Atomic Mechanism of Strain Alleviation and Dislocation Reduction in Highly Mismatched Remote Heteroepitaxy Using a Graphene Interlayer.

Remote heteroepitaxy is known to yield semiconductor films with better quality. However, the atomic mechanisms in systems with large mismatches are still unclear. Herein, low-strain single-crystalline nitride films are achieved on highly mismatched (∼16.3%) sapphire via graphene-assisted remote heteroepitaxy. Because of a weaker interface potential, the in-plane compressive strain at the interface releases by 30%, and dislocations are prevented. Meanwhile, the lattice distortions in the epilayer disappear when the structure climbs over the atomic steps on substrates because graphene renders the steps smooth. In this way, the density of edge dislocations in as-grown nitride films reduces to the same level as that of the screw dislocations, which is rarely observed in heteroepitaxy. Further, the indium composition in InxGa1-xN/GaN multiquantum wells increases to ∼32%, enabling the fabrication of a yellow light-emitting diode. This study demonstrates the advantages of remote heteroepitaxy for bandgap tuning and opens opportunities for photoelectronic and electronic applications.

Quantitative Analyses of the Interfacial Properties of Current Collectors at the Mesoscopic Level in Lithium Ion Batteries by Using Hierarchical Graphene.

At the mesoscopic level of commercial lithium ion battery (LIB), it is widely believed that the poor contacts between current collector (CC) and electrode materials (EM) lead to weak adhesions and large interfacial electric resistances. However, systematic quantitative analyses of the influence of the interfacial properties of CC are still scarce. Here, we built a model interface between CC and electrode materials by directly growing hierarchical graphene films on commercial Al foil CC, and we performed systematic quantitative studies of the interfacial properties therein. Our results show that the interfacial electric resistance dominates, i.e. ∼2 orders of magnitude higher than that of electrode materials. The interfacial resistance could be eliminated by hierarchical graphene interlayer. Cathode on CC with eliminated interfacial resistance could deliver much improved power density outputs. Our work quantifies the mesoscopic factors influencing the battery performance and offers practical guidelines of boosting the performance of LIBs and beyond.

Wearable energy sources based on 2D materials.

Wearable energy sources are in urgent demand due to the rapid development of wearable electronics. Besides flexibility and ultrathin thickness, emerging 2D materials present certain extraordinary properties that surpass the properties of conventional materials, which make them advantageous for high-performance wearable energy sources. Here, we provide a comprehensive review of recent advances in 2D material based wearable energy sources including wearable batteries, supercapacitors, and different types of energy harvesters. The crucial roles of 2D materials in the wearable energy sources are highlighted. Based on the current progress, the existing challenges and future prospects are outlined and discussed.

Graphene-driving strain engineering to enable strain-free epitaxy of AlN film for deep ultraviolet light-emitting diode.

The energy-efficient deep ultraviolet (DUV) optoelectronic devices suffer from critical issues associated with the poor quality and large strain of nitride material system caused by the inherent mismatch of heteroepitaxy. In this work, we have prepared the strain-free AlN film with low dislocation density (DD) by graphene (Gr)-driving strain-pre-store engineering and a unique mechanism of strain-relaxation in quasi-van der Waals (QvdW) epitaxy is presented. The DD in AlN epilayer with Gr exhibits an anomalous sawtooth-like evolution during the whole epitaxy process. Gr can help to enable the annihilation of the dislocations originated from the interface between AlN and Gr/sapphire by impelling a lateral two-dimensional growth mode. Remarkably, it can induce AlN epilayer to pre-store sufficient tensile strain during the early growth stage and thus compensate the compressive strain caused by hetero-mismatch. Therefore, the low-strain state of the DUV light-emitting diode (DUV-LED) epitaxial structure is realized on the strain-free AlN template with Gr. Furthermore, the DUV-LED with Gr demonstrate 2.1 times enhancement of light output power and a better stability of luminous wavelength compared to that on bare sapphire. An in-depth understanding of this work reveals diverse beneficial impacts of Gr on nitride growth and provides a novel strategy of relaxing the vital requirements of hetero-mismatch in conventional heteroepitaxy.

Transfer-Free Quasi-Suspended Graphene Grown on a Si Wafer.

The direct growth of graphene affording wafer-scale uniformity on insulators is paramount to electronic and optoelectronic applications; however, it remains a challenge to date, because it entails an entirely different growth mode than that over metals. Herein, the metal-catalyst-free growth of quasi-suspended graphene on a Si wafer is demonstrated using an interface-decoupling chemical vapor deposition strategy. The employment of lower-than-conventional H2 dosage and concurrent introduction of methanol during growth can effectively weaken the interaction between the synthesized graphene and the underlying substrate. The growth mode can be thus fine-tuned, producing a predominantly monolayer graphene film with wafer-level homogeneity. Graphene thus grown on a 4 inch Si wafer enables the transfer-free fabrication of high-performance graphene-based field-effect transistor arrays that exhibit almost no shift in the charge neutral point, indicating a quasi-suspended feature of the graphene. Moreover, a carrier mobility up to 15 000 cm2 V-1 s-1 can be attained. This study is anticipated to offer meaningful insights into the synthesis of wafer-scale high-quality graphene on dielectrics for practical graphene devices.

Copper acetate-facilitated transfer-free growth of high-quality graphene for hydrovoltaic generators.

