Two-dimensional overdamped fluctuations of the soft perovskite lattice in CsPbBr3.

Lead halide perovskites exhibit structural instabilities and large atomic fluctuations thought to impact their optical and thermal properties, yet detailed structural and temporal correlations of their atomic motions remain poorly understood. Here, these correlations are resolved in CsPbBr3 crystals using momentum-resolved neutron and X-ray scattering measurements as a function of temperature, complemented with first-principles simulations. We uncover a striking network of diffuse scattering rods, arising from the liquid-like damping of low-energy Br-dominated phonons, reproduced in our simulations of the anharmonic phonon self-energy. These overdamped modes cover a continuum of wave vectors along the edges of the cubic Brillouin zone, corresponding to two-dimensional sheets of correlated rotations in real space, and could represent precursors to proposed two-dimensional polarons. Further, these motions directly impact the electronic gap edge states, linking soft anharmonic lattice dynamics and optoelectronic properties. These results provide insights into the highly unusual atomic dynamics of halide perovskites, relevant to further optimization of their optical and thermal properties.

Phason-Dominated Thermal Transport in Fresnoite.

Fast-propagating waves in the phase of incommensurate structures, called phasons, have long been argued to enhance thermal transport. Although supersonic phason velocities have been observed, the lifetimes, from which mean free paths can be determined, have not been resolved. Using inelastic neutron scattering and thermal conductivity measurements, we establish that phasons in piezoelectric fresnoite make a major contribution to thermal conductivity by propagating with higher group velocities and longer mean free paths than phonons. The phason contribution to thermal conductivity is maximum near room temperature, where it is the single largest contributing degree of freedom.

Nuclear quantum effect with pure anharmonicity and the anomalous thermal expansion of silicon.

Despite the widespread use of silicon in modern technology, its peculiar thermal expansion is not well understood. Adapting harmonic phonons to the specific volume at temperature, the quasiharmonic approximation, has become accepted for simulating the thermal expansion, but has given ambiguous interpretations for microscopic mechanisms. To test atomistic mechanisms, we performed inelastic neutron scattering experiments from 100 K to 1,500 K on a single crystal of silicon to measure the changes in phonon frequencies. Our state-of-the-art ab initio calculations, which fully account for phonon anharmonicity and nuclear quantum effects, reproduced the measured shifts of individual phonons with temperature, whereas quasiharmonic shifts were mostly of the wrong sign. Surprisingly, the accepted quasiharmonic model was found to predict the thermal expansion owing to a large cancellation of contributions from individual phonons.

Anharmonic Origin of the Giant Thermal Expansion of NaBr.

All phonons in a single crystal of NaBr are measured by inelastic neutron scattering at temperatures of 10, 300, and 700 K. Even at 300 K, the phonons, especially the longitudinal-optical phonons, show large shifts in frequencies and show large broadenings in energy owing to anharmonicity. Ab initio computations are first performed with the quasiharmonic approximation (QHA) in which the phonon frequencies depend only on V and on T only insofar as it alters V by thermal expansion. This QHA is an unqualified failure for predicting the temperature dependence of phonon frequencies, even 300 K, and the thermal expansion is in error by a factor of 4. Ab initio computations that include both anharmonicity and quasiharmonicity successfully predict both the temperature dependence of phonons and the large thermal expansion of NaBr. The frequencies of longitudinal-optical phonon modes decrease significantly with temperature owing to the real part of the phonon self-energy from explicit anharmonicity originating from the cubic anharmonicity of nearest-neighbor NaBr bonds. Anharmonicity is not a correction to the QHA predictions of thermal expansion and thermal phonon shifts but dominates the behavior.

Observation of High-Frequency Transverse Phonons in Metallic Glasses.

Using inelastic neutron scattering and molecular dynamics simulations on a model Zr-Cu-Al metallic glass, we show that transverse phonons persist well into the high-frequency regime, and can be detected at large momentum transfer. Furthermore, the apparent peak width of the transverse phonons was found to follow the static structure factor. The one-to-one correspondence, which was demonstrated for both Zr-Cu-Al metallic glass and a three-dimensional Lennard-Jones model glass, suggests a universal correlation between the phonon dynamics and the underlying disordered structure. This remarkable correlation, not found for longitudinal phonons, underscores the key role that transverse phonons hold for understanding the structure-dynamics relationship in disordered materials.

Experimental determination of the temperature-dependent Van Hove function in a Zr80Pt20 liquid.

