High-performance lab-scale perovskite solar cells often have a precious metal as the top electrode. However, there are drawbacks to using metal top electrodes on a large scale, such as inducing ...degradation processes, requiring a high-temperature deposition process under vacuum, and having low scalability. Recently many studies have shown the potentials of using a carbon electrode because of its conductivity, flexibility, low cost, and ease of fabrication. This review article presents an overview of using carbon materials to replace the top electrode in perovskite photovoltaics. We discuss various fabrication techniques, various carbon-based device structures, and the advantages of using carbon materials. A collection of research works on device performance, large-scale fabrication, and device stability is presented. As a result, this review offers insight into the future of large-scale flexible solar cells.
To analyze the dominant recombination, researchers often consider the diode ideality factor (nid), determined from the fitting of a semi‐log plot of light intensity–dependent open‐circuit voltage ...(Voc(lnI/I0)) to a linear dependence. This value is called “nid,Voc”. Theoretically, nid is the exponential dependence factor in the recombination rate function of the split of quasi‐Fermi levels. This nid is called “nid,C”. Herein, correlations between nid,Voc, nid,C, and the dominant recombination are reconsidered using a validated numerical drift–diffusion model and a diode current analysis in perovskite solar cell devices having accumulations of charged defects near the carrier transporting interfaces. It is found that the interplay between the recombination processes affects the linearity of the Voc(lnI/I0) plots. Devices having a single dominant recombination process exhibit Voc(lnI/I0) plots that appear to be linear, resulting in nid,Voc ≈ nid,C of the dominant recombination. Conversely, bends in the Voc(lnI/I0) curves indicate that different (multiple) recombination mechanisms dominate at different light intensities, so nid,Voc is an effective nid of the total diode current whose value is not consistent with any nid,C values. This work provides more understanding of nid and how to interpret a Voc(lnI/I0) curve more correctly for the insights into recombination mechanisms.
In planar perovskite solar cell devices having accumulations of charged ions near the interfaces, the interpretation of the diode ideality factor values extracted from light intensity–dependent open‐circuit voltage curves for the dominant recombination process is revisited by comparing the ideality factor values with the values calculated from recombination rates as a function of the local quasi‐Fermi level splitting.
Posttreatment of titanium oxide (TiO2) using lithium (Li) and cobalt (Co) precursors is widely adopted to modify the charge quenching property in perovskite solar cells (PSCs); however, the ...fundamental understanding of the effect of the modification layer on the material itself and, consequently, the photovoltaic performance stability is not complete. In this work, in situ X‐ray diffraction measurements show that the Li and Co ions can diffuse into TiO2 and consequently accelerate the rutile phase transformation. X‐ray photoelectron spectroscopy results reveal the appearance of a Ti3+ feature in both the Li‐ and Co‐treated samples, suggesting that the treatment ions are partially located at the subsurface/surface of the spin‐cast TiO2 layer. The Li‐treated TiO2 exhibits greatly upshifted conduction band edges, which benefits charge extraction properties and improves the average device parameters in a complete PSC. To complement the experiments, density functional theory calculations are performed. While Li treatment initially results in enhanced electronic properties, Li‐treated TiO2 tends to have more surface vacancies over time and is more susceptible to adsorption and accumulation of iodide ions compared to the Co‐treated sample, which is experimentally supported by surface photovoltage spectroscopy and time‐resolved photoluminescence results.
Photovoltaic materials are impacted by the photoinduced charge separation behavior, which can be further improved by modifying the underlying layer that the perovskite is prepared on top of. The impacts of using alkali salts on porous TiO2 from experimental and computational points of view are investigated to understand such surface passivation of a solar cell device.
Photovoltaic Performance Stability
The most fundamental properties of photovoltaic materials are impacted by the photoinduced charge separation behavior, which can be improved by modifying the ...underlying layer that the perovskite is prepared on top. In article number 2201632, Non Thongprong, Nopporn Rujisamphan, and colleagues investigate the impacts of using alkali salts on porous TiO2 from experimental and computational points of view to provide a better understanding of such surface passivation.
An understanding of the spectrum–property relationship of perovskite solar cells when illuminated by light‐emitting diodes that are used for indoor applications is necessary. Herein, it is aimed to ...explore the influences of correlated‐color temperatures on a MAPbI3‐based device under low‐light conditions. Given an irradiance of approximately 3 W m−2 (or ≈1000 lx), a maximum free carrier generation rate of 1.0 × 1021 m−3 s−1 was found. Additionally, power conversion efficiencies (PCEs) up to 31.97%, 30.36%, and 28.98% with maximum power outputs of 13.66, 13.02, and 16.09 μW could be reached at 3000, 4000, and 6500 K, respectively. Additional increases in the PCEs were observed when high‐energy blue light (in a range of 400–550 nm) was excluded during the current–voltage sweeps. In combination with the surface photovoltage measurements, intense blue light (under 6500 K) had a minimal influence on the photoinduced charge separation signals when compared to those caused by 3000 and 4000 K light. As a solar cell, the PCE reached as high as 34.52%, which corresponded to 73.08% of the thermodynamic limit of its bandgap at 3000 K.
Herein, the impacts of the correlated‐color temperatures (CCTs) of LEDs on a single‐cation perovskite material MAPbI3 are highlighted. Based on the irradiant spectrum, an emphasis is placed on the theoretical prediction of the free carrier generation rate and maximum current density as a function of the CCT.
