Efficient metal halide perovskite light-emitting diodes with significantly improved light extraction on nanophotonic substrates.

Metal halide perovskite has emerged as a promising material for light-emitting diodes. In the past, the performance of devices has been improved mainly by optimizing the active and charge injection layers. However, the large refractive index difference among different materials limits the overall light extraction. Herein, we fabricate efficient methylammonium lead bromide light-emitting diodes on nanophotonic substrates with an optimal device external quantum efficiency of 17.5% which is around twice of the record for the planar device based on this material system. Furthermore, optical modelling shows that a high light extraction efficiency of 73.6% can be achieved as a result of a two-step light extraction process involving nanodome light couplers and nanowire optical antennas on the nanophotonic substrate. These results suggest that utilization of nanophotonic structures can be an effective approach to achieve high performance perovskite light-emitting diodes.

Surface Effect on 2D Hybrid Perovskite Crystals: Perovskites Using an Ethanolamine Organic Layer as an Example.

Despite the remarkable progress of optoelectronic devices based on hybrid perovskites, there are significant drawbacks, which have largely hindered their development as an alternative of silicon. For instance, hybrid perovskites are well-known to suffer from moisture instability which leads to surface degradation. Nonetheless, the dependence of the surface effect on the moisture stability and optoelectronic properties of hybrid perovskites has not been fully investigated. In this work, the influence of the surface effect of 2D layered perovskites before and after mechanical exfoliation, representing rough and smooth surfaces of perovskite crystals, are studied. It is found that the smooth 2D perovskite is less sensitive to ambient moisture and exhibits a considerably low dark current, which outperforms the rough perovskites by 23.6 times in terms of photodetectivity. The superior moisture stability of the smooth perovskites over the rough perovskites is demonstrated. Additionally, ethanolamine is employed as an organic linker of the 2D layered perovskite, which further improves the moisture stability. This work reveals the strong dependence of the surface conditions of 2D hybrid perovskite crystals on their moisture stability and optoelectronic properties, which are of utmost importance to the design of practical optoelectronic devices based on hybrid perovskite crystals.

Low-cost, flexible, disinfectant-free and regular-array three-dimensional nanopyramid antibacterial films for clinical applications.

In this work, a low-cost, scalable and highly repeatable approach was developed to prepare polystyrene films with three-dimensional nanopyramids on the surface. The nanopyramids have a tunable aspect ratio and more importantly, their anti-bacterial performance has been systematically studied. The effectiveness of the nanopyramids on E. coli growth inhibition and the role of the nanostructure aspect ratio were carefully studied through scanning electron microscopy and confocal laser scanning microscopy. The results showed an excellent antibacterial performance with more than 90% reduction in the E. coli population in all nanopyramid samples after a 168 h prolonged incubation time. The nanopyramid film developed here can be used for clinical and commercial applications to prevent the growth of pathogenic bacteria on various surfaces.

Multidirection Piezoelectricity in Mono- and Multilayered Hexagonal α-In2Se3.

Piezoelectric materials have been widely used for sensors, actuators, electronics, and energy conversion. Two-dimensional (2D) ultrathin semiconductors, such as monolayer h-BN and MoS2 with their atom-level geometry, are currently emerging as new and attractive members of the piezoelectric family. However, their piezoelectric polarization is commonly limited to the in-plane direction of odd-number ultrathin layers, largely restricting their application in integrated nanoelectromechanical systems. Recently, theoretical calculations have predicted the existence of out-of-plane and in-plane piezoelectricity in monolayer α-In2Se3. Here, we experimentally report the coexistence of out-of-plane and in-plane piezoelectricity in monolayer to bulk α-In2Se3, attributed to their noncentrosymmetry originating from the hexagonal stacking. Specifically, the corresponding d33 piezoelectric coefficient of α-In2Se3 increases from 0.34 pm/V (monolayer) to 5.6 pm/V (bulk) without any odd-even effect. In addition, we also demonstrate a type of α-In2Se3-based flexible piezoelectric nanogenerator as an energy-harvesting cell and electronic skin. The out-of-plane and in-plane piezoelectricity in α-In2Se3 flakes offers an opportunity to enable both directional and nondirectional piezoelectric devices to be applicable for self-powered systems and adaptive and strain-tunable electronics/optoelectronics.

A Self-Powered and Flexible Organometallic Halide Perovskite Photodetector with Very High Detectivity.

