Modifying phonon thermal conductivity in nanomaterials is important not only for fundamental research but also for practical applications. However, the experiments on tailoring the thermal conductivity in nanoscale, especially in two-dimensional materials, are rare due to technical challenges. In this work, we demonstrate in-situ thermal conduction measurement of MoS2 and find that its thermal conductivity can be continuously tuned to a required value from crystalline to amorphous limits. The reduction of thermal conductivity is understood from phonon-defects scatterings that decrease the phonon transmission coefficient. Beyond a threshold, a sharp drop in thermal conductivity is observed, which is believed to be a crystalline-amorphous transition. Our method and results provide guidance for potential applications in thermoelectrics, photoelectronics, and energy harvesting where thermal management is critical with further integration and miniaturization.
We reported the basal-plane thermal conductivity in exfoliated bilayer hexagonal boron nitride h-BN that was measured using suspended prepatterned microstructures. The h-BN sample suitable for thermal measurements was fabricated by dry-transfer method, whose sample quality, due to less polymer residues on surfaces, is believed to be superior to that of PMMA-mediated samples. The measured room temperature thermal conductivity is around 484 Wm-1K-1(+141 Wm-1K-1/ -24 Wm-1K-1) which exceeds that in bulk h-BN, providing experimental observation of the thickness-dependent thermal conductivity in sus…
Establishment of a new technique or extension of an existing technique for thermal and thermoelectric measurements to a more challenging system is an important task to explore the thermal and thermoelectric properties of various materials and systems. The bottleneck lies in the challenges in measuring the thermal contact resistance. In this work, we applied electron beam self-heating technique to derive the intrinsic thermal conductivity of suspended Molybdenum Disulfide (MoS2) ribbons and the thermal contact resistance, with which the interfacial thermal resistance between few-layer MoS2 and …
We investigate the thermal conductivity of suspended graphene as a function of the density of defects, ND, introduced in a controllable way. Graphene layers are synthesized using chemical vapor deposition, transferred onto a transmission electron microscopy grid, and suspended over ~7.5-micrometer size square holes. Defects are induced by irradiation of graphene with the low-energy electron beam (20 keV) and quantified by the Raman D-to-G peak intensity ratio. As the defect density changes from 2.0x10^10 cm-2 to 1.8x10^11 cm-2 the thermal conductivity decreases from ~(1.8+/-0.2)x10^3 W/mK to ~…
Building smaller transistors with enhanced functionality is critical in extending the limits of Moores law and meeting the demands of the electronics industry. Here we demonstrate transistor operation in a suspended single carbon nanotube (CNT) using feedback-enabled radiation pressure of a near-field focused laser that enabled significant changes in conductivity of the CNT. Further, using in-situ tip-enhanced Raman spectroscopy, we show that the change in conductivity of over five orders in magnitude is accompanied by self-induced defect states within the CNT. The entire structure is less tha…
We investigate the dynamical control of the heat flux exchanged in near-field regime between a membrane made with a phase-change material and a substrate when the temperature of the membrane is tuned around its critical value. We show that in interaction with an external source of thermal radiation, this system is multistable and behaves as a thermal transistor, being able to dynamically modulate and even amplify super-Planckian heat fluxes. This behavior could be used to dynamically control heat fluxes exchanged at the nanoscale in systems out of thermal equilibrium and to process thermal inf…
Thermal properties of suspended single-layer graphene membranes are investigated by characterization of their mechanical motion in response to a high-frequency modulated laser. A characteristic delay time $τ$ between the optical intensity and mechanical motion is observed, which is attributed to the time required to raise the temperature of the membrane. We find, however, that the measured time constants are significantly larger than the predicted ones based on values of the specific heat and thermal conductivity. In order to explain the discrepancy between measured and modeled tau, a model is…
We measure the thermal time constants of suspended single layer molybdenum disulfide drums by their thermomechanical response to a high-frequency modulated laser. From this measurement the thermal diffusivity of single layer MoS$_2$ is found to be 1.14 $\times$ 10$^{-5}$ m$^2$/s on average. Using a model for the thermal time constants and a model assuming continuum heat transport, we extract thermal conductivities at room temperature between 10 to 40 W/(m$\cdot$K). Significant device-to-device variation in the thermal diffusivity is observed. Based on statistical analysis we conclude that thes…
Mapping the thermal transport properties of materials at the nanoscale is of critical importance for optimizing heat conduction in nanoscale devices. Several methods to determine the thermal conductivity of materials have been developed, most of them yielding an average value across the sample, thereby disregarding the role of local variations. Here, we present a method for the spatially-resolved assessment of the thermal conductivity of suspended graphene by using a combination of confocal Raman thermometry and a finite-element calculations-based fitting procedure. We demonstrate the working …
