Softening of a flat phonon mode in the kagome ScV6Sn6.

Geometrically frustrated kagome lattices are raising as novel platforms to engineer correlated topological electron flat bands that are prominent to electronic instabilities. Here, we demonstrate a phonon softening at the kz = π plane in ScV6Sn6. The low energy longitudinal phonon collapses at ~98 K and q = [Formula: see text] due to the electron-phonon interaction, without the emergence of long-range charge order which sets in at a different propagation vector qCDW = [Formula: see text]. Theoretical calculations corroborate the experimental finding to indicate that the leading instability is located at [Formula: see text] of a rather flat mode. We relate the phonon renormalization to the orbital-resolved susceptibility of the trigonal Sn atoms and explain the approximately flat phonon dispersion. Our data report the first example of the collapse of a kagome bosonic mode and promote the 166 compounds of kagomes as primary candidates to explore correlated flat phonon-topological flat electron physics.

Order-disorder charge density wave instability in the kagome metal (Cs,Rb)V3Sb5.

The origin of the charge density wave phases in the kagome metal compound AV3Sb5 is still under great scrutiny. Here, we combine diffuse and inelastic x-ray scattering to identify a 3-dimensional precursor of the charge order at the L point that condenses into a CDW through a first order phase transition. The quasi-elastic critical scattering indicates that the dominant contribution to the diffuse precursor is the elastic central peak without phonon softening. However, the inelastic spectra show a small broadening of the Einstein-type phonon mode on approaching TCDW. Our results point to the situation where the Fermi surface instability at the L point is of order-disorder type with critical growth of quasi-static domains. The experimental data indicate that the CDW consists on an alternating Star of David and trihexagonal distortions and its dynamics goes beyond the classical weak-coupling scenario and is discussed within strong-electron phonon coupling and non-adiabatic models.

Spectroscopy of the frustrated quantum antiferromagnet Cs2CuCl4.

We investigate the electronic structure of Cs2CuCl4, a material discussed in the framework of a frustrated quantum antiferromagnet, by means of resonant inelastic x-ray scattering (RIXS) and density functional theory (DFT). From the non-dispersive highly localizedddexcitations, we resolve the crystal field splitting of the Cu2+ions in a strongly distorted tetrahedral coordination. This allows us to model the RIXS spectrum within the crystal field theory (CFT), assign theddorbital excitations and retrieve experimentally the values of the crystal field splitting parametersDq,DsandDτ. The electronic structure obtainedab-initioagrees with the RIXS spectrum and modelled by CFT, highlighting the potential of combined spectroscopic, cluster and DFT calculations to determine the electronic ground state of complex materials.

van der Waals driven anharmonic melting of the 3D charge density wave in VSe2.

Understanding of charge-density wave (CDW) phases is a main challenge in condensed matter due to their presence in high-Tc superconductors or transition metal dichalcogenides (TMDs). Among TMDs, the origin of the CDW in VSe2 remains highly debated. Here, by means of inelastic x-ray scattering and first-principles calculations, we show that the CDW transition is driven by the collapse at 110 K of an acoustic mode at qCDW = (2.25 0 0.7) r.l.u. The softening starts below 225 K and expands over a wide region of the Brillouin zone, identifying the electron-phonon interaction as the driving force of the CDW. This is supported by our calculations that determine a large momentum-dependence of the electron-phonon matrix-elements that peak at the CDW wave vector. Our first-principles anharmonic calculations reproduce the temperature dependence of the soft mode and the TCDW onset only when considering the out-of-plane van der Waals interactions, which reveal crucial for the melting of the CDW phase.

Charge disproportionation and nano phase separation in [Formula: see text].

We have successfully grown centimeter-sized layered [Formula: see text] single crystals under high oxygen pressures of 120-150 bar by the floating zone technique. This enabled us to perform neutron scattering experiments where we observe close to quarter-integer magnetic peaks below [Formula: see text] that are accompanied by steep upwards dispersing spin excitations. Within the high-frequency Ni-O bond stretching phonon dispersion, a softening at the propagation vector for a checkerboard modulation can be observed. We were able to simulate the magnetic excitation spectra using a model that includes two essential ingredients, namely checkerboard charge disproportionation and nano phase separation. The results thus suggest that charge disproportionation is preferred instead of a Jahn-Teller distortion even for this layered [Formula: see text] system.