Flexible and self-powered photodetectors (PDs) are highly desirable for applications in image sensing, smart building, and optical communications. In this paper, a self-powered and flexible PD based on the methylammonium lead iodide (CH3 NH3 PBI3 ) perovskite is demonstrated. Such a self-powered PD can operate even with irregular motion such as human finger tapping, which enables it to work without a bulky external power source. In addition, with high-quality CH3 NH3 PBI3 perovskite thin film fabricated with solvent engineering, the PD exhibits an impressive detectivity of 1.22 × 1013 Jones. In the self-powered voltage detection mode, it achieves a large responsivity of up to 79.4 V mW-1 cm-2 and a voltage response of up to ≈90%. Moreover, as the PD is made of flexible and transparent polymer films, it can operate under bending and functions at 360 ° of illumination. As a result, the self-powered, flexible, 360 ° omnidirectional perovskite PD, featuring high detectivity and responsivity along with real-world sensing capability, suggests a new direction for next-generation optical communications, sensing, and imaging applications.

Progress and Design Concerns of Nanostructured Solar Energy Harvesting Devices.

Integrating devices with nanostructures is considered a promising strategy to improve the performance of solar energy harvesting devices such as photovoltaic (PV) devices and photo-electrochemical (PEC) solar water splitting devices. Extensive efforts have been exerted to improve the power conversion efficiencies (PCE) of such devices by utilizing novel nanostructures to revolutionize device structural designs. The thicknesses of light absorber and material consumption can be substantially reduced because of light trapping with nanostructures. Meanwhile, the utilization of nanostructures can also result in more effective carrier collection by shortening the photogenerated carrier collection path length. Nevertheless, performance optimization of nanostructured solar energy harvesting devices requires a rational design of various aspects of the nanostructures, such as their shape, aspect ratio, periodicity, etc. Without this, the utilization of nanostructures can lead to compromised device performance as the incorporation of these structures can result in defects and additional carrier recombination. The design guidelines of solar energy harvesting devices are summarized, including thin film non-uniformity on nanostructures, surface recombination, parasitic absorption, and the importance of uniform distribution of photo-generated carriers. A systematic view of the design concerns will assist better understanding of device physics and benefit the fabrication of high performance devices in the future.

Efficient, flexible and mechanically robust perovskite solar cells on inverted nanocone plastic substrates.

Utilization of nanostructures on photovoltaic devices can significantly improve the device energy conversion efficiency by enhancing the device light harvesting capability as well as carrier collection efficiency. However, improvements in device mechanical robustness and reliability, particularly for flexible devices, have rarely been reported with in-depth understanding. In this work, we fabricated efficient, flexible and mechanically robust organometallic perovskite solar cells on plastic substrates with inverted nanocone (i-cone) structures. Compared with the reference cell that was fabricated on a flat substrate, it was shown that the device power conversion efficiency could be improved by 37%, and reached up to 11.29% on i-cone substrates. More interestingly, it was discovered that the performance of an i-cone device remained more than 90% of the initial value even after 200 mechanical bending cycles, which is remarkably better than for the flat reference device, which degraded down to only 60% in the same test. Our experiments, coupled with mechanical simulation, demonstrated that a nanostructured template can greatly help in relaxing stress and strain upon device bending, which suppresses crack nucleation in different layers of a perovskite solar cell. This essentially leads to much improved device reliability and robustness and will have significant impact on practical applications.

Inverted nanocone-based thin film photovoltaics with omnidirectionally enhanced performance.

Thin film photovoltaic (PV) technologies are highly attractive for low-cost solar energy conversion and possess a wide range of potential applications from building-integrated PV generation to portable power sources. Inverted nanocones (i-cones) have been demonstrated as a promising structure for practical thin film PV devices/modules, owning to their antireflection effect, self-cleaning function, superior mechanical robustness, and so forth. In this work, we have demonstrated a low-cost and scalable approach to achieve perfectly ordered i-cone arrays. Thereafter, thin film amorphous silicon (a-Si:H) solar cells have been fabricated based on various i-cone substrates with different aspect ratios and pitches to investigate the impact of geometry of i-cone nanostructures on the performance of the as-obtained PV devices. Intriguingly, the optical property investigations and device performance characterizations demonstrated that the 0.5-aspect-ratio i-cone-based device performed the best on both light absorption capability and energy conversion efficiency, which is 34% higher than that of the flat counterpart. Moreover, the i-cone-based device enhanced the light absorption and device performance over the flat reference device omnidirectionally. These results demonstrate a viable and convenient route toward scalable fabrication of nanostructures for high-performance thin film PV devices based on a broad range of materials.

