Correlations and incipient antiferromagnetic order within the linear Mn chains of metallic Ti4MnBi2.

We report measurements on Ti4MnBi2, where a crystal structure involving linear chains of Mn ions suggests one-dimensional magnetic character. The electrical resistivity is metallic, consistent with the results of electronic-structure calculations that find a robust Fermi surface albeit with moderate electronic correlations. A Curie-Weiss fit to the magnetic susceptibility suggests that the Mn moments are in the low-spin S = 1/2 configuration. Neutron diffraction measurements detect weak antiferromagnetic order within the Mn chains, with further evidence for the small staggered moment coming from the entropy associated with the ordering peak in the specific heat as well as from the results of spin-polarized electronic-structure calculations. The antiferromagnetic moments are apparently associated with the d x 2 - y 2 and d xy orbitals of Mn while the remaining Mn orbitals are delocalized and nonmagnetic. Strong quantum fluctuations, possibly related to an electronic instability that forms the Mn moment or to the one-dimensional character of Ti4MnBi2, nearly overcome magnetic order.

Spinon confinement and a sharp longitudinal mode in Yb2Pt2Pb in magnetic fields.

The fundamental excitations in an antiferromagnetic chain of spins-1/2 are spinons, de-confined fractional quasiparticles that when combined in pairs, form a triplet excitation continuum. In an Ising-like spin chain the continuum is gapped and the ground state is Néel ordered. Here, we report high resolution neutron scattering experiments, which reveal how a magnetic field closes this gap and drives the spin chains in Yb2Pt2Pb to a critical, disordered Luttinger-liquid state. In Yb2Pt2Pb the effective spins-1/2 describe the dynamics of large, Ising-like Yb magnetic moments, ensuring that the measured excitations are exclusively longitudinal, which we find to be well described by time-dependent density matrix renormalization group calculations. The inter-chain coupling leads to the confinement of spinons, a condensed matter analog of quark confinement in quantum chromodynamics. Insensitive to transverse fluctuations, our measurements show how a gapless, dispersive longitudinal mode arises from confinement and evolves with magnetic order.

Local quantum phase transition in YFe2Al10.

A phase transition occurs when correlated regions of a new phase grow to span the system and the fluctuations within the correlated regions become long lived. Here, we present neutron scattering measurements showing that this conventional picture must be replaced in YFe2Al10, a compound that forms naturally very close to a [Formula: see text] quantum phase transition. Fully quantum mechanical fluctuations of localized moments are found to diverge at low energies and temperatures; however, the fluctuating moments are entirely without spatial correlations. Zero temperature order in YFe2Al10 is achieved by an entirely local type of quantum phase transition that may originate with the creation of the moments themselves.

Reduction of Raman scattering and fluorescence from anvils in high pressure Raman scattering.

We describe a new design and use of a high pressure anvil cell that significantly reduces the Raman scattering and fluorescence from the anvils in high pressure Raman scattering experiments. The approach is particularly useful in Raman scattering studies of opaque, weakly scattering samples. The effectiveness of the technique is illustrated with measurements of two-magnon Raman scattering in La2CuO4.

Orbital-exchange and fractional quantum number excitations in an f-electron metal, Yb2Pt2Pb.

Exotic quantum states and fractionalized magnetic excitations, such as spinons in one-dimensional chains, are generally expected to occur in 3d transition metal systems with spin 1/2. Our neutron-scattering experiments on the 4f-electron metal Yb2Pt2Pb overturn this conventional wisdom. We observe broad magnetic continuum dispersing in only one direction, which indicates that the underlying elementary excitations are spinons carrying fractional spin-1/2. These spinons are the emergent quantum dynamics of the anisotropic, orbital-dominated Yb moments. Owing to their unusual origin, only longitudinal spin fluctuations are measurable, whereas the transverse excitations such as spin waves are virtually invisible to magnetic neutron scattering. The proliferation of these orbital spinons strips the electrons of their orbital identity, resulting in charge-orbital separation.

