Interfacial Thermal Resistance Research Articles

Effect of interfacial thermal resistance on the near-field photoacoustic signal from gold nanorod in water: a numerical study

The near-field photoacoustics of gold nanoparticle in water has received much attention for its biomedical applications and is strongly affected by the gold–water interfacial thermal resistance. However, the effect of interfacial thermal resistance on near-field photoacoustics has been very little studied. Here we present the numerical simulations of near-field photoacoustic signal generation from a single gold nanorod in water by considering different thermal resistances at the gold–water interface. It is shown that, different from the reported reduction of far-field photoacoustic signals by interfacial thermal resistance, enhancement of near-field photoacoustic signals is obtained with the typical gold–water interfacial thermal resistance. Further analysis reveals that the higher rate of net heat transfer to the surrounding water at the typical interfacial thermal resistance, which corresponds to faster thermal expansion of the surrounding water, accounts for such enhancement of near-field photoacoustic signal and that the enhancement of near-field photoacoustic amplitude is mainly present at a distance within thermal diffusion length.

A new methodology to calculate interface thermal resistance between intumescent coating and steel substrate

Interface thermal resistance (ITR) plays a very important role in heat transfer and thermomechanical coupling response from intumescent coating to steel substrate in fire. However, the dynamic ITR between intumescent coating and steel substrate during burning is seldom reported. In this paper, a new methodology is presented to calculate dynamic ITR between intumescent coating and steel substrate under high incident heat flux based on the interface conservation equation. The new methodology focuses on measuring the temperature distribution and thermal conductivity of intumescent coating and steel substrate, with fewer variables. In this way, the calculation of ITR can be simplified. Firstly, the temperature variation function curves inside the intumescent coating and the steel substrate were fitted separately based on the temperature measurement data. Secondly, the interface temperatures (Tci,Tsi) were determined separately at the interface position by temperature variation function curves inside the intumescent coating or the steel substrate. Finally, the ITR calculation formula was deduced and the key parameters required for ITR calculation were obtained by cone calorimetry et al. An illustrative example was studied and validate the applicability of the new methodology.

Molecular Simulations of Thermal Transport across Iron Oxide-Hydrocarbon Interfaces.

The rational design of dielectric fluids for immersion cooling of batteries requires a molecular-level understanding of the heat flow across the battery casing/dielectric fluid interface. Here, we use nonequilibrium molecular dynamics (NEMD) simulations to quantify the interfacial thermal resistance (ITR) between hematite and poly-α-olefin (PAO), which are representative of the outer surface of the steel battery casing and a synthetic hydrocarbon dielectric fluid, respectively. After identifying the most suitable force fields to model the thermal properties of the individual components, we then compared different solid-liquid interaction potentials for the calculation of the ITR. These potentials resulted in a wide range of ITR values (4-21 K m2 GW-1), with stronger solid-liquid interactions leading to lower ITR. The increase in ITR is correlated with an increase in density of the fluid layer closest to the surface. Since the ITR has not been experimentally measured for the hematite/PAO interface, we validate the solid-liquid interaction potential using the work of adhesion calculated using the dry-surface method. The work of adhesion calculations from the simulations were compared to those derived from experimental contact angle measurements for PAO on steel. We find that all of the solid-liquid potentials overestimate the experimental work of adhesion. The experiments and simulations can only be reconciled by further reducing the strength of the interfacial interactions. This suggests some screening of the solid-liquid interactions, which may be due to the presence of an interfacial water layer between PAO and steel in the contact angle experiments. Using the solid-liquid interaction potential that reproduces the experimental work of adhesion, we obtain a higher ITR (33 K m2 GW-1), suggesting inefficient thermal transport. The results of this study demonstrate the potential for NEMD simulations to improve understanding of the nanoscale thermal transport across industrially important interfaces. This study represents an important step toward the rational design of more effective fluids for immersion cooling systems for electric vehicles and other applications where thermal management is of high importance.

A Molecular Dynamics-Based Approach to Study the Effect of Covalently Bonded Modified Graphene on the Heat Transport Properties of Graphene/Natural Rubber Composite Material Interfaces.

