We report systematic Cu- and F-NMR measurements of five-layered high-Tc cuprates Ba2Ca4Cu5O10(F,O)2. It is revealed that antiferromagnetism (AFM) uniformly coexists with superconductivity (SC) in underdoped regions, and that the critical hole density
pc for AFM is ~ 0.11 in the five-layered compound. We present the layer-number dependence of AFM and SC phase diagrams in hole-doped cuprates, where pc for n-layered compounds, pc(n), increases from pc(1) ~ 0.02 in LSCO or pc(2) ~ 0.05 in YBCO to pc(5) ~ 0.11. The variation of pc(n) is attributed to interlayer magnetic coupling, which becomes stronger with increasing n. In addition, we focus on the ground-state phase diagram of CuO2 planes, where AFM metallic states in slightly doped Mott insulators change into the uniformly mixed phase of AFM and SC and into simple d-wave SC states. The maximum Tc exists just outside the quantum critical hole density, at which AFM moments on a CuO2 plane collapse at the ground state, indicating an intimate relationship between AFM and SC. These characteristics of the ground state are accounted for by the Mott physics based on the t-J model; the attractive interaction of high-Tc SC, which raises Tc as high as 160 K, is an in-plane superexchange interaction Jin (~ 0.12 eV), and the large Jin binds electrons of opposite spins between neighboring sites. It is the Coulomb repulsive interaction U ~ (> 6 eV) between Cu-3d electrons that plays a central role in the physics behind high-Tc phenomena.
We report on the phase diagram of antiferromagnetism (AFM) and superconductivity (SC) in three-layered Ba_2Ca_2Cu_3O_6(F,O)_2 by means of Cu-NMR measurements. It is demonstrated that AFM and SC uniformly coexist in three-layered compounds as well as
in four- and five-layered ones. The critical hole density p_c for the long range AFM order is determined as p_c ~ 0.075, which is larger than p_c ~ 0.02 and 0.055 in single- and bi-layered compounds, and smaller than p_c ~ 0.08-0.09 and 0.10-0.11 in four- and five-layered compounds, respectively. This variation of p_c is attributed to the magnetic interlayer coupling which becomes stronger as the stacking number of CuO_2 layers increases; that is, the uniform coexistence of AFM and SC is a universal phenomenon in underdoped regions when a magnetic interlayer coupling is strong enough to stabilize an AFM ordering. In addition, we highlight an unusual pseudogap behavior in three-layered compounds -- the gap behavior in low-energy magnetic excitations collapses in an underdoped region where the ground state is the AFM-SC mixed phase.
We report that planar CuO_2 hole densities in high-T_c cuprates are consistently determined by the Cu-NMR Knight shift. In single- and bi-layered cuprates, it is demonstrated that the spin part of the Knight shift K_s(300 K) at room temperature monot
onically increases with the hole density $p$ from underdoped to overdoped regions, suggesting that the relationship of K_s(300 K) vs. p is a reliable measure to determine p. The validity of this K_s(300 K)-p relationship is confirmed by the investigation of the p-dependencies of hyperfine magnetic fields and of spin susceptibility for single- and bi-layered cuprates with tetragonal symmetry. Moreover, the analyses are compared with the NMR data on three-layered Ba_2Ca_2Cu_3O_6(F,O)_2, HgBa_2Ca_2Cu_3O_{8+delta}, and five-layered HgBa_2Ca_4Cu_5O_{12+delta}, which suggests the general applicability of the K_s(300 K)-p relationship to multilayered compounds with more than three CuO_2 planes. We remark that the measurement of K_s(300 K) enables us to separately estimate p for each CuO_2 plane in multilayered compounds, where doped hole carriers are inequivalent between outer CuO_2 planes and inner CuO_2 planes.
We report on the observation of high-T_c superconductivity (SC) emerging with the background of an antiferromagnetic (AFM) order in the five-layered cuprate Ba_2Ca_4Cu_5O_10(F,O)_2 through 19F-NMR and zero-field Cu-NMR studies. The measurements of sp
ectrum and nuclear spin-lattice relaxation rates 19(1/T_1) of 19F-NMR give convincing evidence for the AFM order taking place below T_N = 175 K and for the onset of SC below T_c = 52 K, hence both coexisting. The zero-field Cu-NMR study has revealed that AFM moments at Cu sites are 0.14 mu_B at outer CuO_2 layers and 0.20 mu_B at inner ones. We remark that an intimate coupling exists between the AFM state and the SC order parameter below T_c = 52 K; the spin alignment in the AFM state is presumably changed in the SC-AFM mixed state.
