Camille Jubert Tomasso, Thomas Petenzi, Anna Tidu, Rassen Boukraa, Sofia Russi, Giorgio Mattana, Christelle Gautier, Tony Breton, Ivan T. Lucas, Hubert Perrot, Laure Fillaud
{"title":"Elucidation of Switching Mechanisms in Memristive Junctions Integrating a Iron(II)-Ter Pyridine Diazoted Complex","authors":"Camille Jubert Tomasso, Thomas Petenzi, Anna Tidu, Rassen Boukraa, Sofia Russi, Giorgio Mattana, Christelle Gautier, Tony Breton, Ivan T. Lucas, Hubert Perrot, Laure Fillaud","doi":"10.1002/aelm.202400350","DOIUrl":"https://doi.org/10.1002/aelm.202400350","url":null,"abstract":"An original way of elaborating vertical metal/molecules/metal memristive junctions through diazonium electrografting of the organic layer and inkjet-printed top electrodes is reported here. The molecule of interest is a Fe<sup>II</sup> coordination complex with ter-pyridine ligands, having a diazonium anchoring group. The resulting junction exhibits a memristive behavior characterized by a high ON/OFF ratio and plasticity property. Through the application of advanced techniques such as UV–vis and Raman time-resolved spectroelectrochemistry, the study demonstrates the significant role of switchable azo bonds derived from diazo electrografting in memristive behavior.","PeriodicalId":110,"journal":{"name":"Advanced Electronic Materials","volume":"1 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588322","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Joshua J. Maraj, Emily A. Schafer, Michelle M. Mansour, Essraa A. Hussein, Joseph Berryman, Elizabeth Klavon, Jonathan Rivnay, Stephen A. Sarles
{"title":"Highly Resistive Biomembranes Coupled to Organic Transistors enable Ion-Channel Mediated Neuromorphic Synapses","authors":"Joshua J. Maraj, Emily A. Schafer, Michelle M. Mansour, Essraa A. Hussein, Joseph Berryman, Elizabeth Klavon, Jonathan Rivnay, Stephen A. Sarles","doi":"10.1002/aelm.202400526","DOIUrl":"https://doi.org/10.1002/aelm.202400526","url":null,"abstract":"Organic electrochemical transistors (OECTs) functionalized with lipid membranes could enable new hybrid synapses for sensing and neuromorphic computing in biological media. However, prior attempts to pair these components resulted in low quality membranes formed on the OECT surface. We present a new method for forming a highly-resistive phospholipid bilayer coupled to a poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) OECT that avoids the disruptive effects of the rough polymer surface. Transistor coupled droplet bilayers (TCDBs) formed from diphytanoyl phosphatidylcholine lipids exhibit an average specific resistance that is 1000X higher than values reported for solid-supported lipid membranes assembled on PEDOT:PSS. High membrane resistance and the addition of voltage-activated ionophores enable us to demonstrate that selective ion transport and spontaneous membrane resealing in response to dynamic gate voltage imparts selective programming and memory-storage capability to an OECT without chemical modification of the PEDOT:PSS. These capabilities enable paired-pulse facilitation and depression with writing speeds and memory retentions that are both >10X higher than previously reported with membrane-coated OECTs. The high resistance of the TCDB establishes a basis for hybrid biomolecular synapses that can integrate stimuli-responsive membranes and organic electronics for future applications in sensing, signal processing, and neuromorphic computing at the <i>edge of biology</i>.","PeriodicalId":110,"journal":{"name":"Advanced Electronic Materials","volume":"127 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142580573","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Tunable Rectification in 2D Porphyrinic Metal–Organic Framework Nanosheets Molecular Heterojunctions","authors":"Bing Huang, Xiaoyu Wang, Chaoguang He, Yongkang Zhang, Pan Qi, Ying Wang, Tong Li, Huixia Fu, Hui Wei, Cunlan Guo","doi":"10.1002/aelm.202400773","DOIUrl":"https://doi.org/10.1002/aelm.202400773","url":null,"abstract":"As functional electrical devices advance, new strategies for regulating electrical properties are essential for achieving diverse electrical performance. In this study, molecular heterojunction rectifiers are constructed by connecting porphyrinic 2D metal–organic framework (2D MOF) nanosheets and oligophenylene thiols self-assembled monolayers (OPT SAMs) within metal electrodes. The rectification characteristics can be tuned by the molecular length of OPT and the coordinated metal atom in the center of 2D MOFs. Specifically, a rectification ratio of more than 1.67 orders of magnitude is achieved in the heterojunction composed of 2D Zn-TCPP MOF nanosheet (TCCP, tetrakis(4-carboxyphenyl) porphyrin) and OPT3 SAM. Combining Kelvin probe force