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We investigated the magnetic properties of (La$_{1-x}$Ba$_{x}$)(Zn$_{1-x}$Mn$_{x}$)AsO with $x$ varying from 0.005 to 0.05 at an external magnetic field of 1000 Oe. For doping levels of $x$ $\leq$ 0.01, the system remains paramagnetic down to the lowest measurable temperature of 2 K. Only when the doping level increases to $x$ = 0.02 does the ferromagnetic ordering appear. Our analysis indicates that antiferromagnetic exchange interactions dominate for $x$ $\leq$ 0.01, as shown by the negative Weiss temperature fitted from the magnetization data. The Weiss temperature becomes positive, i.e., ferromagnetic coupling starts to dominate, for $x$ $\geq$ 0.02. The Mn-Mn spin interaction parameter $\mid$$2J/k_B$$\mid$ is estimated to be in the order of 10 K for both $x$ $\leq$ 0.01 (antiferromagnetic ordered state) and $x$ $\geq$ 0.02 (ferromagnetic ordered state). Our results unequivocally demonstrate the competition between ferromagnetic and antiferromagnetic exchange interactions in carrier-mediated ferromagnetic systems., Comment: 9 pages, 3 figures

Electronic structure of single crystalline Ba(Zn$_{0.875}$Mn$_{0.125}$)$_{2}$As$_{2}$, parent compound of the recently founded high-temperature ferromagnetic semiconductor, was studied by high-resolution photoemission spectroscopy (ARPES). Through systematically photon energy and polarization dependent measurements, the energy bands along the out-of-plane and in-plane directions were experimentally determined. Except the localized states of Mn, the measured band dispersions agree very well with the first-principle calculations of undoped BaZn$_{2}$As$_{2}$. A new feature related to Mn 3d states was identified at the binding energies of about -1.6 eV besides the previously observed feature at about -3.3 eV. We suggest that the hybridization between Mn and As orbitals strongly enhanced the density of states around -1.6 eV. Although our resolution is much better compared with previous soft X-ray photoemission experiments, no clear hybridization gap between Mn 3d states and the valence bands proposed by previous model calculations was detected.

We report $^{75}$As NMR measurements on the new quasi one-dimensional superconductor K$_{2}$Cr$_{3}$As$_{3}$ ($T_{c} \sim 6.1$~K) [J.\ K.\ Bao et al., Phys. Rev. X {\bf 5}, 011013 (2015)]. We found evidence for strong enhancement of Cr spin fluctuations above $T_c$ in the [Cr$_{3}$As$_{3}$]$_{\infty}$ double-walled subnano-tubes based on the nuclear spin-lattice relaxation rate $1/T_{1}$. The power law temperature dependence, $1/T_{1}T \sim T^{-\gamma}$ ($\gamma \sim 0.25$), is consistent with the Tomonaga-Luttinger liquid. Moreover, absence of the Hebel-Slichter coherence peak of $1/T_{1}$ just below $T_{c}$ suggests unconventional nature of superconductivity., Comment: Final version accepted for publication in PRL

A new diluted ferromagnetic semiconductor (Sr,Na)(Zn,Mn)2As2 is reported, in which charge and spin doping are decoupled via Sr/Na and Zn/Mn substitutions, respectively, being distinguished from classic (Ga,Mn)As where charge & spin doping are simultaneously integrated. Different from the recently reported ferromagnetic (Ba,K)(Zn,Mn)2As2, this material crystallizes into the hexagonal CaAl2Si2-type structure. Ferromagnetism with a Curie temperature up to 20 K has been observed from magnetization. The muon spin relaxation measurements suggest that the exchange interaction between Mn moments of this new system could be different to the earlier DMS systems. This system provides an important means for studying ferromagnetism in diluted magnetic semiconductors., Comment: 18 Pages 4 Figures

