Thermal Transport Measurements Research Articles

Synthesis and Physical Properties of the Misfit Layered Compound (EuS)1.13(NbSe2)2.

A new misfit layered compound with the stoichiometry (EuS)1+δ(NbSe2)2 (δ ≈ 0.13) has been successfully synthesized. High-resolution transmission electron microscopy and powder X-ray diffraction confirm the misfit structure with (EuS)-(EuS) spacing of 18.30(1) Å. Magnetization, electrical resistivity, heat capacity, and thermal transport measurements show that the material is a heavily doped semiconductor or poor metal with a low thermal conductivity of ∼1 W/m K and an antiferromagnetic ordering transition at TN = 4.7 K. In contrast to the parent materials, the misfit is neither ferromagnetic nor superconducting down to T = 0.4 K. We find evidence of a field-driven transition to a ferromagnetic state due to reorientation of ferromagnetic EuS layers at μoH = 0.5 T at T = 2 K.

Anomalous Hall effects in chiral superconductors

We report theoretical results for the electronic contribution to thermal and electrical transport for chiral superconductors belonging to even or odd-parity E1 and E2 representations of the tetragonal and hexagonal point groups. Chiral superconductors exhibit novel properties that depend on the topology of the order parameter and Fermi surface, and—as we highlight—the structure of the impurity potential. An anomalous thermal Hall effect is predicted and shown to be sensitive to the winding number, ν, of the chiral order parameter via Andreev scattering that transfers angular momentum from the chiral condensate to excitations that scatter off the random potential. For heat transport in a chiral superconductor with isotropic impurity scattering, i.e., point-like impurities, a transverse heat current is obtained for ν = ±1, but vanishes for |ν| > 1. This is not a universal result. For finite-size impurities with radii of order or greater than the Fermi wavelength, R ≥ ℏ/pf, the thermal Hall conductivity is finite for chiral order with |ν|≥ 2, and determined by a specific Fermi-surface average of the differential cross-section for electron-impurity scattering. Our results also provide quantitative formulae for analyzing and interpreting thermal transport measurements for superconductors predicted to exhibit broken time-reversal and mirror symmetries.

A three-probe method for accurate nanoscale thermal transport measurements

Measurements of transport phenomena are constantly plagued by contact resistance, prohibiting the sample's intrinsic electrical or thermal conductivity from being accurately determined. This predicament is particularly severe in thermal transport measurements due to the inability to meet similar impedance requirements for a four-probe method used in electrical resistance measurements. Here, we invent a three-probe measurement method that makes an accurate determination of thermal conductivity possible for nanomaterials. Incorporating electron beam heating provided by a scanning electron microscope (SEM) on a diffusive thermal conductor not only quantifies the thermal contact resistance, which may introduce an error of more than 270% to a sample's thermal conductivity, but also eliminates several device uncertainties that may contribute an additional 17% error in a measurement. The method also enables local temperature measurements, revealing nanoscale structural variations unfound by SEM. The high accuracy of the technique would make standardization of nanoscale thermal transport measurement possible.

Moiré Pattern Controlled Phonon Polarizer Based on Twisted Graphene.

Twisted van der Waals materials featuring Moiré patterns present new design possibilities and demonstrate unconventional behaviors in electrical, optical, spintronic, and superconducting properties. However, experimental exploration of thermal transport across Moiré patterns has not been as extensive, despite its critical role in nanoelectronics, thermal management, and energy technologies. Here, thefirst experimental study is conducted on thermal transport across twisted graphene, demonstrating a phonon polarizer concept from the rotational misalignment between stacked layers. The direct thermal and acoustic measurements,structural characterizations, and atomistic modeling, reveal a modulation up to 631% in thermal conductance with various Moiré angles, while maintaining a high acoustic transmission. By comparing experiments with density functional theory and molecular dynamics simulations, mode-dependent phonon transmissions are quantified based on the angle alignment of graphene band structures and attributed to the coupling among flexural phonon modes. The agreement confirms the dominant tuning mechanisms in adjusting phonon transmission from high-frequency thermal modes while having negligible effects on low-frequency acoustic modes near Brillouin zone center. This study offers crucial insights into the fundamental thermal transport in Moiré structures, opening avenues for the invention of quantum thermal devices and new design methodologies based on manipulations of vibrational band structures and phonon spectra.