microscopy measurements and first-principles calculations of the 2D MOF nanosheets, it elucidates that the rectification variations come from the adjustment of energy level alignment at OPT SAMs//2D MOF interface, leading to asymmetric charge transport with the voltage polarities. This strategy can be further extended to Cu-MOF nanosheets, which also exhibit rectification behaviors when placed on OPT2 SAMs. This work provides a universal and flexible strategy for regulating the electrical behaviors of MOFs without the need for specific design and synthesis, paving the way for the development of MOF-based functional electronic devices.","PeriodicalId":110,"journal":{"name":"Advanced Electronic Materials","volume":"191 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142580697","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Long-Channel Effects in Randomly Oriented Carbon Nanotube Thin Film Transistors","authors":"Hai-Yang Liu, Panpan Zhang, Xianmao Cao, Yang Zhang, Jianping He, Maguang Zhu, Mengmeng Xiao, Zhiyong Zhang","doi":"10.1002/aelm.202400660","DOIUrl":"https://doi.org/10.1002/aelm.202400660","url":null,"abstract":"Carbon nanotube (CNT) thin film transistors (TFTs) have demonstrated great potential for application in highly sensitive biosensors and large-area electronics. However, research on the electrical behavior of long-channel CNT TFTs is lacking; thus, the purposeful improvement in the performance of biosensors or circuits is difficult. In this study, the electrical transport characteristics of ionic-liquid-gate CNT TFTs with channel lengths (<i>L</i><sub>ch</sub>) ranging from 10 to 400 µm are investigated. The CNT TFTs present classical drift-diffusion transport at on-state with a carrier mobility of around 27 cm<sup>2</sup> V<sup>−1</sup> s<sup>−1</sup>. In the subthreshold region of the CNT TFTs, an abnormal <i>L</i><sub>ch</sub>-dependent subthreshold swing (SS) relationship, named as the long-channel effect (LCE)is observed, where SS worsens with increasing <i>L</i><sub>ch</sub>. The existence of the junctions between the CNTs results in an unconventional density of states for carriers and a large series resistance for sharing the gate voltage; this dominates the abnormal scaling behavior in the subthreshold region by degrading the electrostatic integrity. The discovery of the abnormal LCE can aid in the construction of device models and purposefully improve the performance of CNT TFTs for biosensors and other large-scale electronic applications.","PeriodicalId":110,"journal":{"name":"Advanced Electronic Materials","volume":"18 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588323","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Steven M. Baksa, Simon Gelin, Seda Oturak, R. Jackson Spurling, Alireza Sepehrinezhad, Leonard Jacques, Susan E. Trolier-McKinstry, Adri C. T. van Duin, Jon-Paul Maria, Andrew M. Rappe, Ismaila Dabo
{"title":"Strain Fluctuations Unlock Ferroelectricity in Wurtzites","authors":"Steven M. Baksa, Simon Gelin, Seda Oturak, R. Jackson Spurling, Alireza Sepehrinezhad, Leonard Jacques, Susan E. Trolier-McKinstry, Adri C. T. van Duin, Jon-Paul Maria, Andrew M. Rappe, Ismaila Dabo","doi":"10.1002/aelm.202400567","DOIUrl":"https://doi.org/10.1002/aelm.202400567","url":null,"abstract":"Ferroelectrics are of practical interest for non-volatile data storage due to their reorientable, crystallographically defined polarization. Yet efforts to integrate conventional ferroelectrics into ultrathin memories have been frustrated by film-thickness limitations, which impede polarization reversal under low applied voltage. Wurtzite materials, including magnesium-substituted zinc oxide (Zn,Mg)O, have been shown to exhibit scalable ferroelectricity as thin films. In this work, the origins of ferroelectricity in (Zn,Mg)O are explained, showing that large strain fluctuations emerge locally in (Zn,Mg)O and can reduce local barriers to ferroelectric switching by more than 40%. Concurrent experimental and computational evidence of these effects are provided by demonstrating polarization switching in ZnO/(Zn,Mg)O/ZnO heterostructures featuring built-in interfacial strain gradients. These results open up an avenue to develop scalable ferroelectrics by controlling strain fluctuations atomistically.","PeriodicalId":110,"journal":{"name":"Advanced Electronic Materials","volume":"137 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142574573","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Effects of Charge Imbalance on Field-Induced Instability of HfO2-Based Ferroelectric Tunnel Junctions","authors":"Wonjun Shin, Chang-Hyeon Han, Jangsaeng Kim, Ryun-Han Koo, Kyung Kyu Min, Daewoong Kwon","doi":"10.1002/aelm.202400299","DOIUrl":"https://doi.org/10.1002/aelm.202400299","url":null,"abstract":"Ferroelectricity