Nanoscale Heat Transport of Vertically Aligned Carbon Nanotube Bundles for Thermal Management Applications.

Electronic devices continue to shrink in size while increasing in performance, making excess heat dissipation challenging. Traditional thermal interface materials (TIMs) such as thermal grease and pads face limitations in thermal conductivity and stability, particularly as devices scale down. Carbon nanotubes (CNTs) have emerged as promising candidates for TIMs because of their exceptional thermal conductivity and mechanical properties. However, the thermal conductivity of CNT films decreases when integrated into devices due to defects and bundling effects. This study employs a novel cross-sectional approach combining high-vacuum scanning thermal microscopy (SThM) with beam-exit cross-sectional polishing (BEXP) to investigate the nanoscale morphology and thermal properties of vertically aligned CNT bundles at low and room temperatures. Using appropriate thermal transport models, we extracted effective thermal conductivities of the vertically aligned nanotubes and obtained 4 W m-1 K-1 at 200 K and 37 W m-1 K-1 at 300 K. Additionally, non-negligible lateral thermal conductance between CNT bundles suggests more complex heat transfer mechanisms in these structures. These findings provide unique insights into nanoscale thermal transport in CNT bundles, which is crucial for optimizing novel thermal management strategies.

Nanoscale Imaging and Measurements of Grain Boundary Thermal Resistance in Ceramics with Scanning Thermal Wave Microscopy.

Material thermal conductivity is a key factor in various applications, from thermal management to energy harvesting. With microstructure engineering being a widely used method for customizing material properties, including thermal properties, understanding and controlling the role of extended phonon-scattering defects, like grain boundaries, is crucial for efficient material design. However, systematic studies are still lacking primarily due to limited tools. In this study, we demonstrate an approach for measuring grain boundary thermal resistance by probing the propagation of thermal waves across grain boundaries with a temperature-sensitive scanning probe. The method, implemented with a spatial resolution of about 100 nm on finely grained Nb-substituted SrTiO3 ceramics, achieves a detectability of about 2 × 10-8 K m2 W-1, suitable for chalcogenide-based thermoelectrics. The measurements indicated that the thermal resistance of the majority of grain boundaries in the STiO3 ceramics is below this value. While there are challenges in improving sensitivity, considering spatial resolution and the amount of material involved in the detection, the sensitivity of the scanning probe method is comparable to that of optical thermoreflectance techniques, and the method opens up an avenue to characterize thermal resistance at the level of single grain boundaries and domain walls in a spectrum of microstructured materials.

Unraveling the Impact of Boron Nitride and Silicon Nitride Nanoparticles on Thermoplastic Polyurethane Fibers and Mats for Advanced Heat Management.

The urgent challenges posed by the energy crisis, alongside the heat dissipation of advanced electronics, have embarked on a rising demand for the development of highly thermally conductive polymer composites. Electrospun composite mats, known for their flexibility, permeability, high concentration and orientational degree of conductive fillers, stand out as one of the prime candidates for addressing this need. This study explores the efficacy of boron nitride (BN) and its potential alternative, silicon nitride (SiN) nanoparticles, in enhancing the thermal performance of the electrospun composite thermoplastic polyurethane (TPU) fibers and mats. The 3D reconstructed models obtained from FIB-SEM imaging provided valuable insights into the morphology of the composite fibers, aiding the interpretation of the measured thermal performance through scanning thermal microscopy for the individual composite fibers and infrared thermography for the composite mats. Notably, we found that TPU-SiN fibers exhibit superior heat conduction compared to TPU-BN fibers, with up to a 6 °C higher surface temperature observed in mats coated on copper pipes. Our results underscore the crucial role of arrangement of nanoparticles and fiber morphology in improving heat conduction in the electrospun composites. Moreover, SiN nanoparticles are introduced as a more suitable filler for heat conduction enhancement of electrospun TPU fibers and mats, suggesting immense potential for smart textiles and thermal management applications.

Thermoelectric Limitations of Graphene Nanodevices at Ultrahigh Current Densities.

Graphene is atomically thin, possesses excellent thermal conductivity, and is able to withstand high current densities, making it attractive for many nanoscale applications such as field-effect transistors, interconnects, and thermal management layers. Enabling integration of graphene into such devices requires nanostructuring, which can have a drastic impact on the self-heating properties, in particular at high current densities. Here, we use a combination of scanning thermal microscopy, finite element thermal analysis, and operando scanning transmission electron microscopy techniques to observe prototype graphene devices in operation and gain a deeper understanding of the role of geometry and interfaces during high current density operation. We find that Peltier effects significantly influence the operational limit due to local electrical and thermal interfacial effects, causing asymmetric temperature distribution in the device. Thus, our results indicate that a proper understanding and design of graphene devices must include consideration of the surrounding materials, interfaces, and geometry. Leveraging these aspects provides opportunities for engineered extreme operation devices.

