Topological magnons driven by the Dzyaloshinskii-Moriya interaction in the centrosymmetric ferromagnet Mn5Ge3.

The phase of the quantum-mechanical wave function can encode a topological structure with wide-ranging physical consequences, such as anomalous transport effects and the existence of edge states robust against perturbations. While this has been exhaustively demonstrated for electrons, properties associated with the elementary quasiparticles in magnetic materials are still underexplored. Here, we show theoretically and via inelastic neutron scattering experiments that the bulk ferromagnet Mn5Ge3 hosts gapped topological Dirac magnons. Although inversion symmetry prohibits a net Dzyaloshinskii-Moriya interaction in the unit cell, it is locally allowed and is responsible for the gap opening in the magnon spectrum. This gap is predicted and experimentally verified to close by rotating the magnetization away from the c-axis with an applied magnetic field. Hence, Mn5Ge3 realizes a gapped Dirac magnon material in three dimensions. Its tunability by chemical doping or by thin film nanostructuring defines an exciting new platform to explore and design topological magnons. More generally, our experimental route to verify and control the topological character of the magnons is applicable to bulk centrosymmetric hexagonal materials, which calls for systematic investigation.

Combined Arrhenius-Merz Law Describing Domain Relaxation in Type-II Multiferroics.

Electric fields were applied to multiferroic TbMnO_{3} single crystals to control the chiral domains, and the domain relaxation was studied over 8 decades in time by means of polarized neutron scattering. A surprisingly simple combination of an activation law and the Merz law describes the relaxation times in a wide range of electric field and temperature with just two parameters, an activation-field constant and a characteristic time representing the fastest possible inversion. Over the large part of field and temperature values corresponding to almost 6 orders of magnitude in time, multiferroic domain inversion is thus dominated by a single process, the domain wall motion. Only when approaching the multiferroic transition other mechanisms yield an accelerated inversion.

Charge disproportionation and nano phase separation in [Formula: see text].

We have successfully grown centimeter-sized layered [Formula: see text] single crystals under high oxygen pressures of 120-150 bar by the floating zone technique. This enabled us to perform neutron scattering experiments where we observe close to quarter-integer magnetic peaks below [Formula: see text] that are accompanied by steep upwards dispersing spin excitations. Within the high-frequency Ni-O bond stretching phonon dispersion, a softening at the propagation vector for a checkerboard modulation can be observed. We were able to simulate the magnetic excitation spectra using a model that includes two essential ingredients, namely checkerboard charge disproportionation and nano phase separation. The results thus suggest that charge disproportionation is preferred instead of a Jahn-Teller distortion even for this layered [Formula: see text] system.

Coexistence of Ferromagnetic and Stripe-Type Antiferromagnetic Spin Fluctuations in YFe_{2}Ge_{2}.

We report neutron scattering measurements of single-crystalline YFe_{2}Ge_{2} in the normal state, which has the same crystal structure as the 122 family of iron pnictide superconductors. YFe_{2}Ge_{2} does not exhibit long-range magnetic order but exhibits strong spin fluctuations. Like the iron pnictides, YFe_{2}Ge_{2} displays anisotropic stripe-type antiferromagnetic spin fluctuations at (π, 0, π). More interesting, however, is the observation of strong spin fluctuations at the in-plane ferromagnetic wave vector (0, 0, π). These ferromagnetic spin fluctuations are isotropic in the (H, K) plane, whose intensity exceeds that of stripe spin fluctuations. Both the ferromagnetic and stripe spin fluctuations remain gapless down to the lowest measured energies. Our results naturally explain the absence of magnetic order in YFe_{2}Ge_{2} and also imply that the ferromagnetic correlations may be a key ingredient for iron-based materials.

Common acoustic phonon lifetimes in inorganic and hybrid lead halide perovskites.

The acoustic phonons in the organic-inorganic lead halide perovskites have been reported to have anomalously short lifetimes over a large part of the Brillouin zone. The resulting shortened mean free paths of the phonons have been implicated as the origin of the low thermal conductivity. We apply neutron spectroscopy to show that the same acoustic phonon energy linewidth broadening (corresponding to shortened lifetimes) occurs in the fully inorganic CsPbBr3 by comparing the results on the organic-inorganic CH3NH3PbCl3. We investigate the critical dynamics near the three zone boundaries of the cubic P m 3 ¯ m Brillouin zone of CsPbBr3 and find energy and momentum broadened dynamics at momentum points where the Cs-site (A-site) motions contribute to the cross section. Neutron diffraction is used to confirm that both the Cs and Br sites have unusually large thermal displacements with an anisotropy that mirrors the low temperature structural distortions. The presence of an organic molecule is not necessary to disrupt the low-energy acoustic phonons at momentum transfers located away from the zone center in the lead halide perovskites and such damping may be driven by the large displacements or possibly disorder on the A site.

