With the advances of the electronics industry, the continuing trend of miniaturization and integration imposes challenges of efficient heat removal in nanoelectronic devices. Two-dimensional (2D) materials, especially graphene and hexagonal boron nitride (h-BN), are widely accepted as ideal candidates for thermal management materials due to their high intrinsic thermal conductivity and good mechanical flexibility. In this review, we introduce phonon dynamics of solid materials and thermal measurement methods at nanoscale, and highlight the unique thermal properties of 2D materials in relation to sample thickness, domain size, and interfaces. In addition, we discuss recent achievements of thermal management applications in which 2D materials act as heat spreader and thermal interface materials based on their controlled growth and selfassembly. Finally, critical consideration on the challenges and opportunities in thermal management applications of 2D materials is presented.

Heat conduction mechanisms in superlattices could be different across different types of interfaces. Van der Waals superlattices are structures physically assembled through weak van der Waals interactions by design and may host properties beyond the traditional superlattices limited by lattice matching and processing compatibility, offering a different type of interface. In this work, natural van der Waals (SnS)1.17(NbS2)n superlattices are synthesized, and their thermal conductivities are measured by time-domain thermoreflectance as a function of interface density. Our results show that heat conduction of (SnS)1.17(NbS2)n superlattices is dominated by interface scattering when the coherent length of phonons is larger than the superlattice period, indicating that incoherent phonon transport dominates through-plane heat conduction in van der Waals superlattices even when the period is atomically thin and abrupt, in contrast to conventional superlattices. Our findings provide valuable insights into the understanding of the thermal behavior of van der Waals superlattices and devise approaches for effective thermal management of superlattices depending on the distinct types of interfaces.

With the irreversible trend of miniaturization and the pursuit of a high power density in electronic devices, heat dissipation has become crucial for designing nextgeneration electronic products. Graphene, which has the highest thermal conductivity among all discovered solid materials, has attracted attention from both academia and the industry. As a two-dimensional material with atom-scale thickness, graphene is suitable for investigating the phonon transport behavior at reduced dimensions. The mass production technique of graphene makes it a promising material for thermal management in consumer electronics, information technology, medical devices, and new energy automobiles. In this review, we summarize the recent progress on the thermal conduction of graphene. In the first part, we introduce the thermal conductivity measurement methods for graphene, including the optothermal Raman method, suspended-pad method, and time-domain thermoreflectance (TDTR) method. The thermal measurement of graphene with high accuracy is key to understanding the heat transfer mechanism of graphene; however, it is still a significant challenge. Despite the development of measurement methods, the thermal measurement of suspended single-layer graphene is limited by the graphene transfer technique, estimation of the thermal contact resistance, sensitivity to the in-plane thermal conductivity in the thermal model, and other factors. In the second part, we discuss the theoretical study of the thermal conductivity of graphene via first principle calculations and molecular dynamics simulation. The "selection rule" of phonon scattering explains the thickness-dependent thermal conductivity of few-layer graphene, and the understanding of the contribution of phonon modes to the thermal conductivity of graphene has been updated recently by taking multiple-phonon scattering into consideration. The size effect on the thermal conductivity of graphene is discussed in this section for a better understanding of the phonon transport behavior of graphene. In the third part, we conclude with the thermal management applications of graphene, including a highly thermally conductive graphene film, graphene fiber, and graphene-enhanced thermal interface materials. For graphene films, which are the pioneering thermal management applications in industrial use, we focus on the challenge of fabricating highly thermally conductive graphene films with large thicknesses and propose possible technical methods. For graphene-enhanced thermal interface materials, we summarize the main factors affecting the thermal properties and discuss the tradeoff between the high thermal conductivity of graphene flakes and the dispersibility of graphene in the polymer matrix. It was demonstrated that a 3D thermal conductive network is essential for efficient heat dissipation in graphene-based composites. Finally, a summary of opportunities and challenges in the thermal study of graphene is presented at the end of the review. Research on the thermal properties of graphene has made imm...

Monolithic honeycomb structures have been attractive to multidisciplinary fields due to their high strength-to-weight ratio. Particularly, microhoneycomb monoliths (MHMs) with micrometer-scale channels are expected as efficient platforms for reactions and separations because of their large surface areas. Up to now, MHMs have been prepared by a unidirectional freeze-drying (UDF) method only from very limited precursors. Herein, we report a protocol from which a series of MHMs consisting of different components can be obtained. Recently, we found that cellulose nanofibers function as a distinct structure-directing agent towards the formation of MHMs through the UDF process. By mixing the cellulose nanofibers with water soluble substances which do not yield MHMs, a variety of composite MHMs can be prepared. This significantly enriches the chemical constitution of MHMs towards versatile applications.

