ABSTRACT
Surface waves can lead to intriguing transport phenomena. In particular, surface phonon polaritons (SPhPs), which result from coupling between infrared light and optical phonons, have been predicted to contribute to heat conduction along polar thin films and nanowires1. However, experimental efforts so far suggest only very limited SPhP contributions2-5. Through systematic measurements of thermal transport along the same 3C-SiC nanowires with and without a gold coating on the end(s) that serves to launch SPhPs, here we show that thermally excited SPhPs can substantially enhance the thermal conductivity of the uncoated portion of these wires. The extracted pre-decay SPhP thermal conductance is more than two orders of magnitude higher than the Landauer limit predicted on the basis of equilibrium Bose-Einstein distributions. We attribute the notable SPhP conductance to the efficient launching of non-equilibrium SPhPs from the gold-coated portion into the uncoated SiC nanowires, which is strongly supported by the observation that the SPhP-mediated thermal conductivity is proportional to the length of the gold coating(s). The reported discoveries open the door for modulating energy transport in solids by introducing SPhPs, which can effectively counteract the classical size effect in many technologically important films and improve the design of solid-state devices.
ABSTRACT
α-Sb2O4 (cervantite) and ß-Sb2O4 (clinocervantite) are mixed valence compounds with equal proportions of SbIII and SbV as represented in the formula SbIIISbVO4. Their structure and properties can be difficult to calculate owing to the SbIII lone-pair electrons. Here, we present a study of the lattice dynamics and vibrational properties using a combination of inelastic neutron scattering, Mössbauer spectroscopy, nuclear inelastic scattering, and density functional theory (DFT) calculations. DFT calculations that account for lone-pair electrons match the experimental densities of phonon states. Mössbauer spectroscopy reveals the ß phase to be significantly harder than the α phase. Calculations with O vacancies reveal the possibility for nonstoichiometric proportions of SbIII and SbV in both phases. An open question is what drives the stability of the α phase over the ß phase, as the latter shows pronounced kinetic stability and lower symmetry despite being in the high-temperature phase. Since the vibrational entropy difference is small, it is unlikely to stabilize the α phase. Our results suggest that the α phase is more stable only because the material is not fully stoichiometric.
ABSTRACT
Dislocations, one-dimensional lattice imperfections, are common to technologically important materials such as III-V semiconductors, and adversely affect heat dissipation in, for example, nitride-based high-power electronic devices. For decades, conventional nonlinear elasticity models have predicted that this thermal resistance is only appreciable when the heat flux is perpendicular to the dislocations. However, this dislocation-induced anisotropic thermal transport has yet to be seen experimentally. Using time-domain thermoreflectance, we measure strong thermal transport anisotropy governed by highly oriented threading dislocation arrays throughout micrometre-thick, single-crystal indium nitride films. We find that the cross-plane thermal conductivity is almost tenfold higher than the in-plane thermal conductivity at 80 K when the dislocation density is ~3 × 1010 cm-2. This large anisotropy is not predicted by conventional models. With enhanced understanding of dislocation-phonon interactions, our results may allow the tailoring of anisotropic thermal transport with line defects, and could facilitate methods for directed heat dissipation in the thermal management of diverse device applications.
ABSTRACT
An amendment to this paper has been published and can be accessed via a link at the top of the paper.
ABSTRACT
The capability to perform high-pressure low-temperature nuclear inelastic scattering on 125Te and 121Sb with a sapphire backscattering monochromator is presented. This technique was applied to measure nuclear inelastic scattering in TeO2 at pressures up to 10 GPa and temperatures down to 25 K. The evaluated partial Te densities of phonon states were compared with theoretical calculations and with Raman scattering measured under the same conditions. The high-pressure cell developed in this work can also be used for other techniques at pressures up to at least 100 GPa.