Due to its excellent thermal conductivity, graphene can have great potential in the thermal conductivity of rubber composites. However, the interfacial thermal resistance between graphene and rubber severely hinders this application. In this work, molecular dynamics methods were used to study the interfacial thermal transport of carboxylated, aminated, hydroxylated, and oxy-bridged graphene in rubber composites. The results showed that the covalently bonded modified graphene significantly improved the thermal conductivity of the composites, with increases in thermal conductivity of 156.56%, 86.83%, 60.71%, and 44.28% and decreases in interfacial thermal resistance of 41.84%, 34.72%, 31.86%, and 16.74%, respectively. By calculating the phonon densities of states of different functionalized graphenes, it was found that covalently bonded functional groups increased the phonon match between graphene and natural rubber. However, when the degree of functionalization was greater than 11.96%, the phonon match was maintained at a stable value, which was why the covalently bonded modified graphene could significantly reduce the interfacial thermal resistance. Moreover, the graphene modified by covalent bonding was more uniformly distributed inside the natural rubber. The results of this study provide important theoretical guidance for preparing graphene/natural rubber composites with high thermal conductivity.

Extremely Low Thermal Resistance of β-Ga2O3 MOSFETs by Co-integrated Design of Substrate Engineering and Device Packaging.

Gallium oxide (Ga2O3) emerges as a promising ultrawide bandgap semiconductor, which is expected to surpass the performance of current wide bandgap materials, like GaN and SiC, in electronic devices. However, widespread application of Ga2O3 is hindered by its extremely low thermal conductivity and lack of effective device-level thermal management strategies. In this work, Ga2O3 metal-oxide-semiconductor field-effect transistors (MOSFETs) are fabricated by conducting co-integrated design of substrate engineering with layer transferring and device packaging. 3D Raman thermography is introduced as a novel method to analyze the temperature distribution within the device, which provides valuable insights into their thermal performances. A high-quality Ga2O3-SiC heterogeneous integrated material is successfully fabricated with an extremely low interface thermal resistance of 6.67 ± 2 m2·K/GW. Compared to the homoepitaxial Ga2O3 MOSFETs, the degradation of Ion/Ioff in Ga2O3-SiC MOSFETs is decreased by 1.5 orders of magnitude, and that of Ron is decreased by 31%, showing the great thermal stability of Ga2O3-SiC MOSFETs. With the additional device packaging, a significant one order-of-magnitude reduction in the thermal resistance of the Ga2O3-SiC MOSFET is achieved, reaching a record-low value of 4.45 K·mm/W in the reported Ga2O3 MOSFETs. This work demonstrates an efficient strategy for device-level thermal management in next-generation Ga2O3 power and RF applications.

Preparation and thermal conductivity properties of CF/SR composites with high orientation and low interfacial thermal resistance based on the synergistic effect of magnetic field, torsional vibration and Diels-Alder reaction

Preparation and thermal conductivity properties of CF/SR composites with high orientation and low interfacial thermal resistance based on the synergistic effect of magnetic field, torsional vibration and Diels-Alder reaction

Application of a thermal circuit model for the prediction of interfacial thermal resistance between water and a nanostructure surface using molecular dynamics simulations

The present study proposes various thermal circuit models (TCMs) to predict interfacial thermal resistances (ITRs) between water and a nanostructure surface. The effects of water models, nanopillar widths on nanostructure surfaces, and composite surfaces on the relationship between ITRs calculated by non-equilibrium molecular dynamics simulations and ITRs predicted by TCMs are investigated in water-copper and water-graphene-copper systems. The results reveal that the ITRs predicted by some TCMs are slightly affected by water pressure, while MD-calculated ITRs of the nanostructure surfaces in the Wenzel states agree with most of the predicted ITRs. Additionally, it is demonstrated that water molecules in the groove of a nanostructure surface play a crucial role in TCMs in the Cassie-Baxter states. Considering the effective contact region of water molecules in the groove in the Cassie-Baxter states, the use of TCMs can effectively reduce the prediction error of ITRs.

Achieving high thermal conductivity and strong bending strength diamond/aluminum composite via nanoscale multi-interface phase structure engineering

