The existed theories and methods for calculating interfacial thermal conductance of solid-solid interface lead to diverse values that deviate from experimental measurements. In this letter, We propose a model to estimate the ITC at high temperature without comprehensive calculations, where the interface between two dissimilar solids can be treated as an amorphous thin layer and the coordination number density across interface becomes a key parameter. Our model predicts that the ITCs of various interfaces at 300K are in a narrow range: 10$^{7}$W m$^{-2}$K$^{-1}$ $\sim $10$^{9}$ W m$^{-2}$ K$^{-1}$, which is in good agreement with the experimental measurement.
Tuning interfacial thermal conductance has been a key task for the thermal management of nanoelectronic devices. Here, it is studied how the interfacial thermal conductance is great influenced by modulating the mass distribution of the interlayer of one-dimensional atomic chain. By nonequilibrium Green's function and machine learning algorithm, the maximum/minimum value of thermal conductance and its corresponding mass distribution are calculated. Interestingly, the mass distribution corresponding to the maximum thermal conductance is not a simple function, such as linear and exponential distr…
Graphene, as a passivation layer, can be used to protect the black phosphorus from the chemical reaction with surrounding oxygen and water. However, black phosphorus and graphene heterostructures have low efficiency of heat dissipation due to its intrinsic high thermal resistance at the interfaces. The accumulated energy from Joule heat has to be removed efficiently to avoid the malfunction of the devices. Therefore, it is of significance to investigate the interfacial thermal dissipation properties and manipulate the properties by interfacial engineering on demand. In this work, the interfaci…
We present the results of classical molecular dynamics simulations to assess the relative contributions to interfacial thermal conductance from inelastic phonon processes at the interface and in the adjacent bulk materials. The simulated system is the prototypical interface between argon and "heavy argon" crystals, which enables comparison with many past computational studies. We run simulations interchanging the Lennard-Jones potential with its harmonic approximation to test the effect of anharmonicity on conductance. The results confirm that the presence of anharmonicity is correlated with i…
Atomically thin materials such as graphene and semiconducting transition metal dichalcogenides have attracted extensive interest in recent years, motivating investigation into multiple properties. In this work, we used the opto thermal Raman technique to measure the thermal transport properties of a popular TMDC material WSe$_2$, in single atomic layer, bilayer, and trilayer forms.
We report the first ever accurate theoretical prediction of thermal conductance of any material interface. Thermal interfacial conductance of aluminum (Al)-sapphire (α-Al2O3) interface along crystal directions (111) Al || (0001) Al2O3 for temperature ranging from 50-500 K is calculated using two fundamentally different methods: interfacial conductance modal analysis (ICMA) and atomistic green function (AGF). While AGF overpredicts interfacial conductance, both the quantitative and qualitative predictions of ICMA are exceptional when compared with the time-domain thermoreflectance (TDTR) experi…
Existing theoretical models of the interfacial thermal conductance, i.e., Kapitza conductance, of insulating solid-fluid interfaces only consider bulk properties, e.g., acoustic mismatch model and diffuse mismatch model. In this work, we propose a classical lattice dynamical model calculation of the Kapitza conductance, thereby incorporating interfacial structural details. In our model, we assume that heat is mostly carried by phonons in the solid, and that sound waves carry diffusive heat from the interface into the bulk of the liquid, where both longitudinal and transverse sound waves are co…
Interfacial thermal transport is critical for many thermal-related applications such as heat dissipation in electronics. While the total interfacial thermal conductance (ITC) can be easily measured or calculated, the ITC spectral mapping has been investigated only recently and is not fully understood. By combining nonequilibrium molecular dynamics simulations and atomistic Green's function method, we systematically investigate the ITC spectrum across an ideal interface, i.e., the argon-heavy argon interface. Our results show that the ITC spectrum increases gradually with temperature as more ph…
