Ni Zhao

Downscaling of self-aligned, all-printed polymer thin-film transistors

Printing is an emerging approach for low-cost, large-area manufacturing of electronic circuits, but it has the disadvantages of poor resolution, large overlap capacitances, and film thickness limitations, resulting in slow circuit speeds and high operating voltages. Here, we demonstrate a self-aligned printing approach that allows downscaling of printed organic thin-film transistors to channel lengths of 100-400 nm. The use of a crosslinkable polymer gate dielectric with 30-50 nm thickness ensures that basic scaling requirements are fulfilled and that operating voltages are below 5 V. The device architecture minimizes contact resistance effects, enabling clean scaling of transistor current with channel length. A self-aligned gate configuration minimizes parasitic overlap capacitance to values as low as 0.2-0.6 pF mm(-1), and allows transition frequencies of fT = 1.6 MHz to be reached. Our self-aligned process provides a way to improve the performance of printed organic transistor circuits by downscaling, while remaining compatible with the requirements of large-area, flexible electronics manufacturing.

Inorganic–Organic Hybrid Solar Cell: Bridging Quantum Dots to Conjugated Polymer Nanowires

Quantum dots show great promise for fabrication of hybrid bulk heterojunction solar cells with enhanced power conversion efficiency, yet controlling the morphology and interface structure on the nanometer length scale is challenging. Here, we demonstrate quantum dot-based hybrid solar cells with improved electronic interaction between donor and acceptor components, resulting in significant improvement in short-circuit current and open-circuit voltage. CdS quantum dots were bound onto crystalline P3HT nanowires through solvent-assisted grafting and ligand exchange, leading to controlled organic-inorganic phase separation and an improved maximum power conversion efficiency of 4.1% under AM 1.5 solar illumination. Our approach can be applied to a wide range of quantum dots and polymer hybrids and is compatible with solution processing, thereby offering a general scheme for improving the efficiency of nanocrystal hybrid solar cells.

Colloidal PbS quantum dot solar cells with high fill factor.

We fabricate PbS colloidal quantum dot (QD)-based solar cells using a fullerene derivative as the electron-transporting layer (ETL). A thiol treatment and oxidation process are used to modify the morphology and electronic structure of the QD films, resulting in devices that exhibit a fill factor (FF) as high as 62%. We also show that, for QDs with a band gap of less than 1 eV, an open-circuit voltage (VOC) of 0.47 V can be achieved. The power conversion efficiency reaches 1.3% under 1 sun AM1.5 test conditions and 2.4% under monochromatic infrared (lambda=1310 nm) illumination. A consistent mechanism for device operation is developed through a circuit model and experimental measurements, shedding light on new approaches for optimization of solar cell performance by modifying the interface between the QDs and the neighboring charge transport layers.

Energy level modification in lead sulfide quantum dot thin films through ligand exchange.

The electronic properties of colloidal quantum dots (QDs) are critically dependent on both QD size and surface chemistry. Modification of quantum confinement provides control of the QD bandgap, while ligand-induced surface dipoles present a hitherto underutilized means of control over the absolute energy levels of QDs within electronic devices. Here, we show that the energy levels of lead sulfide QDs, measured by ultraviolet photoelectron spectroscopy, shift by up to 0.9 eV between different chemical ligand treatments. The directions of these energy shifts match the results of atomistic density functional theory simulations and scale with the ligand dipole moment. Trends in the performance of photovoltaic devices employing ligand-modified QD films are consistent with the measured energy level shifts. These results identify surface-chemistry-mediated energy level shifts as a means of predictably controlling the electronic properties of colloidal QD films and as a versatile adjustable parameter in the performance optimization of QD optoelectronic devices.

Improved Current Extraction from ZnO/PbS Quantum Dot Heterojunction Photovoltaics Using a MoO3 Interfacial Layer

The ability to engineer interfacial energy offsets in photovoltaic devices is one of the keys to their optimization. Here, we demonstrate that improvements in power conversion efficiency may be attained for ZnO/PbS heterojunction quantum dot photovoltaics through the incorporation of a MoO(3) interlayer between the PbS colloidal quantum dot film and the top-contact anode. Through a combination of current-voltage characterization, circuit modeling, Mott-Schottky analysis, and external quantum efficiency measurements performed with bottom- and top-illumination, these enhancements are shown to stem from the elimination of a reverse-bias Schottky diode present at the PbS/anode interface. The incorporation of the high-work-function MoO(3) layer pins the Fermi level of the top contact, effectively decoupling the device performance from the work function of the anode and resulting in a high open-circuit voltage (0.59 ± 0.01 V) for a range of different anode materials. Corresponding increases in short-circuit current and fill factor enable 1.5-fold, 2.3-fold, and 4.5-fold enhancements in photovoltaic device efficiency for gold, silver, and ITO anodes, respectively, and result in a power conversion efficiency of 3.5 ± 0.4% for a device employing a gold anode.