Diamond/aluminum composites, as a new generation of thermal management materials, are caught in the dilemma between inhibiting the formation of Al4C3 and improving the performance. Herein, we proposed a strategy for nanoscale multi-interface phase structure engineering, utilizing a combination of magnetron sputtering and vacuum heat treatment to obtain diamond particles with nanoscale TiC-Ti layers. Prolonging the vacuum heating time increases the content of TiC, but results in significant differences in the morphology and coverage of TiC formed on the diamond(100) and (111) facets. First-principles calculations reveal that the work of adhesion and C-Ti reaction tendency of diamond(100)/Ti are stronger than those of diamond(111)/Ti, clarifying the difference in interfacial properties between diamond/Ti and diamond/TiC. Diamond-TiC-Ti configuration obtained in advance contributes to fabricating the composite with diamond-TiC-Al(Al3Ti) structure, and the multi-interface phase structure is beneficial to improve the interface bonding, adjust the acoustic mismatch, and inhibit the formation of Al4C3. (800 °C 0.5 h)@Ti-coated diamond(100 μm)/aluminum composite with the multi-interface phase exhibits excellent thermal conductivity(646 W m−1 K−1) and outstanding bending strength(358 MPa), exceeding 90 % of the theoretical prediction of the differential effective medium model. The performance of (800 °C 0.5 h)@Ti-coated diamond/aluminum composite is about 30 % higher than that of traditional Ti-coated diamond/aluminum composite. The TiC layer formed by increasing the heat treatment time is thicker and discontinuous, leading to a decrease in the thermal conductivity of the composite and a weakening effect of Al4C3 inhibition. We clarified the formation mechanism of interface structure related to diamond orientation by multi-scale characterization. Based on the thermal conductivity prediction models, the interface structures corresponding to different diamond orientations were considered, and the predicted values showed good consistency with the experimental results. By interface modification engineering, we overcome the dilemma of introducing modified layer to inhibit Al-C reaction while leading to additional interface thermal resistance, providing insights into the interfacial thermal transport mechanism.

Covalent and non‐covalent action‐enhanced cellulose‐based thermally conductive composite (TCC) films fabricated via vacuum‐assisted self assembly with high thermally conductivity and superior mechanical performance

AbstractAs is known, to establish covalent or non‐covalent interaction between filler and matrix, which helps to reduce the interface thermal resistance (ITR) as well as construct good thermal conduction channels, is a good strategy for dealing with the risk of thermal runaway in the extreme service environment of electronic equipment. In this paper, carboxylated nanocellulose fiber (c‐CNF) was used as matrix, and a hybrid filler (M‐CoNPs@GNP) was fabricated by coating cobalt‐nanoparticles (CoNPs) and grafting maleimide on graphene nanosheets (GNPs). M‐CoNPs@GNP/c‐CNF thermally conductive composite (TCC) films were successfully fabricated by combining with c‐CNF. As zero‐dimensional particles, CoNPs can effectively prevent GNPs agglomeration due to surface effects, and “‐NH” in maleimide dehydrates with “‐COOH” in c‐CNF to form “C‐N‐C” covalent bonds, with strong hydrogen bond formed between filler and matrix, which remarkably enhances the interface compatibility between matrix and filler. The ITR has been reduced to form a well‐defined three‐dimensional thermal conduction path, achieving an ultra‐high in‐plane TC (35.9 W·m−1·K−1) for MCGC40, which is 7.9 times that of pure c‐CNF film, in addition to a sufficiently high tensile strength of 123.3 MPa. The combination of high in‐plane TC, excellent mechanical flexibility and good electrical insulation jointly justifies the potential application of M‐CoNPs@GNP/c‐CNF TCC films in effective thermal management of flexible electronic products.Highlights CoNPs effectively inhibit GNPs agglomeration. GNPs exhibit hydrophilicity after modification. Modified fillers interact fairly well with the matrix. High tensile strength and exceptional flexibility are achieved. TCC films exhibit both electrical insulation and hydrophobicity.

Thermal interface materials: From fundamental research to applications

AbstractThe miniaturization, integration, and high data throughput of electronic chips present challenging demands on thermal management, especially concerning heat dissipation at interfaces, which is a fundamental scientific question as well as an engineering problem—a heat death problem called in semiconductor industry. A comprehensive examination of interfacial thermal resistance has been given from physics perspective in 2022 in Review of Modern Physics. Here, we provide a detailed overview from a materials perspective, focusing on the optimization of structure and compositions of thermal interface materials (TIMs) and the interact/contact with heat source and heat sink. First, we discuss the impact of thermal conductivity, bond line thickness, and contact resistance on the thermal resistance of TIMs. Second, it is pointed out that there are two major routes to improve heat transfer through the interface. One is to reduce the TIM's thermal resistance (RTIM) of the TIMs through strategies like incorporating thermal conductive fillers, enhancing interfacial structure and treatment techniques. The other is to reduce the contact thermal resistance (Rc) by improving effective interface contact, strengthening bonding, and utilizing mass gradient TIMs to alleviate vibrational mismatch between TIM and heat source/sink. Finally, such challenges as the fundamental theories, potential developments in sustainable TIMs, and the application of AI in TIMs design are also explored.