From Ising Resonant Fluctuations to Static Uniaxial Order in Antiferromagnetic and Weakly Superconducting CeCo(In_{1-x}Hg_{x})_{5}(x=0.01).

CeCo(In_{0.990}Hg_{0.010})_{5} is a charge doped variant of the d-wave CoCoIn_{5} superconductor with coexistent antiferromagnetic and superconducting transitions occurring at T_{N}=3.4 and T_{c}=1.4 K, respectively. We use neutron diffraction and spectroscopy to show that the magnetic resonant fluctuations present in the parent superconducting phase are replaced by collinear c-axis magnetic order with three-dimensional Ising critical fluctuations. No low-energy transverse spin fluctuations are observable in this doping-induced antiferromagnetic phase and the dynamic resonant spectral weight predominately shifts to the elastic channel. Static (τ>0.2 ns) collinear Ising order is proximate to superconductivity in CeCoIn_{5} and is stabilized through hole doping with Hg.

Spin Fluctuations Drive the Inverse Magnetocaloric Effect in Mn_{5}Si_{3}.

Inelastic neutron scattering measurements are performed on single crystals of the antiferromagnetic compound Mn_{5}Si_{3} in order to investigate the relation between the spin dynamics and the magnetothermodynamics properties. It is shown that, among the two stable antiferromagnetic phases of this compound, the high temperature one has an unusual magnetic excitation spectrum where propagative spin waves and diffuse spin fluctuations coexist. Moreover, it is evidenced that the inverse magnetocaloric effect of Mn_{5}Si_{3}, the cooling by adiabatic magnetization, is associated with field induced spin fluctuations.

Lifetime-shortened acoustic phonons and static order at the Brillouin zone boundary in the organic-inorganic perovskite CH3NH3PbCl3.

Lead halide hybrid perovskites consist of an inorganic framework hosting a molecular cation located in the interstitial space. These compounds have been extensively studied as they have been identified as promising materials for photovoltaic applications with the interaction between the molecular cation and the inorganic framework implicated as influential for the electronic properties. CH3NH3PbCl3 undergoes two structural transitions from a high temperature cubic unit cell to a tetragonal phase at 177 K and then a subsequent orthorhombic transition at 170 K. We have measured the low-frequency lattice dynamics using neutron spectroscopy and observe an energy broadening in the acoustic phonon linewidth towards the high-symmetry point Q X = ( 2 , 1 2 , 0 ) when approaching the transitions. Concomitant with these zone boundary anomalies is a hardening of the entire acoustic phonon branch measured in the q → 0 limit near the (2, 0, 0) Bragg position with decreasing temperature. Measurements of the elastic scattering at the Brillouin zone edges Q X = ( 2 , 1 2 , 0 ) , Q M = ( 3 2 , 1 2 , 0 ) , and Q R = ( 3 2 , 3 2 , 5 2 ) show Bragg peaks appearing below these structural transitions. Based on selection rules of neutron scattering, we suggest that the higher 177 K transition is displacive with a distortion of the local octahedral environment and the lower transition is a rigid tilt transition of the octahedra. We do not observe any critical broadening in energy or momentum, beyond resolution, of these peaks near the transitions. We compare these results to the critical properties reported near the structural transitions in other perovskites and particularly CsPbCl3 [Y. Fujii, S. Hoshino, Y. Yamada, and G. Shirane, Phys. Rev. B 9, 4549 (1974)]. We suggest that the simultaneous onset of static resolution-limited Bragg peaks at the zone boundaries and the changes in acoustic phonon energies near the zone center is evidence of a coupling between the inorganic framework and the molecular cation. The results also highlight the importance of displacive transitions in organic-inorganic hybrid perovskites.

Control of Chiral Magnetism Through Electric Fields in Multiferroic Compounds above the Long-Range Multiferroic Transition.

Polarized neutron scattering experiments reveal that type-II multiferroics allow for controlling the spin chirality by external electric fields even in the absence of long-range multiferroic order. In the two prototype compounds TbMnO_{3} and MnWO_{4}, chiral magnetism associated with soft overdamped electromagnons can be observed above the long-range multiferroic transition temperature T_{MF}, and it is possible to control it through an electric field. While MnWO_{4} exhibits chiral correlations only in a tiny temperature interval above T_{MF}, in TbMnO_{3} chiral magnetism can be observed over several kelvin up to the lock-in transition, which is well separated from T_{MF}.

