The past two decades of vigorous interdisciplinary approaches has seen tremendous breakthroughs in both scientific and technological developments of bulk-heterojunction organic solar cells (OSCs) based on nanocomposites of π-conjugated organic semiconductors. Because of their unique functionalities, the OSC field is expected to enable innovative photovoltaic applications that can be difficult to achieve using traditional inorganic solar cells: OSCs are printable, portable, wearable, disposable, biocompatible, and attachable to curved surfaces. The ultimate objective of this field is to develop cost-effective, stable, and high-performance photovoltaic modules fabricated on large-area flexible plastic substrates via high-volume/throughput roll-to-roll printing processing and thus achieve the practical implementation of OSCs. Recently, intensive research efforts into the development of organic materials, processing techniques, interface engineering, and device architectures have led to a remarkable improvement in power conversion efficiencies, exceeding 11%, which has finally brought OSCs close to commercialization. Current research interests are expanding from academic to industrial viewpoints to improve device stability and compatibility with large-scale printing processes, which must be addressed to realize viable applications. Here, both academic and industrial issues are reviewed by highlighting historically monumental research results and recent state-of-the-art progress in OSCs. Moreover, perspectives on five core technologies that affect the realization of the practical use of OSCs are presented, including device efficiency, device stability, flexible and transparent electrodes, module designs, and printing techniques.

Bulk-Heterojunction Organic Solar Cells: Five Core Technologies for Their Commercialization.

The need for the development of transparent conductive electrodes (TCEs) supported on flexible polymer substrates has explosively increased in response to flexible polymer-based photovoltaic and display technologies; these TCEs replace conventional indium tin oxide (ITO) that exhibits poor performance on heat-sensitive polymers. An efficient, flexible TCE is required to exhibit high electrical conductance and high optical transmittance, as well as excellent mechanical flexibility and long-term stability, simultaneously. Recent advances in technologies utilizing an ultrathin noble-metal film in a dielectric/metal/dielectric structure, or its derivatives, have attracted attention as promising alternatives that can satisfy the requirements of flexible TCEs. This review will survey the background knowledge and recent updates of synthetic strategies and design rules toward highly efficient, flexible TCEs based on ultrathin metal films, with a special focus on the principal features and available methodologies involved in the fabrication of highly transparent, conductive, ultrathin noble-metal films. This survey will also cover the practical applications of TCEs to flexible organic solar cells and light-emitting diodes.

Ultrathin Metal films for Transparent Electrodes of Flexible Optoelectronic Devices

An effective method for depositing highly transparent and conductive ultrathin silver (Ag) electrodes using minimal oxidation is reported. The minimal oxidation of Ag layers signifi cantly improves the intrinsic optical and structural properties of Ag without any degradation of its electrical conductivity. Oxygen-doped Ag (AgO x ) layers of thicknesses as low as 6 nm exhibit completely 2D and continuous morphologies on ZnO fi lms, smaller optical refl ections and absorbances, and smaller sheet resistances compared with those of discontinuous and granular-type Ag layers of the same thickness. A ZnO/AgO x /ZnO (ZAOZ) electrode using an AgO x (O/Ag = 3.4 at%) layer deposited on polyethylene terephthalate substrates at room temperature shows an average transmittance of 91%, with a maximum transmittance of 95%, over spectral range 4001000 nm and a sheet resistance of 20 Ω sq 1 . The average transmittance value is increased by about 18% on replacing a conventional ZnO/Ag/ZnO (ZAZ) electrode with the ZAOZ electrode. The ZAOZ electrode is a promising bottom transparent conducting electrode for highly fl exible inverted organic solar cells (IOSCs), and it achieves a power conversion effi ciency (PCE) of 6.34%, whereas an IOSC using the ZAZ electrode exhibits a much lower PCE of 5.65%.

