Phonon state modulated by interfacial binding at carbon/copper interface

IF 8.3 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Acta Materialia Pub Date : 2025-06-04 DOI:10.1016/j.actamat.2025.121211

Boan Zhong, Jiamiao Ni, Qi Zhang, Haoyu Huang, Yufei Liu, Jian Song, Yue Liu, Tongxiang Fan

{"title":"Phonon state modulated by interfacial binding at carbon/copper interface","authors":"Boan Zhong, Jiamiao Ni, Qi Zhang, Haoyu Huang, Yufei Liu, Jian Song, Yue Liu, Tongxiang Fan","doi":"10.1016/j.actamat.2025.121211","DOIUrl":null,"url":null,"abstract":"Enhancing interfacial binding and vibrational matching has been demonstrated to improve the thermal boundary conductance (TBC) at metal/non-metal interfaces. However, these two factors are inherently interrelated, making it challenging to isolate their individual contributions to TBC. In this study, we aim to disentangle this correlation at classical immiscible carbon/copper (Cu) interfaces, with consideration of both interstitial doping (hydrogenated graphene) and substitutional doping (boron nitride). Density functional theory (DFT) calculations revealed a 32% decrease in vibrational matching at the H-Gr/Cu interface and a 73% increase at the BN/Cu interface. Time-domain thermoreflectance (TDTR) measurements confirmed the changes in vibrational matching follow the trends in TBC, whereas binding energy exhibits an inverse trend. Further phonon density of state (ph-DOS) analysis indicated that the reduced vibrational matching at the H-Gr/Cu interface originates from the suppression of out-of-plane vibrations, caused by the formation of strong interfacial bonds. This finding is further verified by non-equilibrium molecular dynamics (NEMD) simulations. Overall, this study reveals that the adverse impact of strong interfacial binding on low-frequency phonon modes, facilitating a more profound understanding of the phonon behavior and heat transfer mechanisms at metal/2D-material interfaces.","PeriodicalId":238,"journal":{"name":"Acta Materialia","volume":"5 1","pages":""},"PeriodicalIF":8.3000,"publicationDate":"2025-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Acta Materialia","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1016/j.actamat.2025.121211","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}

引用次数: 0

Abstract

Enhancing interfacial binding and vibrational matching has been demonstrated to improve the thermal boundary conductance (TBC) at metal/non-metal interfaces. However, these two factors are inherently interrelated, making it challenging to isolate their individual contributions to TBC. In this study, we aim to disentangle this correlation at classical immiscible carbon/copper (Cu) interfaces, with consideration of both interstitial doping (hydrogenated graphene) and substitutional doping (boron nitride). Density functional theory (DFT) calculations revealed a 32% decrease in vibrational matching at the H-Gr/Cu interface and a 73% increase at the BN/Cu interface. Time-domain thermoreflectance (TDTR) measurements confirmed the changes in vibrational matching follow the trends in TBC, whereas binding energy exhibits an inverse trend. Further phonon density of state (ph-DOS) analysis indicated that the reduced vibrational matching at the H-Gr/Cu interface originates from the suppression of out-of-plane vibrations, caused by the formation of strong interfacial bonds. This finding is further verified by non-equilibrium molecular dynamics (NEMD) simulations. Overall, this study reveals that the adverse impact of strong interfacial binding on low-frequency phonon modes, facilitating a more profound understanding of the phonon behavior and heat transfer mechanisms at metal/2D-material interfaces.

Abstract Image

查看原文本刊更多论文

碳/铜界面结合能调制声子态

增强界面结合和振动匹配已被证明可以改善金属/非金属界面的热边界导率（TBC）。然而，这两个因素本质上是相互关联的，因此很难分离出它们各自对TBC的贡献。在这项研究中，我们的目标是通过考虑间隙掺杂（氢化石墨烯）和取代掺杂（氮化硼），在经典的不混相碳/铜（Cu）界面上解开这种相关性。密度泛函理论（DFT）计算表明，H-Gr/Cu界面的振动匹配度降低了32%，BN/Cu界面的振动匹配度提高了73%。时域热反射（TDTR）测量证实了振动匹配的变化遵循TBC的趋势，而结合能则呈现相反的趋势。进一步的声子态密度（ph-DOS）分析表明，H-Gr/Cu界面上振动匹配的降低是由于强界面键的形成抑制了面外振动。非平衡分子动力学（NEMD）模拟进一步验证了这一发现。总的来说，本研究揭示了强界面结合对低频声子模式的不利影响，促进了对金属/ 2d材料界面声子行为和传热机制的更深刻理解。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文求助全文

来源期刊

Acta Materialia 工程技术-材料科学：综合

CiteScore

16.10

自引率

8.50%

发文量

801

审稿时长

53 days

期刊介绍： Acta Materialia serves as a platform for publishing full-length, original papers and commissioned overviews that contribute to a profound understanding of the correlation between the processing, structure, and properties of inorganic materials. The journal seeks papers with high impact potential or those that significantly propel the field forward. The scope includes the atomic and molecular arrangements, chemical and electronic structures, and microstructure of materials, focusing on their mechanical or functional behavior across all length scales, including nanostructures.