| 1. |
|
|
| 2. |
- Magnaterra, M., et al.
(författare)
-
RIXS interferometry and the role of disorder in the quantum magnet Ba3 Ti3-x Irx O9
- 2023
-
Ingår i: Physical Review Research. - : American Physical Society. - 2643-1564. ; 5:1
-
Tidskriftsartikel (refereegranskat)abstract
- Motivated by several claims of spin-orbit-driven spin-liquid physics in hexagonal Ba3Ti3-xIrxO9 hosting Ir2O9 dimers, we report on resonant inelastic x-ray scattering (RIXS) at the Ir L3 edge for different x. We demonstrate that magnetism in Ba3Ti3-xIrxO9 is governed by an unconventional realization of strong disorder, where cation disorder affects the character of the local moments. RIXS interferometry, studying the RIXS intensity over a broad range of transferred momentum q, is ideally suited to assign different excitations to different Ir sites. We find pronounced Ir-Ti site mixing. Both ions are distributed over two crystallographically inequivalent sites, giving rise to a coexistence of quasimolecular singlet states on Ir2O9 dimers and spin-orbit-entangled j=1/2 moments of 5d5Ir4+ ions. RIXS reveals different kinds of strong magnetic couplings for different bonding geometries, highlighting the role of cation disorder for the suppression of long-range magnetic order in this family of compounds.
|
|
| 3. |
- Revelli, A., et al.
(författare)
-
Quasimolecular electronic structure of the spin-liquid candidate Ba3 InIr2 O9
- 2022
-
Ingår i: Physical Review B. - : American Physical Society. - 2469-9950 .- 2469-9969. ; 106:15
-
Tidskriftsartikel (refereegranskat)abstract
- The mixed-valent iridate Ba3InIr2O9 has been discussed as a promising candidate for quantum spin-liquid behavior. The compound exhibits Ir4.5+ ions in face-sharing IrO6 octahedra forming Ir2O9 dimers with three t2g holes per dimer. Our results establish Ba3InIr2O9 as a cluster Mott insulator. Strong intradimer hopping delocalizes the three t2g holes in quasimolecular dimer states while interdimer charge fluctuations are suppressed by Coulomb repulsion. The magnetism of Ba3InIr2O9 emerges from spin-orbit entangled quasimolecular moments with yet unexplored interactions, opening up a new route to unconventional magnetic properties of 5d compounds. Using single-crystal x-ray diffraction we find the monoclinic space group C2/c already at room temperature. Dielectric spectroscopy shows insulating behavior. Resonant inelastic x-ray scattering reveals a rich excitation spectrum below 1.5 eV with a sinusoidal dynamical structure factor that unambiguously demonstrates the quasimolecular character of the electronic states. Below 0.3 eV, we observe a series of excitations. According to exact diagonalization calculations, such low-energy excitations reflect the proximity of Ba3InIr2O9 to a hopping-induced phase transition based on the condensation of a quasimolecular spin-orbit exciton. The dimer ground state roughly hosts two holes in a bonding j=1/2 orbital and the third hole in a bonding j=3/2 orbital.
|
|
| 4. |
- Revelli, A., et al.
(författare)
-
Spin-orbit entangled j=1/2 moments in Ba(2)CWeIrO(6) : A frustrated fcc quantum magnet
- 2019
-
Ingår i: Physical Review B. - : American Physical Society. - 2469-9950 .- 2469-9969. ; 100:8
-
Tidskriftsartikel (refereegranskat)abstract
- We establish the double perovskite Ba2CeIrO6 as a nearly ideal model system for j = 1/2 moments, with resonant inelastic x-ray scattering indicating that the ideal j = 1/2 state contributes by more than 99% to the ground-state wave function. The local j = 1/2 moments form an fcc lattice and are found to order antiferromagnetically at T-N = 14 K, more than an order of magnitude below the Curie-Weiss temperature. Model calculations show that the geometric frustration of the fcc Heisenberg antiferromagnet is further enhanced by a next-nearest neighbor exchange, and a significant size of the latter is indicated by ab initio theory. Our theoretical analysis shows that magnetic order is driven by a bond-directional Kitaev exchange and by local distortions via a strong magnetoelastic effect. Both, the suppression of frustration by Kitaev exchange and the strong magnetoelastic effect are typically not expected for j = 1/2 compounds making Ba2CeIrO6 a riveting example for the rich physics of spin-orbit entangled Mott insulators.
|
|
| 5. |
- Revelli, A., et al.
