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A. Frano

Publications and source records attributed to A. Frano.

At least 19 recordsLinked to original sources

Contrasting Spin Excitations in Octahedral and Square-Planar n=8 Ruddlesden-Popper Nickelates

The discovery of superconductivity in reduced square-planar nickelates marked a major advance in identifying structural and electronic analogs to the high-$T_c$ cuprates. The more recent observation of superconductivity in parent Ruddlesden-Popper (RP) octahedral nickelates with a clear difference in electron count with respect to cuprates raises new questions about the nature of superconductivity across these related but distinct nickelate families. Here, we use Ni $L_3$-edge resonant inelastic x-ray scattering (RIXS) to probe the low-energy excitations in a representative compound of both families: the parent octahedral $n=8$ RP phase Nd$_9$Ni$_8$O$_{25}$ (p-RP), which is non-superconducting, and its reduced square-planar counterpart Nd$_9$Ni$_8$O$_{18}$ (r-RP), which exhibits superconducting correlations with a $T_c \approx 5$ K. The $n=8$ p-RP develops a spin-density-wave (SDW) ground state with ordering wave vector $q_{\mathrm{SDW}} = (1/4,\, 1/4)$, analogous to the bilayer RP, while the $n=8$ r-RP shows an elastic peak at $q^\star = (1/3,\, 0)$. Polarimetric RIXS shows that the p-RP exhibits low-energy spectra dominated by weakly dispersive paramagnons along the 0$\rightarrow\pi$ and $\pi \!\rightarrow\! \pi$ directions, whereas the r-RP with superconducting correlations displays dispersionless magnetic excitations. Our results comprehensively map out the spin excitations and reveal fundamental differences in the ground state between these two distinct structural families.

cond-mat.str-el

Charge order in the Pr substituted YBa$_2$Cu$_3$O$_7$ from high-field Hall effect measurements

The mechanism of doping in the composite Pr$_x$Y$_{1-x}$Ba$_2$Cu$_3$O$_{7-\delta}$ (Pr-YBCO) system is distinct from that of pure YBCO, offering a means to explore the requirements for the numerous electronic orders appearing in the phase diagram. One such example is the ubiquitous 2D charge order and concomitant Fermi surface reconstruction in underdoped YBCO. Here, using magnetotransport and Hall effect measurements, we find signatures of a Fermi surface reconstruction similar to that in pure YBCO indicating the presence of 2D charge order in Pr-YBCO. Additionally, we find that the phase diagrams of Pr-YBCO and YBCO are decidedly symmetric despite the additional disorder in the former and the distinction between hole depletion through Pr substitution and through O reduction. This indicates that while the mechanism of doping differs, the amount of charge carriers in the planes is the most important factor governing the electronic orders in these systems.

cond-mat.supr-con

Magnetoelastic coupling in intercalated transition metal dichalcogenides

The large van der Waals gap in transition metal dichalcogenides (TMDs) offers an avenue to host external metal atoms that modify the ground state of these 2D materials. Here, we experimentally and theoretically address the charge correlations in a family of intercalated TMDs. While short-range charge fluctuations develop in Co$_{1/3}$TaS$_{2}$ and Fe$_{1/3}$TaS$_{2}$, long-range charge order switches-on in Fe$_{1/3}$NbS$_{2}$ driven by the interplay of magnetic order and lattice degrees of freedom. The magnetoelastic coupling is demonstrated in Fe$_{1/3}$NbS$_{2}$ by the enhancement of the charge modulations upon magnetic field below T$_\mathrm{N}$, although Density Functional Perturbation Theory (DFPT) calculations predict negligible electron(spin)-phonon coupling. Furthermore, we show that Co-intercalated TaS$_2$ displays a kagome-like Fermi surface, hence opening the path to engineer electronic band structures and study the entanglement of spin, charge, and spin-phonon mechanisms in the large family of intercalated TMDs.

cond-mat.str-el

Low-energy quasi-circular electron correlations with charge order wavelength in $\textrm{Bi}_2\textrm{Sr}_2\textrm{Ca}\textrm{Cu}_2\textrm{O}_{8+\delta}$