Passivating electron‐transporting layers (ETLs) with alkali salts have demonstrated a facial approach that is essential in healing defective surfaces, consequently improving the functionality and ...stability of perovskite‐based solar cells (PSCs). Herein, the pseudohalide salt of sodium tetrafluoroborate, whose anions have a higher electronegativity than other halide salts (i.e., iodide and chloride), with the potential to passivate the surface of tin oxide while enhancing the optoelectronic properties of a perovskite film, is presented. Meanwhile, the density functional theory calculations show that BF4−/F− ions exhibit a robust ionic interaction with an uncoordinated Sn4+ site. In contrast, the Na ion is bound to an oxygen atom of the OH− group, which helps reduce surface defect states and improves charge transfer properties. Thus, the best PSC exhibits a current density of 23.51 mA cm−2, an open‐circuit voltage of 1.10 V, and an excellent fill factor of 80.48, providing an efficiency of 20.82%, which exceeds that of a control device (18.38%). Importantly, the retention of the power conversion efficiency on NaBF4‐based PSCs without encapsulation is 18.44% after 1000 h of aging under ambient conditions, whereas the retention of a control device is only 16.08%.
The use of sodium tetrafluoroborate as the surface passivator of tin oxide electron‐transporting layer to improve the performance and stability of perovskite‐based solar cells is demonstrated. With NaBF4 treatment, defects on the SnO2 surface are alleviated, resulting in a considerably lower trap density at the SnO2 perovskite interfaces; consequently, the charge extraction properties are enhanced.
Abstract
Posttreatment of titanium oxide (TiO
2
) using lithium (Li) and cobalt (Co) precursors is widely adopted to modify the charge quenching property in perovskite solar cells (PSCs); however, ...the fundamental understanding of the effect of the modification layer on the material itself and, consequently, the photovoltaic performance stability is not complete. In this work, in situ X‐ray diffraction measurements show that the Li and Co ions can diffuse into TiO
2
and consequently accelerate the rutile phase transformation. X‐ray photoelectron spectroscopy results reveal the appearance of a Ti
3+
feature in both the Li‐ and Co‐treated samples, suggesting that the treatment ions are partially located at the subsurface/surface of the spin‐cast TiO
2
layer. The Li‐treated TiO
2
exhibits greatly upshifted conduction band edges, which benefits charge extraction properties and improves the average device parameters in a complete PSC. To complement the experiments, density functional theory calculations are performed. While Li treatment initially results in enhanced electronic properties, Li‐treated TiO
2
tends to have more surface vacancies over time and is more susceptible to adsorption and accumulation of iodide ions compared to the Co‐treated sample, which is experimentally supported by surface photovoltage spectroscopy and time‐resolved photoluminescence results.
Organic photovoltaics (OPVs) and perovskite solar cells are emerging classes of solar cell that are promising for clean energy alternatives to fossil fuels. Understanding fundamental physics of these ...materials is crucial for improving their energy conversion efficiencies and promoting them to practical applications. Current density-voltage (JV) curves; which are important indicators of OPV efficiency, have direct connections to many fundamental properties of solar cells. They can be described by the Shockley diode equation, resulting in fitting parameters; series and parallel resistance (Rs and Rp), diode saturation current ( J0) and ideality factor (n). However, the Shockley equation was developed specifically for inorganic p-n junction diodes, so it lacks physical meanings when it is applied to OPVs. Hence, the puRposes of this work are to understand the fundamental physics of OPVs and to develop new diode equations in the same form as the Shockley equation that are based on OPV physics. We develop a numerical drift-diffusion simulation model to study bilayer OPVs, which will be called the drift-diffusion for bilayer interface (DD-BI) model. The model solves Poisson, drift-diffusion and current-continuity equations self-consistently for charge densities and potential profiles of a bilayer device with an organic heterojunction interface described by the GWWF model. We also derive new diode equations that have JV curves consistent with the DD-BI model and thus will be called self-consistent diode (SCD) equations. Using the DD-BI and the SCD model allows us to understand working principles of bilayer OPVs and physical definitions of the Shockley parameters. Due to low carrier mobilities in OPVs, space charge accumulation is common especially near the interface and electrodes. Hence, quasi-Fermi levels (i.e. chemical potentials), which depend on charge densities, are modified around the interface, resulting in a splitting of quasi-Fermi levels that works as a driving potential for the heterojunction diode. This brings about the meaning of R s as the resistance that gives rise to the diode voltage equal to the interface quasi-Fermi level splitting instead of the voltage between the electrodes. Quasi-Fermi levels that drop near the electrodes because of unmatched electrode work functions or due to charge injection can also increase Rs. Furthermore, we are able to study dissociation and recombination rates of bound charge pairs across the interface (i.e. polaron pairs or PPs) and arrive at the physical meaning of Rp as recombination resistance of PPs. In the dark, PP density is very low, so Rp is possibly caused by a tunneling leakage current at the interface. Ideality factors are parameters that depend on the split of quasi-Fermi levels and the ratio of recombination rate to recombination rate at equilibrium. Even though they are related to trap characteristics as normally understood, their relations are complicated and careful inte Rpretations of fitted ideality factors are needed. Our models are successfully applied to actual devices, and useful physics can be deduced, for example differences between the Shockley parameters under dark and illumination conditions. Another puRpose of this thesis is to study electronic properties of CsSnBr3 perovskite and processes of growing the perovskite film using an epitaxy technique. Calculation results using density functional theory reveal that a CsSnBr3 film that is grown on a NaCl(100) substrate can undergo a phase transition to CsSn 2Br5, which is a wide-bandgap semiconductor material. Actual mechanisms of the transition and the interface between CsSnBr3 and CsSn2Br5are interesting for future studies.