Time-domain Thermoreflectance Research Articles

Thermal Characterization of Ultrathin MgO Tunnel Barriers.

Magnetic tunnel junctions (MTJs) with ultrathin MgO tunnel barriers are at the heart of magnetic random-access memory (MRAM) and exhibit potential for spin caloritronics applications due to the tunnel magneto-Seebeck effect. However, the high programming current in MRAM can cause substantial heating which degrades the endurance and reliability of MTJs. Here, we report the thermal characterization of ultrathin CoFeB/MgO multilayers with total thicknesses of 4.4, 8.8, 22, and 44 nm, and with varying MgO thicknesses (1.0, 1.3, and 1.6 nm). Through time-domain thermoreflectance (TDTR) measurements and thermal modeling, we extract the intrinsic (∼3.6 W m-1 K-1) and effective (∼0.85 W m-1 K-1) thermal conductivities of annealed 1.0 nm thick MgO at room temperature. Our study reveals the thermal properties of ultrathin MgO tunnel barriers, especially the role of thermal boundary resistance, and contributes to a more precise thermal analysis of MTJs to improve the design and reliability of MRAM technologies.

Improving interfacial thermal transport in silicon-reinforced epoxy resin composites with self-assembled monolayers

Epoxy resin (EP) based composite materials, due to their advantages such as light weight, ease of processing, and mechanical properties, have been widely applied across thermal packaging field. However, the overall thermal conductivity is constrained by the interfacial thermal resistance between the filler and the substrate. Existing studies suggest that self-assembled monolayers (SAM) can enhance the interfacial thermal conductance (ITC) by forming covalent bonds. Nevertheless, limited research has focused on using SAM to form bilateral covalent bonds to regulate ITC. Therefore, SAM capable of forming bilateral covalent bonds at the EP/silicon (Si) interface were employed to enhance ITC. In this study, time-domain thermoreflectance (TDTR) experiments and molecular dynamics (MD) simulations were conducted to investigate the EP/SAM/Si system. The results demonstrate that SAM-NH2 modification, which forms bilateral covalent bonds at the EP/Si interface, increased the interfacial adhesion strength and enhanced ITC to 140%, thereby significantly promoting interfacial heat transfer. Conversely, ITC was reduced with SAM-CH3 due to the formation of single covalent bond. Subsequently, the differential effective medium (DEM) model was used to determine that the thermal conductivity of the composite modified with SAM-NH2 was improved by 11%. This study provides new insights into adjusting ITC using SAM.

Evaluation of AlN insertion layer on the properties of heterogeneous integrated Ga2O3 films on sapphire

Integration of gallium oxide (Ga2O3) with highly thermal conductive AlN/sapphire substrate is more effective to dissipate heat in the Ga2O3-based devices. In this work, the properties of Ga2O3 films grown on sapphire and AlN/sapphire substrates via MOCVD were both examined via various experimental methods. The X-ray diffraction (XRD) analysis showed good crystallinity and different orientations of Ga2O3 and AlN thin films. The absorption properties and band gaps were extracted from UV/Vis spectra. The atomic force microscopy (AFM) scanning images showed smooth Ga2O3 surfaces on sapphire and AlN/sapphire substrates (RMSs of 2.4 nm and 4.8 nm, respectively). The scanning electron microscopy (SEM) highlighted well-defined grains of Ga2O3 and distinct boundaries of both heterostructures. X-ray photoelectron spectroscopy (XPS) analysis depicted the distributions of various components throughout the films. Finally, by using the time-domain thermoreflectance (TDTR) method, the thermal conductivity and the thermal boundary conductivity of Ga2O3 without AlN interlayer were found to be 3.1 W/(m·K) and 70.1 MW/(m2·K) respectively. By comparison, adding AlN interlayer made the thermal conductivity and thermal boundary conductivity rise to 3.3 W/(m·K) and 111.5 MW/(m2·K) respectively. These findings have demonstrated the high-quality Ga2O3/AlN integration and good heat dissipation provided by AlN interlayer, opening up new prospects for Ga2O3/AlN devices in the future.