Even though the viscosity is one of the most fundamental properties of liquids, the connection with the atomic structure of the liquid has proven elusive. By combining inelastic neutron scattering with the electrostatic levitation technique, the time-dependent pair-distribution function (i.e., the Van Hove function) has been determined for liquid Zr80Pt20. We show that the decay time of the first peak of the Van Hove function is directly related to the Maxwell relaxation time of the liquid, which is proportional to the shear viscosity. This result demonstrates that the local dynamics for increasing or decreasing the coordination number of local clusters by one determines the viscosity at high temperature, supporting earlier predictions from molecular dynamics simulations.

Coexistence of Ferromagnetic and Stripe Antiferromagnetic Spin Fluctuations in SrCo_{2}As_{2}.

We use inelastic neutron scattering to study energy and wave vector dependence of spin fluctuations in SrCo_{2}As_{2}, derived from SrFe_{2-x}Co_{x}As_{2} iron pnictide superconductors. Our data reveal the coexistence of antiferromagnetic (AF) and ferromagnetic (FM) spin fluctuations at wave vectors Q_{AF}=(1,0) and Q_{FM}=(0,0)/(2,0), respectively. By comparing neutron scattering results with those of dynamic mean field theory calculation and angle-resolved photoemission spectroscopy experiments, we conclude that both AF and FM spin fluctuations in SrCo_{2}As_{2} are closely associated with a flatband of the e_{g} orbitals near the Fermi level, different from the t_{2g} orbitals in superconducting SrFe_{2-x}Co_{x}As_{2}. Therefore, Co substitution in SrFe_{2-x}Co_{x}As_{2} induces a t_{2g} to e_{g} orbital switching, and is responsible for FM spin fluctuations detrimental to the singlet pairing superconductivity.

Stabilization of Polar Nanoregions in Pb-free Ferroelectrics.

The formation of polar nanoregions through solid-solution additions is known to enhance significantly the functional properties of ferroelectric materials. Despite considerable progress in characterizing the microscopic behavior of polar nanoregions (PNR), understanding their real-space atomic structure and dynamics of their formation remains a considerable challenge. Here, using the method of dynamic pair distribution function, we provide direct insights into the role of solid-solution additions towards the stabilization of polar nanoregions in the Pb-free ferroelectric of Ba(Zr,Ti)O_{3}. It is shown that for an optimum level of substitution of Ti by larger Zr ions, the dynamics of atomic displacements for ferroelectric polarization are slowed sufficiently below THz frequencies, which leads to increased local correlation among dipoles within PNRs. The dynamic pair distribution function technique demonstrates a unique capability to obtain insights into locally correlated atomic dynamics in disordered materials, including new Pb-free ferroelectrics, which is necessary to understand and control their functional properties.

Glassy Phonon Heralds a Strain Glass State in a Shape Memory Alloy.

Shape memory strain glasses are frustrated ferroelastic materials with glasslike slow relaxation and nanodomains. It is possible to change a NiCoMnIn Heusler alloy from a martensitically transforming alloy to a nontransforming strain glass by annealing, but minimal differences are evident in the short- or long-range order above the transition temperature-although there is a structural relaxation and a 0.18% lattice expansion in the annealed sample. Using neutron scattering we find glasslike phonon damping in the strain glass but not the transforming alloy at temperatures well above the transition. Damping occurs in the mode with displacements matching the martensitic transformation. With support from first-principles calculations, we argue that the strain glass originates not with transformation strain pinning but with a disruption of the underlying electronic instability when disorder resonance states cross the Fermi level.

Effective One-Dimensional Coupling in the Highly Frustrated Square-Lattice Itinerant Magnet CaCo_{2-y}As_{2}.

Inelastic neutron scattering measurements on the itinerant antiferromagnet CaCo_{2-y}As_{2} at a temperature of 8 K reveal two orthogonal planes of scattering perpendicular to the Co square lattice in reciprocal space, demonstrating the presence of effective one-dimensional spin interactions. These results are shown to arise from near-perfect bond frustration within the J_{1}-J_{2} Heisenberg model on a square lattice with ferromagnetic J_{1} and hence indicate that the extensive previous experimental and theoretical study of the J_{1}-J_{2} Heisenberg model on local-moment square spin lattices should be expanded to include itinerant spin systems.

Hourglass Dispersion and Resonance of Magnetic Excitations in the Superconducting State of the Single-Layer Cuprate HgBa_{2}CuO_{4+δ} Near Optimal Doping.

