The interplay between structural phase and electronic correlations has been an intriguing topic of research. An prominent example is the pressure-induced uncollapsed to collapsed tetragonal phase transition observed in CaFe$_2$As$_2$, which is accompanied with the emergence of superconductivity in the collapsed phase. Recently, a very similar structural phase transition was discovered in LaFe$_2$As$_2$, but in contrast to CaFe$_2$As$_2$, superconductivity was only observed in the uncollapsed phase, not the collapsed phase. Previous studies have attributed this puzzling observation to the differences in the two materials' band coherence, orbital occupation, and Fermi surface topology. Here, we present a comparative study of LaFe$_2$As$_2$ and CaFe$_2$As$_2$ using the DFT+DMFT method. Surprisingly, we find that although La appears to have a valence higher than Ca, the doped one electron actually primarily resides on the La site. This leads to almost the same total Fe-$3d$ occupancy and electronic correlation strength as well as similar Lifshiftz transition in the Fermi surface topology for the two materials. In addition, we show that the two materials in both structural phases belong to the category of Hund's metals. Our results indicate that the electronic structures of LaFe$_2$As$_2$ and CaFe$_2$As$_2$ are not too different, which further suggest that superconductivity might also be induced in the collapsed phase of LaFe$_2$As$_2$ under similar non-hydrostatic conditions as for CaFe$_2$As$_2$.
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…
We performed $^{31}$P-NMR measurements on LaFe(As$_{1-x}$P$_{x}$)O to investigate the relationship between antiferromagnetism and superconductivity. The antiferromagnetic (AFM) ordering temperature $T_{\rm N}$ and the moment $μ_{\rm ord}$ are continuously suppressed with increasing P content $x$ and disappear at $x = 0.3$ where bulk superconductivity appears. At this superconducting $x = 0.3$, quantum critical AFM fluctuations are observed, indicative of the intimate relationship between superconductivity and low-energy AFM fluctuations associated with the quantum-critical point in LaFe(As$_{1…
The isostructural transition in the tetragonal phase, with sizable change in the anion-height, is realized in heavily H-doped LaFeAsO and (La,P) co-doped CaFe$_2$As$_2$. In these compounds, the superconductivity with higher-Tc (40~50 K) is realized near the isostructural transition. To reveal the origin of the anion-height instability and its important role in realizing the higher-Tc state, we develop the orbital-spin fluctuation theory by including the vertex correction. It is found that the non-nematic orbital fluctuations, which induce the anion-height instability, can develop near the magn…
We report Zn-doping effect in the parent and F-doped LaFeAsO oxy-arsenides. Slight Zn doping in LaFe$_{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 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…
We have performed $^{139}$La,$^{31}$P-NMR studies on a filled skutterudite superconductor LaFe$_{4}$P$_{12}$ with a critical temperature $T_c=4.1$ K. In the normal state, the presence of antiferromagnetic (AFM) fluctuations at finite wave vectors is suggested from the relation between the nuclear spin-lattice relaxation rate $1/T_1$ and the Knight shift. In the superconducting (SC) state, the distinct coherence peak was observed just below $T_c$, and is easily suppressed by the applied field. An exponential decrease of $1/T_1$ was observed, suggestive of the isotropic superconducting gap with …
Pnictogens and chalcogens are both viable anions for promoting Fe-based superconductivity and intense research activity in the related families has established systematic correlation between the Fe-anion height and the superconducting critical temperature $T_c$, with an optimum Fe-anion height of $\sim$ 1.38 Å. Here, we report the discovery of superconductivity in a novel compound LaFeSiO$_{1-δ}$ that incorporates a crystallogen element, Si, and challenges the above picture: considering the strongly squeezed Fe-Si height of 0.94 Å, the superconducting transition at $T_{c}$ = 10 K is unusually …
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…
We report on an experimental study of the effect of Mn impurities in the optimally doped LaFeAsO$_{0.89}$F$_{0.11}$ compound. The results show that a very tiny amount of Mn, of the order of 0.1\%, is enough to destroy superconductivity and to recover at low temperatures both the magnetic ground state and the orthorhombic structure of the pristine LaFeAsO parent compound. The results are discussed within a model where electron correlations enhance the Ruderman-Kittel-Kasuya-Yosida interaction among impurities.