(författare)
-
Spin-orbit entangled j=1/2 moments in Ba2CeIrO6 : A frustrated fcc quantum magnet
- 2019
-
Ingår i: Physical Review B. - 2469-9950 .- 2469-9969. ; 100:8
-
Tidskriftsartikel (refereegranskat)abstract
- We establish the double perovskite Ba2CeIrO6 as a nearly ideal model system for j = 1/2 moments, with resonant inelastic x-ray scattering indicating that the ideal j = 1/2 state contributes by more than 99% to the ground-state wave function. The local j = 1/2 moments form an fcc lattice and are found to order antiferromagnetically at T-N = 14 K, more than an order of magnitude below the Curie-Weiss temperature. Model calculations show that the geometric frustration of the fcc Heisenberg antiferromagnet is further enhanced by a next-nearest neighbor exchange, and a significant size of the latter is indicated by ab initio theory. Our theoretical analysis shows that magnetic order is driven by a bond-directional Kitaev exchange and by local distortions via a strong magnetoelastic effect. Both, the suppression of frustration by Kitaev exchange and the strong magnetoelastic effect are typically not expected for j = 1/2 compounds making Ba2CeIrO6 a riveting example for the rich physics of spin-orbit entangled Mott insulators.
|
|
| 6. |
- Fumagalli, R., et al.
(författare)
-
Mobile orbitons in Ca2CuO3: Crucial role of Hund's exchange
- 2020
-
Ingår i: Physical Review B. - 2469-9969 .- 2469-9950. ; 101:20
-
Tidskriftsartikel (refereegranskat)abstract
- We investigate the CuL3 edge resonant inelastic x-ray scattering (RIXS) spectra of a quasi-1D antiferromagnet Ca2CuO3. In addition to the magnetic excitations, which are well-described by the two-spinon continuum, we observe two dispersive orbital excitations, the 3d(xy) and the 3d(yz) orbitons. We carry out a quantitative comparison of the RIXS spectra, obtained with two distinct incident polarizations, with a theoretical model. We show that any realistic spin-orbital model needs to include a finite, but realistic, Hund's exchange J(H) approximate to 0.5 eV. Its main effect is an increase in orbiton velocities, so that their theoretically calculated values match those observed experimentally. Even though Hund's exchange also mediates some interaction between spinon and orbiton, the picture of spin-orbit separation remains intact and describes orbiton motion in this compound.
|
|
| 7. |
- Arpaia, Riccardo, 1985, et al.
(författare)
-
Signature of quantum criticality in cuprates by charge density fluctuations
- 2023
-
Ingår i: Nature Communications. - 2041-1723 .- 2041-1723. ; 14:1
-
Tidskriftsartikel (refereegranskat)abstract
- The universality of the strange metal phase in many quantum materials is often attributed to the presence of a quantum critical point (QCP), a zero-temperature phase transition ruled by quantum fluctuations. In cuprates, where superconductivity hinders direct QCP observation, indirect evidence comes from the identification of fluctuations compatible with the strange metal phase. Here we show that the recently discovered charge density fluctuations (CDF) possess the right properties to be associated to a quantum phase transition. Using resonant x-ray scattering, we studied the CDF in two families of cuprate superconductors across a wide doping range (up to p = 0.22). At p* ≈ 0.19, the putative QCP, the CDF intensity peaks, and the characteristic energy Δ is minimum, marking a wedge-shaped region in the phase diagram indicative of a quantum critical behavior, albeit with anomalies. These findings strengthen the role of charge order in explaining strange metal phenomenology and provide insights into high-temperature superconductivity.
|
|
| 8. |
- Braicovich, Lucio, et al.
(författare)
-
Determining the electron-phonon coupling in superconducting cuprates by resonant inelastic x-ray scattering: Methods and results on Nd1+xBa2-xCu3O7-δ
- 2020
-
Ingår i: Physical Review Research. - 2643-1564. ; 2:2
-
Tidskriftsartikel (refereegranskat)abstract
- The coupling between lattice vibration quanta and valence electrons can induce charge-density modulations and decisively influence the transport properties of materials, e.g., leading to conventional superconductivity. In high-critical-temperature superconductors, where electronic correlation is the main actor, the actual role of electron-phonon coupling (EPC) is being intensely debated theoretically and investigated experimentally. We present an in-depth study of how the EPC strength can be obtained directly from resonant inelastic x-ray scattering (RIXS) data through the theoretical approach derived by Ament et al. [Europhys. Lett. 95, 27008 (2011)]. The role of the model parameters (e.g., phonon energy ω0, intermediate state lifetime 1/Γ, EPC matrix element M, and detuning energy Ω) is thoroughly analyzed, providing general relations among them that can be used to make quantitative estimates of the dimensionless EPC g=(M/ω0)2 without detailed microscopic modeling. We then apply these methods to very high-resolution Cu L3-edge RIXS spectra of three Nd1+xBa2−xCu3O7−δ films. For the insulating antiferromagnetic parent compound, the value of M as a function of the in-plane momentum transfer is obtained for Cu-O bond-stretching (breathing) and bond-bending (buckling) phonon branches. For the underdoped and the nearly optimally doped samples, the effects of Coulomb screening and of charge-density-wave correlations on M are assessed. In light of the anticipated further improvements of the RIXS experimental resolution, this work provides a solid framework for an exhaustive investigation of the EPC in cuprates and other quantum materials.
