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Laser-ablation deposition and characterization of polycrystalline Nd-modified Pb(Zr,Ti)O<sub>3</sub> thin filmsLappalainen, J. (Jyrki) 03 November 1999 (has links)
Abstract
Nd-modified lead-zirconate-titanate (PNZT) thin films were deposited on MgO(100), Si(100) and Al2O3(1102) single-crystal substrates using the pulsed-laser-ablation technique with a XeCl excimer laser. The post-annealing heat-treatment technique was used for the crystallisation of the films. The structural characterization, microstructure and the chemical composition of the thin films and of the ceramic Pb0.97Nd0.02(Zr0.55Ti0.45)O3 targets after ablation were studied using x-ray diffraction, scanning electron microscopy and energy-dispersive x-ray spectroscopy, respectively. The formation of the particulates on the target surface during the ablation process and the effect of the particulates on the quality of the thin films were studied. Typically, the ferroelectric PNZT thin films for the capacitor structures were deposited at the laser-beam fluence of around 1.0 J/cm2 and annealed at the temperatures from 600 to 700 °C. The dielectric and, especially, the polarization properties and the residual macroscopic stress state of the PNZT thin films were studied. The relationship between the electrical properties of the films and the nature of the stress state was also investigated.
The average growth rate of the PNZT films increased linearly with increasing laser-beam fluence above the threshold value of around 0.4 J/cm2. The composition of the PNZT films varied strongly with the deposition laser-beam fluence and annealing temperature. The phase structure of PNZT films ablated from Pb0.97Nd0.02(Zr0.55Ti0.45)O3 targets could be adjusted between tetragonal and rhombohedral structures by changing the incident laser-beam fluence on the target surface. The surface of the target after ablation was covered by the laser-cone structure and the topmost layer of the target was amorphous having TiO2 and ZrO2 structures with separate segregated lead droplets.
On MgO substrates, values of the relative dielectric constant er from 430 to 560 and of the remanent polarization εr of the order of 18 μC/cm2 were achieved in PNZT films which were under a compressive stress of the order of 300 MPa. On silicon substrates, εr was around 100 and the polarization properties of the films were modest due to a strong tensile stress of the order of 400 MPa. The Poole-Frenkel conduction mechanism with the activation energy of around 0.2 eV was found responsible for the leakage conductivity in the capacitor structures with PNZT films.
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Characterization of HfO<sub>2</sub> Films for Flash Memory ApplicationsGaddipati, Surendra 28 June 2004 (has links)
The scaling of integrated circuits requires the use of alternative dielectric materials as the replacement for silicon dioxide in the submicron devices. The scaling limit for silicon dioxide used in MOSFETs is 1.2nm and the Oxide Nitride Oxide (ONO) stack used in flash memory applications is 13.0nm. The use of alternative dielectrics with high- κ value will alleviate the problem of charge retention and also would help to decrease the programming voltage in case of flash memory cells.
Many alternative high- κ dielectric materials such as TaO2, TiO2, Al2O3 etc., have been examined for this purpose previously. Recently the metal oxides such as ZrO2 and HfO2 have been found to be viable replacements for the existing oxide. The high- κ value along with high bandgap motivates this replacement. A complete modeling of the reactively sputtered HfO2 films in the thickness range of 294Å to 480Å is attempted using the data obtained by one of the group members at the Sharp Laboratories of America, Inc.
The IV and CV data is used to characterize the material properties and conduction mechanism in HfO2 films used as a control dielectric. The slope of the Poole-Frenkel plot is close to the theoretical value in the intermediate region however it starts to deviate at high field regions. Temperature dependent data also suggests that there are two types of vii traps active in the intermediate and high field regions. However the origin of these traps is not known. Temperature dependent data indicates that there is a rapid increase in the leakage current at elevated temperatures in the high field region further suggesting that the charge retention capability of the device would be adversely affected under such conditions.
