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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 plutonium's magnetism, but also suggest an improved understanding of the effects of such electronic dichotomy in complex materials., Comment: 29 pages, 2 figures, 2 tables, supplementary materials

We report extensive measurements on a new compound (Yb0.24Sn0.76)Ru that crystallizes in the cubic CsCl structure. Valence band photoemission and L3 x-ray absorption show no divalent component in the 4f configuration of Yb. Inelastic neutron scattering (INS) indicates that the eight-fold degenerate J-multiplet of Yb3+ is split by the crystalline electric field (CEF) into a {\Gamma}7 doublet ground state and a {\Gamma}8 quartet at an excitation energy 20 meV. The magnetic susceptibility can be fit very well by this CEF scheme under the assumption that a {\Gamma}6 excited state resides at 32 meV; however, the {\Gamma}8/{\Gamma}6 transition expected at 12 meV was not observed in the INS. The resistivity follows a Bloch- Gr\"uneisen law shunted by a parallel resistor, as is typical of systems subject to phonon scattering with no apparent magnetic scattering. All of these properties can be understood as representing simple local moment behavior of the trivalent Yb ion. At 1 K, there is a peak in specific heat that is too broad to represent a magnetic phase transition, consistent with absence of magnetic reflections in neutron diffraction. On the other hand, this peak also is too narrow to represent the Kondo effect in the {\Gamma}7 ground state doublet. On the basis of the field-dependence of the specific heat, we argue that antiferromagnetic shortrange order (possibly co-existing with Kondo physics) occurs at low temperatures. The long-range magnetic order is suppressed because the Yb site occupancy is below the percolation threshold for this disordered compound.

Inelastic neutron scattering is applied to study the role of magnetism in stabilizing the charge ordered state in \emph{R}$_{1/3}$Sr$_{2/3}$FeO$_{3}$ (\emph{R}SFO) (\emph{R} = La, Pr, and Nd). The ratio of the ferromagnetic exchange energy (J$_F$) and antiferromagnetic exchange energy (J$_{AF}$), |J$_F$ /J$_{AF}|, is a key indicator of the stability of the charge ordered and antiferromagnetic ordered state. This ratio is obtained from the spin wave spectrum by inelastic neutron scattering and is sufficiently large to suggest that the magnetic exchange energy alone can stabilize the charge ordered state in La$_{1/3}$Sr$_{2/3}$FeO$_{3}$ and Pr$_{1/3}$Sr$_{2/3}$FeO$_{3}$. The exchange ratio decreases from La$_{1/3}$Sr$_{2/3}$FeO$_{3}$ to Nd1$_{1/3}$Sr$_{2/3}$FeO$_{3}$ which indicates a gradual destabilization of the magnetic exchange mechanism for charge ordering in correspondence with the observed reduction in the ordering temperature.

Magnetic susceptibility results for single crystals of the new cubic compounds UT$_2$Al$_{20}$ (T=Mn, V, and Mo) are reported. Magnetization, specific heat, resistivity, and neutron diffraction results for a single crystal and neutron diffraction and inelastic spectra for a powder sample are reported for UMn$_2$Al$_{20}$. For T = V and Mo, temperature independent Pauli paramagnetism is observed. For UMn$_2$Al$_{20}$, a ferromagnetic transition is observed in the magnetic susceptibility at $T_c$ = 20 K. The specific heat anomaly at $T_c$ is very weak while no anomaly in the resistivity is seen at $T_c$. We discuss two possible origins for this behavior of UMn$_2$Al$_{20}$: moderately small moment itinerant ferromagnetism, or induced local moment ferromagnetism., Comment: 5 pages, 5 figures, to be published in Phys. rev. B

The dynamic susceptibility chi"(deltaE), measured by inelastic neutron scattering measurements, shows a broad peak centered at Emax = 16.5 meV for the cubic actinide compound URu2Zn20 and 7 meV at the (1/2, 1/2, 1/2) zone boundary for the rare earth counterpart compound YbFe2Zn20. For URu2Zn20, the low temperature susceptibility and magnetic specific heat coefficient gamma = Cmag/T take the values chi = 0.011 emu/mole and gamma = 190 mJ/mole-K2 at T = 2 K. These values are roughly three times smaller, and Emax is three times larger, than recently reported for the related compound UCo2Zn20, so that chi and gamma scale inversely with the characteristic energy for spin fluctuations, Tsf = Emax/kB. While chi(T), Cmag(T), and Emax of the 4f compound YbFe2Zn20 are very well described by the Kondo impurity model, we show that the model works poorly for URu2Zn20 and UCo2Zn20, suggesting that the scaling behavior of the actinide compounds arises from spin fluctuations of itinerant 5f electrons., Comment: 7 pages, 5 figures

