An 8.68% Efficiency Chemically-Doped-Free Graphene–Silicon Solar Cell Using Silver Nanowires Network Buried Contacts

Graphene–silicon (Gr-Si) heterojunction solar cells have been recognized as one of the most low-cost candidates in photovoltaics due to its simple fabrication process. However, the high sheet resistance of chemical vapor deposited (CVD) Gr films is still the most important limiting factor for the improvement of the power conversion efficiency of Gr-Si solar cells, especially in the case of large device-active area. In this work, we have fabricated a novel transparent conductive film by hybriding a monolayer Gr film with silver nanowires (AgNWs) network soldered by the graphene oxide (GO) flakes. This Gr-AgNWs hybrid film exhibits low sheet resistance and larger direct-current to optical conductivity ratio, quite suitable for solar cell fabrication. An efficiency of 8.68% has been achieved for the Gr-AgNWs-Si solar cell, in which the AgNWs network acts as buried contacts. Meanwhile, the Gr-AgNWs-Si solar cells have much better stability than the chemically doped Gr-Si solar cells. These results show a new route for the fabrication of high efficient and stable Gr-Si solar cells

Silver Nanoshell Plasmonically Controlled Emission of Semiconductor Quantum Dots in the Strong Coupling Regime

Strong coupling between semiconductor excitons and localized surface plasmons (LSPs) giving rise to hybridized plexciton states in which energy is coherently and reversibly exchanged between the components is vital, especially in the area of quantum information processing from fundamental and practical points of view. Here, in photoluminescence spectra, rather than from common extinction or reflection measurements, we report on the direct observation of Rabi splitting of approximately 160 meV as an indication of strong coupling between excited states of CdSe/ZnS quantum dots (QDs) and LSP modes of silver nanoshells under nonresonant nanosecond pulsed laser excitation at room temperature. The strong coupling manifests itself as an anticrossing-like behavior of the two newly formed polaritons when tuning the silver nanoshell plasmon energies across the exciton line of the QDs. Further analysis substantiates the essentiality of high pump energy and collective strong coupling of many QDs with the radiative dipole mode of the metallic nanoparticles for the realization of strong coupling. Our finding opens up interesting directions for the investigation of strong coupling between LSPs and excitons from the perspective of radiative recombination under easily accessible experimental conditions

Chemical Vapor Deposition of Graphene on Self-Limited SiC Interfacial Layers Formed on Silicon Substrates for Heterojunction Devices

Direct chemical vapor deposition (CVD) of graphene on any desired substrate is always required to manufacture high-quality heterojunctions with excellent interfacial properties. Herein, the growth of graphene on cubic-silicon carbide (3C-SiC) surfaces using conventional high-temperature direct thermal CVD and plasma-enhanced CVD (PECVD) is explored, which is hardly reported to date. Since 3C-SiC substrates are not available, the controlled self-limited 3C-SiC layers on the Si(100) substrates were grown at different temperatures (900–1200 °C) via thermal-CVD technique to obtain virtual 3C-SiC substrates. The direct production of graphene via thermal CVD could not be achieved on such 3C-SiC surfaces. The density functional theory and molecular dynamics simulations confirm that the carbon atom diffusion over the 3C-SiC surface is extremely low, like over the Si surface, which leads to no graphene growth. A similar growth mechanism may be attributed to their similar crystal structure viz diamond cubic for Si and zinc blend for 3C-SiC. However, graphene nanowalls (GNWs) were successfully grown on both Si and 3C-SiC/Si surfaces at 700 °C via the PECVD technique, where similar surface morphologies were observed because the growth mechanism of GNWs is independent of substrate type. Moreover, I–V characterization was performed for different SiC/Si heterostructures and their corresponding GNWs/SiC/Si heterostructures, respectively. The current conduction improved considerably more for GNW/SiC/Si heterostructures as compared to SiC/Si heterostructures, but the creation of a SiC interfacial layer as well as its quality affected the conductivity of GNWs/SiC/Si heterostructures. The inevitable formation of an interfacial SiC layer during the direct graphene growth via thermal CVD on Si substrates can seriously affect the performance of graphene/Si heterojunction devices. Hence, PECVD growth of graphene is an ideal option to fabricate graphene/Si heterojunction devices with excellent interfacial properties or graphene/3C-SiC/Si heterojunction devices for various electronic/optoelectronic applications such as gas sensors and photovoltaic devices