Here, we investigated the interrelationship between pressure and correlation in the LaFeAsO compound by the density functional theory method combined with the dynamical mean field theory (DFT+DMFT) method. The spectral function and the occupation number (ON) of Fe-3d orbitals at different pressures were extracted from the calculations, and the importance of the role of correlation in superconductivity in iron-based compounds was indicated. The measured ON of Fe-3d orbitals demonstrated charge transfer between them and also the crucial role of the Fe-3dxy (xy) orbital in superconductivity in th…
The crystal structure and numerous normal and superconducting state properties of layered tetragonal (P4/nmm) LaFeAsO, with F-doping of 11 %, are reported. Resistivity measurements give an onset transition temperature Tc = 28.2 K, and low field magnetic susceptibility data indicate bulk superconductivity. In applied magnetic field, analysis of the resistive transition results in a critical field Hc2 = 30 T and a coherence length 35 A. An upper limit for the electron carrier concentration of 1 x 10^21 cm-3 is inferred from Hall data just above Tc. Strong electron-electron correlations are sugge…
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…
Recent observations of selective emergence (suppression) of superconductivity in the uncollapsed (collapsed) tetragonal phase of LaFe$_2$As$_2$ has rekindled interest in understanding what features of the band structure control the superconducting T$_c$. We show that the proximity of the narrow Fe-d$_{xy}$ state to the Fermi energy emerges as the primary factor. In the uncollapsed phase this state is at the Fermi energy, and is most strongly correlated and source of enhanced scattering in both single and two particle channels. The resulting intense and broad low energy spin fluctuations suppre…
We report a high-pressure study of simultaneous low-temperature electrical resistivity and Hall effect measurements on high quality single-crystalline KFe2As2 using designer diamond anvil cell techniques with applied pressures up to 33 GPa. In the low pressure regime, we show that the superconducting transition temperature T_c finds a maximum onset value of 7 K near 2 GPa, in contrast to previous reports that find a minimum T_c and reversal of pressure dependence at this pressure. Upon applying higher pressures, this T_c is diminished until a sudden drastic enhancement occurs coincident with a…
We present detailed electronic structure calculations for CaFe2As2. We investigate in particular the `collapsed' tetragonal and orthorhombic regions of the temperature-pressure phase diagram and find properties that distinguish CaFe2As2 from other Fe-pnictide compounds. In contrast to the tetragonal phase of other Fe-pnictides the electronic structure in the `collapsed' tetragonal phase of CaFe2As2 is found to be strongly 3D. We discuss the influence of these properties on the formation of superconductivity and in particular we find evidence that both magnetic and lattice interactions may be i…
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…
Recent investigations of the superconducting iron-arsenide families have highlighted the role of pressure, be it chemical or mechanical, in fostering superconductivity. Here we report that CaFe2As2 undergoes a pressure-induced transition to a non-magnetic, volume "collapsed" tetragonal phase, which becomes superconducting at lower temperature. Spin-polarized total-energy calculations on the collapsed structure reveal that the magnetic Fe moment itself collapses, consistent with the absence of magnetic order in neutron diffraction.
