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The unique characteristics of graphene have generated much excitement due to its utility across a variety of applications. One of the principal issues inhibiting the development of graphene technologies pertains to difficulties in engineering high-quality metal contacts on graphene. In this regard, the thermal transport at the metal/graphene interface plays a significant role in the overall performance of devices. Here, we demonstrate the use of electron beam produced plasmas to chemically modify graphene and how these modifications can be used to tune the thermal transport across metal-graphene interfaces. We show that the operating conditions of the plasma can be adjusted to control the character and quantity of chemical moieties at the interface. Typically, when changes in the surface chemistry favor an increase in adhesion between the graphene and metal, the thermal boundary conductance can be notably improved. Interestingly, the conventional approach of adding a titanium “wetting layer” to improve metal adhesion did not improve the thermal boundary conductance at gold contacts.

The influence of planar organic linkers on thermal boundary conductance across hybrid interfaces has focused on the organic/inorganic interaction energy rather than on vibrational mechanisms in the molecule. As a result, research into interfacial transport at planar organic monolayer junctions has treated molecular systems as thermally ballistic. We show that thermal conductance in phosphonic acid (PA) molecules is ballistic, and the thermal boundary conductance across metal/PA/sapphire interfaces is driven by the same phononic processes as those across metal/sapphire interfaces without PAs, with one exception. We find a more than 40% reduction in conductance across henicosafluorododecylphosphonic acid (F21PA) interfaces, independent of metal contact, despite similarities in structure, composition, and terminal group to the variety of other PAs studied. Our results suggest diffusive scattering of thermal vibrations in F21PA, demonstrating a clear path toward modification of interfacial thermal transport b...

Elementary particles such as electrons or photons are frequent subjects of wave-nature-driven investigations, unlike collective excitations such as phonons. The demonstration of wave-particle crossover, in terms of macroscopic properties, is crucial to the understanding and application of the wave behaviour of matter. We present an unambiguous demonstration of the theoretically predicted crossover from diffuse (particle-like) to specular (wave-like) phonon scattering in epitaxial oxide superlattices, manifested by a minimum in lattice thermal conductivity as a function of interface density. We do so by synthesizing superlattices of electrically insulating perovskite oxides and systematically varying the interface density, with unit-cell precision, using two different epitaxial-growth techniques. These observations open up opportunities for studies on the wave nature of phonons, particularly phonon interference effects, using oxide superlattices as model systems, with extensive applications in thermoelectrics and thermal management.

Graphene-based devices have garnered tremendous attention due to the unique physical properties arising from this purely two-dimensional carbon sheet leading to tremendous efficiency in the transport of thermal carriers (i.e., phonons). However, it is necessary for this two-dimensional material to be able to efficiently transport heat into the surrounding 3D device architecture in order to fully capitalize on its intrinsic transport capabilities. Therefore, the thermal boundary conductance at graphene interfaces is a critical parameter in the realization of graphene electronics and thermal solutions. In this work, we examine the role of chemical functionalization on the thermal boundary conductance across metal/graphene interfaces. Specifically, we metalize graphene that has been plasma functionalized and then measure the thermal boundary conductance at Al/graphene/SiO(2) contacts with time domain thermoreflectance. The addition of adsorbates to the graphene surfaces are shown to influence the cross plane thermal conductance; this behavior is attributed to changes in the bonding between the metal and the graphene, as both the phonon flux and the vibrational mismatch between the materials are each subject to the interfacial bond strength. These results demonstrate plasma-based functionalization of graphene surfaces is a viable approach to manipulate the thermal boundary conductance.

The presented model predicts thermal boundary conductance at interfaces where one material comprising the junction is characterized by high elastic anisotropy. In contrast to previous approaches, the current methodology accounts for contributions from inelastic scattering through consideration of multiple-phonon interactions. Inelastic contributions become significant as the temperature, as well as the degree of acoustic mismatch between the materials, increases. Inclusion of the inelastic interactions is necessary for a variety of interfacial systems including the metal–graphite boundary examined here. Improvement is shown over existing approaches that address only elastic scattering as both three- and four-phonon interactions significantly augment the transport.

Models intended to predict interfacial transport often rely on the principle of detailed balance when formulating the interfacial carrier transmission probability. However, assumptions invoked significantly impact predictions. Here, we present six derivations of the transmission probability, each subject to a different set of preliminary assumptions regarding the type of scattering at the interface. Application of each case to phonon flux and thermal boundary conductance allows for a final quantitative comparison. Depending on the preliminary assumptions, predictions for thermal boundary conductance span over two orders of magnitude, demonstrating the need for transparency when assessing the accuracy of any predictive model.

This work considers the effects of intra- and direct interband transitions on electron heat capacity and the electron-phonon coupling factor in metals. In the event of an interband transition, the population of the electron bands around the Fermi level will change, affecting the electron density of states and subsequently the thermophysical properties. In the event of photon-induced interband transitions, this repopulation can occur even at relatively low temperatures. This introduces a photon energy-dependent population term into density of states calculations when examining the effects of direct interband transitions on electron heat capacity and the electron-phonon coupling factor in temperature regimes where traditionally only intraband transitions are considered. Example calculations are shown for copper and the two-temperature model is solved using the interband-dependent values of electron heat capacity and electron-phonon coupling factor to examine the effect of these transitions on the transient ...