Epitaxial Growth of Twinned Au–Pt Core–Shell Star-Shaped Decahedra as Highly Durable Electrocatalysts

Pt epitaxial layer on a nanoparticle with twinned structure and well-defined shape is highly desirable in order to achieve high performance in both catalytic activity and durability toward oxygen reduction reaction (ORR). However, it remains tremendously challenging to produce conformal, heterogeneous, twinned nanostructures due to the high internal strain and surface energy of Pt. In addition, these twinned nanostructures may be subject to degradation in highly corrosive ORR environments due to the high energy of twin boundary. Here we report the synthesis of Au–Pt core–shell star-shaped decahedra bounded mainly by {111} facets, in which Pt shells with controlled thickness epitaxially grew on Au cores with a 5-fold twinned structure. The incorporation of the amine group decreases the surface energy of Pt by strong adsorption and thus facilitates the epitaxial growth of Pt on Au core instead of the dendritic growth. In addition, Br^– ion could largely stabilize the {111} facets of Pt, which prevent the formation of spherical nanoparticles. The Au–Pt core–shell decahedra with thicker Pt shell exhibited enhanced ORR properties in terms of activity and durability. Specifically, AuPt_1.03 star-shaped decahedra achieved the highest mass activity (0.94 mA/μg_Pt) and area activity (1.09 mA/cm²_Pt), which is ∼6.7 and 5 times, respectively, as high as those of the commercial Pt/C (ETEK). Significantly, such star-shaped decahedra were highly stable with ∼10% loss in area activity and ∼20% loss in mass activity after 30 000 CV cycles in O₂ saturated acid solution

Ambient Engineering for High-Performance Organic–Inorganic Perovskite Hybrid Solar Cells

Considering the evaporation of solvents during fabrication of perovskite films, the organic ambience will present a significant influence on the morphologies and properties of perovskite films. To clarify this issue, various ambiences of <i>N</i>,<i>N</i>-dimethylformamide (DMF), dimethyl sulfoxide (DMSO), and chlorobenzene (CBZ) are introduced during fabrication of perovskite films by two-step sequential deposition method. The results reveal that an ambient CBZ atmosphere is favorable to control the nucleation and growth of CH₃NH₃PbI₃ grains while the others present a negative effect. The statistical results show that the average efficiencies of perovskite solar cells processed in an ambient CBZ atmosphere can be significantly improved by a relatively average value of 35%, compared with those processed under air. The efficiency of the best perovskite solar cells can be improved from 10.65% to 14.55% by introducing this ambience engineering technology. The CH₃NH₃PbI₃ film with large-size grains produced in an ambient CBZ atmosphere can effectively reduce the density of grain boundaries, and then the recombination centers for photoinduced carriers. Therefore, a higher short-circuit current density is achieved, which makes main contribution to the improvement in efficiency. These results provide vital progress toward understanding the role of ambience in the realization of highly efficient perovskite solar cells

Multistage Transformation and Lattice Fluctuation at AgCl–Ag Interface

Solid-state transformation between different materials is often accompanied by mechanical expansion and compression due to their volume change and structural evolution at interfaces. However, these two types of dynamics are usually difficult to monitor in the same time. In this work, we use in situ transmission electron microscopy to directly study the reduction transformation at the AgCl–Ag interface. Three stages of lattice fluctuations were identified and correlated to the structural evolution. During the steady state, a quasi-layered growth mode of Ag in both vertical and lateral directions were observed due to the confinement of AgCl lattices. The development of planar defects and depletion of AgCl are respectively associated with lattice compression and relaxation. Topography and structure of decomposing AgCl was further monitored by in situ scanning transmission electron microscopy. Silver species are suggested to originate from both the surface and the interior of AgCl, and be transported to the interface. Such mass transport may have enabled the steady state and lattice compression in this volume-shrinking transformation

