Memristors Based on Ni(II)‐tetraaza[14]annulene Complexes: Toward an Unconventional Resistive Switching Mechanism

Abstract In this work, a family of Ni‐based dibenzotetraaza[14]annulene (dtaa) complexes are investigated for their application in memristors (memory resistors). A series of four Ni(II) complexes with different peripheral substituents of the dtaa ligand are successfully synthesized. Based on these c...

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Main Authors: Andrzej Sławek, Lulu Alluhaibi, Ewelina Kowalewska, Gisya Abdi, Tomasz Mazur, Agnieszka Podborska, Krzysztof Mech, Marianna Marciszko‐Wiąckowska, Alexey Maximenko, Konrad Szaciłowski
Format: Article
Language:English
Published: Wiley-VCH 2024-12-01
Series:Advanced Electronic Materials
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Online Access:https://doi.org/10.1002/aelm.202300818
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author Andrzej Sławek
Lulu Alluhaibi
Ewelina Kowalewska
Gisya Abdi
Tomasz Mazur
Agnieszka Podborska
Krzysztof Mech
Marianna Marciszko‐Wiąckowska
Alexey Maximenko
Konrad Szaciłowski
author_facet Andrzej Sławek
Lulu Alluhaibi
Ewelina Kowalewska
Gisya Abdi
Tomasz Mazur
Agnieszka Podborska
Krzysztof Mech
Marianna Marciszko‐Wiąckowska
Alexey Maximenko
Konrad Szaciłowski
author_sort Andrzej Sławek
collection DOAJ
description Abstract In this work, a family of Ni‐based dibenzotetraaza[14]annulene (dtaa) complexes are investigated for their application in memristors (memory resistors). A series of four Ni(II) complexes with different peripheral substituents of the dtaa ligand are successfully synthesized. Based on these compounds, two‐terminal thin‐film devices are fabricated in planar architecture. Four metals with different work functions are tested: Mg, Cu, Ni, and Au. It is demonstrated that ITO|[Ni(Me4dtaa)]|Cu devices show hysteretic behavior and offer stable, robust, and reproducible switching between high‐ and low‐resistive states. An in‐depth spectroscopic characterization of the Ni complex is performed, using radiation from infrared, through visible and ultraviolet, to tender X‐rays. Operando X‐ray fluorescence spectroscopy is used to monitor redox and structural changes upon the polarization of the studied memristor with the external electric field. Density functional theory calculations are used to better understand the electronic structure of the studied material, as well as structural rearrangement after electron injection that may be responsible for the modulation of electric conductivity. Finding a unique case of filamentary‐type resistive switching involving redox reactions of stationary molecules within a molecular solid is postulated. Yet, the formation of these filaments is not related to any significant configurational changes at the atomic scale.
