Possible hydrogen doping and enhancement of Tc (= 35 K) in a LaFeAsO-based superconductor
K. Miyazawa, S. Ishida, K. Kihou, P. M. Shirage, M. Nakajima, C. H. Lee, H. Kito, Y. Tomioka, T. Ito, H. Eisaki, H. Yamashita, H. Mukuda, K. Tokiwa, S. Uchida, A. Iyo
备注：
8 pages, 5 figures, 1 table, Appl. Phys. Lett. to be published
We report that the incorporation of hydroxide ions (OH)- significantly enhances the superconducting transition temperature (Tc) in the LnFeAsO-based superconductors (Ln1111: Ln = La, Ce and Pr). For La1111, Tc of the (OH)- incorporated sample synthesized using high-pressure technique becomes 35 K, which is higher by 7 K than the typical optimally-doped La1111 superconductors. Similar enhancement in Tc is also observed for Ce1111 and Pr1111. 1H-NMR measurement have confirmed the existence of hydrogen atoms in the samples. Accompanying the (OH)- incorporation, the lattice parameters are largely contracted, down to the values which have never been attained by any other dopings/substitutions.
We studied the electric and magnetic behavior near the phase boundary between antiferromagnetic (AF) and superconducting (SC) phases for a prototype of high-T_c pnictides LaFeAsO_{1-x}F_{x} by using nuclear magnetic resonance, and found that paramagnetic-metal (PM) domains segregate from AF domains. PM domains grow in size with increasing electron doping level and are accompanied by the onset of superconductivity, and thus application of pressure or increasing the doping level causes superconductivity. The existence of PM domains cannot be explained by the existing paradigm that focuses only o…
The electrical resistivity (Rxx) and Hall resistivity (Rxy) of LaFeAsO1-xFx have been measured over a wide fluorine doping range 0 =< x =< 0.14 using 60 T pulsed magnets. While the superconducting phase diagram (Tc, x) displays the classic dome-shaped structure, we find that the resistive upper critical field (Hc2) increases monotonically with decreasing fluorine concentration, with the largest Hc2 >= 75 T for x = 0.05. This is reminiscent of the composition dependence in high-Tc cuprates and might correlate with opening of a pseudo-gap in the underdoped region. Further, the temperature depend…
Low energy spin fluctuations are studied for the electron-doped Fe-based superconductor LaFeAsO(1-x)F(x) by inelastic neutron scattering up to the energy transfer of w = 15 meV using polycrystalline samples. Superconducting samples (x=0.057, Tc=25 K and x=0.082, Tc=29 K) show dynamical spin susceptibility chi"(w) almost comparable with the parent sample's. However chi"(w) is almost vanished in the x=0.158 sample where the superconductivity is highly suppressed. These results are compatible with the theoretical suggestions that the spin fluctuation plays an important role for the superconductiv…
We report our extensive 57Fe-, 75As-, 139La-, and 1H-NMR studies of La_{0.8}Y_{0.2}FeAsO_{1-y} (La_{0.8}Y_{0.2}1111) and LaFeAsO_{1-y}H_{x}(La1111H), where doping yttrium (Y) and hydrogen (H) into optimally doped LaFeAsO_{1-y} (La1111(OPT)) increases T_c=28 K to 34 and 32 K, respectively. In the superconducting (SC) state, the measurements of nuclear-spin lattice-relaxation rate 1/T_1 have revealed in terms of a multiple fully gapped s_\pm-wave model that the SC gap and T_c in La_{0.8}Y_{0.2}1111 become larger than those in La1111(OPT) without any change in doping level. In La1111H, the SC gap…
The experimental observation of superconductivity in LaFeAsO appearing on doping is analyzed with the group-theoretical approach that evidently led in a foregoing paper (J. Supercond 24:2103, 2011) to an understanding of the cause of both the antiferromagnetic state and the accompanying structural distortion in this material. Doping, like the structural distortions, means also a reduction of the symmetry of the pure perfect crystal. In the present paper we show that this reduction modifies the correlated motion of the electrons in a special narrow half-filled band of LaFeAsO in such a way that…
