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Organic–inorganic hybrid perovskites have electronic and optoelectronic properties that make them appealing in many device applications1–4. Although many approaches focus on polycrystalline materials5–7, single-crystal hybrid perovskites show improved carrier transport and enhanced stability over their polycrystalline counterparts, due to their orientation-dependent transport behaviour8–10 and lower defect concentrations11,12. However, the fabrication of single-crystal hybrid perovskites, and controlling their morphology and composition, are challenging12. Here we report a solution-based lithography-assisted epitaxial-growth-and-transfer method for fabricating single-crystal hybrid perovskites on arbitrary substrates, with precise control of their thickness (from about 600 nanometres to about 100 micrometres), area (continuous thin films up to about 5.5 centimetres by 5.5 centimetres), and composition gradient in the thickness direction (for example, from methylammonium lead iodide, MAPbI3, to MAPb0.5Sn0.5I3). The transferred single-crystal hybrid perovskites are of comparable quality to those directly grown on epitaxial substrates, and are mechanically flexible depending on the thickness. Lead–tin gradient alloying allows the formation of a graded electronic bandgap, which increases the carrier mobility and impedes carrier recombination. Devices based on these single-crystal hybrid perovskites show not only high stability against various degradation factors but also good performance (for example, solar cells based on lead–tin-gradient structures with an average efficiency of 18.77 per cent). A solution-based lithography-assisted epitaxial-growth-and-transfer method is used to fabricate single-crystal hybrid perovskites on any surface, with precise control of the thickness, area and chemical composition gradient.

The ever-increasing demand for faster, smaller, and energy-efficient devices has pushed the frontiers of research toward silicon photonics to meet the challenges for fabricating the next generation of computing systems. In order to design new devices at the nanoscale, it is important to understand and be able to control material properties, which may differ significantly from their bulk counterparts. Here, we demonstrate very large tunability of phonon-photon interactions in Si nanowire cavities by engineering the cavity mode at the emission wavelength. Raman scattering measurements performed to quantify these interactions reveal that the anti-Stokes to Stokes scattering ratio can vary from 0.035 to 0.405 in Si nanowires compared to a value of 0.1 for bulk Si, demonstrating tunability by over an order of magnitude. Moreover, a ratio of 0.85 was attained at a temperature of 580 K, which is the highest value ever reported for Si. Cavity modes that can be easily changed by changing the nanowire diameter, cavity geometry, or excitation wavelength provide efficient ways of tuning these interactions. Nanocavity engineering offers a new approach for tuning phonon-photon interactions in silicon and opens up new avenues of research and applications in the fields of silicon photonics, Raman lasers, telecommunication, and optical cooling.

Nanowire transistors are typically undoped devices whose characteristics depend strongly on the injection of carriers from the electrical contacts. In this letter, we fabricate and characterize SiGe nanowire transistors with an n-p-n doping profile and with a top gate covering only the p-doped section of the nanowire. For each device, we locate the p-segment with scanning capacitance microscopy, where the p-segment position varies along the channel due to the stochastic nature of our dropcast fabrication technique. The current–voltage characteristics for a series of transistors with different gate positions reveal that the on/off ratios for electrons is the highest when the gated p-type section is closest to the source contact, whereas the on/off ratios for holes is the highest when the gated p-type section is closest to the drain contact.

Introducing interfaces through heterostructuring is a common strategy to bring novel functionalities and improve device performances. Emerging nanomaterials, of which heterostructuring is under development, can be utilized with combinations of various conventional semiconductors, such as Si, Ge, and compound semiconductors. I’ll present recent achievements of fabrication of hybrid architectures composed of 2D and conventional materials. The experimental approach was epitaxial growth Si, Ge, and ZnO on various 2D materials including graphene, hexagonal boron nitride, transition metal dichalcogenides. Van der Waals and remote epitaxy techniques were employed. Details of nucleation control, charge transfer in hybrid architectures, and insight of device applications will be discussed.

Strong interactions between excitons are a characteristic feature of two-dimensional (2D) semiconductors, determining important excitonic properties, such as exciton lifetime, coherence, and photon-emission efficiency. Rhenium disulfide ($\mathrm{Re}{\mathrm{S}}_{2}$), a member of the 2D transition-metal dichalcogenide (TMD) family, has recently attracted great attention due to its unique excitons that exhibit excellent polarization selectivity and coherence features. However, an in-depth understanding of exciton-exciton interactions in $\mathrm{Re}{\mathrm{S}}_{2}$ is still lacking. Here we used ultrafast pump-probe spectroscopy to study exciton-exciton interactions in monolayer (1L), bilayer (2L), and triple layer $\mathrm{Re}{\mathrm{S}}_{2}$. We directly measure the rate of exciton-exciton annihilation, a representative Auger-type interaction between excitons. It decreases with increasing layer number, as observed in other 2D TMDs. However, while other TMDs exhibit a sharp weakening of exciton-exciton annihilation between 1L and 2L, such behavior was not observed in $\mathrm{Re}{\mathrm{S}}_{2}$. We attribute this distinct feature in $\mathrm{Re}{\mathrm{S}}_{2}$ to the relatively weak interlayer coupling, which prohibits a substantial change in the electronic structure when the thickness varies. This work not only highlights the unique excitonic properties of $\mathrm{Re}{\mathrm{S}}_{2}$ but also provides novel insight into the thickness dependence of exciton-exciton interactions in 2D systems.