Electronic vs phononic thermal transport in Cr-doped V2O3 thin films across the Mott transition

Understanding the thermal conductivity of chromium-doped V2O3 is crucial for optimizing the design of selectors for memory and neuromorphic devices. We utilized the time-domain thermoreflectance technique to measure the thermal conductivity of chromium-doped V2O3 across varying concentrations, spanning the doping-induced metal–insulator transition. In addition, different oxygen stoichiometries and film thicknesses were investigated in their crystalline and amorphous phases. Chromium doping concentration (0%–30%) and the degree of crystallinity emerged as the predominant factors influencing the thermal properties, while the effect of oxygen flow (600–1400 ppm) during deposition proved to be negligible. Our observations indicate that even in the metallic phase of V2O3, the lattice contribution is the dominant factor in thermal transport with no observable impact from the electrons on heat transport. Finally, the thermal conductivity of both amorphous and crystalline V2O3 was measured at cryogenic temperatures (80–450 K). Our thermal conductivity measurements as a function of temperature reveal that both phases exhibit behavior similar to amorphous materials, indicating pronounced phonon scattering effects in the crystalline phase of V2O3.

Ultralow thermal conductivity of 2D Dion-Jacobson (PDA)(FA)n - 1PbnI3n + 1 perovskite films.

Two-dimensional (2D) perovskites exhibit enhanced thermal stability compared to three-dimensional perovskites, especially the emerging 2D Dion-Jacobson (DJ) phase perovskite. However, the heat transfer mechanisms in DJ phase perovskites are rarely reported. Herein, we determine thermal conductivities of (PDA)(FA)n - 1PbnI3n + 1 films with n = 1-6 by time-domain thermoreflectance. The measured results indicate that the thermal conductivities of these films are extremely low, showing a trend from decline to rise with increasing n values, and reaching to the lowest when n = 2. We measure the propagation of acoustic phonons in films with n = 1-3 by time-domain Brillouin scattering and find phonon velocity plays a key role in the thermal conductivity, which can be explained by the mismatch of spring constants between the inorganic layer and the organic layer using the bead-spring model. The gradually increasing thermal conductivity for larger n values is attributed to the gradual transformation of the grain orientation from horizontal to vertical, which is demonstrated by the grazing-incidence wide-angle x ray scattering (GIWAXS) results. Our work deepens the understanding of the thermal transport process in 2D DJ phase perovskite films and provides insights into thermal management solutions for their devices.

Thermal Property Estimation of Thin-Layered Structures by Means of Thermoreflectance Measurement and Network Identification by Deconvolution Algorithm

Abstract Laser-induced forward transfer (LIFT) is a powerful tool for micro and nanoscale digital printing of metals for electronic packaging. In the metal LIFT process, the donor thin metal film is propelled to the receiving substrate and deposited on it. Morphology of the deposited metal varies with the thermodynamic responses of the donor thin film during and after the laser heating. Thus, the thermophysical properties of the multilayered donor sample are important to predict the LIFT process accurately. Here, we investigated thermophysical properties of a 100 nm-thick gold coated on 0.5 mm-thick sapphire and silicon substrates by means of the nanosecond time-domain thermoreflectance (ns-TDTR) analyzed by the network identification by deconvolution (NID) algorithm, which does not require numerical simulation or analytical solution. The NID algorithm enabled us to extract the thermal time constants of the sample from the nanosecond thermal decay of the sample surface. Furthermore, the cumulative and differential structure functions allowed us to investigate the heat flow path, giving the interfacial thermal resistance and the thermal conductivity of the substrate. After calibration of the NID algorithm using the thermal conductivity of the sapphire, the thermal conductivity of the silicon was determined to be 107–151 W/(m K), which is in good agreement with the widely accepted range of 110–148 W/(m K). Our study shows the feasibility of the structure function obtained from the single-shot TDTR experiments for thermal property estimation in laser processing and electronics packaging applications.

