim$50 K and Curie-Weiss-like in-plane magnetic susceptibility above $sim$50 K. Under high pressures up to 6 GPa, the low-temperature metallicity changes into a state characterized by a Kondo-like resistivity minimum without any signature of superconductivity above 2.5 K. Electronic structure calculations for $x$=0.25 using $2times2times1$ supercell reproduce the hole-doped metallic state. The density of states at Fermi energy have significant As 4$p$ components, suggesting that the 4$p$ holes are mainly responsible for the metallic conduction. Our results suggest that the interplay between itinerant 4$p$ holes and local 3$d$ moments is mostly responsible for the novel metallic state.
A series of high quality NaFe$_{1-x}$Cu$_x$As single crystals has been grown by a self-flux technique, which were systematically characterized via structural, transport, thermodynamic, and high pressure measurements. Both the structural and magnetic transitions are suppressed by Cu doping, and bulk superconductivity is induced by Cu doping. Superconducting transition temperature ($T_c$) is initially enhanced from 9.6 to 11.5 K by Cu doping, and then suppressed with further doping. A phase diagram similar to NaFe$_{1-x}$Co$_x$As is obtained except that insulating instead of metallic behavior is observed in extremely overdoped samples. $T_c$s of underdoped, optimally doped, and overdoped samples are all notably enhanced by applying pressure. Although a universal maximum transition temperature ($T_c^{max}$) of about 31 K under external pressure is observed in underdoped and optimally doped NaFe$_{1-x}$Co$_x$As, $T_c^{max}$ of NaFe$_{1-x}$Cu$_x$As is monotonously suppressed by Cu doping, suggesting that impurity potential of Cu is stronger than Co in NaFeAs. The comparison between Cu and Co doping effect in NaFeAs indicates that Cu serves as an effective electron dopant with strong impurity potential, but part of the doped electrons are localized and do not fill the energy bands as predicted by the rigid-band model.
The parent compounds of iron-based superconductors are magnetically-ordered bad metals, with superconductivity appearing near a putative magnetic quantum critical point. The presence of both Hubbard repulsion and Hunds coupling leads to rich physics in these multiorbital systems, and motivated descriptions of magnetism in terms of itinerant electrons or localized spins. The NaFe$_{1-x}$Cu$_x$As series consists of magnetically-ordered bad metal ($x=0$), superconducting ($xapprox0.02$) and magnetically-ordered semiconducing/insulating ($xapprox0.5$) phases, providing a platform to investigate the connection between superconductivity, magnetism and electronic correlations. Here we use X-ray absorption spectroscopy and resonant inelastic X-ray scattering to study the valence state of Fe and spin dynamics in two NaFe$_{1-x}$Cu$_x$As compounds ($x=0$ and 0.47). We find that magnetism in both compounds arises from Fe$^{2+}$ atoms, and exhibits underdamped dispersive spin waves in their respective ordered states. The dispersion of spin excitations in NaFe$_{0.53}$Cu$_{0.47}$As is consistent with being quasi-one-dimensional. Compared to NaFeAs, the band top of spin waves in NaFe$_{0.53}$Cu$_{0.47}$As is slightly softened with significantly more spectral weight of the spin excitations. Our results indicate the spin dynamics in NaFe$_{0.53}$Cu$_{0.47}$As arise from localized magnetic moments and suggest the iron-based superconductors are proximate to a correlated insulating state with localized iron moments.
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