Publication date: 21st July 2025
Transparent conductive electrodes (TCEs) are critical materials that exhibit a unique combination of low sheet resistance and high optical transparency, making them indispensable in optoelectronic applications. In this work, we optimize a three-layered transparent electrode commonly known as ZAZ (ZnO/AgNW/ZnO) fabricated using simple and straightforward spin coating method (Fig. 1a). The bottom ZnO layer is deposited to overcome the problem of adhesion on glass substrate and top ZnO layer is used to decrease the surface roughness of AgNW which causes the short circuit of electrode when it used in optoelectronic devices. We present a detailed optimization of the ZAZ system compared to ITO, investigating the impact of spin speed, AgNW concentration, thermal annealing conditions and effect of pyridine deposition on individual layer of the ZAZ structure. The initially fabricated ZAZ electrode exhibits transmittance (T) of 83.55% measured by UV-Visible spectrophotometer with sheet resistance (Rsh) of 17.90 Ω/Sq measured by 4-Probe , while ITO shows T= 77.33% and Rsh = 6.85 Ω/Sq at wavelength of 550 nm. The Hackee figure of merit (FoM), typically characterizes the efficiency of electrode is calculated for ITO and ZAZ electrode which is 11.16x10-3 and 9.26x10-3 Ω-1 respectively. Crucially, we systematically investigated the effect of pyridine deposition on individual layers of the ZAZ structure and found that applying it specifically to the top ZnO layer (ZnO/AgNW(2K,1K,60Sec)/ZnO/Pyridine) resulted in a significantly reduced sheet resistance of 13.13 Ω/Sq, while maintaining high transmittance (88.27%) with FoM of 21.69x10-3 Ω-1 and bi-layer of pyridine above AgNW and top ZnO layer(ZnO/AgNW/Pyridine/ZnO/Pyridine) have transmittance (88.50%) and Rsh of 17.33 Ω/Sq with FoM OF 17 x 10-3 Ω-1 at 550 nm which is superior as compared to ITO (Fig. 1b,c). Atomic Force Microscopy (AFM) and Scanning electron Microscopy (SEM) analysis confirmed reduced surface roughness, the surface RMS roughness decreased from 10.41 to 7.16 nm by pyridine coating, improved surface and cross-sectional uniformity in the optimized ZAZ electrode. Long term stability tests revealed the performance retention over 3 months in an open environment. To establish the practical viability of ZAZ electrodes, we fabricated and evaluated organic solar cells employing a donor: acceptor polymer blend (PM6:Y12) (Fig.1d), comparing their performance with conventional devices utilizing indium tin oxide (ITO) as the transparent electrode. The ITO-based reference device, with an active layer thickness of 100 nm, demonstrated a power conversion efficiency (PCE) of 13.22%, characterized by an open-circuit voltage (Voc) of 0.77 V, a short-circuit current density (Jsc) of 25.88 mA/cm², and a fill factor (FF) of 66%. In comparison, the ZAZ-based device, incorporating a thicker active layer of 240 nm, achieved a PCE of 9.25%, with a slightly higher Voc of 0.80 V, Jsc of 19.98 mA/cm², and FF of 58% (Fig. 1e,f). Although the ZAZ device exhibited moderately reduced current density and fill factor, its overall performance remained competitive, especially considering the increased active layer thickness and alternative electrode architecture. These results confirm that the ZAZ electrode structure, comprising a random network of silver nanowires embedded between zinc oxide layers and functionalized via targeted pyridine modification can effectively replace ITO without a significant loss in device efficiency. The solution-processable, low-cost fabrication methods used for ZAZ electrodes, along with their compatibility with scalable deposition techniques, highlight their promise as a sustainable and practical alternative for next-generation optoelectronic applications.
1.This work benefits from a French government grant managed by the French National Research Agency (ANR) under the reference « ANR-22-PEHY-0005 »
2. This work was supported by the PLATINOM platform. We would like to thank Nicolas Parou, Sebastian Rouigher, Romain Lafont, Nicolas R and Lionel Rechignat for their technical assistance regarding physical deposition methods, electrical and optical spectroscopies along with the characterization.