Role of the Metal-Oxide Work Function on Photocurrent Generation in Hybrid Solar Cells
2018, Ehrenreich, Philipp, Wong, Ka Kan, Zimmermann, Eugen, Dorman, James A., Wang, Wei, Fakharuddin, Azhar, Putnik, Martin, Kalb, Julian, Pfadler, Thomas, Schmidt-Mende, Lukas
ZnO is a widely used metal-oxide semiconductor for photovoltaic application. In solar cell heterostructures they not only serve as a charge selective contact, but also act as electron acceptor. Although ZnO offers a suitable interface for exciton dissociation, charge separation efficiencies have stayed rather poor and conceptual differences to organic acceptors are rarely investigated. In this work, we employ Sn doping to ZnO nanowires in order to understand the role of defect and surface states in the charge separation process. Upon doping we are able to modify the metal-oxide work function and we show its direct correlation with the charge separation efficiency. For this purpose, we use the polymer poly(3-hexylthiophene) as donor and the squaraine dye SQ2 as interlayer. Interestingly, neither mobilities nor defects are prime performance limiting factor, but rather the density of available states around the conduction band is of crucial importance for hybrid interfaces. This work highlights crucial aspects to improve the charge generation process of metal-oxide based solar cells and reveals new strategies to improve the power conversion efficiency of hybrid solar cells.
Characterization of perovskite solar cells : towards a reliable measurement protocol
2016-08-19, Zimmermann, Eugen, Wong, Ka Kan, Müller, Michael, Hu, Hao, Ehrenreich, Philipp, Kohlstädt, Markus, Würfel, Uli, Mastroianni, Simone, Pfadler, Thomas, Schmidt-Mende, Lukas
Lead halide perovskite solar cells have shown a tremendous rise in power conversion efficiency with reported record efficiencies of over 20% making this material very promising as a low cost alternative to conventional inorganic solar cells. However, due to a differently severe “hysteretic” behaviour during current density-voltage measurements, which strongly depends on scan rate, device and measurement history, preparation method, device architecture, etc., commonly used solar cell measurements do not give reliable or even reproducible results. For the aspect of commercialization and the possibility to compare results of different devices among different laboratories, it is necessary to establish a measurement protocol which gives reproducible results. Therefore, we compare device characteristics derived from standard current density-voltage measurements with stabilized values obtained from an adaptive tracking of the maximum power point and the open circuit voltage as well as characteristics extracted from time resolved current density-voltage measurements. Our results provide insight into the challenges of a correct determination of device performance and propose a measurement protocol for a reliable characterisation which is easy to implement and has been tested on varying perovskite solar cells fabricated in different laboratories.
Erratum: Role of charge separation mechanism and local disorder at hybrid solar cell interfaces [Phys. Rev. B 91, 035304 (2015)]
2015, Ehrenreich, Philipp, Pfadler, Thomas, Paquin, Francis, Dion-Bertrand, Laura-Isabelle, Paré-Labrosse, Olivier, Silva, Carlos, Weickert, Jonas, Schmidt-Mende, Lukas
Toward High-Efficiency Solution-Processed Planar Heterojunction Sb2S3 Solar Cells
2015, Zimmermann, Eugen, Pfadler, Thomas, Kalb, Julian, Dorman, James A., Sommer, Daniel, Hahn, Giso, Weickert, Jonas, Schmidt-Mende, Lukas
Low-cost hybrid solar cells have made tremendous steps forward during the past decade owing to the implementation of extremely thin inorganic coatings as absorber layers, typically in combination with organic hole transporters. Using only extremely thin films of these absorbers reduces the requirement of single crystalline high-quality materials and paves the way for low-cost solution processing compatible with roll-to-roll fabrication processes. To date, the most efficient absorber material, except for the recently introduced organic–inorganic lead halide perovskites, has been Sb2S3, which can be implemented in hybrid photovoltaics using a simple chemical bath deposition. Current high-efficiency Sb2S3 devices utilize absorber coatings on nanostructured TiO2 electrodes in combination with polymeric hole transporters. This geometry has so far been the state of the art, even though flat junction devices would be conceptually simpler with the additional potential of higher open circuit voltages due to reduced charge carrier recombination. Besides, the role of the hole transporter is not completely clarified yet. In particular, additional photocurrent contribution from the polymers has not been directly shown, which points toward detrimental parasitic light absorption in the polymers. This study presents a fine-tuned chemical bath deposition method that allows fabricating solution-processed low-cost flat junction Sb2S3 solar cells with the highest open circuit voltage reported so far for chemical bath devices and efficiencies exceeding 4%. Characterization of back-illuminated solar cells in combination with transfer matrix-based simulations further allows to address the issue of absorption losses in the hole transport material and outline a pathway toward more efficient future devices.
Controlled Morphologies by Molecular Design and Nano-Imprint Lithography
2017, Pfadler, Thomas, Palumbiny, Claudia M., Pisula, Wojciech, Hesse, Holger C., Feng, Xinliang, Müllen, Klaus, Müller-Buschbaum, Peter, Schmidt-Mende, Lukas
In this review we report on the recent advances concerning molecular design and nano-imprint techniques to improve the morphology of organic solar cells. Advanced scattering techniques allow us to resolve issues pertaining to the alignment and crystallization of the photoactive materials of nanostructured solar cells. Interfacial design at a donor–acceptor heterojunction is one of the key issues for improved device performance.
