Unraveling the High Open Circuit Voltage and High Performance of Integrated Perovskite/Organic Bulk-Heterojunction Solar Cells.

We have demonstrated high-performance integrated perovskite/bulk-heterojunction (BHJ) solar cells due to the low carrier recombination velocity, high open circuit voltage (VOC), and increased light absorption ability in near-infrared (NIR) region of integrated devices. In particular, we find that the VOC of the integrated devices is dominated by (or pinned to) the perovskite cells, not the organic photovoltaic cells. A Quasi-Fermi Level Pinning Model was proposed to understand the working mechanism and the origin of the VOC of the integrated perovskite/BHJ solar cell, which following that of the perovskite solar cell and is much higher than that of the low bandgap polymer based organic BHJ solar cell. Evidence for the model was enhanced by examining the charge carrier behavior and photovoltaic behavior of the integrated devices under illumination of monochromatic light-emitting diodes at different characteristic wavelength. This finding shall pave an interesting possibility for integrated photovoltaic devices to harvest low energy photons in NIR region and further improve the current density without sacrificing VOC, thus providing new opportunities and significant implications for future industry applications of this kind of integrated solar cells.

Working Mechanism for Flexible Perovskite Solar Cells with Simplified Architecture.

In this communication, we report an efficient and flexible perovskite solar cell based on formamidinium lead trihalide (FAPbI3) with simplified configuration. The device achieved a champion efficiency of 12.70%, utilizing direct contact between metallic indium tin oxide (ITO) electrode and perovskite absorber. The underlying working mechanism is proposed subsequently, via a systematic investigation focusing on the heterojunction within this device. A significant charge storage has been observed in the perovskite, which is believed to generate photovoltage and serves as the driving force for charge transferring from the absorber to ITO electrode as well. More importantly, this simplified device structure on flexible substrates suggests its compatibility for scale-up fabrication, which paves the way for commercialization of perovskite photovoltaic technology.

Integrated perovskite/bulk-heterojunction toward efficient solar cells.

We successfully demonstrated an integrated perovskite/bulk-heterojunction (BHJ) photovoltaic device for efficient light harvesting and energy conversion. Our device efficiently integrated two photovoltaic layers, namely a perovskite film and organic BHJ film, into the device. The device structure is ITO/TiO2/perovskite/BHJ/MoO3/Ag. A wide bandgap small molecule DOR3T-TBDT was used as donor in the BHJ film, and a power conversion efficiency (PCE) of 14.3% was achieved in the integrated device with a high short circuit current density (JSC) of 21.2 mA cm(-2). The higher JSC as compared to that of the traditional perovskite/HTL (hole transporting layer) device (19.3 mA cm(-2)) indicates that the BHJ film absorbs light and contributes to the current density of the device. Our result further suggests that the HTL in traditional perovskite solar cell, even with good light absorption capability, cannot contribute to the overall device photocurrent, unless this HTL becomes a BHJ layer (by adding electron transporting material like PC71BM).

Multifunctional Fullerene Derivative for Interface Engineering in Perovskite Solar Cells.

In perovskite based planar heterojunction solar cells, the interface between the TiO2 compact layer and the perovskite film is critical for high photovoltaic performance. The deep trap states on the TiO2 surface induce several challenging issues, such as charge recombination loss and poor stability etc. To solve the problems, we synthesized a triblock fullerene derivative (PCBB-2CN-2C8) via rational molecular design for interface engineering in the perovskite solar cells. Modifying the TiO2 surface with the compound significantly improves charge extraction from the perovskite layer. Together with its uplifted surface work function, open circuit voltage and fill factor are dramatically increased from 0.99 to 1.06 V, and from 72.2% to 79.1%, respectively, resulting in 20.7% improvement in power conversion efficiency for the best performing devices. Scrutinizing the electrical properties of this modified interfacial layer strongly suggests that PCBB-2CN-2C8 passivates the TiO2 surface and thus reduces charge recombination loss caused by the deep trap states of TiO2. The passivation effect is further proven by stability testing of the perovskite solar cells with shelf lifetime under ambient conditions improved by a factor of more than 4, from ∼40 h to ∼200 h, using PCBB-2CN-2C8 as the TiO2 modification layer. This work offers not only a promising material for cathode interface engineering, but also provides a viable approach to address the challenges of deep trap states on TiO2 surface in planar perovskite solar cells.