Smoke-wire flow visualization is employed to investigate the behavior of a round jet issuing from a straight tube and impinging on a cylindrical pedestal mounted on a flat plate. Velocity and turbulence intensity measurements at the jet exit show correlation with the formation of visualized structures near the impingement surface. The effects of jet exit-to-surface spacing (H/d) and Reynolds number (Re) are explored. It is found that as jet exit-surface spacing increases from 2 to 5, small but significant effects can be seen. These effects include a stabilization of the flow, a lengthening of the potential core and a reduction in vortex formation prior to impingement. An increase in Re is found to increase the turbulence in the shear layer and suppress vortex formation. The presence of the cylindrical pedestal is found to stabilize the jet prior to impingement and also creates a recirculation region at the edge of the pedestal for low Re.

The thermal boundary conductance across solid-solid interfaces can be affected by the physical properties of the solid boundary. Atomic composition, disorder, and bonding between materials can result in large deviations in the phonon scattering mechanisms contributing to thermal boundary conductance. Theoretical and computational studies have suggested that the mixing of atoms around an interface can lead to an increase in thermal boundary conductance by creating a region with an average vibrational spectra of the two materials forming the interface. In this paper, we experimentally demonstrate that ion irradiation and subsequent modification of atoms at solid surfaces can increase the thermal boundary conductance across solid interfaces due to a change in the acoustic impedance of the surface. We measure the thermal boundary conductance between thin aluminum films and silicon substrates with native silicon dioxide layers that have been subjected to proton irradiation and post-irradiation surface cleaning procedures. The thermal boundary conductance across the Al/native oxide/Si interfacial region increases with an increase in proton dose. Supported with statistical simulations, we hypothesize that ion beam mixing of the native oxide and silicon substrate within $\ensuremath{\sim}2.2\phantom{\rule{0.3em}{0ex}}\mathrm{nm}$ of the silicon surface results in the observed increase in thermal boundary conductance. This ion mixing leads to the spatial gradation of the silicon native oxide into the silicon substrate, which alters the acoustic impedance and vibrational characteristics at the interface of the aluminum film and native oxide/silicon substrate. We confirm this assertion with picosecond acoustic analyses. Our results demonstrate that under specific conditions, a ``more disordered and defected'' interfacial region can have a lower resistance than a more ``perfect'' interface.

The thermal conductivities of 1μm copper-niobium multilayer films of different period thicknesses are measured by time–domain thermoreflectance at room temperature. The values for thermal conductivity are then used to calculate the thermal conductance between Cu/Nb interfaces using a series resistors model. Results show that Cu/Nb interface conductance increases with the decrease in period thickness reaching a value as high as 20 GWm−2K−1 for a 1×1 Cu/Nb multilayer. At shorter period thicknesses, ballistic electron transport dominates the thermal transport across this interface resulting in high interface conductance. The results are well described by a model that accounts for both ballistic and diffusive transport of electrons. This model assumes that an electron on one side of a metal-metal multilayer may not scatter at the interface but rather move ballistically on to the adjacent material and scatter in the adjacent material.Copyright © 2013 by ASME

Thermal boundary resistance (inverse of conductance) between different material layers can dominate the overall thermal resistance in nanostructures and therefore impact the performance of the thermal property limiting nano devices. Because relationships between material properties and thermal boundary conductance have not been fully understood, optimum devices cannot be developed through a rational selection of materials. Here we develop generic interatomic potentials to enable material properties to be continuously varied in extremely large molecular dynamics simulations to explore the dependence of thermal boundary conductance on the characteristic properties of materials such as atomic mass, stiffness, and interfacial crystallography. To ensure that our study is not biased to a particular model, we employ different types of interatomic potentials. In particular, both a Stillinger–Weber potential and a hybrid embedded-atom-method + Stillinger–Weber potential are used to study metal-on-semiconductor compound interfaces, and the results are analyzed considering previous work based upon a Lennard-Jones (LJ) potential. These studies, therefore, reliably provide new understanding of interfacial transport phenomena particularly in terms of effects of material properties on thermal boundary conductance. Our most important finding is that thermal boundary conductance increases with the overlap of the vibrational spectra between metal modes and the acoustic modes of the semiconductor compound, and increasing the metal stiffness causes a continuous shift of the metal modes. As a result, the maximum thermal boundary conductance occurs at an intermediate metal stiffness (best matched to the semiconductor stiffness) that maximizes the overlap of the vibrational modes.

Thermal boundary resistance dominates the overall resistance of nanosystems. This effect can be utilized to improve the figure of merit of thermoelectric materials. It is also a concern for thermal failures in microelectronic devices. The interfacial resistance depends sensitively on many interrelated structural details including material properties of the two layers, the system dimensions, the interfacial morphology, and the defect concentrations near the interface. The lack of an analytical understanding of these dependencies has been a major hurdle for a science-based design of optimum systems on a nanoscale. Here we have combined an analytical model with extensive, highly converged direct-method molecular dynamics simulations to derive analytical relationships between interfacial thermal boundary resistance and structural features. We discover that thermal boundary resistance linearly decreases with total interfacial area that can be modified by interfacial roughening. This finding is further elucidated using wave-packet analysis and local density of state calculations.

We report on the thermal conductivities of microcrystalline [6,6]-phenyl C(61)-butyric acid methyl ester (PCBM) thin films from 135 to 387 K as measured by time domain thermoreflectance. Thermal conductivities are independent of temperature above 180 K and less than 0.030 ± 0.003 W m(-1) K(-1) at room temperature. The longitudinal sound speed is determined via picosecond acoustics and is found to be 30% lower than that in C(60)/C(70) fullerite compacts. Using Einstein's model of thermal conductivity, we find the Einstein characteristic frequency of microcrystalline PCBM is 2.88 × 10(12) rad s(-1). By comparing our data to previous reports on C(60)/C(70) fullerite compacts, we argue that the molecular tails on the fullerene moieties in our PCBM films are responsible for lowering both the apparent sound speeds and characteristic vibrational frequencies below those of fullerene films, thus yielding the exceptionally low observed thermal conductivities.