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issn 2199-160X
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publisher Wiley-VCH
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series Advanced Electronic Materials
spelling doaj-art-beb7eaaacfd6460fa229bbfd35bb14072025-08-20T02:47:33ZengWiley-VCHAdvanced Electronic Materials2199-160X2024-12-011012n/an/a10.1002/aelm.202300818Memristors Based on Ni(II)‐tetraaza[14]annulene Complexes: Toward an Unconventional Resistive Switching MechanismAndrzej Sławek0Lulu Alluhaibi1Ewelina Kowalewska2Gisya Abdi3Tomasz Mazur4Agnieszka Podborska5Krzysztof Mech6Marianna Marciszko‐Wiąckowska7Alexey Maximenko8Konrad Szaciłowski9Academic Centre for Materials and Nanotechnology AGH University of Krakow al. Mickiewicza 30 Kraków 30–059 PolandAcademic Centre for Materials and Nanotechnology AGH University of Krakow al. Mickiewicza 30 Kraków 30–059 PolandAcademic Centre for Materials and Nanotechnology AGH University of Krakow al. Mickiewicza 30 Kraków 30–059 PolandAcademic Centre for Materials and Nanotechnology AGH University of Krakow al. Mickiewicza 30 Kraków 30–059 PolandAcademic Centre for Materials and Nanotechnology AGH University of Krakow al. Mickiewicza 30 Kraków 30–059 PolandAcademic Centre for Materials and Nanotechnology AGH University of Krakow al. Mickiewicza 30 Kraków 30–059 PolandAcademic Centre for Materials and Nanotechnology AGH University of Krakow al. Mickiewicza 30 Kraków 30–059 PolandAcademic Centre for Materials and Nanotechnology AGH University of Krakow al. Mickiewicza 30 Kraków 30–059 PolandNational Synchrotron Radiation Centre SOLARIS Jagiellonian University ul. Czerwone Maki 98 Kraków 30‑392 PolandAcademic Centre for Materials and Nanotechnology AGH University of Krakow al. Mickiewicza 30 Kraków 30–059 PolandAbstract In this work, a family of Ni‐based dibenzotetraaza[14]annulene (dtaa) complexes are investigated for their application in memristors (memory resistors). A series of four Ni(II) complexes with different peripheral substituents of the dtaa ligand are successfully synthesized. Based on these compounds, two‐terminal thin‐film devices are fabricated in planar architecture. Four metals with different work functions are tested: Mg, Cu, Ni, and Au. It is demonstrated that ITO|[Ni(Me4dtaa)]|Cu devices show hysteretic behavior and offer stable, robust, and reproducible switching between high‐ and low‐resistive states. An in‐depth spectroscopic characterization of the Ni complex is performed, using radiation from infrared, through visible and ultraviolet, to tender X‐rays. Operando X‐ray fluorescence spectroscopy is used to monitor redox and structural changes upon the polarization of the studied memristor with the external electric field. Density functional theory calculations are used to better understand the electronic structure of the studied material, as well as structural rearrangement after electron injection that may be responsible for the modulation of electric conductivity. Finding a unique case of filamentary‐type resistive switching involving redox reactions of stationary molecules within a molecular solid is postulated. Yet, the formation of these filaments is not related to any significant configurational changes at the atomic scale.https://doi.org/10.1002/aelm.202300818annulene complexesmemristorneuromorphic computingresistive switchingsynaptic plasticityXAS spectroscopy
spellingShingle Andrzej Sławek
Lulu Alluhaibi
Ewelina Kowalewska
Gisya Abdi
Tomasz Mazur
Agnieszka Podborska
Krzysztof Mech
Marianna Marciszko‐Wiąckowska
Alexey Maximenko
Konrad Szaciłowski
Memristors Based on Ni(II)‐tetraaza[14]annulene Complexes: Toward an Unconventional Resistive Switching Mechanism
Advanced Electronic Materials
annulene complexes
memristor
neuromorphic computing
resistive switching
synaptic plasticity
XAS spectroscopy
title Memristors Based on Ni(II)‐tetraaza[14]annulene Complexes: Toward an Unconventional Resistive Switching Mechanism
title_full Memristors Based on Ni(II)‐tetraaza[14]annulene Complexes: Toward an Unconventional Resistive Switching Mechanism
title_fullStr Memristors Based on Ni(II)‐tetraaza[14]annulene Complexes: Toward an Unconventional Resistive Switching Mechanism
title_full_unstemmed Memristors Based on Ni(II)‐tetraaza[14]annulene Complexes: Toward an Unconventional Resistive Switching Mechanism
title_short Memristors Based on Ni(II)‐tetraaza[14]annulene Complexes: Toward an Unconventional Resistive Switching Mechanism
title_sort memristors based on ni ii tetraaza 14 annulene complexes toward an unconventional resistive switching mechanism
topic annulene complexes
memristor
neuromorphic computing
resistive switching
synaptic plasticity
XAS spectroscopy
url https://doi.org/10.1002/aelm.202300818
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