In the study of dynamic charge order correlations in the cuprates, most high energy-resolution resonant inelastic x-ray scattering (RIXS) measurements have focused on momenta along the high-symmetry directions of the copper oxide plane. However, electron scattering along other in-plane directions should not be neglected as they may contain information relevant, for example, to the origin of charge order correlations or to our understanding of the isotropic scattering responsible for strange metal behavior in cuprates. We report high-resolution resonant inelastic x-ray scattering (RIXS) experiments that reveal the presence of dynamic electron correlations over the $q_x$-$q_y$ scattering plane in underdoped $\textrm{Bi}_2\textrm{Sr}_2\textrm{Ca}\textrm{Cu}_2\textrm{O}_{8+\delta}$ with $T_c=54$ K. We use the softening of the RIXS-measured bond stretching phonon line as a marker for the presence of charge-order-related dynamic electron correlations. The experiments show that these dynamic correlations exist at energies below approximately $70$ meV and are centered around a quasi-circular manifold in the $q_x$-$q_y$ scattering plane with radius equal to the magnitude of the charge order wave vector, $q_{CO}$. We also demonstrate how this phonon-tracking procedure provides the necessary experimental precision to rule out fluctuations of short-range directional charge order (i.e. centered around $[q_x=\pm q_{CO}, q_y=0]$ and $[q_x=0, q_y=\pm q_{CO}]$) as the origin of the observed correlations.

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Dynamic electron correlations with charge order wavelength along all directions in the copper oxide plane

In strongly correlated systems the strength of Coulomb interactions between electrons, relative to their kinetic energy, plays a central role in determining their emergent quantum mechanical phases. We perform resonant x-ray scattering on Bi$_2$Sr$_2$CaCu$_2$O$_{8+\delta}$, a prototypical cuprate superconductor, to probe electronic correlations within the CuO$_2$ plane. We discover a dynamic quasi-circular pattern in the $x$-$y$ scattering plane with a radius that matches the wave vector magnitude of the well-known static charge order. Along with doping- and temperature-dependent measurements, our experiments reveal a picture of charge order competing with superconductivity where short-range domains along $x$ and $y$ can dynamically rotate into any other in-plane direction. This quasi-circular spectrum, a hallmark of Brazovskii-type fluctuations, has immediate consequences to our understanding of rotational and translational symmetry breaking in the cuprates. We discuss how the combination of short- and long-range Coulomb interactions results in an effective non-monotonic potential that may determine the quasi-circular pattern.

cond-mat.supr-con

Large response of charge stripes to uniaxial stress in $\textrm{La}_{1.475}\textrm{Nd}_{0.4}\textrm{Sr}_{0.125}\textrm{Cu}\textrm{O}_{4}$

The La-based '214' cuprates host several symmetry breaking phases including superconductivity, charge and spin order in the form of stripes, and a structural othorhombic-to-tetragonal phase transition. Therefore, these materials are an ideal system to study the effects of uniaxial stress onto the various correlations that pervade the cuprate phase diagram. We report resonant x-ray scattering experiments on $\textrm{La}_{1.475}\textrm{Nd}_{0.4}\textrm{Sr}_{0.125}\textrm{Cu}\textrm{O}_{4}$ (LNSCO-125) that reveal a significant response of charge stripes to uniaxial tensile-stress of $\sim$ 0.1 GPa. These effects include a reduction of the onset temperature of stripes by $\sim$ 50 K, a 29 K reduction of the low-temperature orthorhombic-to-tetragonal transition, competition between charge order and superconductivity, and a preference for stripes to form along the direction of applied stress. Altogether, we observe a dramatic response of the electronic properties of LNSCO-125 to a modest amount of uniaxial stress.

cond-mat.str-el

Spectral Evidence for Emergent Order in Ba$_{1-x}$Na$_x$Fe$_2$As$_2$

We report an angle-resolved photoemission spectroscopy study of the iron-based superconductor family, Ba$_{1-x}$Na$_x$Fe$_2$As$_2$. This system harbors the recently discovered double-Q magnetic order appearing in a reentrant C$_4$ phase deep within the underdoped regime of the phase diagram that is otherwise dominated by the coupled nematic phase and collinear antiferromagnetic order. From a detailed temperature-dependence study, we identify the electronic response to the nematic phase in an orbital-dependent band shift that strictly follows the rotational symmetry of the lattice and disappears when the system restores C$_4$ symmetry in the low temperature phase. In addition, we report the observation of a distinct electronic reconstruction that cannot be explained by the known electronic orders in the system.

