arXiv subjects
Publications and source records attributed to P. Gegenwart.
In this article we review our angle- and time-resolved photoemission studies (ARPES and trARPES) on various ferropnictides.
Bilayer strontium ruthenate Sr$_3$Ru$_2$O$_7$ displays pronounced non-Fermi liquid behavior at magnetic fields around 8 T, applied perpendicular to the ruthenate planes, which previously has been associated with an itinerant metamagnetic quantum critical end point (QCEP). We focus on the magnetic Grüneisen parameter $Γ_{\rm H}$, which is the most direct probe to characterize field-induced quantum criticality. We confirm quantum critical scaling due to a putative two-dimensional QCEP near 7.845(5) T, which is masked by two ordered phases A and B, identified previously by neutron scattering. In addition we find evidence for a QCEP at 7.53(2) T and determine the quantum critical regimes of both instabilities and the effect of their superposition.
The layered honeycomb magnet $α$-Li$_2$IrO$_3$ has been theoretically proposed as a candidate to display novel magnetic behaviour associated with Kitaev interactions between spin-orbit entangled $j_{\rm eff}=1/2$ magnetic moments on a honeycomb lattice. Here we report single crystal magnetic resonant x-ray diffraction combined with powder magnetic neutron diffraction to reveal an incommensurate magnetic order in the honeycomb layers with Ir magnetic moments counter-rotating on nearest-neighbour sites. This type of magnetic structure has not been reported experimentally before in honeycomb magnets and cannot be explained by a spin Hamiltonian with dominant isotropic (Heisenberg) couplings. The magnetic structure shares many key features with the magnetic order in the structural polytypes $β$ and $γ$-Li$_2$IrO$_3$, understood theoretically to be stabilized by dominant Kitaev interactions between Ir moments located on the vertices of three-dimensional hyperhoneycomb and stripyhoneycomb lattices, respectively. Based on this analogy and a theoretical soft-spin analysis of magnetic ground states for candidate spin Hamiltonians, we propose that Kitaev interactions also dominate in $α$-Li$_2$IrO$_3$, indicative of universal Kitaev physics across all three members of the harmonic honeycomb family of Li$_2$IrO$_3$ polytypes.
In a comprehensive study, we investigate the electronic scattering effects in EuFe$_{2}$(As$_{1-x}$P$_{x}$)$_{2}$ by using Fourier-transform infrared spectroscopy. In spite of the fact that Eu$^{2+}$ local moments order around $T_\text{Eu} \approx 20$\,K, the overall optical response is strikingly similar to the one of the well-known Ba-122 pnictides. The main difference lies within the suppression of the lower spin-density-wave gap feature. By analysing our spectra with a multi-component model, we find that the high-energy feature around 0.7\,eV -- often associated with Hund's rule coupling -- is highly sensitive to the spin-density-wave ordering, this further confirms its direct relationship to the dynamics of itinerant carriers. The same model is also used to investigate the in-plane anisotropy of magnetically detwinned EuFe$_{2}$As$_{2}$ in the antiferromagnetically ordered state, yielding a higher Drude weight and lower scattering rate along the crystallographic $a$-axis. Finally, we analyse the development of the room temperature spectra with isovalent phosphor substitution and highlight changes in the scattering rate of hole-like carriers induced by a Lifshitz transition.
Single crystals of Ca(Fe1-xRux)2As2 (0 0.08. This effect is ascribed to a weakening of interlayer As-As bonds by electron doping. Upon further electron doping filamentary superconductivity with Tc of 41 K at y=0.2 is observed.
Geometrical frustration describes situations where interactions are incompatible with the lattice geometry and stabilizes exotic phases such as spin liquids. Whether geometrical frustration of magnetic interactions in metals can induce unconventional quantum critical points is an active area of research. We focus on the hexagonal heavy fermion metal CeRhSn where the Kondo ions are located on distorted kagome planes stacked along the c axis. Low-temperature specific heat, thermal expansion and magnetic Grüneisen parameter measurements prove a zero-field quantum critical point. The linear thermal expansion, which measures the initial uniaxial pressure derivative of the entropy, displays a striking anisotropy. Critical and noncritical behaviors along and perpendicular to the kagome planes, respectively, prove that quantum criticality is driven by geometrical frustration. We also discovered a spin-flop-type metamagnetic crossover. This excludes an itinerant scenario and suggests that quantum criticality is related to local moments in a spin-liquid like state.
