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Chemical/structural maps provide guidance for discovery of exotic quantum states in f -electron intermetallics.

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 nearT_sp= 32 K, with a spin reconfiguration transition nearT_M= 15 K. Heat capacity measurements show that the phase transitions appear as broad peaks in the vicinity ofT_spandT_M. 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.

Electrical resistivity measurements were performed on single crystals of URu_2–xOs_xSi₂up 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 pressureP_ch(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 pressureP_cis required to induce the HO→LMAFM phase transition. We compare the behavior of theT(x,P) phase boundary reported here for the URu_2-xOs_xSi₂system with previous reports of enhanced HO in URu₂Si₂upon tuning withPor similarly in URu_2–xFe_xSi₂upon tuning with positiveP_ch(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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The synthesis, electronic structure and temperature dependent transport properties of polycrystalline Cu 1+x Mn 2−x InTe 4 ( x = 0, 0.2, 0.3) are reported for the first time. These quaternary chalcogenides were synthesized by direct reaction of the elements, followed by solid state annealing and hot press densification. The thermal conductivity is low for all specimens and intrinsic to the material system. Furthermore, the off-stoichiometry specimens illustrate the sensitivity of the transport properties to stoichiometry, with a greater than two-orders-of magnitude increase in carrier concentration with increased Cu content. First principles calculations of the electronic structure are also reported, and are in agreement with the experimental data. This fundamental investigation shows the potential towards further optimization of the electrical properties that, in addition to the intrinsically low thermal conductivity, provides a basis for further research into the viability of this material system for potential energy-related applications.