Novel wet transfer technology of manufacturing flexible suspended two-dimensional material devices

With the rise of two-dimensional (2D) materials, their excellent optical, electronic, and thermal properties different from bulk materials make them increasingly widely studied and commercialized. 2D materials’ exceptional physical properties and unique structures make them an ideal candidate for next-generation flexible and wearable devices. In this work, we created a manufacturing method to successfully transfer monolayer, bilayer, and trilayer graphene onto the flexible substrate, with trenches of micron size to suspend graphene. Thermal transport measurements have been characterized to prove the suspended region. The achievement of manufacturing 2D materials in suspended condition will allow us to study their intrinsic physical properties at a mechanical strain, as well as contribute to novel flexible and wearable electronic devices and sensors.

Bolometric detection of Josephson inductance in a highly resistive environment

The Josephson junction is a building block of quantum circuits. Its behavior, well understood when treated as an isolated entity, is strongly affected by coupling to an electromagnetic environment. In 1983, Schmid predicted that a Josephson junction shunted by a resistance exceeding the resistance quantum RQ = h/4e2 ≈ 6.45 kΩ for Cooper pairs would become insulating since the phase fluctuations would destroy the coherent Josephson coupling. However, recent microwave measurements have questioned this interpretation. Here, we insert a small Josephson junction in a Johnson-Nyquist-type setup where it is driven by weak current noise arising from thermal fluctuations. Our heat probe minimally perturbs the junction’s equilibrium, shedding light on features not visible in charge transport. We find that the Josephson critical current completely vanishes in DC charge transport measurement, and the junction demonstrates Coulomb blockade in agreement with the theory. Surprisingly, thermal transport measurements show that the Josephson junction acts as an inductor at high frequencies, unambiguously demonstrating that a supercurrent survives despite the Coulomb blockade observed in DC measurements.

Heat transfer modification in an unsteady laminar boundary layer subject to free-stream traveling waves

A laminar, thermal boundary layer was forced computationally by free-stream, traveling-wave velocity fluctuations and the effects on the wall heat flux and skin friction were measured as a function of the phase speed of the disturbances and the streamwise location along the developing flow. The heat flux modification due to the flow forcing was significantly higher than the corresponding skin friction enhancement, and the dependence of these two transport properties on the phase speed was qualitatively different. The skin friction modification exhibited a maximum at an optimal phase speed, which was explained in terms of the overlap of two distinct viscous layers within the boundary layer. The heat flux modification did not exhibit this maximum, although evidence was found to suggest such a maximum may occur with sufficient boundary layer development. Because the magnitude of the wall heat-flux modification scales quadratically with wave amplitude, traveling wave disturbances pose significant challenges for thermal transport measurements in periodically perturbed environments, like turbomachinery, but also new opportunities for the control of heat transfer.

Remarkable heat conduction mediated by non-equilibrium phonon polaritons.

Surface waves can lead to intriguing transport phenomena. In particular, surface phonon polaritons (SPhPs), which result from coupling between infrared light and optical phonons, have been predicted to contribute to heat conduction along polar thin films and nanowires1. However, experimental efforts so far suggest only very limited SPhP contributions2-5. Through systematic measurements of thermal transport along the same 3C-SiC nanowires with and without a gold coating on the end(s) that serves to launch SPhPs, here we show that thermally excited SPhPs can substantially enhance the thermal conductivity of the uncoated portion of these wires. The extracted pre-decay SPhP thermal conductance is more than two orders of magnitude higher than the Landauer limit predicted on the basis of equilibrium Bose-Einstein distributions. We attribute the notable SPhP conductance to the efficient launching of non-equilibrium SPhPs from the gold-coated portion into the uncoated SiC nanowires, which is strongly supported by the observation that the SPhP-mediated thermal conductivity is proportional to the length of the gold coating(s). The reported discoveries open the door for modulating energy transport in solids by introducing SPhPs, which can effectively counteract the classical size effect in many technologically important films and improve the design of solid-state devices.