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Estudo das propriedades elétro-óptica de dispositivos eletroluminescentes confeccionados com um compósito híbridoStefanelo, Josiani Cristina [UNESP] 05 October 2009 (has links) (PDF)
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stefanelo_jc_me_rcla.pdf: 1971755 bytes, checksum: f2545c6a190dc7a872bf14f2c2b4fce6 (MD5) / Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES) / Neste trabalho foi desenvolvido um dispositivo eletroluminescente (EL) constituído de um compósito híbrido (CH), formado por uma blenda polimérica e um material EL inorgânico. A blenda é composta por um polímero condutor, a poli(o-metoxianilina) (POMA) dopada com ácido tolueno sulfônico (TSA), e um polímero isolante, o poli(fluoreto de vinilideno-co-trifluoretileno) (P(VDF-TrFE)). A esta blenda é acrescentado um material EL inorgânico, o silicato de zinco dopado com Manganês (Zn2SiO4:Mn), formando assim, o compósito híbrido. O dispositivo foi construído depositando o compósito por drop casting sobre um substrato de óxido de estanho dopado com flúor (FTO) e após cristalização em uma estufa foi depositado um eletrodo de metal por evaporação à vácuo formando uma estrutura tipo “sanduíche”. Neste trabalho foram construídos dispositivos com eletrodo superior de Alumínio (Al) e Ouro (Au), denominados: FTO/CH/Al e FTO/CH/Au. O comportamento elétrico dos dispositivos de FTO/CH/Al foram analisados aplicando-se as teorias de Emissão Termoiônica, Emissão Schottky e Emissão Poole-Frenkel, o que tornou possível encontrar alguns parâmetros como: altura da barreira para a junção metal/CH, condutividade do CH e fator de retificação. O dispositivo de FTO/CH/Au foi caracterizado pela técnica de espectroscopia de impedância, sendo obtido também a altura da barreira para a junção metal/CH, a condutividade do CH, além da constante dielétrica do compósito e como variam esses dois últimos parâmetros com a temperatura. A aplicação das teorias de Emissão Termoiônica, Emissão Schottky e Emissão Poole-Frenkel produziram resultados semelhantes aos obtidos pela técnica de espectroscopia de impedância. Os espectros de luminescência apresentaram um pico em l = 528 nm com estabilidade temporal de emissão comparável a dos dispositivos inorgânicos puros. / In this work was developed an electroluminescent (EL) device made up with a hybrid composite (CH), that is formed by a polymeric blend and an inorganic EL material. The conductive polymer, poly(o-methoxyaniline) (POMA) doped with p-Toluene sulphonic acid (TSA), and an isolating polymer, the poly(vinylidenefluoride-co-trifluoroethylene) (P(VDFTrFE)), was used to make the polymer blend. An inorganic EL material, the zinc silicate manganese-doped (Zn2SiO4:Mn), was added to the blend, forming the hybrid composite. The composite was deposited by drop-casting over a Fluoride Tin Oxide substrate (FTO) and after the crystallization in an oven a metal electrode was deposited by vacuum evaporation, forming a type “sandwich” structure. In this work were constructed different devices. Aluminum (Al) and Gold (Au) were used as upper electrodes, therefore the device structures were: FTO/CH/Al and FTO/CH/Au. To analyze the electrical behavior of the FTO/CH/Al device was applied the theories of Thermionic Emission, Schottky Emission and Poole- Frenkel Emission. Using these theories was possible to obtain parameters such as; the barrier height from the metal/CH junction, CH conductivity and diode rectifier factor. The FTO/CH/Au device was characterized using the impedance spectroscopy technique. For this device was also possible to obtain the barrier height from the metal/CH junction, CH conductivity and CH dielectric constant. For the last two parameters the dependence with the temperature were also observed. The application of the theories of Thermionic Emission, Schottky Emission and Poole-Frenkel Emission produced similar results to that obtained by the impedance spectroscopy technique. The luminescence spectra, for the devices, showed a peak at l = 528 nm with emission stability in time that it is comparable of pure inorganic devices.
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Electrical Transport In Metal-oxide-semiconductor CapacitorsArikan, Mustafa 01 October 2004 (has links) (PDF)
The current transport mechanisms in metal-oxide-semiconductor (MOS) capacitors have been studied. The devices used in this study have characterized by current-voltage analyses. Physical parameter extractions and computer generated fit methods have been applied to experimental data. Two devices have been investigated: A relatively thick oxide (125 nm) and an ultra-thin oxide (3 nm) MOS structures. The voltage and temperature dependence of these devices have been explained by using present current transport models.
