Silvija Gradečak

Multi-quantum-well nanowire heterostructures for wavelength-controlled lasers

Rational design and synthesis of nanowires with increasingly complex structures can yield enhanced and/or novel electronic and photonic functions. For example, Ge/Si core/shell nanowires have exhibited substantially higher performance as field-effect transistors and low-temperature quantum devices compared with homogeneous materials, and nano-roughened Si nanowires were recently shown to have an unusually high thermoelectric figure of merit. Here, we report the first multi-quantum-well (MQW) core/shell nanowire heterostructures based on well-defined III-nitride materials that enable lasing over a broad range of wavelengths at room temperature. Transmission electron microscopy studies show that the triangular GaN nanowire cores enable epitaxial and dislocation-free growth of highly uniform (InGaN/GaN)n quantum wells with n=3, 13 and 26 and InGaN well thicknesses of 1-3 nm. Optical excitation of individual MQW nanowire structures yielded lasing with InGaN quantum-well composition-dependent emission from 365 to 494 nm, and threshold dependent on quantum well number, n. Our work demonstrates a new level of complexity in nanowire structures, which potentially can yield free-standing injection nanolasers.

Inorganic–Organic Hybrid Solar Cell: Bridging Quantum Dots to Conjugated Polymer Nanowires

Quantum dots show great promise for fabrication of hybrid bulk heterojunction solar cells with enhanced power conversion efficiency, yet controlling the morphology and interface structure on the nanometer length scale is challenging. Here, we demonstrate quantum dot-based hybrid solar cells with improved electronic interaction between donor and acceptor components, resulting in significant improvement in short-circuit current and open-circuit voltage. CdS quantum dots were bound onto crystalline P3HT nanowires through solvent-assisted grafting and ligand exchange, leading to controlled organic-inorganic phase separation and an improved maximum power conversion efficiency of 4.1% under AM 1.5 solar illumination. Our approach can be applied to a wide range of quantum dots and polymer hybrids and is compatible with solution processing, thereby offering a general scheme for improving the efficiency of nanocrystal hybrid solar cells.

GaN nanowire lasers with low lasing thresholds

We report optically pumped room-temperature lasing in GaN nanowires grown by metalorganic chemical vapor deposition (MOCVD). Electron microscopy images reveal that the nanowires grow along a nonpolar ⟨11-20⟩ direction, have single-crystal structures and triangular cross sections. The nanowires function as free-standing Fabry–Perot cavities with cavity mode spacings that depend inversely on length. Optical excitation studies demonstrate thresholds for stimulated emission of 22kW∕cm2 that are substantially lower than other previously reported GaN nanowires. Key contributions to low threshold lasing in these MOCVD GaN nanowire cavities and the development of electrically pumped GaN nanowire lasers are discussed.

ZnO Nanowire Arrays for Enhanced Photocurrent in PbS Quantum Dot Solar Cells

Vertical arrays of ZnO nanowires can decouple light absorption from carrier collection in PbS quantum dot solar cells and increase power conversion efficiencies by 35%. The resulting ordered bulk heterojunction devices achieve short-circuit current densities in excess of 20 mA cm(-2) and efficiencies of up to 4.9%.

Graphene Cathode-Based ZnO Nanowire Hybrid Solar Cells

Growth of semiconducting nanostructures on graphene would open up opportunities for the development of flexible optoelectronic devices, but challenges remain in preserving the structural and electrical properties of graphene during this process. We demonstrate growth of highly uniform and well-aligned ZnO nanowire arrays on graphene by modifying the graphene surface with conductive polymer interlayers. On the basis of this structure, we then demonstrate graphene cathode-based hybrid solar cells using two different photoactive materials, PbS quantum dots and the conjugated polymer P3HT, with AM 1.5G power conversion efficiencies of 4.2% and 0.5%, respectively, approaching the performance of ITO-based devices with similar architectures. Our method preserves beneficial properties of graphene and demonstrates that it can serve as a viable replacement for ITO in various photovoltaic device configurations.