The surprising discovery of tripling the superconducting critical temperature of KFe$_2$As$_2$ at high pressures issued an intriguing question of how the superconductivity in the collapsed tetragonal phase differs from that in the non-collapsed phases of Fe-based superconductors. Here we report $^{89}$Y nuclear magnetic resonance study of YFe$_2$Ge$_{x}$Si$_{2-x}$ compounds whose electronic structure is similar to that of iron-pnictide collapsed tetragonal phases already at ambient pressure. Fe(Ge,Si) layers show strong ferromagnetic spin fluctuations whereas layers are coupled antiferromagnet…
Iron-based superconductors are well-known for their intriguing phase diagrams, which manifest a complex interplay of electronic, magnetic and structural degrees of freedom. Among the phase transitions observed are superconducting, magnetic, and several types of structural transitions, including a tetragonal-to-orthorhombic and a collapsed-tetragonal transition. In particular, the widely-observed tetragonal-to-orthorhombic transition is believed to be a result of an electronic order that is coupled to the crystalline lattice and is, thus, referred to as nematic transition. Nematicity is therefo…
Single crystals of Ca(Fe1-xRux)2As2 (0<x<0.065) and Ca1-yLay(Fe0.973Ru0.027)2As2 (0<y<0.2) have been synthesized and studied with respect to their structural, electronic and magnetic properties. The partial substitution of Fe by Ru induces a decrease of the c-axis constant leading for x<0.023 to a suppression of the coupled magnetic and structural (tetragonal to orthorhombic) transitions. At x_cr=0.023 a first order transition to a collapsed tetragonal (CT) phase is found, which behaves like a Fermi liquid and which is stabilized by further increase of x. The absence of superconductivity near …
Inelastic neutron scattering measurements of CaFe2As2 under applied hydrostatic pressure show that the antiferromagnetic spin fluctuations observed in the ambient pressure, paramagnetic, tetragonal (T) phase are strongly suppressed, if not absent, in the collapsed tetragonal (cT) phase. These results are consistent with a quenched Fe moment in the cT phase and the strong decrease in resistivity observed upon crossing the boundary from the T to cT phase. The suppression or absence of static antiferromagnetic order and dynamic spin fluctuations in the non-superconducting cT phase supports the no…
We report the observation of the pressure-induced, fully-collapsed tetragonal phase of CaRbFe4As4 for P~ 22 GPa via high-pressure x-ray diffraction and magnetotransport measurements. The x-ray measurements, along with resistivity measurements, show that there is an initial half-collapsed tetragonal phase for 6 < P < 22 GPa, in which superconductivity is continuously suppressed from Tc= 35K at P= 3.1 GPa to Tc <2K for P >17.2 GPa, as well as signs of the fully-collapsed tetragonal phase near P=22 GPa. Density functional calculations suggest that both of these transitions are driven by increased…
To understand the amazing variety of the superconducting states of Fe-based superconductors, we analyze the multiorbital Hubbard models for LaFeAsO and LiFeAs going beyond the random-phase approximation (RPA), by calculating the vertex correction (VC) and self-energy correction. Due to the spin+orbital mode coupling described by the VC, both orbital and spin fluctuations mutually develop, consistently with the experimental phase diagram with the orbital and magnetic orders. Due to both fluctuations, the s-wave gap function with sign-reversal ($s_{\pm}$-wave), without sign-reversal ($s_{++}$-wa…
Recent high-pressure studies found that superconductivity can be achieved under very low pressure in the parent iron arsenide compound CaFe2As2, although details of the sharpness and temperature of transitions vary between liquid medium and gas medium measurements. To better understand this issue, we performed high-pressure susceptibility and transport studies on CaFe2As2, using helium as the pressure medium. The signatures of the transitions to the low-temperature orthorhombic and collapsed tetragonal phase remained exceptionally sharp and no signature of bulk superconductivity was found unde…
In correlated metals derived from Mott insulators, the motion of an electron is impeded by Coulomb repulsion due to other electrons. This phenomenon causes a substantial reduction in the electron's kinetic energy leading to remarkable experimental manifestations in optical spectroscopy. The high-Tc superconducting cuprates are perhaps the most studied examples of such correlated metals. The occurrence of high-Tc superconductivity in the iron pnictides puts a spotlight on the relevance of correlation effects in these materials. Here we present an infrared and optical study on single crystals of…
The role of nematic fluctuations for unconventional superconductivity has been subject of intense discussions for many years. In iron-based superconductors, the most established probe for electronic-nematic fluctuations, i.e. the elastoresistivity seems to imply that superconductivity is reinforced by electronic-nematic fluctuations, since the elastoresistivity amplitude peaks at or close to optimal $T_C$. However, on the over-doped side of the superconducting dome, the diminishing elastoresistivity suggests a negligible importance in the mechanism of superconductivity. Here we introduce the N…
