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Instruments / Technical Area	Publication Details	Published
I07-Surface & interface diffraction	Resolving the ultrafast charge carrier dynamics of 2D and 3D domains within a mixed 2D/3D lead-tin perovskite Jake D. Hutchinson , Edoardo Ruggeri , Jack M. Woolley , Geraud Delport , Samuel D. Stranks , Rebecca L. Milot Advanced Functional Materials 32 DOI: 10.1002/adfm.202305736 Diamond Proposal Number(s): [17223] Open Access Show Abstract ▼ Abstract: Mixed 2D/3D perovskite materials are of particular interest to the photovoltaics and light- emitting diode (LED) communities due to their impressive opto-electronic properties alongside improved moisture stability compared to conventional 3D perovskite absorbers. Here, a mixed lead-tin perovskite containing distinct, self-assembled domains of either 3D structures or highly phase-pure Ruddlesden–Popper 2D structures is studied. The complex energy landscape of the material is revealed with ultrafast optical transient absorption measurements. It is shown that charge transfer between these microscale domains only occurs on nanosecond timescales, consistent with the large size of the domains. Using optical pump-terahertz probe spectroscopy, the effective charge-carrier mobility is shown to be an intermediary between analogous pure 2D and 3D perovskites. Furthermore, detailed analysis of the free carrier recombination dynamics is presented. By combining results from a range of excitation wavelengths within a full dynamic model of the photoexcited carrier population, it is shown that the 2D domains in the film exhibit remarkably similar carrier dynamics to the 3D domains, suggesting that long-range charge-transport should not be impeded by the heterogeneous structure of the material.	Aug 2023
I14-Hard X-ray Nanoprobe	Revealing nanomechanical domains and their transient behavior in mixed‐halide perovskite films Ioanna Mela , Chetan Poudel , Miguel Anaya , Geraud Delport , Kyle Frohna , Stuart Macpherson , Tiarnan A. S. Doherty , Anna Scheeder , Samuel D. Stranks , Clemens F. Kaminski Advanced Functional Materials DOI: 10.1002/adfm.202100293 Diamond Proposal Number(s): [20420] Show Abstract ▼ Abstract: Halide perovskites are a versatile class of semiconductors employed for high performance emerging optoelectronic devices, including flexoelectric systems, yet the influence of their ionic nature on their mechanical behavior is still to be understood. Here, a combination of atomic‐force, optical, and compositional X‐ray microscopy techniques is employed to shed light on the mechanical properties of halide perovskite films at the nanoscale. Mechanical domains within and between morphological grains, enclosed by mechanical boundaries of higher Young's Modulus (YM) than the bulk parent material, are revealed. These mechanical boundaries are associated with the presence of bromide‐rich clusters as visualized by nano‐X‐ray fluorescence mapping. Stiffer regions are specifically selectively modified upon light soaking the sample, resulting in an overall homogenization of the mechanical properties toward the bulk YM. This behavior is attributed to light‐induced ion migration processes that homogenize the local chemical distribution, which is accompanied by photobrightening of the photoluminescence within the same region. This work highlights critical links between mechanical, chemical, and optoelectronic characteristics in this family of perovskites, and demonstrates the potential of combinational imaging studies to understand and design halide perovskite films for emerging applications such as photoflexoelectricity.	Mar 2021
I07-Surface & interface diffraction	Controlling the growth kinetics and optoelectronic properties of 2D/3D lead–tin perovskite heterojunctions Edoardo Ruggeri , Miguel Anaya , Krzysztof Galkowski , Geraud Delport , Felix Utama Kosasih , Anna Abfalterer , Sebastian Mackowski , Caterina Ducati , Samuel D. Stranks Advanced Materials DOI: 10.1002/adma.201905247 Diamond Proposal Number(s): [17223] Open Access Show Abstract ▼ Abstract: Halide perovskites are emerging as valid alternatives to conventional photovoltaic active materials owing to their low cost and high device performances. This material family also shows exceptional tunability of properties by varying chemical components, crystal structure, and dimensionality, providing a unique set of building blocks for new structures. Here, highly stable self‐assembled lead–tin perovskite heterostructures formed between low‐bandgap 3D and higher‐bandgap 2D components are demonstrated. A combination of surface‐sensitive X‐ray diffraction, spatially resolved photoluminescence, and electron microscopy measurements is used to reveal that microstructural heterojunctions form between high‐bandgap 2D surface crystallites and lower‐bandgap 3D domains. Furthermore, in situ X‐ray diffraction measurements are used during film formation to show that an ammonium thiocyanate additive delays formation of the 3D component and thus provides a tunable lever to substantially increase the fraction of 2D surface crystallites. These novel heterostructures will find use in bottom cells for stable tandem photovoltaics with a surface 2D layer passivating the 3D material, or in energy‐transfer devices requiring controlled energy flow from localized surface crystallites to the bulk.	Nov 2019

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