Engineering topics

Chamorro, J. R.

Publications and source records attributed to Chamorro, J. R..

4 records

DOE OSTI2022

Electronic ground state of two nonmagnetic pentavalent honeycomb iridates

Here, we investigate the electronic structure of two Ir 5+ honeycomb iridates, Sr 3 CaIr 2 O 9 and NaIrO 3 , by means of resonant x-ray techniques. We confirm that Sr 3 CaIr 2 O 9 realizes a large spin-orbit driven nonmagnetic J eff =0 singlet ground state despite sizable tetragonal distortions of Ir coordinating octahedra. However, the resonant inelastic x-ray spectra of NaIrO 3 are drastically different from expectations for a Mott insulator with octahedrally coordinated Ir 5+ . We find that the data for NaIrO 3 can be best interpreted as originating from a narrow gap nonmagnetic S=0 band insulating ground state. Our results highlight the complex role of the ligand environment in the electronic structure of honeycomb iridates and the essential role of x-ray spectroscopy to characterize electronic ground states of insulating materials.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Electronic structure of the frustrated diamond lattice magnet NiRh 2 O 4

We report the A -site spinel NiRh 2 O 4 is the only known realization of a spin-1 diamond lattice magnet and is predicted to host unconventional magnetic phenomena driven by frustrated nearest and next-nearest neighbor exchange as well as orbital degeneracy. Previous works found no sign of magnetic order but found a gapped dispersive magnetic excitation indicating a possible valence bond magnetic ground state. However, the presence of many competing low energy degrees of freedom and limited empirical microscopic constraints complicates further analysis. Here we carry out resonant inelastic x-ray scattering (RIXS), x-ray absorption spectroscopy (XAS), and inelastic neutron scattering (INS) to characterize the local electronic structure and lattice dynamics of NiRh 2 O 4 . The RIXS data can be partly described by a single-ion model for tetrahedrally coordinated Ni 2+ and indicates a tetragonal distortion Δt 2 = 70 meV that splits the t 2 orbitals into a high energy orbital singlet and lower energy orbital doublet. We identify features of the RIXS spectra that are consistent with a Rh-Ni two-site excitation indicating strong metal-metal hybridization mediated by oxygen in NiRh 2 O 4 . We also identify signatures of electron-phonon coupling through the appearance of phonon sidebands that dress crystal field excitations. These results establish the key energy scales relevant to the magnetism in NiRh 2 O 4 and further demonstrate that covalency and lattice dynamics play essential roles in controlling the magnetic ground states of A -site spinels.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Enhanced hybridization in the electronic ground state of the intercalated honeycomb iridate Ag 3 LiIr 2 O 6

In this work, we use x-ray spectroscopy at the Ir L 3 /L 2 absorption edge to study powder samples of the intercalated honeycomb magnet Ag 3 LiIr 2 O 6 . Based on x-ray absorption and resonant inelastic x-ray scattering measurements, and exact diagonalization calculations including nearest-neighbor Ir-Ir electron hopping integrals, we argue that the intercalation of Ag atoms results in a delocalized electronic structure with enhanced Ir-O hybridization, departing from the local relativistic j eff =1/2 state. We find that the relative orbital contribution to the magnetic moment is increased and the magnetization density is spatially extended and asymmetric in this hybridized state. Our results confirm the importance of metal-ligand hybridization in the magnetism of transition metal oxides and provide empirical guidance for understanding the collective magnetism in intercalated honeycomb iridates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2021

Integer versus half-integer spin on an approximate honeycomb lattice

Recent interest in honeycomb lattice materials has focused on their potential to host quantum spin liquid (QSL) states. Variations in bond angles and spin allow a range of interesting behaviors on this lattice, from the predicted QSL ground state of the Kitaev model to exotic magnetic orders. Here we report the physical properties of two compounds with rare earths on an approximate honeycomb lattice. Here, the isostructural compounds Nd 2 S 5 Sn (J = 9/2) and Pr 2 S 5 Sn (J = 4) permit a direct comparison of half-integer versus integer spins on this lattice. We find strikingly different magnetic properties for the two compounds. Nd 2 S 5 Sn orders antiferromagnetically at T N ≈ 2.5 K and undergoes several magnetic transitions to other ordered states under applied field. Pr 2 S 5 Sn displays no magnetic ordering transition above T = 0.41 K, and may be proximate to a spin liquid state.

36 MATERIALS SCIENCE↗