Interaction between electrons and phonons in solids is a key effect defining the physical properties of materials, such as electrical and thermal conductivity. In transition metal dichalcogenides (TMDCs), the electron-phonon coupling results in the formation of polarons, quasiparticles that manifest themselves as discrete features in the electronic spectral function. In this study, we report the formation of polarons at the alkali-dosed MoSe2 surface, where Rashba-like spin splitting of the conduction band states is caused by an inversion-symmetry breaking electric field. In addition, we observed a crossover from phonon-like to plasmon-like polaronic spectral features at the MoSe2 surface with increasing doping. Our findings support the concept of electron-phonon coupling-mediated superconductivity in electron-doped layered TMDC materials, as observed using ionic liquid gating technology. Furthermore, the discovered spin-splitting at the Fermi level could offer crucial experimental validation for theoretical models of Ising-type superconductivity in these materials.
The discovery of unconventional superconductivity in a broad class of iron-based materials invoked extensive research on the corresponding compounds of other transition metals. For instance, BaNi2P2 exhibits a superconducting transition with a critical temperature Tc = 2.5 K, and is isostructural to the 122 families of the iron arsenides, suggesting that this Ni-based compound may be another example of unconventional superconductivity. Here we report a detailed analysis of the high-pressure behavior of the angle- and magnetic field-dependent electrical resistivity. The experimentally observed decrease of Tc under the applied pressure matches well with the theoretical prediction based on Migdal-Eliashberg theory, providing evidence in favor of a conventional nature of superconductivity in the nickel analogs of the iron superconductors.
The electronic structures of the iron-based superconductors have been intensively studied by using angle-resolved photoemission spectroscopy (ARPES). A considerable amount of research has been focused on the LaFeAsO family, showing the highest transition temperatures, where previous ARPES studies have found much larger Fermi surfaces than bulk theoretical calculations would predict. The discrepancy has been attributed to the presence of termination-dependent surface states. Here, using photoemission spectroscopy with a sub-micron focused beam spot (nano-ARPES) we have successfully measured the electronic structures of both the LaO and FeAs terminations in LaFeAsO. Our data reveal very different band dispersions and core-level spectra for different surface terminations, showing that previous macro-focus ARPES measurements were incomplete. Our results give direct evidence for the surface-driven electronic structure reconstruction in LaFeAsO, including formation of the termination-dependent surface states at the Fermi level. This experimental technique, which we have shown to be very powerful when applied to this prototypical compound, can now be used to study various materials with different surface terminations.
In the novel stoichiometric iron-based material RbEuFe4As4 superconductivity coexists with a peculiar long-range magnetic order of Eu 4f states; their coexistance is puzzling and represents a challenge for both experiment and theory. Using angle-resolved photoemission spectroscopy, resonant photoemission spectroscopy, Andreev reflection spectroscopy and scanning tunneling spectroscopy we have addressed this puzzle and unambigously shown that Fe- and Eu-derived states are largely decoupled and that superconducting and a long range magnetic orders exist almost independently from each other.
In the novel stoichiometric iron-based material RbEuFe4As4, superconductivity coexists with a peculiar long-range magnetic order of Eu 4f states. Using angle-resolved photoemission spectroscopy, we reveal a complex three-dimensional electronic structure and compare it with density functional theory calculations. Multiple super-conducting gaps were measured on various sheets of the Fermi surface. High-resolution resonant photoemission spectroscopy reveals magnetic order of the Eu 4f states deep into the superconducting phase. Both the absolute values and the anisotropy of the superconducting gaps are remarkably similar to the sibling compound without Eu, indicating that Eu magnetism does not affect the pairing of electrons. A complete decoupling between Fe-and Eu-derived states was established from their evolution with temperature, thus unambiguously demonstrating that superconducting and a long-range magnetic orders exist independently from each other. The established electronic structure of RbEuFe4As4 opens opportunities for the future studies of the highly unorthodox electron pairing and phase competition in this family of iron-based superconductors with doping.
