Scholarlink

<p>Understanding lattice dynamics and thermal transport mechanisms in cubic hybrid organic–inorganic perovskites remain challenging due to strong anharmonicity and phase transitions. Here, we investigate the thermal transport behavior in benchmark cubic hybrid perovskite FAPbI<sub>3</sub> by coupling first principles-based anharmonic lattice dynamics with a linearized Wigner transport equation. Using the Temperature-Dependent Effective Potential (TDEP) method, we stabilize the negative soft modes, primarily dominated by organic FA<sup>+</sup> cations. Our calculations predict an ultra-low thermal conductivity of ~<InlineEquation ID="IEq1"> <InlineMediaObject> <ImageObject Color="BlackWhite" FileRef="41524_2025_1785_Article_IEq1.gif" Format="GIF" Height="16" Rendition="HTML" Resolution="72" Type="Linedraw" Width="106" /> </InlineMediaObject> <EquationSource Format="TEX">\(0.63\,{\rm{W}}{{\rm{m}}}^{-1}{{\rm{K}}}^{-1}\)</EquationSource> <EquationSource Format="MATHML"><math> <mrow> <mn>0.63</mn> <mspace width="0.25em" /> <mi mathvariant="normal">W</mi> <msup> <mrow> <mi mathvariant="normal">m</mi> </mrow> <mrow> <mo>−</mo> <mn>1</mn> </mrow> </msup> <msup> <mrow> <mi mathvariant="normal">K</mi> </mrow> <mrow> <mo>−</mo> <mn>1</mn> </mrow> </msup> </mrow> </math></EquationSource> </InlineEquation> at 300 K, following a temperature dependence of <i>T</i><sup>−0.740</sup>. Contrary to common assumptions, we find that the [PbI<sub>3</sub>]<sup>1-</sup> units, rather than FA<sup>+</sup> cations, dominate thermal resistance. Furthermore, we demonstrate that anharmonic force constants are highly temperature-sensitive, relying on 0-K force constants significantly underestimates thermal conductivity. Our study not only elucidates the microscopic mechanisms governing thermal transport in FAPbI<sub>3</sub> but also provides a robust framework for modeling heat conduction in hybrid organic-inorganic compounds.</p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Ineffectiveness of formamidine in suppressing ultralow thermal conductivity in cubic hybrid perovskite FAPbI3

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2025年10月23日

查看全文
  • Jiongzhi Zheng,
  • Zheng Chang,
  • Changpeng Lin,
  • Chongjia Lin,
  • Yanguang Zhou,
  • Baoling Huang,
  • Ruiqiang Guo,
  • Geoffroy Hautier

摘要

Understanding lattice dynamics and thermal transport mechanisms in cubic hybrid organic–inorganic perovskites remain challenging due to strong anharmonicity and phase transitions. Here, we investigate the thermal transport behavior in benchmark cubic hybrid perovskite FAPbI3 by coupling first principles-based anharmonic lattice dynamics with a linearized Wigner transport equation. Using the Temperature-Dependent Effective Potential (TDEP) method, we stabilize the negative soft modes, primarily dominated by organic FA+ cations. Our calculations predict an ultra-low thermal conductivity of ~ \(0.63\,{\rm{W}}{{\rm{m}}}^{-1}{{\rm{K}}}^{-1}\) 0.63 W m − 1 K − 1 at 300 K, following a temperature dependence of T−0.740. Contrary to common assumptions, we find that the [PbI3]1- units, rather than FA+ cations, dominate thermal resistance. Furthermore, we demonstrate that anharmonic force constants are highly temperature-sensitive, relying on 0-K force constants significantly underestimates thermal conductivity. Our study not only elucidates the microscopic mechanisms governing thermal transport in FAPbI3 but also provides a robust framework for modeling heat conduction in hybrid organic-inorganic compounds.