| 1. |
- Aarnio, Harri, et al.
(författare)
-
Spontaneous Charge Transfer and Dipole Formation at the Interface Between P3HT and PCBM
- 2011
-
Ingår i: Advanced Energy Materials. - : Wiley-VCH Verlag Berlin. - 1614-6832 .- 1614-6840. ; 1:5, s. 792-797
-
Tidskriftsartikel (refereegranskat)abstract
- In the pursuit of developing new materials for more efficient bulk-heterojunction solar cells, the blend poly (3-hexylthiophene):[ 6,6]-phenyl-C(61)-butyric acid methyl ester (P3HT:PCBM) serves as an important model system. The success of the P3HT: PCBM blend comes from efficient charge generation and transport with low recombination. There is not, however, a good microscopic picture of what causes these, hindering the development of new material systems. In this report UV photoelectron spectroscopy measurements on both regiorandom-(rra) and regioregular-(rr) P3HT are presented, and the results are interpreted using the Integer Charge Transfer model. The results suggest that spontaneous charge transfer from P3HT to PCBM occurs after heat treatment of P3HT: PCBM blends. The resulting formation of an interfacial dipole creates an extra barrier at the interface explaining the reduced (non-)geminate recombination with increased charge generation in heat treated rr-P3HT: PCBM blends. Extensive photoinduced absorption measurements using both above-and below-bandgap excitation light are presented, in good agreement with the suggested dipole formation.
|
|
| 2. |
- Ajjan, Fátima, 1986-, et al.
(författare)
-
Doped Conjugated Polymer Enclosing a Redox Polymer : Wiring Polyquinones with Poly(3,4‐Ethylenedioxythiophene)
- 2020
-
Ingår i: Advanced Energy and Sustainability Research. - : John Wiley & Sons. - 2699-9412. ; 1:2
-
Tidskriftsartikel (refereegranskat)abstract
- The mass implementation of renewable energies is limited by the absence of efficient and affordable technology to store electrical energy. Thus, the development of new materials is needed to improve the performance of actual devices such as batteries or supercapacitors. Herein, the facile consecutive chemically oxidative polymerization of poly(1-amino-5-chloroanthraquinone) (PACA) and poly(3,4-ethylenedioxythiophene (PEDOT) resulting in a water dispersible material PACA-PEDOT is shown. The water-based slurry made of PACA-PEDOT nanoparticles can be processed as film coated in ambient atmosphere, a critical feature for scaling up the electrode manufacturing. The novel redox polymer electrode is a nanocomposite that withstands rapid charging (16 A g−1) and delivers high power (5000 W kg−1). At lower current density its storage capacity is high (198 mAh g−1) and displays improved cycling stability (60% after 5000 cycles). Its great electrochemical performance results from the combination of the redox reversibility of the quinone groups in PACA that allows a high amount of charge storage via Faradaic reactions and the high electronic conductivity of PEDOT to access to the redox-active sites. These promising results demonstrate the potential of PACA-PEDOT to make easily organic electrodes from a water-coating process, without toxic metals, and operating in non-flammable aqueous electrolyte for large scale pseudocapacitors.
|
|
| 3. |
- Atxabal, Ainhoa, et al.
(författare)
-
Energy Level Alignment at Metal/Solution-Processed Organic Semiconductor Interfaces
- 2017
-
Ingår i: Advanced Materials. - : WILEY-V C H VERLAG GMBH. - 0935-9648 .- 1521-4095. ; 29:19
-
Tidskriftsartikel (refereegranskat)abstract
- Energy barriers between the metal Fermi energy and the molecular levels of organic semiconductor devoted to charge transport play a fundamental role in the performance of organic electronic devices. Typically, techniques such as electron photoemission spectroscopy, Kelvin probe measurements, and in-device hot-electron spectroscopy have been applied to study these interfacial energy barriers. However, so far there has not been any direct method available for the determination of energy barriers at metal interfaces with n-type polymeric semiconductors. This study measures and compares metal/solution-processed electron-transporting polymer interface energy barriers by in-device hot-electron spectroscopy and ultraviolet photoemission spectroscopy. It not only demonstrates in-device hot-electron spectroscopy as a direct and reliable technique for these studies but also brings it closer to technological applications by working ex situ under ambient conditions. Moreover, this study determines that the contamination layer coming from air exposure does not play any significant role on the energy barrier alignment for charge transport. The theoretical model developed for this work confirms all the experimental observations.
|
|
| 4. |
|
|
| 5. |
- Bao, Qinye, et al.
