Frericks, Markus (2022)
Organic Hole Transport Materials: Properties and Interface Formation.
Technische Universität Darmstadt
doi: 10.26083/tuprints-00022397
Dissertation, Erstveröffentlichung, Verlagsversion
Kurzbeschreibung (Abstract)
This dissertation is related to organic semiconductor (OSC) materials for organic light emitting diode (OLED) applications investigated together with our project partner Merck KGaA. One often stated advantage of OSCs is the chemical flexibility to easily synthesize new molecules. A deeper understanding of the connection between molecular structure and device characteristics could lead to faster material screening and development. As contribution to this goal, the here presented work analyzes and discusses the properties of hole transport materials (HTMs) and especially their electronic interface properties. Indium tin oxide (ITO) substrates, a commercially available p-dopant, CPTCFA, a literature-known HTM, m-MTDATA, a commercial HTM from Merck KGaA, HTM-B, and aluminum are characterized as thin films by photoelectron spectroscopy (PES) to obtain the materials’ electronic properties. Ultraviolet, visible, near- and mid-infrared absorption spectroscopy on pure and p-doped HTM thin films correlated with density functional theory calculations provides insight into the doping mechanism. For CPTCFA:m-MTDATA, an integer charge transfer is observed. However, this is not the case for CPTCFA:HTM-B, suggesting the formation of a charge transfer complex in this case. The electronic properties at ITO | (p-)HTM hetero- and p-HTM | HTM homointerfaces are studied by PES in step-by-step deposition experiments. A novel density of states-based model for fitting the PES data is presented. This model is able to reproduce the classically obtained results at the heterointerfaces while providing more details and accurate electrical potential distributions. More importantly the model allows for the analysis of the homointerfaces and reveals an unexpected space charge region in the p-doped HTM layer. After the model is advanced, an increased number of states in the energy gap for the molecules of the undoped layer right at the interface is predicted. The interfaces between Al back-contacts and HTM as well as p-doped HTM layers are investigated. These interfaces are relevant for hole-only devices which are used to study effects on less complex device structures. It is shown that Al tends to diffuse into the organic thin film where it reacts with the dopant molecule, redopes the material, and strongly changes the electronic properties. This could be a problem, as this HTM | Al back-contact interface appears to have a strong influence on the properties of hole-only devices, potentially leading to conclusions which do not hold for full devices, where this interface does not exist. Finally, a low excitation energy electron emission (termed L4E) effect is observed. Free electrons are emitted by shining an ultraviolet LED on m-MTDATA thin films even though the photon energy is lower than the ionization potential of the material. The effect is most likely related to a triplet-triplet-annihilation mechanism and an application as room temperature electron source is discussed.
Typ des Eintrags: | Dissertation | ||||
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Erschienen: | 2022 | ||||
Autor(en): | Frericks, Markus | ||||
Art des Eintrags: | Erstveröffentlichung | ||||
Titel: | Organic Hole Transport Materials: Properties and Interface Formation | ||||
Sprache: | Englisch | ||||
Referenten: | Jaegermann, Prof. Dr. Wolfram ; Ensinger, Prof. Dr. Wolfgang | ||||
Publikationsjahr: | 2022 | ||||
Ort: | Darmstadt | ||||
Kollation: | XIV, 173 Seiten | ||||
Datum der mündlichen Prüfung: | 15 September 2022 | ||||
DOI: | 10.26083/tuprints-00022397 | ||||
URL / URN: | https://tuprints.ulb.tu-darmstadt.de/22397 | ||||
Kurzbeschreibung (Abstract): | This dissertation is related to organic semiconductor (OSC) materials for organic light emitting diode (OLED) applications investigated together with our project partner Merck KGaA. One often stated advantage of OSCs is the chemical flexibility to easily synthesize new molecules. A deeper understanding of the connection between molecular structure and device characteristics could lead to faster material screening and development. As contribution to this goal, the here presented work analyzes and discusses the properties of hole transport materials (HTMs) and especially their electronic interface properties. Indium tin oxide (ITO) substrates, a commercially available p-dopant, CPTCFA, a literature-known HTM, m-MTDATA, a commercial HTM from Merck KGaA, HTM-B, and aluminum are characterized as thin films by photoelectron spectroscopy (PES) to obtain the materials’ electronic properties. Ultraviolet, visible, near- and mid-infrared absorption spectroscopy on pure and p-doped HTM thin films correlated with density functional theory calculations provides insight into the doping mechanism. For CPTCFA:m-MTDATA, an integer charge transfer is observed. However, this is not the case for CPTCFA:HTM-B, suggesting the formation of a charge transfer complex in this case. The electronic properties at ITO | (p-)HTM hetero- and p-HTM | HTM homointerfaces are studied by PES in step-by-step deposition experiments. A novel density of states-based model for fitting the PES data is presented. This model is able to reproduce the classically obtained results at the heterointerfaces while providing more details and accurate electrical potential distributions. More importantly the model allows for the analysis of the homointerfaces and reveals an unexpected space charge region in the p-doped HTM layer. After the model is advanced, an increased number of states in the energy gap for the molecules of the undoped layer right at the interface is predicted. The interfaces between Al back-contacts and HTM as well as p-doped HTM layers are investigated. These interfaces are relevant for hole-only devices which are used to study effects on less complex device structures. It is shown that Al tends to diffuse into the organic thin film where it reacts with the dopant molecule, redopes the material, and strongly changes the electronic properties. This could be a problem, as this HTM | Al back-contact interface appears to have a strong influence on the properties of hole-only devices, potentially leading to conclusions which do not hold for full devices, where this interface does not exist. Finally, a low excitation energy electron emission (termed L4E) effect is observed. Free electrons are emitted by shining an ultraviolet LED on m-MTDATA thin films even though the photon energy is lower than the ionization potential of the material. The effect is most likely related to a triplet-triplet-annihilation mechanism and an application as room temperature electron source is discussed. |
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Alternatives oder übersetztes Abstract: |
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Freie Schlagworte: | Organic semiconductor, Photoelectron spectroscopy, Surface Science, Interfaces, Doping | ||||
Status: | Verlagsversion | ||||
URN: | urn:nbn:de:tuda-tuprints-223973 | ||||
Sachgruppe der Dewey Dezimalklassifikatin (DDC): | 500 Naturwissenschaften und Mathematik > 530 Physik | ||||
Fachbereich(e)/-gebiet(e): | 11 Fachbereich Material- und Geowissenschaften 11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft 11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft > Fachgebiet Oberflächenforschung |
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Hinterlegungsdatum: | 18 Okt 2022 12:12 | ||||
Letzte Änderung: | 19 Okt 2022 06:47 | ||||
PPN: | |||||
Referenten: | Jaegermann, Prof. Dr. Wolfram ; Ensinger, Prof. Dr. Wolfgang | ||||
Datum der mündlichen Prüfung / Verteidigung / mdl. Prüfung: | 15 September 2022 | ||||
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