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Low temperature solution combustion synthesis emerges as a facile method for synthesis of functional metal oxides thin films for electronic applications. We study the solution combustion synthesis process of Cu:NiOx using different molar ratios (w/o, 0.1 and 1.5) of fuel acetylacetone (Acac) to oxidizer (Cu, Ni Nitrates) as a function of thermal annealing tempera-tures 150, 200 and 300 oC. The solution combustion synthesis process, in both thin films and bulk Cu:NiOx, is investigated. Thermal analysis studies using TGA and DTA reveal that the Cu:NiOx thin films show a more gradual mass loss while the bulk Cu:NiOx exhibits a distinct combustion process. The thin films can crystallize to Cu:NiOx at annealing temperature of 300 oC irrespective to the Acac/Oxidizer ratio whereas lower annealing temperatures (150 and 200 oC) produce amorphous materials. A detail characterization study of solution combustion synthesized Cu:NiOx including XPS, UV-Vis, AFM and Contact angle measurements is presented. Finally, 50 nm Cu:NiOx thin films are introduced as HTLs within the inverted perovskite solar cell device architecture. The Cu:NiOx HTL annealed at 150 and 200 oC provided PVSCs with limited functionality whereas efficient triple-cation Cs0.04(MA0.17FA0.83)0.96 Pb(I0.83Br0.17)3 based PVSCs achieved for Cu:NiOx HTLs annealed at temperature 300 oC., Comment: 16 pages, 13 figures

This study outlines the synthesis and physicochemical characteristics of a solution-processable iron manganite (FeMnO3) nanoparticles via a chemical combustion method using tartartic acid as a fuel and demonstrates the performance of this material as a n-type photoactive layer in all-oxide solar cells. It is shown that the solution combustion synthesis (SCS) method enables the formation of pure crystal phase FeMnO3 with controllable particle size. XRD pattern and morphology images from TEM confirm the purity of FeMnO3 phase and the relative small crystallite size (~13 nm), firstly reported in the literature. Moreover, to assemble a network of connected FeMnO3 nanoparticles, \b{eta}-alanine was used as a capping agent and dimethylformamide (DMF) as a polar aprotic solvent for the colloidal dispersion of FeMnO3 NPs. This procedure yields a ~500 nm thick photoactive layer. The proposed method is crucial to obtain functional solution processed NiO/FeMnO3 heterojunction inorganic photovoltaics. The optoelectronic properties of the heterojunction were established. These solar cells demonstrate a high open circuit voltage of 1.31 V with sufficient fill factor of 54.3% and low short circuit current of 0.07 mA cm-2 delivering a power conversion efficiency of 0.05% under 100 mW cm-2 illumination. This work expands on the burgeoning of environmentally friendly, low-cost, sustainable solar cell material that derive from metal oxides., Comment: 19 pages, 8 figures

The performance of solution-processed organic light emitting diodes (OLEDs) is often limited by non-uniform contacts. In this work, we introduce Ni-containing solution-processed metal oxide (MO) interfacial layers inserted between indium tin oxide (ITO) and poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) to improve the bottom electrode contact for OLEDs using the poly(p-phenylene vinylene) (PPV) derivative Super-Yellow (SY) as an emission layer. For ITO/Ni-containing MO/PEDOT:PSS bottom electrode structures we show enhanced wetting properties that result in an improved OLED device efficiency. Best performance is achieved using a Cu-Li co-doped spinel nickel cobaltite [(Cu-Li):NiCo2O4], for which the current efficiency and luminous efficacy of SY OLEDs increased, respectively, by 12% and 11% from the values obtained for standard devices without a Ni-containing MO interface modification between ITO and PEDOT:PSS. The enhanced performance was attributed to the improved morphology of PEDOT:PSS, which consequently increased the hole injection capability of the optimized ITO/(Cu-Li):NiCo2O4/PEDOT:PSS electrode., Comment: 15 pages, 9 figures

Inverted perovskite solar cells (PSCs) using a Cu:NiOx hole transporting layer (HTL) often exhibit stability issues and in some cases J/V hysteresis. In this work, we developed a \b{eta}-alanine surface treatment process on Cu:NiOx HTL that provides J/V hysteresis-free, highly efficient, and thermally stable inverted PSCs. The improved device performance due to \b{eta}-alanine-treated Cu:NiOx HTL is attributed to the formation of an intimate Cu:NiOx/perovskite interface and reduced charge trap density in the bulk perovskite active layer. The \b{eta}-alanine surface treatment process on Cu:NiOx HTL eliminates major thermal degradation mechanisms, providing 40 times increased lifetime performance under accelerated heat lifetime conditions. By using the proposed surface treatment, we report optimized devices with high power conversion efficiency (PCE) (up to 15.51%) and up to 1000 h lifetime under accelerated heat lifetime conditions (60 C, N2)., Comment: 20 pages, 12 figures

