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Register a new userOrbital-selective Kondo entanglement and antiferromagnetic order in USb$_2$
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In heavy-fermion compounds, the dual character of $f$ electrons underlies their rich and often exotic properties like fragile heavy quasipartilces, variety of magnetic orders and unconventional superconductivity. 5$f$-electron actinide materials provide a rich setting to elucidate the larger and outstanding issue of the competition between magnetic order and Kondo entanglement and, more generally, the interplay among different channels of interactions in correlated electron systems. Here, by using angle-resolved photoemission spectroscopy, we present detailed electronic structure of USb$_2$ and observed two different kinds of nearly flat bands in the antiferromagnetic state of USb$_2$. Polarization-dependent measurements show that these electronic states are derived from 5$f$ orbitals with different characters; in addition, further temperature-dependent measurements reveal that one of them is driven by the Kondo correlations between the 5$f$ electrons and conduction electrons, while the other reflects the dominant role of the magnetic order. Our results on the low-energy electronic excitations of USb$_2$ implicate orbital selectivity as an important new ingredient for the competition between Kondo correlations and magnetic order and, by extension, in the rich landscape of quantum phases for strongly correlated $f$ electron systems.
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Novel electronic phenomena frequently form in heavy fermions as a consequence of the mutual nature of localization and itineracy 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 a Kondo lattice can develop inside the magnetically ordered phase. Using spectroscopic imaging with the scanning tunneling microscope, complemented by neutron scattering, x ray absorption spectroscopy, and dynamical mean field theory, we probe the electronic states in the antiferromagnetic USb2 as a function of temperature. We visualize a large gap in the antiferromagnetic phase at high temperatures, T lower than TN 200 K, within which Kondo hybridization gradually develops below Tcoh 80 K. Our dynamical mean field theory calculations indicate the antiferromagnetism and Kondo lattice to reside predominantly on different f orbitals, promoting orbital selectivity as a new conception into how these two phenomena coexist in heavy fermions. Finally, at Tstar 45 K we discover a novel 1st order like electronic transition through the abrupt emergence of non trivial 5f electronic states that may share some resemblance to the hidden order phase of URu2Si2.
We have performed pressure dependent X-ray diffraction and resonant X-ray emission spectroscopy experiments on USb$_2$ to further characterize the AFM-FM transition occurring near 8 GPa. We have found the magnetic transition coincides with a tetragonal to orthorhombic transition resulting in a 17% volume collapse as well as a transient $textit{f}$-occupation enhancement. Compared to UAs$_2$ and UAsS, USb$_2$ shows a reduced bulk modulus and transition pressure and an increased volume collapse at the structural transition. Except for an enhancement across the transition region, the $textit{f}$-occupancy decreases steadily from 1.96 to 1.75.
Electronic localization-delocalization has played a prominent role in realizing beyond-Landau metallic quantum critical points. It typically involves local spins induced by strong correlations. Systems that contain local multipolar moments offer new platforms to explore such quantum criticality. Here, we use an analytical method at zero temperature to study the fate of an SU(4) spin-orbital Kondo state in a multipolar Bose-Fermi Kondo model, which provides an effective description of a multipolar Kondo lattice. We show that a generic trajectory in the parameter space contains two quantum critical points, which are associated with the destruction of the Kondo entanglement in the orbital and spin channels respectively. Our asymptotically exact results reveal a global phase diagram, provides the theoretical basis for the notion of sequential Kondo destruction, and point to new forms of quantum criticality that may still be realized in a variety of strongly correlated metals.
Neutron diffraction and magnetic susceptibility studies of a polycrystalline SrCr$_2$As$_2$ sample reveal that this compound is an itinerant G-type antiferromagnet below the N${rm acute{e}}$el temperature $T_{textrm N}$ = 590(5) K with the Cr magnetic moments aligned along the tetragonal $c$ axis. The system remains tetragonal to the lowest measured temperature ($sim$12 K). The lattice parameter ratio $c/a$ and the magnetic moment saturate at about the same temperature below $sim$ 200 K, indicating a possible magnetoelastic coupling. The ordered moment, $mu=1.9(1)~mu_{rm B}$/Cr, measured at $T = 12$ K, is significantly reduced compared to its localized value ($4~mu_{rm B}$/Cr) due to the itinerant character brought about by the hybridization between the Cr $3d$ and As $4p$ orbitals.
Using {it ab initio} density functional theory, here we systematically study the monolayer MoOCl$_2$ with a $4d^2$ electronic configuration. Our main results is that an orbital-selective Peierls phase (OSPP) develops in MoOCl$_2$, resulting in the dimerization of the Mo chain along the $b$-axis. Specifically, the Mo-$d_{xy}$ orbitals form robust molecular-orbital states inducing localized $d_{xy}$ singlet dimers, while the Mo-$d_{xz/yz}$ orbitals remain delocalized and itinerant. Our study shows that MoOCl$_2$ is globally metallic, with the Mo-$d_{xy}$ orbital bonding-antibonding splittings opening a gap and the Mo-$d_{xz/yz}$ orbitals contributing to the metallic conductivity. Overall, the results resemble the recently much discussed orbital-selective Mott phase but with the localized band induced by a Peierls distortion instead of Hubbard interactions. Finally, we also qualitatively discuss the possibility of OSPP in the $3d^2$ configuration, as in CrOCl$_2$.
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