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Estudo das propriedades elétro-óptica de dispositivos eletroluminescentes confeccionados com um compósito híbrido /Stefanelo, Josiani Cristina. January 2009 (has links)
Orientador: Dante Luis Chinaglia / Banca: Clarissa de Almeida Olivati / Banca: Luiz Francisco Malmonge / Resumo: Neste trabalho foi desenvolvido um dispositivo eletroluminescente (EL) constituído de um compósito híbrido (CH), formado por uma blenda polimérica e um material EL inorgânico. A blenda é composta por um polímero condutor, a poli(o-metoxianilina) (POMA) dopada com ácido tolueno sulfônico (TSA), e um polímero isolante, o poli(fluoreto de vinilideno-co-trifluoretileno) (P(VDF-TrFE)). A esta blenda é acrescentado um material EL inorgânico, o silicato de zinco dopado com Manganês (Zn2SiO4:Mn), formando assim, o compósito híbrido. O dispositivo foi construído depositando o compósito por drop casting sobre um substrato de óxido de estanho dopado com flúor (FTO) e após cristalização em uma estufa foi depositado um eletrodo de metal por evaporação à vácuo formando uma estrutura tipo "sanduíche". Neste trabalho foram construídos dispositivos com eletrodo superior de Alumínio (Al) e Ouro (Au), denominados: FTO/CH/Al e FTO/CH/Au. O comportamento elétrico dos dispositivos de FTO/CH/Al foram analisados aplicando-se as teorias de Emissão Termoiônica, Emissão Schottky e Emissão Poole-Frenkel, o que tornou possível encontrar alguns parâmetros como: altura da barreira para a junção metal/CH, condutividade do CH e fator de retificação. O dispositivo de FTO/CH/Au foi caracterizado pela técnica de espectroscopia de impedância, sendo obtido também a altura da barreira para a junção metal/CH, a condutividade do CH, além da constante dielétrica do compósito e como variam esses dois últimos parâmetros com a temperatura. A aplicação das teorias de Emissão Termoiônica, Emissão Schottky e Emissão Poole-Frenkel produziram resultados semelhantes aos obtidos pela técnica de espectroscopia de impedância. Os espectros de luminescência apresentaram um pico em l = 528 nm com estabilidade temporal de emissão comparável a dos dispositivos inorgânicos puros. / Abstract: In this work was developed an electroluminescent (EL) device made up with a hybrid composite (CH), that is formed by a polymeric blend and an inorganic EL material. The conductive polymer, poly(o-methoxyaniline) (POMA) doped with p-Toluene sulphonic acid (TSA), and an isolating polymer, the poly(vinylidenefluoride-co-trifluoroethylene) (P(VDFTrFE)), was used to make the polymer blend. An inorganic EL material, the zinc silicate manganese-doped (Zn2SiO4:Mn), was added to the blend, forming the hybrid composite. The composite was deposited by drop-casting over a Fluoride Tin Oxide substrate (FTO) and after the crystallization in an oven a metal electrode was deposited by vacuum evaporation, forming a type "sandwich" structure. In this work were constructed different devices. Aluminum (Al) and Gold (Au) were used as upper electrodes, therefore the device structures were: FTO/CH/Al and FTO/CH/Au. To analyze the electrical behavior of the FTO/CH/Al device was applied the theories of Thermionic Emission, Schottky Emission and Poole- Frenkel Emission. Using these theories was possible to obtain parameters such as; the barrier height from the metal/CH junction, CH conductivity and diode rectifier factor. The FTO/CH/Au device was characterized using the impedance spectroscopy technique. For this device was also possible to obtain the barrier height from the metal/CH junction, CH conductivity and CH dielectric constant. For the last two parameters the dependence with the temperature were also observed. The application of the theories of Thermionic Emission, Schottky Emission and Poole-Frenkel Emission produced similar results to that obtained by the impedance spectroscopy technique. The luminescence spectra, for the devices, showed a peak at l = 528 nm with emission stability in time that it is comparable of pure inorganic devices. / Mestre
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Percolation with Plasticity Materials and Their Neuromorphic ApplicationsPatmiou, Maria January 2021 (has links)
No description available.
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Transport elektrického náboje v tantalovém kondenzátoru / Transport of Electric Charge in Tantalum CapacitorPelčák, Jaromír January 2012 (has links)
The task of the thesis was studding of tantalum capacitors with solid electrolytes properties. Ta – Ta2O5 – MnO2 capacitor by its construction represents MIS structure, where tantalum anode has metal conductivity and MnO2 cathode is semiconductor. Isolation layer consists of tantalum pentoxide Ta2O5 with relative permitivity r = 27. Dielectric thickness is typically in range from 30 to 150nm. The capacitor charge is not only stored and accumulated on electrodes but also in localised states (oxide vacancies) in isolation layer. The capacitor connected in normal mode represents MIS structure polarized in reveres direction when the applied voltage higher potential barrier between semiconductor - MnO2 cathode and isolation of Ta2O5. The transport of charge carriers via isolation layer is determined by Poole-Frenkel mechanisms and tunnelling. Poole-Frenkel mechanism of charge transport is dominant in low intensity of electric field. Tunnelling determines current at higher electric field intensity. During low intensity of electric field ohmic component is also presented which is determined by volume of resistance of impurities in isolation layer due to donor states of oxygen vacancies. Based on the modelling of measured VA characteristics is possible to estimate determine dielectric thickness of Ta2O5 and determine share of Poole-Frenkelov and tunnel current and charge transportation. The thesis is described charge transport and charge concentration on tantalum capacitor in low frequency area and analysis of capacitor behaviour at frequency band. The first impulse for the thesis was an effort to create equivalent circuit diagram of tantalum capacitor in respect of its physical and electrical behaviour. There is an opportunity to study and determine electric charge transport and its accumulation based on the equivalent circuit diagram structure. There is also a chance to define and trace potential barriers and charge distribution in the capacitor structure based on an measurement and carried out experiments. This methodology and analysis consists of electrical characteristic determination to create physical model of the capacitor describing it function, properties and behaviour.
