Temperature-Induced Phase Transition in 2D Alkylammonium Lead Halide Perovskites: A Molecular Dynamics Study

卤化物 铅(地质) 相变 化学物理 分子动力学 相(物质) 相变 材料科学 钙钛矿(结构) 动力学(音乐) 凝聚态物理 化学 无机化学 结晶学 工程物理 计算化学 物理 有机化学 地质学 地貌学 声学
作者
Reza Namakian,Maria Vargas,Qing Tu,Ali Erdemir,Wei Gao
标识
DOI:10.26434/chemrxiv-2024-vw2dm
摘要

Molecular dynamics simulations are utilized to unravel the temperature-driven phase transition in double-layered butylammonium (BA) methylammonium (MA) lead halide perovskite (BA)$_{2}$(MA)Pb$_{2}$I$_{7}$, which holds great promise in a wide range of optoelectronics and sensor applications. The simulations successfully capture the structural transition from low to high symmetry phases with rising temperatures, consistent with experimental observations. The phase transition initiates at two critical interfaces: the first is between the inorganic and organic layers, where the melting of N-H bonds in BA leads to significant reduction in hydrogen bonding between BA and iodides, and the second is at the interface between top and bottom organic layers, where the melting of the tail bonds in BA triggers the phase transition. Following this, BA cations exhibit a patterned and synchronized motion reminiscent of a conical pendulum, displaying a mix of ordered and disordered behaviors, prior to evolving into a completely molten and disordered state. While the melting of BA cations is the primary driver of the phase transition, the rotational dynamics of MA cations also plays a critical role in determining the phase transition temperature, influenced by the BA-MA interaction. Such interaction alters the polarization patterns of MA cations across the phase transition. In particular, an anti-parallel polarization pattern is observed in low temperature phase. Additionally, displacive elements of the phase transition are identified in the simulations, characterized by the shear and distortion of the inorganic octahedra. Notably, at lower temperatures, the octahedral distortion follows a bimodal distribution, reflecting significant variations in distortion among octahedra. This variation is attributed to an anisotropic hydrogen bonding network between iodides and BA cations. Our study reveals new phenomena and mechanisms extending beyond the order-disorder transition mechanism, shedding new light on potential phase engineering through strategic tuning of organic and inorganic components.
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
思维隋发布了新的文献求助10
刚刚
2秒前
wangyuan完成签到,获得积分10
4秒前
小不溜完成签到 ,获得积分10
5秒前
5秒前
活泼的巧曼完成签到,获得积分10
5秒前
5秒前
gar完成签到,获得积分10
6秒前
小二郎应助科研通管家采纳,获得10
6秒前
JamesPei应助科研通管家采纳,获得10
6秒前
小蘑菇应助科研通管家采纳,获得10
6秒前
6秒前
Ava应助科研通管家采纳,获得10
6秒前
Ricey应助科研通管家采纳,获得10
6秒前
赘婿应助科研通管家采纳,获得10
6秒前
我是老大应助科研通管家采纳,获得10
6秒前
Owen应助科研通管家采纳,获得30
6秒前
7秒前
7秒前
7秒前
7秒前
7秒前
桐桐应助XY采纳,获得10
8秒前
passerby发布了新的文献求助10
8秒前
8秒前
Starwalker应助U9A采纳,获得20
8秒前
9秒前
852应助gar采纳,获得10
10秒前
令狐子轩完成签到,获得积分10
10秒前
沐晴发布了新的文献求助10
11秒前
11秒前
111发布了新的文献求助10
11秒前
12秒前
SciGPT应助sjr123采纳,获得10
14秒前
格纹完成签到,获得积分10
14秒前
荷珠发布了新的文献求助10
14秒前
崔崔发布了新的文献求助10
15秒前
深情安青应助莫桑采纳,获得10
17秒前
夏安发布了新的文献求助10
18秒前
18秒前
高分求助中
The Mother of All Tableaux: Order, Equivalence, and Geometry in the Large-scale Structure of Optimality Theory 3000
Social Research Methods (4th Edition) by Maggie Walter (2019) 1030
A new approach to the extrapolation of accelerated life test data 1000
Indomethacinのヒトにおける経皮吸収 400
基于可调谐半导体激光吸收光谱技术泄漏气体检测系统的研究 370
Phylogenetic study of the order Polydesmida (Myriapoda: Diplopoda) 370
Robot-supported joining of reinforcement textiles with one-sided sewing heads 320
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 3993533
求助须知:如何正确求助?哪些是违规求助? 3534281
关于积分的说明 11265112
捐赠科研通 3274061
什么是DOI,文献DOI怎么找? 1806303
邀请新用户注册赠送积分活动 883118
科研通“疑难数据库(出版商)”最低求助积分说明 809710