We point out that the effective channel for the interfacial thermal conductance, the inverse of Kapitza resistance, of metal-insulator/semiconductor interfaces is governed by the electron-phonon interaction mediated by the surface states allowed in a thin region near the interface. Our detailed calculations demonstrate that the interfacial thermal conductance across Pb/Pt/Al/Au-diamond interfaces are only slightly different among these metals, and reproduce well the experimental results of the interfacial thermal conductance across metal-diamond interfaces observed by Stoner et al. [Phys. Rev.…
Improving interfacial thermal transport is crucial for heat dissipation in systems. Here, we design a strategy by utilizing the water adsorption-desorption process in porous metal-organic frameworks (MOFs) to tune the interfacial heat transfer. We observe a changeable thermal conductance across the solid/porous MOFs interfaces owing to the dense water channel formed by the adsorbed water molecules in MOFs. Our experimental results show that the interfacial thermal conductance of Au/Cu3(BTC)2 heterointerfaces is increased up to 7.1 folds by this strategy, where Cu3(BTC)2 is a typical porous MOF…
We report experimental and computational studies of thermal transport properties in hexagonal boron nitride (hBN) encapsulated molybdenum disulfide (MoS2) structure using refined optothermal Raman techniques, and reveal very high interfacial thermal conductance between hBN and MoS2. By studying the Raman shift of hBN and MoS2 in suspended and substrate-supported thin films under varying laser power and temperature, we calibrate lateral (in-plane) thermal conductivity of hBN and MoS2 and the vertical interfacial thermal conductance in the hBN/MoS2/hBN heterostructure as well as the interfaces b…
The role of interfacial nonidealities and disorder on thermal transport across interfaces is traditionally assumed to add resistance to heat transfer, decreasing the thermal boundary conductance (TBC).$^1$ However, recent computational works have suggested that interfacial defects can enhance this thermal boundary conductance through emergence of unique vibrations that are intrinsic to the material interface and defect atoms,$^{2-6}$ a finding that contradicts traditional theory and conventional understanding. By manipulating the local heat flux of atomic vibrations that comprise these interfa…
We report the observation of a premelting transition at chemically sharp solid-liquid interfaces using molecular-dynamics simulations. The transition is observed in the solid-Al/liquid-Pb system and involves the formation of a liquid interfacial film of Al with a width that grows logarithmically as the bulk melting temperature is approached from below, consistent with current theories of premelting. The premelting behavior leads to a sharp change in the temperature dependence of the diffusion coefficient in the interfacial region, and could have important consequences for phenomena such as par…
The rich interaction phenomena at antiferromagnet (AFM)/ ferromagnet (FM) interfaces are key ingredients in AFM spintronics, where many underlying mechanisms remain unclear. Here we report a correlation observed between interfacial Dzyaloshinskii-Moriya interaction (DMI) Ds and effective spin mixing conductance g at IrMn/CoFeB interface. Both Ds and g are quantitatively determined with Brillouin light scattering measurements, and increase with IrMn thickness in the range of 2.5~7.5 nm. Such correlation likely originates from the AFM-states-mediated spin-flip transitions in FM, which promote bo…
In this article, we report the influence of the interfacial roughness on the thermal boundary conductance between two crystals, using molecular dynamics. We show evidence of a transition between two regimes, depending on the interfacial roughness: when the roughness is small, the boundary conductance is constant taking values close to the conductance of the corresponding planar interface. When the roughness is larger, the conductance becomes larger than the planar interface conductance, and the relative increase is found to be close to the increase of the interfacial area. The cross-plane cond…
We study ballistic interfacial thermal transport across atomic junctions. Exact expressions for phonon transmission coefficients are derived for thermal transport in one-junction and two-junction chains, and verified by numerical calculation based on a nonequilibrium Green's function method. For a single-junction case, we find that the phonon transmission coefficient typically decreases monotonically with increasing freqency. However, in the range between equal frequency spectrum and equal acoustic impedance, it increases first then decreases, which explains why the Kapitza resistance calculat…