An innovative strategy to enhance the interfacial interaction and effective contribution of BN in thermal conductivity in aramid based composites films

With the escalating concern over electronic device overheating, BN/polymer based thermal conductive composites have experienced remarkable growth in the field of heat dissipation. However, it is challenging to enhance the thermal conductivity of composites while preserving strong interfacial interaction due to the dilemma of chemical inertness of BN, interfacial thermal resistance and filler-polymer interaction. Herein, we utilized the adjustable surface charge of polydopamine under varying pH to fabricate composite films comprising polydopamine-modified boron nitride nanosheets and aramid sheets (BNNS@PDA/ANFS) by electrostatic assembly. The thermal conductivity of the composite rose to 36.9 W/m⋅K−1 with only 20 wt% filler. According to Density functional theory (DFT) simulation and interface thermal resistance calculation, the electrostatic assembly enhanced interface interactions and greatly reduced thermal resistance barrier. Furthermore, the optimal tensile strength of 304 MPa, is 2.32 times higher than pure ANFS film, accompanied by toughness of 33.2 MJ/m−3. These superior performances are the results of a synergistic strategy, combining interfacial and topological enhancements. This work provides an innovative approach to enhance effective filler contribution in matrix and underscores the significant potential of BNNS@PDA/ANFS composite films in applications related to heat management.

Thermophysical Properties' Enhancement of LiNO3-NaNO3-KNO3-NaNO2-KNO2 Mixed with SiO2/MgO Nanoparticles.

The aim of this study is to further enhance the thermal storage and heat transfer performances of a low-melting-point quinary salt. The eutectic salt was prepared using LiNO3, NaNO3, KNO3, NaNO2, and KNO2 as raw materials, followed by the doping of nano-SiO2 and nano-MgO into the base salt using a microwave-assisted method. The thermal properties of the samples were analyzed using a Synchronous Thermal Analyzer and a Laser Flash Apparatus. The co-doping of two types of nanoparticles was found to significantly enhance the specific heat capacity of the base salt. The maximum specific heat reached 2.36 J/(g·K), showing a 50.4% increase compared to the base salt. The thermal conductivity of molten salts can be affected by nanoparticles. An observed sample demonstrated a thermal diffusivity of 0.286 mm2/s, indicating a 19.2% improvement over the base salt, which may be attributed to enhanced phonon thermal efficiency. In addition, this study revealed that while interfacial thermal resistance can enhance specific heat capacity, it can also lead to a decrease in the thermal conductivity efficiency of materials. This work can offer insights and references for the enhancement of molten salt properties.

Interfacial thermal resistance in stanene/ hexagonal boron nitride van der Waals heterostructures: A molecular dynamics study

Recently, the stanene (Sn)/hexagonal boron nitride (h-BN) van der Waals heterostructure (vdW) has garnered significant attention among the scientific community due to its distinctive electrical, optical, and thermal characteristics. Despite the promising potential of this heterostructure, the interfacial thermal resistance (ITR) between the Sn and h-BN layers remains unexplored. Understanding and modulating this ITR are essential steps towards harnessing the maximum potential of these materials in practical nanodevices. This study aims to investigate the interfacial thermal resistance (ITR) between the Sn and h-BN layers through the use of conventional molecular dynamics (MD) simulation. The transient pump–probe heating technique, commonly referred to as the Fast Pump Probe (FPP) approach, is utilized to analyze the ITR of the Sn/h-BN heterostructure. The estimated ITR value of a 30 × 10 nm2 Sn/h-BN nanosheet is found to be around ∼ 7 × 10-8 K.m2/W at room temperature. This study comprehensively investigates the impact of various internal and external parameters including nanosheet size, system temperature, contact pressure, vacancy concentration, and mechanical tensile strain (uniaxial and biaxial) on ITR, providing an extensive understanding of how these factors collectively affect the thermal resistance between Sn and h-BN layers. The simulationresults demonstrate a consistent decline in ITR by approximately ∼ 93 %, ∼45 %, ∼65 %, and ∼ 33 % with the increasing system size, temperature, contact pressure, and defect concentration, respectively. In contrast, increasing mechanical strain leads to a substantial enhancement in ITR, with a maximum increase of approximately ∼ 47 % under uniaxial tensile strain and almost ∼ 99 % under biaxial tensile strain. Moreover, the pristine Sn/h-BN heterostructure exhibits no significant thermal rectification effect. The Phonon Density of States (PDOS) profile of the Sn and h-BN layer is calculated to elucidate this underlying behavior of ITR. The PDOS analysis reveals that heat is transported from h-BN to the Sn layer through efficient coupling of low-frequency flexural phonons between these two materials. This work will provide both theoretical support and logical guidelines for modulating thermal resistance across diverse dissimilar material interfaces, which will be necessary for the development of advanced nanodevices used in next-generation nanoelectronics, nanophotonic, and optoelectronics applications.