This paper investigates anharmonic phonon dispersion relations measured directly from molecular dynamics simulations at finite temperatures and pressure. The measured dynamical matrix and resulting anharmonic dispersion relations do not require an a-priori analytical expression regarding the strength of anharmonic processes. Therefore, no assumptions concerning the degree of anharmonicity are made beyond specifying an interatomic potential. We calculate phonon properties pertinent to thermal transport in graphene. Specifically, we demonstrate the calculation of phonon dispersion relations and group velocities over the entire Brillouin Zone, as well as the branch-dependent contribution to specific heat capacity and ballistic thermal conductance. We highlight the capabilities of this technique to lend fundamental insight into the anharmonic characteristics of phonon-mediated transport. Finally, we discuss how anharmonic phonon dispersion relations may be used to evaluate the differences in phonon properties between various interatomic potentials commonly used in the simulation of phonon-mediated thermal transport.Copyright © 2012 by ASME

We experimentally investigate the role of size effects and boundary scattering on the thermal conductivity of silicon-germanium alloys. The thermal conductivities of a series of epitaxially grown Si(1-x)Ge(x) thin films with varying thicknesses and compositions were measured with time-domain thermoreflectance. The resulting conductivities are found to be 3 to 5 times less than bulk values and vary strongly with film thickness. By examining these measured thermal conductivities in the context of a previously established model, it is shown that long wavelength phonons, known to be the dominant heat carriers in alloy films, are strongly scattered by the film boundaries, thereby inducing the observed reductions in heat transport. These results are then generalized to silicon-germanium systems of various thicknesses and compositions; we find that the thermal conductivities of Si(1-x)Ge(x) superlattices are ultimately limited by finite size effects and sample size rather than periodicity or alloying. This demonstrates the strong influence of sample size in alloyed nanosystems. Therefore, if a comparison is to be made between the thermal conductivities of superlattices and alloys, the total sample thicknesses of each must be considered.

The thermal conductance of interfaces plays a major role in defining the thermal properties of nanostructured materials in which heat transfer is predominantly phonon mediated. Ongoing research has improved the understanding of factors that govern interfacial phonon transport as well as the ability to predict thermal interface conductance. However, despite this progress, the ability to control interface conductance remains a major challenge. In this manuscript, we present a method to enhance and tune thermal interface conductance at vibrationally mismatched solid-solid interfaces. Enhancement is achieved through the insertion of an interfacial film with mediating vibrational properties, such that the vibrational mismatch at the interface is bridged, and consequently, the total interface conductance is enhanced. This phenomena is explored using nonequilibrium molecular dynamics simulations, where the effects of altering the interfacial film thickness, vibrational spectrum, and the temperature of the system are investigated. A systematic study of these pertinent design parameters explores the ability to enhance and tune phonon transport at both ideal (sharp) and nonideal (compositionally disordered) interfaces. Results show that interface conductance can be broadly enhanced by up to 53% in comparison to the vibrationally mismatched baseline interface. Additionally, we find that compositional disorder at an interface does not imply a deterministic change in interface conductance, but instead, that the influence of compositional disorder depends on the characteristics of the disordered region itself. These results, in contrast to macroscopic thermal transport theory, imply that it is possible to increase thermal conductance associated with interface scattering by adding more material along the direction of heat flux.

We investigate the behavior of Kapitza conductance at interfaces between two Lennard-Jones fcc solids as a function of the range and strength of cross-species interactions via molecular dynamics simulations. It is found that decreasing either of these quantities leads to a reduction in the slope of linear temperature dependence of Kapitza conductance, suggesting a corresponding decrease in the probability of inelastic phonon-phonon interactions. To further explore the mechanisms responsible for such behavior, we calculate the phonon density of states and spectral temperature of each of the monolayers adjacent to the interface. It is found that the reduction of the range and strength of cross-species interactions leads to a softening of the density of states near the interface, while the spectral temperature calculations provide further evidence that such reductions decrease the probability of inelastic phonon scattering. These findings help explain varying accounts of the temperature dependence of Kapitza conductance observed in previous works.

Many random substitutional solid solutions (alloys) will display a tendency to atomically order given the appropriate kinetic and thermodynamic conditions. Such order–disorder transitions will result in major crystallographic reconfigurations, where the atomic basis, symmetry, and periodicity of the alloy change dramatically. Consequently, phonon behavior in these alloys will vary greatly depending on the type and degree of ordering achieved. To investigate these phenomena, the role of the order–disorder transition on phononic transport properties of Lennard–Jones type binary alloys is explored via nonequilibrium molecular dynamics simulations. Particular attention is paid to regimes in which the alloy is only partially ordered. It is shown that by varying the degree of ordering, the thermal conductivity of a binary alloy of fixed composition can be tuned across an order of magnitude at 10% of the melt temperature, and by a factor of three at 40% of the melt temperature.

