Colloidal cadmium selenide (CdSe) quantum dots (QDs) have been prepared and exploited as inorganic dyes to sensitize a large-band-gap TiO2 layer for QD-sensitized solar cells. The optimized QD-sensitized solar cells exhibited an unprecedented incident photon-to-charge carrier generation efficiency of 36% and an overall conversion efficiency of over 1.7% at 0.1 sun and 1% at full sun intensity with a cobalt(II/III)-based redox system. The photovoltaic characteristics of CdSe QD-sensitized cells are compared with standard dye-sensitized solar cells, in which the former exhibited about half of the efficiency of the latter. From the kinetics of charge transfer monitored using transient spectroscopic and voltage decay measurements in the CdSe QD-sensitized cell, the regeneration yield of oxidized QDs was found to be close to almost unity, and the electron lifetime was longer in the CdSe QD-sensitized cell than in the dye-sensitized solar cell.
Metal sulfide (PbS and CdS) quantum dots (QDs) were prepared over mesoporous TiO2 films by improved successive ionic layer adsorption and reaction (SILAR) processes. The as-prepared QD-sensitized electrodes were combined with a cobalt complex redox couple [Co(o-phen)3]2+/3+ to make a regenerative liquid-type photovoltaic cell. The optimized PbS QD-sensitized solar cells exhibited promising incident photon-to-current conversion efficiency (IPCE) of over 50% and an overall conversion efficiency of 2% at 0.1 sun in a regenerative mode. The overall photovoltaic performance of the PbS QD-sensitized cells was observed to be dependent on the final turn of the SILAR process, giving a better result when the final deposition was Pb2+, not S2-. However, in the case of CdS QD-sensitized cells, S2- termination was better than that of Cd2+. The cobalt complex herein used as a regenerative redox couple was found to be more efficient in generating photocurrents from PbS QD cells than the typical hole scavenger Na2S in a three-electrode configuration. The CdS-sensitized cell with this redox mediator also showed better defined current-voltage curves and an IPCE reaching 40%.
Synthesis of a size series of colloidal ZnTe/ZnSe (core/shell) quantum dots (QDs) is reported. Because of the unique Type-II characters, their emission can range over an extended wavelength regime, showing photoluminescence (PL) from blue to amber. The PL lifetime measures as long as 77 ns, which clearly indicates the Type-II characteristics. ZnTe/ZnSe (Core/Shell) QDs can be further passivated by ZnS layers, rendered in water, while preserving the optical and chemical stabilities and thus proved their potentials toward “nontoxic” biological or medical applications that are free from concerns regarding heavy-metal leakage. ZnTe/ZnSe Type-II QD/polymer hybrid organic solar cells are also showcased, promising environmentally friendly photovoltaic devices. ZnTe/ZnSe Type-II QD incorporated photovoltaic devices show 11 times higher power conversion efficiency, when compared to that of the control ZnSe QD devices. This results from the Type-II characteristic broad QD absorption up to extended wavelengths and the spatially separated Type-II excitons, which can enhance the carrier extractions. We believe that ZnTe/ZnSe-based Type-II band engineering can open many new possibilities as exploiting the safe material choice.
A model semiconductor-sensitizer layer of CdSe with under- or overlayers of CdS or ZnS by pre- or postadsorption was prepared on the surface of mesoporous TiO2 films by a series of successive ionic layer adsorption and reaction (SILAR) processes in solutions containing corresponding cations and anions. The growth of each semiconductor layer was monitored by taking UV−visible absorption spectra and high-resolution transmission electron microscopy (TEM) images. The all SILAR-prepared multicomponent sensitizer consisting of CdS/CdSe/ZnS layers was evaluated in a polysulfide electrolyte solution as a redox mediator in regenerative photoelectrochemical cells. The CdS and ZnS layers with the CdSe layer sandwiched in between were found to significantly enhance photocurrents. The best photovoltaic performance was obtained from the CdS/CdSe/ZnS-sensitizer with the ZnS layer on the top, yielding an overall power conversion efficiency of 3.44% with a mask around the active film and 3.90% with no mask. The effect of the mask on short-circuit current (J
sc) and overall efficiency (η) measurements was shown to be increasingly critical in semiconductor-sensitized solar cells as they exhibit high photocurrents. The polysulfide electrolyte, which acted as an effective electron transfer mediator for CdS and/or CdSe sensitizers, was not as effective for PbS-based sensitizers prepared by the same SILAR process.
The control over the precursor concentration is used to fabricate sensitized and thin-film perovskite solar cells. The dominating capacitance contributions in these devices reveal the main processes determining the response of perovskite solar cells, which enables the development of an impedance spectroscopy equivalent circuit for perovskite solar cells derived from the well-known circuit for sensitized devices. This tool can provide essential information for the photovoltaic performance in terms of transport and recombination processes.
Planar perovskite solar cells using low‐temperature atomic layer deposition (ALD) of the SnO2 electron transporting layer (ETL), with excellent electron extraction and hole‐blocking ability, offer significant advantages compared with high‐temperature deposition methods. The optical, chemical, and electrical properties of the ALD SnO2 layer and its influence on the device performance are investigated. It is found that surface passivation of SnO2 is essential to reduce charge recombination at the perovskite and ETL interface and show that the fabricated planar perovskite solar cells exhibit high reproducibility, stability, and power conversion efficiency of 20%.
A multilayer of CdSe quantum dots (QDs) was prepared on the mesoporous surface of a nanoparticulate TiO(2) film by a layer-by-layer (LBL) assembly using the electrostatic interaction of the oppositely charged QD surface for application as a sensitizer in QD-sensitized TiO(2) solar cells. To maximize the absorption of incident light and the generation of excitons by CdSe QDs within a fixed thickness of TiO(2) film, the experimental conditions of QD deposition were optimized by controlling the concentration of salt added into the QD-dissolved solutions and repeating the LBL deposition a few times. A proper concentration of salt was found to be critical in providing a deep penetration of QDs into the mesopore, thus leading to a dense and uniform distribution throughout the whole TiO(2) matrix while anchoring the oppositely charged QDs alternately in a controllable way. A series of post-treatments with (1) CdCl(2), (2) thermal annealing, and (3) ZnS-coating was found to be very critical in improving the overall photovoltaic properties, presumably through a better connection between QDs, effective passivation of QD's surface, and a high impedance of recombination, which were proved by transmission electron microscopy (TEM) and electrochemical impedance spectroscopy (EIS) experiments. With a proper post-treatment of multilayered QDs as a sensitizer, the overall power conversion efficiency in the CdSe QD-sensitized TiO(2) solar cells could reach 1.9% under standard illumination condition of simulated AM 1.5G (100 mW/cm(2)).
Novel quinoxaline-based organic sensitizers using vertical (RC-21) and horizontal (RC-22) conjugation between an electron-donating triphenylamine unit and electron-accepting quinoxaline unit have been synthesized and used for dye-sensitized solar cells (DSSCs), leading to the relatively high power conversion efficiencies of 3.30 and 5.56% for RC-21 and RC-22, respectively. This result indicates that the quinoxaline electron-accepting unit is quite a promising candidate in organic sensitizers.
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