Qianglu Lin

High Capacity MoO2/Graphite Oxide Composite Anode for Lithium-Ion Batteries.

Nanostructured MoO2/graphite oxide (GO) composites are synthesized by a simple solvothermal method. X-ray diffraction and transmission electron microscopy analyses show that with the addition of GO and the increase in GO content in the precursor solutions, MoO3 rods change to MoO2 nanorods and then further to MoO2 nanoparticles, and the nanorods or nanoparticles are uniformly distributed on the surface of the GO sheets in the composites. The MoO2/GO composite with 10 wt % GO exhibits a reversible capacity of 720 mAh/g at a current density of 100 mA/g and 560 mAh/g at a high current density of 800 mA/g after 30 cycles. The improved reversible capacity, rate capacity, and cycling performance of the composites are attributed to synergistic reaction between MoO2 and GO.

Enhanced carrier multiplication in engineered quasi-type-II quantum dots

One process limiting the performance of solar cells is rapid cooling (thermalization) of hot carriers generated by higher-energy solar photons. In principle, the thermalization losses can be reduced by converting the kinetic energy of energetic carriers into additional electron-hole pairs via carrier multiplication (CM). While being inefficient in bulk semiconductors this process is enhanced in quantum dots, although not sufficiently high to considerably boost the power output of practical devices. Here we demonstrate that thick-shell PbSe/CdSe nanostructures can show almost a fourfold increase in the CM yield over conventional PbSe quantum dots, accompanied by a considerable reduction of the CM threshold. These structures enhance a valence-band CM channel due to effective capture of energetic holes into long-lived shell-localized states. The attainment of the regime of slowed cooling responsible for CM enhancement is indicated by the development of shell-related emission in the visible observed simultaneously with infrared emission from the core.

Generalized Synthesis of Hybrid Metal–Semiconductor Nanostructures Tunable from the Visible to the Infrared

Hybrid superstructures allow a convenient route to the development of materials with multiple functionalities (e.g., sensor, marker, conductor) out of monofunctional (e.g., excitonic, plasmonic) building blocks. This work describes a general synthetic route to the preparation of metal|dielectric|quantum dot hybrid superstructures that have excitonic and plasmonic resonances independently tunable from the ultraviolet to the mid-infrared spectral region. We demonstrate that structural tuning can be used to control intercomponent coupling leading to the emergence of unique optical properties. We illustrate this capability by demonstrating single- and multicolor emission from coupled systems, and a significant enhancement of two-photon absorption cross sections of quantum dots. Such properties in a robust yet dispersible particle can be useful in a number of applications including bioimaging and microscopy, and in optoelectronic devices, as well as serve as a platform for fundamental studies of metal-semiconductor interactions.

Two-Dimensional V2O5 Sheet Network as Electrode for Lithium-Ion Batteries

Two-dimensional V2O5 and manganese-doped V2O5 sheet network were synthesized by a one-step polymer-assisted chemical solution method and characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, thermal-gravimetric analysis, and galvanostatic discharge-charge analysis. The V2O5 particles were covered with thin carbon layers, which remained after decomposition of the polymer, forming a network-like sheet structure. This V2O5 network exhibits a high capacity of about 300 and 600 mA·h/g at a current density of 100 mA/g when it was used as a cathode and anode, respectively. After doping with 5% molar ratio of manganese, the capacity of the cathode increases from 99 to 165 mA·h/g at a current density of 1 A/g (∼3 C). This unique network structure provides an interconnected transportation pathway for lithium ions. Improvement of electrochemical performance after doping manganese could be attributed to the enhancement of electronic conductivity.

Design and Synthesis of Heterostructured Quantum Dots with Dual Emission in the Visible and Infrared

The unique optical properties exhibited by visible emitting core/shell quantum dots with especially thick shells are the focus of widespread study, but have yet to be realized in infrared (IR)-active nanostructures. We apply an effective-mass model to identify PbSe/CdSe core/shell quantum dots as a promising system for achieving this goal. We then synthesize colloidal PbSe/CdSe quantum dots with shell thicknesses of up to 4 nm that exhibit unusually slow hole intraband relaxation from shell to core states, as evidenced by the emergence of dual emission, i.e., IR photoluminescence from the PbSe core observed simultaneously with visible emission from the CdSe shell. In addition to the large shell thickness, the development of slowed intraband relaxation is facilitated by the existence of a sharp core-shell interface without discernible alloying. Growth of thick shells without interfacial alloying or incidental formation of homogeneous CdSe nanocrystals was accomplished using insights attained via a systematic study of the dynamics of the cation-exchange synthesis of both PbSe/CdSe and the related system PbS/CdS. Finally, we show that the efficiency of the visible photoluminescence can be greatly enhanced by inorganic passivation.