in hafnium-based materials has attracted significant research attention and is used in various applications owing to their complementary metal-oxide-semiconductor compatibility, scalability, and low-power operation. However, their widespread integration into various technologies is hindered by reliability and stability problems, particularly field-induced instability, which causes fluctuations in polarization characteristics during operation. Herein, on the underlying mechanism of field-induced instability is reported in pure hafnium oxide films within metal-ferroelectric-insulator-semiconductor (MFIS) ferroelectric tunnel junctions (FTJs). The comprehensive material analysis combined with low-frequency noise (LFN) measurements reveals that the presence of oxygen vacancies and interface traps within the ferroelectric and dielectric layers induces a charge imbalance in the FTJ, leading to distortion in its polarization characteristics and the onset of cyclic evolution in field-induced instability. Furthermore, high-pressure annealing effectively mitigates field-induced instability by reducing the defects within the film, thereby alleviating the associated charge imbalance. These findings contribute to a deeper understanding of the internal dynamics of FTJs and provide an efficient approach to enhancing their stability.","PeriodicalId":110,"journal":{"name":"Advanced Electronic Materials","volume":"17 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142574574","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Machine Learning Enabled High-Throughput Screening of 2D Ultrawide Bandgap Semiconductors for Flexible Resistive Materials","authors":"Chi Chen, Hao Wang, Houzhao Wan, Dan Sun","doi":"10.1002/aelm.202400435","DOIUrl":"https://doi.org/10.1002/aelm.202400435","url":null,"abstract":"The 2D ultrawide bandgap (UWBG) semiconductors have attracted great attentions for the next generation of electronics and optoelectronics, owing to their superiority on material flexibility, device stability, and power consumption. However, few 2D UWBG semiconductors have been discovered, impeding their prosperous developments and widespread applications. Here, a high-throughput workflow is constructed to screen 2D UWBG semiconductors assisted by machine learning, and 507 potential candidates are obtained. Moreover, by learning, predicting, and screening Young's modulus and Poisson's ratio, 31 flexible 2D UWBG semiconductors are identified. Then the generation and the diffusion of anion vacancies, as well as the corresponding electronic properties are investigated by using the first-principles calculations, and 3 of them are demonstrated as the most promising candidates for the flexible resistive materials. The facile interface tunneling and the increased material conductance caused by the anion vacancies will contribute to the transition from high resistive state to low resistive state. This work provides an efficient high-throughput screening protocol to enrich the family of 2D UWBG semiconductors and is expected to foster their practical applications.","PeriodicalId":110,"journal":{"name":"Advanced Electronic Materials","volume":"17 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142574578","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Philipp Hein, Tobias Romstadt, Fabian Draber, Jinseok Ryu, Thorben Böger, Andreas Falkenstein, Miyoung Kim, Manfred Martin
{"title":"Variable-Range Hopping Conduction in Amorphous, Non-Stoichiometric Gallium Oxide","authors":"Philipp Hein, Tobias Romstadt, Fabian Draber, Jinseok Ryu, Thorben Böger, Andreas Falkenstein, Miyoung Kim, Manfred Martin","doi":"10.1002/aelm.202400407","DOIUrl":"https://doi.org/10.1002/aelm.202400407","url":null,"abstract":"Amorphous, non-stoichiometric gallium oxide (a-GaO<sub><i>x</i></sub>, <i>x</i> < 1.5) is a promising material for many electronic devices, such as resistive switching memories, neuromorphic circuits and photodetectors. So far, all respective measurements are interpreted with the explicit or implicit assumption of n-type band transport above the conduction band mobility edge. In this study, the experimental and theoretical results consistently show for the first time that for an O/Ga ratio <i>x</i> of 0.8 to 1.0 the dominating electron transport mechanism is, however, variable-range hopping (VRH) between localized states, even at room temperature and above. The measured conductivity exhibits the characteristic exponential temperature dependence on <i>T</i><sup>−1/4</sup>, in remarkable agreement with Mott's iconic law for VRH. Localized states near the Fermi level are confirmed by photoelectron spectroscopy and density of states (DOS) calculations. The experimental conductivity