We use neutron scattering to study magnetic excitations near the antiferromagnetic wave vector in the underdoped single-layer cuprate HgBa_{2}CuO_{4+δ} (superconducting transition temperature T_{c}≈88 K, pseudogap temperature T^{*}≈220 K). The response is distinctly enhanced below T^{*} and exhibits a Y-shaped dispersion in the pseudogap state, whereas the superconducting state features an X-shaped (hourglass) dispersion and a further resonancelike enhancement. A large spin gap of about 40 meV is observed in both states. This phenomenology is reminiscent of that exhibited by bilayer cuprates. The resonance spectral weight, irrespective of doping and compound, scales linearly with the putative binding energy of a spin exciton described by an itinerant-spin formalism.

Thermally Driven Electronic Topological Transition in FeTi.

Ab initio molecular dynamics, supported by inelastic neutron scattering and nuclear resonant inelastic x-ray scattering, showed an anomalous thermal softening of the M_{5}^{-} phonon mode in B2-ordered FeTi that could not be explained by phonon-phonon interactions or electron-phonon interactions calculated at low temperatures. A computational investigation showed that the Fermi surface undergoes a novel thermally driven electronic topological transition, in which new features of the Fermi surface arise at elevated temperatures. The thermally induced electronic topological transition causes an increased electronic screening for the atom displacements in the M_{5}^{-} phonon mode and an adiabatic electron-phonon interaction with an unusual temperature dependence.

Orbital Selective Spin Excitations and their Impact on Superconductivity of LiFe_{1-x}Co_{x}As.

We use neutron scattering to study spin excitations in single crystals of LiFe_{0.88}Co_{0.12}As, which is located near the boundary of the superconducting phase of LiFe_{1-x}Co_{x}As and exhibits non-Fermi-liquid behavior indicative of a quantum critical point. By comparing spin excitations of LiFe_{0.88}Co_{0.12}As with a combined density functional theory and dynamical mean field theory calculation, we conclude that wave-vector correlated low energy spin excitations are mostly from the d_{xy} orbitals, while high-energy spin excitations arise from the d_{yz} and d_{xz} orbitals. Unlike most iron pnictides, the strong orbital selective spin excitations in the LiFeAs family cannot be described by an anisotropic Heisenberg Hamiltonian. While the evolution of low-energy spin excitations of LiFe_{1-x}Co_{x}As is consistent with the electron-hole Fermi surface nesting conditions for the d_{xy} orbital, the reduced superconductivity in LiFe_{0.88}Co_{0.12}As suggests that Fermi surface nesting conditions for the d_{yz} and d_{xz} orbitals are also important for superconductivity in iron pnictides.

Evidence for a common physical origin of the Landau and BEC theories of superfluidity.

There are two renowned theories of superfluidity in liquid (4)He, quite different and each with specific domains of application. In the first, the Landau theory, superflow follows from the existence of a well-defined collective mode supported by dense liquid (4)He, the phonon-roton mode. In the second, superflow is a manifestation of Bose-Einstein condensation (BEC) and phase coherence in the liquid. We present combined measurements of superfluidity, BEC and phonon-roton (P-R) modes in liquid (4)He confined in the porous medium MCM-41. The results integrate the two theories by showing that well-defined P-R modes exist where there is BEC. The two are common properties of a Bose condensed liquid and either can be used as a basis of a theory of superfluidity. In addition, the confinement and disorder suppresses the critical temperature for superfluidity, Tc, below that for BEC creating a localized BEC "phase" consisting of islands of BEC and P-R modes. This phase is much like the pseudogap phase in the cuprate superconductors.

Molecular quantum magnetism in LiZn2Mo3O8.

Inelastic neutron scattering at low temperatures T≤30 K from a powder of LiZn2Mo3O8 demonstrates this triangular-lattice antiferromagnet hosts collective magnetic excitations from spin-1/2 Mo3O13 molecules. Apparently gapless (Δ<0.2 meV) and extending at least up to 2.5 meV, the low-energy magnetic scattering cross section is surprisingly broad in momentum space and involves one-third of the spins present above 100 K. The data are compatible with the presence of valence bonds involving nearest-neighbor and next-nearest-neighbor spins forming a disordered or dynamic state.

Neutron scattering measurements of spatially anisotropic magnetic exchange interactions in semiconducting K0.85 Fe1.54Se2 (TN = 280 K.