An iron-based superconductor LaFeAsO$_{1-x}$H$_x$ (0 $\leq x \leq$ 0.6) undergoes two antiferromagnetic (AF) phases upon H doping. We investigated the second AF phase ($x$=0.6) using NMR techniques under pressure. At pressures up to 2 GPa, the ground state is a spin-density-wave state with a large gap; however, the gap closes at 4.0 GPa, suggesting a pressure-induced quantum critical point. Interestingly, the gapped excitation coexists with gapless magnetic fluctuations at pressures between 2 and 4 GPa. This coexistence is attributable to the lift up of the $d_{xy}$ orbital to the Fermi level,…
We perform transport measurements and band structure calculations of electron-doped LaFeAsO1-xHx over a wide range of x from 0.01 to 0.66. The T^2 and sqrt(T) dependency of the resistivity are observed at x ~ 0.17 and 0.41, respectively. The sign change of RH without opening of the spin-density-wave gap for 0.45 < x < 0.58 and T < TN as well as the calculated non-nested Fermi surface at x = 0.5 indicate the more localized nature of the AF2 as compared to spin density wave phase at non-doped sample. Considering the results from band calculations and the finite size of Hund' s rule coupling, the…
We determine the phase diagram of LaFe$_{1-x}$Co$_x$AsO single crystals by using nuclear magnetic resonance (NMR). Up to a nominal doping of $x=0.03$, it follows the phase diagram for F-doped polycrystals. Above $x=0.03$, the F-doped samples become superconducting, whereas for Co-doping the structural and magnetic transitions can be observed up to $x=0.042$, and superconductivity occurs only for higher doping levels and with reduced transition temperatures. For dopings up to $x=0.056$, we find evidence for short-range magnetic order. By means of relaxation-rate measurements, we map out the mag…
We use neutron scattering to study the structural distortion and antiferromagnetic (AFM) order in LaFeAsO$_{1-x}$F$_{x}$ as the system is doped with fluorine (F) to induce superconductivity. In the undoped state, LaFeAsO exhibits a structural distortion, changing the symmetry from tetragonal (space group $P4/nmm$) to orthorhombic (space group $Cmma$) at 155 K, and then followed by an AFM order at 137 K. Doping the system with F gradually decreases the structural distortion temperature, but suppresses the long range AFM order before the emergence of superconductivity. Therefore, while supercond…
The 1111-type iron-based superconductor LnFeAsO1-xFx (Ln stands for lanthanide) is the first material with a Tc above 50 K, other than cuprate superconductors. Electron doping into LaFeAsO by H, rather than F, revealed a double-dome-shaped Tc-x diagram, with a first dome (SC1, 0.05<x<0.20) and a second dome (SC2, 0.2<x<0.5). Here, we report the Tc for the whole hydrogen-doping range in LaFeAsO1-xHx under pressures of up to 19 GPa. Tc rises to 52 K at 6 GPa for the Tc-valley composition between the two Tc domes. This is the first instance of the Tc exceeding 50 K in La-1111-type iron-based supe…
We studied double superconducting (SC) domes in LaFeAsO1-xHx by using 75As- and 1H-nuclear magnetic resonance techniques, and unexpectedly discovered that a new antiferromagnetic (AF) phase follows the double SC domes on further H doping, forming a symmetric alignment of AF and SC phases in the electronic phase diagram. We demonstrated that the new AF ordering originates from the nesting between electron pockets, unlike the nesting between electron and hole pockets as seen in the majority of undoped pnictides. The new AF ordering is derived from the features common to high-Tc pnictides: howeve…
We study how Co- and Ni-substitution affect the electronic structure of the iron-based superconductor, LaFeAsO. We perform {\it ab initio} supercell calculations and unfold the first Brillouin zone (BZ) to calculate the spectral function in the BZ for the normal cell. The charge density distribution in real space shows that doped extra electrons are trapped around Co (Ni) atom. This seems to mean that Co(Ni)-substitution does not work as carrier doping. However, the present momentum-space analysis indicates that the Fermi-surface volume indeed expands by substitutions, which can be well descri…
We report Zn-doping effect in the parent and F-doped LaFeAsO oxy-arsenides. Slight Zn doping in LaFe$_{1-x}$Zn$_{x}$AsO drastically suppresses the resistivity anomaly around 150 K associated with the antiferromagnetic (AFM) spin density wave (SDW) in the parent compound. The measurements of magnetic susceptibility and thermopower confirm further the effect of Zn doping on AFM order. Meanwhile Zn doping does not affect or even enhances the $T_c$ of LaFe$_{1-x}$Zn$_{x}$AsO$_{0.9}$F$_{0.1}$, in contrast to the effect of Zn doping in high-$T_c$ cuprates. We found that the solubility of Zn content …
