Synthesis and Characterization of Transition Metal Oxides and Dichalcogenides and Their Application in Organic Photovoltaics
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This Ph.D. research focused on the development of new materials for alternative renewable energy using organic photovoltaics (OPVs). The first step was to established reliable fabrication and characterization methods of organic photovoltaic devices. The reproducibility of organic photovoltaic cell performance is one of the essential issues that must be achieved before engaging serious investigations of the applications of creative and challenging ideas. Secondly, we thoroughly studied the surface chemistry of the underlying layer and its critical role on the morphology of the BHJ active layer. We showed that when the active layer (which consists of blends of poly(3-hexylthiophene) (P3HT) and phenyl-C60-butyric acid methyl ester (PCBM)) is deposited and annealed over a sol-gel ZnO electron transport layer surface made from monoethanolamine (MEA) containing precursor, PCBM clusters form during annealing and this phase segregation leads to a drastic reduction of OPV parameters due to both low charge generation and high bimolecular recombination. Rinsing the pyrolyzed ZnO films with solvents or using a ZnO recipe without MEA significantly reduced the formation of PCBM clusters and produced devices with good performance. Third, we developed new materials suitable for low-temperature processing and large-area deposition methods to be used as transport layer on OPVs. We achieved the synthesis of MoOx suspensions suitable for large area deposition, with controlled size, stoichiometry, and electronic properties using controlled oxidative dissolution of organometallic powders with H2O2 in n-butanol. The small nanoparticle diameters of ~ 2 nm enabled solution processing of nanoparticle films on ITO with electronic properties comparable to solution processed and vacuum deposited counterparts, without the need for any post processing. We also accomplished the synthesis of transition metal dichalcogenides (TMDs) directly from precursors in solution using a versatile synthesis method. We demonstrate the ability to synthesize few-layer (~ 2 nm) MoS2, MoSe2, WS2, and WSe2 flakes with relatively large lateral sizes (> 2 µm) using a solvothermal method. We demonstrate that the reducing agent, 1,2-hexadecanediol is critical to ensure TMD formation and eliminate corresponding metal oxide. TEM, Raman, PESA, and Kelvin Probe measurements confirmed that all TMDs are p-type, highly crystalline, exhibit 2H phase and present hexagonal crystalline structure. In addition, thickness for all TMDs was consistent with a few-layer flakes. Finally, we studied the use of films spray casted from liquid-exfoliated MoS2 suspensions as hole transport layer for OPVs. Electrical measurements on the devices showed that FF achieved using MoS2 is identical to that using spin-coated polymeric reference material. Calculations showed that the lower Jsc observed in MoS2 devices is explained by reduced light absorption in the active layer region due to less back-reflected light in MoS2 devices. With all these results we have contributed to enable a route towards low-cost OPV and other electronics fabrication.