We show that the addition of 1 % (v/v) nitrobenzene within the perovskite formulation can be used as a method to improve the power conversion efficiency and reliability performance of methylammonium-free (CsFA) inverted perovskite solar cells. Addition of nitrobenzene increased PCE due to defect passivation and provides smoother films resulting in PVSCs with narrower PCE distribution. Moreover, the nitrobenzene additive methylammonium-free hybrid PVSCs exhibit prolonged lifetime compare to additive free PVSCs due to enhanced air and moisture degradation resistance., Comment: 18 pages, 9 figures

Solution processed {\gamma}-Fe2O3 nanoparticles via the solvothermal colloidal synthesis in conjunction with ligand-exchange method are used for interface modification of the top electrode in inverted perovskite solar cells. In comparison to more conventional top electrodes such as PC(70)BM/Al and PC(70)BM/AZO/Al, we show that incorporation of a {\gamma}-Fe2O3 provides an alternative solution processed top electrode (PC(70)BM/{\gamma}-Fe2O3/Al) that not only results in comparable power conversion efficiencies but also improved thermal stability of inverted perovskite photovoltaics. The origin of improved stability of inverted perovskite solar cells incorporating PC(70)BM/ {\gamma}-Fe2O3/Al under accelerated heat lifetime conditions is attributed to the acidic surface nature of {\gamma}-Fe2O3 and reduced charge trapped density within PC(70)BM/ {\gamma}-Fe2O3/Al top electrode interfaces., Comment: 24 pages, 11 figures

We have demonstrated a high-performance low temperature solution processed electron selective contact consisting of 10 at% antimony doped tin oxide (ATO) and the neutral polymer polyethylenimine (PEI). Inverted organic photovoltaics (OPVs) utilizing ATO/PEI as electron selective contact exhibited high power conversion efficiencies for both the reference P3HT: PCBM and the non-fullerene based P3HT- IDTBR active layer OPV material systems. Importantly it is shown that the proposed ATO/PEI carrier selective contact provides light soaking-free inverted OPVs. Furthermore, by increasing the thickness of ATO layer from 40 to 120 nm the power conversion efficiency of the corresponding inverted OPVs remain unaffected a parameter which indicates the potential of the proposed ATO/PEI carrier selective contact for high performance light-soaking-free and reliable roll-to-roll printing solutions processed inverted OPVs., Comment: 20 pages, 4 figures, 2 tables

Solution combustion synthesized hole transport layer of co-doped spinel nickel cobaltite were fabricated using doctor-blading technique for planar inverted perovskite solar cells. Perovskite solar cells incorporating Co-doped spinel nickel cobaltite shown an increase in device performance parameters compared to un-doped spinel nickel cobaltite, leading to PCE of 16.5%. X-ray photoelectron spectroscopy measurements revealed the tendency of Cu cations to replace preferably the surface Ni atoms changing the surface stoichiometry of spinel nickel cobaltite inducing a cathodic polarization. Ultraviolet photoelectron spectroscopy measurements unveiled the increase of the ionization potential by 0.1 eV for co-doped spinel nickel cobaltite film compare to undoped spinel nickel cobaltite-based hole transporting layer. We attribute the enhanced PCE of inverted perovskite solar cells presented due to improved hole extraction properties of co-doped spinel nickel cobaltite hole transporting layer., Comment: 27 pages,12 figures

In this article, the stability of p-i-n perovskite solar cells is studied under accelerated heat lifetime conditions (60 oC ,85oC and N2 atmosphere). By using a combination of buffer layer engineering, impedance spectroscopy and other characterization techniques, we propose the interaction of the perovskite active layer with the top Al metal electrode through diffusion mechanisms as the major thermal degradation pathway for planar inverted perovskite photovoltaics (PVs) under 85oC heat conditions. We show that by using thick solution processed fullerene buffer layer the perovskite active layer can be isolated from the top metal electrode and improve the lifetime performance of the inverted perovskite photovoltaics at 85 oC. Finally, we present an optimized solution processed inverted perovskite PV device using thick fullerene-based diffusion blocking layer with over 1000 hours accelerated heat lifetime performance at 60oC.

