Stephen E Nagler

An NCN-pincer ligand dysprosium single-ion magnet showing magnetic relaxation via the second excited state

Single-molecule magnets are compounds that exhibit magnetic bistability purely of molecular origin. The control of anisotropy and suppression of quantum tunneling to obtain a comprehensive picture of the relaxation pathway manifold, is of utmost importance with the ultimate goal of slowing the relaxation dynamics within single-molecule magnets to facilitate their potential applications. Combined ab initio calculations and detailed magnetization dynamics studies reveal the unprecedented relaxation mediated via the second excited state within a new DyNCN system comprising a valence-localized carbon coordinated to a single dysprosium(III) ion. The essentially C2v symmetry of the DyIII ion results in a new relaxation mechanism, hitherto unknown for mononuclear DyIII complexes, opening new perspectives for means of enhancing the anisotropy contribution to the spin-relaxation barrier.

Two-dimensional resonant magnetic excitation in BaFe1.84Co0.16As2.

Inelastic neutron scattering measurements on single crystals of superconducting BaFe1.84Co0.16As2 reveal a magnetic excitation located at wave vectors (1/2 1/2 L) in tetragonal notation. On cooling below T_{C}, a clear resonance peak is observed at this wave vector with an energy of 8.6(0.5) meV, corresponding to 4.5(0.3) k_{B}T_{C}. This is in good agreement with the canonical value of 5 k_{B}T_{C} observed in the cuprates. The spectrum shows strong dispersion in the tetragonal plane but very weak dispersion along the c axis, indicating that the magnetic fluctuations are two dimensional in nature. This is in sharp contrast to the anisotropic three dimensional spin excitations seen in the undoped parent compounds.

MAGNETIC EXCITATIONS IN THE S = 1/2 ALTERNATING CHAIN COMPOUND (VO)2P2O7

Magnetic excitations in an array of (VO)_2P_2O_7 single crystals have been measured using inelastic neutron scattering. Until now, (VO)_2P_2O_7 has been thought of as a two-leg antiferromagnetic Heisenberg spin ladder with chains running in the a-direction. The present results show unequivocally that (VO)_2P_2O_7 is best described as an alternating spin-chain directed along the crystallographic b-direction. In addition to the expected magnon with magnetic zone-center energy gap \Delta = 3.1 meV, a second excitation is observed at an energy just below 2\Delta. The higher mode may be a triplet two-magnon bound state.

Visualizing the chemistry and structure dynamics in lithium-ion batteries by in-situ neutron diffraction

We report an in-situ neutron diffraction study of a large format pouch battery cell. The succession of Li-Graphite intercalation phases was fully captured under an 1C charge-discharge condition (i.e., charge to full capacity in 1 hour). However, the lithiation and dilithiation pathways are distinctively different and, unlike in slowing charging experiments with which the Li-Graphite phase diagram was established, no LiC24 phase was found during charge at 1C rate. Approximately 75 mol. % of the graphite converts to LiC6 at full charge, and a lattice dilation as large as 4% was observed during a charge-discharge cycle. Our work demonstrates the potential of in-situ, time and spatially resolved neutron diffraction study of the dynamic chemical and structural changes in “real-world” batteries under realistic cycling conditions, which should provide microscopic insights on degradation and the important role of diffusion kinetics in energy storage materials.

Magnetic Spin Ladder (C5H12N)2CuBr4: High Field Magnetization and Scaling Near Quantum Criticality

The magnetization, M(H< or =30 T,0.7< or =T< or =300 K), of (C5H12N)2CuBr4 has been used to identify this system as an S = 1/2 Heisenberg two-leg ladder in the strong-coupling limit, J( perpendicular) = 13.3 K and J( parallel) = 3.8 K, with H(c1) = 6.6 T and H(c2) = 14.6 T. An inflection point in M(H,T = 0.7 K) at half saturation, M(s)/2, is described by an effective XXZ chain. The data exhibit universal scaling behavior in the vicinity of H(c1) and H(c2), indicating that the system is near a quantum critical point.

Three-dimensional magnetic correlations in multiferroic LuFe2O4.

We present single crystal neutron diffraction measurements on multiferroic LuFe(2)O(4). Magnetic reflections are observed below transitions at 240 and 175 K indicating that the magnetic interactions in LuFe(2)O(4) are three-dimensional in character. The magnetic structure is refined as a ferrimagnetic spin configuration below the 240 K transition. Below 175 K a significant broadening of the magnetic peaks is observed along with the buildup of a diffuse component to the magnetic scattering.

Magnetic Excitations in the S=1/2 Alternating Chain Compound (VO) {sub 2}P{sub 2}O{sub 7}

Magnetic excitations in an array of (VO)_2P_2O_7 single crystals have been measured using inelastic neutron scattering. Until now, (VO)_2P_2O_7 has been thought of as a two-leg antiferromagnetic Heisenberg spin ladder with chains running in the a-direction. The present results show unequivocally that (VO)_2P_2O_7 is best described as an alternating spin-chain directed along the crystallographic b-direction. In addition to the expected magnon with magnetic zone-center energy gap \Delta = 3.1 meV, a second excitation is observed at an energy just below 2\Delta. The higher mode may be a triplet two-magnon bound state.

Quantum criticality and universal scaling of a quantum antiferromagnet

Quantum effects dominate the behaviour of many diverse materials. Of particular current interest are those systems in the vicinity of a quantum critical point (QCP). Their physical properties are predicted to reflect those of the nearby QCP with universal features independent of the microscopic details. The prototypical QCP is the Luttinger liquid (LL), which is of relevance to many quasi-one-dimensional materials. The magnetic material KCuF3 realizes an array of weakly coupled spin chains (or LLs) and thus lies close to but not exactly at the LL quantum critical point. By using inelastic neutron scattering we have collected a complete data set of the magnetic correlations of KCuF3 as a function of momentum, energy and temperature. The LL description is found to be valid over an extensive range of these parameters, and departures from this behaviour at high and low energies and temperatures are identified and explained.

Charge order in LuFe2O4: antiferroelectric ground state and coupling to magnetism

X-ray scattering by multiferroic LuFe2O4 is reported. Below 320 K, superstructure reflections indicate an incommensurate charge order with propagation close to (1/3 1/3 3/2). The corresponding charge configuration, also found by electronic structure calculations as most stable, contains polar Fe/O double layers with antiferroelectric stacking. Diffuse scattering at 360 K, with (1/3 1/3 0) propagation, indicates ferroelectric short-range correlations between neighboring double layers. The temperature dependence of the incommensuration indicates that charge order and magnetism are coupled.

Static and dynamic magnetism in underdoped superconductor BaFe1.92Co0.08As2.

We report neutron scattering measurements on single crystals of BaFe1.92Co0.08As2. The magnetic Bragg peak intensity is reduced by 6% upon cooling through TC. The spin dynamics exhibit a gap of 8 meV with anisotropic three-dimensional interactions. Below TC additional intensity appears at an energy of approximately 4.5(0.5) meV, similar to previous observations of a spin resonance in other Fe-based superconductors. No further gapping of the spin excitations is observed below TC for energies down to 2 meV. These observations suggest the redistribution of spectral weight from the magnetic Bragg position to a spin resonance, demonstrating the direct competition between static magnetic order and superconductivity.