{"title":"通过非谐波声子重正化研究二维 Si4C8 材料的导热性","authors":"Peng Gao, Xi-Hao Chen, Xingwu Yan, Longxin Zhang, Xiang Meng, Fuqiang Zhai, Donglin Guo","doi":"10.1039/d4cp02583k","DOIUrl":null,"url":null,"abstract":"In this investigation, we employed the anharmonic phonon renormalization method to analyze the thermal conductivity of two-dimensional (2D) carbon materials, while also examining the inffuence of quartic (fourth-order) scattering on heat transport within this material class. Our study centered on a representative Silicon-Carbon (Si-C) 2D system, Si4C8. Notably, conventional Boltzmann transport equation (BTE) calculations with harmonic phonons are inadequate for estimating the thermal conductivity in these materials due to the emergence of imaginary frequencies. Consequently, to elucidate the primary contributors to its heat transport, we employed an integrated yet novel computational framework rooted in ffrst-principles methodology. This approach combines self-consistent phonon (SCP) theory and the BTE to scrutinize the thermal conduction behavior; and the BTE is resolved in conjunction with SCP theory to comprehensively address the quartic anharmonic effects, encompassing both four-phonon (4ph) scatterings and the temperature-induced shift of phonon frequencies. Based on the calculation results, it is evident that the meticulous incorporation of anharmonicity renormalization is pivotal for precise evaluation of thermal conductivity for 2D Si4C8 and establishing a coherent temperature dependency. Through this comprehensive examination, we aim to establish a systematic methodology for investigating the thermal transport mechanisms of 2D Si-C phases with similar bonding networks, offering insights into the intricate relationships between their structural, mechanical, electronic, and thermal properties.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":null,"pages":null},"PeriodicalIF":2.9000,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Thermal Conductivity Study of 2D Si4C8 material by Anharmonic Phonon Renormalization\",\"authors\":\"Peng Gao, Xi-Hao Chen, Xingwu Yan, Longxin Zhang, Xiang Meng, Fuqiang Zhai, Donglin Guo\",\"doi\":\"10.1039/d4cp02583k\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"In this investigation, we employed the anharmonic phonon renormalization method to analyze the thermal conductivity of two-dimensional (2D) carbon materials, while also examining the inffuence of quartic (fourth-order) scattering on heat transport within this material class. Our study centered on a representative Silicon-Carbon (Si-C) 2D system, Si4C8. Notably, conventional Boltzmann transport equation (BTE) calculations with harmonic phonons are inadequate for estimating the thermal conductivity in these materials due to the emergence of imaginary frequencies. Consequently, to elucidate the primary contributors to its heat transport, we employed an integrated yet novel computational framework rooted in ffrst-principles methodology. This approach combines self-consistent phonon (SCP) theory and the BTE to scrutinize the thermal conduction behavior; and the BTE is resolved in conjunction with SCP theory to comprehensively address the quartic anharmonic effects, encompassing both four-phonon (4ph) scatterings and the temperature-induced shift of phonon frequencies. Based on the calculation results, it is evident that the meticulous incorporation of anharmonicity renormalization is pivotal for precise evaluation of thermal conductivity for 2D Si4C8 and establishing a coherent temperature dependency. Through this comprehensive examination, we aim to establish a systematic methodology for investigating the thermal transport mechanisms of 2D Si-C phases with similar bonding networks, offering insights into the intricate relationships between their structural, mechanical, electronic, and thermal properties.\",\"PeriodicalId\":99,\"journal\":{\"name\":\"Physical Chemistry Chemical Physics\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":2.9000,\"publicationDate\":\"2024-10-11\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Physical Chemistry Chemical Physics\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1039/d4cp02583k\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Physical Chemistry Chemical Physics","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1039/d4cp02583k","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Thermal Conductivity Study of 2D Si4C8 material by Anharmonic Phonon Renormalization
In this investigation, we employed the anharmonic phonon renormalization method to analyze the thermal conductivity of two-dimensional (2D) carbon materials, while also examining the inffuence of quartic (fourth-order) scattering on heat transport within this material class. Our study centered on a representative Silicon-Carbon (Si-C) 2D system, Si4C8. Notably, conventional Boltzmann transport equation (BTE) calculations with harmonic phonons are inadequate for estimating the thermal conductivity in these materials due to the emergence of imaginary frequencies. Consequently, to elucidate the primary contributors to its heat transport, we employed an integrated yet novel computational framework rooted in ffrst-principles methodology. This approach combines self-consistent phonon (SCP) theory and the BTE to scrutinize the thermal conduction behavior; and the BTE is resolved in conjunction with SCP theory to comprehensively address the quartic anharmonic effects, encompassing both four-phonon (4ph) scatterings and the temperature-induced shift of phonon frequencies. Based on the calculation results, it is evident that the meticulous incorporation of anharmonicity renormalization is pivotal for precise evaluation of thermal conductivity for 2D Si4C8 and establishing a coherent temperature dependency. Through this comprehensive examination, we aim to establish a systematic methodology for investigating the thermal transport mechanisms of 2D Si-C phases with similar bonding networks, offering insights into the intricate relationships between their structural, mechanical, electronic, and thermal properties.
期刊介绍:
Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions.
The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.