Roll-to-roll fabrication of large scale and regular arrays of three-dimensional nanospikes for high efficiency and flexible photovoltaics.

Three-dimensional (3-D) nanostructures have demonstrated enticing potency to boost performance of photovoltaic devices primarily owning to the improved photon capturing capability. Nevertheless, cost-effective and scalable fabrication of regular 3-D nanostructures with decent robustness and flexibility still remains as a challenging task. Meanwhile, establishing rational design guidelines for 3-D nanostructured solar cells with the balanced electrical and optical performance are of paramount importance and in urgent need. Herein, regular arrays of 3-D nanospikes (NSPs) were fabricated on flexible aluminum foil with a roll-to-roll compatible process. The NSPs have precisely controlled geometry and periodicity which allow systematic investigation on geometry dependent optical and electrical performance of the devices with experiments and modeling. Intriguingly, it has been discovered that the efficiency of an amorphous-Si (a-Si) photovoltaic device fabricated on NSPs can be improved by 43%, as compared to its planar counterpart, in an optimal case. Furthermore, large scale flexible NSP solar cell devices have been fabricated and demonstrated. These results not only have shed light on the design rules of high performance nanostructured solar cells, but also demonstrated a highly practical process to fabricate efficient solar panels with 3-D nanostructures, thus may have immediate impact on thin film photovoltaic industry.

Efficient photoelectrochemical water splitting with ultrathin films of hematite on three-dimensional nanophotonic structures.

Photoelectrochemical (PEC) solar water splitting represents a clean and sustainable approach for hydrogen (H2) production and substantial research are being performed to improve the conversion efficiency. Hematite (α-Fe2O3) is considered as a promising candidate for PEC water splitting due to its chemical stability, appropriate band structure, and abundance. However, PEC performance based on hematite is hindered by the short hole diffusion length that put a constraint on the active layer thickness and its light absorption capability. In this work, we have designed and fabricated novel PEC device structure with ultrathin hematite film deposited on three-dimensional nanophotonic structure. In this fashion, the nanophotonic structures can largely improve the light absorption in the ultrathin active materials. In addition, they also provide large surface area to accommodate the slow surface water oxidation process. As the result, high current density of 3.05 mA cm(-2) at 1.23 V with respect to the reversible hydrogen electrode (RHE) has been achieved on such nanophotonic structure, which is about three times of that for a planar photoelectrode. More importantly, our systematic analysis with experiments and modeling revealed that the design of high performance PEC devices needs to consider not only total optical absorption, but also the absorption profile in the active material, in addition to electrode surface area and carrier collection.

Three-dimensional metal/oxide nanocone arrays for high-performance electrochemical pseudocapacitors.

Three-dimensional (3D) electrodes are critical for enabling high-performance power sources. We report here on the design and fabrication, by combining imprint and soft-printing technologies, of 3D nanocone arrays as a novel platform for high performance pseudocapacitors. Such purpose-built 3D nanocone arrays have the advantages of simplicity/versatility/reliability of fabrication, generality to a vast range of active materials, high electrode surface area, and ease of electrolyte permeation. As a demonstration of principle, Au and MnO2 were sequentially deposited forming a 3D Au/MnOx nanocone array electrode for a pseudocapacitor device. This device achieved a specific mass (areal) capacitance of 840.3 F g(-1) (88.2 mF cm(-2)) at a current density of 2 A g(-1). Additionally, the asymmetric supercapacitor using the Au/MnOx nanocone array as the positive electrode and a carbon-based material as the negative electrode achieved a capacitance of 108.5 F g(-1) at a current density of 1 A g(-1), corresponding to an energy density of as high as 46.8 W h kg(-1) at a power density of 0.72 kW kg(-1). The cell still preserved 96.5% of the initial capacitance even after 2000 cycles at a current density of 2 A g(-1). The initial result is at least on a par with those of the best asymmetric supercapacitors reported so far, and thus bolsters the development value of the conductive nanocone arrays for high-performance supercapacitors and other energy-storage devices.

Light Management with Nanostructures for Optoelectronic Devices.