Phonon non-equilibrium effects on interface thermal resistance between graphene and substrates

Accurate measurement and deep understanding of interfacial thermal transport through interfaces where two-dimensional (2D) materials are involved are crucial for efficient thermal management in nanodevices. However, there is still a large discrepancy in the measurement on the interfacial thermal resistance (ITR) at interfaces between 2D materials and substrates. In this study, two kinds of molecular dynamics techniques are utilized to investigate the ITR of graphene/silicon interfaces under steady-state and transient conditions. Our results indicate that, in both conditions, phonon non-equilibrium phenomena could lead to an overestimation of the interfacial thermal resistance. In the steady state, the overestimation of ITR arises from an exaggerated interfacial temperature difference when using specific vibrational modes as indicators of the sample temperature. In the transient regime, it is attributed to the extended thermal relaxation time of flexural acoustic modes in graphene caused by weak phonon coupling when recording the temperature evolution to extract the ITR. These findings provide a comprehensive understanding of thermal transport across the graphene/silicon interface, aiding in the optimization of graphene-based nanodevices. The study also underlines the necessity of considering the specific experimental setup and physical processes involved when interpreting ITR data obtained from measurements.

A low-temperature face-centered-cubic polymorph of Cu6GeWSe8 with a semiconductor-like conductivity

Hexagonal Cu6GeWSe8 (H-phase) with an intermediate band gap has been reported lately. In this paper, we show a low-temperature face-centered-cubic modification of Cu6GeWSe8 (C-phase), which crystallizes in the noncentrosymmetric space group F-43m with four formula in the cell of dimension a = 11.1372(2) Å. In the C-phase, double layers organized by MeSe4 (Me = Cu, Ge and W) tetrahedra alternately stack along the <111> direction. A weakly first-order or nearly second-order displacive phase transition from cubic to hexagonal polytypes undergoes initially at ∼ 440 °C upon increasing temperature. Electrical resistivity and Seebeck coefficient reveal a semiconductor-like conduction with holes as the predominant charge carriers. The semiconductivity is also supported by the almost zero electronic specific-heat coefficient γ. The mechanism of thermal conduction was analyzed by abstracting electronic and lattice thermal conductivities through thermal transport measurement and meanwhile the thermoelectric properties were characterized. The differences in band structures and formation energy between the two variants were studied by ab-initio calculations, which indicate that the H-phase is a semiconductor and the C-phase is a semimetal with low density of states, and the hexagonal modification is comparatively stable. The cubic polytype of Cu6GeWSe8 expands the Cu-Ge-W-Se system. A stereo phase diagram making reviews on the rich materials, and multiple crystallographic and electronic states in this system was established, which would be helpful to guide for seeking new materials and to probe the interplay between polymorphism and property in chalcogenide family.

Differential multi-probe thermal transport measurements of multi-walled carbon nanotubes grown by chemical vapor deposition

Carbon nanotubes (CNTs) are quasi-one dimensional nanostructures that display both high thermal conductivity for potential thermal management applications and intriguing low-dimensional phonon transport phenomena. In comparison to the advances made in the theoretical calculation of the lattice thermal conductivity of CNTs, thermal transport measurements of CNTs have been limited by either the poor temperature sensitivity of Raman thermometry technique or the presence of contact thermal resistance errors in sensitive two-probe resistance thermometry measurements. Here we report advances in a multi-probe measurement of the intrinsic thermal conductivity of individual multi-walled CNT samples that are transferred from the growth substrate onto the measurement device. The sample-thermometer thermal interface resistance is directly measured by this multi-probe method and used to model the temperature distribution along the contacted sample segment. The detailed temperature profile helps to eliminate the contact thermal resistance error in the obtained thermal conductivity of the suspended sample segment. A differential electro-thermal bridge measurement method is established to enhance the signal-to-noise ratio and reduce the measurement uncertainty by over 40%. The obtained thermal resistances of multiple suspended segments of the same MWCNT samples increase nearly linearly with increasing length, revealing diffusive phonon transport as a result of phonon-defect scattering in these MWCNT samples. The measured thermal conductivity increases with temperature and reaches up to 390 ± 20 W m−1 K−1 at room temperature for a 9-walled MWCNT. Theoretical analysis of the measurement results suggests submicron phonon mean free paths due to extrinsic phonon scattering by extended defects such as grain boundaries. The obtained thermal conductivity is decreased by a factor of 3 upon electron beam damage and surface contamination of the CNT sample.

