Probing multi-spinon excitations outside of the two-spinon continuum in the antiferromagnetic spin chain cuprate Sr2CuO3.

One-dimensional (1D) magnetic insulators have attracted significant interest as a platform for studying quasiparticle fractionalization, quantum criticality, and emergent phenomena. The spin-1/2 Heisenberg chain with antiferromagnetic nearest neighbour interactions is an important reference system; its elementary magnetic excitations are spin-1/2 quasiparticles called spinons that are created in even numbers. However, while the excitation continuum associated with two-spinon states is routinely observed, the study of four-spinon and higher multi-spinon states is an open area of research. Here we show that four-spinon excitations can be accessed directly in Sr2CuO3 using resonant inelastic x-ray scattering (RIXS) in a region of phase space clearly separated from the two-spinon continuum. Our finding is made possible by the fundamental differences in the correlation function probed by RIXS in comparison to other probes. This advance holds promise as a tool in the search for novel quantum states and quantum spin liquids.

Nematicity in stripe-ordered cuprates probed via resonant x-ray scattering.

In underdoped cuprate superconductors, a rich competition occurs between superconductivity and charge density wave (CDW) order. Whether rotational symmetry-breaking (nematicity) occurs intrinsically and generically or as a consequence of other orders is under debate. Here, we employ resonant x-ray scattering in stripe-ordered superconductors (La,M)2CuO4 to probe the relationship between electronic nematicity of the Cu 3d orbitals, structure of the (La,M)2O2 layers, and CDW order. We find distinct temperature dependences for the structure of the (La,M)2O2 layers and the electronic nematicity of the CuO2 planes, with only the latter being enhanced by the onset of CDW order. These results identify electronic nematicity as an order parameter that is distinct from a purely structural order parameter in underdoped striped cuprates.

Memristive and neuromorphic behavior in a Li(x)CoO2 nanobattery.

The phenomenon of resistive switching (RS), which was initially linked to non-volatile resistive memory applications, has recently also been associated with the concept of memristors, whose adjustable multilevel resistance characteristics open up unforeseen perspectives in cognitive computing. Herein, we demonstrate that the resistance states of Li(x)CoO2 thin film-based metal-insulator-metal (MIM) solid-state cells can be tuned by sequential programming voltage pulses, and that these resistance states are dramatically dependent on the pulses input rate, hence emulating biological synapse plasticity. In addition, we identify the underlying electrochemical processes of RS in our MIM cells, which also reveal a nanobattery-like behavior, leading to the generation of electrical signals that bring an unprecedented new dimension to the connection between memristors and neuromorphic systems. Therefore, these LixCoO2-based MIM devices allow for a combination of possibilities, offering new perspectives of usage in nanoelectronics and bio-inspired neuromorphic circuits.

Low temperature ballistic spin transport in the S = 1/2 antiferromagnetic Heisenberg chain compound SrCuO2.

We report zero and longitudinal magnetic field muon spin relaxation (µSR) measurements of the spin S = 1/2 antiferromagnetic Heisenberg chain material SrCuO2. We find that in a weak applied magnetic field B0 the spin-lattice relaxation rate λ follows a power law λ is proportional to B(0)(-n) with n = 0.9(3). This result is temperature independent for 5 K ≤ T ≤ 300 K. Within conformal field theory and using the Müller ansatz we conclude ballistic spin transport in SrCuO2.

Magnetic order in hybrid frustrated magnets Gd(2-x)Tb(x)Ti2O7 (x = 0.2 and 0.5).

We report on the specific heat, magnetization and ac susceptibility measurements of single crystals of hybrid frustrated magnets Gd(1.8)Tb(0.2)Ti(2)O(7) and Gd(1.5)Tb(0.5)Ti(2)O(7). The analysis of experimental data revealed that, although partial replacing of the Gd(3+) ions by the Tb(3+) ions in the Gd(2)Ti(2)O(7) host lattice slightly enhances antiferromagnetic coupling, as inferred from the evolution of the paramagnetic Curie-Weiss temperature, the ordering temperature gradually decreases. Paramagnetic correlations introduced by the Tb(3+) ions cause this perturbation, altering the effective further neighbor interactions and destabilizing the ground state in Gd(2)Ti(2)O(7). In addition, the low-energy states of Gd(2-x)Tb(x)Ti(2)O(7) are suggested to possess a nature different from those in parent members Tb(2)Ti(2)O(7) and Gd(2)Ti(2)O(7). Finally, the frequency-dependent magnetic susceptibility behavior in Gd(1.5)Tb(0.5)Ti(2)O(7) is consistent with the formation of a spin-glass-like state indicating a pronounced slowing down of the dynamical response of the studied hybrid magnets.

