Concept: Amorphous silicon
We describe the development of solar water-splitting cells comprising earth-abundant elements that operate in near-neutral pH conditions, both with and without connecting wires. The cells consist of a triple junction, amorphous silicon photovoltaic interfaced to hydrogen- and oxygen-evolving catalysts made from an alloy of earth-abundant metals and a cobalt|borate catalyst, respectively. The devices described here carry out the solar-driven water-splitting reaction at efficiencies of 4.7% for a wired configuration and 2.5% for a wireless configuration when illuminated with 1 sun (100 milliwatts per square centimeter) of air mass 1.5 simulated sunlight. Fuel-forming catalysts interfaced with light-harvesting semiconductors afford a pathway to direct solar-to-fuels conversion that captures many of the basic functional elements of a leaf.
Fabrication of thin-film solar cells (TFSCs) on substrates other than Si and glass has been challenging because these nonconventional substrates are not suitable for the current TFSC fabrication processes due to poor surface flatness and low tolerance to high temperature and chemical processing. Here, we report a new peel-and-stick process that circumvents these fabrication challenges by peeling off the fully fabricated TFSCs from the original Si wafer and attaching TFSCs to virtually any substrates regardless of materials, flatness and rigidness. With the peel-and-stick process, we integrated hydrogenated amorphous silicon (a-Si:H) TFSCs on paper, plastics, cell phone and building windows while maintaining the original 7.5% efficiency. The new peel-and-stick process enables further reduction of the cost and weight for TFSCs and endows TFSCs with flexibility and attachability for broader application areas. We believe that the peel-and-stick process can be applied to thin film electronics as well.
Organic thin-film transistors (OTFTs) can be fabricated at moderate temperatures and through cost-effective solution-based processes on a wide range of low-cost flexible and deformable substrates. Although the charge mobility of state-of-the-art OTFTs is superior to that of amorphous silicon and approaches that of amorphous oxide thin-film transistors (TFTs), their operational stability generally remains inferior and a point of concern for their commercial deployment. We report on an exhaustive characterization of OTFTs with an ultrathin bilayer gate dielectric comprising the amorphous fluoropolymer CYTOP and an Al2O3:HfO2 nanolaminate. Threshold voltage shifts measured at room temperature over time periods up to 5.9 × 105 s do not vary monotonically and remain below 0.2 V in microcrystalline OTFTs (μc-OTFTs) with field-effect carrier mobility values up to 1.6 cm2 V-1 s-1. Modeling of these shifts as a function of time with a double stretched-exponential (DSE) function suggests that two compensating aging mechanisms are at play and responsible for this high stability. The measured threshold voltage shifts at temperatures up to 75°C represent at least a one-order-of-magnitude improvement in the operational stability over previous reports, bringing OTFT technologies to a performance level comparable to that reported in the scientific literature for other commercial TFTs technologies.
In this article, we report only 10 atomic layer thick, high mobility, transparent thin film transistors (TFTs) with ambipolar device characteristics fabricated on both a conventional silicon platform as well as on a flexible substrate. Monolayer graphene was used as metal electrodes, 3-4 atomic layers of h-BN were used as the gate dielectric, and finally bilayers of WSe2 were used as the semiconducting channel material for the TFTs. The field effect carrier mobility was extracted to be 45 cm(2)/(V s), which exceeds the mobility values of state of the art amorphous silicon based TFTs by ∼100 times. The active device stack of WSe2-hBN-graphene was found to be more than 88% transparent over the entire visible spectrum and the device characteristics were unaltered for in-plane mechanical strain of up to 2%. The device demonstrated remarkable temperature stability over 77-400 K. Low contact resistance value of 1.4 kΩ-μm, subthreshold slope of 90 mv/decade, current ON-OFF ratio of 10(7), and presence of both electron and hole conduction were observed in our all two-dimensional (2D) TFTs, which are extremely desirable but rarely reported characteristics of most of the organic and inorganic TFTs. To the best of our knowledge, this is the first report of all 2D transparent TFT fabricated on flexible substrate along with the highest mobility and current ON-OFF ratio.
- Proceedings of the National Academy of Sciences of the United States of America
- Published 8 months ago
Nanostructured surfaces with quasi-random geometries can manipulate light over broadband wavelengths and wide ranges of angles. Optimization and realization of stochastic patterns have typically relied on serial, direct-write fabrication methods combined with real-space design. However, this approach is not suitable for customizable features or scalable nanomanufacturing. Moreover, trial-and-error processing cannot guarantee fabrication feasibility because processing-structure relations are not included in conventional designs. Here, we report wrinkle lithography integrated with concurrent design to produce quasi-random nanostructures in amorphous silicon at wafer scales that achieved over 160% light absorption enhancement from 800 to 1,200 nm. The quasi-periodicity of patterns, materials filling ratio, and feature depths could be independently controlled. We statistically represented the quasi-random patterns by Fourier spectral density functions (SDFs) that could bridge the processing-structure and structure-performance relations. Iterative search of the optimal structure via the SDF representation enabled concurrent design of nanostructures and processing.
