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Developing microscopic understanding of the thermal properties of liquids is challenging due to their strong dynamic disorder, which prevents characterization of the atomic degrees of freedom. There have been significant research interests in the past few decades to extend the normal mode analysis for solids to instantaneous structures of liquids. However, the nature of normal modes that arise from these unstable structures is still elusive. In this work, we explore the instantaneous eigenmodes of dynamical matrices of various Lennard-Jones argon liquid/gas systems at high temperatures and show that the normal modes can be interpreted as an interpolation of T \to \infty (gas) and T = 0 (solid) mode descriptions. We find that normal modes become increasingly collisional and translational, recovering atomistic gas-like behavior rather than vibrational with increase in temperature, suggesting that normal modes in liquids may be described by both solid-like and gas-like modes.

Elucidating the atomic structure of liquid and glass is one of the important open questions in condensed matter physics. In the conventional bottom-up approach one starts with focusing on an atom and the short-range order of its neighboring atoms, and the global structure is described in terms of overlapping local clusters of atoms as building units. However, this local approach fails to explain the strong drive to form the medium-range order which is distinct in nature from the short-range order. We propose an even-handed scheme with an additional top-down approach. In the top-down approach one starts with a high-density gas state and seeks to minimize the global potential energy through density waves. The local bottom-up and global top-down driving forces are not compatible, and the competition and compromise between them result in a final structure with the medium-range order. The density waves are pinned to atoms through the phase factors and amplitudes which reflect atomic dynamics. This even-handed approach provides a more intuitive explanation of the structure of simple liquid and glass and its relation to properties of liquid, such as viscosity and fragility., Comment: Continuation of C. W. Ryu and T. Egami, Phys. Rev. E 104, 064109 (2021) and T. Egami and C. W. Ryu, Phys. Rev. E 104, 064110 (2021)

Understanding thermodynamics in liquids at the atomic level is challenging because of strong atomic interactions and lack of symmetry. Recent prior theoretical works have focused on describing heat capacity of liquids in terms of phonon-like excitations but often rely on fitting parameters and ad hoc assumptions. In this work, we perform microscopic analysis on instantaneous normal modes and velocity autocorrelations on molecular dynamics simulations of single element systems over wide ranges of temperature (up to $10^8$ K) and pressure (up to 1 TPa). Our results demonstrate that heat capacity of liquids can be described by a combination of both solid-like and gas-like degrees of freedom, leading to a unified framework to describe heat capacity of all three phases of matter: solid, liquid, and gas.

Experimentally resolving atomic-scale structural changes of a deformed glass remains challenging owing to the disordered nature of glass structure. Here, we show that the structural anisotropy emerges as a general hallmark for different types of glasses (metallic glasses, oxide glass, amorphous selenium, and polymer glass) after thermo-mechanical deformation, and it is highly correlates with local nonaffine atomic displacements detected by the high-energy X-ray diffraction technique. By analyzing the anisotropic pair density function, we unveil the atomic-level mechanism responsible for the plastic flow, which notably differs between metallic glasses and covalent glasses. The structural rearrangements in metallic glasses are mediated through cutting and formation of atomic bonds, which occurs in some localized inelastic regions embedded in elastic matrix, whereas that of covalent glasses is mediated through the rotation of atomic bonds or chains without bond length change, which occurs in a less localized manner., Comment: 19 pages, 4 figures

Slow relaxation and plastic deformation in disordered materials such as metallic glasses and supercooled liquids occur at dynamical heterogeneities, or neighboring particles that rearrange in a correlated, cooperative manner. Dynamical heterogeneities have historically been described by a four-point, time-dependent density correlation function $\chi_4 (r, t)$. In this paper, we posit that $\chi_4 (r, t)$ contains essentially the same information about medium-range order as the Van Hove correlation function $G(r, t)$. In other words, medium-range order is the origin of spatially correlated regions of cooperative particle motion. The Van Hove function is the preferred tool for describing dynamical heterogeneities than the four-point function, for which the physical meaning is less transparent.

The coherence length of the medium-range order (MRO) in metallic liquids is known to display a Curie-Weiss temperature dependence; its inverse is linearly related to temperature, and when extrapolated from temperatures above the glass transition, the coherence length diverges at a negative temperature with a critical exponent of unity. We propose a mean-field pseudospin model that explains this behavior. Specifically, we model the atoms and their local environment as Ising spins with antiferromagnetic exchange interactions. We further superimpose an exchange interaction between dynamical heterogeneities, or clusters of atoms undergoing cooperative motion. The coherence length in the metallic liquid is thus the correlation length between dynamical heterogeneities. Our results reaffirm the idea that the MRO coherence length is a measure of point-to-set correlations, and that local frustrations in the interatomic interactions are prominent in metallic liquids.

