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Organic photovoltaics devices typically utilize illumination through a transparent substrate, such as glass or an optically clear plastic. Utilization of opaque substrates, including low cost foils, papers, and textiles, requires architectures that instead allow illumination through the top of the device. Here, we demonstrate top-illuminated organic photovoltaics, employing a dry vapor-printed poly(3,4-ethylenedioxythiophene) (PEDOT) polymer anode deposited by oxidative chemical vapor deposition (oCVD) on top of a small-molecule organic heterojunction based on vacuum-evaporated tetraphenyldibenzoperiflanthene (DBP) and C60 heterojunctions. Application of a molybdenum trioxide (MoO3) buffer layer prior to oCVD deposition increases the device photocurrent nearly 10 times by preventing oxidation of the underlying photoactive DBP electron donor layer during the oCVD PEDOT deposition, and resulting in power conversion efficiencies of up to 2.8% for the top-illuminated, ITO-free devices, approximately 75% that of the conventional cell architecture with indium-tin oxide (ITO) transparent anode (3.7%). Finally, we demonstrate the broad applicability of this architecture by fabricating devices on a variety of opaque surfaces, including common paper products with over 2.0% power conversion efficiency, the highest to date on such fiber-based substrates.

For the successful integration of graphene as a transparent conducting electrode in organic solar cells, proper energy level alignment at the interface between the graphene and the adjacent organic layer is critical. The role of a hole transporting layer (HTL) thus becomes more significant due to the generally lower work function of graphene compared to ITO. A commonly used HTL material with ITO anodes is poly(3,4-ethylenedioxythiophene) (PEDOT) with poly(styrenesulfonate) (PSS) as the solid-state dopant. However, graphene's hydrophobic surface renders uniform coverage of PEDOT:PSS (aqueous solution) by spin-casting very challenging. Here, we introduce a novel, yet simple, vapor printing method for creating patterned HTL PEDOT layers directly onto the graphene surface. Vapor printing represents the implementation of shadow masking in combination with oxidative chemical vapor deposition (oCVD). The oCVD method was developed for the formation of blanket (i.e., unpatterened) layers of pure PEDOT (i.e., no PSS) with systematically variable work function. In the unmasked regions, vapor printing produces complete, uniform, smooth layers of pure PEDOT over graphene. Graphene electrodes were synthesized under low-pressure chemical vapor deposition (LPCVD) using a copper catalyst. The use of another electron donor material, tetraphenyldibenzoperiflanthene, instead of copper phthalocyanine in the organic solar cells also improves the power conversion efficiency. With the vapor printed HTL, the devices using graphene electrodes yield comparable performances to the ITO reference devices (η(p,LPCVD) = 3.01%, and η(p,ITO) = 3.20%).

We demonstrate series-integrated multijunction organic photovoltaics fabricated monolithically by vapor-deposition in a transposed subcell order with the near-infrared-absorbing subcell in front of the green-absorbing subcell. This transposed subcell order is enabled by the highly complementary absorption spectra of a near-infrared-absorbing visibly-transparent subcell and a visible-absorbing subcell and motivated by the non-spatially-uniform optical intensity in nanoscale photovoltaics. The subcell order and thicknesses are optimized via transfer-matrix formalism and short-circuit current simulations. An efficient charge recombination zone consisting of layers of BCP/Ag/MoOx leads to negligible voltage and series-resistance losses. Under 1-sun illumination the multijunction solar cells exhibit a power conversion efficiency of 5.5 ± 0.2% with an FF of 0.685 ± 0.002 and a V(OC) of 1.65 ± 0.02 V, corresponding to the sum of the V(OC) of the component subcells. These devices exhibit a broad spectral response (in the wavelength range of 350 nm to 850 nm) but are limited by subcell external quantum efficiencies between 20% and 30% over the photoactive spectrum.

We demonstrate efficient zinc sulfide cathode window layers in thin-film organic photovoltaics enabled by n-type doping zinc sulfide (ZnS) with aluminum sulfide (Al2S3) directly through co-deposition. By optimizing the Al2S3 concentration, the power conversion efficiency is improved from 0.6% ± 0.2% in undoped ZnS window layer devices to 1.8% ± 0.1%, identical to control devices. The mechanism for this performance enhancement is shown to stem from the enhanced conductivity and interface energetics of ZnS upon n-type doping. This work expands the catalog of efficient, inorganic, non-toxic, cathode side window layers that could be effective in a range of thin-film photovoltaic technologies.

Integration of transparent photovoltaics into the building envelope creates unique opportunities to reduce the levelized electricity cost of solar power. However, this integration warrants consideration of the angular dependence of these devices as illumination around the building envelope is rarely at normal incidence. Here we correctly update transfer-matrix and equations to accurately model the quantum efficiency and optical properties under oblique illumination. We use this model to demonstrate the various angular performance characteristics possible for proof-of-concept optimizations of transparent planar-heterojunction solar cells and discuss considerations needed to fully account for optical, electrical, and positional configurations in this optimization.

Vacuum and solution processed versions of poly(3,4-ethylenedioxythiophene) (PEDOT) are used as cathode interlayers in inverted organic photovoltaic cells comprising tetraphenyldibenzoperiflanthene as the electron donor and C60 as the electron acceptor. Chemical treatment of the as-deposited PEDOT layers with tetrakis(dimethylamino)ethylene or cesium carbonate reduces the work function by up to 0.8 eV. Inserting these PEDOT layers at the indium tin oxide cathode results in improved electron collection and efficiencies of up to 2.3 ± 0.2%, approaching the 3.2 ± 0.3% of the conventional device. This illustrates the potential for efficient polymer cathode materials and inverted device architectures compatible with either solution or vacuum processing.