Inelastic neutron scattering in valence fluctuation compounds

[摘要] The valence fluctuation compounds are rare earth intermetallics where hybridization of the nearly-localized 4f electrons with the conduction electrons leads to incorporation of the 4f's into the itinerant states. This hybridization slows down the conduction electrons and hence gives them a heavy effective mass, justifying application of the term 'heavy Fermion' (HF) to these materials. During the project period, we grew large single crystals of several such compounds and measured their properties using both standard thermodynamic probes and state-of-the-art inelastic neutron scattering. We obtained three main results. For the intermediate valence compounds CePd{sub 3} and YbAl{sub 3}, we showed that the scattering of neutrons by the fluctuations of the 4f magnetic moment does not have the momentum dependence expected for the itinerant heavy mass state; rather, the scattering is more typical of a localized spin fluctuation. We believe that incoherent scattering localizes the excitation. For the heavy Fermion compound Ce(Ni{sub 0.935}Pd{sub 0.065}){sub 2}Ge{sub 2}, which sits at a T = 0 critical point for transformation into an antiferromagnetic (AF) phase, we showed that the scattering from the AF fluctuations does not exhibit any of the divergences that are expected at a phase transition. We speculate that alloy disorder profoundly suppresses the growth of the fluctuating AF regions, leading to short range clusters rather than regions of infinite size. Finally, we explored the applicability of key concepts used to describe the behavior of rare earth heavy Fermions to uranium based HF compounds where the 5f electrons are itinerant as opposed to localized. We found that scaling laws relating the spin fluctuation energy measured in neutron scattering to the low temperature specific heat and susceptibility are valid for the uranium compounds, once corrections are made for AF fluctuations; however, the degeneracy of the high temperature moment is smaller than expected for rare-earth-like Hund's rule behavior, essentially because the orbital moment is suppressed for itinerant 5f electrons. We also found that the standard local-moment-based theory of the temperature dependence of the specific heat, susceptibility and neutron scattering fails badly for URu{sub 2}Zn{sub 20} and UCo{sub 2}Zn{sub 20}, even though the theory is phenomenally successful for the closely related rare earth compound YbFe{sub 2}Zn{sub 20}. Both these results highlight the distinction between the itineracy of the 5f's and the localization of the 4f's. It is our hope that these results are sufficiently significant as to stimulate deeper investigation of these compounds.

[发布日期] 2011-02-15

[学科分类] 材料科学（综合）

[关键词] ALLOYS;EFFECTIVE MASS;ELECTRONS;EXCITATION;FERMIONS;FLUCTUATIONS;HYBRIDIZATION;INCOHERENT SCATTERING;MAGNETIC MOMENTS;MONOCRYSTALS;NEUTRONS;RARE EARTH COMPOUNDS;RARE EARTHS;SCALING LAWS;SCATTERING;SPECIFIC HEAT;SPIN;TEMPERATURE DEPENDENCE;THERMODYNAMICS;URANIUM;URANIUM COMPOUNDS;VALENCE Neutron scattering;heavy Fermion compounds