1. |
- 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.
|
|
2. |
- Revelli, A., et al.
(författare)
-
Resonant inelastic x-ray incarnation of Young's double-slit experiment
- 2019
-
Ingår i: Science Advances. - : American Association for the Advancement of Science (AAAS). - 2375-2548. ; 5:1
-
Tidskriftsartikel (refereegranskat)abstract
- Young's archetypal double-slit experiment forms the basis for modern diffraction techniques: The elastic scattering of waves yields an interference pattern that captures the real-space structure. Here, we report on an inelastic incarnation of Young's experiment and demonstrate that resonant inelastic x-ray scattering (RIXS) measures interference patterns, which reveal the symmetry and character of electronic excited states in the same way as elastic scattering does for the ground state. A prototypical example is provided by the quasi-molecular electronic structure of insulating Ba3CeIr2O9 with structural Ir dimers and strong spin-orbit coupling. The double "slits" in this resonant experiment are the highly localized core levels of the two Ir atoms within a dimer. The clear double-slit-type sinusoidal interference patterns that we observe allow us to characterize the electronic excitations, demonstrating the power of RIXS interferometry to unravel the electronic structure of solids containing, e.g., dimers, trimers, ladders, or other superstructures.
|
|
3. |
- Warzanowski, P., et al.
(författare)
-
Multiple spin-orbit excitons and the electronic structure of alpha-RuCl3
- 2020
-
Ingår i: Physical Review Research. - : American Physical Society (APS). - 2643-1564. ; 2:4
-
Tidskriftsartikel (refereegranskat)abstract
- The honeycomb compound alpha-RuCl3 is widely discussed as a proximate Kitaev spin-liquid material. This scenario builds on spin-orbit entangled j = 1/2 moments arising for a t(2g)(5) electron configuration with strong spin-orbit coupling lambda and a large cubic crystal field. The actual low-energy electronic structure of alpha-RuCl3, however, is still puzzling. In particular, infrared absorption features at 0.30, 0.53, and 0.75 eV seem to be at odds with a j = 1/2 scenario. Also the energy of the spin-orbit exciton, the excitation from j = 1/2 to 3/2, and thus the value of lambda, are controversial. Combining infrared and Raman data, we show that the infrared features can be attributed to single, double, and triple spin-orbit excitons. We find lambda = 0.16 eV and Delta = 42(4) meV for the observed noncubic crystal-field splitting, supporting the validity of the j = 1/2 picture for alpha-RuCl3. The unusual strength of the double excitation is related to the underlying hopping interactions, which form the basis for dominant Kitaev exchange.
|
|
4. |
- Warzanowski, P., et al.
(författare)
-
Spin-orbit coupling in a half-filled ?2? shell : The case of 5?3 K2ReCl6
- 2024
-
Ingår i: Physical Review B. - 2469-9950 .- 2469-9969. ; 109:15
-
Tidskriftsartikel (refereegranskat)abstract
- The half-filled ?2? shell of the configuration usually, in ?? coupling, hosts a ?=3/2 ground state with quenched orbital moment. This state is not Jahn-Teller active. Sufficiently large spin-orbit coupling ? has been predicted to change this picture by mixing in orbital moment, giving rise to a sizable Jahn-Teller distortion. In 5?3K2ReCl6 we study the electronic excitations using resonant inelastic x-ray scattering and optical spectroscopy. We observe on-site intra-?2? excitations below 2 eV and corresponding overtones with two intra-?2? excitations on adjacent sites, the Mott gap at 2.7 eV, ?2?-to-?? excitations above 3 eV, and charge-transfer excitations at still higher energy. The intra-?2? excitation energies are a sensitive measure of ? and Hund's coupling ?H. The sizable value of ?≈0.29eV places K2ReCl6 into the intermediate coupling regime, but ?/?H≈0.6 is not sufficiently large to drive a pronounced Jahn-Teller effect. We discuss the ground state wave function in a Kanamori picture and find that the ?=3/2 multiplet still carries about 97% of the weight. However, the finite admixture of orbital moment allows for subtle effects. We discuss small temperature-induced changes of the optical data and find evidence for a lowering of the ground state by about 3 meV below the structural phase transitions.
|
|
5. |
- Vergara, I., et al.
(författare)
-
Spin-orbit coupling and crystal-field splitting in Ti-doped Ca2RuO4 studied by ellipsometry
- 2022
-
Ingår i: Physical Review B. - : American Physical Society (APS). - 2469-9950 .- 2469-9969. ; 106:8
-
Tidskriftsartikel (refereegranskat)abstract
- In Ca2RuO4, the competition of spin-orbit coupling ζ and tetragonal crystal-field splitting ΔCF has been discussed controversially for many years. The orbital occupation depends on ΔCF/ζ, which allows us to address this ratio via the optical spectral weights of the lowest intersite Mott-Hubbard excitations. We study the optical conductivity of Ca2Ru0.99Ti0.01O4 in the range of 0.75-5 eV by ellipsometry, using the large single crystals that can be grown for small Ti concentrations. Based on a local multiplet calculation, our analysis results in 2.4≤ΔCF/ζ≲4 at 15 K. The dominant crystal field yields a ground state close to xy orbital order but spin-orbit coupling is essential for a quantitative description of the properties. Furthermore, we observe a pronounced decrease of ΔCF with increasing temperature, as expected based on the reduction of octahedral distortions.
|
|