Here we report the successful synthesis of a spin- & charge-decoupled diluted magnetic semiconductor (Ca,Na)(Zn,Mn)2As2, crystallizing into the hexagonal CaAl2Si2 structure. The compound shows a ferromagnetic transition with a Curie temperature up to 33 K with 10% Na doping, which gives rise to carrier density of np~10^20 cm^-3. The new DMS is a soft magnetic material with HC<400 Oe. The anomalous Hall effect is observed below the ferromagnetic ordering temperature. With increasing Mn doping, ferromagnetic order is accompanied by an interaction between the local spin and mobile charge, giving rise to a minimum in resistivity at low temperatures and localizing the conduction electrons. The system provides an ideal platform for studying the interaction of the local spins and conduction electrons., Comment: 23 Pages 1 Table 4 Figures

We use NMR techniques to investigate the magnetic properties of BaCo2As2 single crystals, the non-superconducting end member of the Co-substituted iron-pnictide high Tc superconductor Ba(Fe1-xCox)2As2 with x = 1. We present 75As NMR evidence for enhancement of low frequency spin fluctuations below ~ 100 K. This enhancement is accompanied by that of static uniform spin susceptibility at the wave vector q = 0, suggesting that the primary channel of the spin correlations is ferromagnetic rather than antiferromagnetic. Comparison between the NMR Knight shift 75K and bulk susceptibility chi(bulk) data uncovers the presence of two separate components of spin susceptibility with distinct temperature dependences, presumably because multiple electronic bands crossing the Fermi energy play different roles in the electronic properties of BaCo2As2., Comment: Submitted to PRB

(La1-xSrx)(Zn1-yMny)AsO is a two dimensional diluted ferromagnetic semiconductor that has the advantage of decoupled charge and spin doping. The substitution of Sr2+ for La3+ and Mn2+ for Zn2+ into the parent semiconductor LaZnAsO introduces hole carriers and spins, respectively. This advantage enables us to investigate the influence of carrier doping on the ferromagnetic ordered state through the control of Sr concentrations in (La1-xSrx)(Zn0.9Mn0.1)AsO. 10 % Sr doping results in a ferromagnetic ordering below TC ~ 30 K. Increasing Sr concentration up to 30 % heavily suppresses the Curie temperature and saturation moments. Neutron scattering measurements indicate that no structural transition occurs for (La0.9Sr0.1)(Zn0.9Mn0.1)AsO below 300 K., Comment: Submitted to EPL

We use muon spin relaxation (muSR) to investigate the magnetic properties of a bulk form diluted ferromagnetic semiconductor (DFS) Li1.15(Zn0.9Mn0.1)P with T_C ~ 22 K. MuSR results confirm the gradual development of ferromagnetic ordering below T_C with a nearly 100% magnetic ordered volume. Despite its low carrier density, the relation between static internal field and Curie temperature observed for Li(Zn,Mn)P is consistent with the trend found in (Ga,Mn)As and other bulk DFSs, indicating these systems share a common mechanism for the ferromagnetic exchange interaction. Li1+y(Zn1-xMnx)P has the advantage of decoupled carrier and spin doping, where Mn2+ substitution for Zn2+ introduces spins and Li+ off-stoichiometry provides carriers. This advantage enables us to investigate the influence of overdoped Li on the ferromagnetic ordered state. Overdoping Li suppresses both T_C and saturation moments for a certain amount of spins, which indicates that more carriers are detrimental to the ferromagnetic exchange interaction, and that a delicate balance between charge and spin densities is required to achieve highest T_C.

We investigate the nature of the SDW (Spin Density Wave) transition in the underdoped regime of an iron-based high Tc superconductor Ba(Fe1-xCox)2As2 by 75As NMR, with primary focus on a composition with x = 0.02 (T_SDW = 99 K).We demonstrate that critical slowing down toward the three dimensional SDW transition sets in at the tetragonal to orthorhombic structural phase transition, Ts = 105 K, suggesting strong interplay between structural distortion and spin correlations. In the critical regime between Ts and T_SDW, the dynamical structure factor of electron spins S(q,Wn) measured with the longitudinal NMR relaxation rate 1/T1 exhibits a divergent behavior obeying a power law, 1/T1~S(q, Wn)~(T/T_SDW-1)^a with the critical exponent a ~ 0.33., Comment: Accepted for publication in PRB