Direct synthesis of high-quality graphene on dielectric substrates without a transfer process is of vital importance for a variety of applications. Current strategies for boosting high-quality graphene growth, such as remote metal catalyzation, are limited by poor performance with respect to the release of metal catalysts and hence suffer from a problem with metal residues. Herein, we report an effective approach that utilizes a metal-containing species, copper acetate, to continuously supply copper clusters in a gaseous form to aid transfer-free growth of graphene over a wafer scale. The thus-derived graphene films were found to show reduced multilayer density and improved electrical performance and exhibited a carrier mobility of 8500 cm2 V-1 s-1. Furthermore, droplet-based hydrovoltaic electricity generator devices based on directly grown graphene were found to exhibit robust voltage output and long cyclic stability, in stark contrast to their counterparts based on transferred graphene, demonstrating the potential for emerging energy harvesting applications. The work presented here offers a promising solution to organize the metal catalytic booster toward transfer-free synthesis of high-quality graphene and enable smart energy generation.

Direct growth of wafer-scale highly oriented graphene on sapphire.

Direct chemical vapor deposition (CVD) growth of wafer-scale high-quality graphene on dielectrics is of paramount importance for versatile applications. Nevertheless, the synthesized graphene is typically a polycrystalline film with high density of uncontrolled defects, resulting in a low carrier mobility and high sheet resistance. Here, we report the direct growth of highly oriented monolayer graphene films on sapphire wafers. Our growth strategy is achieved by designing an electromagnetic induction heating CVD operated at elevated temperature, where the high pyrolysis and migration barriers of carbon species are easily overcome. Meanwhile, the embryonic graphene domains are guided into good alignment by minimizing its configuration energy. The thus obtained graphene film accordingly manifests a markedly improved carrier mobility (~14,700 square centimeters per volt per second at 4 kelvin) and reduced sheet resistance (~587 ohms per square), which compare favorably with those from catalytic growth on polycrystalline metal foils and epitaxial growth on silicon carbide.

Transfer-Medium-Free Nanofiber-Reinforced Graphene Film and Applications in Wearable Transparent Pressure Sensors.

Graphene exhibits properties of atomic thickness, high transparency, and high carrier mobility, which is highly desirable for a flexible transparent conductive material. However, the electronic properties of large-area chemical vapor deposition grown graphene film suffer from insulated polymer contaminations introduced by the transfer process and the easily cracked nature. Here, we report a preparation method of a transfer-medium-free large-area nanofiber-reinforced graphene (a-PAN/G) film simply by annealing the electrostatically spun polyacrylonitrile (PAN) nanofibers on the graphene film. The film could be free-standing on water and suspended in air with high transparency and enhanced electrical and mechanical properties compared to that of a monolayer graphene film. The flexible transparent a-PAN/G films were demonstrated as active materials for sensitive pressure sensors. The obtained pressure sensors demonstrate high sensitivity (44.5 kPa-1 within 1.2 kPa), low operating voltage (0.01-0.5 V), and excellent stability for 5500 loading-unloading cycles, revealing promising potential applications in wearable electronics.

Hierarchical Graphene Foam for Efficient Omnidirectional Solar-Thermal Energy Conversion.

Efficient solar-thermal energy conversion is essential for the harvesting and transformation of abundant solar energy, leading to the exploration and design of efficient solar-thermal materials. Carbon-based materials, especially graphene, have the advantages of broadband absorption and excellent photothermal properties, and hold promise for solar-thermal energy conversion. However, to date, graphene-based solar-thermal materials with superior omnidirectional light harvesting performances remain elusive. Herein, hierarchical graphene foam (h-G foam) with continuous porosity grown via plasma-enhanced chemical vapor deposition is reported, showing dramatic enhancement of broadband and omnidirectional absorption of sunlight, which thereby can enable a considerable elevation of temperature. Used as a heating material, the external solar-thermal energy conversion efficiency of the h-G foam impressively reaches up to ≈93.4%, and the solar-vapor conversion efficiency exceeds 90% for seawater desalination with high endurance.

Graphene-Armored Aluminum Foil with Enhanced Anticorrosion Performance as Current Collectors for Lithium-Ion Battery.

Aluminum (Al) foil, as the most accepted cathode current collector for lithium-ion batteries (LIBs), is susceptible to local anodic corrosions during long-term operations. Such corrosions could lead to the deterioration or even premature failure of the batteries and are generally believed to be a bottleneck for next-generation 5 V LIBs. Here, it is demonstrated that Al foil armored by conformal graphene coating exhibits significantly reinforced anodic corrosion resistance in both LiPF6 and lithium bis(trifluoromethanesulphonyl) imide (LiTFSI) based electrolytes. Moreover, LiMn2 O4 cells using graphene-armored Al foil as current collectors (LMO/GA) demonstrate enhanced electrochemical performance in comparison with those using pristine Al foil (LMO/PA). The long-term discharge capacity retention of LMO/GA cell after ≈950 h straight operations at low rate (0.5 C) reaches up to 91%, remarkably superior to LMO/PA cell (75%). The self-discharge propensity of LMO/GA is clearly relieved and the rate/power performance is also improved with graphene mediations. This work not only contributes to the long-term stable operations of LIBs but also might catalyze the deployment of 5 V LIBs in the future.