Ding-Jiang Xue

Improving the Electrode Performance of Ge through Ge@C Core–Shell Nanoparticles and Graphene Networks

Germanium is a promising high-capacity anode material for lithium ion batteries, but it usually exhibits poor cycling stability because of its huge volume variation during the lithium uptake and release process. A double protection strategy to improve the electrode performance of Ge through the use of Ge@C core-shell nanostructures and reduced graphene oxide (RGO) networks has been developed. The as-synthesized Ge@C/RGO nanocomposite showed excellent cycling performance and rate capability in comparison with Ge@C nanoparticles when used as an anode material for Li ion batteries, which can be attributed to the electronically conductive and elastic RGO networks in addition to the carbon shells and small particle sizes of Ge. The strategy is simple yet very effective, and because of its versatility, it may be extended to other high-capacity electrode materials with large volume variations and low electrical conductivities.

Anisotropic Photoresponse Properties of Single Micrometer-Sized GeSe Nanosheet

Micrometer-sized single-crystal GeSe nanosheets have been synthesized by a solution method. The single GeSe nanosheet exhibits novel anisotropic photoresponse properties in two photodetectors based on individual nanosheet. The on/off switching ratio of the photodetector perpendicular to the nanosheet is 3.5 times higher than that parallel to the nanosheet.

Facile Synthesis of Germanium Nanocrystals and Their Application in Organic–Inorganic Hybrid Photodetectors

lithium-ion batteries, [ 6 , 7 ] and solar cells. [ 8 , 9 ] In particular, germanium NCs have drawn special attention because of its inherent properties: Firstly, Ge is a narrow bandgap semiconductor with a bulk bandgap of 0.67 eV at 300 K, which can be easily tuned by quantization to technologically important wavelengths. Secondly, it has a large exciton Bohr radius ( ≈ 24 nm), which provides a strong quantum confi nement effect [ 10 , 11 ] as well as a large absorption coeffi cient ( ≈ 2 × 10 5 cm − 1 at 2 eV). [ 12 ] Considerable efforts have been recently directed towards the preparation of Ge NCs. The available methods so far include etching, molecular beam epitaxy, plasma-enhanced chemical vapor deposition, and ion implantation, which are characteristically high cost processes and limit the wide applications of Ge NCs. [ 13 ]

Bandgap Engineering of Monodispersed Cu2–xSySe1–y Nanocrystals through Chalcogen Ratio and Crystal Structure

Bandgap engineering is important in light-absorption optimization of nanocrystals (NCs) for applications such as highly efficient solar cells. Herein, a facile one-pot method is developed to synthesize monodispersed ternary alloyed copper sulfide selenide (Cu(2-x)S(y)Se(1-y)) NCs with tunable composition, structure, and morphology. The energy bandgaps can be tuned with the chalcogen ratio, and the crystal structure of the NCs is found to produce an effect on their bandgap and light absorption. The results are significant in bandgap engineering of semiconductor NCs.

General Space-Confined On-Substrate Fabrication of Thickness-Adjustable Hybrid Perovskite Single-Crystalline Thin Films

Organic-inorganic hybrid perovskite single-crystalline thin films (SCTFs) are promising for enhancing photoelectric device performance due to high carrier mobility, long diffusion length, and carrier lifetime. However, bulk perovskite single crystals available today are not suitable for practical device application due to the unfavorable thickness. Herein, we report a facile space-confined solution-processed strategy to on-substrate grow various hybrid perovskite SCTFs in a size of submillimeter with adjustable thicknesses from nano- to micrometers. These SCTFs exhibit photoelectric properties comparable to bulk single crystals with low defect density and good air stability. The clear thickness-dependent colors allow fast visual selection of SCTFs with a suitable thickness for specific device application. The present substrate-independent growth of perovskite SCTFs opens up opportunities for on-chip fabrication of diverse high-performance devices.

Tuning the Fermi-level of TiO2 mesoporous layer by lanthanum doping towards efficient perovskite solar cells

Tuning the band alignment is proved to be an effective way to facilitate carrier transportation and thus enhance the power conversion efficiency (PCE) of solar cells. Doping the compact layer with metal ions or modifying the interfaces among functional layers in perovskite solar cells (PSCs) can appreciably improve the PCE of PSCs. Inspired by the rare earth elemental doping of TiO2, which has witnessed the success in photocatalysis and dye-sensitized solar cells, we firstly demonstrated here that La3+ doping in the mesoporous TiO2 layer of a mesostructured PSC can tune its Fermi level and thus significantly enhance the device PCE. Systematic analysis reveals that doping La3+ into TiO2 raises the Fermi level of TiO2 through scavenging oxygen and inducing vacancies, which subsequently increases the open circuit voltage and the fill factor while reducing the series resistance of the PSC using La3+-doped TiO2 as a mesoporous layer. As a result, a PCE of 15.42% is achieved, which is appreciably higher than the PCE of a device with undoped TiO2 (12.11%).