We investigate the role of anisotropy on interfacial transport across solid interfaces by measuring the thermal boundary conductance from 100 to 500 K across Al/Si and Al/sapphire interfaces with different substrate orientations. The measured thermal boundary conductances show a dependency on substrate crystallographic orientation in the sapphire samples (trigonal conventional cell) but not in the silicon samples (diamond cubic conventional cell). The change in interface conductance in the sapphire samples is ascribed to anisotropy in the Brillouin zone along the principal directions defining the conventional cell. This leads to resultant phonon velocities in the direction of thermal transport that vary nearly 40% based on crystallographic direction.

We examine the fundamental phonon mechanisms affecting the interfacial thermal conductance across a single layer of quantum dots (QDs) on a planar substrate. We synthesize a series of Ge${}_{x}$Si${}_{1\ensuremath{-}x}$ QDs by heteroepitaxial self-assembly on Si surfaces and modify the growth conditions to provide QD layers with different root-mean-square (rms) roughness levels in order to quantify the effects of roughness on thermal transport. We measure the thermal boundary conductance (${h}_{\mathrm{K}}$) with time-domain thermoreflectance. The trends in thermal boundary conductance show that the effect of the QDs on ${h}_{\mathrm{K}}$ are more apparent at elevated temperatures, while at low temperatures, the QD patterning does not drastically affect ${h}_{\mathrm{K}}$. The functional dependence of ${h}_{\mathrm{K}}$ with rms surface roughness reveals a trend that suggests that both vibrational mismatch and changes in the localized phonon transport near the interface contribute to the reduction in ${h}_{\mathrm{K}}$. We find that QD structures with rms roughnesses greater than 4 nm decrease ${h}_{\mathrm{K}}$ at Si interfaces by a factor of 1.6. We develop an analytical model for phonon transport at rough interfaces based on a diffusive scattering assumption and phonon attenuation that describes the measured trends in ${h}_{\mathrm{K}}$. This indicates that the observed reduction in thermal conductivity in SiGe quantum dot superlattices is primarily due to the increased physical roughness at the interfaces, which creates additional phonon resistive processes beyond the interfacial vibrational mismatch.

Substitutional solid solutions that exist in both ordered and disordered states will exhibit markedly different physical properties depending on their exact crystallographic configuration. Many random substitutional solid solutions (alloys) will display a tendency to order given the appropriate kinetic and thermodynamic conditions. Such order-disorder transitions will result in major crystallographic reconfigurations, where the atomic basis, symmetry, and periodicity of the alloy change dramatically. Consequently, the dominant scattering mechanism in ordered alloys will be different than that in disordered alloys. In this study, we present a hypothesis that ordered alloys can exhibit lower thermal conductivities than their disordered counterparts at elevated temperatures. To validate this hypothesis, we investigate the phononic transport properties of disordered and ordered AB Lennard-Jones alloys via non-equilibrium molecular dynamics and harmonic lattice dynamics calculations. It is shown that the thermal conductivity of an ordered alloy is the same as the thermal conductivity of the disordered alloy at ≈0.6T(melt) and lower than that of the disordered alloy above 0.8T(melt).

We present a new model for predicting thermal boundary conductance in the classical limit. This model takes a different form than those of the traditionally used mismatch theories in the fact that the temperature dependence of thermal boundary conductance is driven by the phononic scattering mechanisms of the materials comprising the interface as opposed to the heat capacities of those materials. The model developed in this work assumes that a phonon on one side of an interface may not scatter at the interface itself but instead scatter with phonons in the adjacent material via the scattering processes intrinsic in the adjacent material. We find that this model is in good agreement with classical molecular dynamics simulations of phonon transport across a Si/Ge interface.

Self-assembled monolayers (SAMs) have recently garnered much interest due to their unique electrical, chemical, and thermal properties. Several studies have focused on thermal transport across solid–SAM junctions, demonstrating that interface conductance is largely insensitive to changes in SAM length. In the present study, we have investigated the vibrational spectra of alkanedithiol-based SAMs as a function of the number of methylene groups forming the molecular backbone via Hartree–Fock methods. In the case of Au–alkanedithiol junctions, it is found that despite the addition of nine new vibrational modes per added methylene group, only one of these modes falls below the maximum phonon frequency of Au. In addition, the alkanedithiol one-dimensional density of normal modes (modes per unit energy per unit length) is nearly constant regardless of chain length, explaining the observed insensitivity. Furthermore, we developed a diffusive transport model intended to predict interface conductance at solid–SAM junctions. It is shown that this predictive model is in an excellent agreement with prior experimental data available in the literature.

Continued reduction in characteristic dimensions in nanosystems has given rise to increasing importance of material interfaces on the overall system performance. With regard to thermal transport, this increases the need for a better fundamental understanding of the processes affecting interfacial thermal transport, as characterized by the thermal boundary conductance. When thermal boundary conductance is driven by phononic scattering events, accurate predictions of interfacial transport must account for anharmonic phononic coupling as this affects the thermal transmission. In this paper, a new model for phononic thermal boundary conductance is developed that takes into account anharmonic coupling, or inelastic scattering events, at the interface between two materials. Previous models for thermal boundary conductance are first reviewed, including the diffuse mismatch model, which only considers elastic phonon scattering events, and earlier attempts to account for inelastic phonon scattering, namely, the maximum transmission model and the higher harmonic inelastic model. A new model is derived, the anharmonic inelastic model, which provides a more physical consideration of the effects of inelastic scattering on thermal boundary conductance. This is accomplished by considering specific ranges of phonon frequency interactions and phonon number density conservation. Thus, this model considers the contributions of anharmonic, inelastically scattered phonons to thermal boundary conductance. This new anharmonic inelastic model shows improved agreement between the thermal boundary conductance predictions and experimental data at the Pb/diamond and Au/diamond interfaces due to its ability to account for the temperature dependent changing phonon population in diamond, which can couple anharmonically with multiple phonons in Pb and Au. We conclude by discussing phonon scattering selection rules at interfaces and the probability of occurrence of these higher order anharmonic interfacial phonon processes quantified in this work.

