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DOE OSTI · 2924173

Dynamic nanodomains dictate macroscopic properties in lead halide perovskites

Dubajic, Milos [Univ. of Cambridge (United Kingdom); Univ. of New South Wales, Sydney, NSW (Australia)] (ORCID:0000000194948967)·Neilson, James R. [Colorado State Univ., Fort Collins, CO (United States); Univ. of Oxford (United Kingdom)] (ORCID:0000000192825752)·Klarbring, Johan [Imperial College, London (United Kingdom); Linköping Univ. (Sweden)]·Liang, Xia [Imperial College, London (United Kingdom)]·Bird, Stephanie A. [Australian Nuclear Science and Technology Organisation (ANSTO), Clayton, NSW (Australia)] (ORCID:0000000168011441)·Rule, Kirrily C. [Australian Nuclear Science and Technology Organisation (ANSTO), Kirrawee, NSW (Australia)] (ORCID:0000000195342350)·Auckett, Josie E. [Australian Nuclear Science and Technology Organisation (ANSTO), Clayton, NSW (Australia)]·Selby, Thomas A. [Univ. of Cambridge (United Kingdom)] (ORCID:0009000386555559)·Tumen-Ulzii, Ganbaatar [Univ. of Cambridge (United Kingdom)] (ORCID:0000000176849965)·Lu, Yang [Univ. of Cambridge (United Kingdom)] (ORCID:0000000227932065)·Jung, Young-Kwang [Univ. of Cambridge (United Kingdom)] (ORCID:0000000338488163)·Chosy, Cullen [Univ. of Cambridge (United Kingdom)]·Wei, Zimu [Univ. of Cambridge (United Kingdom)] (ORCID:000000016564637X)·Boeije, Yorrick [Univ. of Cambridge (United Kingdom)] (ORCID:0000000243463123)·Zimmermann, Martin v. [Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)]·Pusch, Andreas [Univ. of New South Wales, Sydney, NSW (Australia)] (ORCID:0000000261159117)·Gu, Leilei [Nanjing Univ. of Science and Technology (China)]·Jia, Xuguang [Changzhou Univ. (China); Univ. Technology Sydney (Australia)] (ORCID:0000000292146917)·Wu, Qiyuan [Univ. of New South Wales, Sydney, NSW (Australia)]·Trowbridge, Julia C. [Colorado State Univ., Fort Collins, CO (United States)]·Mozur, Eve M. [Colorado State Univ., Fort Collins, CO (United States)]·Minelli, Arianna [Univ. of Oxford (United Kingdom)] (ORCID:0000000283103712)·Roth, Nikolaj [Univ. of Oxford (United Kingdom)]·Orr, Kieran W. P. [Stanford Univ., CA (United States); Univ. of Cambridge (United Kingdom)] (ORCID:0000000199961458)·Mahboubi Soufiani, Arman [Univ. of New South Wales, Sydney, NSW (Australia); Helmholtz-Zentrum Berlin (HZB), (Germany). German Research Centre for Materials and Energy]·Kahmann, Simon [Univ. of Cambridge (United Kingdom)] (ORCID:0000000177845333)·Kabakova, Irina [Univ. Technology Sydney (Australia)]·Ding, Jianning [Changzhou Univ. (China); Yangzhou Univ. (China)]·Wu, Tom [Univ. of New South Wales, Sydney, NSW (Australia); Hong Kong Polytechnic Univ. (China)] (ORCID:0000000308454827)·Conibeer, Gavin J. [Univ. of New South Wales, Sydney, NSW (Australia)] (ORCID:0000000322707827)·Bremner, Stephen P. [Univ. of New South Wales, Sydney, NSW (Australia)] (ORCID:0000000193082401)·Nielsen, Michael P. [Univ. of New South Wales, Sydney, NSW (Australia)] (ORCID:0000000204577208)·Walsh, Aron [Imperial College, London (United Kingdom)] (ORCID:0000000154607033)·Stranks, Samuel D. [Univ. of Cambridge (United Kingdom)] (ORCID:0000000283037292)
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Abstract

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.