Toward Efficient Carbon Nanotube/P3HT Solar Cells: Active Layer Morphology, Electrical, and Optical Properties

We demonstrate single-walled carbon nanotube (SWCNT)/P3HT polymer bulk heterojunction solar cells with an AM1.5 efficiency of 0.72%, significantly higher than previously reported (0.05%). A key step in achieving high efficiency is the utilization of semiconducting SWCNTs coated with an ordered P3HT layer to enhance the charge separation and transport in the device active layer. Electrical characteristics of devices with SWCNT concentrations up to 40 wt % were measured and are shown to be strongly dependent on the SWCNT loading. A maximum open circuit voltage was measured for SWCNT concentration of 3 wt % with a value of 1.04 V, higher than expected based on the interface band alignment. Modeling of the open-circuit voltage suggests that despite the large carrier mobility in SWCNTs device power conversion efficiency is governed by carrier recombination. Optical characterization shows that only SWCNT with diameter of 1.3-1.4 nm can contribute to the photocurrent with internal quantum efficiency up to 26%. Our results advance the fundamental understanding and improve the design of efficient polymer/SWCNTs solar cells.

Flexible graphene electrode-based organic photovoltaics with record-high efficiency.

Advancements in the field of flexible high-efficiency solar cells and other optoelectronic devices will strongly depend on the development of electrode materials with good conductivity and flexibility. To address chemical and mechanical instability of currently used indium tin oxide (ITO), graphene has been suggested as a promising flexible transparent electrode but challenges remain in achieving high efficiency of graphene-based polymer solar cells (PSCs) compared to their ITO-based counterparts. Here we demonstrate graphene anode- and cathode-based flexible PSCs with record-high power conversion efficiencies of 6.1 and 7.1%, respectively. The high efficiencies were achieved via thermal treatment of MoO3 electron blocking layer and direct deposition of ZnO electron transporting layer on graphene. We also demonstrate graphene-based flexible PSCs on polyethylene naphthalate substrates and show the device stability under different bending conditions. Our work paves a way to fully graphene electrode-based flexible solar cells using a simple and reproducible process.

Heterojunction Photovoltaics Using GaAs Nanowires and Conjugated Polymers

We demonstrate an organic/inorganic solar cell architecture based on a blend of poly(3-hexylthiophene) (P3HT) and narrow bandgap GaAs nanowires. The measured increase of device photocurrent with increased nanowire loading is correlated with structural ordering within the active layer that enhances charge transport. Coating the GaAs nanowires with TiO(x) shells passivates nanowire surface states and further improves the photovoltaic performance. We find that the P3HT/nanowire cells yield power conversion efficiencies of 2.36% under white LED illumination for devices containing 50 wt % of TiO(x)-coated GaAs nanowires. Our results constitute important progress for the use of nanowires in large area solution processed hybrid photovoltaic cells and provide insight into the role of structural ordering in the device performance.

Controlled Growth of Ternary Alloy Nanowires Using Metalorganic Chemical Vapor Deposition

We report the growth and characterization of ternary AlxGa1- xAs nanowires by metalorganic chemical vapor deposition as a function of temperature and V/III ratio. Transmission electron microscopy and energy dispersive X-ray spectroscopy show that, at high temperatures and high V/III ratios, the nanowires form a core-shell structure with higher Al composition in the nanowire core than in the shell. We develop a growth model that takes into account diffusion of reactants and decomposition rates at the nanowire catalyst and stem to describe the compositional difference and the shell growth rate. Utilizing this model, we have successfully grown compositionally uniform Al0.16Ga0.84As nanowires. The ability to rationally tune the composition of ternary alloy nanowires broadens the application range of nanowires by enabling more complex nanowire heterostructures.

Progress in AlInN–GaN Bragg reflectors: Application to a microcavity light emitting diode

We report on the progress in the growth of highly reflective AlInN-GaN distributed Bragg reflectors deposited by metalorganic vapor phase epitaxy. Al1-xInxN layers with an In content around x similar to 0.17 are lattice-matched to GaN, thus avoiding strain-related issues in the mirror while keeping a high refractive index contrast of about 7%. Consequently, a reflectivity value as high as 99.4% at 450 nm was achieved with a 40-pair crack-free distributed Bragg reflector. We measured an average absorption coefficient alpha [cm(-1)] in the AlInN-GaN Bragg reflectors of 43 +/- 14 cm(-1) at 450 nm and 75 +/- 19 cm(-1) at 400 nm. Application to blue optoelectronics is demonstrated through the growth of an InGaN-GaN microcavity light emitting diode including a 12-pair Al0.82In0.18N-GaN distributed Bragg reflector as bottom mirror. The device exhibits clear microcavity effects, improved directionality in the radiation pattern and an optical output power of 1.7 mW together with a 2.6% external quantum efficiency at 20 mA