We report inelastic neutron scattering measurements on Na2IrO3, a candidate for the Kitaev spin model on the honeycomb lattice. We observe spin-wave excitations below 5 meV with a dispersion that can be accounted for by including substantial further-neighbor exchanges that stabilize zig-zag magnetic order. The onset of long-range magnetic order below 15.3 K is confirmed via the observation of oscillations in zero-field muon-spin rotation experiments. Combining single-crystal diffraction and density functional calculations we propose a revised crystal structure model with significant departures from the ideal 90 deg Ir-O-Ir bonds required for dominant Kitaev exchange.
Angle-resolved photoemission spectroscopy (ARPES) is used to study the band dispersion and the quasiparticle scattering rates in two ferropnictides systems. Our ARPES results show linear-in-energy dependent scattering rates which are constant in a wide range of control parameter and which depend on the orbital character of the bands. We demonstrate that the linear energy dependence gives rise to weakly dispersing band with a strong mass enhancement when the band maximum crosses the chemical potential. In the superconducting phase the related small effective Fermi energy favors a Bardeen-Cooper-Schrieffer (BCS)\,\cite{Bardeen1957}-Bose-Einstein (BE)\,\cite{Bose1924} crossover state.
We report a study of the local magnetism in thin films of SrRuO3 grown on (111) and (001) oriented SrTiO3 substrates using x-ray magnetic circular dichroism spectroscopy (XMCD) at the Ru-L2,3 edges. The application of the sum rules to the XMCD data gives an almost quenched orbital moment and a spin moment close to the value expected for the low spin state S = 1 . Full-multiplet cluster calculations indicate that the low spin state is quite stable and suggest that the occurrence of a transition to the high spin state S = 2 in strained thin films of SrRuO3 is unlikely as it would be too expensive in energy.
The magnetic structure of the Eu2+ moments in the superconducting EuFe2(As1-xPx)2 sample with x = 0.19 has been determined using neutron scattering. We conclude that the Eu2+ moments are aligned along the c direction below T_C = 19.0(1) K with an ordered moment of 6.6(2) mu_B in the superconducting state. An impurity phase similar to the underdoped phase exists within the bulk sample which orders antiferromagnetically below T_N = 17.0(2) K. We found no indication of iron magnetic order, nor any incommensurate magnetic order of the Eu2+ moments in the sample.
Our comprehensive study on EuFe$_2$As$_2$ reveals a dramatic reduction of magnetic detwinning fields compared to other AFe$_2$As$_2$ (A = Ba, Sr, Ca) iron pnictides by indirect magneto-elastic coupling of the Eu$^{2+}$ ions. We find that only 0.1T are sufficient for persistent detwinning below the local Eu$^{2+}$ ordering; above $T_\text{Eu}$ = 19K, higher fields are necessary. Even after the field is switched off, a significant imbalance of twin domains remains constant up to the structural and electronic phase transition (190K). This persistent detwinning provides the unique possibility to study the low temperature electronic in-plane anisotropy of iron pnictides without applying any symmetrybreaking external force.
The recently-synthesized iridate $β$-Li$_2$IrO$_3$ has been proposed as a candidate to display novel magnetic behavior stabilized by frustration effects from bond-dependent, anisotropic interactions (Kitaev model) on a three-dimensional "hyperhoneycomb" lattice. Here we report a combined study using neutron powder diffraction and magnetic resonant x-ray diffraction to solve the complete magnetic structure. We find a complex, incommensurate magnetic order with non-coplanar and counter-rotating Ir moments, which surprisingly shares many of its features with the related structural polytype "stripyhoneycomb" $γ$-Li$_2$IrO$_3$, where dominant Kitaev interactions have been invoked to explain the stability of the observed magnetic structure. The similarities of behavior between those two structural polytypes, which have different global lattice topologies but the same local connectivity, is strongly suggestive that the same magnetic interactions and the same underlying mechanism governs the stability of the magnetic order in both materials, indicating that both $β$- and $γ$-Li$_2$IrO$_3$ are strong candidates to realize dominant Kitaev interactions in a solid state material.
Na2IrO3 is an intriguing material for which spin-orbit coupling plays a key role. Theoretical predictions, so far unverified, have been made that the surface of Na2IrO3 should exhibit a clear signature of the quantum spin Hall effect. We studied the surface of Na2IrO3 using scanning tunneling microscopy and density-functional theory calculations. We observed atomic level resolution of the surface and two types of terminations with different surface periodicity and Na content. By comparing bias-dependent experimental topographic images to simulated images, we determined the detailed atomistic structure of both observed surfaces. One of these reveals a strong relaxation to the surface of Na atoms from the subsurface region two atomic layers below. Such dramatic structural changes at the surface cast doubt on any prediction of surface properties based on bulk electronic structure. Indeed, using spatially resolved tunneling spectroscopy we found no indication of the predicted quantum spin Hall behavior.