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Dubajic, Milos [Univ. of Cambridge (United Kingdom); Univ. of New South Wales, Sydney, NSW (Australia)] (ORCID:0000000194948967), Neilson, James R. [Colorado State Univ., Fort Collins, CO (United States); Univ. of Oxford (United Kingdom)] (ORCID:0000000192825752), Klarbring, Johan [Imperial College, London (United Kingdom); Linköping Univ. (Sweden)], Liang, Xia [Imperial College, London (United Kingdom)], Bird, Stephanie A. [Australian Nuclear Science and Technology Organisation (ANSTO), Clayton, NSW (Australia)] (ORCID:0000000168011441), Rule, Kirrily C. [Australian Nuclear Science and Technology Organisation (ANSTO), Kirrawee, NSW (Australia)] (ORCID:0000000195342350), Auckett, Josie E. [Australian Nuclear Science and Technology Organisation (ANSTO), Clayton, NSW (Australia)], Selby, Thomas A. [Univ. of Cambridge (United Kingdom)] (ORCID:0009000386555559), Tumen-Ulzii, Ganbaatar [Univ. of Cambridge (United Kingdom)] (ORCID:0000000176849965), Lu, Yang [Univ. of Cambridge (United Kingdom)] (ORCID:0000000227932065), Jung, Young-Kwang [Univ. of Cambridge (United Kingdom)] (ORCID:0000000338488163), Chosy, Cullen [Univ. of Cambridge (United Kingdom)], Wei, Zimu [Univ. of Cambridge (United Kingdom)] (ORCID:000000016564637X), Boeije, Yorrick [Univ. of Cambridge (United Kingdom)] (ORCID:0000000243463123), Zimmermann, Martin v. [Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)], Pusch, Andreas [Univ. of New South Wales, Sydney, NSW (Australia)] (ORCID:0000000261159117), Gu, Leilei [Nanjing Univ. of Science and Technology (China)], Jia, Xuguang [Changzhou Univ. (China); Univ. Technology Sydney (Australia)] (ORCID:0000000292146917), Wu, Qiyuan [Univ. of New South Wales, Sydney, NSW (Australia)], Trowbridge, Julia C. [Colorado State Univ., Fort Collins, CO (United States)], Mozur, Eve M. [Colorado State Univ., Fort Collins, CO (United States)], Minelli, Arianna [Univ. of Oxford (United Kingdom)] (ORCID:0000000283103712), Roth, Nikolaj [Univ. of Oxford (United Kingdom)], Orr, Kieran W. P. [Stanford Univ., CA (United States); Univ. of Cambridge (United Kingdom)] (ORCID:0000000199961458), Mahboubi Soufiani, Arman [Univ. of New South Wales, Sydney, NSW (Australia); Helmholtz-Zentrum Berlin (HZB), (Germany). German Research Centre for Materials and Energy], Kahmann, Simon [Univ. of Cambridge (United Kingdom)] (ORCID:0000000177845333), Kabakova, Irina [Univ. Technology Sydney (Australia)], Ding, Jianning [Changzhou Univ. (China); Yangzhou Univ. (China)], Wu, Tom [Univ. of New South Wales, Sydney, NSW (Australia); Hong Kong Polytechnic Univ. (China)] (ORCID:0000000308454827), Conibeer, Gavin J. [Univ. of New South Wales, Sydney, NSW (Australia)] (ORCID:0000000322707827), Bremner, Stephen P. [Univ. of New South Wales, Sydney, NSW (Australia)] (ORCID:0000000193082401), Nielsen, Michael P. [Univ. of New South Wales, Sydney, NSW (Australia)] (ORCID:0000000204577208), Walsh, Aron [Imperial College, London (United Kingdom)] (ORCID:0000000154607033), Stranks, Samuel D. [Univ. of Cambridge (United Kingdom)] (ORCID:0000000283037292). 2025-06-02. Dynamic nanodomains dictate macroscopic properties in lead halide perovskites. https://doi.org/10.1038/s41565-025-01917-0

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