Low Interfacial Thermal Resistance Between Crossed Ultra-Thin Carbon Nanothreads
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This may be the author’s version of a work that was submitted/accepted for publication in the following source: Zhan, Haifei, Zhang, Gang, Zhuang, Xiaoying, Timon, Rabczuk, & Gu, Yuantong (2020) Low interfacial thermal resistance between crossed ultra-thin carbon nan- othreads. Carbon, 165, pp. 216-224. This file was downloaded from: https://eprints.qut.edu.au/201860/ c 2020 Elsevier Ltd This work is covered by copyright. Unless the document is being made available under a Creative Commons Licence, you must assume that re-use is limited to personal use and that permission from the copyright owner must be obtained for all other uses. If the docu- ment is available under a Creative Commons License (or other specified license) then refer to the Licence for details of permitted re-use. It is a condition of access that users recog- nise and abide by the legal requirements associated with these rights. 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If there is any doubt, please refer to the published source. https://doi.org/10.1016/j.carbon.2020.04.065 Low Interfacial Thermal Resistance Between Crossed Ultra-thin Carbon Nanothreads Haifei Zhan1,2, Gang Zhang3,*, Xiaoying Zhuang4, Rabczuk Timon5, and Yuantong Gu1,2,** 1School of Mechanical, Medical, and Process Engineering, Queensland University of Technology (QUT), Brisbane QLD 4001, Australia 2Center for Materials Science, Queensland University of Technology (QUT), Brisbane QLD 4001, Australia 3Institute of High Performance Computing, Agency for Science, Technology and Research, 1 Fusionopolis Way, Singapore 138632, Singapore 4Institute of Continuum Mechanics, Leibniz Universität Hannover, Appelstraße 11, 30157 Hannover, Germany 5Institute of Structural Mech. Bauhaus-Universität Weimar, Marienstraße 15, 99423 Weimar, Germany Abstract To ensure reliable performance and lifetime of electronics, effective and efficient heat removal is essential, which relies heavily on the high thermal conductivity of the packaging substrates and thermal interface materials (TIMs). Highly conductive fillers have been commonly applied to enhance the thermal conductivity of TIMs, while the enhancement effect has been significantly impeded by the interfacial thermal resistance. This work reveals that the new type of ultra-thin carbon nanomaterial – carbon nanothreads, possess a much smaller interfacial thermal resistance (3.1±0.4´10-9 Km2/W) between each other compared with that of the (4,0) carbon nanotubes (8.8±4.6´10-9 Km2/W). Similar as found for carbon nanotubes, the interfacial thermal resistance decreases when the interfacial crossing angle decreases or the contact area increases. Surprisingly, both compressive and stretching interfacial distance are found to enhance the interfacial thermal conductance. It is found that different carbon nanothreads exhibit an interfacial thermal conductance between 60 and 110 pW/K, which can be remarkably enhanced by introducing interfacial cross-linkers. Combining with the ultra-thin nature of carbon nanothreads, our work suggests that carbon nanothreads can be an excellent alternative nanofillers for polymer composites with enhanced thermal conductivity. Keywords: carbon nanothread, kapitza resistance, density of states, carbon nanotube, molecular dynamics simulation *Corresponding author. Email: [email protected] (Gang Zhang) **Corresponding author. Email: [email protected] (Yuantong Gu) 1 Introduction Nanotechnology has continuously minimized the electronic devices/systems, which drastically increases their power density and results in significant heat generation [1]. To ensure reliable performance and lifetime, effective and efficient heat removal is desired, which relies heavily on the high thermal conductivity of the packaging substrates and thermal interface materials (TIMs) [2-4]. Polymer composite is one of the common TIMs in the electronic packing industry, which have received extensive interests from both scientific and engineering communities [5, 6]. They also have broad applications as underfill materials, organic substrate materials, and in flexible electronic devices. The intrinsic thermal conductivity of polymer is very low about 0.2-0.5 Wm-1K-1, due to the strong inherent phonon scattering between chain ends, entanglements and impurities [7]. In this regard, extensive works have been devoted to promote the heat transfer in polymer composites by adding different types fillers with high thermal conductivity. Owing to their high thermal