Thermal conductivity and interfacial thermal conductance play crucial roles in the design of engineering systems where temperature and thermal stress are of concerns. To date, a variety of measurement techniques are available for both bulk and thin film solid-state materials with a broad temperature range. For thermal characterization of bulk material, the steady-state absolute method, laser flash diffusivity method, and transient plane source method are most used. For thin film measurement, the 3ω method and transient thermoreflectance technique including both frequency-domain and time-domain…
Traditional theories of interfacial heat transfer by atomic vibrations, also known as phonons, do not explain how vibrational mode interactions contribute to interface conductance. Traditional methods also use the concept of phonons as particles or waves which propagate and transmit energy through interfaces; such methods are therefore inapplicable to realistic non-crystalline systems where phonons are not propagating. Here we introduce a more general formalism of interfacial phonon transport, rigorously derived from interatomic interactions projected onto the normal modes of the system, showi…
Although the anisotropy of the solid-liquid interfacial free energy for most alloy systems is very small, it plays a crucial role in the growth rate, morphology and crystallographic growth direction of dendrites. Previous work posited a dendrite orientation transition via compositional additions. In this work we examine experimentally the change in dendrite growth behaviour in the Al-Sm (Samarium) system as a function of solute concentration and study its interfacial properties using molecular dynamics simulations. We observe a dendrite growth direction which changes from <100> to <110> as Sm …
Atomically thin monolayers of graphene show excellent electronic properties which have led to a great deal of research on their use in nanoscale devices. However, heat management of such nanoscale devices is essential in order to improve their performance. Graphene supported on hexagonal boron nitride (h-BN) substrate has been reported to show enhanced (opto)electronic and thermal properties as compared to extensively used SiO2/Si supported graphene. Motivated by this, we have performed temperature- and power-dependent Raman Spectroscopic measurements on four different types of (hetero)structu…
We report theoretical investigations on the role of interfacial bonding mechanism and its resulting structures to quantum transport in molecular wires. Two bonding mechanisms for the Au-S bond in an Au(111)/1,4-benzenedithiol(BDT)/Au(111) junction were identified by ab initio calculation, confirmed by a recent experiment, which, we showed, critically control charge conduction. It was found, for Au/ BDT/Au junctions, the hydrogen atom, bound by a dative bond to the Sulfur, is energetically non-dissociative after the interface formation. The calculated conductance and junction breakdown forces o…
Due to its low intrinsic damping, Y$_3$Fe$_5$O$_{12}$ and its substituted variations are often used for ferromagnetic layer at spin pumping experiment. Spin pumping is an interfacial spin current generation in the interface of ferromagnet and non-magnetic metal, governed by spin mixing conductance parameter $G^{\uparrow\downarrow}$. $G^{\uparrow\downarrow}$ has been shown to enhance the damping of the ferromagnetic layer. The theory suggested that the effect of $G^{\uparrow\downarrow}$ on gyromagnetic ratio only come from its negligible imaginary part. In this article, we show that the differe…
We report on the fabrication of conducting interfaces between LaAlO$_3$ and SrTiO$_3$ by 90$^o$ off-axis sputtering in an Ar atmosphere. At a growth pressure of 0.04 mbar the interface is metallic, with a carrier density of the order of $10^{13}$ cm$^{-2}$ at 3 K. By increasing the growth pressure, we observe an increase of the out-of-plane lattice constants of the LaAlO$_3$ films while the in-plane lattice constants do not change. Also, the low-temperature sheet resistance increases with increasing growth pressure, leading to an insulating interface when the growth pressure reaches 0.10 mbar.…
We study the nonlinear interfacial thermal transport across atomic junctions by the quantum self-consistent mean field (QSCMF) theory based on nonequilibrium Green's function approach; the QSCMF theory we propose is very precise and matches well with the exact results from quantum master equations. The nonlinearity at the interface is studied by effective temperature dependent interfacial coupling calculated from the QSCMF theory. We find that nonlinearity can provide an extra channel for phonon transport in addition to the phonon scattering which usually blocks heat transfer. For weak linearl…
Accurate estimation of interfacial thermal conductance between silicon and diamond enabled by a machine learning interatomic potential
