Anisotropic Thermal Conductivity of Crystalline Layered SnSe2.

The degree of thermal anisotropy affects critically key device-relevant properties of layered two-dimensional materials. Here, we systematically study the in-plane and cross-plane thermal conductivity of crystalline SnSe2 films of varying thickness (16-190 nm) and uncover a thickness-independent thermal conductivity anisotropy ratio of about ∼8.4. Experimental data obtained using Raman thermometry and frequency domain thermoreflectance showed that the in-plane and cross-plane thermal conductivities monotonically decrease by a factor of 2.5 with decreasing film thickness compared to the bulk values. Moreover, we find that the temperature-dependence of the in-plane component gradually decreases as the film becomes thinner, and in the range from 300 to 473 K it drops by more than a factor of 2. Using the mean free path reconstruction method, we found that phonons with MFP ranging from ∼1 to 53 and from 1 to 30 nm contribute to 50% of the total in-plane and cross-plane thermal conductivity, respectively.

Two-Dimensional Phononic Crystals: Disorder Matters.

The design and fabrication of phononic crystals (PnCs) hold the key to control the propagation of heat and sound at the nanoscale. However, there is a lack of experimental studies addressing the impact of order/disorder on the phononic properties of PnCs. Here, we present a comparative investigation of the influence of disorder on the hypersonic and thermal properties of two-dimensional PnCs. PnCs of ordered and disordered lattices are fabricated of circular holes with equal filling fractions in free-standing Si membranes. Ultrafast pump and probe spectroscopy (asynchronous optical sampling) and Raman thermometry based on a novel two-laser approach are used to study the phononic properties in the gigahertz (GHz) and terahertz (THz) regime, respectively. Finite element method simulations of the phonon dispersion relation and three-dimensional displacement fields furthermore enable the unique identification of the different hypersonic vibrations. The increase of surface roughness and the introduction of short-range disorder are shown to modify the phonon dispersion and phonon coherence in the hypersonic (GHz) range without affecting the room-temperature thermal conductivity. On the basis of these findings, we suggest a criteria for predicting phonon coherence as a function of roughness and disorder.

Far-Field Radiative Thermal Rectification Based on Asymmetric Emissivity.

This experimental study investigates thermal rectification via asymmetric far-field thermal radiation on a fused silica slab. An asymmetrical distribution of surface emissivity is created over the device by partially covering the fused silica with a 100 nm thick aluminum film. The slab is subjected to a thermal bias, and when this bias is reversed, a small temperature difference is observed between the different configurations. This temperature difference arises from the difference in emissivity between the aluminum layer and fused silica, resulting in the transfer of thermal energy to the surrounding environment through radiation. Experimental findings are supported by finite element simulations, which not only confirm the measured values but also provide valuable insights into the rectification efficiency of the system. The rectification efficiency is found to be approximately 50% at room temperature for a thermal bias of 140 K. Simulations, which are performed by considering different environmental conditions experienced by the radiation and free convection processes, provide further insight into the underlying thermal rectification mechanism. These simulations consider an environmental temperature of 4 K for thermal radiation and an ambient temperature of 294 K for free convection and reveal an enhanced rectification effect with a rectification efficiency up to 600% when a thermal bias of 195 K is applied. This result emphasizes the significance of considering both convection and radiation in the thermal management and rectification of asymmetric systems. The outcomes of this study further our understanding of the thermal rectification phenomenon. They also show the importance of system asymmetry, emissivity disparities, environmental conditions, and the interplay between convection and radiation. Furthermore, the findings have implications for heat transfer and rectification in asymmetric systems, offering potential applications in areas such as energy harvesting, thermal management, and heat transfer optimization in electronic devices.

Impact of Oxygen Stoichiometry on the Thermoelectric Properties of Bi2Sr2Co2Oy Thin Films.

In this study, we present a comprehensive analysis of the thermoelectric (TE) properties of highly c-axis-oriented thin films of layered misfit cobaltates Bi2Sr2Co2Oy. The films exhibit a high c-axis orientation, facilitating precise measurements of electronic transport and TE properties along the a-b crystallographic plane. Our findings reveal that the presence of nearly stoichiometric oxygen content results in high thermopower with metallic conductivity, while the annealing of the films in a reduced oxygen atmosphere eliminates their metallic behavior. According to the well-established Heike's limit, the thermopower tends to become temperature independent when the thermal energy significantly exceeds the bandwidth, which provides a rough estimation of charge carrier density by using the Heike's formula. This observation suggests that the dominant contribution to the thermopower comes from the narrow Co-t2g bands near the Fermi energy. Our study demonstrates that the calculated thermopower value using Heike's formula, based on the Hall electron density of the Bi2Sr2Co2Oy thin films at 300 K, aligns well with the experimental results, shedding light on the intriguing TE properties of this family of layered cobaltate oxide films.

MoS2 phononic crystals for advanced thermal management.

Effective thermal management of electronic devices encounters substantial challenges owing to the notable power densities involved. Here, we propose layered MoS2 phononic crystals (PnCs) that can effectively reduce thermal conductivity (κ) with relatively small disruption of electrical conductivity (σ), offering a potential thermal management solution for nanoelectronics. These layered PnCs exhibit remarkable efficiency in reducing κ, surpassing that of Si and SiC PnCs with similar periodicity by ~100-fold. Specifically, in suspended MoS2 PnCs, we measure an exceptionally low κ down to 0.1 watts per meter kelvin, below the amorphous limit while preserving the crystalline structure. These findings are supported by molecular dynamics simulations that account for the film thickness, porosity, and temperature. We demonstrate the approach efficiency by fabricating suspended heat-routing structures that effectively confine and guide heat flow in prespecified directions. This study underpins the immense potential of layered materials as directional heat spreaders, thermal insulators, and active components for thermoelectric devices.