Wiedemann-Franz Relation and Thermal-transistor Effect in Suspended Graphene
我们提取实验的电子热导率,$K_{e}$,在悬浮的石墨烯,我们掺杂使用背栅电极。我们利用两点直流电子输运在低偏置电压和中间温度(50 - 160 K),电子和晶格温度去耦。热导率与电荷电导率乘以温度成比例,证实了悬浮石墨烯中服从Wiedemann-Franz关系。我们提取Lorenz系数的估计值为1.1至1.7 $\times 10^{-8}$ W $Ω$ K $^{-2}$。$K_e$显示出晶体管效应,并且当电荷载流子密度在$\approx$ 0.5至1.8 $\times 10^{11}$ cm $^{-2}$范围内时,可以用背栅以大于2的因子进行调谐。
Recent experiments have shown surprisingly large thermal time constants in suspended graphene ranging from 10 to 100 ns in drums with a diameter ranging from 2 to 7 microns. The large time constants and their scaling with diameter points towards a thermal resistance at the edge of the drum. However, an explanation of the microscopic origin of this resistance is lacking. Here, we show how phonon scattering at a kink in the graphene, e.g. formed by sidewall adhesion at the edge of the suspended membrane, can cause a large thermal time constant. This kink strongly limits the fraction of flexural …
Monolayer WS2 has been a competitive candidate in electrical and optoelectronic devices due to its superior optoelectronic properties. To tackle the challenge of thermal management caused by the decreased size and concentrated heat in modern ICs, it is of great significance to accurately characterize the thermal conductivity of the monolayer WS2, especially with substrate supported. In this work, the dual-wavelength flash Raman method is used to experimentally measure the thermal conductivity of the suspended and the Si/SiO2 substrate supported monolayer WS2 at a temperature range of 200 K - 4…
Suspended graphene membrane presents a particular structure with fundamental interests and applications in nanomechanics, thermal transport and optoelectronics. Till now, the commonly used geometries are still quite simple and limited to the microscale. We propose here to overcome this problem by making nanostructures in suspended epitaxial bilayer graphene on a large scale and with a large variety of geometries. We also demonstrate a new hybrid thin film of SiC-graphene with an impressive robustness. Since the mechanics and thermal dissipation of a suspended graphene membrane are strongly rel…
The electrical response of two-dimensional electron gas to vibrations of a nanomechanical cantilever containing it is studied. Vibrations of perpendicularly oriented cantilevers are experimentally shown to change oppositely the conductivity near their bases. This indicates the piezoelectric nature of electromechanical coupling. A physical model is developed, which quantitatively explains the experiment. It shows that the main origin of the conductivity change is a rapid change in the mechanical stress on the boundary between suspended and non-suspended areas, rather than the stress itself.
Recent theory has predicted large temperature differences between the in-plane (LA and TA) and out-of-plane (ZA) acoustic phonon baths in locally-heated suspended graphene. To verify these predictions, and their implications for understanding the nonequilibrium thermodynamics of 2D materials, experimental techniques are needed. Here, we present a method to determine the acoustic phonon bath temperatures from the frequency-dependent mechanical response of suspended graphene to a power modulated laser. The mechanical motion reveals two counteracting contributions to the thermal expansion force, …
Studying thermal transport at the nanoscale poses formidable experimental challenges due both to the physics of the measurement process and to the issues of accuracy and reproducibility. The laser-induced transient thermal grating (TTG) technique permits non-contact measurements on nanostructured samples without a need for metal heaters or any other extraneous structures, offering the advantage of inherently high absolute accuracy. We present a review of recent studies of thermal transport in nanoscale silicon membranes using the TTG technique. An overview of the methodology, including an anal…
We investigate the role that nonlinearity in the interatomic potential has on the thermal conductance of a suspended nanoribbon when it is subjected to a longitudinal strain. To focus on the first cubic and quartic nonlinear terms of a general potential, we propose an atomic system based on an $α$-$β$ Fermi-Pasta-Ulam nearest neighbor interaction. We perform classical molecular dynamics simulations to investigate the contribution of longitudinal, transversal and flexural modes to the thermal conductance as a function of the $α$-$β$ parameters and the applied strain. We compare the cases where …
We report a record low thermal conductivity in polycrystalline MoS2 obtained by varying grain sizes and orientations in ultrathin films. By optimizing the sulphurisation parameters of nanometre-thick Mo layer, we could grow MoS2 films with tuneable morphologies. The thermal conductivity is extracted from a Raman laser power-dependent study on suspended samples. The lowest value of thermal conductivity of 0.27 Wm-1K-1, which reaches a similar value as teflon, is obtained in a polycrystalline sample formed by a combination of horizontally and vertically oriented grains, with respect to the bulk …
We evaluate the impact of acoustic Mie resonance in nanoparticles on the thermal conductivity of semiconductor and polymer composites. By appropriately choosing the bulk modulus and density, and selecting the size of the nanoparticle to align the Mie resonances with the dominant portion of the thermal conductivity spectrum, we show that large reductions in thermal conductivity are achievable with dilute concentrations of nanoparticles. In semiconductor alloys, where the spectral thermal conductivity is known, our model can explain the steep reductions in thermal conductivity observed previousl…