(författare)
-
Energy Level Alignment of N-Doping Fullerenes and Fullerene Derivatives Using Air-Stable Dopant
- 2017
-
Ingår i: ACS Applied Materials and Interfaces. - : AMER CHEMICAL SOC. - 1944-8244 .- 1944-8252. ; 9:40, s. 35476-35482
-
Tidskriftsartikel (refereegranskat)abstract
- Doping has been proved to be one of the powerful technologies to achieve significant improvement in the performance of organic electronic devices. Herein, we systematically map out the interface properties of solution-processed air-stable n-type (4(1,3-dimethyl-2,3-dihydro-1H-benzoimidazol-2-yl)phenyl) doping fullerenes and fullerene derivatives and establish a universal energy level alignment scheme for this class of n-doped system. At low doping levels at which the charge-transfer doping induces mainly bound charges, the energy level alignment of the n-doping organic semiconductor can be described by combining integer charger transfer-induced shifts with a so-called double-dipole step. At high doping levels, significant densities of free charges are generated and the charge flows between the organic film and the conducting electrodes equilibrating the Fermi level in a classic "depletion layer" scheme. Moreover, we demonstrate that the model holds for both n- and p-doping of pi-backbone molecules and polymers. With the results, we provide wide guidance for identifying the application of the current organic n-type doping technology in organic electronics.
|
|
| 6. |
- Bao, Qinye, et al.
(författare)
-
Energy Level Bending in Ultrathin Polymer Layers Obtained through Langmuir-Shafer Deposition
- 2016
-
Ingår i: Advanced Functional Materials. - : WILEY-V C H VERLAG GMBH. - 1616-301X .- 1616-3028. ; 26:7, s. 1077-1084
-
Tidskriftsartikel (refereegranskat)abstract
- The semiconductor-electrode interface impacts the function and the performance of (opto) electronic devices. For printed organic electronics the electrode surface is not atomically clean leading to weakly interacting interfaces. As a result, solution-processed organic ultrathin films on electrodes typically form islands due to dewetting. It has therefore been utterly difficult to achieve homogenous ultrathin conjugated polymer films. This has made the investigation of the correct energetics of the conjugated polymer-electrode interface impossible. Also, this has hampered the development of devices including ultrathin conjugated polymer layers. Here, LangmuirShafer-manufactured homogenous mono-and multilayers of semiconducting polymers on metal electrodes are reported and the energy level bending using photoelectron spectroscopy is tracked. The amorphous films display an abrupt energy level bending that does not extend beyond the first monolayer. These findings provide new insights of the energetics of the polymer-electrode interface and opens up for new high-performing devices based on ultrathin semiconducting polymers.
|
|
| 7. |
- Bao, Qinye, 1985-
(författare)
-
Interface Phenomena in Organic Electronics
- 2015
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Organic electronics based on organic semiconductors offer tremendous advantages compared to traditional inorganic counterparts such as low temperature processing, light weight, low manufacturing cost, high throughput and mechanical flexibility. Many key electronic processes in organic electronic devices, e.g. charge injection/extraction, charge recombination and exciton dissociation, occur at interfaces, significantly controlling performance and function. Understanding/modeling the interface energetics at organic-electrode/organic-organic heterojunctions is one of the crucial issues for organic electronic technologies to provide a route for improving device efficiency, which is the aim of the research presented in this thesis.Integer charge transfer (ICT) states pre-existed in the dark and created as a consequence of Fermi level equilibrium at donor-acceptor interface have a profound effect on open circuit voltage in organic bulk heterojunction photovoltaics. ICT state formation causes vacuum level misalignment that yields a roughly constant effective donor ionization potential to acceptor electron affinity energy difference at the donor-acceptor interface, even though there is a large variation in electron affinity for the fullerene series. The large variation in open circuit voltage for the corresponding device series instead is found to be a consequence of trap-assisted recombination via integer charge transfer states. Based on the results, novel design rules for optimizing open circuit voltage and performance of organic bulk heterojunction solar cells are proposed.Doping and insertion of interlayer are two established methods for enhancing charge injection/extraction properties at organic-electrode interface. By studying the energy level alignment behavior at low to intermediate doping levels for molecule-doped conjugated polymer/electrode interfaces, we deduce that two combined processes govern the interface energetics: (i) equilibration of the Fermi level due to oxidation (or reduction) of polymer sites at the interface as per the ICT model and (ii) a double dipole step induced by image charge from the dopant-polymer charge transfer