skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.

Explore Research Products in the PAR
It may take a few hours for recently added research products to appear in PAR search results.


Title: Effects of the on-site energy on the electronic response of Sr3(Ir1−xMnx)2O7
Abstract We investigated the doping and temperature evolutions of the optical response of Sr3(Ir1−xMnx)2O7single crystals with 0 ≤ x ≤ 0.36 by utilizing infrared spectroscopy. Substitution of 3dtransition metal Mn ions into Sr3Ir2O7is expected to induce an insulator-to-metal transition via the decrease in the magnitude of the spin–orbit coupling and the hole doping. In sharp contrast, our data reveal the resilience of the spin–orbit coupling and the incoherent character of the charge transport. Upon Mn substitution, an incoherent in-gap excitation at about 0.25 eV appeared with the decrease in the strength of the optical transitions between the effective total angular momentumJeffbands of the Ir ions. The resonance energies of the optical transitions between theJeffbands which are directly proportional to the magnitude of the spin–orbit coupling hardly varied. In addition to these evolutions of the low-energy response, Mn substitution led to the emergence of a distinct high-energy optical excitation at about 1.2 eV which is larger than the resonance energies of the optical transitions between theJeffbands. This observation indicates that the Mn 3dstates are located away from the Ir 5dstates in energy and that the large difference in the on-site energies of the transition metal ions is responsible for the incoherent charge transport and the robustness of the spin–orbit coupling. The effect of Mn substitution was also registered in the temperature dependence of the electronic response. The anomaly in the optical response of the parent compound observed at the antiferromagnetic transition temperature is notably suppressed in the Mn-doped compounds despite the persistence of the long-range antiferromagnetic ordering. The suppression of the spin-charge coupling could be related to charge disproportionation of the Ir ions.  more » « less
Award ID(s):
1905801
PAR ID:
10473829
Author(s) / Creator(s):
; ; ; ;
Publisher / Repository:
Scientific Reports
Date Published:
Journal Name:
Scientific Reports
Volume:
12
Issue:
1
ISSN:
2045-2322
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. ; ; ; ; ; ; ; ; ; ; et al (, Nature Communications)
    Abstract Polarons and spin-orbit (SO) coupling are distinct quantum effects that play a critical role in charge transport and spin-orbitronics. Polarons originate from strong electron-phonon interaction and are ubiquitous in polarizable materials featuring electron localization, in particular 3d transition metal oxides (TMOs). On the other hand, the relativistic coupling between the spin and orbital angular momentum is notable in lattices with heavy atoms and develops in 5d TMOs, where electrons are spatially delocalized. Here we combine ab initio calculations and magnetic measurements to show that these two seemingly mutually exclusive interactions are entangled in the electron-doped SO-coupled Mott insulator Ba2Na1−xCaxOsO6(0 < x < 1), unveiling the formation ofspin-orbital bipolarons. Polaron charge trapping, favoured by the Jahn-Teller lattice activity, converts the Os 5d1spin-orbital Jeff = 3/2 levels, characteristic of the parent compound Ba2NaOsO6(BNOO), into a bipolaron 5d2Jeff = 2 manifold, leading to the coexistence of different J-effective states in a single-phase material. The gradual increase of bipolarons with increasing doping creates robust in-gap states that prevents the transition to a metal phase even at ultrahigh doping, thus preserving the Mott gap across the entire doping range from d1BNOO to d2Ba2CaOsO6(BCOO). 
    more » « less
  2. ; ; ; ; ; ; ; (, Communications Physics)
    Abstract Search for novel electronically ordered states of matter emerging near quantum phase transitions is an intriguing frontier of condensed matter physics. In ruthenates, the interplay between Coulomb correlations among the 4delectronic states and their spin-orbit interactions, lead to complex forms of electronic phenomena. Here we investigate the double layered Sr3(Ru1−xMnx)2O7and its doping-induced quantum phase transition from a metal to an antiferromagnetic Mott insulator. Using spectroscopic imaging with the scanning tunneling microscope, we visualize the evolution of the electronic states in real- and momentum-space. We find a partial-gap at the Fermi energy that develops with doping to form a weak Mott insulating state. Near the quantum phase transition, we discover a spatial electronic reorganization into a commensurate checkerboard charge order. These findings bear a resemblance to the universal charge order in the pseudogap phase of cuprates and demonstrate the ubiquity of charge order that emanates from doped Mott insulators. 