In this paper, we have studied the effect of short branches on the thermal conductivity of a polyethylene (PE) chain. With a reverse non-equilibrium molecular dynamics method applied, thermal conductivities of the pristine PE chain and the PE-ethyl chain are simulated and compared. It shows that the branch has a positive effect to decrease the thermal conductivity of a PE chain. The thermal conductivity of the PE-ethyl chain decreases with the number density increase of the ethyl branches, until the density becomes larger than about 8 ethyl per 200 segments, where the thermal conductivity satu…
Polymers are usually considered as thermal insulators and their applications are limited by their low thermal conductivity. However, recent studies showed that certain polymers have surprisingly high thermal conductivity, some of which are comparable to that in poor metals or even silicon. In this review, we outline the experimental achievements and theoretical progress of thermal transport in polymers and their nanocomposites. The open questions and challenges of existing theories are discussed. Special attention is given to the mechanism of thermal transport, the enhancement of thermal condu…
Nanostructured silicon is a promising material for thermoelectric conversion, because the thermal conductivity in silicon nanostructures can be strongly reduced with respect to that of bulk materials. We present thermal conductivity measurements, performed with the 3$ω$ technique, of suspended monocrystalline silicon thin films (nanomembranes or nanoribbons) with smooth and rough surfaces. We find evidence for a significant effect of surface roughness on phonon propagation: the measured thermal conductivity for the rough structures is well below that predicted by theoretical models which take …
Investigating thermal transport in van der Waals heterostructure is of scientific interest and practical importance for their applications in a broad range. In this work, thermal conductivity of one-dimensional heterostructure consisting of carbon and boron nitride nanotubes is systematically investigated via molecular dynamics simulations. Thermal conductivity is found to have strong dependences on temperature, length and diameter. In addition, the axial strain and intensity of van der Waals interaction are demonstrated to be able to modulate thermal conductivity up to about 43% and 37%, resp…
Niobium pentoxide (Nb2O5) has been extensively reported for applications of electrochemical energy storage, memristors, solar cells, light emitting diodes (LEDs), and electrochromic devices. The thermal properties of Nb2O5 play a critical role in device performance of these applications. However, very few studies on the thermal properties of Nb2O5 have been reported and a fundamental understanding of heat transport in Nb2O5 is still lacking. The present work closes this gap and provides the first study of thermal conductivity of amorphous Nb2O5 thin films. Ultralow thermal conductivity is obse…
The reduction of the thermal conductivity in nanostructures opens up the possibility of exploiting for thermoelectric purposes also materials such as silicon, which are cheap, available and sustainable but with a high thermal conductivity in their bulk form. The development of thermoelectric devices based on these innovative materials requires reliable techniques for the measurement of thermal conductivity on a nanometric scale. The approximations introduced by conventional techniques for thermal conductivity measurements can lead to unreliable results when applied to nanostructures, because h…
Computationally efficient modeling of the thermal conductivity of materials is crucial to thorough experimental planning and theoretical understanding of thermal properties. We present a modeling approach in this work that utilizes frequency-dependent effective medium to calculate lattice thermal conductivity of nanostructured solids. The method accurately predicts a significant reduction in the thermal conductivity of nanostructured Si80Ge20 systems, along with previous reported thermal conductivities in nanowires and nanoparticles-in-matrix materials. We use our model to gain insight into th…
The measured frequencies and intensities of different first- and second- order Raman peaks of suspended graphene are used to show that optical phonons and different acoustic phonon polarizations are driven out of local equilibrium inside a sub-micron laser spot. The experimental results are correlated with a first principles-based multiple temperature model to suggest a considerably lower equivalent local temperature of the flexural phonons than those of other phonon polarizations. The finding reveals weak coupling between the flexural modes with hot electrons and optical phonons. Since the ul…
We describe Raman spectroscopy based method of measuring thermal conductivity of thin films, and review significant results achieved with this technique pertinent to graphene and other two-dimensional materials. The optothermal Raman method was instrumental for the discovery of unique heat conduction properties of graphene. In this method, Raman spectroscopy is used to determine the local temperature of the sample while the excitation laser is utilized as a heat source. The success of Raman spectroscopy in investigating thermal conductivity of suspended graphene and graphene-based thin films m…