The response of the worldwide scientific community to the discovery in 2008 of superconductivity at Tc = 26 K in the Fe-based compound LaFeAsO_{1-x}F_x has been very enthusiastic. In short order, other Fe-based superconductors with the same or related crystal structures were discovered with Tc up to 56 K. Many experiments were carried out and theories formulated to try to understand the basic properties of these new materials and the mechanism for Tc. In this selective critical review of the experimental literature, we distill some of this extensive body of work, and discuss relationships betw…
We investigate the pressure and temperature dependence of the lattice dynamics of the underdoped, stoichiometric, high temperature superconductor YBa2Cu4O8 by means of Raman spectroscopy and ab initio calculations. This system undergoes a reversible pressure-induced structural phase transition around 10 GPa to a collapsed orthorhombic structure, that is well reproduced by the calculation. The coupling of the B1g-like buckling phonon mode to the electronic continuum is used to probe superconductivity. In the low pressure phase, self-energy effects through the superconducting transition renormal…
The antiferromagnet CaFe$_2$As$_2$ does not become superconducting when subject to ideal hydrostatic pressure conditions, where crystallographic and magnetic states also are well defined. By measuring electrical resistivity and magnetic susceptibility under quasi-hydrostatic pressure, however, we find that a substantial volume fraction of the sample is superconducting in a narrow pressure range where collapsed tetragonal and orthorhombic structures coexist. At higher pressures, the collapsed tetragonal structure is stabilized, with the boundary between this structure and the phase of coexistin…
The structural flexibility at three substitution sites in LaFeAsO enabled investigation of the relation between superconductivity and structural parameters over a wide range of crystal compositions. Substitutions of Nd for La, Sb or P for As, and F or H for O were performed. All these substitutions modify the local structural parameters, while the F/H-substitution also changes band filling. It was found that the superconducting transition temperature $T_{c}$ is strongly affected by the pnictogen height $h_{Pn}$ from the Fe-plane that controls the electron correlation strength and the size of t…
We present high-energy x-ray diffraction data under applied pressures up to p = 29 GPa, neutron diffraction measurements up to p = 1.1 GPa, and electrical resistance measurements up to p = 5.9 GPa, on SrCo2As2. Our x-ray diffraction data demonstrate that there is a first-order transition between the tetragonal (T) and collapsed-tetragonal (cT) phases, with an onset above approximately 6 GPa at T = 7 K. The pressure for the onset of the cT phase and the range of coexistence between the T and cT phases appears to be nearly temperature independent. The compressibility along the a-axis is the same…
Aliovalent rare earth substitution into the alkaline earth site of CaFe2As2 single-crystals is used to fine-tune structural, magnetic and electronic properties of this iron-based superconducting system. Neutron and single crystal x-ray scattering experiments indicate that an isostructural collapse of the tetragonal unit cell can be controllably induced at ambient pressures by choice of substituent ion size. This instability is driven by the interlayer As-As anion separation, resulting in an unprecedented thermal expansion coefficient of $180\times 10^{-6}$ K$^{-1}$. Electrical transport and ma…
In the family of iron-based superconductors, LaFeAsO-type materials possess the simplest electronic structure due to their pronounced two-dimensionality. And yet they host superconductivity with the highest transition temperature Tc=55K. Early theoretical predictions of their electronic structure revealed multiple large circular portions of the Fermi surface with a very good geometrical overlap (nesting), believed to enhance the pairing interaction and thus superconductivity. The prevalence of such large circular features in the Fermi surface has since been associated with many other iron-base…
Motivated by the discovery of superconductivity in F-doped LaFeAsO, we investigated the magnetic fluctuations in a related compound Fe(Se1-xTex)0.92 (x = 0.75, 1) using neutron scattering techniques. Non-superconducting FeTe0.92 shows antiferromagnetic (AF) ordering with the ordering vector |Q| = 0.97 A-1 (Q = (0.5,0,0.5)) at TN ~ 70 K and a structural transition between tetragonal and monoclinic phases. In the AF monoclinic phase, the low-energy spectral weight is suppressed, indicating a possible gap formation. On the other hand, in the paramagnetic tetragonal phase, we observed a pronounced…
We present uniaxial pressure structural relaxations for CaFe2As2 and BaFe2Ase2 within density functional theory and compare them with calculations under hydrostatic pressure conditions as well as available experimental results. We find that CaFe2As2 shows a unique phase transition from a magnetic orthorhombic phase to a nonmagnetic collapsed tetragonal phase for both pressure conditions and no indication of a tetragonal phase is observed at intermediate uniaxial pressures. In contrast, BaFe2As2 shows for both pressure conditions two phase transitions from a magnetic orthorhombic to a collapsed…