Spin-orbital separation in the quasi-one-dimensional Mott insulator Sr2CuO3.

When viewed as an elementary particle, the electron has spin and charge. When binding to the atomic nucleus, it also acquires an angular momentum quantum number corresponding to the quantized atomic orbital it occupies. Even if electrons in solids form bands and delocalize from the nuclei, in Mott insulators they retain their three fundamental quantum numbers: spin, charge and orbital. The hallmark of one-dimensional physics is a breaking up of the elementary electron into its separate degrees of freedom. The separation of the electron into independent quasi-particles that carry either spin (spinons) or charge (holons) was first observed fifteen years ago. Here we report observation of the separation of the orbital degree of freedom (orbiton) using resonant inelastic X-ray scattering on the one-dimensional Mott insulator Sr2CuO3. We resolve an orbiton separating itself from spinons and propagating through the lattice as a distinct quasi-particle with a substantial dispersion in energy over momentum, of about 0.2 electronvolts, over nearly one Brillouin zone.

Pressure-induced colossal piezoresistance effect and the collapse of the polaronic state in the bilayer manganite (La(0.4)Pr(0.6))(1.2)Sr(1.8)Mn2O7.

We have investigated the effect of hydrostatic pressure as a function of temperature on the resistivity of a single crystal of the bilayer manganite (La(0.4)Pr(0.6))(1.2)Sr(1.8)Mn(2)O(7). Whereas a strong insulating behaviour is observed at all temperatures at ambient pressure, a clear transition into a metallic-like behaviour is induced when the sample is subjected to a pressure (P) of ~1.0 GPa at T < 70 K. A huge negative piezoresistance ~10(6) in the low temperature region at moderate pressures is observed. When the pressure is increased further (5.5 GPa), the high temperature polaronic state disappears and a metallic behaviour is observed. The insulator to metal transition temperature exponentially increases with pressure and the distinct peak in the resistivity that is observed at 1.0 GPa almost vanishes for P > 7.0 GPa. A modification in the orbital occupation of the e(g) electron between 3d(x(2)-y(2)) and 3d(z(2)-r(2)) states, as proposed earlier, leading to a ferromagnetic double-exchange phenomenon, can qualitatively account for our data.

Electronic confinement and ordering instabilities in colossal magnetoresistive bilayer manganites.

We present angle-resolved photoemission studies of (La{1-z}Pr{z}){2-2x}Sr{1+2x}Mn{2}O{7} with x=0.4 and z=0.1, 0.2, and 0.4 along with density functional theory calculations and x-ray scattering data. Our results show that the bilayer splitting in the ferromagnetic metallic phase of these materials is small, if not completely absent. The charge carriers are therefore confined to a single MnO{2} layer, which in turn results in a strongly nested Fermi surface. In addition to this, the spectral function also displays clear signatures of an electronic ordering instability well below the Fermi level. The increase of the corresponding interaction strength with z and its magnitude of ∼400 meV make the coupling to a bare phonon highly unlikely. Instead we conclude that fluctuating order, involving electronic and lattice degrees of freedom, causes the observed renormalization of the spectral features.

Anomalous temperature dependence of phonons and photoluminescence bands in pyrochlore Er2Ti2O7: signatures of structural deformation at 130 K.