(Invited) Electrochemical Tuning of Thermoelectric Performance of Carbon Nanotubes

One-dimensional materials have potential for high performance thermoelectric energy conversion. To experimentally understand how one-dimensional electronic structures can enhance thermoelectric performance, we have investigated the thermoelectric properties of single walled carbon nanotubes (SWCNTs) such as the relationships among electronic structures, the location of Fermi-level, Seebeck coefficients, and Power factor by combining thermoelectric measurements and electrolyte gating techniques. Through the studies, we have revealed unique properties such as violation of thermoelectric trade-off, isotropic Seebeck coefficient, and gigantic power factor [1]. However, in addition to that, it is important to understand how the carrier density also affects the thermal conductivity of the carbon nanotube thin films for correct evaluation of ZT value. Therefore, we have developed a measurement system which can evaluate thermal conductivity by tuning the location of Fermi-level through electrochemical gating techniques. Time-domain thermoreflectance (TDTR) measurement is one of methods which can evaluate the thin film thermal conductivity. In conventional TDTR system, Al is used as metal transducer, but Al is electrochemical reactive, and thus it is very difficult to combine the TDTR measurements with electrochemical techniques. To solve this problem, we developed a TDTR system using Au as a metal transducer [2]. By using Au as a metal transducer, we can evaluate both the electrical and thermal properties at the same time. By using system, we can evaluate thermal properties of thin films during electrolyte gating, and have evaluated how the change of charrier density affects the thermal conductivity of carbon nanotube thin films [3]. By preparing the aligned single-walled carbon nanotube thin film, we evaluated the ZT value in the perpendicular direction to the nanotube axis as a function of carrier density. The ZT value in this direction can be maximized to be 0.1 by tuning the Femi-level around 1st van hove singularity [4].

Evaluation of Thermal Transport Characteristics of Three-Dimensional Self-Ordered Multilayered Silicon-Germanium Nanodots

1. Background and purpose Silicon-germanium (SiGe) alloys have much lower thermal conductivity than Si and Ge single crystals and are expected to be candidates for next-generation thermoelectric device materials of internet of things society. It is important to achieve both high carrier mobility and low thermal conductivity on the basis of the dimensionless figure of merit [1]. There are several studies on the thermoelectric properties of SiGe with low-dimensional structures such as superlattice and nanodots [2,3] to dramatically decrease thermal conductivity. However, the relationship between the nanoscale thermal properties and the phonon scattering mechanism of self-ordered multilayer SiGe nanodots with high uniformity grown by Stranski-Krastanov [4] mode is unclear. In this study, we demonstrated the thermal transport characteristics of the self-ordered multilayer SiGe nanodots. 2. Experiments Si/SiGe superlattice and nanodots samples were fabricated by reduced pressure chemical vapor deposition. We set to 20 cycles of Si0.65Ge0.35 / Si superlattice, the staggered Si0.65Ge0.35 nanodots (alternately stacked) and the dot-on-dot Si0.65Ge0.35 nanodots (vertically stacked) by changing growth temperature and precursors for Si spacer growth [4], as shown in Fig. 1. Thermal properties were evaluated by the Time Domain Thermoreflectance (TDTR) method. The strain states and Ge fraction were evaluated by Raman spectroscopy. The focal length and wavenumber resolution of the Raman spectrometer were 2,000 mm and 0.1 cm-1, respectively. The excitation light source was a green laser (wavelength: 532 nm). We obtained the Raman spectra of Si-Si, Si-Ge, and Ge-Ge vibrational modes derived from the SiGe regions. 3. Results and discussion Figure 2 shows the thermal conductivity for the SiGe region of the superlattice and nanodots (dot-on-dot and staggered structures) obtained by TDTR method. We found that the SiGe nanodots with the dot-on-dot structure have the highest thermal conductivity, while the SiGe nanodots with the staggered structure and SiGe superlattice have almost the same thermal conductivity. We consider that the heat flow easily penetrates from the top (surface) to the bottom (Si substrate interface) in the dot-on-dot structures. On the other hand, it is possible that the staggered SiGe nanodots can play a sufficient role as a phonon scatterer compared to the dot-on-dot structures since the superlattice structure and the staggered SiGe nanodots have almost the same thermal properties. In conclusion, we demonstrated the possibility of controlling phonon scattering by changing the arrangement of the self-ordered multilayer SiGe nanodots. Acknowledgement This work was supported by JSPS KAKENHI Grant Number 21K14201, Japan.

