One Stone Two Birds: Anomalously Enhancing the Cross-Plane and In-Plane Heat Transfer in 2D/3D Heterostructures by Defects Engineering.

This study addresses a crucial challenge in two-dimensional (2D) material-based electronic devices-inefficient heat dissipation across the van der Waals (vdW) interface connecting the 2D material to its three-dimensional (3D) substrate. The objective is to enhance the interfacial thermal conductance (ITC) of 2D/3D heterostructures without compromising the intrinsic thermal conductivities (κ) of 2D materials. Using 2D-MoS2/3D-GaN as an example, a novel strategy to enhance both the ITC across 2D/3D interface and κ of 2D material is proposed by introducing a controlled concentration (ρ) of vacancy defects to substrate's bottom surface. Molecular dynamics simulations demonstrate a notable 2.1-fold higher ITC of MoS2/GaN at ρ = 4% compared to the no-defective counterpart, along with an impressive 56% enhancement in κ of MoS2 compared to the conventional upper surface modification approaches. Phonon dynamics analysis attributes the ITC enhancement to increased phonon coupling between MoS2 and GaN, resulting from polarization conversion and hybridization of phonons at the defective surface. Spectral energy density analysis affirms that the improved κ of MoS2 directly results from the proposed strategy, effectively reducing phonon scattering at the interface. This work provides an effective approach for enhancing heat transfer in 2D/3D vdW heterostructures, promisingly advancing electronics' heat dissipation.

Phonon dynamic behaviors induced by amorphous layers at heterointerfaces.

An amorphous layer is commonly found at the interfaces of heterostructures due to lattice and thermal mismatch between dissimilar materials. While existing research has explored the impact of these layers on interfacial thermal transport, a comprehensive understanding of the underlying microscopic mechanisms remains essential for advancing thermal nanodevice development. Through phonon wave packet simulations, we investigated the dynamic behaviors of phonons crossing the amorphous interlayer at the GaN/AlN interface from the mode level. Our results highlight the amorphous layer's capability to notably adjust the polarization properties of incoming phonons, culminating in phonon localization. By examining transmission outcomes on a per-mode basis, we demonstrate the amorphous layer's impediment on phonon transport. Notably, this resistance escalates with an increase in the amorphous layer thickness (L), with certain high-frequency TA phonons showing unexpectedly high transmissivity due to polarization conversion and inelastic scattering at the amorphous interface. In addition, we observe that the amorphous layer prompts multiple reflections of incident phonons, instigating discernible from the two-beam interference equation. Finally, in pursuit of enhanced phonon transport, we employ annealing techniques to optimize the interface morphology, leading to the recrystallization of the amorphous layer. This optimization yields a substantial enhancement of interfacial thermal conductance by up to 38% for L = 3 nm.

Flexible Te/PEDOT:PSS thin films with high thermoelectric power factor and their application as flexible temperature sensors.

Flexible, lightweight, and low-cost thermoelectric thin films are promising for self-powered wearable electronics and sensors. In this work, we report on flexible Te nanostructures/PEDOT:PSS composite thin films with high power factor and their application as flexible temperature sensors. Te nanostructures with high crystallinity and high aspect ratios were synthesized through an environmentally friendly method without using highly toxic chemicals. Individual Te nanostructures achieve a thermoelectric figure of merit (ZT) of 0.13 at 300 K, indicating good potential as inorganic fillers for nanostructures/polymer hybrid materials. Based on the synthesized Te nanostructures, flexible p-type Te/PEDOT:PSS thin films were fabricated through a simple dilution and vacuum filtration method. The power factor of the as-prepared composite thin film outperforms that of either a Te or DMSO-treated PEDOT:PSS thin film, and importantly, it can be further enhanced to 149 µW m-1 K-2 by hot pressing, which is nearly threefold enhancement compared to the values reported for the vacuum-filtered flexible Te/PEDOT:PSS thin films in the literature. The hot-pressed composite thin film shows high flexibility with the electrical conductivity remaining almost unchanged after 1000 bending cycles under a bending radius of 5 mm. Flexible temperature sensors were fabricated based on the hot-pressed Te/PEDOT:PSS thin film, which exhibited high sensitivity in detecting temperature stimuli. The developed temperature sensors were applied onto a two-finger flexible mechanical claw for identifying hot/cold objects in robotic grasping. This work demonstrates an effective approach to enhance the thermoelectric power factor of flexible Te nanostructures/polymer composites and their promising application in flexible thermal sensing.