Metallic glasses exhibit fast mechanical relaxations at temperatures well below the glass transition, one of which shows little variation with temperature known as nearly constant loss (NCL). Despite the important implications of this phenomenon to in aging and deformation, the origin of the relaxation is unclear. Through molecular dynamics simulations of a model metallic glass, Cu_64.5Zr_35.5, we implement dynamic mechanical analysis with system stress decomposed into atomic-level stresses to identify the group of atoms responsible for NCL. This work demonstrates that NCL relaxation is due to fully transient groups of atoms that become normal over picosecond timescales. They are spatially distributed throughout the glass and have no outstanding features, rather than defect-like as previously reported.

The attenuation rate of vibrational excitations in various metallic liquids and glasses has been reported to change from the quadratic dependence on wavevector at low wavevectors to the linear dependence at high wavevectors. However, the origin of this behavior is not clear. Here, the analysis of this phenomenon through molecular dynamics is presented for prototypical metallic liquids, Cu56Zr44 and Fe. It is shown that the crossover wavevector is strongly correlated with the structural coherence length characterizing coarse-grained density correlations. We suggest that the linear dependence is caused by scattering of vibrational excitations by structural activation processes with low activation energies which are distinctively observed in metallic systems.

With their brilliance and temporal structure, X-ray free-electron laser can unveil atomic-scale details of ultrafast phenomena. Recent progress in split-and-delay optics (SDO), which produces two X-ray pulses with time-delays, offers bright prospects for observing dynamics at the atomic-scale. However, their insufficient pulse energy has limited its application either to phenomena with longer correlation length or to measurement with a fixed delay-time. Here we show that the combination of the SDO and self-seeding of X-rays increases the pulse energy and makes it possible to observe the atomic-scale dynamics in a timescale of picoseconds. We show that the speckle contrast in scattering from water depends on the delay-time as expected. Our results demonstrate the capability of measurement using the SDO with seeded X-rays for resolving the dynamics in temporal and spatial scales that are not accessible by other techniques, opening opportunities for studying the atomic-level dynamics., Comment: 22 pages, 5 figures

We propose mechanisms for the spin Hall effect in metallic systems arising from the coupling between conduction electrons and local magnetic moments that are dynamically fluctuating. Both a side-jump-type mechanism and a skew-scattering-type mechanism are considered. In either case, dynamical spin fluctuation gives rise to a nontrivial temperature dependence in the spin Hall conductivity. This leads to the enhancement in the spin Hall conductivity at nonzero temperatures near the ferromagnetic instability. The proposed mechanisms could be observed in $4d$ or $5d$ metallic compounds., Comment: 5 pages for the main text with 4 figures, and 5 pages with 1 figure for the supplementary material

Whereas exceptional mechanical and radiation performances have been found in the emergent medium- and high-entropy alloys (MEAs and HEAs), the importance of their complex atomic environment, reflecting diversity in atomic size and chemistry, to defect transport has been largely unexplored at the atomic level. Here we adopt a local structure approach based on the atomic pair distribution function measurements in combination with density functional theory calculations to investigate a series of body-centered cubic (BCC) MEAs and HEAs. Our results demonstrate that all alloys exhibit local lattice distortions (LLD) to some extent, but an anomalous LLD, merging of the first and second atomic shells, occurs only in the Zr- and/or Hf-containing MEAs and HEAs. In addition, through the ab-initio simulations we show that charge transfer among the elements profoundly reduce the size mismatch effect. The observed competitive coexistence between LLD and charge transfer not only demonstrates the importance of the electronic effects on the local environments in MEAs and HEAs, but also provides new perspectives to in-depth understanding of the complicated defect transport in these alloys., Comment: 5 figures, 2 tables