We report the synthesis and characterization of bulk form diluted magnetic semiconductors I-II-V Li1.1(Zn1-xCrx)As (x = 0.03, 0.05, 0.10, 0.15)with a cubic crystal structure identical to that of III-V GaAs and II-VI zinc-blende ZnSe. With p-type carriers created by excess Li, 10% Cr substitution for Zn results in a ferromagnetic ordering below TC ~ 218 K. Li(Zn,Cr)As represents another magnetic semiconducting system with the advantage of decoupling carriers and spins, where carriers are created by adding extra Li and spins are introduced by Cr substitution for Zn., Comment: arXiv admin note: substantial text overlap with arXiv:1403.4019

We report the synthesis and characterization of bulk form diluted magnetic semiconductors Ba(Zn1-2xMnxCox)2As2 (0 <= x <= 0.15) with a crystal structure identical to that of 122-type Fe-based superconductors. Mn and Co co-doping into the parent compound BaZn2As2 results in a ferromagnetic ordering below TC ~ 80 K. Hall effect measurements indicate that the carrier are n-type with the density of ~10^17/cm3. The common crystal structure and excellent lattice matching between the p-type ferromagnetic (Ba1-yKy)(Zn1-xMnx)2As2, the n-type ferromagnetic Ba(Zn1-2xMnxCox)2As2, the antiferrmagnetic BaMn2As2 and the superconducting Ba(Fe1-xCox)2As2 systems make it possible to make various junctions between these systems through the As layer.

A new diluted magnetic semiconductor system, (Sr3La2O5)(Zn1-xMnx)2As2, has been synthesized and characterized. 10% Mn substitution for Zn in bulk form (Sr3La2O5)Zn2As2 results in a ferromagnetic ordering below Curie temperature, TC ~ 40 K. (Sr3La2O5)(Zn1-xMnx)2As2 has a layered crystal structure identical to that of 32522-type Fe based superconductors, and represents the fifth DMS family that has a direct counterpart among the FeAs high temperature superconductor families., Comment: Accepted for publication in EPL

The doping effect of Sr and transition metals Mn, Fe, Co into the direct-gap semiconductor LaZnAsO has been investigated. Our results indicate that the single phase ZrCuSiAs-type tetragonal crystal structure is preserved in (La1-xSrx)(Zn1-xTMx)AsO (TM = Mn, Fe, Co) with the doping level up to x = 0.1. While the system remains semiconducting, doping with Sr and Mn results in ferromagnetic order with TC ~ 30K, and doping with Sr and Fe results in a spin glass like state below ~6K with a saturation moment of ~0.02 muB/Fe, an order of magnitude smaller than the ~0.4 muB/Mn of Sr and Mn doped samples. The same type of magnetic state is observed neither for (Zn,Fe) substitution without carrier doping, nor for Sr and Co doped specimens., Comment: Accepted for publication in EPL

We report the discovery of a new diluted magnetic semiconductor, Li(Zn,Mn)P, in which charge and spin are introduced independently via lithium off-stoichiometry and the isovalent substitution of Mn2+ for Zn2+, respectively. Isostructural to (Ga,Mn)As, Li(Zn,Mn)P was found to be a p-type ferromagnetic semiconductor with excess Lithium providing charge doping. First principles calculations indicate that excess Li is favored to partially occupy the Zn site, leading to hole doping. Ferromagnetism is mediated in semiconducting samples of relative low mobile carriers with a small coercive force, indicating an easy spin flip., Comment: 18pages, 1 table, 3 Figues

We employ NMR techniques to investigate the nature of Mn spins in the I-II-V diluted magnetic semiconductor Li(Zn1-xMnx)P (x = 0.1, Curie temperature Tc = 25 K). We successfully identify the 7Li NMR signals arising from the Li sites adjacent to Mn2+, and probe the static and dynamic properties of Mn spins. From the NMR spin-lattice relaxation data, we show that the Mn spin-spin interactions extend over many unit cells., Comment: Accepted for publicaton in Physical Review B-Rapid Communications

