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Author |
Do, M.T.; Gauquelin, N.; Nguyen, M.D.; Blom, F.; Verbeeck, J.; Koster, G.; Houwman, E.P.; Rijnders, G. |
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Title |
Interface degradation and field screening mechanism behind bipolar-cycling fatigue in ferroelectric capacitors |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Apl Materials |
Abbreviated Journal |
Apl Mater |
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Volume |
9 |
Issue |
2 |
Pages |
021113 |
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Keywords  |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Polarization fatigue, i.e., the loss of polarization of ferroelectric capacitors upon field cycling, has been widely discussed as an interface related effect. However, mechanism(s) behind the development of fatigue have not been fully identified. Here, we study the fatigue mechanisms in Pt/PbZr0.52Ti0.48O3/SrRuO3 (Pt/PZT/SRO) capacitors in which all layers are fabricated by pulsed laser deposition without breaking the vacuum. With scanning transmission electron microscopy, we observed that in the fatigued capacitor, the Pt/PZT interface becomes structurally degraded, forming a 5 nm-10 nm thick non-ferroelectric layer of crystalline ZrO2 and diffused Pt grains. We then found that the fatigued capacitors can regain the full initial polarization switching if the externally applied field is increased to at least 10 times the switching field of the pristine capacitor. These findings suggest that polarization fatigue is driven by a two-step mechanism. First, the transient depolarization field that repeatedly appears during the domain switching under field cycling causes decomposition of the metal/ferroelectric interface, resulting in a non-ferroelectric degraded layer. Second, this interfacial non-ferroelectric layer screens the external applied field causing an increase in the coercive field beyond the usually applied maximum field and consequently suppresses the polarization switching in the cycled capacitor. Our work clearly confirms the key role of the electrode/ferroelectric interface in the endurance of ferroelectric-based devices. |
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Wos |
000630052100006 |
Publication Date |
2021-02-09 |
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Series Issue |
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Edition |
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ISSN |
2166-532x |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.335 |
Times cited |
5 |
Open Access |
OpenAccess |
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Notes |
This work was supported by the Nederlandse Organisatie voor Wetenschappelijk Onderzoek through Grant No. F62.3.15559. The Qu-Ant-EM microscope and the direct electron detector were partly funded by the Hercules fund from the Flemish Government. N.G. and J.V. acknowledge funding from the GOA project “Solarpaint” of the University of Antwerp. This work has also received funding from the European Union's Horizon 2020 research and innovation program under Grant No. 823717-ESTEEM3. We acknowledge D. Chezganov for his useful insights. |
Approved |
Most recent IF: 4.335 |
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Call Number |
UA @ admin @ c:irua:177663 |
Serial |
6783 |
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Author |
Chen, B.; Gauquelin, N.; Strkalj, N.; Huang, S.; Halisdemir, U.; Nguyen, M.D.; Jannis, D.; Sarott, M.F.; Eltes, F.; Abel, S.; Spreitzer, M.; Fiebig, M.; Trassin, M.; Fompeyrine, J.; Verbeeck, J.; Huijben, M.; Rijnders, G.; Koster, G. |
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Title |
Signatures of enhanced out-of-plane polarization in asymmetric BaTiO3 superlattices integrated on silicon |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
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Volume |
13 |
Issue |
1 |
Pages |
265 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
In order to bring the diverse functionalities of transition metal oxides into modern electronics, it is imperative to integrate oxide films with controllable properties onto the silicon platform. Here, we present asymmetric LaMnO<sub>3</sub>/BaTiO<sub>3</sub>/SrTiO<sub>3</sub>superlattices fabricated on silicon with layer thickness control at the unit-cell level. By harnessing the coherent strain between the constituent layers, we overcome the biaxial thermal tension from silicon and stabilize<italic>c</italic>-axis oriented BaTiO<sub>3</sub>layers with substantially enhanced tetragonality, as revealed by atomically resolved scanning transmission electron microscopy. Optical second harmonic generation measurements signify a predominant out-of-plane polarized state with strongly enhanced net polarization in the tricolor superlattices, as compared to the BaTiO<sub>3</sub>single film and conventional BaTiO<sub>3</sub>/SrTiO<sub>3</sub>superlattice grown on silicon. Meanwhile, this coherent strain in turn suppresses the magnetism of LaMnO<sub>3</sub>as the thickness of BaTiO<sub>3</sub>increases. Our study raises the prospect of designing artificial oxide superlattices on silicon with tailored functionalities. |