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Charge transport and energy levels in organic semiconductors / Ladungstransport und Energieniveaus in organischen HalbleiternWidmer, Johannes 25 November 2014 (has links) (PDF)
Organic semiconductors are a new key technology for large-area and flexible thin-film electronics. They are deposited as thin films (sub-nanometer to micrometer) on large-area substrates. The technologically most advanced applications are organic light emitting diodes (OLEDs) and organic photovoltaics (OPV). For the improvement of performance and efficiency, correct modeling of the electronic processes in the devices is essential. Reliable characterization and validation of the electronic properties of the materials is simultaneously required for the successful optimization of devices. Furthermore, understanding the relations between material structures and their key characteristics opens the path for innovative material and device design.
In this thesis, two material characterization methods are developed, respectively refined and applied: a novel technique for measuring the charge carrier mobility μ and a way to determine the ionization energy IE or the electron affinity EA of an organic semiconductor.
For the mobility measurements, a new evaluation approach for space-charge limited current (SCLC) measurements in single carrier devices is developed. It is based on a layer thickness variation of the material under investigation. In the \"potential mapping\" (POEM) approach, the voltage as a function of the device thickness V(d) at a given current density is shown to coincide with the spatial distribution of the electric potential V(x) in the thickest device. On this basis, the mobility is directly obtained as function of the electric field F and the charge carrier density n. The evaluation is model-free, i.e. a model for μ(F, n) to fit the measurement data is not required, and the measurement is independent of a possible injection barrier or potential drop at non-optimal contacts. The obtained μ(F, n) function describes the effective average mobility of free and trapped charge carriers. This approach realistically describes charge transport in energetically disordered materials, where a clear differentiation between trapped and free charges is impossible or arbitrary.
The measurement of IE and EA is performed by characterizing solar cells at varying temperature T. In suitably designed devices based on a bulk heterojunction (BHJ), the open-circuit voltage Voc is a linear function of T with negative slope in the whole measured range down to 180K. The extrapolation to temperature zero V0 = Voc(T → 0K) is confirmed to equal the effective gap Egeff, i.e. the difference between the EA of the acceptor and the IE of the donor. The successive variation of different components of the devices and testing their influence on V0 verifies the relation V0 = Egeff. On this basis, the IE or EA of a material can be determined in a BHJ with a material where the complementary value is known. The measurement is applied to a number of material combinations, confirming, refining, and complementing previously reported values from ultraviolet photo electron spectroscopy (UPS) and inverse photo electron spectroscopy (IPES).
These measurements are applied to small molecule organic semiconductors, including mixed layers. In blends of zinc-phthalocyanine (ZnPc) and C60, the hole mobility is found to be thermally and field activated, as well as increasing with charge density. Varying the mixing ratio, the hole mobility is found to increase with increasing ZnPc content, while the effective gap stays unchanged. A number of further materials and material blends are characterized with respect to hole and electron mobility and the effective gap, including highly diluted donor blends, which have been little investigated before. In all materials, a pronounced field activation of the mobility is observed. The results enable an improved detailed description of the working principle of organic solar cells and support the future design of highly efficient and optimized devices. / Organische Halbleiter sind eine neue Schlüsseltechnologie für großflächige und flexible Dünnschichtelektronik. Sie werden als dünne Materialschichten (Sub-Nanometer bis Mikrometer) auf großflächige Substrate aufgebracht. Die technologisch am weitesten fortgeschrittenen Anwendungen sind organische Leuchtdioden (OLEDs) und organische Photovoltaik (OPV). Zur weiteren Steigerung von Leistungsfähigkeit und Effizienz ist die genaue Modellierung elektronischer Prozesse in den Bauteilen von grundlegender Bedeutung. Für die erfolgreiche Optimierung von Bauteilen ist eine zuverlässige Charakterisierung und Validierung der elektronischen Materialeigenschaften gleichermaßen erforderlich. Außerdem eröffnet das Verständnis der Zusammenhänge zwischen Materialstruktur und -eigenschaften einen Weg für innovative Material- und Bauteilentwicklung.
Im Rahmen dieser Dissertation werden zwei Methoden für die Materialcharakterisierung entwickelt, verfeinert und angewandt: eine neuartige Methode zur Messung der Ladungsträgerbeweglichkeit μ und eine Möglichkeit zur Bestimmung der Ionisierungsenergie IE oder der Elektronenaffinität EA eines organischen Halbleiters.
Für die Beweglichkeitsmessungen wird eine neue Auswertungsmethode für raumladungsbegrenzte Ströme (SCLC) in unipolaren Bauteilen entwickelt. Sie basiert auf einer Schichtdickenvariation des zu charakterisierenden Materials. In einem Ansatz zur räumlichen Abbildung des elektrischen Potentials (\"potential mapping\", POEM) wird gezeigt, dass das elektrische Potential als Funktion der Schichtdicke V(d) bei einer gegebenen Stromdichte dem räumlichen Verlauf des elektrischen Potentials V(x) im dicksten Bauteil entspricht. Daraus kann die Beweglichkeit als Funktion des elektrischen Felds F und der Ladungsträgerdichte n berechnet werden. Die Auswertung ist modellfrei, d.h. ein Modell zum Angleichen der Messdaten ist für die Berechnung von μ(F, n) nicht erforderlich. Die Messung ist außerdem unabhängig von einer möglichen Injektionsbarriere oder einer Potentialstufe an nicht-idealen Kontakten. Die gemessene Funktion μ(F, n) beschreibt die effektive durchschnittliche Beweglichkeit aller freien und in Fallenzuständen gefangenen Ladungsträger. Dieser Zugang beschreibt den Ladungstransport in energetisch ungeordneten Materialien realistisch, wo eine klare Unterscheidung zwischen freien und Fallenzuständen nicht möglich oder willkürlich ist.