We report the synthesis and characterization of a bulk diluted magnetic semiconductor (La1-xBax)(Zn1-xMnx)AsO (0 <= x <= 0.2) with a layered crystal structure identical to that of the "1111" FeAs superconductors. No ferromagnetic order occurs for (Zn,Mn) substitution in the parent compound LaZnAsO without charge doping. Together with carrier doping via (La,Ba) sub- stitution, a small amount of Mn substituting for Zn results in ferromagnetic order with TC up to ~40 K, although the system remains semiconducting. Muon spin relaxation measurements confirm the development of ferromagnetic order in the entire volume, with the relationship between the internal field and TC consistent with the trend found in (Ga,Mn)As, the "111" Li(Zn,Mn)As, and the "122" (Ba,K)(Zn,Mn)2As2 systems., Comment: Accepted for publication in Physical Review B-Rapid Communications

We report a 75-As single crystal NMR investigation of LaFeAsO, the parent phase of a pnictide high Tc superconductor. We demonstrate that spin dynamics develop a strong two-fold anisotropy within each orthorhombic domain below the tetragonal-orthorhombic structural phase transition at T[TO]~156 K. This intermediate state with a dynamical breaking of the rotational symmetry freezes progressively into a spin density wave (SDW) below T[SDW]~142 K. Our findings are consistent with the presence of a spin nematic state below T[TO] with an incipient magnetic order., Comment: Revised manuscript accepted for publication in Phys. Rev. Lett

We respond to the comment of Bramwell et al (arXiv:1111.4168v1) to our original publication (S. R. Dunsiger et al, Phys. Rev. Lett. 107, 207207 (2011)), detailing muon spin rotation measurements of the Spin Ice compound Dy2Ti2O7., Comment: 2 pages; 1 figure; response to arXiv:1111.4168v1

Theory predicts the low-temperature magnetic excitations in spin ices consist of deconfined magnetic charges, or monopoles. A recent transverse-field (TF) muon spin rotation (muSR) experiment [S T Bramwell et al, Nature 461, 956 (2009)] reports results claiming to be consistent with the temperature and magnetic field dependence anticipated for monopole nucleation - the so-called second Wien effect. We demonstrate via a new series of muSR experiments in Dy_2Ti_2O_7 that such an effect is not observable in a TF muSR experiment. Rather, as found in many highly frustrated magnetic materials, we observe spin fluctuations which become temperature independent at low temperatures, behavior which dominates over any possible signature of thermally nucleated monopole excitations., Comment: 6 pages; 4 figures; published in Phys Rev. Lett. 107, 207207 (2011); Supplementary material and body of paper combined together in 1 file

We have studied the magnetism in superconducting single crystals of EuFe2 As1.4 P0.6 by using the local probe techniques of zero-field muon spin rotation/relaxation and 151 Eu/57 Fe M\"ossbauer spec- troscopy. All of these measurements reveal magnetic hyperfine fields below the magnetic ordering temperature TM = 18 K of the Eu2+ moments. The analysis of the data shows that there is a coexistence of ferromagnetism, resulting from Eu2+ moments ordered along the crystallographic c-axis, and superconductivity below TSC \approx 15 K. We find indications for a change in the dynamics of the small Fe magnetic moments (\sim 0.07 \mu B) at the onset of superconductivity: below TSC the Fe magnetic moments seem to be "frozen" within the ab-plane.

Impurity-induced magnetic order has been observed in many quasi-1D systems including doped variants of the spin-Peierls system CuGeO3. TiOCl is another quasi-1D quantum magnet with a spin-Peierls ground state, and the magnetic Ti sites of this system can be doped with non-magnetic Sc. To investigate the role of non-magnetic impurities in this system, we have performed both zero field and longitudinal field muSR experiments on polycrystalline Ti1-xScxOCl samples with x = 0, 0.01, and 0.03. We verified that TiOCl has a non-magnetic ground state, and we found no evidence for spin freezing or magnetic ordering in the lightly-doped Sc samples down to 1.7 K. Our results instead suggest that these systems remain non-magnetic up to the x = 0.03 Sc doping level., Comment: 5 pages, 4 figures

We will examine the possible link between spin fluctuations and the superconducting mechanism in the iron-based high temperature superconductor Ba(Fe,Co)2As2 based on NMR and high pressure transport measurements., Comment: Invited paper to m2s-IX (2009)

