Atomic‐Level Sculpting of Crystalline Oxides: Toward Bulk Nanofabrication with Single Atomic Plane Precision

Jesse, Stephen; He, Qian; Lupini, Andrew R.; Leonard, Donovan N.; Oxley, Mark P.; Ovchinnikov, O. S.; Unocic, Raymond R.; Tselev, Alexander; Fuentes‐Cabrera, Miguel; Sumpter, Bobby G.; Pennycook, Stephen J.; Kalinin, Sergei V.; Borisevich, Albina Y.

doi:10.1002/smll.201502048

Cited by 87 publications

(88 citation statements)

References 34 publications

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“…Another promising application of beam control in STEM is electron beam induced modification of materials2526, which has the potential to lead to the development of the next-generation of lithography or nanofabrication methods. For example, an atomic-scale, beam-induced amorphous to crystalline phase transformation in SrTiO 3 was performed with 2 nm spatial resolution using an external beam control system27. Furthermore, precision control of electron beam irradiation can be used to induce and direct metal deposition from liquid phase precursors to form nanostructured architectures2628.…”

Section: Resultsmentioning

confidence: 99%

Precision controlled atomic resolution scanning transmission electron microscopy using spiral scan pathways

Sang

Lupini

Ding

et al. 2017

Sci Rep

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Atomic-resolution imaging in an aberration-corrected scanning transmission electron microscope (STEM) can enable direct correlation between atomic structure and materials functionality. The fast and precise control of the STEM probe is, however, challenging because the true beam location deviates from the assigned location depending on the properties of the deflectors. To reduce these deviations, i.e. image distortions, we use spiral scanning paths, allowing precise control of a sub-Å sized electron probe within an aberration-corrected STEM. Although spiral scanning avoids the sudden changes in the beam location (fly-back distortion) present in conventional raster scans, it is not distortion-free. “Archimedean” spirals, with a constant angular frequency within each scan, are used to determine the characteristic response at different frequencies. We then show that such characteristic functions can be used to correct image distortions present in more complicated constant linear velocity spirals, where the frequency varies within each scan. Through the combined application of constant linear velocity scanning and beam path corrections, spiral scan images are shown to exhibit less scan distortion than conventional raster scan images. The methodology presented here will be useful for in situ STEM imaging at higher temporal resolution and for imaging beam sensitive materials.

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Section: Resultsmentioning

confidence: 99%

Precision controlled atomic resolution scanning transmission electron microscopy using spiral scan pathways

Sang

Lupini

Ding

et al. 2017

Sci Rep

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“…An electron beam as fine as an atom is scanned through the specimen to probe its structure 3 . Several groups have used STEM to transform the compositions of layered materials in places 4,5 , crystallize amorphous oxides 6 , move atoms between spaces in a lattice 7 and knock out single atoms from one-layer materials.…”

Section: Feedback Systemmentioning

confidence: 99%

Fire up the atom forge

Kalinin

Borisevich

Jesse

2016

Nature

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Scanning transmission electron microscopy has been used to reveal the hexagonal arrangement of the uranium atoms in a solution of uranyl acetate. material to pinpoint atoms and reveal the material's crystal structure. For imaging, the downside is that the beam can move atoms slightly. But if these modifications can be controlled, it could be a boon. New materials could be built atom by atom by controlling the electron beam precisely. Such bespoke materials might enable new classes of devices for quantum computing, spin sensing and more.

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“…In general, electron-beam illumination is known to cause ionization, heating, electrostatic charging, and knock-on damage in materials (18)(19)(20)(21). These possible effects were therefore investigated.…”

Section: Significancementioning

confidence: 99%

Reversible structure manipulation by tuning carrier concentration in metastable Cu ₂ S

Tao

Chen

et al. 2017

Proc. Natl. Acad. Sci. U.S.A.

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The optimal functionalities of materials often appear at phase transitions involving simultaneous changes in the electronic structure and the symmetry of the underlying lattice. It is experimentally challenging to disentangle which of the two effects--electronic or structural--is the driving force for the phase transition and to use the mechanism to control material properties. Here we report the concurrent pumping and probing of Cu 2 S nanoplates using an electron beam to directly manipulate the transition between two phases with distinctly different crystal symmetries and charge-carrier concentrations, and show that the transition is the result of charge generation for one phase and charge depletion for the other. We demonstrate that this manipulation is fully reversible and nonthermal in nature. Our observations reveal a phase-transition pathway in materials, where electron-induced changes in the electronic structure can lead to a macroscopic reconstruction of the crystal structure. functional and quantum materials--the key properties of functional materials are often born out of strong structural and electronic interactions that are quantum mechanical in nature. Notable examples include colossal magnetoresistance manganites (1), ferroelectrics (2), and valleytronic materials (3). The targeted functions are usually accompanied by symmetry breaking, induced through changes in temperature or under other external perturbations. A prominent question is whether the symmetry reduction has an origin in the lattice (e.g., in the form of displacement of atoms, and could be described reasonably well using first-principles calculations) or the electronic degrees of freedom (charge, spin, and orbital) (4-6). It is of great interest to distinguish the roles of these factors in phase transitions.Cu 2 S provides an intriguing example for addressing the above "chicken-and-egg" question (6), which is critical to the understanding of a wide range of functional and quantum materials. It is a fast ionic conductor (7) with highly mobile Cu ions. A phase transition in the bulk material occurs near 100°C from a semiconducting (8) monoclinic symmetry low-chalcocite phase (9) [hereafter called the "L-s phase" (i.e., low, semiconducting); space group P2 1 /c] to an electrically insulating (10) hexagonal symmetry high-chalcocite phase (7, 11) [hereafter called the "H-i phase" (i.e., high, insulating); space group P6 3 /mmc]. The coinciding changes in the bulk electrical conductivity and crystal structure present a possibility for exploring the relationship between electronic and structural phase transitions. Difficulties in the synthesis of stoichiometric Cu 2 S material and the lack of detailed theoretical treatments of both the crystal and the electronic structures of Cu 2 S have hindered the understanding of the phase transition (7, 11-13). Results and DiscussionWe have recently synthesized high-quality Cu 2 S nanoplates (Materials and Methods), which are on the order of 10-nm thick and 100 nm in lateral dimension ( Fig. 1 A and B)....

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Atomic‐Level Sculpting of Crystalline Oxides: Toward Bulk Nanofabrication with Single Atomic Plane Precision

Cited by 87 publications

References 34 publications

Precision controlled atomic resolution scanning transmission electron microscopy using spiral scan pathways

Precision controlled atomic resolution scanning transmission electron microscopy using spiral scan pathways

Fire up the atom forge

Reversible structure manipulation by tuning carrier concentration in metastable Cu ₂ S

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Atomic‐Level Sculpting of Crystalline Oxides: Toward Bulk Nanofabrication with Single Atomic Plane Precision

Cited by 87 publications

References 34 publications

Precision controlled atomic resolution scanning transmission electron microscopy using spiral scan pathways

Precision controlled atomic resolution scanning transmission electron microscopy using spiral scan pathways

Fire up the atom forge

Reversible structure manipulation by tuning carrier concentration in metastable Cu 2 S

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Product

Resources

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Reversible structure manipulation by tuning carrier concentration in metastable Cu ₂ S