Charge Transport Physics of Conjugated Polymer Field‐Effect Transistors

Field-effect transistors based on conjugated polymers are being developed for large-area electronic applications on flexible substrates, but they also provide a very useful tool to probe the charge transport physics of these complex materials. In this review we discuss recent progress in polymer semiconductor materials, which have brought the performance and mobility of polymer devices to levels comparable to that of small-molecule organic semiconductors. These new materials have also enabled deeper insight into the charge transport physics of high-mobility polymer semiconductors gained from experiments with high charge carrier concentration and better molecular-scale understanding of the electronic structure at the semiconductor/ dielectric interface.

High performance inverted structure perovskite solar cells based on a PCBM:polystyrene blend electron transport layer

Hybrid organic/inorganic perovskite solar cells are among the most competitive emerging photovoltaic technologies. Here, we report on NiO-based inverted structure perovskite solar cells with a high power conversion efficiency of 10.68%, which is achieved by adding a small percentage (1.5 wt%) of high molecular weight polystyrene (PS) into the PCBM electron transport layer (ETL). The addition of PS facilitates the formation of a highly smooth and uniform PCBM ETL that is more effective in preventing undesirable electron–hole recombination between the perovskite layer and the top electrode. As a result, the VOC of the PCBM:PS-based cells is increased from 0.97 V to 1.07 V, which leads to significantly enhanced power conversion efficiencies of the solar cells. Our study provides a simple and low-cost approach to improving the ETL film quality and the performance of inverted perovskite solar cells.

Heterojunction Photovoltaics Using GaAs Nanowires and Conjugated Polymers

We demonstrate an organic/inorganic solar cell architecture based on a blend of poly(3-hexylthiophene) (P3HT) and narrow bandgap GaAs nanowires. The measured increase of device photocurrent with increased nanowire loading is correlated with structural ordering within the active layer that enhances charge transport. Coating the GaAs nanowires with TiO(x) shells passivates nanowire surface states and further improves the photovoltaic performance. We find that the P3HT/nanowire cells yield power conversion efficiencies of 2.36% under white LED illumination for devices containing 50 wt % of TiO(x)-coated GaAs nanowires. Our results constitute important progress for the use of nanowires in large area solution processed hybrid photovoltaic cells and provide insight into the role of structural ordering in the device performance.

Phenylalkylamine Passivation of Organolead Halide Perovskites Enabling High-Efficiency and Air-Stable Photovoltaic Cells

Benzylamine is introduced as a surface passivation molecule that improves the moisture-resistance of the perovskites while simultaneously enhancing their electronic properties. Solar cells based on benzylamine-modified formamidinium lead iodide perovskite films exhibit a champion efficiency of 19.2% and an open-circuit voltage of 1.12 V. The modified FAPbI3 films exhibit no degradation after >2800 h air exposure.

Bias-Stress Effect in 1,2-Ethanedithiol-Treated PbS Quantum Dot Field-Effect Transistors

We investigate the bias-stress effect in field-effect transistors (FETs) consisting of 1,2-ethanedithiol-treated PbS quantum dot (QD) films as charge transport layers in a top-gated configuration. The FETs exhibit ambipolar operation with typical mobilities on the order of μ(e) = 8 × 10(-3) cm(2) V(-1) s(-1) in n-channel operation and μ(h) = 1 × 10(-3) cm(2) V(-1) s(-1) in p-channel operation. When the FET is turned on in n-channel or p-channel mode, the established drain-source current rapidly decreases from its initial magnitude in a stretched exponential decay, manifesting the bias-stress effect. The choice of dielectric is found to have little effect on the characteristics of this bias-stress effect, leading us to conclude that the associated charge-trapping process originates within the QD film itself. Measurements of bias-stress-induced time-dependent decays in the drain-source current (I(DS)) are well fit to stretched exponential functions, and the time constants of these decays in n-channel and p-channel operation are found to follow thermally activated (Arrhenius) behavior. Measurements as a function of QD size reveal that the stressing process in n-channel operation is faster for QDs of a smaller diameter while stress in p-channel operation is found to be relatively invariant to QD size. Our results are consistent with a mechanism in which field-induced nanoscale morphological changes within the QD film result in screening of the applied gate field. This phenomenon is entirely recoverable, which allows us to repeatedly observe bias stress and recovery characteristics on the same device. This work elucidates aspects of charge transport in chemically treated lead chalcogenide QD films and is of relevance to ongoing investigations toward employing these films in optoelectronic devices.