Experimental study of thermal transport across metal/h-BN interfaces: Comparison with metal/graphite interfaces

The continuing miniaturization of layered material electronics highlights the increasingly significant role of interfacial thermal conductance (G) in the efficient nanoscale heat dissipation in these electronics. Despite its importance, the mechanisms of thermal transport across the interfaces of layered materials and the underlying substrate remain unclear. In this work, we comprehensively investigate the interfacial thermal and phonon transport across layered-material interfaces through our ultrafast pump-probe measurements and detailed calculations on G for the interfaces of hexagonal boron nitride (h-BN), one of the most promising layered materials. We first experimentally measure Gc for interfaces between four different metals (Al, Pd, Au and Ti) and h-BN along c-axis using time-domain thermoreflectance (TDTR) from 80 to 300 K. We successfully achieve high accuracy of our measurements with uncertainty <10 % through using the carefully chosen high modulation frequency (15.6 MHz) and relatively large laser spot size (22.5 μm). We find that the measured Gc for interfaces between metals (except Al) and (100) plane of h-BN is lower than that of metal/graphite interfaces, while Gc of Al/h-BN is comparable to that of Al/graphite interfaces. Furthermore, together with our proposed anisotropic model and the diffuse mismatch model (DMM), we determine the transmission probability for the various metal/h-BN interfaces and find that the strong bonding strength enhances the phonon transmission across Ti/h-BN or Ti/graphite interfaces. Finally, we predict the orientation-dependent thermal conductance (i.e., the different interfacial thermal transport along c-axis (Gc) and in-plane (Gab) crystallographic orientations) for both metal/h-BN and metal/graphite. We find Gab between metals and (001) plane is up to 2–3 times higher than Gc. This can be attributed to the highly anisotropic elastic properties in the h-BN and graphite. This work provides important insight into the phonon transmission mechanisms across metal/h-BN interfaces, and thus contributes significantly to the thermal management of layered material electronics.

Thermal conductivity of double polymorph Ga2O3 structures

Recently discovered double gamma/beta (γ/β) polymorph Ga2O3 structures constitute a class of novel materials providing an option to modulate functional properties across interfaces without changing the chemical compositions of materials, in contrast to that in conventional heterostructures. In this work, for the first time, we investigate thermal transport in such homo-interface structures as an example of their physical properties. In particular, the cross-plane thermal conductivity (k) was measured by femtosecond laser-based time-domain thermoreflectance with MHz modulation rates, effectively obtaining depth profiles of the thermal conductivity across the γ-/β-Ga2O3 structures. In this way, the thermal conductivity of γ-Ga2O3 ranging from 1.84 to 2.11 W m−1 K−1 was found to be independent of the initial β-substrates orientations, in accordance with the cubic spinel structure of the γ-phase and consistently with the molecular dynamics simulation data. In turn, the thermal conductivity of monoclinic β-Ga2O3 showed a distinct anisotropy, with values ranging from 10 W m−1 K−1 for [−201] to 20 Wm−1 K−1 for [010] orientations. Thus, for double γ-/β-Ga2O3 polymorph structures formed on [010] β-substrates, there is an order of magnitude difference in thermal conductivity across the γ/β interface, which can potentially be exploited in thermal energy conversion applications.

Correlation of heat transport mechanism and structural properties of GaN high electron mobility transistors

Grain sizes, impurities, and layer thicknesses in the nm-range affect the heat transport and, hence, hinder proper heat dissipation of GaN-based devices. To obtain a clear picture of heat dissipation, the mechanisms of heat transport must be linked to the structural properties of the nitride-based materials in the device. In this paper, a systematic investigation of the typical layers of GaN high-electron mobility transistor stacks was conducted by time-domain thermoreflectance analysis and Raman measurements. The analyzed layers are the AlN nucleation layer, the Al0.3Ga0.7N transition layer, the AlGaN/AlN superlattice, the C-doped GaN back-barrier, and the uid GaN layer. The results were interpreted using the Born–van Karman model, including the suppression function approach to describe the governing heat transport mechanisms. Investigation of this AlN nucleation layer showed that its phonon scattering is dominated by impurity and grain boundary scattering. The Al0.3Ga0.7N transition layer was shown to have a reduced thermal conductivity not only due to alloy scattering but also because of grain boundary scattering. The AlGaN/AlN superlattice showed a thermal conductivity lower than the Al0.3Ga0.7N transition layer, especially at higher temperatures (7.2 ± 0.2 W/mK vs 14.1 ± 0.4 W/mK at 300 °C). Caused by the enhanced AlGaN/AlN interface density, the thermal conductance was found to be 2 GW/m2 K. The AlGaN/AlN superlattice indicated an anisotropic thermal transport with a factor of ∼1.5. The C-doped GaN layers were analyzed in terms of their size-dictated thermal conductivity, resulting in a reduction of ∼66% from 1 μm to 250 nm at 30 °C. Raman spectroscopy revealed that the thicker the GaN layer, the higher the compressive stress in GaN, which additionally results in a higher thermal transport. The investigations of the heat transport depending on the structural properties enabled an accurate determination of the thermal conductivity of the layer stack. These thermal conductivities served as input parameters for 3D simulation to extract the temperature, in terms of the thermal resistance, of such high-electron mobility transistor stacks. This simulation shows the importance of the GaN layer in terms of thermal management. This work uncovers the thermal transport in GaN-based transistor stacks with the aim to improving the thermal design.

