Dynamic disorder, phonon lifetimes, and the assignment of modes to the vibrational spectra of methylammonium lead halide perovskites

卤化物 非谐性 材料科学 钙钛矿(结构) 凝聚态物理 联轴节(管道)
作者
Aurélien M. A. Leguy,Alejandro R. Goñi,Jarvist M. Frost,Jonathan M. Skelton,Federico Brivio,Xabier Rodríguez-Martínez,Oliver J. Weber,Anuradha R. Pallipurath,M. Isabel Alonso,Mariano Campoy-Quiles,Mark T. Weller,Jenny Nelson,Aron Walsh,Piers R. F. Barnes
出处
期刊:Physical Chemistry Chemical Physics [Royal Society of Chemistry]
卷期号:18 (39): 27051-27066 被引量:224
标识
DOI:10.1039/c6cp03474h
摘要

We present Raman and terahertz absorbance spectra of methylammonium lead halide single crystals (MAPbX3, X = I, Br, Cl) at temperatures between 80 and 370 K. These results show good agreement with density-functional-theory phonon calculations. Comparison of experimental spectra and calculated vibrational modes enables confident assignment of most of the vibrational features between 50 and 3500 cm−1. Reorientation of the methylammonium cations, unlocked in their cavities at the orthorhombic-to-tetragonal phase transition, plays a key role in shaping the vibrational spectra of the different compounds. Calculations show that these dynamic effects split Raman peaks and create more structure than predicted from the independent harmonic modes. This explains the presence of extra peaks in the experimental spectra that have been a source of confusion in earlier studies. We discuss singular features, in particular the torsional vibration of the C–N axis, which is the only molecular mode that is strongly influenced by the size of the lattice. From analysis of the spectral linewidths, we find that MAPbI3 shows exceptionally short phonon lifetimes, which can be linked to low lattice thermal conductivity. We show that optical rather than acoustic phonon scattering is likely to prevail at room temperature in these materials.
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
Wangyicong完成签到,获得积分10
刚刚
Lucas应助科研通管家采纳,获得10
1秒前
萧水白应助科研通管家采纳,获得10
1秒前
Lucas应助科研通管家采纳,获得10
1秒前
田様应助科研通管家采纳,获得10
1秒前
大模型应助科研通管家采纳,获得10
1秒前
大模型应助科研通管家采纳,获得10
1秒前
bkagyin应助科研通管家采纳,获得30
1秒前
科研通AI2S应助科研通管家采纳,获得10
1秒前
FashionBoy应助科研通管家采纳,获得10
1秒前
1秒前
1秒前
萧水白应助科研通管家采纳,获得10
1秒前
1秒前
1秒前
1秒前
阿腾发布了新的文献求助10
2秒前
FloppyWow完成签到 ,获得积分10
3秒前
xn201120发布了新的文献求助150
3秒前
舒心的依风完成签到,获得积分10
4秒前
嗯嗯完成签到,获得积分10
5秒前
baba发布了新的文献求助10
6秒前
胡庆余堂小洋参完成签到,获得积分10
6秒前
Akim应助义气萝卜头采纳,获得10
8秒前
眼睛大寻双完成签到,获得积分20
9秒前
Orange应助兴奋雁蓉采纳,获得10
10秒前
猪猪hero应助ElbingX采纳,获得20
12秒前
13秒前
13秒前
14秒前
好旺完成签到,获得积分10
17秒前
CC关闭了CC文献求助
17秒前
深情安青应助霸气安筠采纳,获得20
18秒前
思源应助htx采纳,获得30
18秒前
思源应助苏苏苏only采纳,获得10
19秒前
geopotter完成签到,获得积分10
20秒前
xiewen发布了新的文献求助10
21秒前
ZHANG_Kun完成签到 ,获得积分10
22秒前
星辰大海应助谢谢谢采纳,获得10
22秒前
英姑应助淡水痕采纳,获得10
23秒前
高分求助中
A new approach to the extrapolation of accelerated life test data 1000
Picture Books with Same-sex Parented Families: Unintentional Censorship 700
ACSM’s Guidelines for Exercise Testing and Prescription, 12th edition 500
Nucleophilic substitution in azasydnone-modified dinitroanisoles 500
不知道标题是什么 500
Indomethacinのヒトにおける経皮吸収 400
Phylogenetic study of the order Polydesmida (Myriapoda: Diplopoda) 370
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 内科学 纳米技术 计算机科学 化学工程 复合材料 遗传学 基因 物理化学 催化作用 冶金 细胞生物学 免疫学
热门帖子
关注 科研通微信公众号,转发送积分 3976267
求助须知:如何正确求助?哪些是违规求助? 3520472
关于积分的说明 11203425
捐赠科研通 3257089
什么是DOI,文献DOI怎么找? 1798589
邀请新用户注册赠送积分活动 877785
科研通“疑难数据库(出版商)”最低求助积分说明 806523