where the thermal flux, Q, is related to the change in temperature, T, along the direction of thermal propagation, z, through the thermal conductivity, κ. The thermal conductivity is a temperature dependent material property that is unique to any givenmaterial. Figure 1 shows the measured thermal conductivity of two metals Au and Pt and two semiconductors Si and Ge (Ho et al., 1972). In these bulk materials, the thermal conductivities span three orders of magnitude over the temperature range from 1 1,000 K. Temperature trends in the thermal conductivities are similar depending on the type of material, i.e., Si and Ge show similar thermal conductivity trends with temperature as do Au and Pt. These similarities arise due to the different thermal energy carriers in the different classes of materials. In metals, heat is primarily carried by electrons, whereas in semiconductors, heat moves via atomic vibrations of the crystalline lattice. The macroscopic average of these carriers’ scattering events, which is related to the thermal conductivity of the material, gives rise to the spatial temperature gradient in Eq. 1. This temperature gradient is established from the energy carriers traversing a certain distance, the mean free path, before scattering and losing their thermal energy. In bulk systems, this mean free path is related to the intrinsic properties of the materials. However, in material systems with engineered length scales on the order of the mean free path, additional scattering events arise due to energy carrier scattering with interfaces, inclusions, grain boundaries, etc. These scattering events can substantially change the thermal conductivity of nanostructured systems as compared to that of the bulk constituents (Cahill et al., 2003). In fact, in any given material in which the physical size is less than the mean free path, the carrier scattering events will only occur at the boundaries of the material. Therefore, there will be no temperature gradient established in the material and Eq. 1 will no longer be valid. Typical carrier room temperature mean free paths in metals and semiconductors are about 10 100 nm, respectively (Tien et al., 1998). Clearly, with the wealth of technology and applications that rely on material systems with characteristic lengths scales in the sub-1.0 μm regime (Wolf, 2006), the need to understand thermal conduction at the nanoscale is immensely important for thermal management and engineering applications. In this chapter, the basic concepts of 13

This work develops a new model for calculating the thermal conductivity of polycrystalline silicon using an effective medium approach which discretizes the contribution to thermal conductivity into that of the grain and grain boundary regions. While the Boltzmann transport equation under the relaxation time approximation is used to model the grain thermal conductivity, a lower limit thermal conductivity model for disordered layers is applied in order to more accurately treat phonon scattering in the grain boundary regions, which simultaneously removes the need for fitting parameters frequently used in the traditional formation of grain boundary scattering times. The contributions of the grain and grain boundary regions are then combined using an effective medium approach to compute the total thermal conductivity. The model is compared to experimental data from literature for both undoped and doped polycrystalline silicon films. In both cases, the new model captures the correct temperature dependent trend and demonstrates good agreement with experimental thermal conductivity data from 20 to 300K.Copyright © 2011 by ASME

Continued reduction of characteristic dimensions in nanosystems has given rise to increasing importance of material interfaces on the overall system performance. With regard to thermal transport, this increases the need for a better fundamental understanding of the processes affecting interfacial thermal transport, as characterized by the thermal boundary conductance. When thermal boundary conductance is driven by phononic scattering events, accurate predictions of interfacial transport must account for anharmonic phononic coupling as this affects the thermal transmission. In this paper, a new model for phononic thermal boundary conductance is developed that takes into account anharonic coupling, or inelastic scattering events, at the interface between two materials. Previous models for thermal boundary conductance are first reviewed, including the Diffuse Mismatch Model, which only consdiers elastic phonon scattering events, and earlier attempts to account for inelastic phonon scattering, namely, the Maximum Transmission Model and the Higher Harmonic Inelastic model. A new model is derived, the Anharmonic Inelastic Model, which provides a more physical consideration of the effects of inelastic scattering on thermal boundary conductance. This is accomplished by considering specific ranges of phonon frequency interactions and phonon number density conservation. Thus, this model considers the contributions of anharmonic, inelastically scattered phonons to thermal boundary conductance. This new Anharmonic Inelastic Model shows excellent agreement between model predictions and experimental data at the Pb/diamond interface due to its ability to account for the temperature dependent changing phonon population in diamond, which can couple anharmonically with multiple phonons in Pb.Copyright © 2011 by ASME

Self-assembled monolayers (SAMs) have recently garnered much interest due to their unique electrical and chemical properties. The limited literature detailing SAM thermal properties has suggested that thermal boundary conductance (TBC) at solid-SAM junctions is not only low, but also insensitive to changes in SAM length as the number of methylene groups (-CH2 -) along alkanedithiol chains is varied from 8 to 10. The present study investigates the vibrational spectra of alkanedithiol SAMs as a function of the number of methylene groups forming the molecule backbone via Hartree-Fock methods and the subsequent effects on TBC calculated using a diffuse scattering model. In particular, the vibrational overlap between the alkanedithiol and Au is studied. It is found that despite the addition of 9 new vibrational modes per added methylene group, only one of those modes is elastically accessible to Au. It is believed that this “vibrational inaccessibility” is the cause of the insensitivity of thermal conductance to molecule length.Copyright © 2011 by ASME

