Spin excitations in the overdoped high temperature superconductors Tl_{2}Ba_{2}CuO_{6+δ} and (Bi,Pb)_{2}(Sr,La)_{2}CuO_{6+δ} were investigated by resonant inelastic x-ray scattering (RIXS) as ...functions of doping and detuning of the incoming photon energy above the Cu-L_{3} absorption peak. The RIXS spectra at optimal doping are dominated by a paramagnon feature with peak energy independent of photon energy, similar to prior results on underdoped cuprates. Beyond optimal doping, the RIXS data indicate a sharp crossover to a regime with a strong contribution from incoherent particle-hole excitations whose maximum shows a fluorescencelike shift upon detuning. The spectra of both compound families are closely similar, and their salient features are reproduced by exact-diagonalization calculations of the single-band Hubbard model on a finite cluster. The results are discussed in the light of recent transport experiments indicating a quantum phase transition near optimal doping.
Abstract
In quantum materials, degeneracies and frustrated interactions can have a profound impact on the emergence of long-range order, often driving strong fluctuations that suppress functionally ...relevant electronic or magnetic phases
1–7
. Engineering the atomic structure in the bulk or at heterointerfaces has been an important research strategy to lift these degeneracies, but these equilibrium methods are limited by thermodynamic, elastic and chemical constraints
8
. Here we show that all-optical, mode-selective manipulation of the crystal lattice can be used to enhance and stabilize high-temperature ferromagnetism in YTiO
3
, a material that shows only partial orbital polarization, an unsaturated low-temperature magnetic moment and a suppressed Curie temperature,
T
c
= 27 K (refs.
9–13
). The enhancement is largest when exciting a 9 THz oxygen rotation mode, for which complete magnetic saturation is achieved at low temperatures and transient ferromagnetism is realized up to
T
neq
> 80 K, nearly three times the thermodynamic transition temperature. We interpret these effects as a consequence of the light-induced dynamical changes to the quasi-degenerate Ti
t
2g
orbitals, which affect the magnetic phase competition and fluctuations found in the equilibrium state
14–20
. Notably, the light-induced high-temperature ferromagnetism discovered in our work is metastable over many nanoseconds, underscoring the ability to dynamically engineer practically useful non-equilibrium functionalities.
Abstract Uniaxial pressure provides an efficient approach to control charge density waves in YBa 2 Cu 3 O y . It can enhance the correlation volume of ubiquitous short-range two-dimensional ...charge-density-wave correlations, and induces a long-range three-dimensional charge density wave, otherwise only accessible at large magnetic fields. Here, we use x-ray diffraction to study the strain dependence of these charge density waves and uncover direct evidence for a form of competition between them. We show that this interplay is qualitatively described by including strain effects in a nonlinear sigma model of competing superconducting and charge-density-wave orders. Our analysis suggests that strain stabilizes the 3D charge density wave in the regions between disorder-pinned domains of 2D charge density waves, and that the two orders compete at the boundaries of these domains. No signatures of discommensurations nor of pair density waves are observed. From a broader perspective, our results underscore the potential of strain tuning as a powerful tool for probing competing orders in quantum materials.
Abstract
The unconventional superconductor Sr
2
RuO
4
has long served as a benchmark for theories of correlated-electron materials. The determination of the superconducting pairing mechanism requires ...detailed experimental information on collective bosonic excitations as potential mediators of Cooper pairing. We have used Ru
L
3
-edge resonant inelastic x-ray scattering to obtain comprehensive maps of the electronic excitations of Sr
2
RuO
4
over the entire Brillouin zone. We observe multiple branches of dispersive spin and orbital excitations associated with distinctly different energy scales. The spin and orbital dynamical response functions calculated within the dynamical mean-field theory are in excellent agreement with the experimental data. Our results highlight the Hund metal nature of Sr
2
RuO
4
and provide key information for the understanding of its unconventional superconductivity.
