| Title: |
Dynamic nanodomains dictate macroscopic properties in lead halide perovskites |
| Authors: |
Dubajic, Milos; Neilson, James R.; Klarbring, Johan; Liang, Xia; Bird, Stephanie A.; Rule, Kirrily C.; Auckett, Josie E.; Selby, Thomas A.; Tumen-Ulzii, Ganbaatar; Lu, Yang; Jung, Young-Kwang; Chosy, Cullen; Wei, Zimu; Boeije, Yorrick; Zimmermann, Martin v.; Pusch, Andreas; Gu, Leilei; Jia, Xuguang; Wu, Qiyuan; Trowbridge, Julia C.; Mozur, Eve M.; Minelli, Arianna; Roth, Nikolaj; Orr, Kieran W. P.; Mahboubi Soufiani, Arman; Kahmann, Simon; Kabakova, Irina; Ding, Jianning; Wu, Tom; Conibeer, Gavin J.; Bremner, Stephen P.; Nielsen, Michael P.; Walsh, Aron; Stranks, Samuel D. |
| Publisher Information: |
Linköpings universitet, Teoretisk Fysik; Linköpings universitet, Tekniska fakulteten; Univ Cambridge, England; UNSW Sydney, Australia; Colorado State Univ, CO 80528 USA; Univ Oxford, England; Imperial Coll London, England; Australian Nucl Sci & Technol Org, Australia; Univ Cambridge, England; Deutsch Elektronen Synchrotron DESY, Germany; UNSW Sydney, Australia; Nanjing Univ Sci & Technol, Peoples R China; Changzhou Univ, Peoples R China; Univ Technol Sydney, Australia; Colorado State Univ, CO 80528 USA; Univ Oxford, England; Univ Cambridge, England; Stanford Univ, CA USA; UNSW Sydney, Australia; Helmholtz Zentrum Berlin Materialien & Energie Gmb, Germany; Univ Technol Sydney, Australia; Changzhou Univ, Peoples R China; Yangzhou Univ, Peoples R China; UNSW Sydney, Australia; Hong Kong Polytech Univ, Peoples R China; NATURE PORTFOLIO |
| Publication Year: |
2025 |
| Collection: |
Linköping University Electronic Press (LiU E-Press) |
| Subject Terms: |
Condensed Matter Physics; Den kondenserade materiens fysik |
| Description: |
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. ; Funding Agencies|EPSRC; Swedish Research Council [2022-06725]; National Natural Science Foundation of China [51572037, 91648109, 51335002, 51702024]; Natural Science Foundation of Jiangsu Province [BK20200981]; Changzhou Sci Tech Program [CJ20190050]; Australian Research Council Discovery Project (ARC DP) [DP190101973]; UKRI guarantee funding for Marie Sklodowska-Curie Actions Postdoctoral Fellowships 2022 ... |
| Document Type: |
article in journal/newspaper |
| File Description: |
application/pdf |
| Language: |
English |
| Relation: |
Nature Nanotechnology, 1748-3387, 2025, 20, s. 755-763; PMID 40456909; ISI:001500280100001 |
| DOI: |
10.1038/s41565-025-01917-0 |
| Availability: |
http://urn.kb.se/resolve?urn=urn:nbn:se:liu:diva-214442; https://doi.org/10.1038/s41565-025-01917-0 |
| Rights: |
info:eu-repo/semantics/openAccess |
| Accession Number: |
edsbas.37E60420 |
| Database: |
BASE |