The microscopic deformation mechanism of charged colloidal glasses with extended-range interactions under shear is investigated by in-situ small-angle neutron scattering, and a dynamically correlated region (DCR) is identified. This short-lived region provides the resistance to the configurational rearrangement imposed by the external deformation, as evidenced by the evolution of the size of DCR in the shear thinning regime and the quantitative agreement between the local stress sustained by DCR and the macroscopic stress from rheological measurements at low and mediate shear rates. This finding suggests that DCR is an important quantity for microscopically addressing the flow and deformation behavior of strongly interacting colloids., Comment: arXiv admin note: substantial text overlap with arXiv:1611.03135

The flow of colloidal suspensions is ubiquitous in nature and industry. Colloidal suspensions exhibit a wide range of rheological behavior, which should be closely related to the microscopic structure of the systems. With in-situ small-angle neutron scattering complemented by rheological measurements, we investigated the deformation behavior of a charge-stabilized colloidal glass at particle level undergoing steady shear. A short-lived, localized elastic response at particle level, termed as transient elasticity zone (TEZ), was identified from the neutron spectra. The existence of the TEZ is a signature of the dynamical heterogeneity: The body of fluids under shear behaves like an elastic solid within the spatial range of TEZ but like fluid outside the TEZ. The size of TEZ shrinks as the shear rate increases in the shear thinning region, which shows that the shear thinning is accompanied by a diminishing dynamical heterogeneity. More interestingly, the TEZ is found to be the structural unit that provides the resistance to the imposed shear, as evidenced by the quantitative agreement between the local elastic stress sustained by TEZ and the macroscopic stress from rheological measurements at low and moderate shear rates. Besides the charged-stabilized colloidal suspension, a hard-sphere colloidal suspension at the same volume fraction and shear rates was also measured. The result highlights the key role of the electrostatic interparticle repulsion in promoting the local elasticity. Our findings provide an understanding on the nonlinear rheology of interacting colloidal glasses from a micro-mechanical view., Comment: 18 pages,5 figures

We report the observation of a distinct correlation between the kinetic fragility index $m$ and the reduced Arrhenius crossover temperature $\theta_A = T_A/T_g$ in various glass-forming liquids, identifying three distinguishable groups. In particular, for 11 glass-forming metallic liquids, we universally observe a crossover in the mean diffusion coefficient from high-temperature Arrhenius to low-temperature super-Arrhenius behavior at approximately $\theta_A \approx 2$ which is in the stable liquid phases. In contrast, for fragile molecular liquids, this crossover occurs at much lower $\theta_A \approx 1.4$ and usually in their supercooled states. The $\theta_A$ values for strong network liquids spans a wide range higher than 2. Intriguingly, the high-temperature activation barrier $E_\infty$ is universally found to be $\sim 11\ k_B T_g$ and uncorrelated with the fragility or the reduced crossover temperature $\theta_A$ for metallic and molecular liquids. These observations provide a way to estimate the low-temperature glassy characteristics ($T_g$ and $m$) from the high-temperature liquid quantities ($E_\infty$ and $\theta_A$)., Comment: 6 pages, 4 figures

Oxygen-defect control has long been considered an influential tuning knob for producing various property responses in complex oxide films. In addition to physical property changes, modification to the lattice structure, specifically lattice expansion, with increasing oxygen vacancy concentrations has been reported often and has become the convention for oxide materials. However, the current understanding of the lattice behavior in oxygen-deficient films becomes disputable when considering compounds containing different bonding environments or atomic layering. Moreover, tensile strain has recently been discovered to stabilize oxygen vacancies in epitaxial films, which further complicates the interpretation of lattice behavior resulting from their appearance. Here, we report on the selective strain control of oxygen vacancy formation and resulting lattice responses in the layered, Ruddlesden-Popper phases, La1.85Sr0.15CuO4. We found that a drastically reduced Gibbs free energy for oxygen vacancy formation near the typical growth temperature for tensile-strained epitaxial LSCO accounts for the large oxygen non-stoichiometry. Additionally, oxygen vacancies form preferentially in the equatorial position of the CuO2 plane, leading to a lattice contraction, rather than the expected expansion, observed with apical oxygen vacancies. Since oxygen stoichiometry plays a key role in determining the physical properties of many complex oxides, the strong strain coupling of oxygen nonstoichiometry and the unusual structural response reported here can provide new perspectives and understanding to the structure and property relationships of many other functional oxide materials.