|
|
| 9. |
- Martinelli, L., et al.
(författare)
-
Collective Nature of Orbital Excitations in Layered Cuprates in the Absence of Apical Oxygens
- 2024
-
Ingår i: Physical Review Letters. - 1079-7114 .- 0031-9007. ; 132:6
-
Tidskriftsartikel (refereegranskat)abstract
- We have investigated the 3d orbital excitations in CaCuO2 (CCO), Nd2CuO4 (NCO), and La2CuO4 (LCO) using high-resolution resonant inelastic x-ray scattering. In LCO they behave as well-localized excitations, similarly to several other cuprates. On the contrary, in CCO and NCO the dxy orbital clearly disperses, pointing to a collective character of this excitation (orbiton) in compounds without apical oxygen. We ascribe the origin of the dispersion as stemming from a substantial next-nearest-neighbor (NNN) orbital superexchange. Such an exchange leads to the liberation of the orbiton from its coupling to magnons, which is associated with the orbiton hopping between nearest neighbor copper sites. Finally, we show that the exceptionally large NNN orbital superexchange can be traced back to the absence of apical oxygens suppressing the charge transfer energy.
|
|
| 10. |
- Peng, Y. Y., et al.
(författare)
-
Doping dependence of the electron-phonon coupling in two families of bilayer superconducting cuprates
- 2022
-
Ingår i: Physical Review B. - 2469-9969 .- 2469-9950. ; 105:11
-
Tidskriftsartikel (refereegranskat)abstract
- While electron-phonon coupling (EPC) is crucial for Cooper pairing in conventional superconductors, its role in high-Tc superconducting cuprates is debated. Using resonant inelastic x-ray scattering at the oxygen K edge, we study the EPC in Bi2Sr2CaCu2O8+δ (Bi2212) and Nd1+xBa2-xCu3O7-δ (NBCO) at different doping levels ranging from heavily underdoped (p=0.07) to overdoped (p=0.21). We analyze the data with a localized Lang-Firsov model that allows for the coherent excitations of two phonon modes. While electronic band dispersion effects are non-negligible, we are able to perform a study of the relative values of EPC matrix elements in these cuprate families. In the case of NBCO, the choice of the excitation energy allows us to disentangle modes related to the CuO chains and the CuO2 planes. Combining the results from the two families, we find the EPC strength decreases with doping at q∥=(-0.25,0) r.l.u., but has a nonmonotonic trend as a function of doping at smaller momenta. This behavior is attributed to the screening effect of charge carriers. We also find that the phonon intensity is enhanced in the vicinity of the charge-density-wave excitations while the extracted EPC strength appears to be less sensitive to their proximity. By performing a comparative study of two cuprate families, we are able to identify general trends in the EPC for the cuprates and provide experimental input to theories invoking a synergistic role for this interaction in d-wave pairing.
|
|
| 11. |
- Rossi, Matteo, et al.
(författare)
-
Experimental Determination of Momentum-Resolved Electron-Phonon Coupling
- 2019
-
Ingår i: Physical Review Letters. - 1079-7114 .- 0031-9007. ; 123:2
-
Tidskriftsartikel (refereegranskat)abstract
- We provide a novel experimental method to quantitatively estimate the electron-phonon coupling and its momentum dependence from resonant inelastic x-ray scattering (RIXS) spectra based on the detuning of the incident photon energy away from an absorption resonance. We apply it to the cuprate parent compound NdBa2Cu3O6 and find that the electronic coupling to the oxygen half-breathing phonon branch is strongest at the Brillouin zone boundary, where it amounts to ∼0.17 eV, in agreement with previous studies. In principle, this method is applicable to any absorption resonance suitable for RIXS measurements and will help to define the contribution of lattice vibrations to the peculiar properties of quantum materials.
|
|