Thermal conductance of interfaces between titanium nitride and group IV semiconductors at high temperatures

Measuring the temperature dependence of material properties is a standard method for better understanding the microscopic origins for that property. Surprisingly, only a few experimental studies of thermal boundary conductance at high temperatures exist. This lack of high temperature data makes it difficult to evaluate competing theories for how inelastic processes contribute to thermal conductance. To address this, we report time domain thermoreflectance measurements of the thermal boundary conductance for TiN on diamond, silicon-carbide, silicon, and germanium between 120 and 1000 K. In all systems, the interface conductance increases monotonically without stagnating at higher temperatures. For TiN/SiC interfaces, G ranges from 330 to 1000 MW/m2-K, with a room temperature conductance of 750 MW/m2-K. The interface conductance for TiN/diamond ranges from 140 to 950 MW/m2-K. Notably, for all four interfacial systems, the conductance continues to increase with temperature even after all phonon modes in the vibrationally soft material are thermally excited. This observation suggests that inelastic processes are significant contributors to the thermal conductance in all four interfacial systems, regardless of whether the materials forming the interface are vibrationally similar or dissimilar. Our study fills a notable gap in the literature for how interfacial conductance evolves at high temperatures and tests burgeoning theories for the role of inelastic processes in interfacial thermal transport.

Enhanced through-plane thermal conductivity of graphene membranes by the interlayer microstructure manipulation: Multiscale numerical simulations and experimental verifications

Graphene, with ultrahigh in-plane thermal conductivity (IPTC), has been widely applied in the thermal dissipation of integrated circuits. However, the extremely low through-plane thermal conductivity (TPTC) of graphene limits its further application. In this work, a novel strategy was proposed to enhance the TPTC of graphene membranes (GNMs) by improving the interlayer bonding state through interlayer decoration with metal elements. Molecular dynamics simulations demonstrated that decoration with interlayer elements (Al, Ti, and Ni) enhanced the interfacial thermal conductance. This was attributed to interfacial chemical bonding through strong interfacial interactions (intensive electron localization) formed at the interface between metal and GN sheets as implied by the first principles calculations. Furthermore, the composite GNMs decorated with interlayer metal nanoparticles (Al, Ni, and Co) were prepared through co-reduction using thermal decomposition method. The corresponding TPTC was tested using time-domain thermoreflectance (TDTR) method which was much higher for the composite GNMs (175–400 W/m·K) than for pure GNM (∼140 W/m·K), and this was in consistent with the simulation results. Interlayer decoration, which enhanced the TPTC of GNMs, provides a novel and effective strategy for enhancing the overall thermal management performance of graphene-based materials in both vertical and horizontal directions.

Seeking non-Fourier heat transfer with ultrabroad band thermoreflectance spectroscopy

Studying superdiffusive thermal transport is crucial for advanced thermal management in electronics and nanotechnology, ensuring devices run efficiently and reliably. Such study also contributes to the design of high-performance thermoelectric materials and devices, thereby improving energy efficiency. This work leads to a better understanding of fundamental physics and non-equilibrium phenomena, fostering innovations in numerous scientific and engineering fields. We are showing, from a one shot experiment, that clear deviations from classical Fourier behavior are observed in a semiconductor alloy such as InGaAs. These deviations are a signature of the competition that takes place between ballistic and diffusive heat transfers. Thermal propagation is modelled by a truncated Lévy model. This approach is used to analyze this ballistic-diffusive transition and to determine the thermal properties of InGaAs. The experimental part of this work is based on a combination of time-domain and frequency-domain thermoreflectance methods with an extended bandwidth ranging from a few kHz to 100 GHz. This unique wide-bandwidth configuration allows a clear distinction between Fourier diffusive and non-Fourier superdiffusive heat propagation in semiconductor materials. For diffusive processes, we also demonstrate our ability to simultaneously measure the thermal conductivity, heat capacity and interface thermal resistance of several materials over 3 decades of thermal conductivity.