We report the first NMR investigation of spin dynamics in the overdoped non-superconducting regime of Ba(Fe[1-x]Co[x])2As2 up to x =0.26. We demonstrate that the absence of inter-band transitions with large momentum transfer Q(AF) ~ (pi, 0) between the hole and electron Fermi surfaces results in complete suppression of antiferromagnetic spin fluctuations for x > 0.15. Our experimental results provide direct evidence for a correlation between Tc and the strength of Q(AF) antiferromagnetic spin fluctuations., Comment: Accepted for publication in Phys. Rev. Lett

We report comprehensive resistivity measurements of single crystalline samples of the Ba(Fe(1-x)Co(x))2As2 high Tc superconductor under hydrostatic pressure up to 2.75 GPa and over a broad concentration range, 0 < x < 0.099. We show that application of pressure progressively suppresses the SDW transition temperature, T_SDW, in the underdoped regime. There is no sign of pressure-induced superconductivity in the undoped BaFe2As2 down to 1.8 K, but applied pressure dramatically enhances Tc in the underdoped regime. The effect of pressure on Tc is very small in the optimally and overdoped regimes. As a consequence, the dome of the superconducting phase extends to x 0.02 under pressure. We discuss the implications of our findings in the context of a possible quantum phase transition between the SDW and superconducting phases., Comment: 6 figures

Unlike the parent phases of the iron-arsenide high Tc superconductors, undoped FeSe is not magnetically ordered and exhibits superconductivity with Tc~9K. Equally surprising is the fact that applied pressure dramatically enhances the modest Tc to ~37K. We investigate the electronic properties of FeSe using 77Se NMR to search for the key to the superconducting mechanism. We demonstrate that the electronic properties of FeSe are very similar to those of electron-doped FeAs superconductors, and that antiferromagnetic spin fluctuations are strongly enhanced near Tc. Furthermore, applied pressure enhances spin fluctuations. Our findings suggest a link between spin fluctuations and the superconducting mechanism in FeSe., Comment: Accepted for publication in Phys. Rev. Lett. after minor revision

We investigate the electronic properties of Ba[Fe(1-x)Co(x)]2As2 (x =0.02, 0.04) in the lightly electron-doped regime by 59Co and 75As NMR. We demonstrate that Co doping significantly suppresses the magnetic ordering temperature to the SDW state, T_{SDW}. Furthermore, ordered moments below T_{SDW} exhibit large distribution. Strong spin fluctuations remain even below T_{SDW}, persisting all the way down to 4.2 K. We find no signature of additional freezing of spin degrees of freedom unlike the case of the lightly hole-doped stripe phase of the cuprates., Comment: 4 figures are changed to color online. 4 pages

We report a systematic investigation of Ba[Fe(1-x)Co(x)]2As2 based on transport and 75-As NMR measurements, and establish the electronic phase diagram. We demonstrate that doping progressively suppresses the uniform spin susceptibility and low frequency spin fluctuations. The optimum superconducting phase emerges at x_c~0.08 when the tendency toward spin ordering completely diminishes. Our findings point toward the presence of a quantum critical point near x_c between the SDW (spin density wave) and superconducting phases., Comment: 5 Figures

Application of pressures or electron-doping through Co substitution into Fe sites transforms the itinerant antiferromagnet BaFe(2)As(2) into a superconductor with the Tc exceeding 20K. We carried out systematic transport measurements of BaFe(2-x)Co(x)As(2) superconductors in pressures up to 2.5GPa, and elucidate the interplay between the effects of electron-doping and pressures. For the underdoped sample with nominal composition x = 0.08, application of pressure strongly suppresses a magnetic instability while enhancing Tc by nearly a factor of two from 11K to 21K. In contrast, the optimally doped x=0.20 sample shows very little enhancement of Tc=22K under applied pressure. Our results strongly suggest that the proximity to a magnetic instability is the key to the mechanism of superconductivity in iron-pnictides., Comment: 5 figures

We will probe the intrinsic behavior of spin susceptibility chi_(spin) in the LaFeAsO(1-x)F(x) superconductor (x ~ 0.1, Tc ~ 27K) using 19-F and 75-As NMR techniques. Our new results firmly establish the pseudo-gap behavior with Delta_(PG)/kB ~ 140K. The estimated magnitude of chi_(spin) at 290K, ~1.8x10^(-4) [emu/mol-Fe], is approximately twice larger than that in high Tc cuprates. We also show that chi_(spin) levels off below ~50K down to Tc., Comment: Invited paper to the Proceedings of the International Symposium on Iron-oxypnictide Superconductors (June 28-29, 2008, Tokyo). J. Phys. Soc. Jpn. Suppl. (in press)