Constructing the Snail Shell-Like Framework in Thermal Interface Materials for Enhanced Through-Plane Thermal Conductivity.

Melioration of the through-plane thermal conductivity (TC) of thermal interface materials (TIMs) is a sore need for efficient heat dissipation to handle an overheating concern of high-power-density electronics. Herein, we constructed a snail shell-like thermal conductive framework to facilitate vertical heat conduction in TIMs. With inspiration from spirally growing calcium carbonate platelets of snail shells, a facile double-microrod-assisted curliness method was developed to spirally coil boron nitride nanosheet (BNNS)/aramid nanofiber (ANF) laminates where interconnected BNNSs lie along the horizontal plane. Thus, vertical alignment of BNNSs in the resultant TIM was achieved, exhibiting a through-plane TC enhancement of ∼100% compared to the counterpart with randomly distributed BNNSs at the same BNNS addition (50 wt %). The Foygel's nonlinear model revealed that this unique snail shell-like BNNS framework reduced interfacial thermal resistance by 4 orders of magnitude. Our TIM showed superior interfacial thermal dissipation efficiency, leading to a temperature reduction of 42.6 °C for the LED chip compared to the aforementioned counterpart. Our work paves a valuable way for fabricating high-performance TIMs to ensure reliable operation of electrical devices.

Semi-in-situ thermal transport characterization of thermal interface materials through a low-frequency thermoreflectance technique

Thermal transport characterization of thermal interface materials (TIMs), especially in their application scenario is so far challenging. Herein, we demonstrate a low-frequency frequency domain thermoreflectance technique to measure the semi-in-situ thermal transport properties of TIMs in a sandwiched structure. The measurement ability is first demonstrated by accurate measurement on several well-known materials. Then the thermal conductivity and interface thermal resistance of a thermal gel, a thermal pad composed of phase change materials and an Indium foil, sandwiched in two silicon slides are investigated. Sensitivity analysis emphasized the importance of pump laser spot size and modulation frequency in the measurement. For TIMs with low thermal conductivity, the sensitivity to interface thermal resistance is highly suppressed, while for TIMs with high thermal conductivity, the sensitivity to interface thermal resistance is prominent, which makes it easier to separately determine the TIM thermal conductivity and interface thermal resistance.

Mechanism of interfacial thermal resistance variation in diamond/Cu/CNT tri-layer during thermal cycles

The multilayer materials in aerospace applications generally subject to thermal shock, which may significantly affect the interfacial thermal resistance (ITR) and cause serious overheating issues. Therefore, understanding the interfacial thermal transport under temperature shock is essential for effective thermal management in aerospace devices. In the present study, the variation in ITR within the diamond/Cu/carbon nanotube tri-layer after thermal cycles was investigated through non-equilibrium molecular dynamics (NEMD) simulations. We conducted four groups of investigations, exploring the impact of maximum cycle temperature, heating/cooling rates, number of cycles, and interfacial structure on ITR. The results demonstrate that while the matching degree of phonon density of states remains almost constant, the ITR varies significantly among all groups. The structural deformations and changes in lattice type can be observed in the Cu layer. Based on these findings, we proposed an “atomic distribution method” to elucidate the mechanism behind ITR variation, which was verified as applicable and precise. Additionally, the thermal rectification results demonstrate the significant effect of interfacial structure on the rectification coefficient, indicating that interfacial transport and lattice thermal conduction deserve more in-depth study in the future. This work provides a novel perspective on understanding thermal transport across the irregular and complex interfaces, which is significant for the thermal management in aerospace field.