Precise control of the chemical valence or oxidation state of vanadium in vanadium oxide thin films is highly desirable for not only fundamental research, but also technological applications that utilize the subtle change in the physical properties originating from the metal- insulator transition (MIT) near room temperature. However, due to the multivalent nature of vanadium and the lack of a good understanding on growth control of the oxidation state, stabilization of phase pure vanadium oxides with a single oxidation state is extremely challenging. Here, we systematically varied the growth conditions to clearly map out the growth window for preparing phase pure epitaxial vanadium oxides by pulsed laser deposition for providing a guideline to grow high quality thin films with well-defined oxidation states of V2(+3)O3, V(+4)O2, and V2(+5)O5. A well pronounced MIT was only observed in VO2 films grown in a very narrow range of oxygen partial pressure P(O2). The films grown either in lower (< 10 mTorr) or higher P(O2) (> 25 mTorr) result in V2O3 and V2O5 phases, respectively, thereby suppressing the MIT for both cases. We have also found that the resistivity ratio before and after the MIT of VO2 thin films can be further enhanced by one order of magnitude when the films are further oxidized by post-annealing at a well-controlled oxidizing ambient. This result indicates that stabilizing vanadium into a single valence state has to compromise with insufficient oxidation of an as grown thin film and, thereby, a subsequent oxidation is required for an improved MIT behavior., Comment: 16 pages, 4 figures

It is difficult to relate the properties of liquids and glasses directly to their structure because of complexity in the structure which defies precise definition. The potential energy landscape (PEL) approach is a very insightful way to conceptualize the structure-property relationship in liquids and glasses, particularly on the effect of temperature and history. However, because of the highly multi-dimensional nature of the PEL it is hard to determine, or even visualize, the actual details of the energy landscape. In this article we introduce a modified concept of the local energy landscape (LEL) which is limited in phase space, and demonstrate its usefulness using molecular dynamics simulation on a simple liquid at high temperatures. The local energy landscape is given as a function of the local coordination number, the number of the nearest neighbor atoms. The excitations in the LEL corresponds to the so-called beta-relaxation process. The LEL offers a simple but useful starting point to discuss complex phenomena in liquids and glasses.

We use polarized inelastic neutron scattering (INS) to study spin excitations in superconducting NaFe0.985Co0.015As (C15) with static antiferromagnetic (AF) order along the a-axis of the orthorhombic structure and NaFe0.935Co0.045As (C45) without AF order. In previous unpolarized INS work, spin excitations in C15 were found to have a dispersive sharp resonance near Er1=3.25 meV and a broad dispersionless mode at Er2=6 meV. Our neutron polarization analysis reveals that the dispersive resonance in C15 is highly anisotropic and polarized along the a- and c-axis, while the dispersionless mode is isotropic similar to that of C45. Since the a-axis polarized spin excitations of the anisotropic resonance appear below Tc, our data suggests that the itinerant electrons contributing to the magnetism are also coupled to the superconductivity., Comment: PRB(R), 2014

A novel Einstein relation (fractional Einstein relation, FER) for the electric conduction in non-crystalline semiconductors is presented. FER and the generalized Einstein relation (GER) [Phys. Rev. E 8, 1296 (1998)] are compared to the result of the Monte Carlo (MC) simulation, and is confirmed that FER exhibits better agreement than GER. The cruial feature of FER is that it reflects the violation of the detailed balance in the coarse-grained hopping process, while it is preserved in the original Einstein relation or GER., Comment: 5 pages, 3 figures

The dynamics of soft colloids in solutions is characterized by internal collective motion as well as center-of-mass diffusion. Using neutron scattering we demonstrate that the competition between the relaxation processes associated with these two degrees of freedom results in strong dependence of dynamics and structure on colloid concentration, c, even well below the overlap concentration c*. We show that concurrent with increasing inter-particle collisions, substantial structural dehydration and slowing-down of internal dynamics occur before geometrically defined colloidal overlap develops. While previous experiments have shown that the average size of soft colloids changes very little below c*, we find a marked change in both the internal structure and internal dynamics with concentration. The competition between these two relaxation processes gives rise to a new dynamically-defined dilute threshold concentration well below c*., Comment: 5 pages, 3 figures in the manuscript; 17 pages, 8 figures and 3 tables in the supplementary material