Stabilization of three-dimensional charge order in YBa2Cu3O6+x via epitaxial growth.

Incommensurate charge order (CO) has been identified as the leading competitor of high-temperature superconductivity in all major families of layered copper oxides, but the perplexing variety of CO states in different cuprates has confounded investigations of its impact on the transport and thermodynamic properties. The three-dimensional (3D) CO observed in YBa2Cu3O6+x in high magnetic fields is of particular interest, because quantum transport measurements have revealed detailed information about the corresponding Fermi surface. Here we use resonant X-ray scattering to demonstrate 3D-CO in underdoped YBa2Cu3O6+x films grown epitaxially on SrTiO3 in the absence of magnetic fields. The resonance profiles indicate that Cu sites in the charge-reservoir layers participate in the CO state, and thus efficiently transmit CO correlations between adjacent CuO2 bilayer units. The results offer fresh perspectives for experiments elucidating the influence of 3D-CO on the electronic properties of cuprates without the need to apply high magnetic fields.

Long-range charge-density-wave proximity effect at cuprate/manganate interfaces.

The interplay between charge density waves (CDWs) and high-temperature superconductivity is currently under intense investigation. Experimental research on this issue is difficult because CDW formation in bulk copper oxides is strongly influenced by random disorder, and a long-range-ordered CDW state in high magnetic fields is difficult to access with spectroscopic and diffraction probes. Here we use resonant X-ray scattering in zero magnetic field to show that interfaces with the metallic ferromagnet La2/3Ca1/3MnO3 greatly enhance CDW formation in the optimally doped high-temperature superconductor YBa2Cu3O6+δ (δ ∼ 1), and that this effect persists over several tens of nanometres. The wavevector of the incommensurate CDW serves as an internal calibration standard of the charge carrier concentration, which allows us to rule out any significant influence of oxygen non-stoichiometry, and to attribute the observed phenomenon to a genuine electronic proximity effect. Long-range proximity effects induced by heterointerfaces thus offer a powerful method to stabilize the charge-density-wave state in the cuprates and, more generally, to manipulate the interplay between different collective phenomena in metal oxides.

Momentum-dependent charge correlations in YBa2Cu3O6+δ superconductors probed by resonant X-ray scattering: evidence for three competing phases.

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).

Orbital control of noncollinear magnetic order in nickel oxide heterostructures.

We have used resonant x-ray diffraction to develop a detailed description of antiferromagnetic ordering in epitaxial superlattices based on two-unit-cell thick layers of the strongly correlated metal LaNiO3. We also report reference experiments on thin films of PrNiO3 and NdNiO3. The resulting data indicate a spiral state whose polarization plane can be controlled by adjusting the Ni d-orbital occupation via two independent mechanisms: epitaxial strain and spatial confinement of the valence electrons. The data are discussed in light of recent theoretical predictions.

Distinct charge orders in the planes and chains of ortho-III-ordered YBa2Cu3O(6+δ) superconductors identified by resonant elastic x-ray scattering.

Recently, charge density wave (CDW) order in the CuO(2) planes of underdoped YBa(2)Cu(3)O(6+δ) was detected using resonant soft x-ray scattering. An important question remains: is the chain layer responsible for this charge ordering? Here, we explore the energy and polarization dependence of the resonant scattering intensity in a detwinned sample of YBa(2)Cu(3)O(6.75) with ortho-III oxygen ordering in the chain layer. We show that the ortho-III CDW order in the chains is distinct from the CDW order in the planes. The ortho-III structure gives rise to a commensurate superlattice reflection at Q=[0.33 0 L] whose energy and polarization dependence agrees with expectations for oxygen ordering and a spatial modulation of the Cu valence in the chains. Incommensurate peaks at [0.30 0 L] and [0 0.30 L] from the CDW order in the planes are shown to be distinct in Q as well as their temperature, energy, and polarization dependence, and are thus unrelated to the structure of the chain layer. Moreover, the energy dependence of the CDW order in the planes is shown to result from a spatial modulation of energies of the Cu 2p to 3d(x(2)-y(2)) transition, similar to stripe-ordered 214 cuprates.