We report a Raman study of single crystal pyrochlore Er(2)Ti(2)O(7) as a function of temperature from 12 to 300 K. In addition to the phonons, various photoluminescence (PL) lines of Er(3+) in the visible range are also observed. Our Raman data show an anomalous red-shift of two phonons (one at ~200 cm(-1) and another at ~520 cm(-1)) upon cooling from room temperature which is attributed to phonon-phonon anharmonic interactions. However, the phonons at ~310, 330, and 690 cm(-1) initially show a blue-shift upon cooling from room temperature down to about 130 K, followed by a red-shift, indicating a structural deformation at ~130 K. The intensities of the PL bands associated with the transitions between the various levels of the ground state manifold ((4)I(15/2)) and the (2)H(11/2) as well as (4)S(3/2) excited state manifolds of Er(3+) show a change at ~130 K. Moreover, the temperature dependence of the peak position of the two PL bands shows a change in their slope (dω/dT) at ~130 K, thus further strengthening the proposal of a structural deformation. The temperature dependence of the peak positions of the PL bands has been analyzed using the theory of optical dephasing in crystals.

Photoinduced melting of antiferromagnetic order in La(0.5)Sr(1.5)MnO4 measured using ultrafast resonant soft x-ray diffraction.

We used ultrafast resonant soft x-ray diffraction to probe the picosecond dynamics of spin and orbital order in La(0.5)Sr(1.5)MnO(4) after photoexcitation with a femtosecond pulse of 1.5 eV radiation. Complete melting of antiferromagnetic spin order is evidenced by the disappearance of a (1/4,1/4,1/2) diffraction peak. On the other hand, the (1/4,1/4,0) diffraction peak, reflecting orbital order, is only partially reduced. We interpret the results as evidence of destabilization in the short-range exchange pattern with no significant relaxation of the long-range Jahn-Teller distortions. Cluster calculations are used to analyze different possible magnetically ordered states in the long-lived metastable phase. Nonthermal coupling between light and magnetism emerges as a primary aspect of photoinduced phase transitions in manganites.

Evidence for charge orbital and spin stripe order in an overdoped manganite.

Overdoped La0.42Sr1.58MnO4 exhibits a complex ordering of charges, orbitals, and spins. Neutron diffraction experiments reveal three incommensurate and one commensurate order parameters to be tightly coupled. The position and the shape of the distinct superstructure scattering as well as higher-order signals are inconsistent with a harmonic charge and spin-density-wave picture but point to a stripe arrangement in which ferromagnetic zigzag chains are disrupted by excess Mn(4+).

The zero-field glassy ground state and field-induced ferromagnetic transition in (La0.4Pr0.6)1.2Sr1.8Mn2O7.

We have investigated glassy magnetic freezing in(La0.4Pr0.6)1.2Sr1.8Mn2O7 single crystals together with the field-induced transition to a metastable ferromagnetic phase using ac magnetic susceptibility and heat capacity measurements. The magnetization measurements show evidence for the development of a zero-field glassy ground state below 45 K along with a hysteretic, field-induced change in susceptibility associated with the transition to the ferromagnetic phase above 5 T. The heat capacity develops a clear peak at higher temperatures with the application of large magnetic fields, consistent with the development of a ferromagnetic order, while at low temperatures the Sommerfeld coefficient is monotonically reduced by an applied field, suggesting suppression of spin fluctuations. The heat capacity shows hysteretic behaviour, accompanied by a sharp decrease at a critical field, when held at fixed temperature, which does not recover on reducing the field back to zero. These measurements suggest that the zero-field ground state for (La0.4Pr0.6)1.2Sr1.8Mn2O7 consists of frozen disordered spin clusters, which develop into a metastable ferromagnetic state in modest magnetic fields.

Multiple spin-flop phase diagram of BaCu2Si2O7.

The quasi-one-dimensional compound BaCu(2)Si(2)O(7) demonstrates numerous spin-reorientation transitions both for a magnetic field applied along the easy axis of magnetization and a magnetic field applied perpendicular to it. The magnetic phase diagram for all three principal orientations is obtained by magnetization and specific heat measurements. Values of all critical fields and low-temperature values of magnetization jumps are determined for all transitions.

Macroscopic quantum coherence of the spin triplet in the spin-ladder compound Sr14Cu24O41.

We report the direct observation by inelastic neutron scattering experiments of a spin triplet of magnetic excitations in the response associated with the ladders in the composite cuprate Sr14Cu24O41. This appears as a peak at q(Q1D)=π and energy Δ1=32.5 meV, and we conjecture that all the triplets making up this conspicuous peak have the same phase and therefore interpret it as the signature of the occurrence of quantum coherence along the ladder direction between entangled spin pairs. From the comparison with previous neutron and x-ray data, we conclude that the temperature evolution of this mode is driven by the crystallization of holes into a charge density wave in the ladder sublattice.

