Antibonding valence states induce low lattice thermal conductivity in metal halide semiconductors

反键分子轨道 卤化物 半导体 价(化学) 金属 材料科学 凝聚态物理 热导率 格子(音乐) 化学 无机化学 物理 冶金 光电子学 原子轨道 复合材料 量子力学 声学 电子
作者
Mohammad Ubaid,Paribesh Acharyya,Suneet K. Maharana,Kanishka Biswas,Koushik Pal
出处
期刊:Applied physics reviews [American Institute of Physics]
卷期号:11 (4) 被引量:8
标识
DOI:10.1063/5.0227080
摘要

Reduction of phonon mediated thermal transport properties, i.e., lattice thermal conductivity (κL), of semiconductors can strongly affect the performance of thermoelectrics and optoelectronics. Although extrinsic routes to reduce κL have been achieved through selective scattering of phonons via doping, alloying, and hierarchical nano-structuring, semiconductors with intrinsically low κL have recently gained widespread attention due to their ability to decouple electronic and phonon transports. While innate low κL in crystalline semiconductors is a desired requirement to achieve high performance thermoelectrics, the solar upconversion efficiency of photovoltaics based on metal halide perovskites (MHPs) have been shown to increase due to their ultralow κL through the hot-phonon bottleneck effect. Therefore, understanding the microscopic mechanisms underlying ultralow κL in crystalline semiconductors is extremely important. Several structural factors that are intrinsic to a material have been shown to strongly influence the reduction of κL. Among them, the presence of rattling atoms, lone-pair electrons, and large lattice anharmonicity have been widely studied. Here, we bring out yet another largely unexplored intrinsic characteristic of materials related to the filled antibonding valence states (AVS) near the Fermi level, which are shown to induce low κL in crystalline compounds. We focus our review on an emerging class of compounds–metal halide semiconductors including MHPs and investigate the interplay between structures, chemical bonding and κL, carefully curating from literature a list of 33 compounds having different structure dimensionality with known κL. We established a universal connection between the elastic moduli, speeds of sound, and κL with the presence of AVS just below the Fermi level. We found that large peak in the AVS correlates positively with lower values of elastic moduli, speeds of sound, and κL, providing antibonding states based design criteria of low-κL compounds. Furthermore, we discuss different synthesis strategies, which are crucial for experimental realization of ultralow κL through structure manipulation. Additionally, we outline how chemical bonding data can be utilized in machine learning models for predictive modeling of κL. We hope that our approach of understanding low-κL through the viewpoint of chemical bonding theory would encourage exploration of phonon transport properties in other families of materials having filled AVS that can provide further insights on the structure-bonding-property relationships aiding novel materials design approaches.
最长约 10秒,即可获得该文献文件

科研通智能强力驱动
Strongly Powered by AbleSci AI
更新
PDF的下载单位、IP信息已删除 (2025-6-4)

科研通是完全免费的文献互助平台,具备全网最快的应助速度,最高的求助完成率。 对每一个文献求助,科研通都将尽心尽力,给求助人一个满意的交代。
实时播报
XD824发布了新的文献求助10
3秒前
FashionBoy应助leo采纳,获得10
9秒前
AmyHu完成签到,获得积分10
9秒前
Lucky完成签到 ,获得积分10
13秒前
留胡子的松完成签到 ,获得积分10
13秒前
Beverly完成签到,获得积分10
13秒前
万能图书馆应助伞镜采纳,获得10
15秒前
i2stay完成签到,获得积分10
17秒前
绿色之梦完成签到 ,获得积分10
23秒前
冷傲凝琴完成签到,获得积分10
24秒前
小葵花完成签到 ,获得积分10
26秒前
尊敬火完成签到 ,获得积分10
36秒前
帆帆帆完成签到 ,获得积分10
38秒前
儒雅沛凝完成签到 ,获得积分10
43秒前
小蔡完成签到,获得积分10
43秒前
Panini完成签到 ,获得积分10
45秒前
yurunxintian完成签到,获得积分10
48秒前
51秒前
falling_learning完成签到 ,获得积分10
53秒前
三百一十四完成签到 ,获得积分10
54秒前
不可靠月亮完成签到,获得积分10
57秒前
leo发布了新的文献求助10
57秒前
1分钟前
Hello应助橙红采纳,获得10
1分钟前
fangtong完成签到,获得积分10
1分钟前
1分钟前
科研通AI2S应助haochi采纳,获得10
1分钟前
龙王爱吃糖完成签到 ,获得积分10
1分钟前
1分钟前
llhh2024完成签到,获得积分10
1分钟前
ssxxx发布了新的文献求助10
1分钟前
67完成签到 ,获得积分10
1分钟前
可靠月亮完成签到,获得积分10
1分钟前
韧迹完成签到 ,获得积分0
1分钟前
1分钟前
木南完成签到 ,获得积分10
1分钟前
1分钟前
小徐发布了新的文献求助10
1分钟前
深情的友易完成签到,获得积分10
1分钟前
醋溜爆肚儿完成签到,获得积分10
1分钟前
高分求助中
(应助此贴封号)【重要!!请各用户(尤其是新用户)详细阅读】【科研通的精品贴汇总】 10000
The Social Work Ethics Casebook: Cases and Commentary (revised 2nd ed.). Frederic G. Reamer 800
Holistic Discourse Analysis 600
Vertébrés continentaux du Crétacé supérieur de Provence (Sud-Est de la France) 600
A complete Carnosaur Skeleton From Zigong, Sichuan- Yangchuanosaurus Hepingensis 四川自贡一完整肉食龙化石-和平永川龙 600
Vertebrate Palaeontology, 5th Edition 500
Fiction e non fiction: storia, teorie e forme 500
热门求助领域 (近24小时)
化学 材料科学 医学 生物 工程类 有机化学 生物化学 物理 纳米技术 计算机科学 内科学 化学工程 复合材料 物理化学 基因 遗传学 催化作用 冶金 量子力学 光电子学
热门帖子
关注 科研通微信公众号,转发送积分 5325617
求助须知:如何正确求助?哪些是违规求助? 4465988
关于积分的说明 13895182
捐赠科研通 4358329
什么是DOI,文献DOI怎么找? 2394019
邀请新用户注册赠送积分活动 1387457
关于科研通互助平台的介绍 1358311