An itinerant antiferromagnetic metal without magnetic constituents.

The origin of magnetism in metals has been traditionally discussed in two diametrically opposite limits: itinerant and local moments. Surprisingly, there are very few known examples of materials that are close to the itinerant limit, and their properties are not universally understood. In the case of the two such examples discovered several decades ago, the itinerant ferromagnets ZrZn2 and Sc3In, the understanding of their magnetic ground states draws on the existence of 3d electrons subject to strong spin fluctuations. Similarly, in Cr, an elemental itinerant antiferromagnet with a spin density wave ground state, its 3d electron character has been deemed crucial to it being magnetic. Here, we report evidence for an itinerant antiferromagnetic metal with no magnetic constituents: TiAu. Antiferromagnetic order occurs below a Néel temperature of 36 K, about an order of magnitude smaller than in Cr, rendering the spin fluctuations in TiAu more important at low temperatures. This itinerant antiferromagnet challenges the currently limited understanding of weak itinerant antiferromagnetism, while providing insights into the effects of spin fluctuations in itinerant-electron systems.

Protected Fe valence in quasi-two-dimensional α-FeSi2.

We report the first comprehensive study of the high temperature form (α-phase) of iron disilicide. Measurements of the magnetic susceptibility, magnetization, heat capacity and resistivity were performed on well characterized single crystals. With a nominal iron d(6) configuration and a quasi-two-dimensional crystal structure that strongly resembles that of LiFeAs, α-FeSi2 is a potential candidate for unconventional superconductivity. Akin to LiFeAs, α-FeSi2 does not develop any magnetic order and we confirm its metallic state down to the lowest temperatures (T = 1.8 K). However, our experiments reveal that paramagnetism and electronic correlation effects in α-FeSi2 are considerably weaker than in the pnictides. Band theory calculations yield small Sommerfeld coefficients of the electronic specific heat γ = Ce/T that are in excellent agreement with experiment. Additionally, realistic many-body calculations further corroborate that quasi-particle mass enhancements are only modest in α-FeSi2. Remarkably, we find that the natural tendency to vacancy formation in the iron sublattice has little influence on the iron valence and the density of states at the Fermi level. Moreover, Mn doping does not significantly change the electronic state of the Fe ion. This suggests that the iron valence is protected against hole doping and indeed the substitution of Co for Fe causes a rigid-band like response of the electronic properties. As a key difference from the pnictides, we identify the smaller inter-iron layer spacing, which causes the active orbitals near the Fermi level to be of a different symmetry in α-FeSi2. This change in orbital character might be responsible for the lack of superconductivity in this system, providing constraints on pairing theories in the iron based pnictides and chalcogenides.

Quantum critical fluctuations in layered YFe2Al10.

The absence of thermal fluctuations at T = 0 makes it possible to observe the inherently quantum mechanical nature of systems where the competition among correlations leads to different types of collective ground states. Our high precision measurements of the magnetic susceptibility, specific heat, and electrical resistivity in the layered compound YFe2Al10 demonstrate robust field-temperature scaling, evidence that this system is naturally poised without tuning on the verge of ferromagnetic order that occurs exactly at T = 0, where magnetic fields drive the system away from this quantum critical point and restore normal metallic behavior.

Size-dependent vibronic coupling in α-Fe2O3.

We report the discovery of finite length scale effects on vibronic coupling in nanoscale α-Fe2O3 as measured by the behavior of vibronically activated d-d on-site excitations of Fe(3+) as a function of size and shape. An oscillator strength analysis reveals that the frequency of the coupled symmetry-breaking phonon changes with size, a crossover that we analyze in terms of increasing three-dimensional character to the displacement pattern. These findings demonstrate the flexibility of mixing processes in confined systems and suggest a strategy for both enhancing and controlling charge-lattice interactions in other materials.

Intrinsic nanostructure in Zr2-xFe4Si16-y(x = 0.81, y = 6.06).

