Sculpting Nanoscale Functional Channels in Complex Oxides Using Energetic Ions and Electrons

Ritesh Sachan; Eva Zarkadoula; Xin Ou; Christina Trautmann; Yanwen Zhang; Matthew F. Chisholm; William J. Weber

doi:10.1021/acsami.8b02326

Sculpting Nanoscale Functional Channels in Complex Oxides Using Energetic Ions and Electrons

Ritesh Sachan, Eva Zarkadoula, Xin Ou, Christina Trautmann, Yanwen Zhang, Matthew F. Chisholm, William J. Weber

Nanomaterials Theory Institute

Research output: Contribution to journal › Article › peer-review

8 Scopus citations

Abstract

The formation of metastable phases has attracted significant attention because of their unique properties and potential functionalities. In the present study, we demonstrate the phase conversion of energetic-ion-induced amorphous nanochannels/tracks into a metastable defect fluorite in A₂B₂O₇ structured complex oxides by electron irradiation. Through in situ electron irradiation experiments in a scanning transmission electron microscope, we observe electron-induced epitaxial crystallization of the amorphous nanochannels in Yb₂Ti₂O₇ into the defect fluorite. This energetic-electron-induced phase transformation is attributed to the coupled effect of ionization-induced electronic excitations and local heating, along with subthreshold elastic energy transfers. We also show the role of ionic radii of A-site cations (A = Yb, Gd, and Sm) and B-site cations (Ti and Zr) in facilitating the electron-beam-induced crystallization of the amorphous phase to the defect-fluorite structure. The formation of the defect-fluorite structure is eased by the decrease in the difference between ionic radii of A- and B-site cations in the lattice. Molecular dynamics simulations of thermal annealing of the amorphous phase nanochannels in A₂B₂O₇ draw parallels to the electron-irradiation-induced crystallization and confirm the role of ionic radii in lowering the barrier for crystallization. These results suggest that employing guided electron irradiation with atomic precision is a useful technique for selected area phase formation in nanoscale printed devices.

Original language	English
Pages (from-to)	16731-16738
Number of pages	8
Journal	ACS Applied Materials and Interfaces
Volume	10
Issue number	19
DOIs	https://doi.org/10.1021/acsami.8b02326
State	Published - May 16 2018

Funding

This research was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division under contract number DE-AC05-00OR22725. A part of this work was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. The computational research used resources of the National Energy Research Scientific Computing Center, supported by the Office of Science, U.S. Department of Energy, under Contract No. DEAC02-05CH11231. We acknowledge that the 55 MeV I ion irradiation was performed at the Ion Beam Center of Helmholtz-Zentrum Dresden-Rossendorf.

Funders	Funder number
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Division of Materials Sciences and Engineering	DE-AC05-00OR22725, DEAC02-05CH11231

Keywords

Ion irradiation
electron irradiation
in situ scanning transmission electron microscopy
molecular dynamics
phase transformation

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10.1021/acsami.8b02326

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title = "Sculpting Nanoscale Functional Channels in Complex Oxides Using Energetic Ions and Electrons",

abstract = "The formation of metastable phases has attracted significant attention because of their unique properties and potential functionalities. In the present study, we demonstrate the phase conversion of energetic-ion-induced amorphous nanochannels/tracks into a metastable defect fluorite in A2B2O7 structured complex oxides by electron irradiation. Through in situ electron irradiation experiments in a scanning transmission electron microscope, we observe electron-induced epitaxial crystallization of the amorphous nanochannels in Yb2Ti2O7 into the defect fluorite. This energetic-electron-induced phase transformation is attributed to the coupled effect of ionization-induced electronic excitations and local heating, along with subthreshold elastic energy transfers. We also show the role of ionic radii of A-site cations (A = Yb, Gd, and Sm) and B-site cations (Ti and Zr) in facilitating the electron-beam-induced crystallization of the amorphous phase to the defect-fluorite structure. The formation of the defect-fluorite structure is eased by the decrease in the difference between ionic radii of A- and B-site cations in the lattice. Molecular dynamics simulations of thermal annealing of the amorphous phase nanochannels in A2B2O7 draw parallels to the electron-irradiation-induced crystallization and confirm the role of ionic radii in lowering the barrier for crystallization. These results suggest that employing guided electron irradiation with atomic precision is a useful technique for selected area phase formation in nanoscale printed devices.",

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author = "Ritesh Sachan and Eva Zarkadoula and Xin Ou and Christina Trautmann and Yanwen Zhang and Chisholm, {Matthew F.} and Weber, {William J.}",

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AU - Zhang, Yanwen

AU - Chisholm, Matthew F.

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AB - The formation of metastable phases has attracted significant attention because of their unique properties and potential functionalities. In the present study, we demonstrate the phase conversion of energetic-ion-induced amorphous nanochannels/tracks into a metastable defect fluorite in A2B2O7 structured complex oxides by electron irradiation. Through in situ electron irradiation experiments in a scanning transmission electron microscope, we observe electron-induced epitaxial crystallization of the amorphous nanochannels in Yb2Ti2O7 into the defect fluorite. This energetic-electron-induced phase transformation is attributed to the coupled effect of ionization-induced electronic excitations and local heating, along with subthreshold elastic energy transfers. We also show the role of ionic radii of A-site cations (A = Yb, Gd, and Sm) and B-site cations (Ti and Zr) in facilitating the electron-beam-induced crystallization of the amorphous phase to the defect-fluorite structure. The formation of the defect-fluorite structure is eased by the decrease in the difference between ionic radii of A- and B-site cations in the lattice. Molecular dynamics simulations of thermal annealing of the amorphous phase nanochannels in A2B2O7 draw parallels to the electron-irradiation-induced crystallization and confirm the role of ionic radii in lowering the barrier for crystallization. These results suggest that employing guided electron irradiation with atomic precision is a useful technique for selected area phase formation in nanoscale printed devices.

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Sculpting Nanoscale Functional Channels in Complex Oxides Using Energetic Ions and Electrons

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