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Register a new userWhat is the valence of a correlated solid? The double life of delta-plutonium
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Plutonium displays phase transitions with enormous volume differences among its phases and both its Pauli like magnetic susceptibility and resistivity are an order of magnitude larger than those of simple metals. Curium is also highly resistive but its susceptibility is Curie-like at high temperatures and orders antiferromagnetically at low temperatures. The anomalous properties of the late actinides stem from the competition between the itinerancy and localization of its f electrons, which makes the late actinides elemental strongly correlated materials. A central problem in this field is to understand the mechanism by which these materials resolve these conflicting tendencies. In this letter we identify the electronic mechanisms responsible for the anomalous behaviour of late actinides. We revisit the concept of valence using theoretical approach that treats magnetism, Kondo screening, atomic multiplet effects, spin orbit coupling and crystal field splitting on the same footing. Plutonium is found to be in a rare mixed valent state, namely its ground state is a superposition of two distinct valencies. Curium settles in a single valence magnetically ordered state at low temperatures. The f7 atomic configuration of Curium is contrasted with the multiple configuration manifolds present in Plutonium ground state which we characterize by a valence histogram. The balance between the Kondo screening and magnetism is determined by the competition between spin orbit coupling and the strength of atomic multiplets which is in turn regulated by the degree of itinerancy. The approach presented here, highlights the electronic origin of the bonding anomalies in plutonium and can be applied to predict generalized valences and the presence or absence of magnetism in other compounds starting from first principles.
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Ab-initio relativistic dynamical mean-field theory is applied to resolve the long-standing controversy between theory and experiment in the simple face-centered cubic phase of plutonium called delta-Pu. In agreement with experiment, neither static nor dynamical magnetic moments are predicted. In addition, the quasiparticle density of states reproduces not only the peak close to the Fermi level, which explains the large coefficient of electronic specific heat, but also main 5f features observed in photoelectron spectroscopy.
A central issue in material science is to obtain understanding of the electronic correlations that control complex materials. Such electronic correlations frequently arise due to the competition of localized and itinerant electronic degrees of freedom. While the respective limits of well-localized or entirely itinerant ground states are well-understood, the intermediate regime that controls the functional properties of complex materials continues to challenge theoretical understanding. We have used neutron spectroscopy to investigate plutonium, which is a prototypical material at the brink between bonding and non-bonding configurations. Our study reveals that the ground state of plutonium is governed by valence fluctuations, that is, a quantum-mechanical superposition of localized and itinerant electronic configurations as recently predicted by dynamical mean field theory. Our results not only resolve the long-standing controversy between experiment and theory on plutoniums magnetism, but also suggest an improved understanding of the effects of such electronic dichotomy in complex materials.
We present a theoretical model of the electronic structure of delta-Pu that is consistent with many of the electronic structure related properties of this complex metal. In particular we show that the theory is capable of reproducing the valence band photoelectron spectrum of delta-Pu. We report new experimental photoelectron spectra at several photon energies and present evidence that the electronic structure of delta-Pu is unique among the elements, involving a 5f shell with four 5f electrons in a localized multiplet, hybridizing with valence states, and approximately one 5f electron forming a completely delocalized band state.
Elucidating the phase diagram of lattice gauge theories with fermionic matter in 2+1 dimensions has become a problem of considerable interest in recent years, motivated by physical problems ranging from chiral symmetry breaking in high-energy physics to fractionalized phases of strongly correlated materials in condensed matter physics. For a sufficiently large number $N_f$ of flavors of four-component Dirac fermions, recent sign-problem-free quantum Monte Carlo studies of lattice quantum electrodynamics (QED$_3$) on the square lattice have found evidence for a continuous quantum phase transition between a power-law correlated conformal QED$_3$ phase and a confining valence-bond-solid phase with spontaneously broken point-group symmetries. The critical continuum theory of this transition was shown to be the $O(2)$ QED$_3$-Gross-Neveu model, equivalent to the gauged Nambu-Jona-Lasinio model, and critical exponents were computed to first order in the large-$N_f$ expansion and the $epsilon$ expansion. We extend these studies by computing critical exponents to second order in the large-$N_f$ expansion and to four-loop order in the $epsilon$ expansion below four spacetime dimensions. In the latter context, we also explicitly demonstrate that the discrete $mathbb{Z}_4$ symmetry of the valence-bond-solid order parameter is dynamically enlarged to a continuous $O(2)$ symmetry at criticality for all values of $N_f$.
Some of the most remarkable phenomena---and greatest theoretical challenges---in condensed matter physics arise when $d$ or $f$ electrons are neither fully localized around their host nuclei, nor fully itinerant. This localized/itinerant duality underlies the correlated electronic states of the high-$T_c$ cuprate superconductors and the heavy-fermion intermetallics, and is nowhere more apparent than in the $5f$ valence electrons of plutonium. Here we report the full set of symmetry-resolved elastic moduli of $PuCoGa_5$---the highest $T_c$ superconductor of the heavy fermions ($T_c$=18.5 K)---and find that the bulk modulus softens anomalously over a wide range in temperature above $T_c$. Because the bulk modulus is known to couple strongly to the valence state, we propose that plutonium valence fluctuations drive this elastic softening. This elastic softening is observed to disappear when the superconducting gap opens at $T_c$, suggesting that plutonium valence fluctuations have a strong footprint on the Fermi surface, and that $PuCoGa_5$ avoids a valence-transition by entering the superconducting state. These measurements provide direct evidence of a valence instability in a plutonium compound, and suggest that the unusually high-$T_c$ in this system is driven by valence fluctuations.
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