Spin‐Phonon Scattering‐Induced Low Thermal Conductivity in a van der Waals Layered Ferromagnet Cr2Si2Te6

AbstractLayered van der Waals (vdW) magnets are prominent playgrounds for developing magnetoelectric, magneto‐optic, and spintronic devices. In spintronics, particularly in spincaloritronic applications, low thermal conductivity (κ) is highly desired. Herein, by combining thermal transport measurements with density functional theory calculations, this study demonstrates low κ down to 1 W m−1 K−1 in a typical vdW ferromagnet Cr2Si2Te6. In the paramagnetic state, development of magnetic fluctuations way above Tc = 33 K strongly reduces κ via spin‐phonon scattering, leading to low κ ≈ 1 W m−1 K−1 over a wide temperature range, in comparable to that of amorphous silica. In the magnetically ordered state, emergence of resonant magnon‐phonon scattering limits κ below ≈2 W m−1 K−1, which will be three times larger if magnetic scatterings are absent. Application of magnetic fields strongly suppresses the spin‐phonon scattering, giving rise to large enhancements of κ. This study's calculations well capture these complex behaviors of κ by taking the temperature‐ and magnetic‐field‐dependent spin‐phonon scattering into account. Realization of low κ, which is easily tunable by magnetic fields in Cr2Si2Te6, may further promote spincaloritronic applications of vdW magnets. This study's theoretical approach may also provide a generic understanding of spin‐phonon scattering, which appears to play important roles in various systems.

Thermal optimization and magnetization of nanofluid under shape effects of nanoparticles

The measurements of thermal transport are complex to optimize from high temperatures; this is because increased thermal-management performance have typically been accompanied for the sake of applicability in thermal barriers and heat dissipation. In this manuscript, an investigation for the flow of Brinkman nanofluid is carried out in which shapes of nanoparticles are suspended in ethylene glycol and their thermophysical properties have been emphasized. In order to have an optimized heat and mass transfer, the mathematical modeling is traced out for temperature, concentration and velocity profiles through non-singularized fractional technique. The analytical solutions for temperature, concentration and velocity profiles have been derived by invoking integral transforms. Special analytical solutions have been traced out for Stoke's first and second problems by varying boundary conditions of the problem. The rheological parameters have shown the pertinent effects on the basis of numerical variations and similarities. The results suggested that velocity of ethylene glycol-alumina is slower than ethylene glycol-copper, ethylene glycol-gold and ethylene glycol-silver during non-magnetization process.

Picosecond magneto-optic thermometry measurements of nanoscale thermal transport in AlN thin films

The thermal conductivity Λ of wide bandgap semiconductor thin films, such as AlN, affects the performance of high-frequency devices, power devices, and optoelectronics. However, accurate measurements of Λ in thin films with sub-micrometer thicknesses and Λ &amp;gt; 100 W m−1 K−1 is challenging. Widely used pump/probe metrologies, such as time–domain thermoreflectance (TDTR) and frequency–domain thermoreflectance, lack the spatiotemporal resolution necessary to accurately quantify thermal properties of sub-micrometer thin films with high Λ. In this work, we use a combination of magneto-optic thermometry and TiN interfacial layers to significantly enhance the spatiotemporal resolution of pump/probe thermal transport measurements. We use our approach to measure Λ of 100, 400, and 1000 nm AlN thin films. We coat AlN thin films with a ferromagnetic thin-film transducer with the geometry of (1 nm-Pt/0.4 nm-Co)x3/(2 nm-TiN). This PtCo/TiN transducer has a fast thermal response time of &amp;lt;50 ps, which allows us to differentiate between the thermal response of the transducer, AlN thin film, and substrate. For the 100, 400, and 1000 nm thick AlN films, we determine Λ to be 200 ± 80, 165 ± 35, and 300 ± 70 W m−1 K−1, respectively. We conclude with an uncertainty analysis that quantifies the errors associated with pump/probe measurements of thermal conductivity, as a function of transducer type, thin-film thermal conductivity, and thin-film thickness. Time resolved magneto-optic Kerr effect experiments can measure films that are three to five times thinner than is possible with standard pump/probe metrologies, such as TDTR. This advance in metrology will enable better characterization of nanoscale heat transfer in high thermal conductivity material systems like wide bandgap semiconductor heterostructures and devices.

Charge fluctuations above TCDW revealed by glasslike thermal transport in kagome metals AV3Sb5 (A=K,Rb,Cs)

We present heat capacity, electrical, and thermal transport measurements of kagome metals $A{\mathrm{V}}_{3}{\mathrm{Sb}}_{5}$ $(A=\mathrm{K},\mathrm{Rb},\mathrm{Cs})$. In all three compounds, the development of short-range charge fluctuations above the charge density wave (CDW) transition temperature ${T}_{\mathrm{CDW}}$ strongly scatters phonons via the electron-phonon coupling, leading to the glasslike phonon heat transport, i.e., the phonon thermal conductivity decreases weakly upon cooling. Once the long-range charge order sets in below ${T}_{\mathrm{CDW}}$, short-range charge fluctuations are quenched, and the typical Umklapp scattering dominated phonon heat transport is recovered. The charge-fluctuations-induced glasslike phonon thermal conductivity implies sizable electron-phonon coupling in $A{\mathrm{V}}_{3}{\mathrm{Sb}}_{5}$.

