The thermal conductivity of crystalline materials cannot be arbitrarily low as the intrinsic limit depends on the phonon dispersion. We used complementary strategies to suppress the contribution of the longitudinal and transverse phonons to heat transport in layered materials containing different types of intrinsic chemical interface. BiOCl and Bi2O2Se encapsulate these design principles for longitudinal and transverse modes respectively, and the bulk superlattice material Bi4O4SeCl2 combines these effects by ordering both interface types within its unit cell to reach an extremely low thermal conductivity of 0.1 W K−1 m−1 at room temperature along its stacking direction. This value comes within a factor of four of air. We demonstrated that chemical control of the spatial arrangement of distinct interfaces can synergically modify vibrational modes to minimize thermal conductivity.
Recent theoretical proposals have argued that cobaltates with edge-sharing octahedral coordination can have significant bond-dependent exchange couplings thus offering a platform in 3d ions for such physics beyond the much-explored realisations in 4d and 5d materials. Here we present high-resolution inelastic neutron scattering data within the magnetically ordered phase of the stacked honeycomb magnet CoTiO3 revealing the presence of a finite energy gap and demonstrate that this implies the presence of bond-dependent anisotropic couplings. We also show through an extensive theoretical analysis that the gap further implies the existence of a quantum order-by-disorder mechanism that, in this material, crucially involves virtual crystal field fluctuations. Our data also provide an experimental observation of a universal winding of the scattering intensity in angular scans around linear band-touching points for both magnons and dispersive spin-orbit excitons, which is directly related to the non-trivial topology of the quasiparticle wavefunction in momentum space near nodal points.
B-site ordered A2B'B''O6 double perovskites have a variety of applications as magnetic materials.Here we show that diamagnetic d 10 and d 0 B'' cations have a significant effect on the magnetic interactions in these materials. We present a neutron scattering and theoretical study of the Mn 2+ double perovskite Ba2MnTeO6 with a 4d 10 Te 6+ cation on the B''-site. It is found to be a Type I antiferromagnet with a dominant nearest-neighbor J1 interaction. In contrast, the 5d 0 W 6+ analogue Ba2MnWO6 is a Type II antiferromagnet with a significant next-nearest-neighbor J2 interaction. This is due to a d 10 /d 0 effect, where the different orbital hybridization with oxygen 2p results in different superexchange pathways. We show that d 10 B'' cations promote nearest neighbor and d 0 cations promote next-nearest-neighbor interactions. The d 10 /d 0 effect could be used to tune magnetic interactions in double perovskites.
FePS 3 is a van der Waals compound with a honeycomb lattice that is a good example of a two-dimensional antiferromagnet with Ising-like anisotropy. Neutron spectroscopy data from FePS 3 were previously analyzed using a straightforward Heisenberg Hamiltonian with a single-ion anisotropy. The analysis captured most of the elements of the data; however, some significant discrepancies remained. The discrepancies were most obvious at the Brillouin zone boundaries. The data are subsequently reanalyzed, allowing for unequal exchange between nominally equivalent nearest-neighbors, which resolves the discrepancies. The source of the unequal exchange is attributed to a biquadratic exchange term in the Hamiltonian, which most probably arises from a strong magnetolattice coupling. The new parameters show that there are features consistent with Dirac magnon nodal lines along certain Brillouin zone boundaries.
The recent discovery of topological Kondo insulating behaviour in strongly correlated electron systems has generated considerable interest in Kondo insulators both experimentally and theoretically. The Kondo semiconductors CeT 2 Al 10 (T=Fe, Ru and Os) possessing a c-f hybridization gap have received considerable attention recently because of the unexpected high magnetic ordering temperature of CeRu 2 Al 10 (T N =27 K) and CeOs 2 Al 10 (T N =28.5 K) and the Kondo insulating behaviour observed in the valence fluctuating compound CeFe 2 Al 10 with a paramagnetic ground state down to 50 mK. We are investigating this family of compounds, both in polycrystalline and single crystal form, using inelastic neutron scattering to understand the role of anisotropic c-f hybridization on the spin gap formation as well as on their magnetic properties. We have observed a clear sign of a spin gap in all three compounds from our polycrystalline study as well as the existence of a spin gap above the magnetic ordering temperature in T=Ru and Os. Our inelastic neutron scattering studies on single crystals of CeRu 2 Al 10 and CeOs 2 Al 10 revealed dispersive gapped spin wave excitations below T N . Analysis of the spin wave spectrum reveals the presence of strong anisotropic exchange, along the c-axis (or z-axis) stronger than in the ab-plane. These anisotropic exchange interactions force the magnetic moment to align along the c-axis, competing with the single ion crystal field anisotropy, which prefers moments along the a-axis. In the paramagnetic state (below 50 K) of the Kondo insulator CeFe 2 Al 10 , we have also observed dispersive gapped magnetic excitations which transform into quasi-elastic scattering on heating to 100 K. We will discuss the origin of the anisotropic hybridization gap in CeFe 2 Al 10 based on theoretical models of heavy-fermion semiconductors.
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