The ferroelectric (FE) control of electronic transport is one of the emerging technologies in oxide heterostructures. Many previous studies in FE tunnel junctions (FTJs) exploited solely the differences in the electrostatic potential across the FTJs that are induced by changes in the FE polarization direction. Here, we show that in practice the junction current ratios between the two polarization states can be further enhanced by the electrostatic modification in the correlated electron oxide electrodes, and that FTJs with nanometer thin layers can effectively produce a considerably large electroresistance ratio at room temperature. To understand these surprising results, we employed an additional control parameter, which is related to the crossing of electronic and magnetic phase boundaries of the correlated electron oxide. The FE-induced phase modulation at the heterointerface ultimately results in an enhanced electroresistance effect. Our study highlights that the strong coupling between degrees of freedom across heterointerfaces could yield versatile and novel applications in oxide electronics., Comment: 23 pages, 5 figures, 1 supporting information

We use inelastic neutron scattering to show that superconductivity in electron-underdoped NaFe0.985Co0.015As induces a dispersive sharp resonance near Er1 = 3:25 meV and a broad dis- persionless mode at Er2 = 6 meV. However, similar measurements on overdoped superconducting NaFe0:955Co0:045As find only a single sharp resonance at Er = 7 meV. We connect these results with the observations of angle-resolved photoemission spectroscopy that the superconducting gaps in the electron Fermi pockets are anisotropic in the underdoped material but become isotropic in the overdoped case. Our analysis indicates that both the double neutron spin resonances and gap anisotropy originate from the orbital dependence of the superconducting pairing in the iron pnic- tides. Our discovery also shows the importance of the inelastic neutron scattering in detecting the multiorbital superconducting gap structures of iron pnictides.

DC electric field effect on the anomalous exponent of the hopping conduction in the disorder model is investigated. First, we explain the model and derive an analytical expression of the effective waiting time for the general case. We show that the exponent depends on the external field. Then we focus on a one-dimensional system in order to illustrate the features of the anomalous exponent. We derive approximate expressions of the anomalous exponent of the system analytically. For the case of a weak field, the anomalous exponent is consistent with that of diffusive systems. This is consistent with the treatments of Barkai et al. [Phys. Rev. E {\bf 63}, 046118 (2001)] and our result supports their theory. On the other hand, for the case of a strong field and a strong disorder, the time evolution of the exponent clearly differs from that in the weak field. The exponent is consistent with the well-known expression of the anomalous exponent in the Multiple Trapping Model at mesoscopic time scales. In the long time limit, a transition of the anomalous exponent to the same value of the weak field occurs. For the case of a strong field and a weak disorder, the exponent is equal to 1 and thus the diffusion is normal. These findings are verified by the Monte Carlo simulation., Comment: 14 pages, 7 figures

We use polarized inelastic neutron scattering (INS) to study spin excitations of optimally hole-doped superconductor Ba$_{0.67}$K$_{0.33}$Fe$_2$As$_{2}$ ($T_c=38$ K). In the normal state, the imaginary part of the dynamic susceptibility, $\chi^{\prime\prime}(Q,\omega)$, shows magnetic anisotropy for energies below $\sim$7 meV with c-axis polarized spin excitations larger than that of the in-plane component. Upon entering into the superconducting state, previous unpolarized INS experiments have shown that spin gaps at $\sim$5 and 0.75 meV open at wave vectors $Q=(0.5,0.5,0)$ and $(0.5,0.5,1)$, respectively, with a broad neutron spin resonance at $E_r=15$ meV. Our neutron polarization analysis reveals that the large difference in spin gaps is purely due to different spin gaps in the c-axis and in-plane polarized spin excitations, resulting resonance with different energy widths for the c-axis and in-plane spin excitations. The observation of spin anisotropy in both opitmally electron and hole-doped BaFe$_2$As$_2$ is due to their proximity to the AF ordered BaFe$_2$As$_2$ where spin anisotropy exists below $T_N$., Comment: 5 pages, 4 figures

We fabricated ultrathin ferroelectric/correlated electron oxide heterostructures composed of the ferroelectric Pb(Zr0.2Ti0.8)O3 and the correlated electron oxide (CEO) La0.8Sr0.2MnO3 on SrTiO3 substrates by pulsed laser epitaxy. The hole accumulation in the ultrathin CEO layer was substantially modified by heterostructuring with the ferroelectric layer, resulting in an insulator-metal transition. In particular, our thickness dependent study showed that drastic changes in transport and magnetic properties were strongly coupled to the modulation of charge carriers by ferroelectric field effect, which was confined to the vicinity of the interface. Thus, our results provide crucial evidence that strong ferroelectric field effect control can be achieved in ultrathin (10 nm) heterostructures, yielding at least a 100,000-fold change in resistivity.

