Energy quantization in solution-processed layers of indium oxide and their application in resonant tunneling diodes

\u3cp\u3eThe formation of quantized energy states in ultrathin layers of indium oxide (In\u3csub\u3e2\u3c/sub\u3eO\u3csub\u3e3\u3c/sub\u3e) grown via spin coating and thermally annealed at 200°C in air is studied. Optical absorption measurements reveal a characteristic widening of the optical band gap with reducing In\u3csub\u3e2\u3c/sub\u3eO\u3csub\u3e3\u3c/sub\u3e layer thickness from ≈43 to ≈3 nm in agreement with theoretical predictions for an infinite quantum well. Through sequential deposition of In\u3csub\u3e2\u3c/sub\u3eO\u3csub\u3e3\u3c/sub\u3e and gallium oxide (Ga\u3csub\u3e2\u3c/sub\u3eO\u3csub\u3e3\u3c/sub\u3e) layers, superlattice-like structures with controlled dimensionality and spatially varying conduction band characteristics are demonstrated. This simple method is then explored for the fabrication of functional double-barrier resonant tunneling diodes. Nanoscale current mapping analysis using conductive atomic force microscopy reveals that resonant tunneling is not uniform but localized in specific regions of the apparent device area. The latter observation is attributed to variation in the layer(s) thickness of the In\u3csub\u3e2\u3c/sub\u3eO\u3csub\u3e3\u3c/sub\u3e quantum well and/or the Ga\u3csub\u3e2\u3c/sub\u3eO\u3csub\u3e3\u3c/sub\u3e barrier layers. Despite the nonidealities, the tremendous potential of solution-processable oxide semiconductors for the development of quantum effect devices that have so far been demonstrated only via sophisticated growth techniques is demonstrated.\u3c/p\u3

High Electron Mobility Thin-Film Transistors Based on Solution-Processed Semiconducting Metal Oxide Heterojunctions and Quasi-Superlattices

High mobility thin‐film transistor technologies that can be implemented using simple and inexpensive fabrication methods are in great demand because of their applicability in a wide range of emerging optoelectronics. Here, a novel concept of thin‐film transistors is reported that exploits the enhanced electron transport properties of low‐dimensional polycrystalline heterojunctions and quasi‐superlattices (QSLs) consisting of alternating layers of In(2)O(3), Ga(2)O(3,) and ZnO grown by sequential spin casting of different precursors in air at low temperatures (180–200 °C). Optimized prototype QSL transistors exhibit band‐like transport with electron mobilities approximately a tenfold greater (25–45 cm(2) V(−1) s(−1)) than single oxide devices (typically 2–5 cm(2) V(−1) s(−1)). Based on temperature‐dependent electron transport and capacitance‐voltage measurements, it is argued that the enhanced performance arises from the presence of quasi 2D electron gas‐like systems formed at the carefully engineered oxide heterointerfaces. The QSL transistor concept proposed here can in principle extend to a range of other oxide material systems and deposition methods (sputtering, atomic layer deposition, spray pyrolysis, roll‐to‐roll, etc.) and can be seen as an extremely promising technology for application in next‐generation large area optoelectronics such as ultrahigh definition optical displays and large‐area microelectronics where high performance is a key requirement

Toward Improved Lifetimes of Organic Solar Cells under Thermal Stress: Substrate-Dependent Morphological Stability of PCDTBT:PCBM Films and Devices

Morphological stability is a key requirement for outdoor operation of organic solar cells. We demonstrate that morphological stability and lifetime of polymer/fullerene based solar cells under thermal stress depend strongly on the substrate interface on which the active layer is deposited. In particular, we find that the stability of benchmark PCDTBT/PCBM solar cells under modest thermal stress is substantially increased in inverted solar cells employing a ZnO substrate compared to conventional devices employing a PEDOT:PSS substrate. This improved stability is observed to correlate with PCBM nucleation at the 50 nm scale, which is shown to be strongly influenced by different substrate interfaces. Employing this approach, we demonstrate remarkable thermal stability for inverted PCDTBT:PC70BM devices on ZnO substrates, with negligible (<2%) loss of power conversion efficiency over 160 h under 85 °C thermal stress and minimal thermally induced “burn-in” effect. We thus conclude that inverted organic solar cells, in addition to showing improved environmental stability against ambient humidity exposure as widely reported previously, can also demonstrate enhanced morphological stability. As such we show that the choice of suitable substrate interfaces may be a key factor in achieving prolonged lifetimes for organic solar cells under thermal stress conditions

A piperidinium salt stabilizes efficient metal-halide perovskite solar cells

Longevity has been a long-standing concern for hybrid perovskite photovoltaics. We demonstrate high-resilience positive-intrinsic-negative perovskite solar cells by incorporating a piperidinium-based ionic compound into the formamidinium-cesium lead-trihalide perovskite absorber. With the bandgap tuned to be well suited for perovskite-on-silicon tandem cells, this piperidinium additive enhances the open-circuit voltage and cell efficiency. This additive also retards compositional segregation into impurity phases and pinhole formation in the perovskite absorber layer during aggressive aging. Under full-spectrum simulated sunlight in ambient atmosphere, our unencapsulated and encapsulated cells retain 80 and 95% of their peak and post-burn-in efficiencies for 1010 and 1200 hours at 60° and 85°C, respectively. Our analysis reveals detailed degradation routes that contribute to the failure of aged cells

Exploring Two-Dimensional Transport Phenomena in Metal Oxide Heterointerfaces for Next-Generation, High-Performance, Thin-Film Transistor Technologies.