Transparent Ultrathin Oxygen-Doped Silver Electrodes for Flexible Organic Solar Cells

Advances in flexible optoelectronic devices have led to an increasing need for developing highly efficient, low-cost, flexible transparent conducting electrodes. Copper-based electrodes have been unattainable due to the relatively low optical transmission and poor oxidation resistance of copper. Here, we report the synthesis of a completely continuous, smooth copper ultra-thin film via limited copper oxidation with a trace amount of oxygen. The weakly oxidized copper thin film sandwiched between zinc oxide films exhibits good optoelectrical performance (an average transmittance of 83% over the visible spectral range of 400-800 nm and a sheet resistance of 9 Ω sq(-1)) and strong oxidation resistance. These values surpass those previously reported for copper-based electrodes; further, the record power conversion efficiency of 7.5% makes it clear that the use of an oxidized copper-based transparent electrode on a polymer substrate can provide an effective solution for the fabrication of flexible organic solar cells.

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Stable ultrathin partially oxidized copper film electrode for highly efficient flexible solar cells.

Transparent heat regulating (THR) materials and coatings for energy saving window applications: Impact of materials design, micro-structural, and interface quality on the THR performance

ZnO/Cu/ZnO multilayer structures are obtained with the highest conductivity of dielectric-metal-dielectric films reported in literature with a carrier concentration of 1.2×1022 cm−3 and resistivity of 6.9×10−5 Ω-cm at the optimum copper layer thickness. The peak transmittance, photopic averaged transmittance, and Haacke figure of merit are 88%, 75%, and 8.7×10−3 Ω−1, respectively. The conduction mechanism involves metal to oxide carrier injection prior to the formation of a continuous metal conduction pathway. Optical transmission is elucidated in terms of copper’s absorption due to d-band to Fermi surface transitions at short wavelengths and reflectance combined with scattering losses at long wavelengths.

Metallic conductivity and the role of copper in ZnO/Cu/ZnO thin films for flexible electronics

Gold-embedded zinc oxide structures are obtained in which the conduction mechanism changes from conduction through the oxide and activated tunneling between discontinuous metal islands to metallic conduction through a near-continuous layer, with increase in gold thickness. These structures can show resistivity as low as 5.2×10−5 Ω cm. Optical transmission is elucidated in terms of gold’s absorption due to interband electronic transitions, and free carrier absorption losses combined with limitation of the mean free path in discontinuous nanoparticles. The structures show transmittance, photopic averaged transmittance, and Haacke figure of merit values of 93%, 84%, and 15.1×10−3 Ω−1, respectively.

Conduction and transmission analysis in gold nanolayers embedded in zinc oxide for flexible electronics

ZnO/Cu/ZnO multilayer structures with very high conductivity have been obtained by magnetron sputtering. The Hall resistivity of the films was as low as 6.9×10−5 Ω-cm with a carrier concentration of 1.2×1022 cm−3 at the optimum copper layer thickness. The conduction mechanism has been explained in terms of metal to oxide carrier injection at low copper thickness and metal layer conduction at higher Cu thicknesses. The peak transmittance of the films is 88% and the photopic averaged transmittance is 75%. Optical transmission behavior of the films involves absorption by copper due to d-band to Fermi-surface transitions at short wavelengths and reflectance combined with scattering losses at long wavelengths. A Burstein–Moss shift in the band gap of the films is seen to take place with increase in thickness of the copper layer. The Haacke figure of merit has been calculated for the films with the best value being 8.7×10−3 Ω−1. Pole figure results reveal that the copper midlayer acts as a hindrance to (002) Zn...

K. Sivaramakrishnan

Papers

Metallic conductivity and the role of copper in ZnO/Cu/ZnO thin films for flexible electronics

Conduction and transmission analysis in gold nanolayers embedded in zinc oxide for flexible electronics

The role of copper in ZnO/Cu/ZnO thin films for flexible electronics

The effect of sputtering pressure on electrical, optical and structure properties of indium tin oxide on glass

The properties of radio frequency sputtered transparent and conducting ZnO:F films on polyethylene naphthalate substrate