Shape-controlled narrow-gap SnTe nanostructures: From nanocubes to nanorods and nanowires

The rational design and synthesis of narrow-gap colloidal semiconductor nanocrystals (NCs) is an important step toward the next generation of solution-processable photovoltaics, photodetectors, and thermoelectric devices. SnTe NCs are particularly attractive as a Pb-free alternative to NCs of narrow-gap lead chalcogenides. Previous synthetic efforts on SnTe NCs have focused on spherical nanoparticles. Here we report new strategies for synthesis of SnTe NCs with shapes tunable from highly monodisperse nanocubes, to nanorods (NRs) with variable aspect ratios, and finally to long, straight nanowires (NWs). Reaction at high temperature quickly forms thermodynamically favored nanocubes, but low temperatures lead to elongated particles. Transmission electron microscopy studies of reaction products at various stages of the synthesis reveal that the growth and shape-focusing of monodisperse SnTe nanocubes likely involves interparticle ripening, while directional growth of NRs and NWs may be initiated by particle dimerization via oriented attachment.

Structure and magnetotransport properties of epitaxial nanocomposite La0.67Ca0.33MnO3:SrTiO3 thin films grown by a chemical solution approach

Epitaxial La0.67Ca0.33MnO3:SrTiO3 (LCMO:STO) composite thin films have been grown on single crystal LaAlO3(001) substrates by a cost effective polymer-assisted deposition method. Both x-ray diffraction and high-resolution transmission electron microscopy confirm the growth of epitaxial films with an epitaxial relationship between the films and the substrates as (002)film||(002)sub and [202]film||[202]sub. The transport property measurement shows that the STO phase significantly increases the resistivity and enhances the magnetoresistance (MR) effect of LCMO and moves the metal-insulator transition to lower temperatures. For example, the MR values measured at magnetic fields of 0 and 3 T are −44.6% at 255 K for LCMO, −94.2% at 125 K for LCMO:3% STO, and −99.4% at 100 K for LCMO:5% STO, respectively.

Polymer-assisted chemical solution approach to YVO4:Eu nanoparticle networks

Phosphor YVO4:Eu nanoparticle networks were synthesized using water soluble ethylenediaminetetraacetic acid (EDTA) and polyethyleneimine (PEI) as binding ligands. The morphology, particle size, BET surface area, and photoluminescence of YVO4:Eu processed at different annealing temperatures (500, 600, 700, and 800 °C) and EDTA/PEI mass ratios (1 : 4, 1 : 2.5, 1 : 2, 1 : 1.5, 1 : 1, 2 : 1, and 4 : 1) were determined by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, fluorescence spectrophotometer, and N2 adsorption and desorption. The red emission was observed with increasing the annealing temperature. Importantly, the nanoparticles did not aggregate at high annealing temperatures up to 800 °C. The smallest size of the YVO4:Eu nanoparticles is about 18 nm and the surface area is 35 m2 g−1 with the EDTA/PEI mass ratios of 1 : 1–2.5.

Nanoconfined surfactant templated electrodeposition to porous hierarchical nanowires and nanotubes

Porous metal (Pd and Co) and semiconductor (ZnO) nanowires, porous metal (Pt and Ni) nanotubes, and unique multiple Pt nanowires are prepared from a novel nanoconfined surfactant templated electrodeposition approach. More specifically, the overall diameter of nanowires or nanotubes is defined by the pore channels of membranes. Surfactant assembled structure nanoconfined within the pores of membranes is used to generate the porosity and to control the texture of the nanowires or nanotubes. As compared to solid nanowires and nanotubes, the porous nanowires and nanotubes exhibit unique properties. For example, porous cobalt nanowires show higher coercivity.

Phase-Transfer Ligand Exchange of Lead Chalcogenide Quantum Dots for Direct Deposition of Thick, Highly Conductive Films

The use of semiconductor nanocrystal quantum dots (QDs) in optoelectronic devices typically requires postsynthetic chemical surface treatments to enhance electronic coupling between QDs and allow for efficient charge transport in QD films. Despite their importance in solar cells and infrared (IR) light-emitting diodes and photodetectors, advances in these chemical treatments for lead chalcogenide (PbE; E = S, Se, Te) QDs have lagged behind those of, for instance, II-VI semiconductor QDs. Here, we introduce a method for fast and effective ligand exchange for PbE QDs in solution, resulting in QDs completely passivated by a wide range of small anionic ligands. Due to electrostatic stabilization, these QDs are readily dispersible in polar solvents, in which they form highly concentrated solutions that remain stable for months. QDs of all three Pb chalcogenides retain their photoluminescence, allowing for a detailed study of the effect of the surface ionic double layer on electronic passivation of QD surfaces, which we find can be explained using the hard/soft acid-base theory. Importantly, we prepare highly conductive films of PbS, PbSe, and PbTe QDs by directly casting from solution without further chemical treatment, as determined by field-effect transistor measurements. This method allows for precise control over the surface chemistry, and therefore the transport properties of deposited films. It also permits single-step deposition of films of unprecedented thickness via continuous processing techniques, as we demonstrate by preparing a dense, smooth, 5.3-μm-thick PbSe QD film via doctor-blading. As such, it offers important advantages over laborious layer-by-layer methods for solar cells and photodetectors, while opening the door to new possibilities in ionizing-radiation detectors.