Controllable self-induced passivation of hybrid lead iodide perovskites toward high performance solar cells.

To improve the performance of the polycrystalline thin film devices, it requires a delicate control of its grain structures. As one of the most promising candidates among current thin film photovoltaic techniques, the organic/inorganic hybrid perovskites generally inherit polycrystalline nature and exhibit compositional/structural dependence in regard to their optoelectronic properties. Here, we demonstrate a controllable passivation technique for perovskite films, which enables their compositional change, and allows substantial enhancement in corresponding device performance. By releasing the organic species during annealing, PbI2 phase is presented in perovskite grain boundaries and at the relevant interfaces. The consequent passivation effects and underlying mechanisms are investigated with complementary characterizations, including scanning electron microscopy (SEM), X-ray diffraction (XRD), time-resolved photoluminescence decay (TRPL), scanning Kelvin probe microscopy (SKPM), and ultraviolet photoemission spectroscopy (UPS). This controllable self-induced passivation technique represents an important step to understand the polycrystalline nature of hybrid perovskite thin films and contributes to the development of perovskite solar cells judiciously.

Planar heterojunction perovskite solar cells via vapor-assisted solution process.

Hybrid organic/inorganic perovskites (e.g., CH3NH3PbI3) as light absorbers are promising players in the field of third-generation photovoltaics. Here we demonstrate a low-temperature vapor-assisted solution process to construct polycrystalline perovskite thin films with full surface coverage, small surface roughness, and grain size up to microscale. Solar cells based on the as-prepared films achieve high power conversion efficiency of 12.1%, so far the highest efficiency based on CH3NH3PbI3 with the planar heterojunction configuration. This method provides a simple approach to perovskite film preparation and paves the way for high reproducibility of films and devices. The underlying kinetic and thermodynamic parameters regarding the perovskite film growth are discussed as well.

Chloroboron (III) subnaphthalocyanine as an electron donor in bulk heterojunction photovoltaic cells.

In this work, chloroboron (III) subnaphthalocyanine (SubNc) was used as an electron donor, combined with a [6,6]-phenyl-C71-butyric acid methyl ester (PC70BM) or fullerene C70 acceptor in bulk heterojunction photovoltaic cells. In spite of the limited solubility of SubNc in organic solvents, the solution processed device exhibited an efficiency of 4.0% under 1 sun, AM1.5G solar irradiation at room temperature, and 5.0% at 80 ° C due to the temperature-dependence of the carrier mobilities. SubNc:C70 bulk heterojunctions were also fabricated via thermal co-evaporation, demonstrating an efficiency of 4.4%. This result shows that SubNc is a promising material for photovoltaic applications via various processing techniques, such as vacuum deposition and wet coating.

Solution-processed organic photovoltaics based on indoline dye molecules developed in dye-sensitized solar cells.

A donor-acceptor (D-A) type indoline dye, D149, was used as an electron donor in solution-processed organic solar cells (OSCs). For bulk-heterojunction (BHJ) type OSCs with PC70BM as electron acceptor, the power conversion efficiency (PCE) is sensitive to the amount of D149 in the D149/PC70BM blend film. When the concentration of D149 in the blend film was as low as 5%, the highest PCE of up to 1.29%, together with a short-circuit current density (Jsc) of 4.58 mA·cm-2, an open-circuit voltage (Voc) of 0.90 V and a fill factor (FF) of 0.31, was achieved. In order to improve the PCE of D149-based OSCs, a bilayer-heterojunction configuration with C70 as electron acceptor has been employed. By optimizing the thickness of the D149 layer and varying the electron- and hole-transport layers, a highest PCE of up to 2.28% with a Jsc of 4.38 mA·cm-2, a Voc of 0.77 V, and an FF of 0.62 was achieved under AM 1.5G solar illumination (100 mW·cm-2).

Solution-processed organic photovoltaic cells based on a squaraine dye.