We have investigated experimentally and theoretically the series (Na$_{1-x}$Li$_{x}$)$_{2}$IrO$_{3}$. Contrary to what has been believed so far, only for $x\leq0.25$ the system forms uniform solid solutions. For larger Li content, as evidenced by powder X-ray diffraction, scanning electron microscopy and density functional theory calculations, the system shows a miscibility gap and a phase separation into an ordered Na$_{3}$LiIr$_2$O$_{6}$ phase with alternating Na$_3$ and LiIr$_2$O$_6$ planes, and a Li-rich phase close to pure Li$_{2}$IrO$_{3}$. For $x\leq 0.25$ we observe (1) an increase of $c/a$ with Li doping up to $x=0.25$, despite the fact that $c/a$ in pure Li$_{2}$IrO$_{3}$ is smaller than in Na$_{2}$IrO$_{3}$, and (2) a gradual reduction of the antiferromagnetic ordering temperature $T_{N}$ and ordered moment. The previously proposed magnetic quantum phase transition at $x\approx 0.7$ may occur in a multiphase region and its nature needs to be re-evaluated.
We have synthesized single crystals of Na$_2$(Ir$_{1-x}$Ti$_x$)O$_3$ and polycrystals of Li$_2$(Ir$_{1-x}$Ti$_x$)O$_3$ and studied the effect of magnetic depletion on the magnetic properties by measurements of the magnetic susceptibility, specific heat and magnetocaloric effect at temperatures down to 0.1~K. In both systems, the non-magnetic substitution rapidly changes the magnetically ordered ground state into a spin glass, indicating strong frustration. While for the Li system the Weiss temperature $Θ_{\rm W}$ remains unchanged up to $x=0.55$, a strong decrease $|Θ_{\rm W}|$ is found for the Na system. This suggests that only for the former system magnetic exchange beyond nearest neighbors is dominating. This is also corroborated by the observation of a smeared quantum phase transition in Li$_2$(Ir$_{1-x}$Ti$_x$)O$_3$ near $x=0.5$, i.e. much beyond the site percolation threshold of the honeycomb lattice.
A burning question in the emerging field of spin-orbit driven insulating iridates, such as Na2IrO3 and Li2IrO3 is whether the observed insulating state should be classified as a Mott-Hubbard insulator derived from a half-filled relativistic j_eff=1/2 band or as a band insulator where the gap is assisted by spin-orbit interaction, or Coulomb correlations, or both. The difference between these two interpretations is that only for the former, strong spin-orbit coupling (lambda >~ W, where W is the band width) is essential. We have synthesized the isostructural and isoelectronic Li2RhO3 and report its electrical resistivity and magnetic susceptibility. Remarkably it shows insulating behavior together with fluctuating effective S=1/2 moments, similar to Na2IrO3 and Li2IrO3, although in Rh4+ (4d5) the spin-orbit coupling is greatly reduced. We show that this behavior has non-relativistic one-electron origin (although Coulomb correlations assist in opening the gap), and can be traced down to formation of quasi-molecular orbitals, similar to those in Na2IrO3.
When magnetic order is suppressed by frustrated interactions, spins form a highly correlated fluctuating "spin liquid" state down to low temperatures. Magnetic order of local moments can also be suppressed when they are fully screened by conduction electrons through the Kondo effect. Thus, the combination of strong geometrical frustration and Kondo screening may lead to novel types of quantum phase transitions. We report low-temperature thermodynamic measurements on the frustrated Kondo lattice Pr$_2$Ir$_2$O$_7$, which displays a chiral spin liquid state below 1.5 K due to the frustrated interaction between Ising 4f local moments and their interplay with Ir conduction electrons. Our results provide a first clear example of zero-field quantum critical scaling that emerges in a spin liquid state of a highly frustrated metal.
The magnetic structure of the Eu2+ moments in the superconducting EuFe2(As1-xPx)2 sample with x = 0.15 has been determined using element specific x-ray resonant magnetic scattering. Combining magnetic, thermodynamic and scattering measurements, we conclude that the long range ferromagnetic order of the Eu2+ moments aligned primarily along the c axis coexists with the bulk superconductivity at zero field. At an applied magnetic field >= 0.6 T, superconductivity still coexists with the ferromagnetic Eu2+ moments which are polarized along the field direction. We propose a spontaneous vortex state for the coexistence of superconductivity and ferromagnetism in EuFe2(As0.85P0.15)2.