Anisotropic resonance modes emerging in an antiferromagnetic superconducting state.

Two strong arguments in favor of magnetically driven unconventional superconductivity arise from the coexistence and closeness of superconducting and magnetically ordered phases on the one hand, and from the emergence of magnetic spin-resonance modes at the superconducting transition on the other hand. Combining these two arguments one may ask about the nature of superconducting spin-resonance modes occurring in an antiferromagnetic state. This problem can be studied in underdoped BaFe2 As2, for which the local coexistence of large moment antiferromagnetism and superconductivity is well established by local probes. However, polarized neutron scattering experiments are required to identify the nature of the resonance modes. In the normal state of Co underdoped BaFe2 As2 the antiferromagnetic order results in broad magnetic gaps opening in all three spin directions that are reminiscent of the magnetic response in the parent compound. In the superconducting state two distinct anisotropic resonance excitations emerge, but in contrast to numerous studies on optimum and over-doped BaFe2 As2 there is no isotropic resonance excitation. The two anisotropic resonance modes appearing within the antiferromagnetic phase are attributed to a band selective superconducting state, in which longitudinal magnetic excitations are gapped by antiferromagnetic order with sizable moment.

Hydrostatic pressure effects on the static magnetism in Eu(Fe0.925Co0.075)2As2.

EuFe2As2-based iron pnictides are quite interesting compounds, due to the two magnetic sublattices in them and the tunability to superconductors by chemical doping or application of external pressure. The effects of hydrostatic pressure on the static magnetism in Eu(Fe0.925Co0.075)2As2 are investigated by complementary electrical resistivity, ac magnetic susceptibility and single-crystal neutron diffraction measurements. A specific pressure-temperature (P-T) phase diagram of Eu(Fe0.925Co0.075)2As2 is established. The structural phase transition, as well as the spin-density-wave order of Fe sublattice, is suppressed gradually with increasing pressure and disappears completely above 2.0 GPa. In contrast, the magnetic order of Eu sublattice persists over the whole investigated pressure range up to 14 GPa, yet displaying a non-monotonic variation with pressure. With the increase of the hydrostatic pressure, the magnetic state of Eu evolves from the canted antiferromagnetic structure in the ground state, via a pure ferromagnetic structure under the intermediate pressure, finally to an "unconfirmed" antiferromagnetic structure under the high pressure. The strong ferromagnetism of Eu coexists with the pressure-induced superconductivity around 2 GPa. Comparisons between the P-T phase diagrams of Eu(Fe0.925Co0.075)2As2 and the parent compound EuFe2As2 were also made.

Strong interplay between stripe spin fluctuations, nematicity and superconductivity in FeSe.

In iron-based superconductors the interactions driving the nematic order (that breaks four-fold rotational symmetry in the iron plane) may also mediate the Cooper pairing. The experimental determination of these interactions, which are believed to depend on the orbital or the spin degrees of freedom, is challenging because nematic order occurs at, or slightly above, the ordering temperature of a stripe magnetic phase. Here, we study FeSe (ref. )-which exhibits a nematic (orthorhombic) phase transition at Ts = 90 K without antiferromagnetic ordering-by neutron scattering, finding substantial stripe spin fluctuations coupled with the nematicity that are enhanced abruptly on cooling through Ts. A sharp spin resonance develops in the superconducting state, whose energy (∼4 meV) is consistent with an electron-boson coupling mode revealed by scanning tunnelling spectroscopy. The magnetic spectral weight in FeSe is found to be comparable to that of the iron arsenides. Our results support recent theoretical proposals that both nematicity and superconductivity are driven by spin fluctuations.

Single to Multiquasiparticle Excitations in the Itinerant Helical Magnet CeRhIn(5).

CeRhIn(5) is an itinerant magnet where the Ce(3+) spins order in a simple helical phase. We investigate the spin excitations and observe sharp spin waves parameterized by a nearest-neighbor exchange, J(RKKY)=0.88±0.05 meV. At higher energies, the spin fluctuations are heavily damped, where single-quasiparticle excitations are replaced by a momentum- and energy-broadened continuum constrained by kinematics of energy and momentum conservation. The delicate energy balance between localized and itinerant characters results in the breakdown of the single-quasiparticle picture in CeRhIn(5).

Competing ferri- and antiferromagnetic phases in geometrically frustrated LuFe2O4.