Preparation of multilayer samples for scanning thermal microscopy examination.

Thin film multilayer materials are very important for a variety of key technologies such as hard drive storage. However, their multilayered nature means it can be difficult to examine them after production and determining properties of individual layers is harder still. Here, methods of preparing multilayer samples for examination using scanning thermal microscopy are compared, showing that both a combination of mechanical and ion beam polishing, and ion beam milling to form a crater produce suitable surfaces for scanning thermal microscopy examination. However, the larger exposed surfaces of the ion beam milled crater are the most promising for distinguishing between the layers and comparison of their thermal transport properties.

Bridging a Gap in Thermal Conductivity and Heat Transfer in Hybrid Fibers and Yarns via Polyimide and Silicon Nitride Composites.

The pressing issues of the energy crisis and rapid electronics development have sparked a growing interest in the production of highly thermally conductive polymer composites. Due to the challenges related to the poor processability of hybrid materials and filler distribution to achieve high thermal conductivity, electrospinning is employed to create composite nanofibers and yarns using polyimide (PI) and thermally conductive silicon nitride (SiN) nanoparticles. The thermal performance of the individual nanofibers is evaluated using scanning thermal microscopy (SThM), providing significant insights into their heat transfer performance. Next, the nanofibers are applied as coatings on resistance wires to assess the thermal conductivity and insulation properties. Notably, the samples containing 35 wt.% of SiN exhibit a 25% increase in surface temperature. These innovative materials hold great promise as exceptional candidates for smart textiles and thermal management applications, addressing the growing demand for effective heat dissipation and regulation.

Realizing the Accurate Measurements of Thermal Conductivity over a Wide Range by Scanning Thermal Microscopy Combined with Quantitative Prediction of Thermal Contact Resistance.

Quantitative thermal performance measurements and thermal management at the micro-/nano scale are becoming increasingly important as the size of electronic components shrinks. Scanning thermal microscopy (SThM) is an emerging method with high spatial resolution that accurately reflects changes in local thermal signals based on a thermally sensitive probe. However, because of the unclear thermal resistance at the probe-sample interface, quantitative characterization of thermal conductivity for different kinds of materials still remains limited. In this paper, the heat transfer process considering the thermal contact resistance between the probe and sample surface is analyzed using finite element simulation and thermal resistance network model. On this basis, a mathematical empirical function is developed applicable to a variety of material systems, which depicts the relationship between the thermal conductivity of the sample and the probe temperature. The proposed model is verified by measuring ten materials with a wide thermal conductivity range, and then further validated by two materials with unknown thermal conductivity. In conclusion, this work provides the prospect of achieving quantitative characterization of thermal conductivity over a wide range and further enables the mapping of local thermal conductivity to microstructures or phases of materials.

Nanoscale Thermal Strain Engineering-Driven Ferroelastic Domain Evolution in CH3NH3PbI3 Perovskites.

A local thermal strain engineering approach via an ac-heated thermal probe was incorporated into methylammonium lead triiodide (MAPbI3) crystals and acts as a driving force for ferroic twin domain dynamics, local ion migration, and property tailoring. Periodically, striped ferroic twin domains and their dynamic evolutions were successfully induced by local thermal strain and high-resolution thermal imaging, giving decisive evidence of the ferroelastic nature in MAPbI3 perovskites at room temperature. Local thermal ionic imaging and chemical mappings demonstrate that domain contrasts are from local methylammonium (MA+) redistribution into the stripes of chemical segregation in response to the local thermal strain fields. The present results reveal an inherent coupling among local thermal strains, ferroelastic twin domains, local chemical-ion segregations, and physical properties and offer a potential path to improve the functionality of metal halide perovskite-based solar cells.

Probing the optical near-field of plasmonic nano structure using scanning thermal microscopy.