We report on stacked high-contrast grating reflectors with virtually angular independent reflectance for transverse-magnetic polarized light. The investigated structure consists of two-layer pairs of amorphous silicon and silicondioxide that are designed for a wavelengths of 1550 nm. The large angular tolerance results from coupling of the two involved silicon gratings and is achieved if the modal fields in the reflectors are matched. With this approach, a reflectance of more than 96% in the entire angular spectrum is feasible. Experimentally we demonstrate a reflectance of more than 98% for incidence angles up to 60° and more than 90% up to 80°.
Recent advances in the use of organic-inorganic hybrid perovskites for optoelectronics have been rapid, with reported power conversion efficiencies of up to 22 per cent for perovskite solar cells. Improvements in stability have also enabled testing over a timescale of thousands of hours. However, large-scale deployment of such cells will also require the ability to produce large-area, uniformly high-quality perovskite films. A key challenge is to overcome the substantial reduction in power conversion efficiency when a small device is scaled up: a reduction from over 20 per cent to about 10 per cent is found when a common aperture area of about 0.1 square centimetres is increased to more than 25 square centimetres. Here we report a new deposition route for methyl ammonium lead halide perovskite films that does not rely on use of a common solvent or vacuum: rather, it relies on the rapid conversion of amine complex precursors to perovskite films, followed by a pressure application step. The deposited perovskite films were free of pin-holes and highly uniform. Importantly, the new deposition approach can be performed in air at low temperatures, facilitating fabrication of large-area perovskite devices. We reached a certified power conversion efficiency of 12.1 per cent with an aperture area of 36.1 square centimetres for a mesoporous TiO2-based perovskite solar module architecture.
Organic-inorganic perovskites are well suited for optoelectronic applications. In particular, perovskite single and perovskite tandem solar cells with silicon are close to their market entry. Despite their swift rise in efficiency to more than 21%, solar cell lifetimes are way below the needed 25 years. In fact, comparison of the time when the device performance has degraded to 80% of its initial value (T80 lifetime) of numerous solar cells throughout the literature reveals a strongly reduced stability under illumination. Herein, the various detrimental effects are discussed. Most notably, moisture- and heat-related degradation can be mitigated easily by now. Recently, however, several photoinduced degradation mechanisms have been observed. Under illumination, mixed perovskites tend to phase segregate, while, further, oxygen catalyzes deprotonation of the organic cations. Additionally, during illumination photogenerated charge can be trapped in the NH antibonding orbitals causing dissociation of the organic cation. On the other hand, organic-inorganic perovskites exhibit a high radiation hardness that is superior to crystalline silicon. Here, the proposed degradation mechanisms reported in the literature are thoroughly reviewed and the microscopic mechanisms and their implications for solar cells are discussed.
Solid silicon monoxide is an amorphous material which has been commercialized for many functional applications. However, the amorphous structure of silicon monoxide is a long-standing question because of the uncommon valence state of silicon in the oxide. It has been deduced that amorphous silicon monoxide undergoes an unusual disproportionation by forming silicon- and silicon-dioxide-like regions. Nevertheless, the direct experimental observation is still missing. Here we report the amorphous structure characterized by angstrom-beam electron diffraction, supplemented by synchrotron X-ray scattering and computer simulations. In addition to the theoretically predicted amorphous silicon and silicon-dioxide clusters, suboxide-type tetrahedral coordinates are detected by angstrom-beam electron diffraction at silicon/silicon-dioxide interfaces, which provides compelling experimental evidence on the atomic-scale disproportionation of amorphous silicon monoxide. Eventually we develop a heterostructure model of the disproportionated silicon monoxide which well explains the distinctive structure and properties of the amorphous material.
We demonstrate experimentally ultrafast all-optical switching in subwavelength nonlinear dielectric nanostructures exhibiting localized magnetic Mie resonances. We employ amorphous silicon nanodisks to achieve strong self-modulation of femtosecond pulses with a depth of 60\% at picojoule-per-disk pump energies. In the pump-probe measurements, we reveal that switching in the nanodisks can be governed by pulse-limited 65-fs-long two-photon absorption being enhanced by a factor of 80 with respect to the unstructured silicon film. We also show that undesirable free-carrier effects can be suppressed by a proper spectral positioning of the magnetic resonance, making such a structure the fastest all-optical switch operating at the nanoscale.