Simultaneous determination of the phase boundary thermal resistance and thermal conductivity in phase-separated TiO2 thin films

Phase boundaries, most often between crystalline and amorphous phases of a material, are ubiquitous lattice imperfections in thin films, particularly deposited by low temperature processes such as atomic layer deposition (ALD). Thermal resistances from these boundaries may impede phonon transport and reduce thermal conductivity. However, to date, there have been no reports on the direct measurement of the phase boundary thermal resistance, due in part to challenges associated with fabricating an atomically flat yet geometrically planar interface between different phases within a film. Here, we present a systematic study to simultaneously determine the phase boundary thermal resistance and thermal conductivity in a series of phase-separated titanium oxide (TiO2) thin films prepared via plasma-enhanced ALD (PEALD). A precise implementation of per-cycle plasma treatment enables extremely localized crystallization—i.e., plasma-assisted atomic layer annealing (ALA)—and the fabrication of crystalline/amorphous layered structures with their respective thicknesses systematically varied. Frequency-domain thermoreflectance measures the effective thermal conductivity of each film and its top and bottom interfaces, confirmed independently using time-domain thermoreflectance. We simultaneously solve a system of linear equations generated by applying a series resistor model to each film, yielding the phase boundary thermal resistance of 5.1 m2 K GW–1 between crystalline and amorphous TiO2, as well as the thermal conductivities of 5.1 and 2.1 W m–1 K–1 for crystalline and amorphous TiO2, respectively. The results suggest that the crystalline/amorphous phase boundary acts like a layer of crystalline (amorphous) TiO2 with equivalent thickness ∼26 (∼11) nm.

Multiscale phonon thermal transport in nano-porous silicon

We performed a comprehensive multi-scale phonon-mediated thermal transport study of nano-porous silicon (np-Si) films with average porosities in the range of φ = 30%–70%. This depth-resolved thermal characterization involves a combination of optical methods, including femtosecond laser-based time-domain thermo-reflectance (TDTR) with MHz modulation rates, opto-thermal micro-Raman spectroscopy, and continuum laser wave-based frequency domain thermo-reflectance (FDTR) with kHz modulation rates probing depths of studied samples over 0.5–1.2, 2–3.2, and 23–34 μm, respectively. We revealed a systematic decrease in thermal conductivity (k) with the rise of φ, i.e., with the lowering of the Si crystalline phase volumetric fraction. These data were used to validate our semi-classical phonon Monte Carlo and finite element mesh simulations of heat conduction, taking into account disordered geometry configurations with various φ and pore size, as well as laser-induced temperature distributions, respectively. At high φ, the decrease in k is additionally influenced by the disordering of the crystal structure, as evidenced by the near-surface sensitive TDTR and Rutherford backscattering spectroscopy measurements. Importantly, the k values measured by FDTR over larger depths inside np-Si were found to be anisotropic and lower than those detected by the near-surface sensitive TDTR and Raman thermal probes. This finding is supported by the cross-sectional scanning electron microscopy image indicating enhanced φ distribution over these micrometer-scale probed depths. Our study opens an avenue for nano-to-micrometer scale thermal depth profiling of porous semiconducting media with inhomogeneous porosity distributions applicable for efficient thermoelectric and thermal management.

Electronic interfacial thermal conductance between metal nano-films in sub-picosecond non-equilibrium transport process

Interfaces play a critical role in nanoscale thermal transport, and understanding thermal transport mechanisms across metal/metal interfaces at the non-equilibrium states is urgently needed for highly integrated electronic structures or devices. In this work, the electronic interfacial thermal conductance hee of two metal interfaces, Au/Pt and Au/Al, was measured by time domain thermoreflectance (TDTR) at the non-equilibrium states and an extended two-temperature model was applied to well describe the interactions of electrons between the metal films. For the Au/Pt structure, the measured hee is 4.4 ± 1.8 GWm−2K−1, which is consistent with the predicted value by the electronic diffuse mismatch model (DMM). While for the Au/Al structure, the measured hee (0.13±0.05 GWm−2K−1) is an order of magnitude smaller than that of Au/Pt and the predicted value of the electronic DMM. The results indicate that even the extremely thin oxide layer at the Au/Al interface can significantly hinder the electron thermal transport across the metal interface. Overall, our findings contribute to revealing the non-equilibrium interfacial thermal transport mechanisms and pave the way for designing the highly integrated electronic devices.

