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  1. Delocalized−localized electron interactions are central to strongly correlated electron phenomena. Here, we study the Kondo effect, a prototypical strongly correlated phenomena, in a tunable fashion using gold nanostructures (nanoparticle, NP, and nanoshell, NS) + molecule cross-linkers (butanedithiol, BDT). NP films exhibit hallmark signatures of the Kondo effect, including (1) a log temperature resistance upturn as temperature decreases in a metallic regime, and (2) zero-bias conductance peaks (ZBCPs) that are well fit by a Frota function near a percolation insulator transition, previously used to model Kondo peaks observed using tunnel junctions. Remarkably, NP + NS films exhibit ZBCPs that persist to >220 K, i.e., >10-fold higher than that in NP films. Magnetic measurements reveal that moments in NP powders align, and in NS powders, they antialign at low temperatures. Based on these observations, we propose a mechanism in which varying such material nanobuilding blocks can modify electron−electron interactions to such a large degree.
    Free, publicly-accessible full text available January 1, 2024
  2. Free, publicly-accessible full text available December 1, 2023
  3. Free, publicly-accessible full text available February 28, 2024
  4. Chemical/structural maps provide guidance for discovery of exotic quantum states in f -electron intermetallics.
    Free, publicly-accessible full text available August 12, 2023
  5. Free, publicly-accessible full text available September 1, 2023
  6. Abstract

    The crystal structure, electron energy-loss spectroscopy (EELS), heat capacity, and anisotropic magnetic and resistivity measurements are reported for Sn flux grown single crystals of orthorhombic Pr2Co3Ge5(U2Co3Si5-type,Ibam). Our findings show thato-Pr2Co3Ge5hosts nearly trivalent Pr ions, as evidenced by EELS and fits to temperature dependent magnetic susceptibility measurements. Complex magnetic ordering with a partially spin-polarized state emerges nearTsp= 32 K, with a spin reconfiguration transition nearTM= 15 K. Heat capacity measurements show that the phase transitions appear as broad peaks in the vicinity ofTspandTM. The magnetic entropy further reveals that crystal electric field splitting lifts the Hund’s rule degeneracy at low temperatures. Taken together, these measurements show that Pr2Co3Ge5is an environment for complexfstate magnetism with potential strongly correlated electron states.

  7. Free, publicly-accessible full text available November 22, 2023
  8. 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 ofmore »Ru and its isoelectronic Fe and Os substituents in URu2Si2.

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