Atomic Resolution Imaging of Halide Perovskites.

The radiation-sensitive nature of halide perovskites has hindered structural studies at the atomic scale. We overcome this obstacle by applying low dose-rate in-line holography, which combines aberration-corrected high-resolution transmission electron microscopy with exit-wave reconstruction. This technique successfully yields the genuine atomic structure of ultrathin two-dimensional CsPbBr3 halide perovskites, and a quantitative structure determination was achieved atom column by atom column using the phase information of the reconstructed exit-wave function without causing electron beam-induced sample alterations. An extraordinarily high image quality enables an unambiguous structural analysis of coexisting high-temperature and low-temperature phases of CsPbBr3 in single particles. On a broader level, our approach offers unprecedented opportunities to better understand halide perovskites at the atomic level as well as other radiation-sensitive materials.

[1]  Richard L. Brutchey,et al.  On the crystal structure of colloidally prepared CsPbBr3 quantum dots. , 2016, Chemical communications.

[2]  C. Kisielowski,et al.  In-line three-dimensional holography of nanocrystalline objects at atomic resolution , 2016, Nature Communications.

[3]  A. Minor,et al.  Observation of polar vortices in oxide superlattices , 2016, Nature.

[4]  Giovanni Bertoni,et al.  Solution Synthesis Approach to Colloidal Cesium Lead Halide Perovskite Nanoplatelets with Monolayer-Level Thickness Control , 2016, Journal of the American Chemical Society.

[5]  A Paul Alivisatos,et al.  Highly Luminescent Colloidal Nanoplates of Perovskite Cesium Lead Halide and Their Oriented Assemblies. , 2015, Journal of the American Chemical Society.

[6]  Lin-wang Wang,et al.  Materials and Methods Supplementary Text Fig. S1 Reference (35) Database S1 Atomically Thin Two-dimensional Organic-inorganic Hybrid Perovskites , 2022 .

[7]  Yi Yu,et al.  Solution-Phase Synthesis of Cesium Lead Halide Perovskite Nanowires. , 2015, Journal of the American Chemical Society.

[8]  Christopher H. Hendon,et al.  Nanocrystals of Cesium Lead Halide Perovskites (CsPbX3, X = Cl, Br, and I): Novel Optoelectronic Materials Showing Bright Emission with Wide Color Gamut , 2015, Nano letters.

[9]  J.C. Meyer,et al.  Atomic structure from large-area, low-dose exposures of materials: A new route to circumvent radiation damage☆ , 2014, Ultramicroscopy.

[10]  Ursel Bangert,et al.  Atomically resolved imaging of highly ordered alternating fluorinated graphene , 2014, Nature Communications.

[11]  A. Kirkland,et al.  Exit wave reconstruction of radiation-sensitive materials from low-dose data , 2014 .

[12]  A. Alivisatos,et al.  Controlling electron beam-induced structure modifications and cation exchange in cadmium sulfide-copper sulfide heterostructured nanorods. , 2013, Ultramicroscopy.

[13]  Henry J. Snaith,et al.  Efficient planar heterojunction perovskite solar cells by vapour deposition , 2013, Nature.

[14]  Lin-wang Wang,et al.  Real-time sub- Å ngstrom imaging of reversible and irreversible conformations in rhodium catalysts and graphene , 2013 .

[15]  Yonggang Zhao,et al.  Atomic-scale study of topological vortex-like domain pattern in multiferroic hexagonal manganites , 2013 .

[16]  Sergei V. Kalinin,et al.  Probing oxygen vacancy concentration and homogeneity in solid-oxide fuel-cell cathode materials on the subunit-cell level. , 2012, Nature materials.

[17]  Fu-Rong Chen,et al.  ‘Big Bang’ tomography as a new route to atomic-resolution electron tomography , 2012, Nature.

[18]  P. Nellist The Principles of STEM Imaging , 2011 .

[19]  J. Jinschek,et al.  Quantitative atomic 3-D imaging of single/double sheet graphene structure , 2010 .

[20]  Fu-Rong Chen,et al.  Direct structure inversion from exit waves: Part I: Theory and simulations , 2010 .

[21]  Q. Ramasse,et al.  High-resolution low-dose scanning transmission electron microscopy. , 2010, Journal of electron microscopy.

[22]  S. Pennycook,et al.  Atom-by-atom structural and chemical analysis by annular dark-field electron microscopy , 2010, Nature.

[23]  R. Turchetta,et al.  Enhanced imaging in low dose electron microscopy using electron counting , 2009, Ultramicroscopy.

[24]  D. Muller,et al.  Atomic-Scale Chemical Imaging of Composition and Bonding by Aberration-Corrected Microscopy , 2008, Science.

[25]  Marin Alexe,et al.  Atomic-scale study of electric dipoles near charged and uncharged domain walls in ferroelectric films. , 2008, Nature materials.

[26]  M. Lehmann,et al.  Off-axis electron holography: Materials analysis at atomic resolution , 2006 .

[27]  Fu-Rong Chen,et al.  Resolution extension and exit wave reconstruction in complex HREM. , 2004, Ultramicroscopy.

[28]  C. L. Jia,et al.  Atomic-Resolution Imaging of Oxygen in Perovskite Ceramics , 2003, Science.

[29]  Kirkland,et al.  Discrete atom imaging of one-dimensional crystals formed within single-walled carbon nanotubes , 2000, Science.