Due to the high intrinsic thermal conductivity of graphitic structures, much interest has developed in incorporating these materials into modern nano-devices for improved thermal abatement. In order to be integrated successfully, thermal energy must be able to transport efficiently through the graphitic materials and into the surrounding structure, most commonly a metal. However, thermal boundary conductance at metal-graphite interfaces is traditionally poor in comparison to non-graphitic substrates, due in large part to the weak van der Waals adhesion force between the metal and underlying carbon structure. To be applicable as thermal abatement materials, an enhanced understanding of the role of the metal-carbon interface is required. This paper reports the changes to phononic thermal transport across the interface between metallic thin films and highly oriented pyrolitic graphite (HOPG) substrates due to changes in interface structure and chemistry. The temperature dependent thermal boundary conductance is measured using transient thermoreflectance from 100 K to 400 K. It is found that the differences in metal-carbon bonding and structure at the interface have a significant impact on the thermal conductance between the metallic thin films and the HOPG substrates.

Many random substitutional solid solutions (alloys) will display a tendency to chemically order given the appropriate kinetic and thermodynamic conditions. Such order-disorder transitions will result in major crystallographic reconfigurations, where the atomic basis, symmetry, and periodicity of the alloy change dramatically. Consequently, phonon behavior in these alloys will vary greatly depending on the type and degree of ordering achieved. To investigate these phenomena, the role of the order-disorder transition on phononic transport properties of Lennard-Jones type binary alloys is explored via non-equilibrium molecular dynamics simulations. Particular attention is paid to regimes in which the alloy is only partially ordered. It is shown that, through exploitation of the long-range order parameter, thermal conductivity of binary alloys can be effectively tuned across half an order of magnitude at low-to-moderate temperatures.Copyright © 2011 by ASME

Thermal transport at the interface between Lennard-Jones crystals is explored via non-equilibrium molecular dynamics simulations. The vibrational properties of each crystal are varied by changing the atomic mass of the crystal. By applying a constant thermal flux across the two-crystal composite system, a steady-state temperature gradient is established and thermal boundary conductance at the interface between the crystals is calculated via Fourier’s law. With the material properties of the two crystals fixed, thermal boundary conductance can be affected by an intermediate layer inserted between the two crystals. It is found that when the interstitial layer atomic mass is between those values of the crystals comprising the interface, interfacial transport is enhanced. This layer helps bridge the gap between the different vibrational spectra of the two materials, thus enhancing thermal transport, which is maximized when the interstitial layer atomic mass approaches the average mass of the two fixed crystals. The degree of enhancement depends on the vibrational mismatch between the interstitial layer and the crystals comprising the interface, and we report an increase in thermal boundary conductance of up to 50%.

Due to the high intrinsic thermal conductivity of carbon allotropes, there have been many attempts to incorporate such structures into existing thermal abatement technologies. In particular, carbon nanotubes (CNTs) and graphitic materials (i.e., graphite and graphene flakes or stacks) have garnered much interest due to the combination of both their thermal and mechanical properties. However, the introduction of these carbon-based nanostructures into thermal abatement technologies greatly increases the number of interfaces per unit length within the resulting composite systems. Consequently, thermal transport in these systems is governed as much by the interfaces between the constituent materials as it is by the materials themselves. This paper reports the behavior of phononic thermal transport across interfaces between isotropic thin films and graphite substrates. Elastic and inelastic diffusive transport models are formulated to aid in the prediction of conductance at a metal-graphite interface. The temperature dependence of the thermal conductance at Au-graphite interfaces is measured via transient thermoreflectance from 78 to 400 K. It is found that different substrate surface preparations prior to thin film deposition have a significant effect on the conductance of the interface between film and substrate.

We report on the thermal conductivities of amorphous Stillinger-Weber and Lennard-Jones superlattices as determined by non-equilibrium molecular dynamics simulations. Thermal conductivities decrease with increasing interface density, demonstrating that interfaces contribute a non-negligible thermal resistance. Interestingly, Kapitza resistances at interfaces between amorphous materials are lower than those at interfaces between the corresponding crystalline materials. We find that Kapitza resistances within the Stillinger-Webber based Si/Ge amorphous superlattices are not a function of interface density, counter to what has been observed in crystalline superlattices. Furthermore, the widely used thermal circuit model is able to correctly predict the interfacial resistance within the Stillinger-Weber based amorphous superlattices. However, we show that the applicability of this widely used thermal circuit model is invalid for Lennard-Jones based amorphous superlattices, suggesting that the assumptions made in the model do not hold for these systems.

We study the interplay between the contributions of electron thermal flux and interface scattering to the Kapitza conductance across metal-metal interfaces through measurements of thermal conductivity of copper-niobium multilayers. Thermal conductivities of copper-niobium multilayer films of period thicknesses ranging from 5.4 to 96.2 nm and sample thicknesses ranging from 962 to 2677 nm are measured by time-domain thermoreflectance over a range of temperatures from 78 to 500 K. The Kapitza conductances between the Cu and Nb interfaces in multilayer films are determined from the thermal conductivities using a series resistor model and are in good agreement with the electron diffuse mismatch model. Our results for the thermal boundary conductance between Cu and Nb are compared to literature values for the thermal boundary conductance across Al-Cu and Pd-Ir interfaces, and demonstrate that the interface conductance in metallic systems is dictated by the temperature derivative of the electron energy flux in the metallic layers, rather than electron mean free path or scattering processes at the interface.