Die Messung von IE und EA wird mithilfe temperaturabhängiger Messungen an Solarzellen durchgeführt. In geeigneten Bauteilen mit einem Mischschicht-Heteroübergang (\"bulk heterojunction\" BHJ) ist die Leerlaufspannung Voc im gesamten Messbereich oberhalb 180K eine linear fallende Funktion der Temperatur T. Es kann bestätigt werden, dass die Extrapolation zum Temperaturnullpunkt V0 = Voc(T → 0K) mit der effektiven Energielücke Egeff , d.h. der Differenz zwischen EA des Akzeptor-Materials und IE des Donator-Materials, übereinstimmt. Die systematische schrittweise Variation einzelner Bestandteile der Solarzellen und die Überprüfung des Einflusses auf V0 bestätigen die Beziehung V0 = Egeff. Damit kann die IE oder EA eines Materials bestimmt werden, indem man es in einem BHJ mit einem Material kombiniert, dessen komplementärer Wert bekannt ist. Messungen per Ultraviolett-Photoelektronenspektroskopie (UPS) und inverser Photoelektronenspektroskopie (IPES) werden damit bestätigt, präzisiert und ergänzt.
Die beiden entwickelten Messmethoden werden auf organische Halbleiter aus kleinen Molekülen einschließlich Mischschichten angewandt. In Mischschichten aus Zink-Phthalocyanin (ZnPc) und C60 wird eine Löcherbeweglichkeit gemessen, die sowohl thermisch als auch feld- und ladungsträgerdichteaktiviert ist. Wenn das Mischverhältnis variiert wird, steigt die Löcherbeweglichkeit mit zunehmendem ZnPc-Anteil, während die effektive Energielücke unverändert bleibt. Verschiedene weitere Materialien und Materialmischungen werden hinsichtlich Löcher- und Elektronenbeweglichkeit sowie ihrer Energielücke charakterisiert, einschließlich bisher wenig untersuchter hochverdünnter Donator-Systeme. In allen Materialien wird eine deutliche Feldaktivierung der Beweglichkeit beobachtet. Die Ergebnisse ermöglichen eine verbesserte Beschreibung der detaillierten Funktionsweise organischer Solarzellen und unterstützen die künftige Entwicklung hocheffizienter und optimierter Bauteile.
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Charge transport and energy levels in organic semiconductorsWidmer, Johannes 02 October 2014 (has links)
Organic semiconductors are a new key technology for large-area and flexible thin-film electronics. They are deposited as thin films (sub-nanometer to micrometer) on large-area substrates. The technologically most advanced applications are organic light emitting diodes (OLEDs) and organic photovoltaics (OPV). For the improvement of performance and efficiency, correct modeling of the electronic processes in the devices is essential. Reliable characterization and validation of the electronic properties of the materials is simultaneously required for the successful optimization of devices. Furthermore, understanding the relations between material structures and their key characteristics opens the path for innovative material and device design.
In this thesis, two material characterization methods are developed, respectively refined and applied: a novel technique for measuring the charge carrier mobility μ and a way to determine the ionization energy IE or the electron affinity EA of an organic semiconductor.
For the mobility measurements, a new evaluation approach for space-charge limited current (SCLC) measurements in single carrier devices is developed. It is based on a layer thickness variation of the material under investigation. In the \"potential mapping\" (POEM) approach, the voltage as a function of the device thickness V(d) at a given current density is shown to coincide with the spatial distribution of the electric potential V(x) in the thickest device. On this basis, the mobility is directly obtained as function of the electric field F and the charge carrier density n. The evaluation is model-free, i.e. a model for μ(F, n) to fit the measurement data is not required, and the measurement is independent of a possible injection barrier or potential drop at non-optimal contacts. The obtained μ(F, n) function describes the effective average mobility of free and trapped charge carriers. This approach realistically describes charge transport in energetically disordered materials, where a clear differentiation between trapped and free charges is impossible or arbitrary.
The measurement of IE and EA is performed by characterizing solar cells at varying temperature T. In suitably designed devices based on a bulk heterojunction (BHJ), the open-circuit voltage Voc is a linear function of T with negative slope in the whole measured range down to 180K. The extrapolation to temperature zero V0 = Voc(T → 0K) is confirmed to equal the effective gap Egeff, i.e. the difference between the EA of the acceptor and the IE of the donor. The successive variation of different components of the devices and testing their influence on V0 verifies the relation V0 = Egeff. On this basis, the IE or EA of a material can be determined in a BHJ with a material where the complementary value is known. The measurement is applied to a number of material combinations, confirming, refining, and complementing previously reported values from ultraviolet photo electron spectroscopy (UPS) and inverse photo electron spectroscopy (IPES).