Enhanced Thermoelectric Properties of Misfit Bi2Sr2-xCaxCo2Oy: Isovalent Substitutions and Selective Phonon Scattering.

Layered Bi-misfit cobaltates, such as Bi2Sr2Co2Oy, are the natural superlattice of an electrically insulating rocksalt (RS) type Bi2Sr2O4 layer and electrically conducting CoO2 layer, stacked along the crystallographic c-axis. RS and CoO2 layers are related through charge compensation reactions (or charge transfer). Therefore, thermoelectric transport properties are affected when doping or substitution is carried out in the RS layer. In this work, we have shown improved thermoelectric properties of spark plasma sintered Bi2Sr2-xCaxCo2Oy alloys (x = 0, 0.3 and 0.5). The substitution of Ca atoms affects the thermal properties by introducing point-defect phonon scattering, while the electronic conductivity and thermopower remain unaltered.

Excitation and detection of acoustic phonons in nanoscale systems.

Phonons play a key role in the physical properties of materials, and have long been a topic of study in physics. While the effects of phonons had historically been considered to be a hindrance, modern research has shown that phonons can be exploited due to their ability to couple to other excitations and consequently affect the thermal, dielectric, and electronic properties of solid state systems, greatly motivating the engineering of phononic structures. Advances in nanofabrication have allowed for structuring and phonon confinement even down to the nanoscale, drastically changing material properties. Despite developments in fabricating such nanoscale devices, the proper manipulation and characterization of phonons continues to be challenging. However, a fundamental understanding of these processes could enable the realization of key applications in diverse fields such as topological phononics, information technologies, sensing, and quantum electrodynamics, especially when integrated with existing electronic and photonic devices. Here, we highlight seven of the available methods for the excitation and detection of acoustic phonons and vibrations in solid materials, as well as advantages, disadvantages, and additional considerations related to their application. We then provide perspectives towards open challenges in nanophononics and how the additional understanding granted by these techniques could serve to enable the next generation of phononic technological applications.

Unraveling Heat Transport and Dissipation in Suspended MoSe2 from Bulk to Monolayer.

Understanding heat flow in layered transition metal dichalcogenide (TMD) crystals is crucial for applications exploiting these materials. Despite significant efforts, several basic thermal transport properties of TMDs are currently not well understood, in particular how transport is affected by material thickness and the material's environment. This combined experimental-theoretical study establishes a unifying physical picture of the intrinsic lattice thermal conductivity of the representative TMD MoSe2 . Thermal conductivity measurements using Raman thermometry on a large set of clean, crystalline, suspended crystals with systematically varied thickness are combined with ab initio simulations with phonons at finite temperature. The results show that phonon dispersions and lifetimes change strongly with thickness, yet the thinnest TMD films exhibit an in-plane thermal conductivity that is only marginally smaller than that of bulk crystals. This is the result of compensating phonon contributions, in particular heat-carrying modes around ≈0.1 THz in (sub)nanometer thin films, with a surprisingly long mean free path of several micrometers. This behavior arises directly from the layered nature of the material. Furthermore, out-of-plane heat dissipation to air molecules is remarkably efficient, in particular for the thinnest crystals, increasing the apparent thermal conductivity of monolayer MoSe2 by an order of magnitude. These results are crucial for the design of (flexible) TMD-based (opto-)electronic applications.

Heat Transport Control and Thermal Characterization of Low-Dimensional Materials: A Review.

Heat dissipation and thermal management are central challenges in various areas of science and technology and are critical issues for the majority of nanoelectronic devices. In this review, we focus on experimental advances in thermal characterization and phonon engineering that have drastically increased the understanding of heat transport and demonstrated efficient ways to control heat propagation in nanomaterials. We summarize the latest device-relevant methodologies of phonon engineering in semiconductor nanostructures and 2D materials, including graphene and transition metal dichalcogenides. Then, we review recent advances in thermal characterization techniques, and discuss their main challenges and limitations.

Quantifying thermal transport in buried semiconductor nanostructures via cross-sectional scanning thermal microscopy.

Managing thermal transport in nanostructures became a major challenge in the development of active microelectronic, optoelectronic and thermoelectric devices, stalling the famous Moore's law of clock speed increase of microprocessors for more than a decade. To find the solution to this and linked problems, one needs to quantify the ability of these nanostructures to conduct heat with adequate precision, nanoscale resolution, and, essentially, for the internal layers buried in the 3D structure of modern semiconductor devices. Existing thermoreflectance measurements and "hot wire" 3ω methods cannot be effectively used at lateral dimensions of a layer below a micrometre; moreover, they are sensitive mainly to the surface layers of a relatively high thickness of above 100 nm. Scanning thermal microscopy (SThM), while providing the required lateral resolution, provides mainly qualitative data of the layer conductance due to undefined tip-surface and interlayer contact resistances. In this study, we used cross-sectional SThM (xSThM), a new method combining scanning probe microscopy compatible Ar-ion beam exit nano-cross-sectioning (BEXP) and SThM, to quantify thermal conductance in complex multilayer nanostructures and to measure local thermal conductivity of oxide and semiconductor materials, such as SiO2, SiGex and GeSny. By using the new method that provides 10 nm thickness and few tens of nm lateral resolution, we pinpoint crystalline defects in SiGe/GeSn optoelectronic materials by measuring nanoscale thermal transport and quantifying thermal conductivity and interfacial thermal resistance in thin spin-on materials used in extreme ultraviolet lithography (eUV) fabrication processing. The new capability of xSThM demonstrated here for the first time is poised to provide vital insights into thermal transport in advanced nanoscale materials and devices.