Isotopically purified semiconductors potentially dissipate heat better than their natural, isotopically mixed counterparts as they have higher thermal conductivity (). But the benefit is low for Si at room temperature, amounting to only ~ 10% higher  for bulk 28 Si than for bulk natural Si ( nat Si).We show that in stark contrast to this bulk behavior, 28 Si (99.92% enriched) nanowires have up to 150% higher  than nat Si nanowires with similar diameters and surface morphology. Using firstprinciples phonon dispersion model, this giant isotope effect is attributed to a mutual enhancement of isotope scattering and surface scattering of phonons in nat Si nanowires, correlated via transmission of phonons to the native amorphous SiO2 shell. The work discovers the strongest isotope effect of  at room temperature among all materials reported to date and inspires potential applications of isotopically enriched semiconductors in microelectronics.

Understanding thermal transport across metal/semiconductor interfaces is crucial for the heat dissipation of electronics. The dominant heat carriers in non-metals, phonons, are thought to transport elastically across most interfaces, except for a few extreme cases where the two materials that formed the interface are highly dissimilar with a large difference in Debye temperature. In this work, we show that even for two materials with similar Debye temperatures (Al/Si, Al/GaN), a substantial portion of phonons will transport inelastically across their interfaces at high temperatures, significantly enhancing interface thermal conductance. Moreover, we find that interface sharpness strongly affects phonon transport process. For atomically sharp interfaces, phonons are allowed to transport inelastically and interface thermal conductance linearly increases at high temperatures. With a diffuse interface, inelastic phonon transport diminishes. Our results provide new insights on phonon transport across interfaces and open up opportunities for engineering interface thermal conductance specifically for materials of relevance to microelectronics.

Achieving high interface thermal conductance is one of the biggest challenges in the nanoscale heat transport of GaN-based devices such as light emitting diodes (LEDs), and high electron mobility transistors (HEMTs). In this work, we experimentally measured thermal boundary conductance (TBC) at interfaces between GaN and the substrates with AuSn alloy as a commonly-used adhesive layer by time-domain thermoreflectance (TDTR). We find that the TBCs of GaN/Ti/AuSn/Ti/Si, GaN/ Ti/AuSn/Ti/SiC, and GaN/Ti/AuSn/Ti/diamond, are 16.5, 14.8, and 13.2 MW•m -2 •K -1 at room temperature, respectively. Our measured results show that the TBC of GaN/Ti/AuSn/Ti/SiC interface is inferior to the TBC of pristine GaN/SiC interface, due to the large mismatch of phonon modes between AuSn/Ti and substrates, shown as the difference of Debye temperature of two materials. Overall, we measured the TBC at interface between GaN and thermal conductive substrates, and provided a guideline for designing the interface between GaN and substrate at HEMT from a thermal management point of view.

Monolithic honeycomb structures have been attractive to multidisciplinary fields due to their high strength-to-weight ratio. Particularly, microhoneycomb monoliths (MHMs) with micrometer-scale channels are expected as efficient platforms for reactions and separations because of their large surface areas. Up to now, MHMs have been prepared by a unidirectional freeze-drying (UDF) method only from very limited precursors. Herein, we report a protocol from which a series of MHMs consisting of different components can be obtained. Recently, we found that cellulose nanofibers function as a distinct structure-directing agent towards the formation of MHMs through the UDF process. By mixing the cellulose nanofibers with water soluble substances which do not yield MHMs, a variety of composite MHMs can be prepared. This significantly enriches the chemical constitution of MHMs towards versatile applications. Video LinkThe video component of this article can be found at https://www.jove.com/video/57144/ 10 , fiber 11 , and fishbone 12 structures are likely to form rather than the MHMs. As a result, the formation of MHMs has been reported only in limited precursors, and this has significantly hampered the diversity of their chemical property. We have recently found that cellulose nanofibers have a strong structure-directing function toward forming the MHM structure through the UDF process 13 . Simply by mixing the cellulose nanofibers with other water-dispersible components, it is possible to prepare a variety of MHMs with different chemical properties. Moreover, their exterior shapes and channel sizes are flexibly and easily controlled 13 . Thus, MHMs are expected to be used as filters, catalyst supports, flow-type electrodes, sensors and scaffolds for biomaterials.In this paper, we first explain the basic preparation technique of MHMs from the aqueous dispersion of cellulose nanofibers through the UDF process in detail. Moreover, we demonstrate the preparation of several different types of composite MHMs.