These measurements are applied to small molecule organic semiconductors, including mixed layers. In blends of zinc-phthalocyanine (ZnPc) and C60, the hole mobility is found to be thermally and field activated, as well as increasing with charge density. Varying the mixing ratio, the hole mobility is found to increase with increasing ZnPc content, while the effective gap stays unchanged. A number of further materials and material blends are characterized with respect to hole and electron mobility and the effective gap, including highly diluted donor blends, which have been little investigated before. In all materials, a pronounced field activation of the mobility is observed. The results enable an improved detailed description of the working principle of organic solar cells and support the future design of highly efficient and optimized devices.:1. Introduction
2. Organic semiconductors and devices
2.1. Organic semiconductors
2.1.1. Conjugated π system
2.1.2. Small molecules and polymers
2.1.3. Disorder in amorphous materials
2.1.4. Polarons
2.1.5. Polaron hopping
2.1.6. Fermi-Dirac distribution and Fermi level
2.1.7. Quasi-Fermi levels
2.1.8. Trap states
2.1.9. Doping
2.1.10. Excitons
2.2. Interfaces and blend layers
2.2.1. Interface dipoles
2.2.2. Energy level bending
2.2.3. Injection from metal into semiconductor, and extraction
2.2.4. Excitons at interfaces
2.3. Charge transport and recombination in organic semiconductors
2.3.1. Drift transport
2.3.2. Charge carrier mobility
2.3.3. Thermally activated transport
2.3.4. Diffusion transport
2.3.5. Drift-diffusion transport
2.3.6. Space-charge limited current
2.3.7. Recombination
2.4. Mobility measurement
2.4.1. SCLC and TCLC
2.4.2. Time of flight
2.4.3. Organic field effect transistors
2.4.4. CELIV
2.5. Organic solar cells
2.5.1. Exciton diffusion towards the interface
2.5.2. Dissociation of CT states
2.5.3. CT recombination
2.5.4. Flat and bulk heterojunction
2.5.5. Transport layers
2.5.6. Thin film optics
2.5.7. Current-voltage characteristics and equivalent circuit
2.5.8. Solar cell efficiency
2.5.9. Limits of efficiency
2.5.10. Correct solar cell characterization
2.5.11. The \"O-Factor\"
3. Materials and experimental methods
3.1. Materials
3.2. Device fabrication and layout
3.2.1. Layer deposition
3.2.2. Encapsulation
3.2.3. Homogeneity of layer thickness on a wafer
3.2.4. Device layout
3.3. Characterization
3.3.1. Electrical characterization
3.3.2. Sample illumination
3.3.3. Temperature dependent characterization
3.3.4. UPS
4. Simulations
5.1. Design of single carrier devices
5.1.1. General design requirements
5.1.2. Single carrier devices for space-charge limited current
5.1.3. Ohmic regime
5.1.4. Design of injection and extraction layers
5.2. Advanced evaluation of SCLC – potential mapping
5.2.1. Potential mapping by thickness variation
5.2.2. Further evaluation of the transport profile
5.2.3. Injection into and extraction from single carrier devices
5.2.4. Majority carrier approximation
5.3. Proof of principle: POEM on simulated data
5.3.1. Constant mobility
5.3.2. Field dependent mobility
5.3.3. Field and charge density activated mobility
5.3.4. Conclusion
5.4. Application: Transport characterization in organic semiconductors
5.4.1. Hole transport in ZnPc:C60
5.4.2. Hole transport in ZnPc:C60 – temperature variation
5.4.3. Hole transport in ZnPc:C60 – blend ratio variation
5.4.4. Hole transport in ZnPc:C70
5.4.5. Hole transport in neat ZnPc
5.4.6. Hole transport in F4-ZnPc:C60
5.4.7. Hole transport in DCV-5T-Me33:C60
5.4.8. Electron transport in ZnPc:C60
5.4.9. Electron transport in neat Bis-HFl-NTCDI
5.5. Summary and discussion of the results
5.5.1. Phthalocyanine:C60 blends
5.5.2. DCV-5T-Me33:C60
5.5.3. Conclusion
6. Organic solar cell characteristics: the influence of temperature
6.1. ZnPc:C60 solar cells
6.1.1. Temperature variation
6.1.2. Illumination intensity variation
6.2. Voc in flat and bulk heterojunction organic solar cells
6.2.1. Qualitative difference in Voc(I, T)
6.2.2. Interpretation of Voc(I, T)
6.3. BHJ stoichiometry variation
6.3.1. Voc upon variation of stoichiometry and contact layer
6.3.2. V0 upon stoichiometry variation
6.3.3. Low donor content stoichiometry
6.3.4. Conclusion from stoichiometry variation
6.4. Transport material variation
6.4.1. HTM variation
6.4.2. ETM variation
6.5. Donor:acceptor material variation
6.5.1. Donor variation
6.5.2. Acceptor variation
6.6. Conclusion
7. Summary and outlook
7.1. Summary
7.2. Outlook
A. Appendix
A.1. Energy pay-back of this thesis
A.2. Tables and registers / Organische Halbleiter sind eine neue Schlüsseltechnologie für großflächige und flexible Dünnschichtelektronik. Sie werden als dünne Materialschichten (Sub-Nanometer bis Mikrometer) auf großflächige Substrate aufgebracht. Die technologisch am weitesten fortgeschrittenen Anwendungen sind organische Leuchtdioden (OLEDs) und organische Photovoltaik (OPV). Zur weiteren Steigerung von Leistungsfähigkeit und Effizienz ist die genaue Modellierung elektronischer Prozesse in den Bauteilen von grundlegender Bedeutung. Für die erfolgreiche Optimierung von Bauteilen ist eine zuverlässige Charakterisierung und Validierung der elektronischen Materialeigenschaften gleichermaßen erforderlich. Außerdem eröffnet das Verständnis der Zusammenhänge zwischen Materialstruktur und -eigenschaften einen Weg für innovative Material- und Bauteilentwicklung.