    more » « less
  3. ; ; ; ; ; ; ; ; ; ; et al (, npj Quantum Materials)
    Abstract Quantum spin systems such as magnetic insulators usually show magnetic order, but such classical states can give way toquantum liquids with exotic entanglementthrough two known mechanisms of frustration: geometric frustration in lattices with triangle motifs, and spin-orbit-coupling frustration in the exactly solvable quantum liquid of Kitaev’s honeycomb lattice. Here we present the experimental observation of a new kind of frustrated quantum liquid arising in an unlikely place: the magnetic insulator Ba4Ir3O10where Ir3O12trimers form an unfrustrated square lattice. The crystal structure shows no apparent spin chains. Experimentally we find a quantum liquid state persisting down to 0.2 K that is stabilized by strong antiferromagnetic interaction with Curie–Weiss temperature ranging from −766 to −169 K due to magnetic anisotropy. The anisotropy-averaged frustration parameter is 2000, seldom seen in iridates. Heat capacity and thermal conductivity are both linear at low temperatures, a familiar feature in metals but here in an insulator pointing to an exotic quantum liquid state; a mere 2% Sr substitution for Ba produces long-range order at 130 K and destroys the linear-T features. Although the Ir4+(5d5) ions in Ba4Ir3O10appear to form Ir3O12trimers of face-sharing IrO6octahedra, we propose that intra-trimer exchange is reduced and the lattice recombines into an array of coupled 1D chains with additional spins. An extreme limit of decoupled 1D chains can explain most but not all of the striking experimental observations, indicating that the inter-chain coupling plays an important role in the frustration mechanism leading to this quantum liquid. 
    more » « less
  4. ; ; (, Journal of Materials Science)
    Abstract This study investigates the structural, electronic, and magnetic properties of XBr2, XI2, and XBrI (X = Mn, Co) compounds using density functional theory, incorporating spin–orbit coupling and the GGA + U framework. Cohesive and formation energy calculations reveal that MnBr2is most stable in the ferromagnetic phase, while the other compounds favor antiferromagnetic ordering. The inclusion of the effective Coulomb screening potential (Ueff) enhances the localization of 3d orbitals, leading to increased magnetic moments. Electronic structure analyses show that most compounds transition to semiconducting behavior in the antiferromagnetic phase—except CoI2—while MnBr2, CoBr2, and CoI2exhibit half-metallicity in the ferrimagnetic phase. In the antiferromagnetic phase, MnBr2, MnI2, and MnBrI display topological Dirac-like points between theRand Γ points, suggesting the presence of massless fermions and enabling phenomena such as the quantum Hall effect and ultra-high carrier mobility. The computational results are consistent with available experimental data, highlighting the potential of Mn- and Co-based van der Waals compounds for spintronic and quantum applications. 
    more » « less
  5. ; ; (, Advanced Functional Materials)
    Abstract The recent discovery of topological flat bands in twisted transition metal dichalcogenide homobilayers and multilayer graphene has sparked significant research interest. Here, a new platform for realizing tunable topological moiré flat bands: twisted type‐II Rashba homobilayers, is proposed. By maintaining centrosymmetry, the interplay between Rashba spin‐orbit coupling and interlayer interactions generates an effective pseudo‐antiferromagnetic field, opening a gap within the Dirac cone with non‐zero Berry curvature. Using twisted BiTeI bilayers as an example, it is predicted that the emergence of flat topological bands with a remarkably narrow bandwidth (below 20 meV). Notably, the system undergoes a transition from a valley Hall insulator to a quantum spin Hall insulator as the twisting angle increases. This transition arises from a competition between the twisting‐driven effective spin‐orbit coupling and sublattice onsite energies presented in type‐II Rashba moiré structures. The high tunability of Rashba materials in terms of the spin‐orbit coupling strength, interlayer interaction, and twisting angle expands the range of materials suitable for functionalizing and manipulating correlated topological properties. 
    more » « less
  • Citation Formats
  • MLA
  • APA
  • Chicago
  • BibTeX
  • Save / Share this Record
  • Send to Email