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A Novel, Diode-Based Organic Memory Device Technische Universität Dresden pinMOS Memory: A novel, diode-based organic memory device Yichu Zheng, M. E. der Fakultät Elektrotechnik und Informationstechnik der Technischen Universität Dresden zur Erlangung des akademischen Grades Doktoringenieur (Dr.-Ing.) genehmigte Dissertation Vorsitzender: Prof. Dr.-Ing. Prof. Hubert Lakner Tag der Einreichung: 24.10.2019 Gutachter: Prof. Dr. rer. nat. Stefan Mannsfeld Tag der Verteidigung: 07.08.2020 Gutachter: Prof. Dr. Koen Vandewal ii Abstract A novel, non-volatile, organic capacitive memory device called p-i-n-metal-oxide-semiconductor (pinMOS) memory is demonstrated with multiple-bit storage that can be programmed and read out electrically and optically. The diode-based architecture simplifies the fabrication process, and makes further optimizations easy, and might even inspire new derived capacitive memory devices. Furthermore, this innovative pinMOS memory device features local charge up of an integrated capacitance rather than of an extra floating gate. Before the device can perform as desired, the leakage current due to the lateral charge up of the doped layers outside the active area needs to be suppressed. Therefore, in this thesis, lateral charging effects in organic light-emitting diodes (OLEDs) are studied first. By comparing the results from differently structured devices, the presence of centimeter-scale lateral current flows in the n-doped and p-doped layers is shown, which results in undesirable capacitance increases and thus extra leakage currents. Such lateral charging can be controlled via structuring the doped layers, leading to extremely low steady-state leakage currents in the OLED (here 10-7 mA/cm2 at -1 V). It is shown that these lateral currents can be utilized to extract the conductivity as well as the activation energy of each doped layer when modeled with an RC circuit model. Secondly, pinMOS memory devices that are based on the diode with structured doped layers are investigated. The memory behavior, which is demonstrated as capacitance switching for electrical signals, and light emission for optical signals, can be tuned either by the applied voltage or ultraviolet light illumination, respectively. The working mechanism is explained by the existence of quasi steady-states as well as the width variation of space charge zones. The pinMOS memory shows excellent repeatability, an endurance of more than 104 write-read-erase-read cycles, and currently already over 24 h retention time. Furthermore, an early-stage investigation on emulating synaptic plasticity reveals the potential of pinMOS memory for applications in neuromorphic computing. Overall, the results indicate that pinMOS memory in principle is promising for a variety of future applications in both electronic and photonic circuits. A detailed understanding of this new concept of memory device, for which this thesis lays an important foundation, is necessary to proceed with further enhancements. iv Zusammenfassung Es wird ein neuartiges, organisches kapazitives Speicherelement demonstriert, das p-i-n-Metalloxid- Halbleiter (pinMOS) Speicher genannt wird und eine Mehrfachbitspeicherung besitzt, die elektrisch und optisch programmiert und ausgelesen werden kann. Die auf einer Diode basierende Architektur vereinfacht den Herstellungsprozess sowie die weitere Optimierung und könnte sogar Inspiration für neue kapazitive Speichermedien sein. Darüber hinaus basiert dieses innovative pinMOS Speicherelement auf der lokalen Aufladung einer integrierten Kapazität und nicht auf einem zusätzlichem “Floating Gate”. Bevor das Speicherelement wie gewünscht funktioniert, muss der Leckstrom, der durch die laterale Aufladung der dotierten Schichten außerhalb des aktiven Bereichs verursacht wird, unterdrückt werden. Deshalb werden in dieser Arbeit zuerst die lateralen Aufladungseffekte in organischen Leuchtdioden (OLEDs) untersucht. Beim Vergleich verschiedener Device-Strukturen wird die Existenz von lateralen Stromflüssen im Zentimeterbereich in den n- und p-dotierten Schichten gezeigt, was zu einer unerwünschten erhöhten Kapazität und folglich einem höheren Leckstrom führt. Diese laterale Aufladung kann durch die Strukturierung der dotierten Schichten kontrolliert werden, was zu extrem geringen Gleichgewichtsleckströmen in den OLEDs (10-7 mA/cm2 bei -1 V) resultiert. Es wird auch gezeigt, dass die lateralen Ströme genutzt werden können um die spezifische Leitfähigkeit sowie die Aktivierungsenergie der einzelnen dotierten Schichten zu extrahieren, wenn diese mit einem RC-Modell modelliert werden. Im zweiten Teil werden pinMOS Speicherelemente, die auf der Diode mit strukturierten dotierten Schichten basieren, untersucht. Das Speicherverhalten, dass durch Kapazitätsschaltung für elektrische Signale und als Lichtemission für optische Signale gezeigt wird, kann entweder durch die angelegte Spannung, beziehungsweise durch die Belichtung mit ultraviolettem Licht eingestellt werden. Die Wirkungsweise wird durch die Existenz quasistatischer Gleichgewichte sowie durch die Größenänderung der Raumladungszonen erklärt. Der pinMOS Speicher zeigt eine hervorragende Wiederholbarkeit, eine Beständigkeit über mehr als 104 Schreiben-Lesen-Löschen-Lesen Zyklen und aktuell schon eine Retentionszeit von über 24 h. Weiterhin offenbaren erste Versuche in der Nachahmung von Neuronaler Plastizität das Potenzial von pinMOS Speichern für Anwendungen im “Neuromorphic Computing”. Insgesamt deuten die Ergebnisse an, dass pinMOS Speicher prinzipiell vielversprechend für eine Vielzahl von zukünftigen Anwendungen in elektronischen und photonischen Schaltkreisen ist. Ein tiefgreifendes Verständnis von diesem Konzept neuartiger Speicherelemente, für das diese Arbeit eine wichtige Grundlage bildet, ist notwendig, um weitere Verbesserungen zu entwickeln. vi Contents 1 Introduction .........................................................................................................................1 2 Fundamentals of organic semiconductors .........................................................................5 2.1 Electronic states of a molecule .......................................................................................5 2.1.1 Atomic orbitals and molecular orbitals ................................................................5 2.1.2 Solid states ............................................................................................................9 2.1.3 Singlet and triplet states......................................................................................12 2.2 Charge transport ...........................................................................................................13 2.2.1 Charge carrier mobility.......................................................................................13 2.2.2 Charge carrier transport ......................................................................................14 2.3 Charge injection ...........................................................................................................17 2.3.1 Current limitation ...............................................................................................17 2.3.2 Charge injection mechanisms .............................................................................20 2.4 Doping ..........................................................................................................................22 3 Organic junctions and devices ..........................................................................................25 3.1 Metal-semiconductor junction ......................................................................................25 3.1.1 Schottky junction ................................................................................................25 3.1.2 Surface states ......................................................................................................27 3.2 Metal-oxide-semiconductor capacitor ..........................................................................29 3.3 Junctions and diodes .....................................................................................................31 3.3.1 PN junction and diode ........................................................................................31 3.3.2 PIN junction and diode .......................................................................................32 4 Organic non-volatile memory devices .............................................................................35 4.1 Basic concepts ..............................................................................................................35 4.2 Organic resistive memory devices................................................................................37 4.2.1 Device architecture and switching behavior .......................................................38 4.2.2 Working mechanisms .........................................................................................38 4.3 Organic transistor-based memory devices ....................................................................41 4.3.1 Organic field-effect transistor and memory devices based thereon ....................41 4.3.2 Floating gate memory .........................................................................................43 4.3.3 Charge trapping memory ....................................................................................45 viii 4.4 Organic ferroelectric memory devices .........................................................................46
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