In this work, 2,4-bis[4-(N,N-diisobutylamino)-2,6-dihydroxyphenyl] squaraine (SQ) was systematically studied as an electron donor in solution processed photovoltaic cells, showing power conversion efficiency of >4.0% under AM1.5G 1 sun illumination at room temperature. Low mobilities were found to limit charge transport in the bulk heterojunctions. Efficiency was thus improved to 5.1% at 80 °C mainly due to improvement of photocurrent extraction. We also demonstrated that the SQ compound synthesized via a simple method has high purity, and thus can be used in photovoltaic cells without further purification. Our results suggest the huge potential of SQ and its analogs in organic photovoltaic applications.

High efficiency polymer solar cells with vertically modulated nanoscale morphology.

Nanoscale morphology has been shown to be a critical parameter governing charge transport properties of polymer bulk heterojunction (BHJ) solar cells. Recent results on vertical phase separation have intensified the research on 3D morphology control. In this paper, we intend to modify the distribution of donors and acceptors in a classical BHJ polymer solar cell by making the active layer richer in donors and acceptors near the anode and cathode respectively. Here, we chose [6,6]-phenyl- C(61)-butyric acid methyl ester (PCBM) to be the acceptor material to be thermally deposited on top of [poly(3-hexylthiophene)] P3HT: the PCBM active layer to achieve a vertical composition gradient in the BHJ structure. Here we report on a solar cell with enhanced power conversion efficiency of 4.5% which can be directly correlated with the decrease in series resistance of the device.

Author Correction: Solution-processed hybrid perovskite photodetectors with high detectivity.

This Article contains an error in Equation 2 in that the denominator is inverted. This has not been fixed in the PDF or HTML versions of the Article but can be seen in the associated Correction.

Preparation, photo- and electro-luminescent properties of a novel complex of Tb (III) with a tripod ligand.

A novel Tb(III) complex TbL (L=tris[2-(2-carboxyphenoxy)ethyl]amine, H3L) was synthesized and characterized by means of elemental analyses, IR spectra, thermal analyses, and molar conductivity measurement. The photoluminescent properties of the complex were investigated. In addition, PVK doping Tb(III) complex was fabricated as the emissive layer by spin-coating and its electroluminescent properties were studied, in which the structure of the device was ITO (indium tin oxide)/PVK (polyvinylcarbazole)/PVK: TbL/PBD (2-(4-biphenylyl)-5-(4-tert-butylphenyl)-1,3,4-oxadiazole)/LiF/Al. It was indicated that pure green and narrow bandwidth emission at 545nm from photoluminescence of TbL complex film and the organic electroluminescent device is the characteristic emission of Tb(III) ion, and the electroluminescence spectrum of the device was very similar to that of the photoluminescence of TbL complex film. The lowest triplet level of the ligand was calculated from the phosphorescence spectrum of GdL in N,N-dimethyl formamide (DMF) dilute solution determined at 77K, and the energy transfer mechanisms in TbL complex were discussed.

Comparison of the Solution and Vacuum-Processed Squaraine:Fullerene Small-Molecule Bulk Heterojunction Solar Cells.

Squaraine dyes have shown promising properties for high performance organic solar cells owing to their advantages of intense absorption and high absorption coefficients in the visible and near-infrared (NIR) regions. In this work, to directly compare the photovoltaic performance of solution- and vacuum-processed small-molecule bulk heterojunction (SMBHJ) solar cells, we employed a squaraine small molecular dye, 2,4-bis[4-(N,N-diisobutylamino)-2,6-dihydroxyphenyl] squaraine (DIBSQ), as an electron donor combined with fullerene acceptors to fabricate SMBHJ cells either from solution or vacuum deposition process. The solution-processed SMBHJ cell possesses a power conversion efficiency (PCE) of ~4.3%, while the vacuum-processed cell provides a PCE of ~6.3%. Comparison of the device performance shows that the vacuum-processed SMBHJ cells possess higher short-circuit current density, fill factor and thus higher PCE than the solution-processed devices, which should be assigned to more efficient charge transport and charge extraction in the vacuum-processed SMBHJ cells. However, solution-processed SMBHJ cells demonstrate more pronounced temperature-dependent device performance and higher device stability. This study indicates the great potential of DIBSQ in photovoltaic application via both of solution and vacuum processing techniques.

Pure Formamidinium-Based Perovskite Light-Emitting Diodes with High Efficiency and Low Driving Voltage.