Thermal boundary conductance is of critical importance to gallium nitride (GaN)-based device performance. While the GaN-substrate interface has been well studied, insufficient attention has been paid to the metal contacts in the device. In this work, we measure the thermal boundary conductance across interfaces of Au, Al, and Au-Ti contact layers and GaN. We show that in these basic systems, metal-GaN interfaces can impose a thermal resistance similar to that of GaN-substrate interfaces. We also show that these thermal resistances decrease with increasing operating temperature and can be greatly affected by inclusion of a thin adhesion layers.

We study the scattering mechanisms driving electron-phonon relaxation in thin gold films via pump-probe time-domain thermoreflectance. Electron-electron scattering can enhance the effective rate of electron-phonon relaxation when the electrons are out of equilibrium with the phonons. In order to correctly and consistently infer electron-phonon coupling factors in films on different substrates, we must account for the increase in steady-state lattice temperature due to laser heating. Our data provide evidence that a thermalized electron population will not directly exchange energy with the substrate during electron-phonon relaxation, whereas this pathway can exist between a non-equilibrium distribution of electrons and a non-metallic substrate.

We report on the thermal conductivities of poly(3,4-ethylenedioxythiophene) poly(styrenesulfonate), [6,6]-phenyl C61-butyric acid methyl ester (PCBM), poly(3-hexylthiophene-2,5-diyl) (P3HT), and P3HT:PCBM blend thin films as measured by time domain thermoreflectance. Thermal conductivities vary from 0.031±0.005 to 0.227 ± 0.014 W m−1 K−1 near room temperature and exhibit minimal temperature dependence across the range from 319 to 396 K. Thermal conductivities of blend films follow a rule of mixtures, and no percolation threshold is found. Thermal annealing of blend films has a variable effect on thermal conductivity. Finally, the thermal conductivities of P3HT films do not vary with changes in film thickness from 77 to 200 nm.

In nanosystems, the thermal resistance between materials typically dominates the overall resistance. While size effects on thermal conductivity are well documented, size effects on thermal boundary conductance have only been speculated. In response, we characterize the relationship between interfacial resistance and material dimension using molecular dynamics. We find that the interfacial resistance increases linearly with inverse system length but is insensitive to cross-sectional area. Also, from the temperature-dependence of interfacial resistance, we conclude that contributions of short-wavelength phonons dominate. Lastly, by coupling the molecular dynamics to a two-temperature model, we show that electron-mediated transport has little effect on thermal resistance.

We measure the Kapitza conductances at Au:Si contacts from 100 to 296 K via time-domain thermoreflectance. Contacts are fabricated by evaporating Au films onto Si substrates. Prior to Au deposition, the Si substrates receive pretreatments in order to modify interfacial properties, i.e., bonding and structural disorder. Through the inclusion of a Ti adhesion layer and the removal of the native oxide, Kapitza conductance can be enhanced by a factor of four at 296 K. Furthermore, interfacial roughness is found to have a negligible effect, which we attribute to the already low conductances of poorly bonded Au:Si contacts.

With the characteristic lengths of electronic and thermal devices approaching the mean free paths of the pertinent energy carriers, thermal transport across these devices must be characterized and understood, especially across interfaces. Thermal interface conductance can be strongly affected by the strength of the bond between the solids comprising the interface and the presence of an impurity mass between them. In this work, we investigate the effects of impurity masses and mechanical adhesion at molecular junctions on phonon transmission via non-equilibrium Green's functions (NEGF) formalisms. Using NEGF, we derived closed form solutions to the phonon transmission across an interface with an impurity mass and variable bonding. We find that the interface spring constant that yields the maximum transmission for all frequencies is the harmonic mean of the spring constants on either side of the interface, while for a mass impurity, the arithmetic average of the masses on either side of the interface yields the maximum transmission. However, the maximum transmission for each case is not equal. For the interface mass case, the maximum transmission is the transmission predicted by a frequency dependent form of the acoustic mismatch model, which we will refer to as the phonon mismatch model (PMM), which is valid for specular phonon scattering outside the continuum limit. However, in the interface spring case, the maximum transmission can be higher or lower than the transmission predicted by the PMM.

We measure the thermal conductivities of nano-grained strontium titanate (ng-SrTiO3) films deposited on sapphire substrates via time-domain thermoreflectance. The 170 nm thick oxide films of varying grain-size were prepared from a chemical solution deposition process. We find that the thermal conductivity of ng-SrTiO3 decreases with decreasing average grain size and attribute this to increased phonon scattering at grain boundaries. Our data are well described by a model that accounts for the spectral nature of anharmonic Umklapp scattering along with grain boundary scattering and scattering due to the film thickness.

We investigate the influence of crystallographic orientation and anisotropy on local phonon density of states, phonon transmissivity, and Kapitza conductance at interfaces between Lennard-Jones solids via classical molecular dynamics simulations. In agreement with prior works, we find that the Kapitza conductance at an interface between two face-centered cubic materials is independent of crystallographic orientation. On the other hand, at an interface between a face-centered cubic material and a tetragonal material, the Kapitza conductance is strongly dependent on the relative orientation of the tetragonal material, albeit this dependence is subject to the overlap in vibrational spectra of the cubic and tetragonal materials. Furthermore, we show that interactions between acoustic phonons in the cubic material and optical phonons in the tetragonal material can lead to the interface exhibiting greater “thermal anisotropy” as compared to that of the constituent materials. Finally, it is noted that the relati...