Long-range incommensurate charge fluctuations in (Y,Nd)Ba2Cu3O(6+x).

The concept that superconductivity competes with other orders in cuprate superconductors has become increasingly apparent, but obtaining direct evidence with bulk-sensitive probes is challenging. We have used resonant soft x-ray scattering to identify two-dimensional charge fluctuations with an incommensurate periodicity of ~3.2 lattice units in the copper-oxide planes of the superconductors (Y,Nd)Ba(2)Cu(3)O(6+)(x), with hole concentrations of 0.09 to 0.13 per planar Cu ion. The intensity and correlation length of the fluctuation signal increase strongly upon cooling down to the superconducting transition temperature (T(c)); further cooling below T(c) abruptly reverses the divergence of the charge correlations. In combination with earlier observations of a large gap in the spin excitation spectrum, these data indicate an incipient charge density wave instability that competes with superconductivity.

Long-range transfer of electron-phonon coupling in oxide superlattices.

The electron-phonon interaction is of central importance for the electrical and thermal properties of solids, and its influence on superconductivity, colossal magnetoresistance and other many-body phenomena in correlated-electron materials is the subject of intense research at present. However, the non-local nature of the interactions between valence electrons and lattice ions, often compounded by a plethora of vibrational modes, presents formidable challenges for attempts to experimentally control and theoretically describe the physical properties of complex materials. Here we report a Raman scattering study of the lattice dynamics in superlattices of the high-temperature superconductor YBa(2)Cu(3)O(7) (YBCO) and the colossal-magnetoresistance compound La(2/3)Ca(1/3)MnO(3) that suggests a new approach to this problem. We find that a rotational mode of the MnO(6) octahedra in La(2/3)Ca(1/3)MnO(3) experiences pronounced superconductivity-induced line-shape anomalies, which scale linearly with the thickness of the YBCO layers over a remarkably long range of several tens of nanometres. The transfer of the electron-phonon coupling between superlattice layers can be understood as a consequence of long-range Coulomb forces in conjunction with an orbital reconstruction at the interface. The superlattice geometry thus provides new opportunities for controlled modification of the electron-phonon interaction in complex materials.

Enhanced dimerization of TiOCl under pressure: spin-Peierls to Peierls transition.

We report x-ray diffraction and magnetization measurements under pressure combined with ab initio calculations to show that high-pressure TiOCl corresponds to an enhanced Ti3+-Ti3+ dimerized phase existing already at room temperature. Our results demonstrate the formation of a metal-metal bond between Ti3+ ions along the b axis of TiOCl, accompanied by a strong reduction of the electronic gap. The evolution of the dimerization with pressure suggests a crossover from the spin-Peierls to a conventional Peierls situation at high pressures.

Homopolar bond formation in ZnV2O4 close to a metal-insulator transition.

Electronic structure calculations for spinel vanadate ZnV2O4 show that partial electronic delocalization in this system leads to a structural instability, with the formation of V-V dimers along the [011] and [101] directions, and readily accounts for the intriguing magnetic structure of this material. The formation of V-V bonds is a consequence of the proximity to the itinerant-electron boundary and is not related to orbital ordering. We discuss how this mechanism naturally couples charge and lattice degrees of freedom in magnetic insulators close to such a crossover.

Enhanced pressure dependence of magnetic exchange in A2+[V2]O4 spinels approaching the itinerant electron limit.

We report a systematic enhancement of the pressure dependence of T(N) in A(2+)[V(2)]O(4) spinels as the V-V separation approaches the critical separation for a transition to itinerant-electron behavior. An intermediate phase between localized and itinerant-electron behavior is identified in Zn[V(2)]O(4) and Mg[V(2)]O(4) exhibiting mobile holes as large polarons. Partial electronic delocalization, cooperative ordering of V-V pairs in Zn[V(2)]O(4) below T(s) approximately T(N) and dT(N)/dP<0, signals that lattice instabilities associated with the electronic crossover are a universal phenomenon.