In the last decade, metal oxides have emerged as a fascinating class of electronic material, exhibiting a wide range of unique and technologically relevant characteristics. For example, thin-film transistors formed from amorphous or polycrystalline metal oxide semiconductors offer the promise of low-cost, large-area, and flexible electronics, exhibiting performances comparable to or in excess of incumbent silicon-based technologies. Atomically flat interfaces between otherwise insulating or semiconducting complex oxides, are also found to be highly conducting, displaying 2-dimensional (2D) charge transport properties, strong correlations, and even superconductivity. Field-effect devices employing such carefully engineered interfaces are hoped to one day compete with traditional group IV or III-V semiconductors for use in the next-generation of high-performance electronics. In this Concept article we provide an overview of the different metal oxide transistor technologies and potential future research directions. In particular, we look at the recent reports of multilayer oxide thin-film transistors and the possibility of 2D electron transport in these disordered/polycrystalline systems and discuss the potential of the technology for applications in large-area electronics. Exotic charge-transport phenomena have been reported for several 2D semiconducting systems and their devices. Recent experimental results suggest that similar phenomena can be achieved in metal oxide-based systems. In this article, an overview of different transistor technologies, the operation of which relies on low-dimensional charge-transport, is given and potential future research directions in the area of thin-film transistors are discussed

Signatures of Quantized Energy States in Solution-Processed Ultrathin Layers of Metal-Oxide Semiconductors and Their Devices

Physical phenomena such as energy quantization have to-date been overlooked in solution-processed inorganic semiconducting layers, owing to heterogeneity in layer thickness uniformity unlike some of their vacuum-deposited counterparts. Recent reports of the growth of uniform, ultrathin (<5 nm) metal-oxide semiconductors from solution, however, have potentially opened the door to such phenomena manifesting themselves. Here, a theoretical framework is developed for energy quantization in inorganic semiconductor layers with appreciable surface roughness, as compared to the mean layer thickness, and present experimental evidence of the existence of quantized energy states in spin-cast layers of zinc oxide (ZnO). As-grown ZnO layers are found to be remarkably continuous and uniform with controllable thicknesses in the range 2-24 nm and exhibit a characteristic widening of the energy bandgap with reducing thickness in agreement with theoretical predictions. Using sequentially spin-cast layers of ZnO as the bulk semiconductor and quantum well materials, and gallium oxide or organic self-assembled monolayers as the barrier materials, two terminal electronic devices are demonstrated, the current-voltage characteristics of which resemble closely those of double-barrier resonant-tunneling diodes. As-fabricated all-oxide/hybrid devices exhibit a characteristic negative-differential conductance region with peak-to-valley ratios in the range 2-7

Solution-processed dye-sensitized ZnO phototransistors with extremely high photoresponsivity

We report the fabrication of light-sensing thin-film transistors based on solution processed films of ZnO, as the channel material, functionalized with an organic dye as the light sensitizer. Due to the presence of the dye, the hybrid devices show exceptionally high photosensitivity to green light of 10 6 and a maximum photoresponsivity on the order of 10 4 A/W. The high performance is argued to be the result of the grain barrier limited nature of electron transport across the polycrystalline ZnO film and its dependence on charge carrier density upon illumination with green light. In addition to the excellent photoresponsivity and signal gain, the hybrid ZnO-dye photoactive layer exhibits high optical transparency. The unique combination of simple device fabrication and distinctive physical characteristics, such as optical transparency, renders the technology attractive for application in large-area transparent photodetectors. © 2012 American Institute of Physics

Long-range charge carrier mobility in metal halide perovskite thin-films and single crystals via transient photo-conductivity

Charge carrier mobility is a fundamental property of semiconductor materials that governs many electronic device characteristics. For metal halide perovskites, a wide range of charge carrier mobilities have been reported using different techniques. Mobilities are often estimated via transient methods assuming an initial charge carrier population after pulsed photoexcitation and measurement of photoconductivity via non-contact or contact techniques. For nanosecond to millisecond transient methods, early-time recombination and exciton-to-free-carrier ratio hinder accurate determination of free-carrier population after photoexcitation. By considering both effects, we estimate long-range charge carrier mobilities over a wide range of photoexcitation densities via transient photoconductivity measurements. We determine long-range mobilities for FA0.83Cs0.17Pb(I0.9Br0.1)3, (FA0.83MA0.17)0.95Cs0.05Pb(I0.9Br0.1)3 and CH3NH3PbI3-xClx polycrystalline films in the range of 0.3 to 6.7 cm2 V−1 s−1. We demonstrate how our data-processing technique can also reveal more precise mobility estimates from non-contact time-resolved microwave conductivity measurements. Importantly, our results indicate that the processing of polycrystalline films significantly affects their long-range mobility