complex that causes a shift of the work function. Such behavior is expected to hold in general for low to intermediate level doped organic semiconductor systems. The unified model is further extended to be suitable for conjugated electrolyte/electrode interfaces, revealing the design rules for achieving the smallest charge injection/extraction barrier for both thin tunneling and thick charge transporting conjugated electrolyte interlayers.To probe into the energy level spatial extension at interfaces, we employ the original approach of building and characterizing multilayers composed of a well-defined number of polymer monolayers with the Langmuir-Shäfer method to control polymer film uniformity and thicknesses, avoiding the problems associated with spin-coating ultrathin films. The disordered/amorphous films feature smaller, and in fact negligible, energy level bending compared to the more well-ordered films, in contradiction with existing models. It is found that that energy level bending depends on the ICT state distribution rather than the density of states of the neutral polymer chains in relation to the Fermi energy, thus taking into account the Coulomb energy associated with charging the polymer chain and transferring a charge across the interface. Based on this work, a general model for energy level bending in absence of significant doping of conjugated polymer films is proposed.Organic semiconductors are sensitive to ambient atmosphere that can influence the energetics. The degradation effects of common PCBM film induced by oxygen and water are found to be completely different. Upon exposure to oxygen, the work function is down-shifted by ~ 0.15 eV compared to the ICT curve of the pristine PCBM film, originating from the weak interaction between the fullerene part of PCBM and oxygen, and this can be reversed by thermal treatment in vacuum. The down-shift in energetics will cause a loss in open circuit voltage at electrode interface, but aids free charge generation at donor-acceptor interface. Upon exposure to water, there is irreversible extensive broadening and bleaching of the valence electronic structure features as well as a substantial decrease of work function and ionization potential, severely degrading the transport properties.Overall, the research results in this thesis thus give a deeper understanding of interface phenomena in organic electronics, especially regard to organic solar cells, aimed to further improve the device operation efficiency and lifetime.
|
|
| 8. |
- Bao, Qinye, et al.
(författare)
-
Interfaces of (Ultra)thin Polymer Films in Organic Electronics
- 2019
-
Ingår i: Advanced Materials Interfaces. - : WILEY. - 2196-7350. ; 6:1
-
Forskningsöversikt (refereegranskat)abstract
- In this short review the energy level alignment of interfaces involving solution-processed conjugated polymer (and soluble small molecules) films is described. Some general material properties of conjugated polymers and their solution-processed films are introduced, and the basic physics involved in energy level alignment at their interfaces is then discussed. An overview of energy level bending in (ultra)thin conjugated polymer films (often referred to as "band bending") is given and the effects of ion-containing interlayers typically used in organic electronic devices such as polymer light emitting diodes and organic bulk heterojunction solar cells are explored. The review finishes by describing a few of the available computational models useful for predicting and/or modeling energy level alignment at interfaces of solution-processed polymer films and discusses their respective strengths and weaknesses.
|
|
| 9. |
- Bao, Qinye, et al.
(författare)
-
Oxygen- and Water-Based Degradation in [6,6]-Phenyl-C-61-Butyric Acid Methyl Ester (PCBM) Films
- 2014
-
Ingår i: Advanced Energy Materials. - : Wiley-VCH Verlag. - 1614-6832 .- 1614-6840. ; 4:6
-
Tidskriftsartikel (refereegranskat)abstract
- Effects of in situ oxygen/water exposure on the energetics of [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) films are presented. For oxygen exposure, the work function is downshifted by ≈0.15 eV compared to the ideal integer charge transfer (ICT) curve for pristine PCBM, which is incompatible with significant introduction of electron trap states or p-doping. Water induces the highest occupied molecular orbital (HOMO) structure to undergo strong, irreversible modifications accompanied by a chemical interaction with PCBM.
|
|
| 10. |
- Bao, Qinye, et al.
(författare)
-
Regular Energetics at Conjugated Electrolyte/Electrode Modifier for Organic Electronics and Their Implications of Design Rules
- 2015
-
Ingår i: Advanced Materials Interfaces. - : John Wiley & Sons. - 2196-7350. ; 2:12, s. 1-6
-
Tidskriftsartikel (refereegranskat)abstract
- Regular energetics at a conjugated electrolyte/electrode modifier are found and controlled by equilibration of the Fermi level and an additional interface double dipole step induced by ionic functionality. Based on the results, design rules for conjugated electrolyte/electrode modifiers to achieve the smallest charge injection/exaction barrier and break through the current thickness limitation are proposed.
|
|