We present $^{75}$As Nuclear Magnetic and Quadrupole Resonance results (NMR, NQR) on a new set of LaFeAsO$_{1-x}$F$_x$ polycrystalline samples. Improved synthesis conditions led to more homogenized samples with better control of the fluorine content. The structural$\equiv$nematic, magnetic, and superconducting transition temperatures have been determined by NMR spin-lattice relaxation rate and AC susceptibility measurements. The so-determined phase diagram deviates from the published one especially for low F-doping concentrations. However, if the doping level is determined from the NQR spectra…
Undoped LaFeAsO, parent compound of the newly found high-Tc superconductor, exhibits a sharp decrease in the temperature-dependent resistivity at ~160 K. The anomaly can be suppressed by F doping and the superconductivity appears correspondingly, suggesting a close associate of the anomaly with the superconductivity. We examined the crystal structures, magnetic properties and superconductivity of undoped (normal conductor) and 14 at.% F-doped LaFeAsO (Tc = 20 K) by synchrotron X-ray diffraction, DC magnetic measurements, and ab initio calculations to demonstrate that the anomaly is associated …
The Nernst effect has recently proven as a sensitive probe for detecting unusual normal state properties of unconventional superconductors. Here we present a systematic study of the Nernst effect of the iron pnictide superconductor \laf with a particular focus on its evolution upon doping. For the parent compound we observe a huge negative Nernst coefficient accompanied with a severe violation of the Sondheimer cancellation in the spin density wave (SDW) ordered state. Surprisingly, an unusual and enhanced Nernst signal is also found at underdoping ($x=0.05$) despite the presence of bulk super…
Here we report the superconductivity in the LaFeAsO1-xFx system prepared by high pressure synthesis. The highest onset superconducting transition temperature (Tc) in this La-based system is 41.0 K with the nominal composition of LaFeAsO1-xFx (x = 0.6), which is higher than that reported previously by ambient pressure synthesis. The increase of Tc can be attributed to the further shrinkage of crystal lattice that causes the stronger chemical pressure on the Fe-As plane, which is induced by the increased F-doping level under high pressure synthesis.
The low energy electronic structure of LaFeAsO1-xHx (0.0 < x < 0.60), the system which exhibits two superconducting domes in its phase diagram, is investigated by utilizing the laser photoemission spectroscopy. From the precise temperature-dependent measurement of the spectra near the Fermi level, we find the suppression of the density of states with cooling, namely the pseudogap formation, for all doping range. The pseudogap in the low x range (i.e. the first superconducting dome regime) gets suppressed with increasing x, more or less similarly to the previous results in F-doped LaFeAsO syste…
We report systematic 57Fe-NMR and 75As-NMR/NQR studies on an underdoped sample (T_c=20 K), an optimally doped sample (T_c=28 K), and an overdoped sample (T_c=22 K) of oxygen-deficient iron (Fe)-based oxypnictide superconductor LaFeAsO_{1-y}$. A microscopic phase separation between superconducting domains and magnetic domains is shown to take place in the underdoped sample, indicating a local inhomogeneity in association with the density distribution of oxygen deficiencies. As a result, 1/T_1T in the normal state of the superconducting domain decreases significantly upon cooling at both the Fe …
We have studied the interplay of magnetism and superconductivity in LaFeAsO$_{1-x}$F$_x$ and Ca(Fe$_{1-x}$Co$_x$)$_2$As$_2$. While antiferromagnetic spin density wave formation is suppressed and superconductivity evolves, all samples show a doping independent strong increase of the normal state susceptibility upon heating which appears a general feature of iron pnictides. The data provide evidence for robust local antiferromagnetic correlations persisting even in the superconducting regime of the phase diagram.