Uniform Large-Area Free-Standing Silver Nanowire Arrays on Transparent Conducting Substrates
2016-06-14, Feng, Yuyi, Kim, Kwang-Dae, Nemitz, Clayton A., Kim, Paul, Pfadler, Thomas, Gerigk, Melanie, Polarz, Sebastian, Dorman, James A., Weickert, Jonas, Schmidt-Mende, Lukas
Arrays of silver nanowires have received increasing attention in a variety of applications such as surface-enhanced Raman scattering (SERS), plasmonic biosensing and electrode for photoelectric devices. However, until now, large scale fabrication of device-suitable silver nanowire arrays on supporting substrates has seen very limited success. Here we show the synthesis of free-standing silver nanowire arrays on indium-tin oxide (ITO) coated glass by pulsed electrodeposition into anodic aluminum oxide (AAO) templates. We use an in situ oxygen plasma cleaning process and a sputtered Ti layer to enhance the adhesion between the template and ITO glass. An ultrathin gold layer (2 nm) is deposited as a nucleation layer for the electrodeposition of silver. An unprecedented high level of uniformity and control of the nanowire diameter, spacing and length has been achieved. The absorption measurements show that the free-standing silver nanowire arrays possess tunable plasmonic resonances.
A comparison of light-coupling into high and low index nanostructured photovoltaic thin films
2015, Pfadler, Thomas, Stärk, Martin, Zimmermann, Eugen, Putnik, Martin, Boneberg, Johannes, Weickert, Jonas, Schmidt-Mende, Lukas
Periodically structured electrodes are typically introduced to thin-film photovoltaics for the purpose of light management. Highly effective light-trapping and optimal in-coupling of light is crucial to enhance the overall device performance in such thin-film systems. Here, wavelength-scale structures are transferred via direct laser interference patterning to electron-selective TiO2 electrodes. Two representative thin-film solar cell architectures are deposited on top: an organic solar cell featuring blended P3HT:PCBM as active material, and a hybrid solar cell with Sb2S3 as inorganic active material. A direct correlation in the asymmetry in total absorption enhancement and in structure-induced light in-coupling is spectroscopically observed for the two systems. The structuring is shown to be beneficial for the total absorption enhancement if a high n active material is deposited on TiO2, but detrimental for a low n material. The refractive indices of the employed materials are determined via spectroscopic ellipsometry. The study outlines that the macroscopic Fresnel equations can be used to investigate the spectroscopically observed asymmetry in light in-coupling at the nanostructured TiO2 active material interfaces by visualizing the difference in reflectivity caused by the asymmetry in refractive indices.
H-aggregate analysis of P3HT thin films-Capability and limitation of photoluminescence and UV/Vis spectroscopy
2016-09-01, Ehrenreich, Philipp, Birkhold, Susanne T., Zimmermann, Eugen, Hu, Hao, Kim, Kwang-Dae, Weickert, Jonas, Pfadler, Thomas, Schmidt-Mende, Lukas
Polymer morphology and aggregation play an essential role for efficient charge carrier transport and charge separation in polymer-based electronic devices. It is a common method to apply the H-aggregate model to UV/Vis or photoluminescence spectra in order to analyze polymer aggregation. In this work we present strategies to obtain reliable and conclusive information on polymer aggregation and morphology based on the application of an H-aggregate analysis on UV/Vis and photoluminescence spectra. We demonstrate, with P3HT as model system, that thickness dependent reflection behavior can lead to misinterpretation of UV/Vis spectra within the H-aggregate model. Values for the exciton bandwidth can deviate by a factor of two for polymer thicknesses below 150 nm. In contrast, photoluminescence spectra are found to be a reliable basis for characterization of polymer aggregation due to their weaker dependence on the wavelength dependent refractive index of the polymer. We demonstrate this by studying the influence of surface characteristics on polymer aggregation for spin-coated thin-films that are commonly used in organic and hybrid solar cells.
Structure-induced resonant tail-state regime absorption in polymer : fullerene bulk-heterojunction solar cells
2016-05-18, Pfadler, Thomas, Kiel, Thomas, Stärk, Martin, Werra, Julia F. M., Matyssek, Christian, Sommer, Daniel, Boneberg, Johannes, Busch, Kurt, Weickert, Jonas, Schmidt-Mende, Lukas
In this work, we present resonant tail-state regime absorption enhanced organic photovoltaics. We combine periodically structured TiO2 bottom electrodes with P3HT-PCBM bulk-heterojunction solar cells in an inverted device configuration. The wavelength-scale patterns are transferred to the electron-selective bottom electrodes via direct laser interference patterning, a fast method compatible with roll-to-roll processing. Spectroscopic and optoelectronic device measurements suggest polarization-dependent absorption enhancement along with photocurrent generation unambiguously originating from the population of tail states. We discuss the effects underlying these absorption patterns with the help of electromagnetic simulations using the discontinuous Galerkin time domain method. For this, we focus on the total absorption spectra along with spatially resolved power loss densities. Our simulations stress the tunability of the absorption resonances towards arbitrary wavelength regions.
Decoupling optical and electronic optimization of organic solar cells using high-performance temperature-stable TiO2/Ag/TiO2 electrodes
2015, Kim, Kwang-Dae, Pfadler, Thomas, Zimmermann, Eugen, Feng, Yuyi, Dorman, James A., Weickert, Jonas, Schmidt-Mende, Lukas
An electrode structured with a TiO2/Ag/TiO2 (TAT) multilayer as indium tin oxide (ITO) replacement with a superior thermal stability has been successfully fabricated. This electrode allows to directly tune the optical cavity mode towards maximized photocurrent generation by varying the thickness of the layers in the sandwich structure. This enables tailored optimization of the transparent electrode for different organic thin film photovoltaics without alteration of their electro-optical properties. Organic photovoltaic featuring our TAT multilayer shows an improvement of ∼12% over the ITO reference and allows power conversion efficiencies (PCEs) up to 8.7% in PTB7:PC71BM devices.