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Formation of KNbO3 Thin Films for Self-Powered ReRAM Devices and Artificial Synapses PDF

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Springer Theses Recognizing Outstanding Ph.D. Research Tae-Ho Lee Formation of KNbO 3 Thin Films for Self-Powered ReRAM Devices and Artificial Synapses Springer Theses Recognizing Outstanding Ph.D. Research Aims and Scope The series “Springer Theses” brings together a selection of the very best Ph.D. theses from around the world and across the physical sciences. Nominated and endorsed by two recognized specialists, each published volume has been selected foritsscientificexcellenceandthehighimpactofitscontentsforthepertinentfield of research. For greater accessibility to non-specialists, the published versions includeanextendedintroduction,aswellasaforewordbythestudent’ssupervisor explainingthespecialrelevanceoftheworkforthefield.Asawhole,theserieswill provide a valuable resource both for newcomers to the research fields described, and for other scientists seeking detailed background information on special questions. Finally, it provides an accredited documentation of the valuable contributions made by today’s younger generation of scientists. Theses are accepted into the series by invited nomination only and must fulfill all of the following criteria (cid:129) They must be written in good English. (cid:129) ThetopicshouldfallwithintheconfinesofChemistry,Physics,EarthSciences, Engineeringandrelatedinterdisciplinary fields such asMaterials,Nanoscience, Chemical Engineering, Complex Systems and Biophysics. (cid:129) The work reported in the thesis must represent a significant scientific advance. (cid:129) Ifthethesisincludespreviouslypublishedmaterial,permissiontoreproducethis must be gained from the respective copyright holder. (cid:129) They must have been examined and passed during the 12 months prior to nomination. (cid:129) Each thesis should include a foreword by the supervisor outlining the signifi- cance of its content. (cid:129) The theses should have a clearly defined structure including an introduction accessible to scientists not expert in that particular field. More information about this series at http://www.springer.com/series/8790 Tae-Ho Lee Formation of KNbO Thin 3 Films for Self-Powered ReRAM Devices fi and Arti cial Synapses Doctoral Thesis accepted by Korea University, Seoul, Korea (Republic of) 123 Author Supervisor Dr. Tae-HoLee Prof. SahnNahm Korea Electronics Technology Institute Department ofMaterials Science Seongnam,Korea (Republicof) andEngineering Korea University Seoul, Korea (Republicof) ISSN 2190-5053 ISSN 2190-5061 (electronic) SpringerTheses ISBN978-981-13-2534-2 ISBN978-981-13-2535-9 (eBook) https://doi.org/10.1007/978-981-13-2535-9 LibraryofCongressControlNumber:2018954028 ©SpringerNatureSingaporePteLtd.2018 Thisworkissubjecttocopyright.AllrightsarereservedbythePublisher,whetherthewholeorpart of the material is concerned, specifically the rights of translation, reprinting, reuse of illustrations, recitation, broadcasting, reproduction on microfilms or in any other physical way, and transmission orinformationstorageandretrieval,electronicadaptation,computersoftware,orbysimilarordissimilar methodologynowknownorhereafterdeveloped. The use of general descriptive names, registered names, trademarks, service marks, etc. in this publicationdoesnotimply,evenintheabsenceofaspecificstatement,thatsuchnamesareexemptfrom therelevantprotectivelawsandregulationsandthereforefreeforgeneraluse. The publisher, the authors, and the editorsare safeto assume that the adviceand informationin this book are believed to be true and accurate at the date of publication. Neither the publisher nor the authorsortheeditorsgiveawarranty,expressorimplied,withrespecttothematerialcontainedhereinor for any errors or omissions that may have been made. The publisher remains neutral with regard to jurisdictionalclaimsinpublishedmapsandinstitutionalaffiliations. ThisSpringerimprintispublishedbytheregisteredcompanySpringerNatureSingaporePteLtd. Theregisteredcompanyaddressis:152BeachRoad,#21-01/04GatewayEast,Singapore189721, Singapore ’ Supervisor s Foreword KNbO (KN) thin films have shown excellent electro-optic properties, high non- 3 linear optical coefficients, and good photorefractive and piezoelectric properties. Therefore, KN films have been extensively investigated for application to the variousnonlinearopticalandelectro-opticaldevices.However,ithasbeendifficult togrowstoichiometricKNthinfilmsbecauseK Oevaporatedduringthegrowth.In 2 ordertoovercomethisproblem,theK Oexcesstargetanddualtargetsconsistingof 2 KNandK CO havebeenused.However,since thecomposition ofthetargetwas 2 3 differentfromthatofthefilm,itwasdifficulttocontrolthecompositionoftheKN thin film. Dr. Tae-Ho Kim showed in his thesis how to grow the homogeneous crystalline KN film without secondary phase and then he also investigated the growthoftheamorphousKNthinfilmcontainingKNnanocrystals.Moreover,the applicationsoftheKNfilmsuchasapiezoelectricnanogenerator,resistiverandom accessmemory(ReRAM)device,andtheartificialsynapsewereinvestigatedinhis thesis. First, he has investigated the growth behavior of the KN film. He found that a K Nb O secondaryphase wasformed intheKNfilmwhenthedepositionand 2.88 5 15 the annealing temperatures were greater than room temperature (RT) and 800 °C, respectively, owing to the evaporation of K O. On the other hand, KNb O and 2 3 8 K Nb O secondary phases were formed in the KN films when the annealing 3 5.45 15 temperature was less than 800 °C. Based on these results, he showed that the stoichiometricKNfilmswereobtainedwhentheamorphousKNfilmgrownatRT wasannealedunderK Oatmosphereat800°CtocompensatetheevaporatedK O. 2 2 This KN film showed the promising electrical, dielectric, and piezoelectric properties. He has investigated on the amorphous KN films containing KN nanocrystals in the second part of his thesis. Piezoelectric nanogenerators (PNG) were also fabri- cated using this KN films grown on the TiN/Polyimide/PET substrates and PNG fabricated with the KN film showed an open-circuit output voltage of 2.5 V and a short-circuit current of 70 nA. Moreover, he found that this KN film exhibited a bipolarresistiveswitchingbehaviorwithgoodreliabilitycharacteristicsthatcanbe v vi Supervisor’sForeword explained by the formation and rupture of the oxygen vacancy filaments. He also showed that the KN resistive random access memory device, which was powered by the KN PNG, showed promising resistive switching behavior. Finally, he investigated the synaptic properties of the KN thin film for the application to the neuromorphic computing system. He proved that the Pt/KN/TiN memristor exhibited reliable bipolar switching behavior with multiple resistance levels, confirming that the KN film can be used as the artificial synapse and transmission properties of a biological synapse with a good conductance modula- tion linearity. Moreover, he showed that the KN memristor can emulate various biological synaptic plasticity characteristics including short-term plasticity, long-term plasticity, spike-rate dependent plasticity, paired-pulse facilitation, and post-tetanic potentiation by controlling the number and rate of the potentiation spike.Inhisthesis,healsoshowedthatspike-timing-dependentplasticity,whichis an essential property of biological synapses, is realized in KN memristor. The synaptic plasticity of the KN memristor can be explained by oxygen vacancy movement and oxygen vacancy filaments. Moreover, he proved that the meta- plasticity of biological synapses was also implemented in the KN memristor, including metaplasticities of long-term potentiation and depression, and of STDP.Therefore,heclearlyprovedinhisthesisthattheKNmemristorcanbeused as an artificial synapse in neuromorphic computing systems. Histhesis showsthathow togrow theKN-basedthinfilm andtheseresultscan be used for the fabrication of the various electrical devices. Moreover, his thesis alsoprovesthattheKNfilmcanbeusedasthepiezoelectricnanogeneratorforthe biological device as well as the artificial synapse for the neuromorphic computing systems. Seoul, Korea (Republic of) Prof. Sahn