Imam Khomeini International University（伊玛目霍梅尼国际大学）；Institut Lumière Matière, Université Claude Bernard Lyon 1-CNRS, Université de Lyon（光物质研究所，里昂第一大学-CNRS，里昂大学）；Chair of Computational Science and Simulation Technology, Institute of Photonics, Department of Mathematics and Physics, Leibniz Universität Hannover（莱布尼茨汉诺威大学计算科学与仿真技术教席、光子学研究所、数学与物理系）；School of Energy Science and Engineering, Harbin Institute of Technology（哈尔滨工业大学能源学院）
In this paper, we investigate three-phase eutectic growth during thin-film directional solidification of a model symmetric ternary eutectic alloy. In contrast to two-phase eutectics that have only a single possibility, $αβαβ$..., as the growth pattern, during three-phase eutectic growth infinite possibilities exist. Here, we explore the possible existence of pattern selection influenced by the change in the solid-solid interfacial energies and the diffusivities. We begin the study by estimating the undercooling vs. spacing variation for the simplest possible configurations of pattern lengths 3…
The Heusler ferromagnetic (FM) compound Co2FeAl interfaced with a high-spin orbit coupling non-magnetic (NM) layer is a promising candidate for energy efficient spin logic circuits. The circuit potential depends on the strength of angular momentum transfer across the FM/NM interface; hence, requiring low spin memory loss and high spin-mixing conductance. To highlight this issue, spin pumping and spin-transfer torque ferromagnetic resonance measurements have been performed on Co_2FeAl/β-Ta heterostructures tailored with Cu interfacial layers. The interface tailored structure yields an enhanceme…
The defect induced interfacial states are created in an atomically thin two-dimensional molybdenum disulfide channel by underlying a narrow pattern of a graphene layer in a field effect transistor. Nondestructive method for the generation of charge-state allowed a highly sensitive molecular interaction with the sensitivity of nearly three-order of magnitude at room temperature. The presence of interfacial states in the channel lead to a conductance fluctuation and its magnitude is modulated using the nitrogen dioxide gas molecules in the subthreshold region. The study provides a systematic app…
Atomic-scale order enables high thermal boundary conductance at $β$-Ga$_2$O$_3$/4H-SiC interfaces
Tsinghua University（清华大学）；Beijing University of Posts and Telecommunications（北京邮电大学）；University of Cambridge（剑桥大学）；Nanchang University（南昌大学）；Max Planck Institute for Polymer Research（马克斯·普朗克聚合物研究所）
Tuning Cu/Diamond Interfacial Thermal Conductance via Nitrogen-Termination Engineering
Beijing Huairou Laboratory（北京怀柔实验室）；China Southern Power Grid Novel Electric Power System (BEIJING) Research Institute Co., Ltd（中国南方电网新型电力系统（北京）研究院有限公司）
A Materials Project based open-source Python tool, MPInterfaces, has been developed to automate the high-throughput computational screening and study of interfacial systems. The framework encompasses creation and manipulation of interface structures for solid/solid hetero-structures, solid/implicit solvents systems, nanoparticle/ligands systems; and the creation of simple system-agnostic workflows for in depth computational analysis using density-functional theory or empirical energy models. The package leverages existing open-source high-throughput tools and extends their capabilities towards…
We discuss the conductance of a molecular bridge between mesoscopic electrodes supporting low-dimensional transport and bearing an internal structure. As an example for such nanoelectrodes we assume semi-infinite (carbon) nanotubes. In the Landauer scattering matrix approach, we show that the conductance of this hybrid is very sensitive to the geometry of the contact unlike the usual behaviour in the presence of bulk electrodes.
Interfacial undercooling is of significant importance on microscopic pattern formation in the solidification of colloidal suspensions. Two kinds of interfacial undercooling are supposed to be involved in freezing colloidal suspensions, i.e. solute constitutional supercooling (SCS) caused by additives in the solvent and particulate constitutional supercooling (PCS) caused by particles. However, quantitatively identification of the interfacial undercooling of freezing colloidal suspensions is still absent and it is still unknown which undercooling is dominant. The revealing of interfacial underc…
We have examined the interfacial thermal conductance σint of single and multi-layer graphene samples prepared on fused SiO2 substrates by mechanical exfoliation of graphite. By using an ultrafast optical pump pulse and monitoring the transient reflectivity on the picosecond time scale, we obtained an average σint of 5,000 W/cm2K for the graphene-SiO2 system. We observed significant variation in σint between individual samples, but found no systematic dependence on the thickness of the graphene layers.