We use neutron scattering to study the spin excitations associated with the stripe antiferromagnetic order in semiconducting K(0.85)Fe(1.54)Se(2) (T(N) = 280 K). We show that the spin-wave spectra can be accurately described by an effective Heisenberg Hamiltonian with highly anisotropic inplane couplings at T = 5 K. At high temperature (T = 300 K) above T(N), short-range magnetic correlation with anisotropic correlation lengths are observed. Our results suggest that, despite the dramatic difference in the Fermi surface topology, the inplane anisotropic magnetic couplings are a fundamental property of the iron-based compounds; this implies that their antiferromagnetism may originate from local strong correlation effects rather than weak coupling Fermi surface nesting.

Chiral and flat-band magnetic quasiparticles in ferromagnetic and metallic kagome layers.

Magnetic kagome metals are a promising platform to develop unique quantum transport and optical phenomena caused by the interplay between topological electronic bands, strong correlations, and magnetic order. This interplay may result in exotic quasiparticles that describe the coupled electronic and spin excitations on the frustrated kagome lattice. Here, we observe novel elementary magnetic excitations within the ferromagnetic Mn kagome layers in TbMn6Sn6 using inelastic neutron scattering. We observe sharp, collective acoustic magnons and identify flat-band magnons that are localized to a hexagonal plaquette due to the special geometry of the kagome layer. Surprisingly, we observe another type of elementary magnetic excitation; a chiral magnetic quasiparticle that is also localized on a hexagonal plaquette. The short lifetime of localized flat-band and chiral quasiparticles suggest that they are hybrid excitations that decay into electronic states.

Inelastic neutron scattering study of a nonmagnetic collapsed tetragonal phase in nonsuperconducting CaFe2As2: evidence of the impact of spin fluctuations on superconductivity in the iron-arsenide compounds.

The relationship between antiferromagnetic spin fluctuations and superconductivity has become a central topic of research in studies of superconductivity in the iron pnictides. We present unambiguous evidence of the absence of magnetic fluctuations in the nonsuperconducting collapsed tetragonal phase of CaFe2As2 via inelastic neutron scattering time-of-flight data, which is consistent with the view that spin fluctuations are a necessary ingredient for unconventional superconductivity in the iron pnictides. We demonstrate that the collapsed tetragonal phase of CaFe2As2 is nonmagnetic, and discuss this result in light of recent reports of high-temperature superconductivity in the collapsed tetragonal phase of closely related compounds.

Stripe antiferromagnetic spin fluctuations in SrCo2As2.

Inelastic neutron scattering measurements of paramagnetic SrCo2As2 at T=5 K reveal antiferromagnetic (AFM) spin fluctuations that are peaked at a wave vector of Q(AFM)=(1/2,1/2,1) and possess a large energy scale. These stripe spin fluctuations are similar to those found in AFe2As2 compounds, where spin-density wave AFM is driven by Fermi surface nesting between electron and hole pockets separated by Q(AFM). SrCo2As2 has a more complex Fermi surface and band-structure calculations indicate a potential instability toward either a ferromagnetic or stripe AFM ground state. The results suggest that stripe AFM magnetism is a general feature of both iron and cobalt-based arsenides and the search for spin fluctuation-induced unconventional superconductivity should be expanded to include cobalt-based compounds.

Orbital character of the spin-reorientation transition in TbMn6Sn6.

Ferromagnetic (FM) order in a two-dimensional kagome layer is predicted to generate a topological Chern insulator without an applied magnetic field. The Chern gap is largest when spin moments point perpendicular to the kagome layer, enabling the capability to switch topological transport properties, such as the quantum anomalous Hall effect, by controlling the spin orientation. In TbMn6Sn6, the uniaxial magnetic anisotropy of the Tb3+ ion is effective at generating the Chern state within the FM Mn kagome layers while a spin-reorientation (SR) transition to easy-plane order above TSR = 310 K provides a mechanism for switching. Here, we use inelastic neutron scattering to provide key insights into the fundamental nature of the SR transition. The observation of two Tb excitations, which are split by the magnetic anisotropy energy, indicates an effective two-state orbital character for the Tb ion, with a uniaxial ground state and an isotropic excited state. The simultaneous observation of both modes below TSR confirms that orbital fluctuations are slow on magnetic and electronic time scales < ps and act as a spatially-random orbital alloy. A thermally-driven critical concentration of isotropic Tb ions triggers the SR transition.