We present a study of the crystal structure and physical properties of single crystals of a new Fe-based ternary compound, Zr2-xFe4Si16-y(x = 0.81, y = 6.06). Zr1.19Fe4Si9.94 is a layered compound, where stoichiometric ß-FeSi2-derived slabs are separated by Zr-Si planes with substantial numbers of vacancies. High resolution transmission electron microscopy (HRTEM) experiments show that these Zr-Si layers consist of 3.5 nm domains where the Zr and Si vacancies are ordered within a supercell sixteen times the volume of the stoichiometric cell. Within these domains, the occupancies of the Zr and Si sites obey symmetry rules that permit only certain compositions, none of which by themselves reproduce the average composition found in x-ray diffraction experiments. Magnetic susceptibility and magnetization measurements reveal a small but appreciable number of magnetic moments that remain freely fluctuating to 1.8 K, while neutron diffraction confirms the absence of bulk magnetic order with a moment of 0.2µB or larger down to 1.5 K. Electrical resistivity measurements find that Zr1.19Fe4Si9.94 is metallic, and the modest value of the Sommerfeld coefficient of the specific heat γ = C/T suggests that quasi-particle masses are not particularly strongly enhanced. The onset of superconductivity at Tc ≃ 6 K results in a partial resistive transition and a small Meissner signal, although a bulk-like transition is found in the specific heat. Sharp peaks in the ac susceptibility signal the interplay of the normal skin depth and the London penetration depth, typical of a system in which nano-sized superconducting grains are separated by a non-superconducting host. Ultra low field differential magnetic susceptibility measurements reveal the presence of a surprisingly large number of trace magnetic and superconducting phases, suggesting that the Zr-Fe-Si ternary system could be a potentially rich source of new bulk superconductors.

Spin liquids and antiferromagnetic order in the Shastry-Sutherland-lattice compound Yb2Pt2Pb.

We present measurements of the magnetic susceptibility χ and the magnetization M of single crystals of metallic Yb(2)Pt(2)Pb, where localized Yb moments lie on the dimerized and frustrated Shastry-Sutherland lattice (SSL). Strong magnetic frustration is found in this quasi-two-dimensional system, which orders antiferromagnetically at T(N) = 2.02 K from a paramagnetic liquid of Yb dimers, having a gap Δ = 4.6 K between the singlet ground state and the triplet excited states. Magnetic fields suppress the antiferromagnetic (AF) order, which vanishes at a 1.23 T quantum critical point. The spin gap Δ persists to 1.5 T, indicating that dimer singlets survive the collapse of the B = 0 AF state. Quantized steps are observed in M(B) within the AF state, a signature of SSL systems. Our results show that Yb(2) Pt(2)Pb is unique, both as a metallic SSL system that is close to an AF quantum critical point, and as a heavy fermion compound where quantum frustration plays a decisive role.

From antiferromagnetic insulator to correlated metal in pressurized and doped LaMnPO.

Widespread adoption of superconducting technologies awaits the discovery of new materials with enhanced properties, especially higher superconducting transition temperatures T(c). The unexpected discovery of high T(c) superconductivity in cuprates suggests that the highest T(c)s occur when pressure or doping transform the localized and moment-bearing electrons in antiferromagnetic insulators into itinerant carriers in a metal, where magnetism is preserved in the form of strong correlations. The absence of this transition in Fe-based superconductors may limit their T(c)s, but even larger T(c)s may be possible in their isostructural Mn analogs, which are antiferromagnetic insulators like the cuprates. It is generally believed that prohibitively large pressures would be required to suppress the effects of the strong Hund's rule coupling in these Mn-based compounds, collapsing the insulating gap and enabling superconductivity. Indeed, no Mn-based compounds are known to be superconductors. The electronic structure calculations and X-ray diffraction measurements presented here challenge these long held beliefs, finding that only modest pressures are required to transform LaMnPO, isostructural to superconducting host LaFeAsO, from an antiferromagnetic insulator to a metallic antiferromagnet, where the Mn moment vanishes in a second pressure-driven transition. Proximity to these charge and moment delocalization transitions in LaMnPO results in a highly correlated metallic state, the familiar breeding ground of superconductivity.

