Ultrasensitive barocaloric material for room-temperature solid-state refrigeration.

One of the greatest obstacles to the real application of solid-state refrigeration is the huge driving fields. Here, we report a giant barocaloric effect in inorganic NH4I with reversible entropy changes of [Formula: see text] ∼71 J K-1 kg-1 around room temperature, associated with a structural phase transition. The phase transition temperature, Tt, varies dramatically with pressure at a rate of dTt/dP ∼0.79 K MPa-1, which leads to a very small saturation driving pressure of ΔP ∼40 MPa, an extremely large barocaloric strength of [Formula: see text] ∼1.78 J K-1 kg-1 MPa-1, as well as a broad temperature span of ∼41 K under 80 MPa. Comprehensive characterizations of the crystal structures and atomic dynamics by neutron scattering reveal that a strong reorientation-vibration coupling is responsible for the large pressure sensitivity of Tt. This work is expected to advance the practical application of barocaloric refrigeration.

Reducing Kapitza resistance between graphene/water interface via interfacial superlattice structure.

The control of thermal transport across solid/liquid interface has attracted great interests for efficient thermal management in the integrated devices. Based on molecular dynamics simulations, we study the effect of interfacial superlattice structure on the Kapitza resistance between graphene/water interface. Compared to the original interface, introducing interfacial superlattice structure can result in an obvious reduction of Kapitza resistance by as large as 40%, exhibiting a decreasing trend of Kapitza resistance with the decrease of superlattice period. Surprisingly, by analyzing the structure of water block and atomic vibration characteristics on both sides of the interface, we find the interfacial superlattice structure has a minor effect on the water structure and overlap in the vibrational spectrum, suggesting that the improved interfacial heat transfer is not mainly originated from the liquid block. Instead, the spectral energy density analysis reveals that phonon scattering rate in the interfacial graphene layer is significantly enhanced after superlattice decoration, giving rise to the increased thermal resistance between the interfacial graphene layer and its nearest neighboring layer. As this thermal resistance is coupled to the Kapitza resistance due to the local nature of interfacial superlattice decoration, the enhanced thermal resistance in the solid segment indirectly reduces the Kapitza resistance between graphene/water interface, which is supported by the enhancement of the spectral interfacial thermal conductance upon superlattce decoration at microscopic level. Our study uncovers the physical mechanism for controlling heat transfer across solid/liquid interface via interfacial superlattice structure, which might provide valuable insights for designing efficient thermal interfaces.

The Impact of Interlayer Rotation on Thermal Transport Across Graphene/Hexagonal Boron Nitride van der Waals Heterostructure.

Graphene/hexagonal boron nitride (h-BN) van der Waals (vdW) heterostructure has aroused great interest because of the unique Moiré pattern. In this study, we use molecular dynamics simulation to investigate the influence of the interlayer rotation angle θ on the interfacial thermal transport across graphene/h-BN heterostructure. The interfacial thermal conductance G of graphene/h-BN interface reaches 509 MW/(m2K) at 500 K without rotation, and it decreases monotonically with the increase of the rotation angle, exhibiting around 50% reduction of G with θ = 26.33°. The phonon transmission function reveals that G is dominantly contributed by the low-frequency phonons below 10 THz. Upon rotation, the surface fluctuation in the interfacial graphene layer is enhanced, and the transmission function for the low-frequency phonon is reduced with increasing θ, leading to the rotation angle-dependent G. This work uncovers the physical mechanisms for controlling interfacial thermal transport across vdW heterostructure via interlayer rotation.

Dimer rattling mode induced low thermal conductivity in an excellent acoustic conductor.

A solid with larger sound speeds usually exhibits higher lattice thermal conductivity. Here, we report an exception that CuP2 has a quite large mean sound speed of 4155 m s-1, comparable to GaAs, but single crystals show very low lattice thermal conductivity of about 4 W m-1 K-1 at room temperature, one order of magnitude smaller than GaAs. To understand such a puzzling thermal transport behavior, we have thoroughly investigated the atomic structures and lattice dynamics by combining neutron scattering techniques with first-principles simulations. This compound crystallizes in a layered structure where Cu atoms forming dimers are sandwiched in between P atomic networks. In this work, we reveal that Cu atomic dimers vibrate as a rattling mode with frequency around 11 meV, which is manifested to be remarkably anharmonic and strongly scatters acoustic phonons to achieve the low lattice thermal conductivity.

