Cheng-Min Tsai

Control of preferred orientation with slow crystallization for carbon-based mesoscopic perovskite solar cells attaining efficiency 15%

To produce mesoscopic carbon-electrode-based solar cells free of a hole-conduction layer, we developed a simple one-step drop-cast method (temperature 20 °C, relative humidity 50%) to grow uniform and compact perovskite nanocrystals via slow crystallization (SC). X-ray diffraction (XRD) results indicated that perovskite nanocrystals produced inside the mesoporous TiO2/Al2O3/C layers according to our SC approach with N-methyl-2-pyrrolidone (NMP) as a precursor solvent showed a preferred orientation at facet (004) with large crystalline grains, whereas those produced with other solvents or via thermal annealing (TA) methods showed greater intensity at facet (220) with small crystals. After the SC (NMP) procedure was completed, additional TA treatment would change the preferred orientation from (004) back to facet (220), which would break the connectivity and lose the uniformity of the crystals, causing the grains to become significantly smaller. Transient photoluminescence (PL) decay profiles of the SC devices made with four precursor solvents, NMP, γ-butyrolactone (GBL), dimethylformamide (DMF) and dimethyl sulfoxide (DMSO), were recorded to show the trend of charge separation kinetics of the perovskite crystals inside the mesoporous films, which is consistent with the trend of the corresponding device performance showing the same order. The SC (NMP) device attained the best efficiency of power conversion (PCE), 15.0%, with average value (13.9 ± 0.5%), which is much superior to those devices from either the traditional one-step TA (DMF) method (5.2 ± 1.0%) or the traditional sequential TA method (10.1 ± 0.7%). This work emphasizes the significance of the control of preferred orientation of perovskite nanocrystals using the SC approach, to obtain high-performance carbon-based mesoscopic solar cells with excellent reproducibility and stability.

Formation of Stable Tin Perovskites Co‐crystallized with Three Halides for Carbon‐Based Mesoscopic Lead‐Free Perovskite Solar Cells

We synthesized and characterized methylammonium (MA) mixed tri-halide tin perovskites (MASnIBr2-x Clx ) for carbon-based mesoscopic solar cells free of lead and hole-transporting layers. Varied SnCl2 /SnBr2 ratios yielded tin perovskites with three halides (I, Br, and Cl) co-crystallized inside the tin-perovskite. When the SnCl2 proportion was ≥50 % (x≥1), phase separation occurred to give MASnI3-y Bry and MASnCl3-z Brz in the stoichiometric proportions of their precursors, confirmed by XRD. A device with MASnIBr1.8 Cl0.2 (SnCl2 =10 %) showed the best photovoltaic performance: JSC =14.0 mA cm-2 , VOC =380 mV, FF=0.573, and PCE=3.1 %, and long-term stability. Electrochemical impedance spectra (EIS) show superior charge recombination and dielectric relaxation properties for the MASnIBr1.8 Cl0.2 cell. Transient PL decays showed the intrinsic problem of tin-based perovskites with average lifetimes less than 100 ps.

Interfacial Investigation on Printable Carbon-Based Mesoscopic Perovskite Solar Cells with NiOx/C Back Electrode

Solar cells with high efficiency, low cost, and high stability are the target for the new generation of solar cells. A fully printable perovskite (CH3NH3PbI3) solar cell (PSC) with device architecture FTO/TiO2/Al2O3/NiOx/C is fabricated in the current research as a low-cost and relatively stable structure and is investigated to determine how different fabrication factors such as the thickness of the insulating spacer layer (Al2O3) or treatments such as heat and UV-O3 treatments can affect the interfacial properties of this multilayer mesoporous structure. X-ray photoelectron spectra (XPS) show that UV-O3 treatment increases the Ni3+(Ni2O3) phase on the surface of the black nickel oxide layer leading to better charge extraction and increasing open-circuit voltage (VOC) up to 0.945 V. We observe improved CH3NH3PbI3 formation inside the mesoporous layers by the PbI2 penetration at a higher temperature. Impedance spectral together with current-voltage measurements show the effect of thickness for the insulator layer in the internal and interfacial resistances and photovoltaic characteristics of the cell. The best performance of the carbon-based PSC attains power conversion efficiency of 12.1% with the thickness of the Al2O3 layer at 450 nm.

Interfacial Engineering with Cross-Linkable Fullerene Derivatives for High-Performance Perovskite Solar Cells

Two fullerene derivatives with styryl and oxetane cross-linking groups served as interfacial materials to modify an electron-transporting layer (ETL) of TiO2, doped with Au nanoparticles, processed under low-temperature conditions to improve the performance of perovskite solar cells (PSC). The cross-linkable [6,6]-phenyl-C61-butyric styryl dendron ester was produced via thermal treatment at 160 °C for 20 min, whereas the cross-linkable [6,6]-phenyl-C61-butyric oxetane dendron ester (C-PCBOD) was obtained via UV-curing treatment for 45 s. Both cross-linked fullerenes can passivate surface-trap states of TiO2 and have also excellent surface coverage on the TiO2 layer shown in the corresponding atomic force microscopy images. To improve the crystallinity of perovskite, we propose a simple co-solvent method involving mixing dimethylformamide (DMF) and dimethyl sulfoxide (DMSO) in a specific ratio (DMF/DMSO = 90/10). The fullerene derivative layer between the ETL and perovskite layers significantly improved electron extraction and suppressed charge recombination by decreasing the density of traps at the ETL surface. A planar PSC device was fabricated with the configuration indium tin oxide/TiO2 (Au)/C-PCBOD/perovskite/spiro-OMeTAD/Au to attain a power conversion efficiency (PCE) of 15.9%. The device performance was optimized with C-PCBOD as an interfacial mediate to modify the surface of the mesoporous TiO2 ETL; the C-PCBOD-treated device attained a significantly enhanced performance, PCE 18.3%. Electrochemical impedance spectral and photoluminescence decay measurements were carried out to understand the characteristics of electron transfer and charge recombination of the perovskite/TiO2 samples with and without a fullerene interfacial layer.

Low-temperature, simple and efficient preparation of perovskite solar cells using Lewis bases urea and thiourea as additives: stimulating large grain growth and providing a PCE up to 18.8%

We demonstrated that two Lewis bases – urea and thiourea – acted as efficient additives for CH3NH3(MA)PbI3−xClx and MAPbI3 perovskite solar cells (PSCs) and observed a significant increase in PCE for the MAPbI3 devices in the presence of 1% urea with a remarkable PCE of 18.8% using an extremely low annealing temperature (85 °C).