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: From hidden order to antiferromagnetism: Electronic structure changes in Fe-doped URu 2 Si 2
In matter, any spontaneous symmetry breaking induces a phase transition characterized by an order parameter, such as the magnetization vector in ferromagnets, or a macroscopic many-electron wave function in superconductors. Phase transitions with unknown order parameter are rare but extremely appealing, as they may lead to novel physics. An emblematic and still unsolved example is the transition of the heavy fermion compound U R u 2 S i 2 (URS) into the so-called hidden-order (HO) phase when the temperature drops below T 0 = 17.5 K. Here, we show that the interaction between the heavy fermion and the conduction band states near the Fermi level has a key role in the emergence of the HO phase. Using angle-resolved photoemission spectroscopy, we find that while the Fermi surfaces of the HO and of a neighboring antiferromagnetic (AFM) phase of well-defined order parameter have the same topography, they differ in the size of some, but not all, of their electron pockets. Such a nonrigid change of the electronic structure indicates that a change in the interaction strength between states near the Fermi level is a crucial ingredient for the HO to AFM phase transition.  more » « less
Award ID(s):
1810310
PAR ID:
10288884
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ; ; ; ; ;
Date Published:
Journal Name:
Proceedings of the National Academy of Sciences
Volume:
118
Issue:
27
ISSN:
0027-8424
Page Range / eLocation ID:
e2020750118
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. ; ; ; ; ; ; ; ; ; ; et al (, Proceedings of the National Academy of Sciences)
    Electrical resistivity measurements were performed on single crystals of URu2–xOsxSi2up tox= 0.28 under hydrostatic pressure up toP= 2 GPa. As the Os concentration,x, is increased, 1) the lattice expands, creating an effective negative chemical pressurePch(x); 2) the hidden-order (HO) phase is enhanced and the system is driven toward a large-moment antiferromagnetic (LMAFM) phase; and 3) less external pressurePcis required to induce the HO→LMAFM phase transition. We compare the behavior of theT(x,P) phase boundary reported here for the URu2-xOsxSi2system with previous reports of enhanced HO in URu2Si2upon tuning withPor similarly in URu2–xFexSi2upon tuning with positivePch(x). It is noteworthy that pressure, Fe substitution, and Os substitution are the only known perturbations that enhance the HO phase and induce the first-order transition to the LMAFM phase in URu2Si2. We present a scenario in which the application of pressure or the isoelectronic substitution of Fe and Os ions for Ru results in an increase in the hybridization of the U-5f-electron and transition metald-electron states which leads to electronic instability in the paramagnetic phase and the concurrent formation of HO (and LMAFM) in URu2Si2. Calculations in the tight-binding approximation are included to determine the strength of hybridization between the U-5f-electron states and thed-electron states of Ru and its isoelectronic Fe and Os substituents in URu2Si2. 
    more » « less
  2. ; ; ; ; ; ; ; ; ; (, Electronic Structure)
    Abstract Previous high-resolution angle-resolved photoemission (ARPES) studies of URu2Si2have characterized the temperature-dependent behavior of narrow-band states close to the Fermi level (EF) at low photon energies near the zone center, with an emphasis on electronic reconstruction due to Brillouin zone folding. A substantial challenge to a proper description is that these states interact with other hole-band states that are generally absent from bulk-sensitive soft x-ray ARPES measurements. Here we provide a more globalk-space context for the presence of such states and their relation to the bulk Fermi surface (FS) topology using synchrotron-based wide-angle and photon energy-dependent ARPES mapping of the electronic structure using photon energies intermediate between the low-energy regime and the high-energy soft x-ray regime. Small-spot spatial dependence,f-resonant photoemission, Si 2pcore-levels, x-ray polarization, surface-dosing modification, and theoretical surface slab calculations are employed to assist identification of bulk versus surface state character of theEF-crossing bands and their relation to specific U- or Si-terminations of the cleaved surface. The bulk FS topology is critically compared to density functional theory (DFT) and to dynamical mean field theory calculations. In addition to clarifying some aspects of the previously measured high symmetry Γ,ZandXpoints, incommensurate 0.6a* nested Fermi-edge states located alongZ–N–Zare found to be distinctly different from the DFT FS prediction. The temperature evolution of these states aboveTHO, combined with a more detailed theoretical investigation of this region, suggests a key role of theN-point in the hidden order transition. 