ABSTRACT
Conventional optical components are limited to size scales much larger than the wavelength of light, as changes to the amplitude, phase and polarization of the electromagnetic fields are accrued gradually along an optical path. However, advances in nanophotonics have produced ultrathin, so-called 'flat' optical components that beget abrupt changes in these properties over distances significantly shorter than the free-space wavelength. Although high optical losses still plague many approaches, phonon polariton (PhP) materials have demonstrated long lifetimes for sub-diffractional modes in comparison to plasmon-polariton-based nanophotonics. We experimentally observe a threefold improvement in polariton lifetime through isotopic enrichment of hexagonal boron nitride (hBN). Commensurate increases in the polariton propagation length are demonstrated via direct imaging of polaritonic standing waves by means of infrared nano-optics. Our results provide the foundation for a materials-growth-directed approach aimed at realizing the loss control necessary for the development of PhP-based nanophotonic devices.
ABSTRACT
The lattice thermal conductivity, k_{L}, of typical metallic and nonmetallic crystals decreases rapidly with increasing temperature because phonons interact more strongly with other phonons than they do with electrons. Using first principles calculations, we show that k_{L} can become nearly independent of temperature in metals that have nested Fermi surfaces and large frequency gaps between acoustic and optic phonons. Then, the interactions between phonons and electrons become much stronger than the mutual interactions between phonons, giving the fundamentally different k_{L} behavior. This striking trend is revealed here in the group V transition metal carbides, vanadium carbide, niobium carbide, and tantalum carbide, and it should also occur in several other metal compounds. This work gives insights into the physics of heat conduction in solids and identifies a new heat flow regime driven by the interplay between Fermi surfaces and phonon dispersions.
ABSTRACT
BAs was predicted to have an unusually high thermal conductivity with a room temperature value of 2000 W m^{-1} K^{-1}, comparable to that of diamond. However, the experimentally measured thermal conductivity of BAs single crystals is still lower than this value. To identify the origin of this large inconsistency, we investigate the lattice structure and potential defects in BAs single crystals at the atomic scale using aberration-corrected scanning transmission electron microscopy (STEM). Rather than finding a large concentration of As vacancies (V_{As}), as widely thought to dominate the thermal resistance in BAs, our STEM results show an enhanced intensity of some B columns and a reduced intensity of some As columns, suggesting the presence of antisite defects with As_{B} (As atom on a B site) and B_{As} (B atom on an As site). Additional calculations show that the antisite pair with As_{B} next to B_{As} is preferred energetically among the different types of point defects investigated and confirm that such defects lower the thermal conductivity for BAs. Using a concentration of 1.8(8)% (6.6±3.0×10^{20} cm^{-3} in density) for the antisite pairs estimated from STEM images, the thermal conductivity is estimated to be 65-100 W m^{-1} K^{-1}, in reasonable agreement with our measured value. Our study suggests that As_{B}-B_{As} antisite pairs are the primary lattice defects suppressing thermal conductivity of BAs. Possible approaches are proposed for the growth of high-quality crystals or films with high thermal conductivity. Employing a combination of state-of-the-art synthesis, STEM characterization, theory, and physical insight, this work models a path toward identifying and understanding defect-limited material functionality.
ABSTRACT
We compare vibrational properties and phonon thermal conductivities (κ) of monolayer InSe, GaSe, and GaS systems using density functional theory and Peierls-Boltzmann transport methods. In going from InSe to GaSe to GaS, system mass decreases giving both increasing acoustic phonon velocities and decreasing scattering of these heat-carrying modes with optic phonons, ultimately giving [Formula: see text]. This behavior is demonstrated by correlating the scattering phase space limited by fundamental conservation conditions with mode scattering rates and phonon dispersions for each material. We also show that, unlike flat monolayer systems such as graphene, in InSe, GaSe and GaS thermal transport is governed by in-plane vibrations. Alloying of InSe, GaSe, and GaS systems provides an effective method for modulating their κ through intrinsic vibrational modifications and phonon scattering from mass disorder giving reductions â¼2-3.5 times. This disorder also suppresses phonon mean free paths in the alloy systems compared to those in their crystalline counterparts. This work provides fundamental insights of lattice thermal transport from basic vibrational properties for an interesting set of two-dimensional materials.