Heavy fermion compounds on the geometrically frustrated Shastry-Sutherland lattice.

We present measurements of the basic properties of Ce(2)Ge(2)Mg, Yb(2)Pt(2)Pb and Ce(2)Pt(2)Pb, which are members of a new class of geometrically frustrated magnets R(2)T(2)X (R = rare earth, T = transition metal, X = main group). Here, the moment-bearing R atoms are confined to layers where they are arranged in the Shastry-Sutherland lattice. Magnetic susceptibility and specific heat measurements indicate that Ce(2)Ge(2)Mg orders antiferromagnetically at 9.4 K and Yb(2)Pt(2)Pb at 2.07 K. No long ranged order is observed in Ce(2)Pt(2)Pb above 0.05 K. Analysis of Schottky peaks in the specific heat indicates that all three compounds have doublet ground states that are well separated in energy from the excited states of the crystal-field-split manifold. Electrical resistivity measurements show that Ce(2)Ge(2)Mg and Yb(2)Pt(2)Pb are excellent metals with small residual resistivities. However, the measured resistivity of Ce(2)Pt(2)Pb is large and almost temperature-independent, suggesting that strong disorder or perhaps strong quantum critical fluctuations saturate the quasiparticle scattering in this compound. The magnetic entropy develops very slowly above the onset of antiferromagnetic order and we discuss the possibility that a nonordered fluid of dimerized moments exists above T(N) in Ce(2)Ge(2)Mg and Yb(2)Pt(2)Pb, and for a wide range of temperatures in Ce(2)Pt(2)Pb, which appears to be close to a frustration-driven quantum critical point.

Magnetic transition and spin fluctuations in the unconventional antiferromagnetic compound Yb3Pt4.

Muon spin rotation and relaxation measurements have been carried out on the unconventional antiferromagnet Yb3Pt4. Oscillations are observed below T(N) = 2.22(1) K, consistent with the antiferromagnetic (AFM) Néel temperature observed in bulk experiments. In agreement with neutron diffraction experiments the oscillation frequency ω(µ)(T)/2π follows an S = 1/2 mean-field temperature dependence, yielding a quasistatic local field of 1.71(2) kOe at T = 0. A crude estimate gives an ordered moment of ∼ 0.66 µ(B) at T = 0, comparable to 0.81 µ(B) from neutron diffraction. As T-->T(N) from above the dynamic relaxation rate λ(d) exhibits no critical slowing down, consistent with a mean-field transition. In the AFM phase a T-linear fit to λ(d)(T), appropriate to a Fermi liquid, yields highly enhanced values of λ(d)/T and the Korringa constant K(µ)(2)T/λ(d), with K(µ) the estimated muon Knight shift. A strong suppression of λ(d) by applied field is observed in the AFM phase. These properties are consistent with the observed large Sommerfeld-Wilson and Kadowaki-Woods ratios in Yb3Pt4 (although the data do not discriminate between Fermi-liquid and non-Fermi-liquid states), and suggest strong enhancement of q≈0 spin correlations between large-Fermi-volume band quasiparticles in the AFM phase of Yb3Pt4.

Water-dispersible, multifunctional, magnetic, luminescent silica-encapsulated composite nanotubes.

A multifunctional one-dimensional nanostructure incorporating both CdSe quantum dots (QDs) and Fe(3)O(4) nanoparticles (NPs) within a SiO(2)-nanotube matrix is successfully synthesized based on the self-assembly of preformed functional NPs, allowing for control over the size and amount of NPs contained within the composite nanostructures. This specific nanostructure is distinctive because both the favorable photoluminescent and magnetic properties of QD and NP building blocks are incorporated and retained within the final silica-based composite, thus rendering it susceptible to both magnetic guidance and optical tracking. Moreover, the resulting hydrophilic nanocomposites are found to easily enter into the interiors of HeLa cells without damage, thereby highlighting their capability not only as fluorescent probes but also as possible drug-delivery vehicles of interest in nanobiotechnology.