Anisotropic Fourier Heat Conduction and phonon Boltzmann transport equation based simulation of time domain thermo-reflectance experiments

The anisotropic Fourier Heat Conduction Equation (FHCE) and the multidimensional phonon Boltzmann Transport Equation (BTE) were solved numerically in cylindrical coordinates and in time domain to simulate a Time Domain Thermo-Reflectance (TDTR) experimental silicon/aluminum substrate/transducer setup. The out-of-phase response of the probe laser was predicted at various beam offset distances for a pump laser pulse frequency of 80 MHz and modulation frequency of 10 MHz and compared against experimental measurements for a silicon substrate. The isotropic FHCE was also solved for comparison. Results show that the isotropic FHCE with bulk thermal conductivity of 145 W/m/K significantly underpredicts the out-of-phase temperature difference, particularly at smaller beam offsets. With an isotropic thermal conductivity of 105 W/m/K, the computed results match experimental data at smaller beam offsets well, but overpredicts the experimental data at larger beam offsets. An almost-perfect match is obtained by using an anisotropic thermal conductivity wherein the radial (in-plane) thermal conductivity is set to 85 W/m/K and the axial (through-plane) conductivity is set to 130 W/m/K. The multidimensional frequency and polarization dependent phonon BTE is next solved. The BTE results for the out-of-phase temperature difference match experimental observations well at small and intermediate beam offsets, but overpredicts the experimental data at larger beam offsets. FHCE results are fitted to the BTE predictions, and the extracted (best fit) thermal conductivity is found to be 110 W/m/K.

Electron–phonon coupling and non-equilibrium thermal conduction in ultra-fast heating systems

A discrete unified gas kinetic scheme is developed to solve the Boltzmann transport equation (BTE) with coupled electron and phonon thermal transport, whose time step is not limited by the relaxation time. The key of the present scheme is that the electron/phonon advection, scattering and electron–phonon interactions are coupled together within one time step by solving the BTE again at the cell interface. Numerical results show that the present scheme can correctly predict the electron–phonon coupling effects, and is in agreement with typical two-temperature model and experimental results in existing literatures and our performed time-domain thermoreflectance technique. It can also capture the ballistic effects when the characteristic length is comparable to or smaller than the mean free path where the two-temperature model fails. In addition, two anomalous heat conduction phenomena are predicted by the present scheme, namely, heat flows from phonon to electron in transient thermal grating geometry and re-rise reflected signal appears in Au/Pt bilayer metal structure. The present work can provide theoretical guidance for the study of electron–phonon coupling and offer a useful tool for multi-scale thermal management.

Greatly Enhanced Radiative Transfer Enabled by Hyperbolic Phonon Polaritons in α‐MoO3

AbstractOrthorhombic molybdenum trioxide (α‐MoO3) is a highly anisotropic hyperbolic material in nature. Within its wide Reststrahlen bands, α‐MoO3 has hyperboloidal dispersion that supports bulk propagation of high‐k phonon polariton modes. These modes can serve as energy transport channels to greatly enhance radiative heat transfer inside the material. In this work, large radiative transfer enabled by phonon polaritons in α‐MoO3 is demonstrated. The study first determines the temperature‐dependent permittivity of α‐MoO3 from polarized Fourier‐Transform Infrared (FTIR) spectroscopy measurements and then uses a many‐body radiative heat transfer model to predict the equivalent radiative thermal conductivity of hyperbolic phonon polariton. Contribution of radiative transfer to the total thermal transport is experimentally determined from the Time‐Domain Thermoreflectance (TDTR) measurements in a temperature range from −100 to 300 °C. It is found that radiative transfer can account for ≈60% of the total thermal transport at a temperature of 300 °C. That is, conductive thermal transport is enhanced by &gt;100% by radiative transfer, or radiation inside α‐MoO3 is greater than that of conduction. These additional energy pathways will have important implications in thermal management in new materials and devices.