We reexamine the novel phase diagrams of antiferromagnetism (AFM) and high-Tc$ superconductivity (HTSC) for a disorder-free CuO$_2$ plane based on an evaluation of local hole density ($p$) by site-selective Cu-NMR studies on multilayered copper oxide
s. Multilayered systems provide us with the opportunity to research the characteristics of the disorder-free CuO$_2$ plane. The site-selective NMR is the best and the only tool used to extract layer-dependent characteristics. Consequently, we have concluded that the uniform mixing of AFM and SC is a general property inherent to a single CuO$_2$ plane in an underdoped regime of HTSC. The $T$=0 phase diagram of AFM constructed here is in quantitative agreement with the theories in a strong correlation regime which is unchanged even with mobile holes. This {it Mott physics} plays a vital role for mediating the Cooper pairs to make $T_c$ of HTSC very high. By contrast, we address from extensive NMR studies on electron-doped iron-oxypnictides La1111 compounds that the increase in $T_c$ is not due to the development of AFM spin fluctuations, but because the structural parameters, such as the bond angle $alpha$ of the FeAs$_4$ tetrahedron and the a-axis length, approach each optimum value. Based on these results, we propose that a stronger correlation in HTSC than in FeAs-based superconductors may make $T_c$ higher significantly.
Extensive Cu-NMR studies on multilayered high-Tc cuprates have deduced the following results;(1) Antiferromagnetic (AFM) moment M_{AFM} is decreased with doping, regardless of the number of CuO_2 layers n, and collapses around a carrier density N_h =
0.17. (2) The AFM ordering temperature is enhanced as the out-of-plane coupling J_{out} increases with increasing n. (3) The in-plane superexchange J_{in} is invariant with doping, but is even increased. (4) The dome shape of T_c from the underdoped to the overdoped regime with a maximum T_c at N_h = 0.22 does not depend on n, but its maximum value of T_c seems to depend on n moderately. The present results strongly suggest that the AFM interaction plays the vital role as the glue for the Cooper pairs, which will lead us to a genuine understanding of why the T_c of cuprate superconductors is so high.
We report Cu-NMR/NQR and F-NMR studies on the multilayered high-T_c copper oxides Ba_2Ca_{n-1}Cu_nO_{2n}F_2 with n=2,3,4, where n is the number of CuO_2 planes. It is revealed that bi-layered Ba_2CaCu_2O_4F_2 is an underdoped superconductor with hole
carriers, which are introduced into CuO_2 planes by an unexpected deviation from the nominal content of apical fluorines. In a previous paper, we proposed a self-doping mechanism as the origin of carrier doping in n=3 and n=4; in the mechanism, electrons are transferred from the inner CuO_2 plane (IP) to the outer one (OP). However, since it has been found that the bi-layered compound is hole doped, we have reexamined the superconducting and magnetic properties in n=3 and n=4 by Cu-NMR/NQR and F-NMR. The extensive NMR studies have confirmed that the apical-fluorine compounds are not self-doped but hole-doped, and that antiferromagnetism (AFM) and superconductivity (SC) coexist in a single CuO_2 plane. In n=4, the AFM ordering occurs at T_N = 80 K, well above T_c=55 K, where the respective AFM moments are M_AFM=0.11 mu_B and 0.18 mu_B at the OP and the IP. In n=3, on the other hand, the underdoped single IP exhibits a spontaneous moment M_AFM=0.12 mu_B at low temperatures and a peak in the nuclear-spin-lattice relaxation rate 1/T_1 of F at T_N=23 K, much lower than T_c = 76 K. We note that the increase in the number of IPs from one to two leads to an increase in T_N due to strengthening the interlayer coupling, although the doping levels for both compounds are almost comparable. The present results strongly suggest that the uniform mixing of AFM and SC is a general property inherent to a single CuO_2 plane in the underdoped regime for hole-doping.
We report on magnetic characteristics in four-layered high-T_c superconductors Ba_2Ca_3Cu_4O_8(F_yO_{1-y})_2 with apical fluorine through Cu- and F-NMR measurements. The substitution of oxygen for fluorine at the apical site increases the carrier den
sity (N_h) and T_c from 55 K up to 102 K. The NMR measurements reveal that antiferromagnetic order, which can uniformly coexist with superconductivity, exists up to N_h = 0.15, which is somewhat smaller than N_h = 0.17 being the quantum critical point (QCP) for five-layered compounds. The fact that the QCP for the four-layered compounds moves to a region of lower carrier density than for five-layered ones ensures that the decrease in the number of CuO_2 layers makes an interlayer magnetic coupling weaker.
We report Cu- and F-NMR studies on a four-layered high-temperature superconductor Ba2Ca3Cu4O8F2(0234F(2.0)) with apical fluorine (F-1), an undoped 55 K-superconductor with a nominal Cu2+ valence on average. We reveal that this compound exhibits the a
ntiferromagnetism (AFM) with a Neel temperature TN=100 K despite being a Tc= 55 K-superconductor. Through a comparison with a related tri-layered cuprate Ba2Ca2Cu3O6F2 (0223F(2.0)), it is demonstrated that electrons are transferred from the inner plane (IP) to the outer plane (OP) in 0234F(2.0) and 0223F(2.0), confirming the self-doped high-temperature superconductivity (HTSC) having electron and hole doping in a single compound. Remarlably, uniform mixing of AFM and HTSC takes place in both the electron-doped OPs and the hole-doped IPs in 0234F(2.0).