Magnetic-Field Control of Topological Electronic Response near Room Temperature in Correlated Kagome Magnets.

Strongly correlated kagome magnets are promising candidates for achieving controllable topological devices owing to the rich interplay between inherent Dirac fermions and correlation-driven magnetism. Here we report tunable local magnetism and its intriguing control of topological electronic response near room temperature in the kagome magnet Fe_{3}Sn_{2} using small angle neutron scattering, muon spin rotation, and magnetoresistivity measurement techniques. The average bulk spin direction and magnetic domain texture can be tuned effectively by small magnetic fields. Magnetoresistivity, in response, exhibits a measurable degree of anisotropic weak localization behavior, which allows the direct control of Dirac fermions with strong electron correlations. Our work points to a novel platform for manipulating emergent phenomena in strongly correlated topological materials relevant to future applications.

Disorder limits the coherent phonon transport in two-dimensional phononic crystal structures.

Recently, increasing efforts are being made to control thermal transport via coherent phonons in periodic phononic structures; however, the direct observation of coherent phonon transport is experimentally very difficult at ambient temperature, and the importance of coherent phonons to the total thermal conductivity has not been critically assessed to date. In this study, using the non-equilibrium molecular dynamics simulations, we studied coherent phonon transport in a C3N phononic crystal (CNPnC) structure at room temperature by changing the porosity. When the holes were randomly distributed to construct the disordered C3N (D-C3N) structure, the localization of the coherent phonons was revealed by the phonon transmission coefficient, phonon wave packet simulation, phonon participation ratio and spatial energy density, which led to a significant reduction in the thermal conductivity. Finally, the effects of the length, temperature and strain on the thermal conductivity of CNPnC and D-C3N have also been discussed. Our study provides a solid understanding of the coherent phonon transport behavior, which will be beneficial for phononic-related control based on coherent phonons.

Colossal barocaloric effects in plastic crystals.

Refrigeration is of vital importance for modern society-for example, for food storage and air conditioning-and 25 to 30 per cent of the world's electricity is consumed for refrigeration1. Current refrigeration technology mostly involves the conventional vapour compression cycle, but the materials used in this technology are of growing environmental concern because of their large global warming potential2. As a promising alternative, refrigeration technologies based on solid-state caloric effects have been attracting attention in recent decades3-5. However, their application is restricted by the limited performance of current caloric materials, owing to small isothermal entropy changes and large driving magnetic fields. Here we report colossal barocaloric effects (CBCEs) (barocaloric effects are cooling effects of pressure-induced phase transitions) in a class of disordered solids called plastic crystals. The obtained entropy changes in a representative plastic crystal, neopentylglycol, are about 389 joules per kilogram per kelvin near room temperature. Pressure-dependent neutron scattering measurements reveal that CBCEs in plastic crystals can be attributed to the combination of extensive molecular orientational disorder, giant compressibility and highly anharmonic lattice dynamics of these materials. Our study establishes the microscopic mechanism of CBCEs in plastic crystals and paves the way to next-generation solid-state refrigeration technologies.

Effect of boundary chain folding on thermal conductivity of lamellar amorphous polyethylene.

Thermal transport properties of amorphous polymers depend significantly on the chain morphology, and boundary chain folding is a common phenomenon in bulk or lamellar polymer materials. In this work, by using molecular dynamics simulations, we study thermal conductivity of lamellar amorphous polyethylene (LAPE) with varying chain length (L 0). For a short L 0 without boundary chain folding, thermal conductivity of LAPE is homogeneous along the chain length direction. In contrast, boundary chain folding takes place for large L 0, and the local thermal conductivity at the boundary is notably lower than that of the central region, indicating inhomogeneous thermal transport in LAPE. By analysing the chain morphology, we reveal that the boundary chain folding causes the reduction of both the orientation order parameter along the heat flow direction and the radius of gyration, leading to the reduced local thermal conductivity at the boundary. Further vibrational spectrum analysis reveals that the boundary chain folding shifts the vibrational spectrum to the lower frequency, and suppresses the transmission coefficient for both C-C vibration and C-H vibration. Our study suggests that the boundary chain folding is an important factor for polymers to achieve desirable thermal conductivity for plastic heat exchangers and electronic packaging applications.