We present the functionalization process of a conductive and transparent copper aluminum oxide, copper oxide alloy. The copper aluminum oxide, copper oxide powders were developed by flame spray pyrolysis and their stabilized dispersions were treated by sonication and centrifugation methods. We show that when the supernatant part of the treated copper aluminum oxide, copper oxide dispersions is used for the development of hole transporting layers the corresponding inverted perovskite solar cells show improved functionality and power conversion efficiency with negligible hysteresis effect., Comment: 39 pages, 18 figures

The charge accumulation properties of p-i-n perovskite solar cells were investigated using three representative organic and inorganic hole transporting layer (HTLs): a) Poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate) (PEDOT:PSS, Al 4083), b) copper-doped nickel oxide (Cu:NiOx) and c) Copper oxide (CuO). Through impedance spectroscopy analysis and modelling it is shown that charge accumulation is decreased in the HTL/Perovskite interface, between PEDOT:PSS to Cu:NiOx and CuO respectively. This was indicative from the decrease in double layer capacitance (Cdl) and interfacial charge accumulation capacitance (Cel), resulting in an increase to recombination resistance (Rrec), thus decreased charge recombination events between the three HTLs. Through AFM measurements it is also shown that the reduced recombination events (followed by the increase in Rrec) is also a result of increased grain size between the three HTLs, thus reduction in the grain boundaries area. These charge accumulation properties of the three HTLs have resulted in an increase to the power conversion efficiency between the PEDOT:PSS (8.44%), Cu:NiOx (11.45%) and CuO (15.3%)-based devices.

High power conversion efficiency (PCE) inverted organic photovoltaics (OPVs) usually use thermally evaporated MoO3 as a hole transporting layer (HTL). Despite the high PCE values reported, stability investigations are still limited and the exact degradation mechanisms of inverted OPVs using thermally evaporated MoO3 HTL remain unclear under different environmental stress factors. In this study, we monitor the accelerated lifetime performance of non-encapsulated inverted OPVs using thiophene-based active layer materials and evaporated MoO3 under the ISOS D-2 protocol (heat conditions 65 {\deg}C). The investigation of degradation mechanisms presented focus on optimized P3HT:PC[70]BM-based inverted OPVs. Specifically, we present a systematic study on the thermal stability of inverted P3HT:PC[70]BM OPVs using solution processed PEDOT:PSS and evaporated MoO3 HTL. Using a series of measurements and reverse engineering methods we report that the P3HT:PC[70]BM/MoO3 interface is the main origin of failure of P3HT:PC[70]BM-based inverted OPVs under intense heat conditions.

We present a solvothermal synthetic route to produce monodispersed CuO nanoparticles (NPs) in the range of 5-10 nm that can be used as hole selective interfacial layer between indium tin oxide (ITO) and perovskite active layer for p-i-n perovskite solar cells by a spin casting the dispersions at room temperature. The bottom electrode interface modification provided by spherical CuO-NPs at room temperature promotes the formation of high quality perovskite photoactive layers with large crystal size and strong optical absorption. Furthermore, it is shown that the nanoparticulate nature of the CuO hole transporting interfacial layer can be used to improve light manipulation within perovskite solar cell device structure. The corresponding p-i-n CH3NH3PbI3-based solar cells show high Voc values of 1.09 V, which is significantly higher compared to the Voc values obtained with conventional PEDOT:PSS hole selective contact based perovskite solar cells.

In the present study, we report the synthesis and characterization of a low-temperature solution-processable monodispersed nickel cobaltite (NiCo2O4) nanoparticles via a combustion synthesis using tartaric acid as fuel and demonstrate its performance as hole transport layer (HTL) for Perovskite Solar Cells (PVSCs). NiCo2O4 is a p-type semiconductor consisting of environmentally friendly, abundant elements and higher conductivity compared to NiO. We show that the combustion synthesis of spinel NiCo2O4 using tartaric acid as fuel can be used to control the NPs size and provide smooth, compact and homogeneous functional HTLs processed by blade coating. Study of PVSCs with different NiCo2O4 thickness as HTL reveal a difference on hole extraction efficiency and for 15 nm optimized thickness enhanced hole carrier collection is achieved. As a result, p-i-n structure of PVSCs with 15 nm NiCo2O4 HTLs showed reliable performance and power conversion efficiency values in the range of 15.5 % with negligible hysteresis.