Scanning thermal microscopy (SThM) enables to obtain thermal characteristic information such as temperature and thermal conductivity from the signals obtained by scanning a thermometer probe over a sample surface. Particularly, the precise control of the thermometer probe makes it possible to study near-field radiative heat transfer by measuring the near-field thermal energy, which implies that when light is used as a local heat source, photothermal energy can be detected from the optical near-field by approaching the probe in the near-field region. In this study, SThM is applied to generate sub-wavelength near-field optical image in the plasmonic grating coupler. Herein, by controlling the surface plasmon polariton generation, we show that the dominant component of SThM signal is from the optical response rather than the thermal response. The obtained near-field optical images have a spatial resolution of 40 nm and signal to noise ratio of up to 19.8. In addition, field propagation images in theZ-direction can be visualised with the precise control of the distance between the thermometer probe and the sample.

High Spatial Resolution Thermal Mapping of Volatile Switching in NbOx-Based Memristor Using In Situ Scanning Thermal Microscopy.

Temperature mapping by in situ thermoreflectance thermal imaging (TRTI) or midwave infrared spectroscopy has played an important role in understanding the origins of threshold switching and the effect of insulator-metal transitions in oxide-based memrsitive devices. In this study, we use scanning thermal microscopy (SThM) as an alternative thermal mapping technique that offers high spatial resolution imaging (∼100 nm) and is independent of material. Specifically, SThM is used to map the temperature distribution in NbOx-based cross-bar and nanovia devices with Pt top electrodes. The measurements on cross-bar devices reproduce the current redistribution and confinement processes previously observed by TRTI but without the need to coat the electrodes with a material of high thermo-reflectance coefficient (e.g., Au), while those on the nanovia devices highlight the spatial resolution of the technique. The measured temperature distributions are compared with those obtained from physics-based finite-element simulations and suggest that thermal boundary resistance plays an important role in heat transfer between the active device volume and the top electrode.

Pico-Watt Scanning Thermal Microscopy for Thermal Energy Transport Investigation in Atomic Materials.

The thermophysical properties at the nanoscale are key characteristics that determine the operation of nanoscale devices. Additionally, it is important to measure and verify the thermal transfer characteristics with a few nanometer or atomic-scale resolutions, as the nanomaterial research field has expanded with respect to the development of molecular and atomic-scale devices. Scanning thermal microscopy (SThM) is a well-known method for measuring the thermal transfer phenomena with the highest spatial resolution. However, considering the rapid development of atomic materials, the development of an ultra-sensitive SThM for measuring pico-watt (pW) level heat transfer is essential. In this study, to measure molecular- and atomic-scale phenomena, a pico-watt scanning thermal microscopy (pW-SThM) equipped with a calorimeter capable of measuring heat at the pW level was developed. The heat resolution of the pW-SThM was verified through an evaluation experiment, and it was confirmed that the temperature of the metal line heater sample could be quantitatively measured by using the pW-SThM. Finally, we demonstrated that pW-SThM detects ultra-small differences of local heat transfer that may arise due to differences in van der Waals interactions between the graphene sheets in highly ordered pyrolytic graphite. The pW-SThM probe is expected to significantly contribute to the discovery of new heat and energy transfer phenomena in nanodevices and two-dimensional materials that have been inaccessible through experiments.

Quantitative Mapping of Unmodulated Temperature Fields with Nanometer Resolution.

Quantitative mapping of temperature fields with nanometric resolution is critical in various areas of scientific research and emerging technology, such as nanoelectronics, surface chemistry, plasmonic devices, and quantum systems. A key challenge in achieving quantitative thermal imaging with scanning thermal microscopy (SThM) is the lack of knowledge of the tip-sample thermal resistance (RTS), which varies with local topography and is critical for quantifying the sample temperature. Recent advances in SThM have enabled simultaneous quantification of RTS and topography in situations where the temperature field is modulated enabling quantitative thermometry even when topographical features cause significant variations in RTS. However, such an approach is not applicable to situations where the temperature modulation of the device is not readily possible. Here we show, using custom-fabricated scanning thermal probes (STPs) with a sharp tip (radius ∼25 nm) and an integrated heater/thermometer, that one can quantitatively map unmodulated temperature fields, in a single scan, with ∼7 nm spatial resolution and ∼50 mK temperature resolution in a bandwidth of 1 Hz. This is accomplished by introducing a modulated heat input to the STP and measuring the AC and DC responses of the probe's temperature which allow for simultaneous mapping of the tip-sample thermal resistance and sample surface temperature. The approach presented here─contact resistance resolved scanning thermal microscopy (CR-SThM)─can greatly facilitate temperature mapping of a variety of microdevices under practical operating conditions.

Thermal characterization of morphologically diverse copper phthalocyanine thin layers by scanning thermal microscopy.

