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Register a new userElectronic Landscape of Ce-based Intermetallics: CeCu$_2$Si$_2$ at an Extreme
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CeCu$_2$Si$_2$ is an exemplary correlated electron metal that features two domes of unconventional superconductivity in its temperature-pressure phase diagram. The first dome surrounds an antiferromagnetic quantum critical point, whereas the more exotic second dome may span the termination point of a line of $f$-electron valence transitions. This behavior has received intense interest, but what has been missing are ways to access the high pressure behavior under milder conditions. Here we study Si $rightarrow$ P chemical substitution, which compresses the unit cell volume but simultaneously weakens the hybridization between the $f$- and conduction electron states and encourages complex magnetism. At concentrations that show magnetism, applied pressure suppresses the magnetic ordering temperature and superconductivity is recovered for samples with low disorder. These results reveal that the electronic behavior in this system is controlled by a nontrivial combination of effects from unit cell volume and electronic shell filling. Guided by this topography we discuss prospects for uncovering a valence fluctuation quantum phase transition in the broader family of Ce-based ThCr$_2$Si$_2$-type materials through chemical substitution.
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The crystal-field ground state wave function of CeCu$_2$Si$_2$ has been investigated with linear polarized $M$-edge x-ray absorption spectroscopy from 250mK to 250K, thus covering the superconducting ($T_{text{c}}$=0.6K), the Kondo ($T_{text{K}}$$approx$20K) as well as the Curie-Weiss regime. The comparison with full-multiplet calculations shows that the temperature dependence of the experimental linear dichroism is well explained with a $Gamma_7^{(1)}$ crystal-field ground-state and the thermal population of excited states at around 30meV. The crystal-field scheme does not change throughout the entire temperature range thus making the scenario of orbital switching unlikely. Spectroscopic evidence for the presence of the Ce 4$f^0$ configuration in the ground state is consistent with the possibility for a multi-orbital character of the ground state. We estimate from the Kondo temperature and crystal-field splitting energies that several percents of the higher lying $Gamma_6$ state and $Gamma_7^{(2)}$ crystal-field states are mixed into the primarily $Gamma_7^{(1)}$ ground state. This estimate is also supported by re-normalized band-structure calculations that uses the experimentally determined crystal-field scheme.
In this paper the low-temperature properties of two isostructural canonical heavy-fermion compounds are contrasted with regards to the interplay between antiferromagnetic (AF) quantum criticality and superconductivity. For CeCu$_2$Si$_2$, fully-gapped d-wave superconductivity forms in the vicinity of an itinerant three-dimensional heavy-fermion spin-density-wave (SDW) quantum critical point (QCP). Inelastic neutron scattering results highlight that both quantum critical SDW fluctuations as well as Mott-type fluctuations of local magnetic moments contribute to the formation of Cooper pairs in CeCu$_2$Si$_2$. In YbRh$_2$Si$_2$, superconductivity appears to be suppressed at $Tgtrsim~10$ mK by AF order ($T_N$ = 70 mK). Ultra-low temperature measurements reveal a hybrid order between nuclear and 4f-electronic spins, which is dominated by the Yb-derived nuclear spins, to develop at $T_A$ slightly above 2 mK. The hybrid order turns out to strongly compete with the primary 4f-electronic order and to push the material towards its QCP. Apparently, this paves the way for heavy-fermion superconductivity to form at $T_c$ = 2 mK. Like the pressure - induced QCP in CeRhIn$_5$, the magnetic field - induced one in YbRh$_2$Si$_2$ is of the local Kondo-destroying variety which corresponds to a Mott-type transition at zero temperature. Therefore, these materials form the link between the large family of about fifty low-$T$ unconventional heavy - fermion superconductors and other families of unconventional superconductors with higher $T_c$s, notably the doped Mott insulators of the cuprates, organic charge-transfer salts and some of the Fe-based superconductors. Our study suggests that heavy-fermion superconductivity near an AF QCP is a robust phenomenon.
The application of pressure as well as the successive substitution of Ru with Fe in the hidden order (HO) compound URu$_2$Si$_2$ leads to the formation of the large moment antiferromagnetic phase (LMAFM). Here we have investigated the substitution series URu$_{2-x}$Fe$_x$Si$_2$ with $x$ = 0.2 and 0.3 with non-resonant inelastic x-ray scattering (NIXS) and 4$f$ core-level photoelectron spectroscopy with hard x-rays (HAXPES). NIXS shows that the substitution of Fe has no impact on the symmetry of the ground-state wave function. In HAXPES we find no shift of spectral weight that would be indicative for a change of the 5$f$-electron count. Consequently, changes in the exchange interaction $cal{J}$ due to substitution must be minor so that the conjecture of chemical pressure seems unlikely. An alternative scenario is discussed, namely the formation of long range magnetic order due the substitution induced local enhancement of the magnetization in the vicinity of the $f$-electron ions while the overall electronic structure remains unchanged.
Quantum materials are epitomized by the influence of collective modes upon their macroscopic properties. Relatively few examples exist, however, whereby coherence of the ground-state wavefunction directly contributes to the conductivity. Notable examples include the quantizing effects of high magnetic fields upon the 2D electron gas, the collective sliding of charge density waves subject to high electric fields, and perhaps most notably the macroscopic phase coherence that enables superconductors to carry dissipationless currents. Here we reveal that the low temperature hidden order state of URu$_2$Si$_2$ exhibits just such a connection between the quantum and macroscopic worlds -- under large voltage bias we observe non-linear contributions to the conductivity that are directly analogous to the manifestation of phase slips in one-dimensional superconductors [1], suggesting a complex order parameter for hidden order
We present time-domain THz spectroscopy data of a thin film of the Kondo-lattice antiferromagnet CeCu$_2$Ge$_2$. The low frequency complex conductivity has been obtained down to temperatures below the onset of magnetic order. At low temperatures a narrow Drude-like peak forms, which is similar to ones found in other heavy fermion compounds that do not exhibit magnetic order. Using this data in conjunction with DC resistivity measurements, we obtain the frequency dependence of the scattering rate and effective mass through an extended Drude model analysis. The zero frequency limit of this analysis yields evidence for large mass renormalization even in the magnetic state, the scale of which agrees closely with that obtained from thermodynamic measurements.
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