Study of Quantum Dot/Inorganic Layer/Dye Molecule Sandwich Structure for Electrochemical Solar Cells

A highly efficient quantum dot (QD)/inorganic layer/dye molecule sandwich structure was designed and applied in electrochemical QD-sensitized solar cells. The key component TiO₂/CdS/ZnS/N719 hybrid photoanode with ZnS insertion between the two types of sensitizers was demonstrated not only to efficiently extend the light absorption but also to suppress the charge recombination from either TiO₂ or CdS QDs to electrolyte redox species, yielding a photocurrent density of 11.04 mA cm^–2, an open-circuit voltage of 713 mV, a fill factor of 0.559, and an impressive overall energy conversion efficiency of 4.4%. More importantly, the cell exhibited enhanced photostability with the help of the synergistic stabilizing effect of both the organic and the inorganic passivation layers in the presence of a corrosive electrolyte

Type-II Quantum-Dot-Sensitized Solar Cell Spanning the Visible and Near-Infrared Spectrum

Type-II heterostructure CdTe/CdSe core/shell nanocrystals (quantum dots, QDs) are explored as sensitizers in a QD-sensitized photoelectrochemical solar cell. These QDs comprise a hole-localizing core and an electron-localizing shell. Among their advantages is the significant red shift of the absorption edge of the heterostructured QD relative to its two constituents due to spatially indirect absorption leading to improved absorption characteristics, intraparticle exciton dissociation upon photoexcitation, and a relatively small content of the less abundant tellurium element. Upon incorporation in a sensitized solar cell utilizing a porous TiO₂ and a polysulfide electrolyte, these QDs exhibited efficient charge separation and high internal quantum efficiency despite hole localization in the CdTe core. Monochromatic incident photon-to-current conversion efficiency (IPCE) measurement shows a spectrally broad photoresponse spanning the whole visible spectrum and reaching up to ∼900 nm

Working from Both Sides: Composite Metallic Semitransparent Top Electrode for High Performance Perovskite Solar Cells

We report herein perovskite solar cells using solution-processed silver nanowires (AgNWs) as transparent top electrode with markedly enhanced device performance, as well as stability by evaporating an ultrathin transparent Au (UTA) layer beneath the spin-coated AgNWs forming a composite transparent metallic electrode. The interlayer serves as a physical separation sandwiched in between the perovskite/hole transporting material (HTM) active layer and the halide-reactive AgNWs top-electrode to prevent undesired electrode degradation and simultaneously functions to significantly promote ohmic contact. The as-fabricated semitransparent PSCs feature a <i>V</i>_oc of 0.96 V, a <i>J</i>_sc of 20.47 mA cm^–2, with an overall PCE of over 11% when measured with front illumination and a <i>V</i>_oc of 0.92 V, a <i>J</i>sc of 14.29 mA cm^–2, and an overall PCE of 7.53% with back illumination, corresponding to approximately 70% of the value under normal illumination conditions. The devices also demonstrate exceptional fabrication repeatability and air stability

Rational Design of Solution-Processed Ti–Fe–O Ternary Oxides for Efficient Planar CH₃NH₃PbI₃ Perovskite Solar Cells with Suppressed Hysteresis

Electron-extraction layer (EEL) plays a critical role in determining the charge extraction and the power conversion efficiencies of the organometal-halide perovskite solar cells (PSCs). In this work, Ti–Fe–O ternary oxides were first developed to work as an efficient EEL in planar PSC. Compared with the widely used TiO<i>_x</i> and the pure FeO<i>_x</i>, the ternary composites show superior properties in multiple aspects including the excellent stability of the precursor solution, good coverage on the substrates, outstanding electrical properties, and suitable energy levels. By varying the Fe content from 0 to 100% in the Ti–Fe–O composites, the conductivity of the resultant compact layer was markedly improved, confirmed by consistent results from the conductive atomic force microscopy and the linear sweep voltammetry measurements. Meanwhile, the compositional engineering tunes the energy level alignment of the Ti–Fe–O EEL/CH₃NH₃PbI₃ interface to a region that is favorable for obtaining excellent charge-extraction property. The combinational advantages of the Ti–Fe–O composites significantly improved the photovoltaic performance of the as-prepared solar cells. An increase of over 20% in the short-circuit current (<i>J</i>_SC) density has been achieved due to a modified EEL conductivity and energy alignment with the perovskite layer. The reduction in the surface recombination and enhancement of the charge collection efficiency also result in about 15% increase in the fill factor. Notably, the device also showed remarkably alleviated hysteresis behavior, revealing a prominently inhibited surface recombination