conductivity, carbon-based nanomaterials are one type of the frequently used thermally conductive fillers for polymer composites, such as one-dimensional (1D) carbon nanotube or nanowire [8-10], two-dimensional (2D) graphene, and three-dimensional (3D) nanoarchitectures like carbon foams. For instance, CNTs are shown with a thermal conductivity as high as ~ 3,000-3,500 W/mK at room temperature [11, 12]. It is believed that to enable an efficient heat transfer while not deteriorating other properties (such as mechanical and electrical insulation characteristics) of the polymer, a percolation network is desired, within which the nanofillers are interconnected with each other. However, studies shown that even at high loading fillers well above the geometric percolation – only a minor enhancement in the overall thermal conductivity is observed for the composite system, which is well below the prediction based on the rule of mixture [13]. For illustration, most of the reported polymer composites with CNT fillers are still well below 5 W/mK [7]. In theory, many factors can constrain the enhancement from the CNT, such as the thermal resistance at the CNT/CNT and CNT/matrix interfaces, the dispersion and alignment of CNTs, and the geometrical parameters of CNTs (e.g., size and shape) [14]. Among these factors, the thermal resistance at the filler/filler and filler/matrix interfaces are the two main constraints that restrict effective heat transfer [15]. Different strategies have been proposed to enhance the heat transfer at the CNT/CNT interface or contacts that is influenced by several factors, including the CNT diameter, aspect ratio, 2 deformation, number of walls, external force, and others [16-22]. The most effective way is to introduce covalent bonds to the interface, which however will remarkably suppress the intrinsic thermal conductivity of CNTs. Recently, a new class of one-dimensional (1D) carbon nanostructure – carbon nanothread, has been reported [23-25], which provides a novel thermally conductive filler for polymer nanocomposites. Unlike the sp2 bonding in CNT, carbon nanothreads have an ultra-thin sp3-bonded carbon structure with a fully hydrogenated surface. Their hydrogenated surface allows for the introduction of covalent bonds between carbon nanothreads, or the attachment of functional groups to the nanothreads, while retaining the threadlike morphology and their excellent mechanical properties [26]. According to our previous work, the nanothread-based bundles exhibit an order of magnitude higher interfacial shear strength than CNT bundles due to the irregular surface-induced stick-slip motion [27], and they also show a good load transfer efficiency with the polymer matrix they are embedded in [28]. Apart from that, preliminary studies have shown that carbon nanothreads possess a tailorable thermal conductivity [8, 29]. Combining its intriguing features (including ultrathin diameter, good thermal conductivity, hydrogenated surface, and high interfacial load transfer efficient), it is expected that the carbon nanothreads can be a new filler for polymer composites with a high mechanical and thermal transport performance. To this end, this work assesses the thermal resistance at the interface of two carbon nanothreads mimicking the nanothread junctions or percolated nanothread networks in the polymer composites. Our results establish for the first time a comprehensive understanding of the heat transfer at the nanothread junction with varying parameters (such as nanothread types, crossing angle, inter-thread distance, interface linkers), which will pave the way for its application in polymer nanocomposites. Methods Nonequilibrium molecular dynamics (NEMD) simulations were employed to acquire the thermal resistance between carbon nanothreads at 300 K. Such simulation scheme has been widely utilized to investigate the thermal conductivity of CNTs or interfacial thermal resistance between CNTs [30, 31], which show good agreement with the experimental measurements [32, 33]. The model was configurated by two carbon nanothreads that cross over each other, which was firstly optimized by the conjugate gradient minimization method and then equilibrated using Nosé- 3 Hoover thermostat [34, 35] for 400 ps. During the energy minimization, both nanothreads were not constrained. While, both two ends of the two nanothreads were fixed during the relaxation process and thermal transport simulation. The temperatures of the heat source (320 K) and sink (280 K) were controlled by the Langevin thermostat [36], with a temperature difference of 40 K. The system was firstly simulated