Light management is of paramount importance to improve the performance of optoelectronic devices including photodetectors, solar cells, and light-emitting diodes. Extensive studies have shown that the efficiency of these optoelectronic devices largely depends on the device structural design. In the case of solar cells, three-dimensional (3-D) nanostructures can remarkably improve device energy conversion efficiency via various light-trapping mechanisms, and a number of nanostructures were fabricated and exhibited tremendous potential for highly efficient photovoltaics. Meanwhile, these optical absorption enhancement schemes can benefit photodetectors by achieving higher quantum efficiency and photon extraction efficiency. On the other hand, low extraction efficiency of a photon from the emissive layer to outside often puts a constraint on the external quantum efficiency (EQE) of LEDs. In this regard, different designs of device configuration based on nanostructured materials such as nanoparticles and nanotextures were developed to improve the out-coupling efficiency of photons in LEDs under various frameworks such as waveguides, plasmonic theory, and so forth. In this Perspective, we aim to provide a comprehensive review of the recent progress of research on various light management nanostructures and their potency to improve performance of optoelectronic devices including photodetectors, solar cells, and LEDs.

Programmable nanoengineering templates for fabrication of three-dimensional nanophotonic structures.

Porous anodic alumina membranes (AAMs) have attracted great amount of attention due to their potential application as templates for nanoengineering. Template-guided fabrication and assembly of nanomaterials based on AAMs are cost-effective and scalable methods to program and engineer the shape and morphology of nanostructures and nanomaterials. In this work, perfectly ordered AAMs with the record large pitch up to 3 µm have been fabricated by properly controlling the anodization conditions and utilization of nanoimprint technique. Due to the capability of programmable structural design and fabrication, a variety of nanostructures, including nanopillar arrays, nanotower arrays, and nanocone arrays, have been successfully fabricated using nanoengineered AAM templates. Particularly, amorphous Si nanocones have been fabricated as three-dimensional nanophotonic structures with the characterization of their intriguing optical anti-reflection property. These results directly indicate the potential application of the reported approach for photonics and optoelectronics.

Efficient light absorption with integrated nanopillar/nanowell arrays for three-dimensional thin-film photovoltaic applications.

Efficient light absorption in thin-film photovoltaic (PV) devices is crucial for improving their efficiency and reducing cost. Here we have not only developed a low-cost and scalable method to fabricate a unique type of integrated-nanopillar-nanowell (i-NPW) structure by integrating nanopillar and nanowell arrays together vertically, but also demonstrated the attractive optical property of the i-NPW arrays by leveraging the advantages of "positive" and "negative" nanostructures for photon harvesting. Impressively, the 2 µm thick i-NPW arrays with only 40 nm a-Si coating obtained a day-integrated absorption of 89.27%, as opposed to only 33.45% for the planar control sample. These results suggest the feasibility and clear advantage of vertical integration of three-dimensional (3-D) nanophotonic structures, and meanwhile also pave a viable and convenient way toward a 3-D ultrathin film PV module with potency for high energy conversion efficiency.

Efficient photon capturing with ordered three-dimensional nanowell arrays.

Unique light-matter interaction at nanophotonic regime can be harnessed for designing efficient photonic and optoelectronic devices such as solar cells, lasers, and photodetectors. In this work, periodic photon nanowells are fabricated with a low-cost and scalable approach, followed by systematic investigations of their photon capturing properties combining experiments and simulations. Intriguingly, it is found that a proper periodicity greatly facilitates photon capturing process in the nanowells, primarily owing to optical diffraction. Meanwhile, the nanoengineered morphology renders the nanostructures with a broad-band efficient light absorption. The findings in this work can be utilized to implement a new type of nanostructure-based solar cells. Also, the methodology applied in this work can be generalized to rational design of other types of efficient photon-harvesting devices.

Strong light absorption of self-organized 3-D nanospike arrays for photovoltaic applications.

Three-dimensional (3-D) nanostructures have been widely explored for efficient light trapping; however, many of the nanostructure fabrication processes reported have high cost and/or limited scalability. In this work, self-organized 3-D Al nanospike arrays were successfully fabricated on thin Al foils with controlled nanospike geometry such as height and pitch. Thereafter, photovoltaic materials of a-Si and CdTe thin films were conformally deposited on the nanospikes structures thus forming 3-D nanostructures with strong light absorption over a broad wavelength range and photon incident angle. Specifically, 100 nm-thick CdTe film on nanospikes showed 97% peak absorption, and up to 95% day-integrated sunlight absorption. These results indicate that self-organized 3-D Al nanospike arrays can serve as lightweight and low cost substrates for cost-effective thin film photovoltaics.