Hydrogen (H)-doped LaFeAsO is a prototypical iron-based superconductor. However, its phase diagram extends beyond the standard framework, where a superconducting (SC) phase follows an antiferromagnetic (AF) phase upon carrier doping; instead, the SC phase is sandwiched between two AF phases appearing in lightly and heavily H-doped regimes. We performed nuclear magnetic resonance (NMR) measurements under pressure, focusing on the second AF phase in the heavily H-doped regime. The second AF phase is strongly suppressed when a pressure of 3.0 GPa is applied, and apparently shifts to a highly H-do…
We present measurements of the thermal expansion coefficient alpha of polycrystalline LaFeAsO1-xFx (x <= 0.1). The magnetic and structural transitions of the samples with x <= 0.04 give rise to large anomalies in alpha(T), while the onset of superconductivity in the crystals with x >= 0.05 is not resolved. Above the structural transition, the thermal expansion coefficient of LaFeAsO is significantly enhanced. This is attributed to fluctuations, which also affect the electrical transport properties of the compound. The complete absence of these fluctuations in the superconducting samples even f…
The wave-vector (q) and doping dependences of the magnetic energy, iron moment, and effective exchange interactions in LaFeAsO, BaFe2As2, and SrFe2As2\ are studied by self-consistent LSDA calculations for co-planar spin spirals. For the undoped compounds, the calculated total energy, E(q), reaches its minimum at q corresponding to stripe anti-ferromagnetic order. In LaFeAsO, this minimum becomes flat already at low levels of electron-doping and shifts to an incommensurate q at delta=0.2, where delta is the number of additional electrons (delta>0) or holes (delta<0) per Fe. In BaFe2As2 and SrFe…
Inelastic neutron scattering was performed for an iron-based superconductor LaFeAsO0.9D0.1, where most of D (deuterium) replaces oxygen, while a tiny amount goes into interstitial sites. By first-principle calculation, we characterize the interstitial sites for D (and for H slightly mixed) with four equivalent potential minima. Below the superconducting transition temperature Tc = 26 K,new excitations emerge in the range 5-15 meV, while they are absent in the reference system LaFeAsO0.9F0.1. The strong excitations at 14.5 meV and 11.1 meV broaden rapidly around 15 K and 20 K, respectively, whe…
The coupling of Fe magnetic moments in LaFeAsO$_{1-x}$F$_{x}$ with the As $A_{1g}$ phonon is calculated. We present first principles calculations of the atomic and electronic structure of LaFeAsO as a function of electron doping. We perform calculations using the virtual crystal approximation as well as supercell calculations with F substitutional impurity atoms. The results validate the virtual crystal approximation for the electronic structure near the Fermi level. Its is found that the electronic density of states at the Fermi level is maximum for x=0.125, enhancing the electron-phonon inte…
Iron arsenide superconductors based on the material LaFeAsO1-xFx are characterized by a two-dimensional Fermi surface (FS) consisting of hole and electron pockets yielding structural and antiferromagnetic transitions at x = 0. Electron doping by substituting O2- with F- suppresses these transitions and gives rise to superconductivity with a maximum Tc = 26 K at x = 0.1. However, the over-doped region cannot be accessed due to the poor solubility of F- above x = 0.2. Here we overcome this problem by doping LaFeAsO with hydrogen. We report the phase diagram of LaFeAsO1-xHx (x < 0.53) and, in add…
By a systematic study of the hydrogen-doped LaFeAsO system by means of dc resistivity, dc magnetometry, and muon-spin spectroscopy we addressed the question of universality of the phase diagram of rare-earth-1111 pnictides. In many respects, the behaviour of LaFeAsO_(1-x)H_(x) resembles that of its widely studied F-doped counterpart, with H^- realizing a similar (or better) electron-doping in the LaO planes. In a x = 0.01 sample we found a long-range SDW order with T_n = 119 K, while at x = 0.05 the SDW establishes only at 38 K and, below T_c = 10 K, it coexists at a nanoscopic scale with bulk…
