DataVXACS Energy LettersPaper
journal article·2017-05-12Open access

Determining Atomic-Scale Structure and Composition of Organo-Lead Halide Perovskites by Combining High-Resolution X-ray Absorption Spectroscopy and First-Principles Calculations

Walter S. Drisdell, Linn Leppert, Carolin M. Sutter-Fella, Yufeng Liang, Yanbo Li, Quynh P. Ngo, Liwen F. Wan, Sheraz Gul, Thomas Kroll, Dimosthenis Sokaras, Ali Javey, Junko Yano, Jeffrey B. Neaton, Francesca M. Toma, David Prendergast, Ian D. Sharp

ACS Energy Letters· Volume 2· Issue 5
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Source abstract

Abstract

We combine high-energy resolution fluorescence detection (HERFD) X-ray absorption spectroscopy (XAS) measurements with first-principles density functional theory (DFT) calculations to provide a molecular-scale understanding of local structure, and its role in defining optoelectronic properties, in CH 3 NH 3 Pb(I 1– x Br x ) 3 perovskites. The spectra probe a ligand field splitting in the unoccupied d states of the material, which lie well above the conduction band minimum and display high sensitivity to halide identity, Pb-halide bond length, and Pb-halide octahedral tilting, especially for apical halide sites. The spectra are also sensitive to the organic cation. We find that the halides in these mixed compositions are randomly distributed, rather than having preferred octahedral sites, and that thermal tilting motions dominate over any preferred structural distortions as a function of halide composition. These findings demonstrate the utility of the combined HERFD XAS and DFT approach for determining structural details in these materials and connecting them to optoelectronic properties observed by other characterization methods.
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Research context

Electronic materials

OpenAlex topics: Perovskite Materials and Applications · Solid-state spectroscopy and crystallography · Luminescence Properties of Advanced Materials

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States

Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States

Department of Physics, University of California, Berkeley, California 94720, United States

Department of Electrical Engineering and Computer Sciences, University of California, Berkeley, California 94720, United States

Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States

Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States

Stanford Synchrotron Radiation Lightsource (SSRL), SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States

Kavli Energy NanoScience Institute at Berkeley, Berkeley, California 94720, United States

Funding

Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung · Office of Science · Alexander von Humboldt-Stiftung

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