Electromechanically active pairs dynamics in Gd-doped ceria single crystal

Simone Santucci; Haiwu Zhang; Ahsanul Kabir; Carlo  Marini; Simone Sanna; Jyn Kyu  Han; Gregor  Ulbrich; Eva Maria  Heppke; Ivano Eligio Castelli; Vincenzo Esposito

doi:10.1039/D1CP00748C

Electromechanically active pairs dynamics in Gd-doped ceria single crystal

Simone Santucci^*, Haiwu Zhang, Ahsanul Kabir, Carlo Marini, Simone Sanna, Jyn Kyu Han, Gregor Ulbrich, Eva Maria Heppke, Ivano Eligio Castelli, Vincenzo Esposito^*

^*Corresponding author for this work

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Abstract

Oxygen defective ceria, e.g. Gd-doped ceria, shows giant electromechanical properties related to a complex local rearrangement of its lattice. Although they are not entirely identified, the electroactive mechanisms arise from cations and oxygen vacancies (V_O) pairs (Ce-V_O), and the local structural elastic distortion in their surroundings. Here, we study the geometry and behaviour of Ce-Vo pairs in a grain boundaries-free bulk Ce_0.9Gd_0.1O_1.95 single crystal under an AC electric field of ca. 11 kV/cm. The analysis was carried out through X-ray absorption spectroscopy (XAS) techniques at Ce L-III edge. Using Density Functional Theory (DFT) calculations, we investigated the effects of the strain on states' density and orbitals at the valence band edge. Our research indicates that the electrostriction increases at low temperatures. The electromechanical strain has a structural nature and can rise of one order of magnitude, i.e., from 5·10^-4 at room temperature to 5·10^-3 at -193 °C, due to an increase in the population of the electrically active pairs. At a constant VO concentration, the material can thus configure heterogeneous pairs and elastic nanodomains that are either mechanically responsive or not.

Original language	English
Journal	Physical Chemistry Chemical Physics
Volume	23
Issue number	19
Pages (from-to)	11233-11239
Number of pages	7
ISSN	1463-9076
DOIs	https://doi.org/10.1039/D1CP00748C
Publication status	Published - 2021

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title = "Electromechanically active pairs dynamics in Gd-doped ceria single crystal",

abstract = "Oxygen defective ceria, e.g. Gd-doped ceria, shows giant electromechanical properties related to a complex local rearrangement of its lattice. Although they are not entirely identified, the electroactive mechanisms arise from cations and oxygen vacancies (VO) pairs (Ce-VO), and the local structural elastic distortion in their surroundings. Here, we study the geometry and behaviour of Ce-Vo pairs in a grain boundaries-free bulk Ce0.9Gd0.1O1.95 single crystal under an AC electric field of ca. 11 kV/cm. The analysis was carried out through X-ray absorption spectroscopy (XAS) techniques at Ce L-III edge. Using Density Functional Theory (DFT) calculations, we investigated the effects of the strain on states' density and orbitals at the valence band edge. Our research indicates that the electrostriction increases at low temperatures. The electromechanical strain has a structural nature and can rise of one order of magnitude, i.e., from 5·10-4 at room temperature to 5·10-3 at -193 °C, due to an increase in the population of the electrically active pairs. At a constant VO concentration, the material can thus configure heterogeneous pairs and elastic nanodomains that are either mechanically responsive or not.",

author = "Simone Santucci and Haiwu Zhang and Ahsanul Kabir and Carlo Marini and Simone Sanna and Han, {Jyn Kyu} and Gregor Ulbrich and Heppke, {Eva Maria} and Castelli, {Ivano Eligio} and Vincenzo Esposito",

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doi = "10.1039/D1CP00748C",

language = "English",

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journal = "Physical Chemistry Chemical Physics",

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publisher = "Royal Society of Chemistry",

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TY - JOUR

T1 - Electromechanically active pairs dynamics in Gd-doped ceria single crystal

AU - Santucci, Simone

AU - Zhang, Haiwu

AU - Kabir, Ahsanul

AU - Marini, Carlo

AU - Sanna, Simone

AU - Han, Jyn Kyu

AU - Ulbrich, Gregor

AU - Heppke, Eva Maria

AU - Castelli, Ivano Eligio

AU - Esposito, Vincenzo

PY - 2021

Y1 - 2021

N2 - Oxygen defective ceria, e.g. Gd-doped ceria, shows giant electromechanical properties related to a complex local rearrangement of its lattice. Although they are not entirely identified, the electroactive mechanisms arise from cations and oxygen vacancies (VO) pairs (Ce-VO), and the local structural elastic distortion in their surroundings. Here, we study the geometry and behaviour of Ce-Vo pairs in a grain boundaries-free bulk Ce0.9Gd0.1O1.95 single crystal under an AC electric field of ca. 11 kV/cm. The analysis was carried out through X-ray absorption spectroscopy (XAS) techniques at Ce L-III edge. Using Density Functional Theory (DFT) calculations, we investigated the effects of the strain on states' density and orbitals at the valence band edge. Our research indicates that the electrostriction increases at low temperatures. The electromechanical strain has a structural nature and can rise of one order of magnitude, i.e., from 5·10-4 at room temperature to 5·10-3 at -193 °C, due to an increase in the population of the electrically active pairs. At a constant VO concentration, the material can thus configure heterogeneous pairs and elastic nanodomains that are either mechanically responsive or not.

AB - Oxygen defective ceria, e.g. Gd-doped ceria, shows giant electromechanical properties related to a complex local rearrangement of its lattice. Although they are not entirely identified, the electroactive mechanisms arise from cations and oxygen vacancies (VO) pairs (Ce-VO), and the local structural elastic distortion in their surroundings. Here, we study the geometry and behaviour of Ce-Vo pairs in a grain boundaries-free bulk Ce0.9Gd0.1O1.95 single crystal under an AC electric field of ca. 11 kV/cm. The analysis was carried out through X-ray absorption spectroscopy (XAS) techniques at Ce L-III edge. Using Density Functional Theory (DFT) calculations, we investigated the effects of the strain on states' density and orbitals at the valence band edge. Our research indicates that the electrostriction increases at low temperatures. The electromechanical strain has a structural nature and can rise of one order of magnitude, i.e., from 5·10-4 at room temperature to 5·10-3 at -193 °C, due to an increase in the population of the electrically active pairs. At a constant VO concentration, the material can thus configure heterogeneous pairs and elastic nanodomains that are either mechanically responsive or not.

U2 - 10.1039/D1CP00748C

DO - 10.1039/D1CP00748C

M3 - Journal article

SN - 1463-9076

VL - 23

SP - 11233

EP - 11239

JO - Physical Chemistry Chemical Physics

JF - Physical Chemistry Chemical Physics

IS - 19

ER -

Electromechanically active pairs dynamics in Gd-doped ceria single crystal

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