Morphologically diverse copper phthalocyanine (CuPc) thin layers were thermally characterized by scanning thermal microscopy (SThM). The organic layers with thicknesses below 1 µm were deposited by physical vapor deposition in a high vacuum on the N-BK 7 glass substrates. Four set of samples were fabricated and studied. Atomic Force Microscopy imaging revealed strong differences in the surface roughness, mean grain size/height, as well as distances between grains for the CuPc layers. For quantitative thermal investigations, three active SThM operating modes were applied using either a Wollaston thermal probe (ThP) or KNT ThP as thermal probe heated with a DC, an AC (3ω-SThM) current or their combination (DC/AC SThM). Meanwhile, qualitative analysis was performed by thermal surface imaging. The results of this study revealed a correlation between the morphology and the local thermophysical properties of the examined CuPc thin layers. It was found that the heat transport properties in such layers will deteriorate with the increase of the surface roughness and porosity. Those results can be a valuable contribution to the further development of phthalocyanine-based devices.

Thermal Imaging of Block Copolymers with Sub-10 nm Resolution.

Thermal silicon probes have demonstrated their potential to investigate the thermal properties of various materials at high resolution. However, a thorough assessment of the achievable resolution is missing. Here, we present a probe-based thermal-imaging technique capable of providing sub-10 nm lateral resolution at a sub-10 ms pixel rate. We demonstrate the resolution by resolving microphase-separated PS-b-PMMA block copolymers that self-assemble in 11 to 19 nm half-period lamellar structures. We resolve an asymmetry in the heat flux signal at submolecular dimensions and assess the ratio of heat flux into both polymers in various geometries. These observations are quantitatively compared with coarse-grained molecular simulations of energy transport that reveal an enhancement of transport along the macromolecular backbone and a Kapitza resistance at the internal interfaces of the self-assembled structure. This comparison discloses a tip-sample contact radius of a ≈ 4 nm and identifies combinations of enhanced intramolecular transport and Kapitza resistance.

Scanning Thermal Microscopy of Ultrathin Films: Numerical Studies Regarding Cantilever Displacement, Thermal Contact Areas, Heat Fluxes, and Heat Distribution.

New micro- and nanoscale devices require electrically isolating materials with specific thermal properties. One option to characterize these thermal properties is the atomic force microscopy (AFM)-based scanning thermal microscopy (SThM) technique. It enables qualitative mapping of local thermal conductivities of ultrathin films. To fully understand and correctly interpret the results of practical SThM measurements, it is essential to have detailed knowledge about the heat transfer process between the probe and the sample. However, little can be found in the literature so far. Therefore, this work focuses on theoretical SThM studies of ultrathin films with anisotropic thermal properties such as hexagonal boron nitride (h-BN) and compares the results with a bulk silicon (Si) sample. Energy fluxes from the probe to the sample between 0.6 µW and 126.8 µW are found for different cases with a tip radius of approximately 300 nm. A present thermal interface resistance (TIR) between bulk Si and ultrathin h-BN on top can fully suppress a further heat penetration. The time until heat propagation within the sample is stationary is found to be below 1 µs, which may justify higher tip velocities in practical SThM investigations of up to 20 µms-1. It is also demonstrated that there is almost no influence of convection and radiation, whereas a possible TIR between probe and sample must be considered.

Nano/Microscale Thermal Field Distribution: Conducting Thermal Decomposition of Pyrolytic-Type Polymer by Heated AFM Probes.

In relevant investigations and applications of the heated atomic force microscope (AFM) probes, the determination of the actual thermal distribution between the probe and the materials under processing or testing is a core issue. Herein, the polyphthalaldehyde (PPA) film material and AFM imaging of the decomposition structures (pyrolytic region of PPA) were utilized to study the temperature distribution in the nano/microscale air gap between heated tips and materials. Different sizes of pyramid decomposition structures were formed on the surface of PPA film by the heated tip, which was hovering at the initial tip-sample contact with the preset temperature from 190 to 220 °C for a heating duration ranging from 0.3 to 120 s. According to the positions of the 188 °C isothermal surface in the steady-state probe temperature fields, precise 3D boundary conditions were obtained. We also established a simplified calculation model of the 3D steady-state thermal field based on the experimental results, and calculated the temperature distribution of the air gap under any preset tip temperature, which revealed the principle of horizontal (<700 nm) and vertical (<250 nm) heat transport. Based on our calculation, we fabricated the programmable nano-microscale pyramid structures on the PPA film, which may be a potential application in scanning thermal microscopy.

On the Limits of Scanning Thermal Microscopy of Ultrathin Films.

