M. C. Aronson

CaMn2Sb2: Spin waves on a frustrated antiferromagnetic honeycomb lattice

We present inelastic neutron scattering measurements of the antiferromagnetic insulator CaMn2Sb2:, which consists of corrugated honeycomb layers of Mn. The dispersion of magnetic excitations has been measured along the H and L directions in reciprocal space, with a maximum excitation energy of ≈ 24 meV. These excitations are well described by spin waves in a Heisenberg model, including first and second neighbor exchange interactions, J1 and J2, in the Mn plane and also an exchange interaction between planes. The determined ratio J2/J1 ≈ 1/6 suggests that CaMn2Sb2: is the first example of a compound that lies very close to the mean field tricritical point, known for the classical Heisenberg model on the honeycomb lattice, where the N´eel phase and two different spiral phases coexist. The magnitude of the determined exchange interactions reveal a mean field ordering temperature ≈ 4 times larger than the reported N´eel temperature TN = 85 K, suggesting significant frustration arising from proximity to the tricritical point.

Magnetic structure of Yb2Pt2Pb: Ising moments on the Shastry-Sutherland lattice

Here, we have synthesized single crystals of Yb2Pt2Pb, which crystallize in the layered U2Pt2Sn-type structure, where planes of Yb ions lie on a triangular network. Here, we report the results of magnetization, specific heat, and electrical resistivity experiments. The lattice constants and high temperature magnetic susceptibility indicate that the Yb ions are trivalent, while the Schottky peaks in the specific heat show that the ground state is a well isolated doublet. A significant magnetic anisotropy is observed, with the ratio of susceptibilities perpendicular and parallel to the magnetic planes differing by as much as a factor of 30 at the lowest temperatures. Antiferromagnetic order occurs at a Neel temperature TN = 2.07 K. Evidence of short range magnetic fluctuations is found in the magnetic susceptibility and electrical resistivity, which have broad peaks above TN, and in the slow development of the magnetic entropy at TN. Our experiments indicate that Yb2Pt2Pb is a quasi-two-dimensional and localized moment system, where strong magnetic frustration may arise from the geometry of the underlying Shastry-Sutherland lattice.

Near-field spectroscopic investigation of dual-band heavy fermion metamaterials

Broadband tunability is a central theme in contemporary nanophotonics and metamaterials research. Combining metamaterials with phase change media offers a promising approach to achieve such tunability, which requires a comprehensive investigation of the electromagnetic responses of novel materials at subwavelength scales. In this work, we demonstrate an innovative way to tailor band-selective electromagnetic responses at the surface of a heavy fermion compound, samarium sulfide (SmS). By utilizing the intrinsic, pressure sensitive, and multi-band electron responses of SmS, we create a proof-of-principle heavy fermion metamaterial, which is fabricated and characterized using scanning near-field microscopes with <50u2009nm spatial resolution. The optical responses at the infrared and visible frequency ranges can be selectively and separately tuned via modifying the occupation of the 4f and 5d band electrons. The unique pressure, doping, and temperature tunability demonstrated represents a paradigm shift for nanoscale metamaterial and metasurface design.Understanding the electromagnetic responses at subwavelength scales is important for achieving tunability. Using a combination of the near-field and far-field spectroscopy, the authors demonstrate a heavy fermion metamaterial with tunable dual-band optical responses by selectively and separately modifying the 4f and 5d band electrons.

Local quantum phase transition in YFe2Al10

Significance We report the discovery of a type of phase transition that occurs at T=0. In continuous phase transitions, order occurs when the size and lifetime of small ordered regions increase until they span the system and become static. Reported here is experimental evidence of a transition where this paradigm fails. Our observed phase transition is local, where each magnetic moment in YFe2Al10 is independent of every other moment, yet each moment follows the same spectrum of quantum critical fluctuations. The phase transition present in YFe2Al10 is a realization of a scenario only hinted at by theory, corresponding to the formation of magnetic moments, with no evidence for the breaking of translational symmetry that accompanies magnetic order. 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 T=0 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.

Combined computational and experimental investigation of the La2CuO4–xSx (0 ≤ x ≤ 4) quaternary system

Significance Discovery of new materials enabling new technologies, from novel electronics to better magnets, has so far relied on serendipity. Computational advances show promise that new materials can be designed in a computer and not in the lab, a proposal called “Materials by Design.” We present here a detailed comparison between theory and experiment, carrying out the synthesis of a high-temperature superconductor in an X-ray beam to elucidate the sequence of chemical reactions as the compound forms. Parallel computations of the stabilities of possible compounds that could form from the selected elements accurately predict the observed reactions. Paired with our chemical intuition, this methodology provides understanding and potentially control of the essential chemical principles responsible for stabilizing virtually any compound. The lack of a mechanistic framework for chemical reactions forming inorganic extended solids presents a challenge to accelerated materials discovery. We demonstrate here a combined computational and experimental methodology to tackle this problem, in which in situ X-ray diffraction measurements monitor solid-state reactions and deduce reaction pathways, while theoretical computations rationalize reaction energetics. The method has been applied to the La2CuO4−xSx (0 ≤ x ≤ 4) quaternary system, following an earlier prediction that enhanced superconductivity could be found in these new lanthanum copper(II) oxysulfide compounds. In situ diffraction measurements show that reactants containing Cu(II) and S(2−) ions undergo redox reactions, leaving their ions in oxidation states that are incompatible with forming the desired new compounds. Computations of the reaction energies confirm that the observed synthetic pathways are indeed favored over those that would hypothetically form the suggested compounds. The consistency between computation and experiment in the La2CuO4−xSx system suggests a role for predictive theory: to identify and to explicate new synthetic routes for forming predicted compounds.

Unconventional large linear magnetoresistance in Cu2−xTe

We report a large linear magnetoresistance in Cu2−xTe, reaching Δρ/ρ(0) = 250% at 2 K in a 9 T field, for samples with x = 0.13 to 0.22. These results are comparable to those for Ag2X materials, though for Cu2−xTe the carrier densities are considerably larger. Examining the magnitudes and the crossover from quadratic to high-field linear behavior, we show that models based on classical transport behavior best explain the observed results. The effects are traced to the misdirection of currents in high mobility transport channels, likely due to behavior at grain boundaries such as topological surface states or a high mobility interface phase. The resistivity also exhibits a T2 dependence in the temperature range where the large linear MR appears, an indicator of electron-electron interaction effects within the high mobility states. Thus this is an example of a system in which electron-electron interactions dominate the low-temperature linear magnetoresistance.We report a large linear magnetoresistance in Cu2−xTe, reaching Δρ/ρ(0) = 250% at 2 K in a 9 T field, for samples with x = 0.13 to 0.22. These results are comparable to those for Ag2X materials, though for Cu2−xTe the carrier densities are considerably larger. Examining the magnitudes and the crossover from quadratic to high-field linear behavior, we show that models based on classical transport behavior best explain the observed results. The effects are traced to the misdirection of currents in high mobility transport channels, likely due to behavior at grain boundaries such as topological surface states or a high mobility interface phase. The resistivity also exhibits a T2 dependence in the temperature range where the large linear MR appears, an indicator of electron-electron interaction effects within the high mobility states. Thus this is an example of a system in which electron-electron interactions dominate the low-temperature linear magnetoresistance.