Bridging charge-orbital ordering and Fermi surface instabilities in half-doped single-layered manganite La(0.5)Sr(1.5)MnO4.

The single-layered half-doped manganite La(0.5)Sr(1.5)MnO4 (LSMO), was studied by means of the angle-resolved photoemission spectroscopy (ARPES), scanning tunneling microscopy (STM), and resistivity measurements. STM revealed a smooth reconstruction-free surface; the density of states, extracted from photoemission and tunneling spectroscopy, is in agreement with transport measurements. The derived from ARPES Fermi surface (FS) nesting properties correspond to the known pattern of the charge-orbital ordering (COO), which implies that FS instability is related to the propensity to form a COO state in LSMO.

Effect of pressure on lattice distortion, transport and magnetic properties of Pr-substituted La(1.2)Sr(1.8)Mn(2)O(7) bilayered manganite.

We have studied the effect of pressure on the anomalous lattice striction, both in the ab-plane and along the c-axis, of (La,Pr)(1.2)Sr(1.8)Mn(2)O(7) single crystals over the temperature region where the paramagnetic insulator to ferromagnetic metal transition takes place. We have examined the temperature dependence of the resistivity and the magnetization under applied pressure. The chemical pressure effect due to Pr-substitution at the La site suppresses the transition temperature of the parent crystal, while the application of external pressure on Pr-substituted crystals enhances the double exchange driven metallic state, resulting in a stable rise of T(c).

Steplike lattice deformation of single crystalline (La0.4Pr0.6)1.2Sr1.8Mn2O7 bilayered manganite.

We report a steplike lattice transformation of single crystalline (La0.4Pr0.6)1.2Sr1.8Mn2O7 bilayered manganite accompanied by both magnetization and magnetoresistive jumps, and examine the ultrasharp nature of the field-induced first-order transition from a paramagnetic insulator to a ferromagnetic metal phase accompanied by a huge decrease in resistance. Our findings support that the abrupt magnetostriction is closely related to an orbital frustration existing in the inhomogeneous paramagnetic insulating phase rather than a martensitic scenario between competing two phases.

Quasiparticlelike peaks, kinks, and electron-phonon coupling at the (pi,0) regions in the CMR oxide La2-2x Sr1+2x Mn2 O7.

Using angle-resolved photoemission, we have observed sharp quasiparticlelike peaks in the prototypical layered manganite La(2-2x)Sr(1+2x)Mn(2)O(7) (x=0.36,0.38). We focus on the (pi,0) regions of k space and study their electronic scattering rates and dispersion kinks, uncovering bilayer-split bands, the critical energy scales, momentum scales, and strengths of the interactions that renormalize the electrons. To identify these bosons, we measured phonon dispersions in the energy range of the kink by inelastic neutron scattering, finding a good match in both energy and momentum to the oxygen bond-stretching phonons.

Orbital polaron lattice formation in lightly doped.

By resonant x-ray scattering at the Mn K edge on La(7/8)Sr(1/8)MnO3, we show that an orbital polaron lattice (OPL) develops at the metal-insulator transition of this compound. This orbital reordering explains consistently the unexpected coexistence of ferromagnetic and insulating properties at low temperatures, the quadrupling of the lattice structure parallel to the MnO2 planes, and the observed polarization and azimuthal dependencies. The OPL is a clear manifestation of strong orbital-hole interactions, which play a crucial role for the colossal magnetoresistance effect and the doped manganites in general.

Structural aspects of metamagnetism in Ca2-xSrxRuO4: evidence for field tuning of orbital occupation.

The crystal structure of Ca(2-x)Sr(x)RuO(4) with 0.2 < or = x < or = 1.0 has been studied by diffraction techniques and by high resolution capacitance dilatometry as a function of temperature and magnetic field. Upon cooling in zero magnetic field, the crystal structure and the octahedra shrink along the c direction and elongate in the a and b planes, whereas the opposite occurs upon cooling at high field (x = 0.2 and 0.5). These findings yield evidence for an orbital rearrangement driven by temperature and magnetic field, which accompanies the metamagnetic transition at low temperature. The temperature and magnetic-field dependencies are found to be governed by the same energy scale.