Electronic and magnetic properties of the heavily H-doped LaFeAsO$_{1-x}$H$_x$ $(x\sim0.5 )$ were studied in the framework of the density functional theory combined with the dynamical mean field theory (DFT+DMFT). We found a stripe-like-ordered structure of hydrogen and oxygen atoms, as a ground state, with the same configuration as the antiferromagnetic (AF) order. The new configuration could explain the existing experimental results related to the heavily H-doped LaFeAsO$_{1-x}$H$_x$, such as an in-plane electronic anisotropy and a non-uniform magnetic behavior. A significant anisotropy was …
The ionization energy theory is used to calculate the evolution of the resistivity and specific heat curves with respect to different doping elements in the recently discovered superconducting Pnictide materials. Subsequently, the electron-conduction mechanism in the Pnictides above the structural transition temperature is explained unambiguously, which is also consistent with other strongly correlated matter, such as cuprates, manganites, titanates and magnetic semiconductors. Therefore, the superconductivity is not uniquely corresponds to the electronic properties above the structural transi…
We have measured element-specific Fe-phonon densities of states (Fe-PDOS) of LaFeAsO_{1-x}F_{x} (x = 0, 0.11) and La_{1-x}Ca_{x}FePO (x = 0.13) by using nuclear resonant inelastic scattering of synchrotron radiation. The Fe-PDOS of superconductor LaFeAsO_{0.89}F_{0.11} (Tc = 26 K) and that of non-superconductor LaFeAsO have similar structures to both below Tc (15 K) and above Tc (298 K) and, therefore, fluorine doping does not have notable effect on the Fe-PDOS. As for the superconductor La_{0.87}Ca_{0.13}FePO (Tc = 5.4K), the entire structure of Fe-PDOS resembles with that of LaFeAsO_{1-x}F_{…
The wave-vector q and doping (x,y) dependences of the magnetic energy, iron moment, and effective exchange interactions in LaFeAsO{1-x}F{x} and Ba{1-2y}K{2y}Fe2As2 are studied by self-consistent LSDA calculations for co-planar spin spirals. For the undoped compounds (x=0, y=0), the minimum of the calculated total energy, E(q), is for q corresponding to stripe antiferromagnetic order. Already at low levels of electron doping (x), this minimum becomes flat in LaFeAsO{1-x}F{x} and for x>=5, it shifts to an incommensurate q. In Ba{1-2y}K{2y}Fe2As2, stripe order remains stable for hole doping up to…
We studied the quantum critical behavior of the second antiferromagnetic (AF) phase in the heavily electron-doped high-$T_c$ pnictide, LaFeAsO$_{1-x}$H$_x$ by using $^{75}$As and $^{1}$H nuclear-magnetic-resonance (NMR) technique. In the second AF phase, we observed a spatially modulated spin-density-wave-like state up to $x$=0.6 from the NMR spectral lineshape and detected a low-energy excitation gap from the nuclear relaxation time $T_1$ of $^{75}$As. The excitation gap closes at the AF quantum critical point (QCP) at $x \approx 0.49$. The superconducting (SC) phase in a lower-doping regime …
The evolution of low-energy spin dynamics in the iron-based superconductor LaFeAsO$_{1-x}$F$_x$ was studied over a broad doping, temperature, and magnetic field range (x = 0 - 0.15, T up to 480K, H up to 30T) by means of As nuclear magnetic resonance (NMR). An enhanced spin-lattice relaxation rate divided by temperature, 1/T1T, in underdoped superconducting samples (x = 0.045, 0.05 and 0.075) suggests the presence of antiferromagnetic spin fluctuations, which are strongly reduced in optimally-doped (x = 0.10) and completely absent in overdoped (x = 0.15) samples. In contrast to previous analys…
$^{75}$As Nuclear Magnetic (NMR) and Quadrupolar (NQR) Resonance were used, together with Mössbauer spectroscopy, to investigate the magnetic state induced by Mn for Fe substitutions in F-doped LaFe$_{1-x}$Mn$_{x}$AsO superconductors. The results show that $0.5$% of Mn doping is enough to suppress the superconducting transition temperature $T_c$ from 27 K to zero and to recover the magnetic structure observed in the parent undoped LaFeAsO. Also the tetragonal to orthorhombic transition of the parent compound is recovered by introducing Mn, as evidenced by a sharp drop of the NQR frequency. The…
Density functional studies of 26K superconducting LaFeAs(O,F) are reported. We find a low carrier density, high density of states, $N(E_F)$ and modest phonon frequencies relative to $T_c$. The high $N(E_F)$ leads to proximity to itinerant magnetism, with competing ferromagnetic and antiferromagnetic fluctuations and the balance between these controlled by doping level. Thus LaFeAs(O,F) is in a unique class of high $T_c$ superconductors: high $N(E_F)$ ionic metals near magnetism.