    more » « less
  3. ; ; ; ; ; ; ; ; ; ; et al (, Science Advances)
    Novel electronic phenomena frequently form in heavy-fermions because of the mutual localized and itinerant nature of f -electrons. On the magnetically ordered side of the heavy-fermion phase diagram, f -moments are expected to be localized and decoupled from the Fermi surface. It remains ambiguous whether Kondo lattice can develop inside the magnetically ordered phase. Using spectroscopic imaging with scanning tunneling microscope, complemented by neutron scattering, x-ray absorption spectroscopy, and dynamical mean field theory, we probe the electronic states in antiferromagnetic USb 2 . We visualize a large gap in the antiferromagnetic phase within which Kondo hybridization develops below ~80 K. Our calculations indicate the antiferromagnetism and Kondo lattice to reside predominantly on different f -orbitals, promoting orbital selectivity as a new conception into how these phenomena coexist in heavy-fermions. Finally, at 45 K, we find a novel first order–like transition through abrupt emergence of nontrivial 5 f -electronic states that may resemble the “hidden-order” phase of URu 2 Si 2 . 
    more » « less
  4. ; ; ; (, Materials Chemistry Frontiers)
    The design and development of efficient and stable nuclear waste hosts has drawn intensive interest for long-lived lanthanides and actinides. A detailed investigation of their structure and potential structural evolution are crucial. In this study, we have synthesized lanthanum hafnate La 2 Hf 2 O 7 nanoparticles (NPs) doped with uranium at different concentrations (0–10%) and investigated their structural transition. We have discovered that in our La 2 Hf 2 O 7 :U NPs, the uranium dopants are stabilized at both U 4+ and U 6+ oxidation states in which the U 6+ oxidation state exists in octahedral uranate UO 6 6− form. We also confirmed that the U 4+ ions substituted the Hf 4+ ions with a lifetime of ∼1.0 μs and the UO 6 6− ions resided at the La 3+ sites with a lifetime of ∼9.0 μs. More interestingly, the proportion of the U 4+ ions in the La 2 Hf 2 O 7 :U NPs was higher than that of the UO 6 6− ions at low doping level, but at the doping level higher than 2.5%, the fraction of the UO 6 6− ions was greater than that of the U 4+ ions. Furthermore, we studied the structural phase transformation from order pyrochlore to cotunnite of these La 2 Hf 2 O 7 :U NPs with increasing uranium doping level, and found that ordered pyrochlore phase favors the U 4+ ions whereas disordered cotunnite phase favors the UO 6 6− ions. We further used in situ Raman spectroscopy to confirm the reversible cotunnite to pyrochlore phase transformation of the La 2 Hf 2 O 7 :10%U NPs at 900 °C. Therefore, this work demonstrated the successful development of uranium doped La 2 Hf 2 O 7 NPs and thorough characterization of the fundamental spectra of uranium ions, doping induced phase transformation, and structure–optical property correlation. 
    more » « less
  5. ; ; ; ; ; ; ; ; ; ; et al (, Advanced Materials)
    Abstract Since the initial discovery of 2D van der Waals (vdW) materials, significant effort has been made to incorporate the three properties of magnetism, band structure topology, and strong electron correlations—to leverage emergent quantum phenomena and expand their potential applications. However, the discovery of a single vdW material that intrinsically hosts all three ingredients has remained an outstanding challenge. Here, the discovery of a Kondo‐interacting topological antiferromagnet is reported in the vdW 5felectron system UOTe. It has a high antiferromagnetic (AFM) transition temperature of 150 K, with a unique AFM configuration that breaks the combined parity and time reversal (PT) symmetry in an even number of layers while maintaining zero net magnetic moment. This angle‐resolved photoemission spectroscopy (ARPES) measurements reveal Dirac bands near the Fermi level, which combined with the theoretical calculations demonstrate UOTe as an AFM Dirac semimetal. Within the AFM order, the presence of the Kondo interaction is observed, as evidenced by the emergence of a 5fflat band near the Fermi level below 100 K and hybridization between the Kondo band and the Dirac band. The density functional theory calculations in its bilayer form predict UOTe as a rare example of a fully‐compensated AFM Chern insulator. 
    more » « less
  • Citation Formats
  • MLA
  • APA
  • Chicago
  • BibTeX
  • Save / Share this Record
  • Send to Email