Transport properties of CrP

CrP has many exotic physical properties due to a four-fold degenerate band crossing at the Y point of the Brillouin zone, which is protected by the nonsymmorphic symmetry of the space group. We carried out the heat capacity, electrical and thermal transport measurements on CrP and extracted the electron thermal conductivity. Due to the difference in energy and momentum relaxation time during electron–phonon inelastic scattering, the normalized Lorentz number decreases below about 160 K. Below 25.6 K, the normalized Lorentz number begins to recover, which is due to the dominance of elastic scattering between electrons and defects at low temperatures.

A universal sensitivity matrix reduction technique (SMART) to uncover governing thermal transport relationships

Sensitivity analysis is a powerful technique to analyze the behaviors of models and experimental data. Most state-of-the-art characterization techniques rely on fitting experimental data to a theoretical multivariate model that can have multiple unknown properties other than the target property. Often, these unknowns cannot be measured separately and are unavoidably fitted for their values simultaneously using a single set of measured data. No rigorous method exists to evaluate their accuracy and elucidate the inherent governing relationships that can change with different measurement conditions. Here, we formulate a systematic approach based on sensitivity analysis to obtain these hidden relationships in a complex multivariate model. Criteria for simultaneously estimating the values of multiple unknowns are also clarified. We demonstrate this approach for a transient thermal transport measurement technique. This approach is versatile and can be applied to most measurement techniques in various disciplines that involve multivariate theoretical models to improve their measurement accuracy and throughput.

Prediction of hot zone-center optical phonons in laser-irradiated molybdenum disulfide with a semiconductor multitemperature model

A previous multitemperature model (MTM) resolving phonon temperatures at the polarization level and measurements have uncovered remarkable nonequilibrium among different phonon polarizations in laser-irradiated graphene and metals. Here, we develop a semiconductor-specific MTM (SC-MTM) by including electron-hole pair generation, diffusion, and recombination, and show that a phonon polarization-level model does not yield observable polarization-based nonequilibrium in laser-irradiated molybdenum disulfide (${\mathrm{MoS}}_{2}$). In contrast, appreciable nonequilibrium is predicted between zone-center optical phonons and the other modes. The momentum-based nonequilibrium ratio is found to increase with decreasing laser spot size and interaction with a substrate. This finding is relevant to the understanding of the energy relaxation process in two-dimensional optoelectronic devices and Raman measurements of thermal transport.

Developing compact tuning fork thermometers for sub-mK temperatures and high magnetic fields

There is a growing demand for experiments on calorimetric and thermal transport measurements at ultra-low temperatures below 1 mK and high magnetic fields up to 16 T. Particularly, milligram-sized solid samples are of great interest. We present the development of scalable thermometers based on quartz tuning fork resonators immersed in liquid 3He and adapt hydrodynamic models to provide an improved description of temperature dependence in the high viscosity regime between 1 and 10mK. We demonstrate successful thermometer operation and discuss the feasibility of fast and compact thermal probes suitable for small samples.

Direct determination of the topological thermal conductance via local power measurement

Thermal conductance measurements are sensitive to both charge and chargeless energy flow and are an essential measurement technique in condensed-matter physics. For two-dimensional topological insulators, the determination of thermal Hall (transverse) conductance and thermal longitudinal conductance is crucial for the understanding of topological order in the underlying state. Such measurements have not been accomplished, even in the extensively studied quantum Hall effect regime. Here we report a local power measurement technique that we use to reveal the topological thermal Hall conductance, going beyond the ubiquitous two-terminal conductance. For example, we show that the thermal Hall conductance is approximately zero in the v = 2/3 particle–hole conjugated state. This is in contrast to the two-terminal thermal conductance that gives a non-universal value that depends on the extent of thermal equilibration between the counter-propagating edge modes. Moreover, we demonstrate the utility of this technique in studying the power carried by the current fluctuations of a partitioned edge mode with an out-of-equilibrium distribution. Careful thermal transport measurements identify the topological nature of transverse thermal conductance in the fractional quantum Hall regime.