We study hydrogen doping effects in an iron-based superconductor LaFeAsO_(1-y) by using the first-principles calculation and explore the reason why the superconducting transition temperature is remarkably enhanced by the hydrogen doping. The present calculations reveal that a hydrogen cation stably locating close to an iron atom attracts a negatively-charged FeAs layer and results in structural distortion favorable for further high temperature transition. In fact, the lattice constant a averaged over the employed supercell shrinks and then the averaged As-Fe-As angle approaches 109.74 degrees …
We have studied Ni-substitution effect in LaFe$_{1-x}$Ni$_{x}$AsO ($0\leq x \leq0.1$) by the measurements of x-ray diffraction, electrical resistivity, magnetic susceptibility, and heat capacity. The nickel doping drastically suppresses the resistivity anomaly associated with spin-density-wave ordering in the parent compound. Superconductivity emerges in a narrow region of $0.03\leq x \leq0.06$ with the maximum $T_c$ of 6.5 K at $x$=0.04, where enhanced magnetic susceptibility shows up. The upper critical field at zero temperature is estimated to exceed the Pauli paramagnetic limit. The much l…
The Fe-based Oxypnicide superconductors have generated a huge amount of interest; they are a high temperature superconductor, with a Tc of 55K, but do not have the two dimensional copper oxygen layer that was thought essential for superconductivity at these high temperatures. Initial studies have hinted towards the possibility of a spin density wave (SDW) in these compounds and how they could play an important role in the superconductivity. SDW's occur at low temperatures in low-dimensional materials with strong electron correlations or in metals with a high density of states at the Fermi surf…
The local structure of the parent and doped LaFeAsO1-xFx (pnictide) compounds were studied by x-ray absorption spectroscopy. In the doped system, the Fe-As and Fe-Fe correlations are well modeled by an Einstein model with no low temperature anomalies. For the Fe-As bonds, the Einstein temperatures are identical for the doped (11%) and undoped samples, but the doped sample is found to have a lower level of static disorder. For the Fe-Fe correlation, doping enhances the effective Einstein temperature of Fe-Fe atom correlation. The results suggest that the onset of superconductivity in the F dope…
Here, we present an electrical transport study in single crystals of LaFe$_{0.92}$Co$_{0.08}$AsO ($T_c \simeq 9.1$ K) under high magnetic fields. In contrast to most of the previously reported Fe based superconductors, and despite its relatively low $T_c$, LaFe$_{1-x}$Co$_x$AsO shows a superconducting anisotropy which is comparable to those seen for instance in the cuprates or $γ_H = H_{c2}^{ab}/H_{c2}^{c} = m_c/m_{ab} \simeq 9$, where $m_c/m_{ab}$ is the effective mass anisotropy. Although, in the present case and as in all Fe based superconductors, $γ\rightarrow 1$ as $T \rightarrow 0$. Unde…
Specific heats and transport quantities of the LaFe1-yNiyAsO0.89F0.11 system have been measured, and the results are discussed together with those reported previously by our group mainly for LaFe1-yCoyAsO0.89F0.11 and LaFeAsO0.89-xF0.11+x systems. The y dependence of the electronic specific heat coefficient gamma can basically be understood by using the rigid-band picture, where Ni ions provide 2 electrons to the host conduction bands and behave as nonmagnetic impurities. The superconducting transition temperature Tc of LaFe1-yNiyAsO0.89F0.11 becomes zero, as the carrier density p (=2y+0.11) d…
Here we demonstrate the technique to stabilize the ErFeAsO-based superconductor with the smallest lattice constants in LnFeAsO1-y (Ln = lanthanide) series using hydrogen doping method. Polycrystalline samples were synthesized by heating pellets with nominal compositions of ErFeAsO1-y (1-y = 0.75 ~ 0.95) sandwiched between pellets of LaFeAsO0.8H0.8 compositions at 1100 °C under a pressure of 5.0 - 5.5 GP. The sample with lattice constants of a = 3.8219 Å and c = 8.2807 Å shows the highest superconducting critical temperatures (Tc) of 44.5 K and 41.0 K determined by onset transitions of resistiv…