GeSe Thin-Film Solar Cells Fabricated by Self-Regulated Rapid Thermal Sublimation

GeSe has recently emerged as a promising photovoltaic absorber material due to its attractive optical and electrical properties as well as earth-abundant and low-toxic constituent elements. However, no photovoltaic device has been reported based on this material so far, which could be attributed to the inevitable coexistence of phase impurities Ge and GeSe2, leading to detrimental recombination-center defects and seriously degrading the device performance. Here we overcome this issue by introducing a simple and fast (4.8 μm min-1) rapid thermal sublimation (RTS) process designed according to the sublimation feature of the layered structured GeSe. This new method offers a compelling combination of assisting raw material purification to suppress deleterious phase impurities and preventing the formation of detrimental point defects through congruent sublimation of GeSe, thus providing an in situ self-regulated process to fabricate high quality polycrystalline GeSe films. Solar cells fabricated following this process show a power conversion efficiency of 1.48% with good stability. This preliminary efficiency and high stability, combined with the self-regulated RTS process (also extended to the fabrication of other binary IV-VI chalcogenide films, i.e., GeS), demonstrates the great potential of GeSe for thin-film photovoltaic applications.

Synthesis of Wurtzite Cu2ZnGeSe4 Nanocrystals and their Thermoelectric Properties

An unusual wurtzite phase of Cu2ZnGeSe4 (CZGSe) has been discovered and its corresponding nanocrystals (NCs) were synthesized by using a facile hot-injection solution-phase synthesis method. Moreover, the formation mechanism of this new phase of CZGSe, instead of the typically observed stannite structure, has been investigated in detail, which indicates that wurtzite CZGSe, which represents the kinetic phase, could be prepared by using a kinetic growth process without phase transformation into the thermodynamically stable stannite structure during the colloidal synthesis. In addition, the potential of wurtzite CZGSe as a thermoelectric material is demonstrated by characterizing the thermoelectric properties of as-synthesized wurtzite CZGSe NCs. This work allows for a rational manipulation of the NCs with a desired crystal structure through adjusting the thermodynamics and kinetics without using any additives and, because of its simplicity and versatility, it may be extended to the phase-controlled synthesis of other chalcogenide NCs.

Air-Stable In-Plane Anisotropic GeSe2 for Highly Polarization-Sensitive Photodetection in Short Wave Region

In-plane anisotropic layered materials such as black phosphorus (BP) have emerged as an important class of two-dimensional (2D) materials that bring a new dimension to the properties of 2D materials, hence providing a wide range of opportunities for developing conceptually new device applications. However, all of recently reported anisotropic 2D materials are relatively narrow-bandgap semiconductors (<2 eV), and there has been no report about this type of materials with wide bandgap, restricting the relevant applications such as polarization-sensitive photodetection in short wave region. Here we present a new member of the family, germanium diselenide (GeSe2) with a wide bandgap of 2.74 eV, and systematically investigate the in-plane anisotropic structural, vibrational, electrical, and optical properties from theory to experiment. Photodetectors based on GeSe2 exhibit a highly polarization-sensitive photoresponse in short wave region due to the optical absorption anisotropy induced by in-plane anisotropy in crystal structure. Furthermore, exfoliated GeSe2 flakes show an outstanding stability in ambient air which originates from the high activation energy of oxygen chemisorption on GeSe2 (2.12 eV) through our theoretical calculations, about three times higher than that of BP (0.71 eV). Such unique in-plane anisotropy and wide bandgap, together with high air stability, make GeSe2 a promising candidate for future 2D optoelectronic applications in short wave region.

Polar Solvent Induced Lattice Distortion of Cubic CsPbI3 Nanocubes and Hierarchical Self-Assembly into Orthorhombic Single-Crystalline Nanowires

Despite the recent surge of interest in inorganic lead halide perovskite nanocrystals, there are still significant gaps in their stability disturbance and the understanding of their destabilization, assembly, and growth processes. Here, we discover that polar solvent molecules can induce the lattice distortion of ligand-stabilized cubic CsPbI3, leading to the phase transition into orthorhombic phase, which is unfavorable for photovoltaic applications. Such lattice distortion triggers the dipole moment on CsPbI3 nanocubes, which subsequently initiates the hierarchical self-assembly of CsPbI3 nanocubes into single-crystalline nanowires. The systematic investigations and in situ monitoring on the kinetics of the self-assembly process disclose that the more amount or the stronger polarity of solvent can induce the more rapid self-assembly and phase transition. These results not only elucidate the destabilization mechanism of cubic CsPbI3 nanocrystals, but also open up opportunities to synthesize and store cubic CsPbI3 for their practical applications in photovoltaics and optoelectronics.