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Wos |
000741852200073 |
Publication Date |
2022-01-11 |
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Edition |
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ISSN |
2041-1723 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
16.6 |
Times cited |
11 |
Open Access |
OpenAccess |
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Notes |
This project has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No 823717—ESTEEM3. B.C. is sponsored by Shanghai Sailing Program 21YF1410700. J.V. and N.G. acknowledge funding through the GOA project “Solarpaint” of the University of Antwerp. The microscope used in this work was partly funded by the Hercules Fund from the Flemish Government. D.J. acknowledges funding from FWO Project G093417N from the Flemish fund for scientific research. M.T., N.S., M.F.S. and M.F. acknowledge the financial support by the EU European Research Council (Advanced Grant 694955—INSEETO). M.T. acknowledges the Swiss National Science Foundation under Project No. 200021-188414. N.S. acknowledges support under the Swiss National Science Foundation under Project No. P2EZP2-199913. M.S. acknowledges funding from Slovenian Research Agency (Grants No. J2-2510, N2-0149 and P2-0091). B.C. acknowledges Prof. C.D.; Prof. F.Y.; Prof. B.T. and Dr. K.J. for valuable discussions.; esteem3reported; esteem3TA |
Approved |
Most recent IF: 16.6 |
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Call Number |
EMAT @ emat @c:irua:185179 |
Serial |
6902 |
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Author |
Verdierre, G.; Gauquelin, N.; Jannis, D.; Birkhölzer, Y.A.; Mallik, S.; Verbeeck, J.; Bibes, M.; Koster, G. |
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Title |
Epitaxial growth of the candidate ferroelectric Rashba material SrBiO3by pulsed laser deposition |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
APL materials |
Abbreviated Journal |
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Volume |
11 |
Issue |
3 |
Pages |
031109 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Among oxides, bismuthates have been gaining much interest due to their unique features. In addition to their superconducting properties, they show potential for applications as topological insulators and as possible spin-to-charge converters. After being first investigated in their bulk form in the 1980s, bismuthates have been successfully grown as thin films. However, most efforts have focused on BaBiO<sub>3</sub>, with SrBiO<sub>3</sub>receiving only little attention. Here, we report the growth of epitaxial films of SrBiO<sub>3</sub>on both TiO<sub>2</sub>-terminated SrTiO<sub>3</sub>and NdO-terminated NdScO<sub>3</sub>substrates by pulsed laser deposition. SrBiO<sub>3</sub>has a pseudocubic lattice constant of ∼4.25 Å and grows relaxed on NdScO<sub>3</sub>. Counter-intuitively, it grows with a slight tensile strain on SrTiO<sub>3</sub>despite a large lattice mismatch, which should induce compressive strain. High-resolution transmission electron microscopy reveals that this occurs as a consequence of structural domain matching, with blocks of 10 SrBiO<sub>3</sub>unit planes matching blocks of 11 SrTiO<sub>3</sub>unit planes. This work provides a framework for the synthesis of high quality perovskite bismuthates films and for the understanding of their interface interactions with homostructural substrates. |
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Wos |
000953363800004 |
Publication Date |
2023-03-01 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2166-532X |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
6.1 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
This work received support from the ERC Advanced grant (Grant No. 833973) “FRESCO” and funding from the European Union’s Horizon 2020 Research and Innovation Program under Grant Agreement No. 823717—ESTEEM3, Van Gogh travel grant, Nuffic, The Netherlands (CF No. 42582SB).; esteem3reported; esteem3TA |
Approved |
Most recent IF: 6.1; 2023 IF: 4.335 |
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Call Number |
EMAT @ emat @c:irua:196135 |
Serial |
7377 |
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Author |
Kante, M.V.; Weber, M.L.; Ni, S.; van den Bosch, I.C.G.; van der Minne, E.; Heymann, L.; Falling, L.J.; Gauquelin, N.; Tsvetanova, M.; Cunha, D.M.; Koster, G.; Gunkel, F.; Nemsak, S.; Hahn, H.; Estrada, L.V.; Baeumer, C. |
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Title |
A high-entropy oxide as high-activity electrocatalyst for water oxidation |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
ACS nano |
Abbreviated Journal |
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Volume |