We performed nuclear magnetic resonance (NMR) measurements to investigate the evolution of spin-density-wave (SDW) and superconducting (SC) states upon electron doping in CaFe_{1-x}Co_{x}AsF, which exhibits an intermediate phase diagram between those of LaFeAsO_{1-x}F_x and Ba(Fe_{1-x}Co_x)_2As_2. We found that homogeneous coexistence of the incommensurate SDW and SC states occurs only in a narrow doping region around the crossover regime, which supports S_{+-}-wave symmetry. However, only the structural phase transition survives upon further doping, which agrees with predictions from orbital …
We present the first comprehensive derivation of the intrinsic electronic phase diagram of the iron-oxypnictide superconductors in the normal state based on the analysis of the electrical resistivity $ρ$ of both LaFeAsO$_{1-x}$F$_x$ and SmFeAsO$_{1-x}$F$_x$ for a wide range of doping. Our data give clear-cut evidence for unusual normal state properties in these new materials. In particular, the emergence of superconductivity at low doping levels is accompanied by distinct anomalous transport behavior in $ρ$ of the normal state which is reminiscent of the spin density wave (SDW) signature in th…
We investigate the doping dependence of the magnetic excitations in two-superconducting-dome-system LaFeAsO1-xDx. Using inelastic neutron scattering, spin fluctuations at different wavenumbers were observed under both superconducting domes around x = 0.1 and 0.4, but vanished at x = 0.2 corresponding to the Tc valley. Theoretical calculations indicate that the characteristic doping dependence of spin fluctuations is rationally explained as a consequence of the switching of the two intra-orbital nestings within Fe-3dYZ, ZX and 3dX2-Y2 by electron doping. The present results imply that the multi…
Utilizing the high stability of calcium and rare earth hydrides, CaFeAsF1-xHx (x = 0.0-1.0) and SmFeAsO1-xHx (x = 0.0-0.47) have been first synthesized using high pressure to form hydrogen-substituted 1111 type iron-arsenide superconductors. Neutron diffraction and density functional calculations have demonstrated that the hydrogens are incorporated as H- ions occupying F- sites in the blocking layer of CaFeAsF. The resulting CaFeAsF1-xHx is non-superconducting, whereas SmFeAsO1-xHx is a superconductor, with an optimal Tc = 55 K at x 0.2. It was found that up to 40% of the O2- ions can be repl…
Muon Spin Rotation ($μ$SR) and $^{19}$F Nuclear Magnetic Resonance (NMR) measurements were performed to investigate the effect of Mn for Fe substitutions in La$_{1-y}$Y$_{y}$Fe$_{1-x}$Mn$_x$AsO$_{0.89}$F$_{0.11}$ superconductors. While for $y = 0$ a very low critical concentration of Mn ($x = 0.2$%) is needed to quench superconductivity, as $y$ increases the negative chemical pressure introduced by Y for La substitution stabilizes superconductivity and for $y= 20$% it is suppressed at Mn contents an order of magnitude larger. A magnetic phase arises once superconductivity is suppressed both fo…
Design of a 60.8 K superconducting hydride LiMgZr2H12 at ambient pressure via Lithium doping
School of Physics, Xidian University（西安电子科技大学物理学院）；College of Physics and Optoelectronic Technology, Baoji University of Arts and Sciences（宝鸡文理学院物理与光电技术学院）
Chemical doping has recently become a very important strategy to induce superconductivity especially in complex compounds. Distinguished examples include Ba-doped La$_2$CuO$_4$ (the first high temperature superconductor), K-doped BaBiO$_3$, K-doped C$_{60}$ and Na$_{x}$CoO$_{2}\cdot y$H$_{2}$O. The most recent example is F-doped LaFeAsO, which leads to a new class of high temperature superconductors. One notes that all the above dopants are non-magnetic, because magnetic atoms generally break superconducting Cooper pairs. In addition, the doping site was out of the (super)conducting structural…
Pressurized hydrogen-rich compounds, which could be viewed as precompressed metallic hydrogen, exhibit high superconductivity, thereby providing a viable route toward the discovery of high-temperature superconductors. Of particular interest is to search for high-temperature superconductors with low stable pressure in terms of pressure-stabilized hydrides. In this work, with the aim of obtaining high-temperature superconducting compounds at low pressure, we attempt to study the doping effects for high-temperature superconductive $ \mathrm{H_3S} $ with supercells up to 64 atoms using first princ…