Heat transfer processes in micro- and nanoscale devices have become more and more important during the last decades. Scanning thermal microscopy (SThM) is an atomic force microscopy (AFM) based method for analyzing local thermal conductivities of layers with thicknesses in the range of several nm to µm. In this work, we investigate ultrathin films of hexagonal boron nitride (h-BN), copper iodide in zincblende structure (γ-CuI) and some test sample structures fabricated of silicon (Si) and silicon dioxide (SiO2) using SThM. Specifically, we analyze and discuss the influence of the sample topography, the touching angle between probe tip and sample, and the probe tip temperature on the acquired results. In essence, our findings indicate that SThM measurements include artefacts that are not associated with the thermal properties of the film under investigation. We discuss possible ways of influence, as well as the magnitudes involved. Furthermore, we suggest necessary measuring conditions that make qualitative SThM measurements of ultrathin films of h-BN with thicknesses at or below 23 nm possible.

Localized Heating and Switching in MoTe2-Based Resistive Memory Devices.

Two-dimensional (2D) materials have recently been incorporated into resistive memory devices because of their atomically thin nature, but their switching mechanism is not yet well understood. Here we study bipolar switching in MoTe2-based resistive memory of varying thickness and electrode area. Using scanning thermal microscopy (SThM), we map the surface temperature of the devices under bias, revealing clear evidence of localized heating at conductive "plugs" formed during switching. The SThM measurements are correlated to electro-thermal simulations, yielding a range of plug diameters (250 to 350 nm) and temperatures at constant bias and during switching. Transmission electron microscopy images reveal these plugs result from atomic migration between electrodes, which is a thermally-activated process. However, the initial forming may be caused by defect generation or Te migration within the MoTe2. This study provides the first thermal and localized switching insights into the operation of such resistive memory and demonstrates a thermal microscopy technique that can be applied to a wide variety of traditional and emerging memory devices.

Three-Dimensional Nanothermistors for Thermal Probing.

Accessing the thermal properties of materials or even full devices is a highly relevant topic in research and development. Along with the ongoing trend toward smaller feature sizes, the demands on appropriate instrumentation to access surface temperatures with high thermal and lateral resolution also increase. Scanning thermal microscopy is one of the most powerful technologies to fulfill this task down to the sub-100 nm regime, which, however, strongly depends on the nanoprobe design. In this study, we introduce a three-dimensional (3D) nanoprobe concept, which acts as a nanothermistor to access surface temperatures. Fabrication of nanobridges is done via 3D nanoprinting using focused electron beams, which allows direct-write fabrication on prestructured, self-sensing cantilever. As individual branch dimensions are in the sub-100 nm regime, mechanical stability is first studied by a combined approach of finite-element simulation and scanning electron microscopy-assisted in situ atomic force microscopy (AFM) measurements. After deriving the design rules for mechanically stable 3D nanobridges with vertical stiffness up to 50 N m-1, a material tuning approach is introduced to increase mechanical wear resistance at the tip apex for high-quality AFM imaging at high scan speeds. Finally, we demonstrate the electrical response in dependence of temperature and find a negative temperature coefficient of -(0.75 ± 0.2) 10-3 K-1 and sensing rates of 30 ± 1 ms K-1 at noise levels of ±0.5 K, which underlines the potential of our concept.

Spatial Mapping of Hot-Spots at Lateral Heterogeneities in Monolayer Transition Metal Dichalcogenides.

Lateral heterogeneities in atomically thin 2D materials such as in-plane heterojunctions and grain boundaries (GBs) provide an extrinsic knob for manipulating the properties of nano- and optoelectronic devices and harvesting novel functionalities. However, these heterogeneities have the potential to adversely affect the performance and reliability of the 2D devices through the formation of nanoscopic hot-spots. In this report, scanning thermal microscopy (SThM) is utilized to map the spatial distribution of the temperature rise within monolayer transition metal dichalcogenide (TMD) devices upon dissipating a high electrical power through a lateral interface. The results directly demonstrate that lateral heterojunctions between MoS2 and WS2 do not largely impact the distribution of heat dissipation, while GBs of MoS2 appreciably localize heating in the device. High-resolution scanning transmission electron microscopy reveals that the atomic structure is nearly flawless around heterojunctions but can be quite defective near GBs. The results suggest that the interfacial atomic structure plays a crucial role in enabling uniform charge transport without inducing localized heating. Establishing such structure-property-processing correlation provides a better understanding of lateral heterogeneities in 2D TMD systems which is crucial in the design of future all-2D electronic circuitry with enhanced functionalities, lifetime, and performance.