The electronic spectral function of BaNi$_2$As$_2$ is investigated using both the angle-resolved photoemission spectroscopy (ARPES) and a combined computational scheme of local density approximation together with dynamical mean-field theory (LDA+DMFT). In contrast to well studied isostructural iron arsenide high temperature superconductors, the BaNi$_2$As$_2$ demonstrate weak correlation effects although Ni-3d elections have even lager on-site interaction than Fe-3d ones. LDA+DMFT effective mass enhancement for bands crossing the Fermi level is found to be only about $1.2$ which agrees well with ARPES data. This reduction of the correlation manifestation with respect to iron pnictides comes from the increase of 3d-orbital filling, when going from Fe to Ni. The electron correlations cause remarkable reconstruction of the bare BaNi$_2$As$_2$ LDA band structure below $-0.8$ eV due to self-energy effect. A simplified toy model to understand weakness of correlation effects in BaNi$_2$As$_2$ and to describe the LDA+DMFT self-energy shape is discussed. For more realistic comparison of LDA+DMFT spectral function maps with ARPES data we take into account several experimental features: the photoemission cross-section, the experimental energy and angular resolutions and the photo-hole lifetime effects. Thus presented here LDA+DMFT calculations with experimental features included provide nearly qualitative agreement with ARPES data and assure the observation of a dramatic apparent decrease of the correlation strength compared to the Fe compounds.
In the novel stoichiometric iron-based material RbEuFe4As4 superconductivity coexists with a peculiar long-range magnetic order of Eu 4f states; their coexistance is puzzling and represents a challenge for both experiment and theory. Using angle-resolved photoemission spectroscopy, resonant photoemission spectroscopy, Andreev reflection spectroscopy and scanning tunneling spectroscopy we have addressed this puzzle and unambigously shown that Fe- and Eu-derived states are largely decoupled and that superconducting and a long range magnetic orders exist almost independently from each other.
In the novel stoichiometric iron-based material RbEuFe_4As_4 superconductivity coexists with a peculiar long-range magnetic order of Eu 4f states. Using angle-resolved photoemission spectroscopy, we reveal a complex three dimensional electronic structure and compare it with density functional theory calculations. Multiple superconducting gaps were measured on various sheets of the Fermi surface. High resolution resonant photoemission spectroscopy reveals magnetic order of the Eu 4f states deep into the superconducting phase. Both the absolute values and the anisotropy of the superconducting gaps are remarkably similar to the sibling compound without Eu, indicating that Eu magnetism does not affect the pairing of electrons. A complete decoupling between Fe- and Eu-derived states was established from their evolution with temperature, thus unambiguously demonstrating that superconducting and a long range magnetic orders exist independently from each other. The established electronic structure of RbEuFe_4As_4 opens opportunities for the future studies of the highly unorthodox electron pairing and phase competition in this family of iron-based superconductors with doping.
We measure the electronic structure of FeSe from within individual orthorhombic domains. Enabled by an angle-resolved photoemission spectroscopy beamline with a highly focused beamspot (nano-ARPES), we identify clear stripe-like orthorhombic domains in FeSe with a length scale of approximately 1-5~$\mu$m. Our photoemission measurements of the Fermi surface and band structure within individual domains reveal a single electron pocket at the Brillouin zone corner. This result provides clear evidence for a one-electron pocket electronic structure of FeSe, observed without the application of uniaxial strain, and calls for further theoretical insight into this unusual Fermi surface topology. Our results also showcase the potential of nano-ARPES for the study of correlated materials with local domain structures.