A formamidinium(FA)-based perovskite showns superior optoelectronic properties including better stability than methylammonium-based counterparts. Pure FA-perovskite-based light-emitting diodes (LEDs) with high efficiency are reported. Interestingly, the LED clearly shows a sub-bandgap emission at 1.7 V (bandgap 2.3 eV). This important discovery provides further insights of the charge transport mechanism in perovskite-based optoelectronic devices.

Perovskite Solar Cells Employing Dopant-Free Organic Hole Transport Materials with Tunable Energy Levels.

Conjugated small-molecule hole-transport materials (HTMs) with tunable energy levels are designed and synthesized for efficient perovskite solar cells. A champion device with efficiency of 16.2% is demonstrated using a dopant-free DERDTS-TBDT HTM, while the DORDTS-DFBT-HTM-based device shows an inferior performance of 6.2% due to its low hole mobility and unmatched HOMO level with the valence band of perovskite film.

High-efficiency robust perovskite solar cells on ultrathin flexible substrates.

Wide applications of personal consumer electronics have triggered tremendous need for portable power sources featuring light-weight and mechanical flexibility. Perovskite solar cells offer a compelling combination of low-cost and high device performance. Here we demonstrate high-performance planar heterojunction perovskite solar cells constructed on highly flexible and ultrathin silver-mesh/conducting polymer substrates. The device performance is comparable to that of their counterparts on rigid glass/indium tin oxide substrates, reaching a power conversion efficiency of 14.0%, while the specific power (the ratio of power to device weight) reaches 1.96 kW kg(-1), given the fact that the device is constructed on a 57-µm-thick polyethylene terephthalate based substrate. The flexible device also demonstrates excellent robustness against mechanical deformation, retaining >95% of its original efficiency after 5,000 times fully bending. Our results confirmed that perovskite thin films are fully compatible with our flexible substrates, and are thus promising for future applications in flexible and bendable solar cells.

Low-Temperature TiOx Compact Layer for Planar Heterojunction Perovskite Solar Cells.

Here, we demonstrate an effective low-temperature approach to fabricate a uniform and pinhole-free compact TiO2 layer for enhancing photovoltaic performance of perovskite solar cells. TiCl4 was used to modify TiO2 for efficient charge generation and significantly reduced recombination loss. We found that a TiO2 layer with an appropriate TiCl4 treatment possesses a smooth surface with full coverage of the conductive electrode. Further studies on charge carrier dynamics confirmed that the TiCl4 treatment improves the contact of the TiO2/perovskite interface, facilitating charge extraction and suppressing charge recombination. On the basis of the treatment, we improved the open circuit voltage from 1.01 V of the reference cell to 1.08 V, and achieved a power conversion efficiency of 16.4%.

Improved air stability of perovskite solar cells via solution-processed metal oxide transport layers.

Lead halide perovskite solar cells have recently attracted tremendous attention because of their excellent photovoltaic efficiencies. However, the poor stability of both the perovskite material and the charge transport layers has so far prevented the fabrication of devices that can withstand sustained operation under normal conditions. Here, we report a solution-processed lead halide perovskite solar cell that has p-type NiO(x) and n-type ZnO nanoparticles as hole and electron transport layers, respectively, and shows improved stability against water and oxygen degradation when compared with devices with organic charge transport layers. Our cells have a p-i-n structure (glass/indium tin oxide/NiO(x)/perovskite/ZnO/Al), in which the ZnO layer isolates the perovskite and Al layers, thus preventing degradation. After 60 days storage in air at room temperature, our all-metal-oxide devices retain about 90% of their original efficiency, unlike control devices made with organic transport layers, which undergo a complete degradation after just 5 days. The initial power conversion efficiency of our devices is 14.6 ± 1.5%, with an uncertified maximum value of 16.1%.

Toward Highly Sensitive Polymer Photodetectors by Molecular Engineering.

Modified 3,4-ethylenedioxythiophene is employed as the conjugated side chain in conjugated polymers, which can significantly depress the dark current of the polymer photodetectors with little associated decrease in photovoltaic properties, thus enhanceing the detectivities. This approach can be applied to a variety of conjugated polymers covering a photoresponse range from UV to NIR.