We performed inelastic neutron experiments on underdoped La_2-xSr_xCuO_4(x=0.10, T_c=28.6K) using a time-of-flight neutron scattering technique. Four incommensurate peaks on the two-dimensional reciprocal plane disperse inwards toward an antiferromagnetic zone center as the energy increases. These peaks merge into a single peak at an energy E_cross around w=40+-3meV. Beyond E_cross, the peak starts to broaden and ``hourglass-like'' excitations are observed. The E_cross in the underdoped sample is smaller than that reported for the optimally doped La_1.84Sr_0.16CuO_4. The reduction of the E_cross is explained by the doping-independent slope of the downward dispersion below the E_cross combined with the smaller incommensurability in the underdoped sample. In the energy spectrum of chi"(w), we observed a similar "peak-dip-hump" structure in the energy region of 10~45meV to that reported for the optimally doped sample. We discuss the relation between the hourglass-shaped dispersion and the peak-dip-hump energy spectrum., Comment: 4pages, 3figures. submitted to PRB Rapid Communications. submitted to PRB Rapid Communications

Inelastic neutron scattering experiments show that spin dynamics in the charge ordered insulating ground state of the double-layer perovskite YBaFe2O5 is well described in terms of eg superexchange interactions. Above the Verwey transition at TV = 308 K, t2g double exchange-type conduction within antiferromagnetic FeO2--BaO--FeO2 double layers proceeds by an electron hopping process that requires a spin flip of the five-fold coordinated Fe ions, costing an energy 5S^2 of approximately 0.1 eV. The hopping process disrupts near-neighbor spin correlations, leading to massive damping of zone-boundary spin waves., Comment: RevTeX, 4 pages, 4 figures, submitted to Phys. Rev. Lett

The magnetic exchange energies in charge ordered La_(1/3)Sr_(2/3)FeO_(3-d) (LSFO) and its parent compound LaFeO_(3) (LFO) have been determined by inelastic neutron scattering. In LSFO, the measured ratio of ferromagnetic exchange between Fe3+ - Fe5+ pairs (J_F) and antiferromagnetic exchange between Fe3+ - Fe3+ pairs (J_AF) fulfills the criterion for charge ordering driven by magnetic interactions (|J_F/J_AF| > 1). The 30% reduction of J_AF as compared to LFO indicates that doped holes are delocalized, and charge ordering occurs without a dominant influence from Coulomb interactions., Comment: 18 pages, 4 color figures

The intermediate valence compounds Yb2M3Ga9 (M = Rh, Ir) exhibit an anisotropic magnetic susceptibility. We report measurements of the temperature dependence of the 4f occupation number, nf(T), for Yb2M3Ga9 as well as the magnetic inelastic neutron scattering spectrum Smag at 12 and 300 K for Yb2Rh3Ga9. Both nf(T) and Smag were calculated for the Anderson impurity model with crystal field terms within an approach based on the non-crossing approximation. These results corroborate the importance of crystal field effects in these materials; they also suggest that Anderson lattice effects are important to the physics of Yb2M3Ga9., Comment: 17 pages, 3 figures, submitted to Phys. Rev. B

We have measured the crystalline electric field (CEF) excitations of the CeMIn5 (M = Co, Rh, Ir) series of heavy fermion superconductors by means of inelastic neutron scattering. Fits to a CEF model reproduce the inelastic neutron scattering spectra and the high temperature magnetic susceptibility. The CEF parameters, energy level splittings, and wavefunctions are tabulated for each member of the CeMIn5 series and compared to each other as well as to the results of previous measurements. Our results indicate that the CEF level splitting in all three materials is similar, and can be thought of as being derived from the cubic parent compound CeIn3 in which an excited state quartet at ~12 meV is split into two doublets by the lower symmetry of the tetragonal environment of the CeMIn5 materials. In each case, the CEF excitations are observed as broad lines in the inelastic neutron scattering spectrum. We attribute this broadening to Kondo hybridization of the localized f moments with the conduction electrons. The evolution of the superconducting transition temperatures in the different members of CeMIn5 can then be understood as a direct consequence of the strength of this hybridization. Due to the importance of Kondo spin fluctuations in these materials, we also present calculations within the non-crossing approximation (NCA) to the Anderson impurity model including the effect of CEF level splitting for the inelastic neutron scattering spectra and the magnetic susceptibility., Comment: 30 pages, 6 figures, submitted to Phys. Rev. B