We investigate the influence of substitutional impurities on Kapitza conductance at coherent interfaces via non-equilibrium molecular dynamics simulations. The reference interface is comprised of two mass-mismatched Lennard-Jones solids with atomic masses of 40 and 120 amu. Substitutional impurity atoms with varying characteristics, e.g., mass or bond, are arranged about the interface in Gaussian distributions. When the masses of impurities fall outside the atomic masses of the reference materials, substitutional impurities impede interfacial thermal transport; on the other hand, when the impurity masses fall within this range, impurities enhance transport. Local phonon density of states calculations indicate that this observed enhancement can be attributed to a spatial grading of vibrational properties near the interface. Finally, for the range of parameters investigated, we find that the mass of the impurity atoms plays a dominant role as compared to the impurity bond characteristics.

The performance of many micro- and nanoscale devices depends on the ability to control interfacial thermal transport, which is predominantly mediated by phonons in semiconductor systems. The phonon transmissivity at an interface is therefore a quantity of interest. In this work, an empirical model, termed the thermal mismatch model, is developed to predict transmissivity at ideal interfaces between semiconductor materials, producing an excellent agreement with molecular dynamics simulations of wave packets. To investigate propagation through multilayered structures, this thermal mismatch model is then incorporated into a simulation scheme that represents wave packets as particles, showing a good agreement with a similar scheme that used molecular dynamics simulations as input [P. K. Schelling and S. R. Phillpot, J. Appl. Phys. 93, 5377 (2003)]. With these techniques validated for both single interfaces and superlattices, they are further used to identify ways to tune the transmissivity of multilayered structures. It is shown that by introducing intermediate layers of certain atomic masses, the total transmissivity can either be systematically enhanced or reduced compared to that of a single interface. Thus, this model can serve as a computationally inexpensive means of developing strategies to control phonon transmissivity in applications that may benefit from either enhancement (e.g., microelectronics) or reduction (e.g., thermoelectrics) in thermal transport.

We measure the thermal interface conductance between thin aluminum films and silicon substrates via time-domain thermoreflectance from 100 to 300 K. The substrates are chemically etched prior to aluminum deposition, thereby offering a means of controlling interface roughness. We find that conductance can be systematically varied by manipulating roughness. In addition, transmission electron microscopy confirms the presence of a conformal oxide for all roughnesses, which is then taken into account via a thermal resistor network. This etching process provides a robust technique for tuning the efficiency of thermal transport while alleviating the need for laborious materials growth and/or processing.

We report on the thermal boundary conductance across structurally-variant GaSb/GaAs interfaces characterized by different dislocations densities, as well as variably-rough Al/GaSb interfaces. The GaSb/GaAs structures are epitaxially grown using both interfacial misfit (IMF) and non-IMF techniques. We measure the thermal boundary conductance from 100 to 450 K with time-domain thermoreflectance. The thermal boundary conductance across the GaSb/GaAs interfaces decreases with increasing strain dislocation density. We develop a model for interfacial transport at structurally-variant interfaces in which phonon propagation and scattering parallels photon attenuation. We find that this model describes the measured thermal boundary conductances well.

The electronic scattering rates in metals after ultrashort pulsed laser heating can be drastically different than those predicted from free electron theory. The large electron temperature achieved after ultrashort pulsed absorption and subsequent thermalization can lead to excitation of subconduction band thermal excitations of electron orbitals far below the Fermi energy. In the case of noble metals, which all have a characteristic flat d-band several electron volts well below the Fermi energy, the onset of d-band excitations has been shown to increase electron-phonon scattering rates by an order of magnitude. In this paper, we investigate the effects of these large electronic thermal excitations on the ultrafast thermoelectric transport properties of gold, a characteristic noble metal. Under conditions of strong electron-phonon nonequilibrium (relatively high electron temperatures and relatively low lattice temperatures, Te⪢TL), we find that the Wiedemann–Franz law breaks down and the Seebeck coefficien...

The diffuse mismatch model (DMM) is one of the most widely implemented models for predicting thermal boundary conductance at interfaces where phonons dominate interfacial thermal transport. In the original presentation of the DMM, the materials comprising the interface were described as Debye solids. Such a treatment, while accurate in the low temperature regime for which the model was originally intended, is less accurate at higher temperatures. Here, the DMM is reformulated such that, in place of Debye dispersion, the materials on either side of the interface are described by an isotropic dispersion obtained from exact phonon dispersion diagrams in the [100] crystallographic direction. This reformulated model is applied to three interfaces of interest: Cr–Si, Cu–Ge, and Ge–Si. It is found that Debye dispersion leads to substantially higher predictions of thermal boundary conductance. Additionally, it is shown that optical phonons play a significant role in interfacial thermal transport, a notion not previously explored. Lastly, the role of the assumed dispersion is more broadly explored for Cu–Ge interfaces. The prediction of thermal boundary conductance via the DMM with the assumed isotropic [100] dispersion relationships is compared to predictions with isotropic [111] and exact three-dimensional phonon dispersion relationships. It is found that regardless of the chosen crystallographic direction, the predictions of thermal boundary conductance using isotropic phonon dispersion relationships are within a factor of two of those predictions using an exact three-dimensional phonon dispersion.

Thermal boundary conductance (TBC) is a performance determinant for many microsystems due to the numerous interfaces contained within their structure. To assess this transport, theoretical approaches often account for only the acoustic phonons as optical modes are assumed to contribute negligibly due to their low group velocities. To examine this approach, the diffuse mismatch model is reformulated to account for more realistic dispersions containing optical modes. Using this reformulation, it is found that optical phonons contribute to TBC by as much as 80% for a variety of material combinations in the limit of both inelastic and elastic scattering.