Scholarlink

<p>Lead halide perovskites have emerged as promising materials for solar energy conversion and X-ray detection owing to their remarkable optoelectronic properties. However, the microscopic origins of their superior performance remain unclear. Here we show that low-symmetry dynamic nanodomains present in the high-symmetry average cubic phases, whose characteristics are dictated by the A-site cation, govern the macroscopic behaviour. We combine X-ray diffuse scattering, inelastic neutron spectroscopy, hyperspectral photoluminescence microscopy and machine-learning-assisted molecular dynamics simulations to directly correlate local nanoscale dynamics with macroscopic optoelectronic response. Our approach reveals that methylammonium-based perovskites form densely packed, anisotropic dynamic nanodomains with out-of-phase octahedral tilting, whereas formamidinium-based systems develop sparse, isotropic, spherical nanodomains with in-phase tilting, even when crystallography reveals cubic symmetry on average. We demonstrate that these sparsely distributed isotropic nanodomains present in formamidinium-based systems reduce electronic dynamic disorder, resulting in a beneficial optoelectronic response, thereby enhancing the performance of formamidinium-based lead halide perovskite devices. By elucidating the influence of the A-site cation on local dynamic nanodomains, and consequently, on the macroscopic properties, we propose leveraging this relationship to engineer the optoelectronic response of these materials, propelling further advancements in perovskite-based photovoltaics, optoelectronics and X-ray imaging.</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

Dynamic nanodomains dictate macroscopic properties in lead halide perovskites

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2025年6月2日

查看全文
  • Milos Dubajic,
  • James R. Neilson,
  • Johan Klarbring,
  • Xia Liang,
  • Stephanie A. Bird,
  • Kirrily C. Rule,
  • Josie E. Auckett,
  • Thomas A. Selby,
  • Ganbaatar Tumen-Ulzii,
  • Yang Lu,
  • Young-Kwang Jung,
  • Cullen Chosy,
  • Zimu Wei,
  • Yorrick Boeije,
  • Martin v. Zimmermann,
  • Andreas Pusch,
  • Leilei Gu,
  • Xuguang Jia,
  • Qiyuan Wu,
  • Julia C. Trowbridge,
  • Eve M. Mozur,
  • Arianna Minelli,
  • Nikolaj Roth,
  • Kieran W. P. Orr,
  • Arman Mahboubi Soufiani,
  • Simon Kahmann,
  • Irina Kabakova,
  • Jianning Ding,
  • Tom Wu,
  • Gavin J. Conibeer,
  • Stephen P. Bremner,
  • Michael P. Nielsen,
  • Aron Walsh,
  • Samuel D. Stranks

摘要

Lead halide perovskites have emerged as promising materials for solar energy conversion and X-ray detection owing to their remarkable optoelectronic properties. However, the microscopic origins of their superior performance remain unclear. Here we show that low-symmetry dynamic nanodomains present in the high-symmetry average cubic phases, whose characteristics are dictated by the A-site cation, govern the macroscopic behaviour. We combine X-ray diffuse scattering, inelastic neutron spectroscopy, hyperspectral photoluminescence microscopy and machine-learning-assisted molecular dynamics simulations to directly correlate local nanoscale dynamics with macroscopic optoelectronic response. Our approach reveals that methylammonium-based perovskites form densely packed, anisotropic dynamic nanodomains with out-of-phase octahedral tilting, whereas formamidinium-based systems develop sparse, isotropic, spherical nanodomains with in-phase tilting, even when crystallography reveals cubic symmetry on average. We demonstrate that these sparsely distributed isotropic nanodomains present in formamidinium-based systems reduce electronic dynamic disorder, resulting in a beneficial optoelectronic response, thereby enhancing the performance of formamidinium-based lead halide perovskite devices. By elucidating the influence of the A-site cation on local dynamic nanodomains, and consequently, on the macroscopic properties, we propose leveraging this relationship to engineer the optoelectronic response of these materials, propelling further advancements in perovskite-based photovoltaics, optoelectronics and X-ray imaging.