Anisotropic Dirac Fermions in BaMnBi2 and BaZnBi2.

We investigate the electronic structure of BaMnBi2 and BaZnBi2 using angle-resolved photoemission spectroscopy and first-principles calculations. Although they share similar structural properties, we show that their electronic structure exhibit dramatic differences. A strong anisotropic Dirac dispersion is revealed in BaMnBi2 with a decreased asymmetry factor compared with other members of AMnBi2 (A = alkali earth or rare earth elements) family. In addition to the Dirac cones, multiple bands crossing the Fermi energy give rise to a complex Fermi surface topology for BaZnBi2. We further show that the strength of hybridization between Bi-p and Mn-d/Zn-s states is the main driver of the differences in electronic structure for these two related compounds.

Observation of Various and Spontaneous Magnetic Skyrmionic Bubbles at Room Temperature in a Frustrated Kagome Magnet with Uniaxial Magnetic Anisotropy.

The quest for materials hosting topologically protected skyrmionic spin textures continues to be fueled by the promise of novel devices. Although many materials have demonstrated the existence of such spin textures, major challenges remain to be addressed before devices based on magnetic skyrmions can be realized. For example, being able to create and manipulate skyrmionic spin textures at room temperature is of great importance for further technological applications because they can adapt to various external stimuli acting as information carriers in spintronic devices. Here, the first observation of skyrmionic magnetic bubbles with variable topological spin textures formed at room temperature in a frustrated kagome Fe3 Sn2 magnet with uniaxial magnetic anisotropy is reported. The magnetization dynamics are investigated using in situ Lorentz transmission electron microscopy, revealing that the transformation between different magnetic bubbles and domains is via the motion of Bloch lines driven by an applied external magnetic field. These results demonstrate that Fe3 Sn2 facilitates a unique magnetic control of topological spin textures at room temperature, making it a promising candidate for further skyrmion-based spintronic devices.

Flower-like dynamics of coupled Skyrmions with dual resonant modes by a single-frequency microwave magnetic field.

Resonant excitations of confined systems have aroused much attention because of their potential application in future microwave devices and spintronics. Under resonant excitations, the motion of topo-logical objects exhibits circular, elliptical or even stadium-like dynamics. However, more complex non-linear resonant excitations of topological objects in confined systems have seldom been reported and the associated physical mechanism remains unclear. Here, we present an observation of flower-like resonant excitations for coupled skyrmions in Co/Ru/Co nanodisks activated by a single-frequency microwave magnetic field by means of numerical simulation. We find that flower-like dynamics of coupled skyrmions is always accompanied by an excitation of an eigenfrequency near 1.15 GHz, which is strongly associated with the large non-local deformation of the topological density distribution of coupled skyrmions. These results distinguish a skyrmion from other topological objects in dynamics and will be instrumental to the manipulation of skyrmions for applications.

Variable-composition structural optimization and experimental verification of MnB3 and MnB4.

In combination with variable-composition evolutionary algorithm calculations and first-principles calculations, we have systematically searched for all the stable compounds and their crystal structures in the extensively investigated binary Mn-B system. Our results have uncovered four viable ground-state compounds, with Mn2B, MnB, and MnB4, and previously never reported MnB3 and two metastable compounds, MnB2 and Mn3B4. Our calculations demonstrate that the early characterized mC10 structure of MnB4 showed dynamic instability with large imaginary phonon frequencies and, instead, a new mP20 structure is predicted to be stable both dynamically and thermodynamically, with a considerable energy gain and no imaginary phonon frequencies. The new MnB3 compound crystallizes in the monoclinic mC16 structure which lies 3.2 meV per atom below the MnB (oP8) ↔ MnB4 (mP20) tie-line at T = 0 K. Furthermore, these proposed phases have been verified by our annealed samples after arc-melting synthesis and corresponding powder XRD measurements.

Unveiling the electronic origin of anion order in CrO(2-x)F(x).

Electron-diffraction and high-resolution lattice images reveal superstructure stripes with wave vectors of (1/3, 0, 1/3) and (-1/3, 0, 1/3), which are associated with the ordered arrangement of F(-). Charge density distribution suggests that these stripes manifest themselves electronically as F(-)-Cr(3+)-F(-) zigzag chains, driven by the anisotropic charge interaction of F(-) anions.