cond-mat.supr-con

Stabilization of three-dimensional charge order in YBa$_2$Cu$_3$O$_{6+x}$ 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 YBa$_2$Cu$_3$O$_{6+x}$ 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 YBa$_2$Cu$_3$O$_{6+x}$ films grown epitaxially on SrTiO$_3$ 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 CuO$_2$ 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.

cond-mat.str-el

Transfer of magnetic order and anisotropy through epitaxial integration of 3$d$ and 4$f$ spin systems

Resonant x-ray scattering at the Dy $M_5$ and Ni $L_3$ absorption edges was used to probe the temperature and magnetic field dependence of magnetic order in epitaxial LaNiO$_3$-DyScO$_3$ superlattices. For superlattices with 2 unit cell thick LaNiO$_3$ layers, a commensurate spiral state develops in the Ni spin system below 100 K. Upon cooling below $T_{ind} = 18$ K, Dy-Ni exchange interactions across the LaNiO$_3$-DyScO$_3$ interfaces induce collinear magnetic order of interfacial Dy moments as well as a reorientation of the Ni spins to a direction dictated by the strong magneto-crystalline anisotropy of Dy. This transition is reversible by an external magnetic field of 3 T. Tailored exchange interactions between rare-earth and transition-metal ions thus open up new perspectives for the manipulation of spin structures in metal-oxide heterostructures and devices.

cond-mat.str-el

Multiple supersonic phase fronts launched at a complex-oxide hetero-interface

Selective optical excitation of a substrate lattice can drive phase changes across hetero-interfaces. This phenomenon is a non-equilibrium analogue of static strain control in heterostructures and may lead to new applications in optically controlled phase change devices. Here, we make use of time-resolved non-resonant and resonant x-ray diffraction to clarify the underlying physics, and to separate different microscopic degrees of freedom in space and time. We measure the dynamics of the lattice and that of the charge disproportionation in NdNiO3, when an insulator-metal transition is driven by coherent lattice distortions in the LaAlO3 substrate. We find that charge redistribution propagates at supersonic speeds from the interface into the NdNiO3 film, followed by a sonic lattice wave. When combined with measurements of magnetic disordering and of the metal-insulator transition, these results establish a hierarchy of events for ultrafast control at complex oxide hetero-interfaces.

cond-mat.str-el

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 La$_{2/3}$Ca$_{1/3}$MnO$_3$ greatly enhance CDW formation in the optimally doped high-temperature superconductor YBa$_2$Cu$_3$O$_{6+\delta}$ ($\bf \delta \sim 1$), and that this effect persists over several tens of nm. 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.

cond-mat.str-el

Quantitative determination of bond order and lattice distortions in nickel oxide heterostructures by resonant x-ray scattering

We present a combined study of Ni $K$-edge resonant x-ray scattering and density functional calculations to probe and distinguish electronically driven ordering and lattice distortions in nickelate heterostructures. We demonstrate that due to the low crystal symmetry, contributions from structural distortions can contribute significantly to the energy-dependent Bragg peak intensities of a bond-ordered NdNiO$_3$ reference film. For a LaNiO$_3$-LaAlO$_3$ superlattice that exhibits magnetic order, we establish a rigorous upper bound on the bond-order parameter. We thus conclusively confirm predictions of a dominant spin density wave order parameter in metallic nickelates with a quasi-two-dimensional electronic structure.

cond-mat.str-el

Tunable Charge and Spin Order in PrNiO$_3$ Thin Films and Superlattices

We have used polarized Raman scattering to probe lattice vibrations and charge ordering in 12 nm thick, epitaxially strained PrNiO$_3$ films, and in superlattices of PrNiO$_3$ with the band-insulator PrAlO$_3$. A carefully adjusted confocal geometry was 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.