The role of nematic order for the mechanism of high-temperature superconductivity is highly debated. In most iron-based superconductors (IBSs) the tetragonal symmetry is broken already in the normal state, resulting in orthorhombic lattice distortions, static stripe magnetic order, or both. Superconductivity then emerges, at least at weak doping, already from the state with broken C-4 rotational symmetry. One of the few stoichiometric IBSs, lithium iron arsenide superconducts below 18 K and does not display either structural or magnetic transition in the normal state. Here we demonstrate, using angle-resolved photoemission spectroscopy, that even the superconducting state in LiFeAs is also a nematic one. We observe spontaneous breaking of the rotational symmetry in the gap amplitude on all Fermi surfaces, as well as unidirectional distortion of the Fermi pockets. Remarkably, these deformations are hardly visible above superconducting T-c. Our results demonstrate the realization of the phenomenon of superconductivity-induced nematicity in IBSs, emphasizing the intimate relation between them. We suggest a theoretical explanation based on the emergence of a secondary instability inside the superconducting state, which leads to the nematic order and s-d mixing in the gap function.
The BaNi$_2$As$_2$ compound is investigated using both the angle-resolved photoemission spectroscopy (ARPES) in a wide binding energy range and combined computational scheme of local density approximation together with dynamical mean-field theory (LDA+DMFT). For more realistic comparison of LDA+DMFT spectral functions with ARPES data we take into account several experimental features: the photoemission cross-section, the experimental energy and angular resolutions and the photo-hole lifetime effects. In contrast to isostructural iron arsenides the BaNi$_2$As$_2$ within LDA+DMFT appears to be weakly correlated (effective mass enhancement about $1.2$). This dramatic reduction of the correlation strength comes from the increase of 3d-orbital filling, when going from Fe to Ni, together with rather large bare Ni-3d LDA bandwidth. Nevertheless, even weakened electron correlations cause remarkable reconstruction of the bare BaNi$_2$As$_2$ LDA band structure and corresponding LDA+DMFT calculations provide better agreement with ARPES than just renormalized LDA results.
Spectroscopic detection of Dirac and Weyl fermions in real materials is vital for both, promising applications and fundamental bridge between high-energy and condensed-matter physics. While the presence of Dirac and noncentrosymmetric Weyl fermions is well established in many materials, the magnetic Weyl semimetals still escape direct experimental detection. In order to find a time-reversal symmetry breaking Weyl state we design two materials and present here experimental and theoretical evidence of realization of such a state in one of them, YbMnBi 2 . We model the time-reversal symmetry breaking observed by magnetization and magneto-optical microscopy measurements by canted antiferromagnetism and find a number of Weyl points. Using angle-resolved photoemission, we directly observe two pairs of Weyl points connected by the Fermi arcs. Our results not only provide a fundamental link between the two areas of physics, but also demonstrate the practical way to design novel materials with exotic properties.
A fundamental part of the puzzle of unconventional superconductivity in the Fe-based superconductors is the understanding of the magnetic and nematic instabilities of the parent compounds. The issues of which of these can be considered the leading instability, and whether weak- or strong-coupling approaches are applicable, are both critical and contentious. Here, we revisit the electronic structure of BaFe 2 As 2 using angle-resolved photoemission spectroscopy (ARPES). Our high-resolution measurements of samples “detwinned” by the application of a mechanical strain reveal a highly anisotropic 3D Fermi surface in the low-temperature antiferromagnetic phase. By comparison of the observed dispersions with ab initio calculations, we argue that overall it is magnetism, rather than orbital/nematic ordering, which is the dominant effect, reconstructing the electronic structure across the Fe 3 d bandwidth. Finally, using a state-of-the-art nano-ARPES system, we reveal how the observed electronic dispersions vary in real space as the beam spot crosses domain boundaries in an unstrained sample, enabling the measurement of ARPES data from within single antiferromagnetic domains, and showing consistence with the effective mono-domain samples obtained by detwinning.
We propose a novel mechanism of flat band formation based on the relative biasing of only one sublattice against other sublattices in a honeycomb lattice bilayer. The mechanism allows modification of the band dispersion from parabolic to "Mexican hat"-like through the formation of a flattened band. The mechanism is well applicable for bilayer graphene-both doped and undoped. By angle-resolved photoemission from bilayer graphene on SiC, we demonstrate the possibility of realizing this extremely flattened band (< 2-meV dispersion), which extends two-dimensionally in a k-space area around the K¯ point and results in a disk-like constant energy cut. We argue that our two-dimensional flat band model and the experimental results have the potential to contribute to achieving superconductivity of graphene- or graphite-based systems at elevated temperatures.