Synthesis and characterization of V2O3 nanorods.

In this work, VO2 nanorods have been initially generated as reactive nanoscale precursors to their subsequent conversion to large quantities of highly crystalline V2O3 with no detectable impurities. Structural changes in VO2, associated with the metallic-to-insulating transition from the monoclinic form to the rutile form, have been investigated and confirmed using X-ray diffraction and synchrotron data, showing that the structural transition is reversible and occurs at around 63 degrees C. When this VO2 one-dimensional sample was subsequently heated to 800 degrees C in a reducing atmosphere, it was successfully transformed into V2O3 with effective retention of its nanorod morphology. We have also collected magnetic and transport data on these systems that are comparable to bulk behavior and consistent with trends observed in previous experiments.

Manipulating the magnetic structure of Co core/CoO shell nanoparticles: implications for controlling the exchange bias.

We present an experimental study of the effects of oxidation on the magnetic and crystal structures of exchange biased epsilon-Co/CoO core-shell nanoparticles. Transmission electron microscopy measurements reveal that oxidation creates a Co-CoO interface which is highly directional and epitaxial in quality. Neutron diffraction measurements find that below a Néel temperature TN of approximately 235 K the magnetization of the CoO shell is modulated by two wave vectors, q1=(1/2 1/2 1/2)2pi/a and q2=(100)2pi/a. Oxidation affects the q1 component of the magnetization very little, but hugely enhances the q2 component, resulting in the magnetic decompensation of the core-shell interface. We propose that the large exchange bias effect results from the highly ordered interface between the Co core and CoO shell, and from enhanced core-shell coupling by the uncompensated interface moment.

Critical phenomena and the quantum critical point of ferromagnetic Zr(1-x)NbxZn2.

We present a study of the magnetic properties of Zr(1-x)NbxZn2, using an Arrott plot analysis of the magnetization. The Curie temperature Tc is suppressed to zero temperature for Nb concentration xc = 0.083+/-0.002, while the spontaneous moment vanishes linearly with Tc as predicted by the Stoner theory. The initial susceptibility chi displays critical behavior for x or= xc we find that chi(-1) = chi0(-1) + aT(4/3), where chi0(-1) vanishes as x-->xc. The resulting magnetic phase diagram shows that the quantum critical behavior extends over the widest range of temperatures for x=xc, and demonstrates how a finite transition temperature ferromagnet is transformed into a paramagnet, via a quantum critical point.

Extended versus local fluctuations in quantum critical Ce(Ru1-xFex)2Ge2 (x=xc=0.76).

We present inelastic neutron scattering experiments, performed near the antiferromagnetic quantum critical point in Ce(Ru0.24Fe0.76)2Ge2. Both local and long-range fluctuations of the local moments are observed, but due to the Kondo effect only the latter are critical. We propose a phenomenological expression which fits the energy E, temperature T, and wave vector q dependences of the dynamic susceptibility, describing the non-Fermi liquid E/T scaling found at every q.

Magnetic correlations and the quantum critical point of UCu5-xPdx (x = 1,1.5).

We have used inelastic neutron scattering to determine the magnetic susceptibility chi(q,omega,T) of the non-Fermi-liquid compounds UCu(5-x)Pdx (x = 1,1.5) for energies omega between 0.2 and 2 meV, and for temperatures T between 1.6 and 250 K. Spatial correlations in both UCu4Pd and UCu 3.5Pd1.5 extend over length scales comparable to the unit cell, and display very little temperature dependence. In contrast, the wave vector independent susceptibility diverges as T-->0. We find that the excitations at all q, and for all T and omega accessed display the same type of non-Fermi-liquid omega/T scaling.