We report an NMR investigation of the superconductivity in BaFe(2)As(2) induced by Co doping (Tc=22K). We demonstrate that Co atoms form an alloy with Fe atoms and donate carriers without creating localized moments. Our finding strongly suggests that the underlying physics of iron-pnictide superconductors is quite different from the widely accepted physical picture of high Tc cuprates as doped Mott insulators. We also show a crossover of electronic properties into a low temperature pseudo-gap phase with a pseudo-gap Delta 560K, where chi(spin) constant and resisitivty T. The NMR Knight shift below Tc decreases for both along the c-axis and ab-plane, and is consistent with the singlet pairing scenario., Comment: Accepted for publication in J. Phys. Soc. Jpn. (4 pages)

We report 19-F NMR investigation of the new high temperature superconductor LaFeAsO(0.89)F(0.11) (Tc ~ 28K). We demonstrate that low frequency spin fluctuations exhibit pseudo gap behavior above Tc. We also deduce the London penetration depth lambda from NMR line broadening below Tc., Comment: Accepted for publication in Phys. Rev. B (Rapid) with the original submission date

The CoO$_{2}$ layers in sodium-cobaltates Na$_{x}$CoO$_{2}$ may be viewed as a spin $S=1/2$ triangular-lattice doped with charge carriers. The underlying physics of the cobaltates is very similar to that of the high $T_{c}$ cuprates. We will present unequivocal $^{59}$Co NMR evidence that below $T_{CO}\sim51 K$, the insulating ground state of the itinerant antiferromagnet Na$_{0.5}$CoO$_{2}$ ($T_{N}\sim 86 K$) is induced by charge ordering., Comment: Phys. Rev. Lett. 100 (2008), in press. 4 figures

The sodium cobaltate family (NaxCoO2) is unique among transition metal oxides because the Co sits on a triangular lattice and its valence can be tuned over a wide range by varying the Na concentration x. Up to now detailed modeling of the rich phenomenology (which ranges from unconventional superconductivity to enhanced thermopower) has been hampered by the difficulty of controlling pure phases. We discovered that certain Na concentrations are specially stable and are associated with superlattice ordering of the Na clusters. This leads naturally to a picture of co-existence of localized spins and itinerant charge carriers. For x = 0.84 we found a remarkably small Fermi energy of 87 K. Our picture brings coherence to a variety of measurements ranging from NMR to optical to thermal transport. Our results also allow us to take the first step towards modeling the mysterious ``Curie-Weiss'' metal state at x = 0.71. We suggest the local moments may form a quantum spin liquid state and we propose experimental test of our hypothesis., Comment: 16 pages, 5 figures

This paper has been withdrawn. The sample was a mixed phase., Comment: 5 figures

We report the first 17-O NMR studies of a triangular-lattice superconductor Na{1/3}CoO{2}-[4/3]H{2}O and the host material Na{x}CoO{2} (x=0.35 and 0.72). Knight shift measurements reveal that p-d hybridization induces sizable spin polarization in the O triangular-lattice layers. Water-intercalation makes CoO{2} planes homogeneous, and enhances low frequency spin fluctuations near T{c}=4.5 K at some finite wave-vectors different from both the ferromagnetic and ``120 degree'' modes., Comment: 4 pages, 4 figures. Revised manuscript accepted for publication in Phys. Rev. Lett

We probed the local electronic properties of the mixed-valent Co(+4-x) triangular-lattice in Na{x}CoO{2}-yH{2}O by 59-Co NMR. We observed two distinct types of Co sites for x>=1/2, but the valence seems averaged out for x~1/3. Local spin fluctuations exhibit qualitatively the same trend down to ~100 K regardless of the carrier-concentration x, and hence the nature of the electronic ground state. A canonical Fermi-liquid behavior emerges below ~100 K only for x~1/3., Comment: 4 figures. Submitted to PRL on May 13, 2004