By adjusting the interface energy, curvature, and velocity, the anisotropy plays an important role in the interaction between interfacial processes and transport processes, determining the solidification structures. In this paper, through the quantitative phase-field model, the influence of anisotropy on the evolution of interfacial morphologies in directional solidification is investigated. To represent different interfacial anisotropies, the solidification processes with different preferred crystallographic orientations are performed. Then the effect of anisotropy on morphological evolution …
Topographical and diffuse interface reconfigurations occur with a change in the solidification rate. In this article we pursue the hypothesis that the interface configuration during solidification is determined by the rate of entropy production in the region between a rigorous solid and rigorous liquid phase. We posit that when an interface begins to migrate, there are several stable configurations that are possible. These include atomistically-planar, diffuse-planar, facet non-planar and cellular non-planar. The configuration and topographical condition that affords the maximum entropy produc…
Instability of a binary eutectic solidification front to morphological perturbations due to rejection of a ternary impurity leads to the formation of eutectic colonies. Whereas, the instability dynamics and the resultant mi- crostructural features are reasonably well understood for isotropic systems, several experimental observations point to the existence of colonies in systems with anisotropic interfaces. In this study, we extend the un- derstanding of eutectic colonies to anisotropic systems, where only certain orientations of the solid-liquid or solid-solid interfaces are thermodynamically…
It has recently been suggested that many contact mechanics problems between solids can be accurately studied by mapping the problem on an effective one dimensional (1D) elastic foundation model. Using this 1D mapping we calculate the contact area and the average interfacial separation between elastic solids with nominally flat but randomly rough surfaces. We show, by comparison to exact numerical results, that the 1D mapping method fails even qualitatively. We also calculate the normal interfacial stiffness $K$ and compare it with the result of an analytical study. We attribute the failure of …
A new formalism for extracting the modal contributions to thermal interface conductance with full inclusion of anharmonicity is presented. The results indicate that when two materials are joined a new set of vibrational modes are required to correctly describe the transport across the interface. Among these new modes, certain classifications emerge, as most modes extend at least partially into the other material. Localized interfacial modes are also present and exhibit the highest conductance contributions on a per mode basis. The results also show that anharmonicity enables inelastic scatteri…
Recent studies showed that the in-plane and inter-plane thermal conductivities of two-dimensional (2D) MoS2 are low, posing a significant challenge in heat management in MoS2-based electronic devices. To address this challenge, we design the interfaces between MoS2 and graphene by fully utilizing graphene, a 2D material with an ultra-high thermal conduction. We first perform ab initio atomistic simulations to understand the bonding nature and structure stability of the interfaces. Our results show that the designed interfaces, which are found to be connected together by strong covalent bonds b…
Atomically thin materials such as graphene and semiconducting transition metal dichalcogenides (TMDCs) have attracted extensive interest in recent years, motivating investigation into multiple properties. In this work, we demonstrate a refined version of the optothermal Raman technique to measure the thermal transport properties of two TMDC materials, MoS2 and MoSe2, in single-layer (1L) and bi-layer (2L) forms. This new version incorporates two crucial improvements over previous implementations. First, we utilize more direct measurements of the optical absorption of the suspended samples unde…
Pure spin currents hold promises for an energy-friendlier spintronics. They can be generated by a flow of charge along a non-magnetic metal having a large spin-orbit coupling. It produces a spin accumulation at its surfaces, controllable by the magnetization of an adjacent ferromagnetic layer. Paramagnetic metals typically used are close to a ferromagnetic instability and thus magnetic proximity effects can contribute to the observed angular-dependent magnetoresistance (ADMR). As interface phenomena govern the spin conductance across the metal/ferromagnetic-insulator heterostructures, unraveli…
The detailed atomistic modeling of electrochemically deposited metal monolayers is challenging due to the complex structure of the metal-solution interface and the critical effects of surface elec- trification during electrode polarization. Accurate models of interfacial electrochemical equilibria are further challenged by the need to include entropic effects to obtain accurate surface chemical potentials. We present an embedded quantum-continuum model of the interfacial environment that addresses each of these challenges and study the underpotential deposition of silver on the gold (100) surf…
Turning Insulators into Accelerators: Deciphering the Interfacial Conductivity Boost in ZrO2-Li2ZrCl6 Composites through Machine Learning Molecular Dynamics Simulations
A diffuse-interface model for predicting the evolution of metallic negative electrodes and interfacial voids in solid-state batteries with homogeneous and polycrystalline solid electrolyte separators
We consider a porous medium being saturated with a pore fluid (Biot's theory). The fluid is assumed as incompressible. It is shown that the general integral of the elastic and pressure equations can be written in form of a time dependent vectorpotential ${\bf F}$ being a solution of a homogeneous, fourth order differential equation. The obtained equation for ${\bf F}$ is of a more general form than the corresponding thermo-elastic vectorpotential, being a solution of a time dependent and inhomogeneous vector bi-Laplacian. Both vectorpotentials do, however, agree for stationary problems in gene…
