Unconventional superconductivity often emerges at the border of long-range magnetic orders. Understanding the low-energy charge dynamics may provide crucial information on the formation of superconductivity. Here we report the unpolarized/polarized optical conductivity study of high quality MnP single crystals at ambient pressure. Our data reveal two types of charge carriers with very different lifetimes. In combination with the first-principles calculations, we show that the short-lifetime carriers have flat Fermi sheets which become gapped in the helimagnetic phase, causing a dramatic change in the low-frequency optical spectra, while the long-lifetime carriers are anisotropic three-dimensional like which are little affected by the magnetic transitions and provide major contributions to the transport properties. This orbital-dependent charge dynamics originates from the special crystal structure of MnP and may have an influence on the unconventional superconductivity and its interplay with helimagnetism at high pressures.
We studied the crystal structure and spin state of MnP under high pressure with synchrotron X-ray diffraction and X-ray emission spectroscopy. MnP has an exceedingly strong anisotropy in compressibility, with the primary compressible direction along the b axis of the Pnma structure. X-ray emission spectroscopy reveals a pressure-driven quenching of the spin state in MnP. Firstprinciples calculations suggest that the strongly anisotropic compression behavior significantly enhances the dispersion of the Mn d-orbitals and the splitting of the d orbital levels compared to the hypothetical isotropi…
Unconventional superconductors are often characterized by numerous competing and even intertwined orders in their phase diagrams. In particular, the electronic nematic phases, which spontaneously break rotational symmetry and often simultaneously involve spin, charge and/or orbital orders, appear conspicuously in both the cuprate and iron-based superconductors. The fluctuations associated with these phases may provide the exotic pairing glue that underlies their high-temperature superconductivity. Helimagnet MnP, the first Mn-based superconductor under pressure, lacks high rotational symmetry.…
We theoretically examine the orbital excitations coupled to the spin degree of freedom in the parent state of the iron-arsenide superconductor, based on the calculation in a five-band itinerant model. The calculated Fe $L_3$-edge resonant inelastic x-ray scattering (RIXS) spectra disclose the presence of spin-flip excitations involving several specific orbitals. Magnon excitations predominantly composed of a single orbital component can be seen in experiments, although its spectral weight is smaller than spin-flipped interorbital high-energy excitations. The detailed polarization and momentum …
We report a polarization-resolved Raman spectroscopy study of the orbital dependence of the quasiparticles properties in the prototypical multi-band Fermi liquid Sr\textsubscript{2}RuO\textsubscript{4}. We show that the quasiparticle scattering rate displays $ω^{2}$ dependence as expected for a Fermi liquid. Besides, we observe a clear polarization-dependence in the energy and temperature dependence of the quasiparticle scattering rate and mass, with the $d_{xz/yz}$ orbital derived quasiparticles showing significantly more robust Fermi liquid properties than the $d_{xy}$ orbital derived ones. …
We have performed an angle-resolved photoemission study of the hole-overdoped iron pnictide superconductor KFe2As2, which shows a low Tc of ~4 K. Most of the observed Fermi surfaces show nearly two-dimensional shapes, while a band near the Fermi level shows a strong dispersion along the kz direction and forms a small three-dimensional hole pocket centered at the Z point, as predicted by band-structure calculation. However, hole Fermi surfaces of yz and zx orbital character centered at the Γpoint of the two-dimensional Brillouin zone are smaller than those predicted by the calculation while the…
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…
In this work, we study a biquadratic Heisenberg model with coupled orbital degree of freedom using Monte Carlo simulation in order to investigate the phase transitions in iron-based superconductors. The antiferro-quadrupolar state, which may be related to the magnetism of FeSe [Phys. Rev. Lett. 115, 116401 (2015)], is stabilized by the anisotropic biquadratic interaction induced by a ferro-orbital-ordered state. It is revealed that the orbital and nematic transitions occur at the same temperature for all the cases, supporting the mechanism of the orbital-driven nematicity as revealed in most r…
Ag$_5$Pb$_2$O$_6$ has attracted considerable attention due to its novel nearly-free-electron superconductivity, but its electronic structure and orbital character of the Cooper-pair electrons remain controversial. Here, we present a method utilizing core-level photoemission to show that Pb 6$s$ electrons dominate near the Fermi level. We observe a strongly asymmetric Pb 4$f_{7/2}$ core-level spectrum, while a Ag 3$d_{5/2}$ spectrum is well explained by two symmetric peaks. The asymmetry in the Pb 4$f_{7/2}$ spectrum originates from the local attractive interaction between conducting Pb 6$s$ el…
We report transient optical signatures of the orbital-selective Mottness in superconducting KxFe2-ySe2 crystals by using dual-color pump-probe spectroscopy. Besides multi-exponential decay recovery dynamics of photo-induced quasiparticles, a damped oscillatory component due to coherent acoustic phonons emerges when the superconducting phase is suppressed by increasing the temperature or excitation power. The oscillatory component diminishes with significant enhancement of a slow decay component upon raising temperature to 150-160 K. These results are in consistence with the picture of orbital-…