Atomic correlations in a simple liquid in steady-state flow under shear stress were studied by molecular dynamics simulation. The local atomic level strain was determined through the anisotropic pair-density function (PDF). The atomic level strain has a limited spatial extension whose range is dependent on the strain rate and extrapolates to zero at the critical strain rate. A failure event is identified with altering the local topology of atomic connectivity by exchanging bonds among neighboring atoms.

We present a shear-transformation-zone (STZ) theoretical analysis of molecular-dynamics simulations of a rapidly sheared metallic glass. These simulations are especially revealing because, although they are limited to high strain rates, they span temperatures ranging from well below to well above the glass transition. With one important discrepancy, the STZ theory reproduces the simulation data, including the way in which those data can be made to collapse onto simple curves by a scaling transformation. The STZ analysis implies that the system's behavior at high strain rates is controlled primarily by effective-temperature thermodynamics, as opposed to system-specific details of the molecular interactions. The discrepancy between theory and simulations occurs at the lower strain rates for temperatures near the glass transition. We argue that this discrepancy can be resolved by the same multi-species generalization of STZ theory that has been proposed recently for understanding frequency-dependent viscoelastic responses, Stokes-Einstein violations, and stretched-exponential relaxation in equilibrated glassy materials., Comment: 9 pages, 6 figures

Space-time dependence of the anomalous exponent of electric transport in the disorder model is presented. We show that the anomalous exponent depends on time, according to the time-evolution of the number of the effective neighbouring sites. Transition from subdiffusive to normal transport at long-enough time is recovered. The above result indicates that the spatial structure, specifically the network structure, of the hopping sites might be a novel element which determines the anomalous exponent. This leads to the feature that the scaling property of the electric transport to time is insensitive to other elements, such as the distance of the sites or the spatial dimension of the system. These findings are verified by means of Monte Carlo simulation. The relation of the result to the conventional knowledge of the Multiple Trapping Model is shown by deriving it as a special case of the disorder model., Comment: 8 pages, 3 figures, accepted for publication in J. Phys. A: Math. Theor

We use inelastic neutron scattering to show that the spin waves in the iron chalcogenide Fe$_{1.05}$Te display novel dispersion clearly different from those in the related iron pnictide systems. By fitting the spin waves to a Heisenberg Hamiltonian, we extract magnetic exchange couplings that are dramatically different from both predictions by density functional calculations and measurements on the iron pnictide CaFe$_2$As$_2$. While the nearest-neighbor exchange couplings in CaFe$_2$As$_2$ and Fe$_{1.05}$Te are quite different, their next-nearest-neighbor exchange couplings are similar. These results suggest that superconductivity in the pnictides and chalcogenides share a common magnetic origin that is intimately associated with the next-nearest-neighbor magnetic coupling between the irons., Comment: Includes supplementary information as appendices

Spinor and twistor formulations of tensionless bosonic strings in 4-dimensional Minkowski space are constructed. We begin with a first-order action that is equivalent to the Nambu-Goto action in the tensionful case and that leads to a spinorial action in the tensionless case. From this spinorial action, we find an alternative spinorial action useful for constructing a simple twistor formulation of tensionless strings. The twistor formulation is steadily constructed in accordance with a fundamental concept of twistor theory. We investigate local internal symmetries inherent in the twistorial action for a tensionless string and carry out some classical analyses of the tensionless string expressed in a twistorial form., Comment: 30 pages, no figures, minor corrections, a footnote added, published version

Bulk magnetic order in two dimensional La4Ni3O8 nickelate with Ni1+/Ni2+ (d9/d8), isoelectronic with superconducting cuprates is demonstrated experimentally and theoretically. Magnetization, specific heat and 139La NMR evidence a transition at 105 K to an antiferromagnetic state. Theoretical calculations by DFT relate the transition to a nesting instability of the Fermi surface with ordering wave-vector Q = [1/3, 1/3, 0].

We use polarized inelastic neutron scattering to show that the neutron spin resonance below $T_c$ in superconducting BaFe$_{1.9}$Ni$_{0.1}$As$_2$ ($T_c=20$ K) is purely magnetic in origin. Our analysis further reveals that the resonance peak near 7~meV only occurs for the planar response. This challenges the common perception that the spin resonance in the pnictides is an isotropic triplet excited state of the singlet Cooper pairs, as our results imply that only the $S_{001}=\pm1$ components of the triplet are involved.