Multistage Transformation and Lattice Fluctuation at AgCl–Ag Interface

Solid-state transformation between different materials is often accompanied by mechanical expansion and compression due to their volume change and structural evolution at interfaces. However, these two types of dynamics are usually difficult to monitor in the same time. In this work, we use in situ transmission electron microscopy to directly study the reduction transformation at the AgCl–Ag interface. Three stages of lattice fluctuations were identified and correlated to the structural evolution. During the steady state, a quasi-layered growth mode of Ag in both vertical and lateral directions were observed due to the confinement of AgCl lattices. The development of planar defects and depletion of AgCl are respectively associated with lattice compression and relaxation. Topography and structure of decomposing AgCl was further monitored by in situ scanning transmission electron microscopy. Silver species are suggested to originate from both the surface and the interior of AgCl, and be transported to the interface. Such mass transport may have enabled the steady state and lattice compression in this volume-shrinking transformation

Light-Emitting Diodes Based on Colloidal Silicon Quantum Dots with Octyl and Phenylpropyl Ligands

Colloidal silicon quantum dots (Si QDs) hold ever-growing promise for the development of novel optoelectronic devices such as light-emitting diodes (LEDs). Although it has been proposed that ligands at the surface of colloidal Si QDs may significantly impact the performance of LEDs based on colloidal Si QDs, little systematic work has been carried out to compare the performance of LEDs that are fabricated using colloidal Si QDs with different ligands. Here, colloidal Si QDs with rather short octyl ligands (Octyl-Si QDs) and phenylpropyl ligands (PhPr-Si QDs) are employed for the fabrication of LEDs. It is found that the optical power density of PhPr-Si QD LEDs is larger than that of Octyl-Si QD LEDs. This is due to the fact that the surface of PhPr-Si QDs is more oxidized and less defective than that of Octyl-Si QDs. Moreover, the benzene rings of phenylpropyl ligands significantly enhance the electron transport of QD LEDs. It is interesting that the external quantum efficiency (EQE) of PhPr-Si QD LEDs is lower than that of Octyl-Si QD LEDs because the benzene rings of phenylpropyl ligands suppress the hole transport of QD LEDs. The unbalance between the electron and hole injection in PhPr-Si QD LEDs is more serious than that in Octyl-Si QD LEDs. The currently obtained highest optical power density of ∼0.64 mW/cm² from PhPr-Si QD LEDs and highest EQE of ∼6.2% from Octyl-Si QD LEDs should encourage efforts to further advance the development of high-performance optoelectronic devices based on colloidal Si QDs

Multistage Transformation and Lattice Fluctuation at AgCl–Ag Interface

Solid-state transformation between different materials is often accompanied by mechanical expansion and compression due to their volume change and structural evolution at interfaces. However, these two types of dynamics are usually difficult to monitor in the same time. In this work, we use in situ transmission electron microscopy to directly study the reduction transformation at the AgCl–Ag interface. Three stages of lattice fluctuations were identified and correlated to the structural evolution. During the steady state, a quasi-layered growth mode of Ag in both vertical and lateral directions were observed due to the confinement of AgCl lattices. The development of planar defects and depletion of AgCl are respectively associated with lattice compression and relaxation. Topography and structure of decomposing AgCl was further monitored by in situ scanning transmission electron microscopy. Silver species are suggested to originate from both the surface and the interior of AgCl, and be transported to the interface. Such mass transport may have enabled the steady state and lattice compression in this volume-shrinking transformation

In situ Study of Oxidative Etching of Palladium Nanocrystals by Liquid Cell Electron Microscopy

Oxidative etching has widely prevailed in the synthesis of a crystal and played a critical role in determining the final growth behavior. In this Letter, we report an in situ microscopic study on the oxidative etching of palladium cubic nanocrystals by liquid cell scanning transmission electron microscopy. The etching was realized with oxidative radiation reactants from electron–water interaction in the presence of Br^– ions. Dissolution dynamics of monodispersed and aggregated nanocrystals were both investigated and compared. Analyses on the dissolution kinetics of nanocrystals and the diffusion kinetics of the dissolved agents were carried out based on the scanning transmission electron microscopy characterizations. The results presented here pave a way toward the quantitative understanding of the oxidative etching reaction and its application in the functionally orientated fabrication of nanocrystals with certain sizes, structures, and morphologies