Aluminum-Doped Zinc Oxide as Highly Stable Electron Collection Layer for Perovskite Solar Cells

Although low-temperature, solution-processed zinc oxide (ZnO) has been widely adopted as the electron collection layer (ECL) in perovskite solar cells (PSCs) because of its simple synthesis and excellent electrical properties such as high charge mobility, the thermal stability of the perovskite films deposited atop ZnO layer remains as a major issue. Herein, we addressed this problem by employing aluminum-doped zinc oxide (AZO) as the ECL and obtained extraordinarily thermally stable perovskite layers. The improvement of the thermal stability was ascribed to diminish of the Lewis acid–base chemical reaction between perovskite and ECL. Notably, the outstanding transmittance and conductivity also render AZO layer as an ideal candidate for transparent conductive electrodes, which enables a simplified cell structure featuring glass/AZO/perovskite/Spiro-OMeTAD/Au. Optimization of the perovskite layer leads to an excellent and repeatable photovoltaic performance, with the champion cell exhibiting an open-circuit voltage (<i>V</i>_oc) of 0.94 V, a short-circuit current (<i>J</i>_sc) of 20.2 mA cm^–2, a fill factor (FF) of 0.67, and an overall power conversion efficiency (PCE) of 12.6% under standard 1 sun illumination. It was also revealed by steady-state and time-resolved photoluminescence that the AZO/perovskite interface resulted in less quenching than that between perovskite and hole transport material

Inverted Hysteresis in CH₃NH₃PbI₃ Solar Cells: Role of Stoichiometry and Band Alignment

J–V hysteresis in perovskite solar cells is known to be strongly dependent on many factors ranging from the cell structure to the preparation methods. Here we uncover one likely reason for such sensitivity by linking the stoichiometry in pure CH₃NH₃PbI₃ (MAPbI₃) perovskite cells with the character of their hysteresis behavior through the influence of internal band offsets. We present evidence indicating that in some cells the ion accumulation occurring at large forward biases causes a temporary and localized increase in recombination at the MAPbI₃/TiO₂ interface, leading to inverted hysteresis at fast scan rates. Numerical semiconductor models including ion accumulation are used to propose and analyze two possible origins for these localized recombination losses: one based on band bending and the other on an accumulation of ionic charge in the perovskite bulk

Light and Electrically Induced Phase Segregation and Its Impact on the Stability of Quadruple Cation High Bandgap Perovskite Solar Cells

Perovskite material with a bandgap of 1.7–1.8 eV is highly desirable for the top cell in a tandem configuration with a lower bandgap bottom cell, such as a silicon cell. This can be achieved by alloying iodide and bromide anions, but light-induced phase-segregation phenomena are often observed in perovskite films of this kind, with implications for solar cell efficiency. Here, we investigate light-induced phase segregation inside quadruple-cation perovskite material in a complete cell structure and find that the magnitude of this phenomenon is dependent on the operating condition of the solar cell. Under short-circuit and even maximum power point conditions, phase segregation is found to be negligible compared to the magnitude of segregation under open-circuit conditions. In accordance with the finding, perovskite cells based on quadruple-cation perovskite with 1.73 eV bandgap retain 94% of the original efficiency after 12 h operation at the maximum power point, while the cell only retains 82% of the original efficiency after 12 h operation at the open-circuit condition. This result highlights the need to have standard methods including light/dark and bias condition for testing the stability of perovskite solar cells. Additionally, phase segregation is observed when the cell was forward biased at 1.2 V in the dark, which indicates that photoexcitation is not required to induce phase segregation