We report a comprehensive study of the tridimensional nature and orbital character of the low-energy electronic structure in 50% Cobalt doped Ba(Fe1−xCox)2As2 (d6.5), by using polarization- and photon energy-dependent angle-resolved photoemission spectroscopy. An extra electron-like Fermi surface is observed around the Brillouin zone boundary compared with isoelectronic KyFe2−xSe2 (d6.5). The bands near the Fermi level (EF) are mainly derived from Fe/Co 3d t2g orbitals, revealing visible dispersions along the kz direction. In combination with the local density approximation and the dynamical mean-field theory calculations, we find that the As 4p bands are non-renormalized and the whole 3d band needs to be renormalized by a “single” factor of ∼1.6, indicating moderate electronic correlation effects. The “single” factor description of the correlation strength among the different 3d orbitals is also in sharp contrast to orbital-dependent correlation effects in BaFe2As2. Our findings indicate a remarkable reduction of correlation effects with little difference among 3d orbitals in BaFeCoAs2, due to the increased filling of the electronic 3d shell in the presence of significant Hund's coupling. The results support that the electronic correlation effects and multiple orbital physics play an important role in the superconductivity of the 122 system and in other ferropnictides.
The role of nematic order for the mechanism of high-temperature superconductivity is highly debated. In most iron-based superconductors (IBS) the tetragonal symmetry is broken already in the normal state, resulting in orthorhombic lattice distortions, static stripe magnetic order, or both. Superconductivity then emerges, at least at weak doping, already from the state with broken $C_4$ rotational symmetry. One of the few stoichiometric IBS, lithium iron arsenide, superconducts below 18 K and does not display either structural or magnetic transition in the normal state. Here we demonstrate, using angle-resolved photoemission, that even superconducting state in LiFeAs is also a nematic one. We observe spontaneous breaking of the rotational symmetry in the gap amplitude on all Fermi surfaces, as well as unidirectional distortion of the Fermi pockets. Remarkably, these deformations disappear above superconducting $T_c$. Our results demonstrate the realization of a novel phenomenon of superconductivity-induced nematicity in IBS, emphasizing the intimate relation between them. We suggest a theoretical explanation based on the emergence of a secondary instability inside the superconducting state, which leads to the nematic order and s-d mixing in the gap function.
We use high-resolution angle-resolved photoemission spectroscopy to map the three-dimensional momentum dependence of the superconducting gap in FeSe. We find that on both the hole and electron Fermi surfaces, the magnitude of the gap follows the distribution of d(yz) orbital weight. Furthermore, we theoretically determine the momentum dependence of the superconducting gap by solving the linearized gap equation using a tight-binding model which quantitatively describes both the experimental band dispersions and orbital characters. By considering a Fermi surface only including one electron pocket, as observed spectroscopically, we obtain excellent agreement with the experimental gap structure. Our finding of a scaling between the superconducting gap and the d(yz) orbital weight supports the interpretation of superconductivity mediated by spin fluctuations in FeSe.
The interplay of high- and low-energy mass renormalizations with band shifts reflected by the positions of van Hove singularities (VHS) in the normal-state spectrum of the most strongly hole-overdoped correlated AFe 2 As 2 (A122) with A=K, Cs is discussed phenomenologically from ARPES data and band-structure (GGA) calculations with full spin-orbit coupling. The big increase of the Sommerfeld coefficient γ from K122 to Cs122 is ascribed to an enhanced coupling to low-energy bosons in the vicinity of a quantum critical point to an unknown, yet incommensurate phase different from the commensurate Mott one. We find no sizeable increase in correlations for Cs122 in contrast to Eilers et al. (Phys. Rev. Lett. 116 , 237003 2016 ). The empirical (ARPES) VHS positions as compared with GGA predictions point even to slightly weaker correlations in Cs122 in accord with low- T magnetic susceptibility χ ( T ) data and a decreasing Wilson ratio ∝ χ (0)/ γ .