Im Rahmen dieser Dissertation werden zwei Methoden für die Materialcharakterisierung entwickelt, verfeinert und angewandt: eine neuartige Methode zur Messung der Ladungsträgerbeweglichkeit μ und eine Möglichkeit zur Bestimmung der Ionisierungsenergie IE oder der Elektronenaffinität EA eines organischen Halbleiters.
Für die Beweglichkeitsmessungen wird eine neue Auswertungsmethode für raumladungsbegrenzte Ströme (SCLC) in unipolaren Bauteilen entwickelt. Sie basiert auf einer Schichtdickenvariation des zu charakterisierenden Materials. In einem Ansatz zur räumlichen Abbildung des elektrischen Potentials (\"potential mapping\", POEM) wird gezeigt, dass das elektrische Potential als Funktion der Schichtdicke V(d) bei einer gegebenen Stromdichte dem räumlichen Verlauf des elektrischen Potentials V(x) im dicksten Bauteil entspricht. Daraus kann die Beweglichkeit als Funktion des elektrischen Felds F und der Ladungsträgerdichte n berechnet werden. Die Auswertung ist modellfrei, d.h. ein Modell zum Angleichen der Messdaten ist für die Berechnung von μ(F, n) nicht erforderlich. Die Messung ist außerdem unabhängig von einer möglichen Injektionsbarriere oder einer Potentialstufe an nicht-idealen Kontakten. Die gemessene Funktion μ(F, n) beschreibt die effektive durchschnittliche Beweglichkeit aller freien und in Fallenzuständen gefangenen Ladungsträger. Dieser Zugang beschreibt den Ladungstransport in energetisch ungeordneten Materialien realistisch, wo eine klare Unterscheidung zwischen freien und Fallenzuständen nicht möglich oder willkürlich ist.
Die Messung von IE und EA wird mithilfe temperaturabhängiger Messungen an Solarzellen durchgeführt. In geeigneten Bauteilen mit einem Mischschicht-Heteroübergang (\"bulk heterojunction\" BHJ) ist die Leerlaufspannung Voc im gesamten Messbereich oberhalb 180K eine linear fallende Funktion der Temperatur T. Es kann bestätigt werden, dass die Extrapolation zum Temperaturnullpunkt V0 = Voc(T → 0K) mit der effektiven Energielücke Egeff , d.h. der Differenz zwischen EA des Akzeptor-Materials und IE des Donator-Materials, übereinstimmt. Die systematische schrittweise Variation einzelner Bestandteile der Solarzellen und die Überprüfung des Einflusses auf V0 bestätigen die Beziehung V0 = Egeff. Damit kann die IE oder EA eines Materials bestimmt werden, indem man es in einem BHJ mit einem Material kombiniert, dessen komplementärer Wert bekannt ist. Messungen per Ultraviolett-Photoelektronenspektroskopie (UPS) und inverser Photoelektronenspektroskopie (IPES) werden damit bestätigt, präzisiert und ergänzt.