We investigate the employment of carefully selected solvent additives in the processing of a commercial perovskite precursor ink and analyze their impact on the performance of organometal trihalide perovskite photovoltaic devices. We provide evidence that the use of benzaldehyde can be used as an effective method to preserve the stoichiometry of the perovskite precursors in solution. Benzaldehyde based additive engineering shows to improve perovskite solid state film morphology and device performance of trihalide perovskite based solar cells.

Delafossites like CuGaO2 have appeared as promising p-type semiconductor materials for opto-electronic applications mainly due to their high optical transparency and electrical conductivity. However, existing synthetic efforts usually result in particles with large diameter limiting their performance relevant to functional electronic applications. In this article, we report a novel surfactant-assisted hydrothermal synthesis method, which allows the development of ultrafine (~5 nm) monodispersed p-type CuGaO2 nanoparticles (NPs). We show that DMSO can be used as a ligand and dispersing solvent for stabilizing the CuGaO2 NPs. The resulting dispersion is used for the fabrication of dense, compact functional CuGaO2 electronic layer with properties relevant to advanced optoelectronic applications. As a proof of concept, the surfactant-assisted hydrothermal synthesized CuGaO2 is incorporated as a hole transporting layer (HTL) in the inverted p-i-n perovskite solar cell device architecture providing improved hole carrier selectivity and power conversion efficiency compared to conventional PEDOT:PSS HTL based perovskite solar cells.

A detailed investigation of the functionality of inverted organic photovoltaics (OPVs) using bare Ag contacts as top electrode is presented. The inverted OPVs without hole transporting layer (HTL) exhibit a significant gain in hole carrier selectivity and power conversion efficiency (PCE) after exposure in ambient conditions. Inverted OPVs comprised of ITO/ZnO/poly(3-hexylthiophene-2,5-diyl):phenyl-C61-butyric acid methyl ester (P3HT:PCBM)/Ag demonstrate over 3.5% power conversion efficiency only if the devices are exposed in air for over 4 days. As concluded through a series of measurements, the oxygen presence is essential to obtain fully operational solar cell devices without HTL. Moreover, accelerated stability tests under damp heat conditions (RH=85% and T=65oC) performed to non-encapsulated OPVs demonstrate that HTL-free inverted OPVs exhibit comparable stability to the reference inverted OPVs. Importantly, it is shown that bare Ag top electrodes can be efficiently used in inverted OPVs using various high performance polymer:fullerene bulk heterojunction material systems demonstrating 6.5% power conversion efficiencies.

Perovskite photovoltaics (PVs) have attracted attention because of their excellent power conversion efficiency (PCE). Critical issues related to large area PV performance, reliability and lifetime need to be addressed. Here, we show that doped metal oxides can provide ideal electron selectivity, improved reliability and stability for perovskite PVs. We report p-i-n perovskite PVs with device areas ranging from 0.09cm2 to 0.5cm2 incorporating a thick aluminum doped zinc oxide (AZO) electron selective contact with hysteresis-free PCE of over 13% and high fill factor values in the range of 80%. AZO provides suitable energy levels for carrier selectivity, neutralizes the presence of pinholes and provides intimate interfaces. Devices using AZO exhibit an average PCE increase of over 20% compared with the devices without AZO and maintain the high PCE for the larger area devices reported. Furthermore, the device stability of p-i-n perovskite solar cells under the ISOS-D-1 is enhanced when AZO is used, and maintains 100% of the initial PCE for over 1000 hours of exposure when AZO/Au is used as the top electrode. Our results indicate the importance of doped metal oxides as carrier selective contacts to achieve reliable and high performance long lived large area perovskite solar cells.

We present the results of XPS measurements (core levels and valence bands) of solution processed TiOx thin films prepared from titanium butoxide (C16H36O4Ti) diluted in isopropanol which is a common sol-gel route for fabricating TiOx electron selective contacts for ITO/TiOx inverted organic photovoltaics bottom electrodes. XPS Ti 2p and valence band spectra show the presence of additional features which are absent in spectra of titanium butoxide deposited on Si and are attributed to appearance of Ti^{3+} valence states in ITO/TiOx. This conclusion is confirmed by density functional theory electronic structure calculations of stoichiometric TiO2 and oxygen deficient TiO_{2-1/8}. XPS C 1s measurements show the formation of C-O and O-C=O bonds which evidence the presence of residual carbon which can draw oxygen from the film network and induce the formation of fraction of Ti3+ states in TiOx films.