cond-mat.str-el

Resonant X-ray Scattering Study of Charge Density Wave Correlations in YBa$_2$Cu$_3$O$_{6+x}$

We report the results a comprehensive study of charge density wave (CDW) correlations in untwinned YBCO6+x single crystals with 0.4 0.09) an enhancement of the signal when an external magnetic field up to 6 T is applied in the superconducting state. For samples with p~0.08, where prior work has revealed a field-enhancement of incommensurate magnetic order, the RXS signal is field-independent. This supports a previously suggested scenario in which incommensurate charge and spin orders compete against each other, in addition to individually competing against. We discuss the relationship of these results to stripe order 214, the pseudogap phenomenon, superconducting fluctuations, and quantum oscillations.

cond-mat.supr-con

Nonlinear lattice dynamics as a basis for enhanced superconductivity in YBa2Cu3O6.5

THz-frequency optical pulses can resonantly drive selected vibrational modes in solids and deform their crystal structure. In complex oxides, this method has been used to melt electronic orders, drive insulator to metal transitions or induce superconductivity. Strikingly, coherent interlayer transport strongly reminiscent of superconductivity can be transiently induced up to room temperature in YBa2Cu3O6+x. By combining femtosecond X-ray diffraction and ab initio density functional theory calculations, we determine here the crystal structure of this exotic non-equilibrium state. We find that nonlinear lattice excitation in normal-state YBa2Cu3O6+x at 100 K causes a staggered dilation/contraction of the Cu-O2 intra/inter- bilayer distances, accompanied by anisotropic changes in the in-plane O-Cu-O bond buckling. Density functional theory calculations indicate that these motions cause dramatic changes in the electronic structure. Amongst these, the enhancement in the dx2-y2 character of the in-plane electronic structure is likely to favor superconductivity.

cond-mat.supr-con

The symmetry of charge order in cuprates

Charge-ordered ground states permeate the phenomenology of 3d-based transition metal oxides, and more generally represent a distinctive hallmark of strongly-correlated states of matter. The recent discovery of charge order in various cuprate families fueled new interest into the role played by this incipient broken symmetry within the complex phase diagram of high-Tc superconductors. Here we use resonant X-ray scattering to resolve the main characteristics of the charge-modulated state in two cuprate families: Bi2201 and YBCO. We detect no signatures of spatial modulations along the nodal direction in Bi2201, thus clarifying the inter-unit-cell momentum-structure of charge order. We also resolve the intra-unit-cell symmetry of the charge ordered state, which is revealed to be best represented by a bond-order with modulated charges on the O-2p orbitals and a prominent d-wave character. These results provide insights on the microscopic description of charge order in cuprates, and on its origin and interplay with superconductivity.

cond-mat.supr-con

Charge order driven by Fermi-arc instability in Bi2201

The understanding of the origin of superconductivity in cuprates has been hindered by the apparent diversity of intertwining electronic orders in these materials. We combined resonant x-ray scattering (REXS), scanning-tunneling microscopy (STM), and angle-resolved photoemission spectroscopy (ARPES) to observe a charge order that appears consistently in surface and bulk, and in momentum and real space within one cuprate family, Bi2201. The observed wave vectors rule out simple antinodal nesting in the single-particle limit but match well with a phenomenological model of a many-body instability of the Fermi arcs. Combined with earlier observations of electronic order in other cuprate families, these findings suggest the existence of a generic charge-ordered state in underdoped cuprates and uncover its intimate connection to the pseudogap regime.

cond-mat.supr-con

Strain and composition dependence of the orbital polarization in nickelate superlattices

A combined analysis of x-ray absorption and resonant reflectivity data was used to obtain the orbital polarization profiles of superlattices composed of four-unit-cell-thick layers of metallic LaNiO3 and layers of insulating RXO3 (R=La, Gd, Dy and X=Al, Ga, Sc), grown on substrates that impose either compressive or tensile strain. This superlattice geometry allowed us to partly separate the influence of epitaxial strain from interfacial effects controlled by the chemical composition of the insulating blocking layers. Our quantitative analysis reveal orbital polarizations up to 25%. We further show that strain is the most effective control parameter, whereas the influence of the chemical composition of the blocking layers is comparatively small.

cond-mat.str-el