Die beiden entwickelten Messmethoden werden auf organische Halbleiter aus kleinen Molekülen einschließlich Mischschichten angewandt. In Mischschichten aus Zink-Phthalocyanin (ZnPc) und C60 wird eine Löcherbeweglichkeit gemessen, die sowohl thermisch als auch feld- und ladungsträgerdichteaktiviert ist. Wenn das Mischverhältnis variiert wird, steigt die Löcherbeweglichkeit mit zunehmendem ZnPc-Anteil, während die effektive Energielücke unverändert bleibt. Verschiedene weitere Materialien und Materialmischungen werden hinsichtlich Löcher- und Elektronenbeweglichkeit sowie ihrer Energielücke charakterisiert, einschließlich bisher wenig untersuchter hochverdünnter Donator-Systeme. In allen Materialien wird eine deutliche Feldaktivierung der Beweglichkeit beobachtet. Die Ergebnisse ermöglichen eine verbesserte Beschreibung der detaillierten Funktionsweise organischer Solarzellen und unterstützen die künftige Entwicklung hocheffizienter und optimierter Bauteile.:1. Introduction
2. Organic semiconductors and devices
2.1. Organic semiconductors
2.1.1. Conjugated π system
2.1.2. Small molecules and polymers
2.1.3. Disorder in amorphous materials
2.1.4. Polarons
2.1.5. Polaron hopping
2.1.6. Fermi-Dirac distribution and Fermi level
2.1.7. Quasi-Fermi levels
2.1.8. Trap states
2.1.9. Doping
2.1.10. Excitons
2.2. Interfaces and blend layers
2.2.1. Interface dipoles
2.2.2. Energy level bending
2.2.3. Injection from metal into semiconductor, and extraction
2.2.4. Excitons at interfaces
2.3. Charge transport and recombination in organic semiconductors
2.3.1. Drift transport
2.3.2. Charge carrier mobility
2.3.3. Thermally activated transport
2.3.4. Diffusion transport
2.3.5. Drift-diffusion transport
2.3.6. Space-charge limited current
2.3.7. Recombination
2.4. Mobility measurement
2.4.1. SCLC and TCLC
2.4.2. Time of flight
2.4.3. Organic field effect transistors
2.4.4. CELIV
2.5. Organic solar cells
2.5.1. Exciton diffusion towards the interface
2.5.2. Dissociation of CT states
2.5.3. CT recombination
2.5.4. Flat and bulk heterojunction
2.5.5. Transport layers
2.5.6. Thin film optics
2.5.7. Current-voltage characteristics and equivalent circuit
2.5.8. Solar cell efficiency
2.5.9. Limits of efficiency
2.5.10. Correct solar cell characterization
2.5.11. The \"O-Factor\"
3. Materials and experimental methods
3.1. Materials
3.2. Device fabrication and layout
3.2.1. Layer deposition
3.2.2. Encapsulation
3.2.3. Homogeneity of layer thickness on a wafer
3.2.4. Device layout
3.3. Characterization
3.3.1. Electrical characterization
3.3.2. Sample illumination
3.3.3. Temperature dependent characterization
3.3.4. UPS
4. Simulations
5.1. Design of single carrier devices
5.1.1. General design requirements
5.1.2. Single carrier devices for space-charge limited current
5.1.3. Ohmic regime
5.1.4. Design of injection and extraction layers
5.2. Advanced evaluation of SCLC – potential mapping
5.2.1. Potential mapping by thickness variation
5.2.2. Further evaluation of the transport profile
5.2.3. Injection into and extraction from single carrier devices
5.2.4. Majority carrier approximation
5.3. Proof of principle: POEM on simulated data
5.3.1. Constant mobility
5.3.2. Field dependent mobility
5.3.3. Field and charge density activated mobility
5.3.4. Conclusion
5.4. Application: Transport characterization in organic semiconductors
5.4.1. Hole transport in ZnPc:C60
5.4.2. Hole transport in ZnPc:C60 – temperature variation
5.4.3. Hole transport in ZnPc:C60 – blend ratio variation
5.4.4. Hole transport in ZnPc:C70
5.4.5. Hole transport in neat ZnPc
5.4.6. Hole transport in F4-ZnPc:C60
5.4.7. Hole transport in DCV-5T-Me33:C60
5.4.8. Electron transport in ZnPc:C60
5.4.9. Electron transport in neat Bis-HFl-NTCDI
5.5. Summary and discussion of the results
5.5.1. Phthalocyanine:C60 blends
5.5.2. DCV-5T-Me33:C60
5.5.3. Conclusion
6. Organic solar cell characteristics: the influence of temperature
6.1. ZnPc:C60 solar cells
6.1.1. Temperature variation
6.1.2. Illumination intensity variation
6.2. Voc in flat and bulk heterojunction organic solar cells
6.2.1. Qualitative difference in Voc(I, T)
6.2.2. Interpretation of Voc(I, T)
6.3. BHJ stoichiometry variation
6.3.1. Voc upon variation of stoichiometry and contact layer
6.3.2. V0 upon stoichiometry variation
6.3.3. Low donor content stoichiometry
6.3.4. Conclusion from stoichiometry variation
6.4. Transport material variation
6.4.1. HTM variation
6.4.2. ETM variation
6.5. Donor:acceptor material variation
6.5.1. Donor variation
6.5.2. Acceptor variation
6.6. Conclusion
7. Summary and outlook
7.1. Summary
7.2. Outlook
A. Appendix
A.1. Energy pay-back of this thesis
A.2. Tables and registers
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