17 |
Issue |
6 |
Pages |
5329-5339 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
High-entropy materials are an emerging pathway in the development of high-activity (electro)catalysts because of the inherent tunability and coexistence of multiple potential active sites, which may lead to earth-abundant catalyst materials for energy-efficient electrochemical energy storage. In this report, we identify how the multication composition in high-entropy perovskite oxides (HEO) contributes to high catalytic activity for the oxygen evolution reaction (OER), i.e., the key kinetically limiting half-reaction in several electrochemical energy conversion technologies, including green hydrogen generation. We compare the activity of the (001) facet of LaCr0.2Mn0.2Fe0.2Co0.2Ni0.2O3-delta with the parent compounds (single B-site in the ABO3 perovskite). While the single B-site perovskites roughly follow the expected volcano-type activity trends, the HEO clearly outperforms all of its parent compounds with 17 to 680 times higher currents at a fixed overpotential. As all samples were grown as an epitaxial layer, our results indicate an intrinsic composition-function relationship, avoiding the effects of complex geometries or unknown surface composition. In-depth X-ray photoemission studies reveal a synergistic effect of simultaneous oxidation and reduction of different transition metal cations during the adsorption of reaction intermediates. The surprisingly high OER activity demonstrates that HEOs are a highly attractive, earth-abundant material class for high-activity OER electrocatalysts, possibly allowing the activity to be fine-tuned beyond the scaling limits of mono-or bimetallic oxides. |
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Wos |
000953440900001 |
Publication Date |
2023-03-13 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1936-0851 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
17.1 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 17.1; 2023 IF: 13.942 |
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Call Number |
UA @ admin @ c:irua:196097 |
Serial |
7390 |
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Author |
Ni, S.; Houwman, E.; Gauquelin, N.; Chezganov, D.; Van Aert, S.; Verbeeck, J.; Rijnders, G.; Koster, G. |
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Title |
Stabilizing perovskite Pb(Mg0.33Nb0.67)O3-PbTiO3 thin films by fast deposition and tensile mismatched growth template |
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A1 Journal article |
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Year |
2024 |
Publication |
ACS applied materials and interfaces |
Abbreviated Journal |
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Volume |
16 |
Issue |
10 |
Pages |
12744-12753 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Because of its low hysteresis, high dielectric constant, and strong piezoelectric response, Pb(Mg1/3Nb2/3)O-3-PbTiO3 (PMN-PT) thin films have attracted considerable attention for the application in PiezoMEMS, field-effect transistors, and energy harvesting and storage devices. However, it remains a great challenge to fabricate phase-pure, pyrochlore-free PMN-PT thin films. In this study, we demonstrate that a high deposition rate, combined with a tensile mismatched template layer can stabilize the perovskite phase of PMN-PT films and prevent the nucleation of passive pyrochlore phases. We observed that an accelerated deposition rate promoted mixing of the B-site cation and facilitated relaxation of the compressively strained PMN-PT on the SrTiO3 (STO) substrate in the initial growth layer, which apparently suppressed the initial formation of pyrochlore phases. By employing La-doped-BaSnO3 (LBSO) as the tensile mismatched buffer layer, 750 nm thick phase-pure perovskite PMN-PT films were synthesized. The resulting PMN-PT films exhibited excellent crystalline quality close to that of the STO substrate. |
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Wos |
001176343700001 |
Publication Date |
2024-02-29 |
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Series Editor |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1944-8244 |
ISBN |
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Additional Links |
UA library record; WoS full record |
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Impact Factor |
9.5 |
Times cited |
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Open Access |
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Notes |
We would like to acknowledge the Netherlands Organization for Scientific Research (NWO) for the financial support of this work. This project has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No. 823717-ESTEEM3. |
Approved |
Most recent IF: 9.5; 2024 IF: 7.504 |
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Call Number |
UA @ admin @ c:irua:204754 |
Serial |
9174 |
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