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Abstract:

Electron donors and acceptors in organic solar cells (OSCs) shall strike a favorable vertical phase separation that acceptors and donors have sufficient contact and gradient accumulation near the cathodes and anodes, respectively. Random mixing of donors/acceptors at surface will result in charge accumulation and severe recombination for low carrier-mobility organic materials. However, it is challenging to tune the vertical distribution in bulk-heterojunction films as they are usually made from a well-mixed donor/acceptor solution. Here, for the first time, it presents with solid evidence that the commonly used 1-chloronaphthalene (CN) additive can tune the donor/acceptor vertical distribution and establish the mechanism. Different from the previous understanding that ascribed the efficiency enhancement brought by CN to the improved molecular stacking/crystallization, it is revealed that the induced vertical distribution is the dominant factor leading to the significantly increased performance. Importantly, the vertical distribution tunability is effective in various hot nonfullerene OSC systems and creates more channels for the collection of dissociated carriers at corresponding organic/electrode interfaces, which contributes the high efficiency of 18.29%. This study of the material vertical distribution and its correlation with molecular stacking offers methods for additives selection and provides insights for the understanding and construction of high-performance OSCs.

Abstract:

<jats:title>Abstract</jats:title> <jats:p>A correct determination of voltage losses is crucial for the development of organic solar cells (OSCs) with improved performance. This requires an in-depth understanding of the properties of interfacial charge transfer (CT) states, which not only set the upper limit for the open-circuit voltage of a system, but also govern radiative and non-radiative recombination processes. Over the last decade, different approaches have emerged to classify voltage losses in OSCs that rely on a generic detailed balance approach or additionally include CT state parameters that are specific to OSCs. In the latter case, a correct determination of CT state properties is paramount. In this work, we summarize the different frameworks used today to calculate voltage losses and provide an in-depth discussion of the currently most important models used to characterize CT state properties from absorption and emission data of organic thin films and solar cells. We also address practical concerns during the data recording, analysis, and fitting process. Departing from the classical two-state Marcus theory approach, we discuss the importance of quantized molecular vibrations and energetic hybridization effects in organic donor-acceptor systems with the goal to providing the reader with a detailed understanding of when each model is most appropriate.</jats:p>

Abstract:

Copper(I) thiocyanate (CuSCN) is an effective interlayer material for hole injection and transport in organic electronic devices but its solution processing has conventionally utilized undesirable di-n-alkyl sulfide solvents such as diethyl- (DES) and dipropyl-sulfide (DPS). Herein, this paper reports on the use of N,N-dimethylformamide (DMF) and 1-methyl-2-pyrrolidinone (NMP) as alternative solvents for CuSCN interlayers and performs a detailed comparison of the resulting properties relative to films processed from DES and DPS and two other recent alternatives, dimethyl sulfoxide (DMSO) and ammonium hydroxide. The surface roughness, polymorphism, and surface chemistry of the resulting CuSCN layers are reported. The interlayer surface energy and ionization potential that are key to the overlying semiconductor microstructure and interfacial energy barrier, and hence to charge transport and injection, are also discussed. Finally, systematic device tests using well-known organic semiconductors in light-emitting diode, solar cell and field-effect transistor structures demonstrate the overall suitability of DMSO and DMF as solvents for CuSCN interlayer deposition to achieve better device performance. This study broadens the applicability of CuSCN as a highly efficient hole injection/transport material for organic semiconductor devices by expanding the documented range of suitable CuSCN solvents.

Abstract:

This contains all data used in the paper: ACS Energy Lett. 2022, 7, 7, 2311–2322, DOI: https://doi.org/10.1021/acsenergylett.2c01094. Data has been sorted into raw and processed, and organised by which figure they appear in. Arrays require Python and the numpy package to load (np.load('filename.npy')). All other data is in text format of some form, easily openable. Some plots require Origin labs to open, but no data in these files are inaccessible from the txt files/ csvs etc.

Abstract:

Vacuum-thermal evaporation (VTE) is a highly relevant fabrication route for organic solar cells (OSCs), especially on an industrial scale as proven by the commercialisation of organic light emitting diode (OLED) based displays. While OSC performance is reported for a range of VTE-deposited molecules, a comprehensive assessment of donor:acceptor blend properties with respect to their photovoltaic performance is scarce. Here, we fabricate organic thin films and solar cells of three select systems and measure ellipsometry, external quantum efficiency with high dynamic range, as well as OTRACE to quantify absorption, voltage losses, and charge carrier mobility. These parameters are key to explain OSC performance and will help to rationalize the performance of other material systems reported in literature as our methodology is applicable beyond VTE systems. Furthermore, it could help to judge the prospects of new molecules in general. We find large differences in the measured values and find that today's VTE OSCs can reach high extinction coefficients, but only moderate mobility and voltage loss compared to their solution-processed counterparts. We outline what needs to improve for VTE organic solar cells to again catch up with their solution-processed counterparts in terms of power conversion efficiency. This article is protected by copyright. All rights reserved.