Nahm April 2018 Abstract Biomedical devices inserted into the human body and microelectronicapplications require miniaturization and reliable safe battery to operate. In particular, self- poweredbiomedicalapplicationsworkbythepiezoelectricnanogenerators(PNGs), which present numerous advantage, including high voltage, efficiency, low cost, high versatility, simplicity in structural design and fabrication, stability and robustness, and environmental friendliness. To improve the performance of these self-powered biomedical devices, the development of energy efficient memory device is important. In this study, ReRAM based memristors as artificial synapses are proved for high efficient memory devices and combined with a piezoelectric nanogenerators (PNGs) for self-powered biomedical devices that can be used in neuromorphic systems. First, Self-powered Resistive Random Access Memory (ReRAM) devices and ArtificialSynapsesforneuromorphicdeviceswereinvestigated.AmorphousKNbO 3 (KN)filmcontainingKNnanocrystalswithasizeofapproximately5.0nmwasgrown onTiN/SiO /Sisubstrateat350°C.ThisKNfilmshowedadielectricconstant(e)and 2 r piezoelectricstrainconstant(d )of43and80pm/Vat10V,respectively,owingto 33 theexistenceofKNnanocrystals.PiezoelectricNanogenerators(PNGs)werefabri- catedusingKNfilmsgrownontheTiN/Polyimide/PETsubstrates.PNGfabricated withtheKNfilmgrownat350°Cshowedanopen-circuitoutputvoltageof2.5Vand a short-circuit current of 70 nA. The KN film grown at 350 °C exhibited a bipolar resistiveswitchingbehaviorwithgoodreliabilitycharacteristicsthatcanbeexplained bytheformationandruptureoftheoxygenvacancyfilaments.TheResistiveRandom AccessMemory(ReRAM)devicepoweredbytheKNPNGalsoshowedpromising resistiveswitchingbehaviorwithON/OFFratioof10.Moreover,theKNfilmshows goodbiocompatibility. vii viii Abstract Taking astepforwardaparticularlygoodefficient memory device,theKNfilm grown at 350 °C was used to synthesize the KN ReRAM based memristor for an artificial synapse. The sensitivity of memristor synapse devices changed when repetitive signals are applied, and this property can perform the self-learning abilities to neuromorphic devices similar to neural network system. This charac- teristic is expressed as the biological synapse including short-term/long-term plasticity (STP/LTP), spike-rate-dependent plasticity (SRDP), spike-timing- dependent plasticity (STDP), and synaptic plasticity. Synaptic characteristics of KN memristor are controlled by voltage intensity and time tuning of pulsed signal basedonresistanceswitching.ThesynapticpropertiesoftheKNmemristorcanbe explained based on the oxygen vacancy movements and the shape change of oxygenvacancyfilaments.MetaplasticityofLTPwasprovedintheKNmemristor to achieve bio-realistic synaptic functions. Moreover, the metaplasticity of STDP wasalsoshownintheKNmemristorwithaprimingstimulus.Alloftheresults,in this thesis, evidently indicated the probability of ReRAM device not only in the memory application but also in the neuromorphic system application. Parts of this thesis have been published in the following articles: 1. B. Y. Kim, H. G. Hwang, J. U. Woo, W. H. Lee, T. H. Lee, C. Y. Kang and S. Nahm, “Nanogenerator-induced synaptic plasticity and metaplasticity of bio-realistic artificial synapses” NPG Asia Mater. E381, 1–9 (2017). 2. T. H. Lee, D. H. Kim, B. Y. Kim, H. Y. Choi, J. H. Oh, C. Y. Kang and S. Nahm, “Structural and electrical properties of KNbO thin film grown on a 3 Pt/Ti/SiO /SisubstrateusingtheRFmagnetronsputteringmethod”ActaMater. 2 112, 53–58 (2016). 3. T.H.Lee,H.G.Hwang,S.Jang,G.Wang,S.Han,D.H.Kim,C.Y.Kangand S.Nahm,“Low-Temperature-GrownKNbO ThinFilmsandTheirApplication 3 to Piezoelectric Nanogenerators and Self-Powered ReRAM device” ACS Appl. Mater. Interfaces 9, 43220–43229 (2017). 4. T. H. Lee, H. G. Hwang, J. U. Woo, D. H. Kim, T. W. Kim and S. Nahm, “Synaptic Plasticity and Metaplasticity of Biological Synapse Realized in a KNbO Memristor for Application to Artificial Synapse” ACS Appl. Mater. 3 Interfaces. https://doi.org/10.1021/acsami.8b04550 (2018). ix

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