Dual regulation of thermal conductivity and mechanical performance of nano cellulose-based composite via mimicking plant cell wall structure

Combining thermal conductive fillers and flexible polymers is an agile approach to fabricating composites with heat-conducting performance. However, the thermal conductivity of the composites is hard to reach an equal level to the functional fillers. The mainspring is that the thermally conductive pathways within the composite could not be well-constructed due to the air-induced interface thermal resistance. Herein, inspired by the plant cell wall structure, polyvinyl alcohol (PVA) with abundant hydroxyl groups was adopted as a binder for boosting the thermally conductive pathways construction between cellulose nanofiber (CNF) and alkalized hexagonal boron nitride (BN-OH), also for strengthening the mechanical performance of the composite. The results showed that the tensile strength and through-plane thermal conductivity of the composite were high up to 91.0 MPa and 2.2 W m−1 K−1 at 40 wt% PVA content, exhibiting 121 % and 450 % enhancements compared to pure CNF film (41.2 MPa and 0.4 W m−1 K−1). Moreover, the composite also presented high thermal stability (decomposition temperature of onset was 218 °C) and good hydrophobicity properties. Overall, this study innovatively proposes an idea for enhancing the thermal conductivity and improving the mechanical properties of the composite, which is indispensable for developing thermal management materials for next-generation electronics.

Interfacial heat transport properties of graphene/natural rubber composites studied based on molecular dynamics approach

The interface between graphene and natural rubber significantly impacts the thermal properties of graphene/natural rubber composites. This paper uses molecular dynamics to investigate interfacial heat transport. The study found that the thermal conductivity of the composites increases non-linearly with graphene content: a 136 % increase at 10.5 % graphene and only 12.23 % at 16.4 % graphene. As graphene content increases, graphene agglomerates within the natural rubber due to weak van der Waals forces. The interfacial thermal resistance of the composites increases with temperature, rising by 69.94 % from 200K to 450K. When pressure increases from 0.1 MPa to 2.5 MPa, the maximum change in interfacial thermal resistance is 24.39 %. The study also found that interfacial thermal resistance increases with the number of graphene layers. Thus, the interfacial thermal resistance between graphene and natural rubber is the main reason for the minor change in the thermal conductivity of the composites, with temperature having a greater impact.

Ti3C2Tx MXene/Graphene hybrid frameworks for constructing thermally conductive phase change composites with solar-thermal conversion ability

Application of three-dimensional (3D) carbon framework in phase change material (PCM) has aroused a tremendous interest. However, implementing a high alignment carbon framework with low interfacial thermal resistance (ITR) remain challenging. Herein, we demonstrated a synergetic effect strategy by Ti3C2Tx MXene and graphene nanoplate (GNP) to achieve a 3D thermally conductive framework with high alignment skeleton and low filler-to-filler ITR. Typically, the 3D anisotropic carbon framework is fabricated by unidirectional ice template freezing cellulose nanofibers (CNF)/GNP solution with the assistance of MXene. The abundant functional groups of MXene and the similar layered structure promote the dispersion stability of GNP in CNF aqueous solution, resulting in the significant improvement in GNP alignment and the filler-to-filler ITR. Therefore, the final phase change composites obtained by impregnating polyethylene glycol (PEG) into the framework achieves a satisfactory thermal conductivity (TC) of up to 3.49 W/m K at only 6.25 vol% filler loading. Combining the solar-thermal conversion ability of graphene and MXene, the PCM reveals a rapid energy conversion, transfer and storage capability. More importantly, the phase change enthalpy of the PCM can be as high as 164.3 J/g, with little change even after 50 heating-cooling cycles, and the existence of carbon framework can effectively prevent the leakage phenomenon in solid-liquid conversion process, ensuring its shape stability.

Effects of diamond/Al interface structure evolution on interfacial thermal conductance during the carbonization of the Cr interlayer

The correlation between the interface structure evolution and the interfacial thermal conductance (ITC) in diamond particles reinforced Al matrix (diamond/Al) composites has been largely unclear. Herein, diamond/Cr/Al nanolayered structures with the interlayers in different carbonization stages were prepared via magnetron sputtering and annealing treatment to simulate the interfaces in diamond/Al composites. As the annealing time increases, the formed Cr3C2 phase progressively grows from discrete particles to a continuous layer at the diamond/Cr interface, during which the thickness of the carbide layer gradually increases. The formation of Cr3C2 phase improves the interface bonding and provides a more convenient channel for the heat exchange of hot carriers between the interfaces. Accordingly, the ITCs of the samples gradually increases with the annealing time and reaches the maximum value of 436.66 MW/(m2·K) at 120 min due to the formation of a thin and continues Cr3C2 layer. However, considering high interfacial thermal resistance was introduced at the interface when the Cr3C2 interlayer is too thick, the ITC of the sample decreased to 321 MW/(m2·K) as the annealing time extended to 240 min. In addition, Al8Cr5 phase is generated at the Al/Cr interface, but its impact on the ITC of the samples is negligible due to the small amount.