ABSTRACT
Using the Boltzmann-Peierls equation for phonon transport approach with the inputs of interatomic force constants from the self-consistent charge density functional tight binding method, we calculate the room-temperature in-plane lattice thermal conductivities k of multilayer graphene (up to four layers) and graphite under different isotropic tensile strains. The calculated in-plane k of graphite, finite monolayer graphene and 3-layer graphene agree well with previous experiments. For unstrained graphene systems, both the intrinsic k and the extent of the diffusive transport regime present a drastic dimensional transition in going from monolayer to 2-layer graphene and thereafter a gradual transition to the graphite limit. We find a peak enhancement of intrinsic k for multilayer graphene and graphite with increasing strain with the largest enhancement amplitude â¼40%. Competition between the decreased mode heat capacities and the increased lifetimes of flexural phonons with increasing strain contribute to this k behavior. Similar k behavior is observed for 2-layer hexagonal boron nitride systems. This study provides insights into engineering k of multilayer graphene and boron nitride by strain and into the nature of thermal transport in quasi-two-dimensional and highly anisotropic systems.
ABSTRACT
The notion that phonons can carry pseudo-angular momentum has many major consequences, including topologically protected phonon chirality, Berry curvature of phonon band structure, and the phonon Hall effect. When a phonon is resonantly coupled to an orbital state split by its crystal field environment, a so-called vibronic bound state forms. Here, a vibronic bound state is observed in NaYbSe2 , a quantum spin liquid candidate. In addition, field and polarization dependent Raman microscopy is used to probe an angular momentum transfer of ΔJz = ±â between phonons and the crystalline electric field mediated by the vibronic bound stat. This angular momentum transfer between electronic and lattice subsystems provides new pathways for selective optical addressability of phononic angular momentum via electronic ancillary states.
ABSTRACT
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 paper, we explore the instantaneous eigenmodes of dynamical matrices of various Lennard-Jones argon liquid and gas systems at high temperatures and show that the normal modes can be interpreted as an interpolation of Tâ∞ (gas) and T=0 (solid) mode descriptions. We find that normal modes become increasingly collisional and translational, recovering atomistic gaslike behavior rather than vibrational with increase in temperature, suggesting that normal modes in liquids may be described by both solidlike and gaslike modes.
ABSTRACT
In general, vibrational physics has been well described by quantum perturbation theory to provide footprint characteristics for common crystals. However, despite weak phonon anharmonicity, the recently discovered cubic crystals have shown anomalous vibrational dynamics with elusive fundamental origin. Here, we developed a non-perturbative ab initio approach, in together with spectroscopy and high-pressure experiments, to successfully determine the exact dynamic evolutions of the vibrational physics for the first time. We found that the local fluctuation and coupling isotopes significantly dictate the vibrational spectra, through the Brillouin zone folding that has been previously ignored in literature. By decomposing vibrational spectra into individual isotope eigenvectors, we observed both positive and negative contributions to Raman intensity from constitutional atoms (10B, 11B, 75As or 31P). Importantly, our non-perturbative theory predicts that a novel vibrational resonance appears at high hydrostatic pressure due to broken translational symmetry, which was indeed verified by experimental measurement under a pressure up to 31.5 GPa. Our study develops fundamental understandings for the anomalous lattice physics under the failure of quantum perturbation theory and provides a new approach in exploring novel transport phenomena for materials of extreme properties.