In this work, we study crystalline electric field effects in the heavy fermion superconductor CeIrIn5. We observe two regions of broad magnetic response in the inelastic neutron scattering spectra at 10 K. The first corresponds to the transition between the gamma7 groundstate doublet and the first excited state doublet at 4 meV interwoven with a broad quasielastic contribution. The second region corresponds to the transition between the ground state and the second excited state doublet at 28 meV. The large Lorentzian half-widths of the peaks (~10 meV) calls into question calculations for the specific heat and magnetic susceptibility that assume sharp crystal field levels. Consequently, we have calculated the inelastic neutron scattering spectra and magnetic susceptibility using the Anderson impurity model within the non-crossing approximation (NCA) including the effects of crystal field level splitting., Comment: submitted to J. Neutron Research

The crystalline electric field (CEF) energy level scheme of the heavy fermion superconductor CeCoIn_5 has been determined by means of inelastic neutron scattering (INS). Peaks observed in the INS spectra at 8 meV and 27 meV with incident neutron energies between E_i=30-60 meV and at a temperature T = 10 K correspond to transitions from the ground state to the two excited states, respectively. The wavevector and temperature dependence of these peaks are consistent with CEF excitations. Fits of the data to a CEF model yield the CEF parameters B^0_2=-0.80 meV, B^0_4=0.059 meV, and |B^4_4|= 0.137 meV corresponding to an energy level scheme: Gamma_7^(1) (0)[=0.487|+/-5/2> - 0.873|-/+3/2>], Gamma_7^(2) (8.6 meV, 100 K), and Gamma_6 (24.4 meV, 283 K)., Comment: uses latex packages revtex4,amsmath,graphicx,natbib, 9th Annual MMM-Intermag Conference, (Accepted for publication in J. Appl. Phys.) 7 pages, 2 figures

We report zero-field inelastic neutron scattering experiments on a deuterated powder sample of Mn12-Acetate consisting of a large number of nominally identical spin-10 magnetic clusters. Our resolution enables us to see a series of peaks corresponding to transitions between the anisotropy levels within the spin-10 manifold. A fit to the spin Hamiltonian yields an anisotropy constant D=0.54 K and a fourth-order diagonal anisotropy coefficient A = 1.2x10^-3 K. Performed in the absence of a magnetic field, our experiments do not involve the g-values as fitting parameters, thereby yielding particularly reliable values of D and A., Comment: Submission to Conference on Magnetism and Magnetic Materials. Will appear in proceedings of the conference published in JAP in April 1999

Cu_{2}(1,4-diazacycloheptane)_{2}Cl_{4} contains double chains of spin 1/2 Cu^{2+} ions. We report ac susceptibility, specific heat, and inelastic neutron scattering measurements on this material. The magnetic susceptibility, $\chi(T)$, shows a rounded maximum at T = 8 K indicative of a low dimensional antiferromagnet with no zero field magnetic phase transition. We compare the $\chi(T)$ data to exact diagonalization results for various one dimensional spin Hamiltonians and find excellent agreement for a spin ladder with intra-rung coupling $J_1 = 1.143(3)$ meV and two mutually frustrating inter-rung interactions: $J_2 = 0.21(3)$ meV and $J_3 = 0.09(5)$ meV. The specific heat in zero field is exponentially activated with an activation energy $\Delta = 0.89(1)$ meV. A spin gap is also found through inelastic neutron scattering on powder samples which identify a band of magnetic excitations for $0.8 < \hbar\omega < 1.5$ meV. Using sum-rules we derive an expression for the dynamic spin correlation function associated with non-interacting propagating triplets in a spin ladder. The van-Hove singularities of such a model are not observed in our scattering data indicating that magnetic excitations in Cu_{2}(1,4-diazacycloheptane)_{2}Cl_{4} are more complicated. For magnetic fields above $H_{c1} \simeq 7.2$ T specific heat data versus temperature show anomalies indicating a phase transition to an ordered state below T = 1 K., Comment: 9 pages, 8 postscript figures, LaTeX, Submitted to PRB 8/4/97, e-mail Comments to dhr@pha.jhu.edu