Atomic-Scale Surface Engineering for Giant Thermal Transport Enhancement Across 2D/3D van der Waals Interfaces.

Heat dissipation in two-dimensional (2D) material-based electronic devices is a critical issue for their applications. The bottleneck for this thermal issue is inefficient for heat removal across the van der Waals (vdW) interface between the 2D material and its supporting three-dimensional (3D) substrate. In this work, we demonstrate that an atomic-scale thin amorphous layer atop the substrate surface can remarkably enhance the interfacial thermal conductance (ITC) of the 2D-MoS2/3D-GaN vdW interface by a factor of 4 compared to that of the untreated crystalline substrate surface. Meanwhile, the ITC can be broadly manipulated through adjusting substrate surface roughness. Phonon dynamic and heat flux spectrum analyses show that this giant enhancement is attributed to the increased phonon densities and channels at the interfaces and enhanced phonon coupling. The slight surface fluctuation in MoS2 and the increased diffuse interfacial scattering facilitate energy transfer from MoS2's in-plane phonons to its out-of-plane phonons and then to the substrate. In addition, it is further found that the substrate and its surface topology can dramatically influence the thermal conductivity of MoS2 due to the reduction of phonon relaxation time, especially for low-frequency acoustic phonons. This study elucidates the effects of the amorphous surface of the substrate on thermal transport across 2D/3D vdW interfaces and provides a new dimension to aid in the heat dissipation of 2D-based electronic devices via atomic-scale surface engineering.

Chemically Switchable n-Type and p-Type Conduction in Bismuth Selenide Nanoribbons for Thermoelectric Energy Harvesting.

Realizing switchable n-type and p-type conduction in bismuth selenide (Bi2Se3), a traditional thermoelectric material and a topological insulator, is highly beneficial for the development of thermoelectric devices and also of great interest for spintronics and quantum computing. In this work, switching between n-type and p-type conduction in single Bi2Se3 nanoribbons is achieved by a reversible copper (Cu) intercalation method. Density functional theory calculations reveal that such a switchable behavior arises from the electronic band structure distortion caused by the high-concentration Cu intercalation and the Cu substitution for Bi sites in the host lattice. A proof-of-concept in-plane thermoelectric generator is fabricated with one pair of the pristine n-type and intercalated p-type Bi2Se3 nanoribbons on a microfabricated device, which gives rise to an open-circuit voltage of 4.8 mV and a maximum output power of 0.3 nW under a temperature difference of 29.2 K. This work demonstrates switchable n-type and p-type electrical conduction in Bi2Se3 nanoribbons via a facile chemical approach and the practical application of nanoribbons in a thermoelectric device.

Effective Lorenz Number of the Point Contact between Silver Nanowires.

Electrical and thermal transport through metal point contacts, a key issue in the design and operation of various engineering devices, is of great recent interest. The effective Lorenz number (L), which relates the thermal to electrical conductance of point contacts, could provide valuable information on the relative contribution of electrons and phonons to thermal transport. Through measuring electrical and thermal transport across point contacts between silver nanowires, we report that L significantly deviates from the Sommerfeld value by up to 5.2 times and exhibits nonmonotonic variation with temperature. Analyses show that these observations are due to the more important phonon contribution to the thermal conductance of the point contact as Sharvin resistance greatly hinders electron transport, which is further confirmed by the size dependence of L with a higher value for a smaller contact size. These results provide critical insights into engineering designs involving point contacts between metal nanostructures.

A setup for measuring the Seebeck coefficient and the electrical resistivity of bulk thermoelectric materials.

This paper presents a setup for measuring the Seebeck coefficient and the electrical resistivity of bulk thermoelectric materials. The sample holder was designed to have a compact structure and can be directly mounted in a standard cryostat system for temperature-dependent measurements. For the Seebeck coefficient measurement, a thin bar-shaped sample is mounted bridging two copper bases; and two ceramic heaters are used to generate a temperature gradient along the sample. Two type T thermocouples are used to determine both temperature and voltage differences between two widely separated points on the sample. The thermocouple junction is flattened into a disk and pressed onto the sample surface by using a spring load. The flexible fixation method we adopted not only simplifies the sample mounting process but also prevents thermal contact deterioration due to the mismatch of thermal expansion coefficients between the sample and other parts. With certain modifications, the sample holder can also be used for four-probe electrical resistivity measurements. High temperature measurements are essential for thermoelectric power generation. The experimental system we developed is capable of measuring the Seebeck coefficient and the electrical resistivity of bulk thermoelectric materials in a wide temperature range from 80 to 500 K, which can be further extended to even higher temperatures. Measurements on two standard materials, constantan and nickel, confirmed the accuracy and the reliability of the system.