We report the charge doping of KCr$_3$As$_3$ via H intercalation. We show that the previously reported ethanol bath deintercalation of K$_2$Cr$_3$As$_3$ to KCr$_3$As$_3$ has a secondary effect whereby H from the bath enters the quasi-one-dimensional Cr$_6$As$_6$ chains. Furthermore, we find that - contrary to previous interpretations - the difference between non-superconducting as-grown KCr$_3$As$_3$ samples and superconducting hydrothermally annealed samples is not a change in crystallinity but due to charge doping, with the latter treatment increasing the H concentration in the CrAs tubes ef…
We report the realization of superconductivity by an isovalent doping with phosphorus in LaFeAsO. X-ray diffraction shows that, with the partial substitution of P for As, the Fe$_2$As$_2$ layers are squeezed while the La$_2$O$_2$ layers are stretched along the c-axis. Electrical resistance and magnetization measurements show emergence of bulk superconductivity at $\sim$10 K for the optimally-doped LaFeAs$_{1-x}$P$_{x}$O ($x=0.25\sim0.3$). The upper critical fields at zero temperature is estimated to be 27 T, much higher than that of the LaFePO superconductor. The occurrence of superconductivit…
We report single-crystal growth of La$_{0.34}$Na$_{0.66}$Fe$_2$As$_2$ iron-based superconductor with the size of several millimeters. The samples were accidentally obtained in trying to grow LaFeAsO$_{1-y}$F$_y$ ( $y \geq$ 0.8 ) single crystals with NaAs and NaF flux. The sample shows both antiferromagnetic and structural transitions at 106 K. The superconducting transition temperature is about 27 K with the superconducting anisotropy of about 1.9. These values and the temperature dependence of the Hall coefficient suggest that La$_{0.34}$Na$_{0.66}$Fe$_2$As$_2$ belongs to hole-doped "122" fam…
Measurements of the electrical resistivities, Hall coefficients, thermoelectric powers, electronic specific heat coefficients have been carried out for samples of LnFe1-yMyAsO1-xFx (Ln=La, Nd; M=Co, Mn; x=0.11) obtained by M atom dopings to the superconducting LnFeAsO1-xFx (Ln1111) system. The NMR longitudinal relaxation rates 1/T1 have also been measured for samples of LaFe1-yCoyAsO1-xFx with various x values. Co atoms doped to the superconducting LnFeAsO1-xFx are nonmagnetic, and the Tc-suppression by the Co atoms has been found to be too weak to understand by the pair breaking effect expect…
The recently synthesized air-insensitive hydrogen doped KCr$_3$As$_3$ superconductor has aroused great research interests. This material has, for the first time in the research area of the quasi-one-dimensional Cr-based superconductivity (SC), realized a tunability through charge doping, which will potentially significantly push the development of this area. Here based on the band structure from first-principle calculations, we construct a six-band tight-binding (TB) model equipped with multi-orbital Hubbard interactions, and adopt the random-phase-approximation approach to study the hydrogen-…
The difference in thermal stability of F- and H- in 1111-type iron based superconductors, allows selective hydrogen elimination from non-superconductive CaFeAsF0.8H0.2 by thermal annealing. The analyzed chemical composition of the resulting samples indicates that incorporated hydrogen was selectively eliminated by thermal annealing at 553 K for 72 hours. The resulting hydrogen-eliminated sample shows bulk superconductivity with Tc = 29 K. This technique may be used for indirect electron doping for AeFeAeF (Ae; alkali-earth metal) iron based superconductor described by CaFeAsF1-xHx => CaFeAsF1-…
Hydrogen is the simplest bipolar element and its valence state can be controlled from +1 to -1. We synthesized the 1111-type CaFeAsH and LnFeAsO1-xHx (Ln = lanthanide) with the ZrCuSiAs type structure by a high-pressure synthesis method. The position and valence state of the substituted H were determined by neutron diffraction and density functional theory calculations. The close similarity in the structural and electrical properties of CaFeAsH and CaFeAsF indicated the formation of the hydride ion (H-), which is isovalent with the fluoride ion (F-), in the 1111-type iron arsenides. When some …