We present a detailed study of magnetism in LuFe(2)O(4), combining magnetization measurements with neutron and soft x-ray diffraction. The magnetic phase diagram in the vicinity of T(N) involves a metamagnetic transition separating an antiferro- and a ferrimagnetic phase. For both phases the spin structure is refined by neutron diffraction. Observed diffuse magnetic scattering far above T(N) is explained in terms of near degeneracy of the magnetic phases.

Magnetic Coulomb phase in the spin ice Ho2Ti2O7.

Spin-ice materials are magnetic substances in which the spin directions map onto hydrogen positions in water ice. Their low-temperature magnetic state has been predicted to be a phase that obeys a Gauss' law and supports magnetic monopole excitations: in short, a Coulomb phase. We used polarized neutron scattering to show that the spin-ice material Ho2Ti2O7 exhibits an almost perfect Coulomb phase. Our result proves the existence of such phases in magnetic materials and strongly supports the magnetic monopole theory of spin ice.

Flop of electric polarization driven by the flop of the Mn spin cycloid in multiferroic TbMnO3.

Using in-field single-crystal neutron diffraction, we have determined the magnetic structure of TbMnO(3) in the high field P parallel a phase. We unambiguously establish that the ferroelectric polarization arises from a cycloidal Mn spin ordering, with spins rotating in the ab plane. Our results demonstrate directly that the flop of the ferroelectric polarization in TbMnO(3) with applied magnetic field is caused from the flop of the Mn cycloidal plane.

Field-induced paramagnons at the metamagnetic transition of Ca1.8Sr0.2RuO4.

The magnetic excitations in Ca1.8Sr0.2RuO4 were studied across the metamagnetic transition and as a function of temperature using inelastic neutron scattering. At low temperature and low magnetic field the magnetic response is dominated by a complex superposition of incommensurate antiferromagnetic fluctuations. Upon increasing the magnetic field across the metamagnetic transition, paramagnon and finally well-defined magnon scattering is induced, partially suppressing the incommensurate signals. The high-field phase in Ca1.8Sr0.2RuO4, therefore, has to be considered as an intrinsically ferromagnetic state stabilized by the magnetic field.

Mercaptan and dicarboxylate inhibitors of hamster dihydroorotase.

In mammals, dihydroorotase is part of a trifunctional protein, dihydroorotate synthetase, which catalyzes the first three reactions of de novo pyrimidine biosynthesis. Dihydroorotase catalyzes the formation of a peptide-like bond between the terminal ureido nitrogen and the beta-carboxyl group of N-carbamyl-L-aspartate to yield heterocyclic L-dihydroorotate. A variety of evidence suggests that dihydroorotase may have a catalytic mechanism similar to that of a zinc protease [Christopherson, R. I., & Jones, M. E. (1980) J. Biol. Chem. 255, 3358-3370]. Tight-binding inhibitors of the zinc proteases, carboxypeptidase A, thermolysin, and angiotensin-converting enzyme have been synthesized that combine structural features of the substrates with a thiol or carboxyl group in an appropriate position to coordinate a zinc atom bound at the catalytic site. We have synthesized (4R)-2-oxo-6-thioxohexahydropyrimidine-4-carboxylate (L-6-thiodihydroorotate) and have found that this analogue is a potent competitive inhibitor of dihydroorotase with a dissociation constant (Ki) in the presence of excess Zn2+ ion of 0.17 +/- 0.02 microM at pH 7.4. The potency of inhibition by L-6-thiodihydroorotate in the presence of divalent metal ions decreases in the order Zn2+ greater than Ca2+ greater than Co2+ greater than Mn2+ greater than Ni2+; L-6-thiodihydroorotate alone is less inhibitory and has a Ki of 0.85 +/- 0.14 microM. 6-Thioorotate has a Ki of 82 +/- 8 microM which decreases to 3.8 +/- 1.4 microM in the presence of Zn2+. Zn2+ alone is a moderate inhibitor of dihydroorotase and does not enhance the potency of other inhibitors.(ABSTRACT TRUNCATED AT 250 WORDS)

Metabolites of Dactylaria lutea. The structures of dactylariol and the antiprotozoal antibiotic dactylarin.

The metabolites of the predacious fungus Dactylaria lutea ROUTIEN include the anthraquinone macrosporin (2) and three hydroxylated 1,2,3,4-tetrahydro derivatives of this anthraquinone, altersolanol A (5), altersolanol B (4) and dactylariol (6). The structure and relative configuration of dactylariol are established from spectroscopic studies, and its absolute configuration is proposed as 1R, 2R, 3R by virtue of its co-occurrence with altersolanol B. Dactylarin, suggested by other authors to have the structure (1), is shown to be identical with altersolanol B (4).