Significantly enhanced thermal conductivity of indium arsenide nanowires via sulfur passivation.

ABSTARCT: In this work, we experimentally investigated the effect of sulfur passivation on thermal transport in indium arsenide (InAs) nanowires. Our measurement results show that thermal conductivity can be enhanced by a ratio up to 159% by sulfur passivation. Current-voltage (I-V) measurements were performed on both unpassivated and S-passivated InAs nanowires to understand the mechanism of thermal conductivity enhancement. We observed a remarkable improvement in electrical conductivity upon sulfur passivation and a significant contribution of electrons to thermal conductivity, which account for the enhanced thermal conductivity of the S-passivated InAs nanowires.

Structure-induced variation of thermal conductivity in epoxy resin fibers.

The ability to control thermal conductivity is important in a wide variety of applications, especially in heat removal, heat insulation, and thermoelectric energy conversion. Herein, we reveal that the thermal conductivity of epoxy resin fibers increases on decreasing the fiber diameter and surpasses the bulk value (0.25 W m-1 K-1 at 300 K) for the fiber with a diameter of 211 nm. The variation of thermal conductivity in epoxy resin fibers can likely be attributed to their microstructure change-enhanced interface phonon scattering between amorphous and crystalline regions and the enhanced alignment of the molecular chain orientation.

Length-dependent thermal transport in one-dimensional self-assembly of planar π-conjugated molecules.

This work reports a thermal transport study in quasi-one-dimensional organic nanostructures self-assembled from conjugated planar molecules via π-π interactions. Thermal resistances of single crystalline copper phthalocyanine (CuPc) and perylenetetracarboxylic diimide (PTCDI) nanoribbons are measured via a suspended thermal bridge method. We experimentally observed the deviation from the linear length dependence for the thermal resistance of single crystalline ß-phase CuPc nanoribbons, indicating possible subdiffusion thermal transport. Interestingly, a gradual transition to the linear length dependence is observed with the increase of the lateral dimensions of CuPc nanoribbons. The measured thermal resistance of single crystalline CuPc nanoribbons shows an increasing trend with temperature. However, the trend of temperature dependence of thermal resistance is reversed after electron irradiation, i.e., decreasing with temperature, indicating that the single crystalline CuPc nanoribbons become 'amorphous'. Similar behavior is also observed for PTCDI nanoribbons after electron irradiation, proving that the electron beam can induce amorphization of single crystalline self-assembled nanostructures of planar π-conjugated molecules. The measured thermal resistance of the 'amorphous' CuPc nanoribbon demonstrates a roughly linear dependence on the nanoribbon length, suggesting that normal diffusion dominates thermal transport.

Thermoelectric characterization of individual bismuth selenide topological insulator nanoribbons.

Bismuth selenide (Bi2Se3) nanoribbons have attracted tremendous research interest recently to study the properties of topologically protected surface states that enable new opportunities to enhance the thermoelectric performance. However, the thermoelectric characterization of individual Bi2Se3 nanoribbons is rare due to the technological challenges in the measurements. One challenge is to ensure good contacts between the nanoribbon and electrodes in order to determine the thermal and electrical properties accurately. In this work, we report the thermoelectric characterization of individual Bi2Se3 nanoribbons via a suspended microdevice method. Through careful measurements, we have demonstrated that contact thermal resistance is negligible after the electron-beam-induced deposition (EBID) of platinum/carbon (Pt/C) composites at the contacts between the nanoribbon and electrodes. It is shown that the thermal conductivity of the Bi2Se3 nanoribbons is less than 50% of the bulk value over the whole measurement temperature range, which can be attributed to enhanced phonon boundary scattering. Our results indicate that intrinsic Bi2Se3 nanoribbons prepared in this work are highly doped n-type semiconductors, and therefore the Fermi level should be in the conduction band and no topological transport behavior can be observed in the intrinsic system.