Real-space charge-density imaging with sub-ångström resolution by four-dimensional electron microscopy

Gao, Wenpei; Addiego, Christopher; Wang, Hui; Yan, Xingxu; Hou, Yusheng; Ji, Dianxiang; Heikes, Colin; Zhang, Yi; Li, Linze; Huyan, Huaixun; Blum, Thomas; Aoki, Toshihiro; Nie, Yuefeng; Schlom, Darrell G.; Wu, Ruqian; Pan, Xiaoqing

doi:10.1038/s41586-019-1649-6

Cited by 160 publications

(141 citation statements)

References 49 publications

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“…DPC results were obtained using an FEI Talos F200X with a field-emission gun and an accelerating voltage of 200 kV. According to the established DPC methodology 23,24,[27][28][29] , the electric field (E) at a site with the coordinates of (x, y) in a sample can be obtained from four DPC images (see a set of typical DPC images in Supplementary Fig. 5) using the following equation:…”

Section: Discussionmentioning

confidence: 99%

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In-situ visualization of the space-charge-layer effect on interfacial lithium-ion transport in all-solid-state batteries

Xie²,

et al. 2020

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The space charge layer (SCL) is generally considered one of the origins of the sluggish interfacial lithium-ion transport in all-solid-state lithium-ion batteries (ASSLIBs). However, in-situ visualization of the SCL effect on the interfacial lithium-ion transport in sulfide-based ASSLIBs is still a great challenge. Here, we directly observe the electrode/electrolyte interface lithium-ion accumulation resulting from the SCL by investigating the net-charge-density distribution across the high-voltage LiCoO2/argyrodite Li6PS5Cl interface using the in-situ differential phase contrast scanning transmission electron microscopy (DPC-STEM) technique. Moreover, we further demonstrate a built-in electric field and chemical potential coupling strategy to reduce the SCL formation and boost lithium-ion transport across the electrode/electrolyte interface by the in-situ DPC-STEM technique and finite element method simulations. Our findings will strikingly advance the fundamental scientific understanding of the SCL mechanism in ASSLIBs and shed light on rational electrode/electrolyte interface design for high-rate performance ASSLIBs.

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Section: Discussionmentioning

confidence: 99%

“…According to Gauss's law, the charge-density map can be obtained by calculating the differential of the electric field map 23,24,[59][60][61][62] . Then, according to the relation between the electric field (E) and charge density (ρ) 49,51 ρ…”

Section: Discussionmentioning

confidence: 99%

In-situ visualization of the space-charge-layer effect on interfacial lithium-ion transport in all-solid-state batteries

Xie²,

et al. 2020

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“…The future research frontiers of AET bring up more challenges and opportunities in solving fundamental problems such as disorder structures, electron beam sensitive structures and in situ 3D atomic dynamics. Several novel techniques could be employed to further improve the capabilities of AET, such as ptychography, [79][80][81] atomic elemental mapping, [82][83] 4D-STEM, [84][85] dose-efficient STEM, 86 low-dose modality imaging schemes with either advanced direct electron detectors 87 or cryogen temperature environment, [88][89] and in situ atomic imaging microscopy. [90][91] On the algorithm and method side, new method, 92 new reconstruction algorithm 93 and machine learning could further extend the applicability of AET to 2D materials, heterostructures, thin films and other material systems.…”

Section: Discussionmentioning

confidence: 99%

Atomic electron tomography in three and four dimensions

et al. 2020

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“…To improve the signal-to-noise ratio (SNR) and to minimize the image distortion of HAADF and ABF images, 10 serial frames were acquired with a short dwell time (2 μs/pixel), aligned and added afterward. 27 EELS acquisition was performed by a Gatan GIF Quantum ERS imaging filter with dual-EELS acquisition capability with a convergent semiangle of 20.4 mrad and a probe size of 1 Å (5C), which is larger than that of STEM imaging. While the spatial resolution becomes worse as the probe size increases, the probe current rises, allowing for enhanced EELS analysis with a higher signal-to-noise ratio.…”

Section: Methodsmentioning

confidence: 99%

Probing Charge Accumulation at SrMnO₃/SrTiO₃ Heterointerfaces via Advanced Electron Microscopy and Spectroscopy

et al. 2020

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The last three decades have seen a growing trend toward studying the interfacial phenomena in complex oxide heterostructures. Of particular concern is the charge distribution at interfaces, which is a crucial factor in controlling the interface transport behavior. However, the study of the charge distribution is very challenging due to its small length scale and the intricate structure and chemistry at interfaces. Furthermore, the underlying origin of the interfacial charge distribution has been rarely studied in-depth and is still poorly understood. Here, by a combination of aberration-corrected scanning transmission electron microscopy (STEM) and spectroscopy techniques, we identify the charge accumulation in the SrMnO 3 (SMO) side of SrMnO 3 /SrTiO 3 heterointerfaces and find that the charge density attains the maximum of 0.13 ± 0.07 e – /unit cell (uc) at the first SMO monolayer. Based on quantitative atomic-scale STEM analyses and first-principle calculations, we explore the origin of interfacial charge accumulation in terms of epitaxial strain-favored oxygen vacancies, cationic interdiffusion, interfacial charge transfer, and space-charge effects. This study, therefore, provides a comprehensive description of the charge distribution and related mechanisms at the SMO/STO heterointerfaces, which is beneficial for the functionality manipulation via charge engineering at interfaces.

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Real-space charge-density imaging with sub-ångström resolution by four-dimensional electron microscopy

Cited by 160 publications

References 49 publications

In-situ visualization of the space-charge-layer effect on interfacial lithium-ion transport in all-solid-state batteries

In-situ visualization of the space-charge-layer effect on interfacial lithium-ion transport in all-solid-state batteries

Atomic electron tomography in three and four dimensions

Probing Charge Accumulation at SrMnO₃/SrTiO₃ Heterointerfaces via Advanced Electron Microscopy and Spectroscopy

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Real-space charge-density imaging with sub-ångström resolution by four-dimensional electron microscopy

Cited by 160 publications

References 49 publications

In-situ visualization of the space-charge-layer effect on interfacial lithium-ion transport in all-solid-state batteries

In-situ visualization of the space-charge-layer effect on interfacial lithium-ion transport in all-solid-state batteries

Atomic electron tomography in three and four dimensions

Probing Charge Accumulation at SrMnO3/SrTiO3 Heterointerfaces via Advanced Electron Microscopy and Spectroscopy

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Product

Resources

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Probing Charge Accumulation at SrMnO₃/SrTiO₃ Heterointerfaces via Advanced Electron Microscopy and Spectroscopy