We have investigated the electronic structure of BiS$_2$-based CeO$_{0.5}$F$_{0.5}$BiS$_2$ superconductor using polarization-dependent angle-resolved photoemission spectroscopy (ARPES), and succeeded in elucidating the orbital characters on the Fermi surfaces. In the rectangular Fermi pockets around X point, the straight portion parallel to the $k_y$ direction is dominated by Bi $6p_x$ character. The orbital polarization indicates the underlying quasi-one-dimensional electronic structure of the BiS$_2$ system. Moreover, distortions on tetragonally aligned Bi could give rise to the band Jahn-Te…
In its ground state, RuO2 was long thought to be an ordinary metallic paramagnet. Recent neutron and x-ray diffraction revealed that bulk RuO2 is an antiferromagnet (AFM) with TN above 300 K. Furthermore, epitaxial strain induces novel superconductivity in thin films of RuO2 below 2 K. Here, we present a resonant elastic x-ray scattering (REXS) study at the Ru L2 edge of the strained RuO2 films exhibiting the strain-induced superconductivity. We observe an azimuthal modulation of the 100 Bragg peak consistent with canted AFM found in bulk. Most notably, in the strained films displaying novel s…
We performed temperature dependent X-ray linear dichroism (XLD) experiments on an iron pnictide system, Ba(Fe$_{1-x}$Co$_x$)$_2$As$_2$ with $x$=0.00 and 0.05, to experimentally verify existence of orbital ordering (OO). We observed clear XLD in polarization dependent X-ray absorption spectra of Fe $L$ edges. By exploiting the difference in the temperature dependent behaviors, we were able to separate OO and structure contributions to XLD. The observed OO signal indicates different occupation numbers for $d_{yz}$ and $d_{zx}$ orbitals and supports existence of a ferro-OO. The results are also c…
We measure the nuclear quadrupole resonance (NQR) signal on the Zn site in nearly optimally doped YBa$_2$Cu$_3$O$_{6.92}$, when Cu is substituted by 3\% of isotopically pure $^{67}$Zn. We observe that Zn creates large insulating islands, confirming two earlier conjectures: that doping provokes an orbital transition in the CuO$_2$ plane, which is locally reversed by Zn substitution, and that the islands are antiferromagnetic. Also, we find that the Zn impurity locally induces a breaking of the D$_4$ symmetry. Cluster and DFT calculations show that the D$_4$ symmetry breaking is due to the same …
Recent several experiments revealed that novel bipartite magnetic/superconducting phases widely exist in iron pnictides and chalcogenides. Nevertheless, the origin of the two-dome superconducting phases in iron-based compounds still remains unclear. Here we theoretically investigated the electronic structures, magnetic and superconducting properties of three representative iron-based systems, i.e. LaFeAsO1-xHx, LaFeAs1-xPxO and KFe2As2. We found that in addition to the degenerate in-plane anisotropic xz/yz orbitals, the quasi-degenerate in-plane isotropic orbitals drive these systems entering …
Orbital-Selective Coexistence of Interlayer Spin-Singlet Formation and SDW Order with Anomalous Spin Reconfiguration in Bilayer Nickelate La$_{3}$Ni$_{2}$O$_{7}$ Revealed by $^{17}$O-NMR
The University of Osaka（大阪大学）；The University of Tokyo（东京大学）；National Institute for Materials Science (NIMS)（国立材料研究所）
We use quantum oscillation measurements to distinguish between spin and orbital components of the lowest energy quasiparticle excitations in YBa2Cu3O6.54, each of which couple differently to a magnetic field. Our measurements reveal the phase of the observed quantum oscillations to remain uninverted over a wide angular range, indicating that the twofold spin degeneracy of the Landau levels is virtually unaltered by the magnetic field. The inferred suppression of the spin degrees of freedom indicates a spin density-wave is responsible for creation of the small Fermi surface pockets in underdope…
Spin-orbit coupling has been conjectured to play a key role in the low-energy electronic structure of Sr2RuO4. Using circularly polarized light combined with spin- and angle-resolved photoemission spectroscopy, we directly measure the value of the effective spin-orbit coupling to be 130 +/- 30 meV. This is even larger than theoretically predicted and comparable to the energy splitting of the dxy and dxz,yz orbitals around the Fermi surface, resulting in a strongly momentum-dependent entanglement of spin and orbital character. As demonstrated by the spin expectation value obtained for a pair of…
We report on 31P-NMR studies of LaFe(As_{1-x}P_x)(O_{1-y}F_{y}) over wide compositions for 0<x<1 and 0<y<0.14, which provide clear evidence that antiferromagnetic spin fluctuations (AFMSFs) are one of the indispensable elements for enhancing Tc. Systematic 31P-NMR measurements revealed two types of AFMSFs in the temperature evolution, that is, one is the AFMSFs that develop rapidly down to Tc with low-energy characteristics, and the other, with relatively higher energy than the former, develops gradually upon cooling from high temperature. The low-energy AFMSFs in low y (electron doping) over …
The puzzling nature of magnetic and lattice phase transitions of iron pnictides is investigated via a first-principles Wannier function analysis of representative parent compound LaOFeAs. A rare ferro-orbital ordering is found to give rise to the recently observed highly anisotropic magnetic coupling, and drive the phase transitions--without resorting to widely employed frustration or nesting picture. The revealed necessity of the additional orbital physics leads to a correlated electronic structure fundamentally distinct from that of the cuprates. In particular, the strong coupling to the mag…
Magnetic Field Dependence of the Spin Susceptibility on Conventional s-wave Superconductor LaRu$_4$P$_{12}$ Revealed by $^{31}$P-NMR and $^{139}$La-NMR
The weak interlayer Van Der Waals material \{beta}-Bi2Pd has recently been established as a strong topological superconductor candidate with unconventional spin-triplet pairing and Majorana zero modes at vortices. In this letter, we study the topological characters and the superconducting pairing, which are still obscure in monolayer \{beta}-Bi2Pd, in light of our effective theoretical model. We find that the non-Rashba spin-orbital coupling plays a critical role in realizing and tuning various novel topological natures. In particular, the spin-triplet p-wave superconducting pairing with Major…