ABSTRACT
We obtain exact results for the orbital angular momentum (OAM) of magnons at the high symmetry points of ferromagnetic (FM) and antiferromagnetic (AF) honeycomb lattices in the presence of Dzyallonshinskii-Moriya (DM) interactions. For the FM honeycomb lattice in the absence of DM interactions, the values of the OAM at the corners of the Brillouin zone (BZ) (k1∗=(0,23/9)2π/a,k2∗=(1/3,3/9)2π/a, ) are alternately±3â/16for both magnon bands. The presence of DM interactions dramatically changes those values by breaking the degeneracy of the two magnon bands. The OAM values are alternately3â/8and 0 for the lower magnon band and-3â/8and 0 for the upper magnon band. For the AF honeycomb lattice, the values of the OAM at the corners of the BZ are∓(3â/16)κon one of the degenerate magnon bands and±(3â/8)(1+κ/2)on the other, whereκmeasures the anisotropy and the result is independent of the DM interaction.
ABSTRACT
Two-dimensional (2D) materials offer unique opportunities in engineering the ultrafast spatiotemporal response of composite nanomechanical structures. In this work, we report on high frequency, high quality factor (Q) 2D acoustic cavities operating in the 50-600 GHz frequency (f) range with f × Q up to 1 × 1014. Monolayer steps and material interfaces expand cavity functionality, as demonstrated by building adjacent cavities that are isolated or strongly-coupled, as well as a frequency comb generator in MoS2/h-BN systems. Energy dissipation measurements in 2D cavities are compared with attenuation derived from phonon-phonon scattering rates calculated using a fully microscopic ab initio approach. Phonon lifetime calculations extended to low frequencies (<1 THz) and combined with sound propagation analysis in ultrathin plates provide a framework for designing acoustic cavities that approach their fundamental performance limit. These results provide a pathway for developing platforms employing phonon-based signal processing and for exploring the quantum nature of phonons.
ABSTRACT
Solids with ultralow thermal conductivity are of great interest as thermal barrier coatings for insulation or thermoelectrics for energy conversion. However, the theoretical limits of lattice thermal conductivity (κ) are unclear. In typical crystals a phonon picture is valid, whereas lowest κ values occur in highly disordered materials where this picture fails and heat is supposedly carried by random walk among uncorrelated oscillators. Here we identify a simple crystal, Tl3VSe4, with a calculated phonon κ [0.16 Watts per meter-Kelvin (W/m-K)] one-half that of our measured κ (0.30 W/m-K) at 300 K, approaching disorder κ values, although Raman spectra, specific heat, and temperature dependence of κ reveal typical phonon characteristics. Adding a transport component based on uncorrelated oscillators explains the measured κ and suggests that a two-channel model is necessary for crystals with ultralow κ.
ABSTRACT
The lattice thermal conductivity (κ) of hexagonal Ge2Sb2Te5 (h-GST) is studied via direct first-principles calculations. We find significant intrinsic anisotropy (κa/κc~2) of κ in bulk h-GST, with the dominant contribution to κ from optic phonons, ~75%. This is extremely unusual as the acoustic phonon modes are the majority heat carriers in typical semiconductors and insulators. The anisotropy derives from varying bonding along different crystal directions, specifically from weak interlayer bonding along the c-axis, which gives anisotropic phonon dispersions. The phonon spectrum of h-GST has very dispersive optic branches with higher group velocities along the a-axis as compared to flat optic bands along the c-axis. The large optic mode contributions to the thermal conductivity in low-κ h-GST is unusual, and development of fundamental physical understanding of these contributions may be critical to better understanding of thermal conduction in other complex layered materials.
ABSTRACT
The reported thermal conductivity (kappa) of suspended graphene, 3000 to 5000 watts per meter per kelvin, exceeds that of diamond and graphite. Thus, graphene can be useful in solving heat dissipation problems such as those in nanoelectronics. However, contact with a substrate could affect the thermal transport properties of graphene. Here, we show experimentally that kappa of monolayer graphene exfoliated on a silicon dioxide support is still as high as about 600 watts per meter per kelvin near room temperature, exceeding those of metals such as copper. It is lower than that of suspended graphene because of phonons leaking across the graphene-support interface and strong interface-scattering of flexural modes, which make a large contribution to kappa in suspended graphene according to a theoretical calculation.