data is reproduced quantitatively by kinetic Monte Carlo (KMC) simulations of the VRH mechanism, based on the ab-initio DOS. High electric field strengths <i>F</i> cause elevated electron temperatures and an exponential increase of the conductivity with <i>F</i><sup>1/2</sup>. Novel results concerning surface oxidation, magnetoresistance, Hall effect, thermopower and electron diffusion are also reported. The findings lead to a new understanding of a-GaO<sub><i>x</i></sub> devices, also with regard to metal|a-GaO<sub><i>x</i></sub> Schottky barriers.","PeriodicalId":110,"journal":{"name":"Advanced Electronic Materials","volume":"87 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142574283","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Fabian Gärisch, Vincent Schröder, Emil J. W. List-Kratochvil, Giovanni Ligorio
{"title":"Scalable Fabrication of Neuromorphic Devices Using Inkjet Printing for the Deposition of Organic Mixed Ionic-Electronic Conductor","authors":"Fabian Gärisch, Vincent Schröder, Emil J. W. List-Kratochvil, Giovanni Ligorio","doi":"10.1002/aelm.202400479","DOIUrl":"https://doi.org/10.1002/aelm.202400479","url":null,"abstract":"Recent advancements in artificial intelligence (AI) have highlighted the critical need for energy-efficient hardware solutions, especially in edge-computing applications. However, traditional AI approaches are plagued by significant power consumption. In response, researchers have turned to biomimetic strategies, drawing inspiration from the ion-mediated operating principle of biological synapses, to develop organic neuromorphic devices as promising alternatives. Organic mixed ionic-electronic conductor (OMIEC) materials have emerged as particularly noteworthy in this field, due to their potential for enhancing neuromorphic computing capabilities. Together with device performance, it is crucial to select devices that allow fabrication via scalable techniques. This study investigates the fabrication of OMIEC-based neuromorphic devices using inkjet printing, providing a scalable and material-efficient approach. Employing a commercially available polymer mixed ionic-electronic conductor (BTEM-PPV) and a lithium salt, inkjet-printed devices exhibit performance comparable to those fabricated via traditional spin-coating methods. These two-terminal neuromorphic devices demonstrate functionality analogous to literature-known devices and demonstrate promising frequency-dependent short-term plasticity. Furthermore, comparative studies with previous light-emitting electrochemical cells (LECs) and neuromorphic OMIEC devices validate the efficacy of inkjet printing as a potential fabrication technique. The findings suggest that inkjet printing is suitable for large-scale production, offering reproducible and stable fabrication processes. By adopting the OMIEC material system, inkjet printing holds the potential for further enhancing device performance and functionality. Overall, this study underscores the viability of inkjet printing as a scalable fabrication method for OMIEC-based neuromorphic devices, paving the way for advancements in AI hardware.","PeriodicalId":110,"journal":{"name":"Advanced Electronic Materials","volume":"109 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142574575","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hanna Świątek, Sylwia Gutowska, Michał J. Winiarski, Bartlomiej Wiendlocha, Tomasz Klimczuk
{"title":"Superconductivity in Ternary Mg4Pd7As6","authors":"Hanna Świątek, Sylwia Gutowska, Michał J. Winiarski, Bartlomiej Wiendlocha, Tomasz Klimczuk","doi":"10.1002/aelm.202400284","DOIUrl":"https://doi.org/10.1002/aelm.202400284","url":null,"abstract":"The synthesis and characterization of a new compound Mg<sub>4</sub>Pd<sub>7</sub>As<sub>6</sub>, which is found to be a superconductor with <i>T</i><sub><i>c</i></sub> = 5.45 K is reported. Powder X-ray diffraction confirms the U<sub>4</sub>Re<sub>7</sub>Si<sub>6</sub> structure (space group <i>Im</i>-3<i>m</i>, no. 229) with the lattice parameter <i>a</i> = 8.2572(1) Å. Magnetization, specific heat, and electrical resistivity measurements indicate that it is a moderate-coupling (λ = 0.72) type-II superconductor. The electronic and phonon structures are calculated, highlighting the importance of antibonding Pd–As interactions in determining the properties of this material. The calculated electron–phonon coupling parameter λ = 0.76 agrees very well with the experimental finding, which confirms the conventional pairing mechanism in Mg<sub>4</sub>Pd<sub>7</sub>As<sub>6</sub>.","PeriodicalId":110,"journal":{"name":"Advanced Electronic Materials","volume":"20 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142574577","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}