Heavy-fermion metals exhibit a plethora of low-temperature ordering phenomena . Among these are the so-called hidden-order phases that, in contrast to conventional magnetic order, are invisible to ...standard neutron diffraction experiments. One of the structurally most simple hidden-order compounds, CeB6, has been intensively studied for an elusive phase that was attributed to the antiferroquadrupolar ordering of cerium-4f moments . As the ground state of CeB6 is characterized by a more conventional antiferromagnetic (AFM) order , the low-temperature physics of this system has generally been assumed to be governed solely by AFM interactions between the dipolar and multipolar Ce moments . Here we overturn this established picture by observing an intense ferromagnetic (FM) low-energy collective mode that dominates the magnetic excitation spectrum of CeB6. Inelastic neutron-scattering data reveal that the intensity of this FM excitation significantly exceeds that of conventional spin-wave magnons emanating from the AFM wavevectors, thus placing CeB6 much closer to a FM instability than previously anticipated. This propensity for ferromagnetism may account for much of the unexplained behaviour of CeB6, and should lead to a re-examination of existing theories that have so far largely neglected the role of FM interactions.
We use polarized Raman scattering to probe lattice vibrations and charge ordering in 12 nm thick, epitaxially strained PrNiO3 films, and in superlattices of PrNiO3 with the band insulator PrAlO3. A ...carefully adjusted confocal geometry is used to eliminate the substrate contribution to the Raman spectra. In films and superlattices under tensile strain which undergo a metal-insulator transition upon cooling, the Raman spectra reveal phonon modes characteristic of charge ordering. These anomalous phonons do not appear in compressively strained films, which remain metallic at all temperatures. For superlattices under compressive strain, the Raman spectra show no evidence of anomalous phonons indicative of charge ordering, while complementary resonant x-ray scattering experiments reveal antiferromagnetic order associated with a modest increase in resistivity upon cooling. This confirms theoretical predictions of a spin density wave phase driven by spatial confinement of the conduction electrons.
The electric-current stabilized semimetallic state in the quasi-two-dimensional Mott insulator Ca2RuO4 exhibits an exceptionally strong diamagnetism. Through a comprehensive study using neutron and ...x-ray diffraction, we show that this nonequilibrium phase assumes a crystal structure distinct from those of equilibrium metallic phases realized in the ruthenates by chemical doping, high pressure, and epitaxial strain, which in turn leads to a distinct electronic band structure. Dynamical mean field theory calculations based on the crystallographically refined atomic coordinates and realistic Coulomb repulsion parameters indicate a semimetallic state with partially gapped Fermi surface. Our neutron diffraction data show that the nonequilibrium behavior is homogeneous, with antiferromagnetic long-range order completely suppressed. These results provide a new basis for theoretical work on the origin of the unusual nonequilibrium diamagnetism in Ca2RuO4.
We use resonant x-ray scattering to determine the momentum-dependent charge correlations in YBa(2)Cu(3) O(6.55) samples with highly ordered chain arrays of oxygen acceptors (ortho-II structure). The ...results reveal nearly critical, biaxial charge density wave (CDW) correlations at in-plane wave vectors (0.315, 0) and (0, 0.325). The corresponding scattering intensity exhibits a strong uniaxial anisotropy. The CDW amplitude and correlation length are enhanced as superconductivity is weakened by an external magnetic field. Analogous experiments are carried out on a YBa(2)Cu(3)O(6.6) crystal with a dilute concentration of spinless (Zn) impurities, which had earlier been shown to nucleate incommensurate magnetic order. Compared to pristine crystals with the same doping level, the CDW amplitude and correlation length are found to be strongly reduced. These results indicate a three-phase competition between spin-modulated, charge-modulated, and superconducting states in underdoped YBa(2)Cu(3)O(6+δ).
We use high-resolution resonant inelastic x-ray scattering (RIXS) to study a thin film ofNdNiO3, a compound whose unusual spin- and bond-ordered electronic ground state has been of long-standing ...interest. Below the magnetic ordering temperature, we observe well-defined collective magnon excitations along different high-symmetry directions in momentum space. The magnetic spectra depend strongly on the incident photon energy, which we attribute to RIXS coupling to different local electronic configurations of the expanded and compressedNiO6octahedra in the bond-ordered state. Both the noncollinear magnetic ground state and the observed site-dependent magnon excitations are well described by a model that assumes strong competition between the antiferromagnetic superexchange and ferromagnetic double-exchange interactions. Our study provides direct insight into the magnetic dynamics and exchange interactions of the rare-earth nickelates and demonstrates that RIXS can serve as a site-selective probe of magnetism in these and other materials.