Si/Ge core/shell nanowire heterostructures have been expected to provide high energy and power densities for lithium ion battery anodes due to the large capacity of Si and the high electrical and ionic conductivities of Ge. Although the battery anode performances of Si/Ge core/shell nanowire heterostructures have been characterized, the degradation of Si/Ge core/shell nanowire heterostructures has not been thoroughly investigated. Here we report the compositional and structural changes of the Si/Ge core/shell nanowire heterostructure over cycling of lithiation and delithiation at different charging rates. The Si/Ge core/shell nanowire heterostructure holds the core and shell structure at a charging rate of 0.8 A g−1 up to 50 cycles. On the other hand, compositional intermixing and loss of Si occur at a charging rate of 20 A g−1 within 50 cycles. The operation condition-dependent degradation provides a new aspect of materials research for the development of high performance lithium ion battery anodes with a long cycle life.

Two-dimensional atomic layered materials (2d-ALMs) are emerging candidates for use as epitaxial seed substrates for transferrable epilayers. However, the micrometer-sized domains of 2d-ALMs preclude their practical use in epitaxy because they cause crystallographically in-plane disordering of the overlayer. Ultrathin graphene can penetrate the electric dipole momentum from an underlying crystal layer to the graphene surface, which then drives it to crystallize the overlayer during the initial growth stage, thus resulting in substantial energy saving. This study demonstrates the remote homoepitaxy of ZnO microrods (MRs) on ZnO substrates across graphene layers via a hydrothermal method. Despite the presence of poly-domain graphene in between the ZnO substrate and ZnO MRs, the MRs were epitaxially grown on a- and c-plane ZnO substrates, whose in-plane alignments were homogeneous within the wafer's size. Transmission electron microscopy revealed a homoepitaxial relationship between the overlayer MRs and the substrate. Density-functional theory calculations suggested that the charge redistribution occurring near graphene induces the electric dipole formation, so the attracted adatoms led to the formation of the remote homoepitaxial overlayer. Due to a strong potential field caused by long-range charge transfer given from the substrate, even the use of bi-layer and tri-layer graphene resulted in remote homoepitaxial ZnO MRs. The effects of substrate crystal planes were also theoretically and empirically investigated. The ability of graphene, which can be released from the mother substrate without covalent bonds, was utilized to transfer the overlayer MR arrays. This method opens a way for producing well aligned, transferrable epitaxial nano/microstructure arrays while regenerating the substrate for cost-saving device manufacturing.

Recent advances in 3D/2D heterostructures have opened up tremendous opportunities in building highly flexible and durable optoelectronic devices. However, the inherit lack of interfacial bonding and low surface energy of van der Waals surfaces limit the nucleation and growth of 3D materials. Enhancing wettability by providing a porous buffer is effective in growing compound semiconductors on graphene while van der Waals epitaxy of Ge remains challenging. Here, the nucleation of Ge has been significantly improved from an islanded mode to granular modes by using a TiN/AlN multilayered buffer prior to Ge/graphene integration. Highly textured Ge growth with dominating (111), (220), and (311) peaks are identified by x-ray diffraction. The microstructure of the buffer TiN/AlN demonstrates a polycrystalline quality with clean interfaces between each interlayer and the substrate. Kelvin probe force microscopy measurements along the lateral TiN/AlN interface identify a potential drop corresponding to the AlN phase. This contact potential difference between TiN and AlN is the key in generating the out-of-plane dipole moment that modifies the surface energy of the monolayer graphene, resulting in enhanced wettability of the Ge adatoms nucleated on top. Surface dipole induced nucleation of 3D semiconductor thin films on 2D materials via the proper design of buffer layer is fundamentally important to enhance the 3D/2D growth toward flexible optoelectronic applications.

Two-dimensional (2D) materials as contacts for semiconductor devices have attracted much attention due to minimizing Fermi level pinning. Schottky–Mott physics has been widely employed to design 2D material-based electrodes and to elucidate their contact behavior. In this study, we revealed that charge transfer across a 2D/semiconductor heterointerface and materials characteristics besides work function should be accounted for in fabrication of electrodes based on 2D materials. Our density functional theory (DFT) calculations predicted that charge transfer between ZnO and NbSe2 lowers the barrier height at the heterojunction and that conductive surface states of ZnO provide an additional conduction channel in the ZnO/NbSe2 heterostructures. Crystalline ZnO/NbSe2 heterostructures were prepared by the hydrothermal method. Electrical characterizations of the ZnO/NbSe2 heterostructures showed Ohmic-like behavior as predicted by the DFT calculations, opposed to the prediction based on the Schottky–Mott model.

We report on strain-induced structural defect formation in core Si nanowires of a Si/Ge core/shell nanowire heterostructure and the influence of the structural defects on the electrochemical performances in lithium-ion battery anodes based on Si/Ge core/shell nanowire heterostructures. The induced structural defects consisting of stacking faults and dislocations in the core Si nanowire were observed for the first time. The generation of stacking faults in the Si/Ge core/shell nanowire heterostructure is observed to prefer settling in either only the Ge shell region or in both the Ge shell and Si core regions and is associated with the increase of the shell volume fraction. The relaxation of the misfit strain in the [112] oriented core/shell nanowire heterostructure leads to subsequent gliding of Shockley partial dislocations, preferentially forming the twins. The observation of crossover of defect formation is of great importance for understanding heteroepitaxy in radial heterostructures at the nanoscale and for building three dimensional heterostructures for the various applications. Furthermore, the effect of the defect formation on the nanomaterial's functionality is investigated using electrochemical performance tests. The Si/Ge core/shell nanowire heterostructures enhance the gravimetric capacity of lithium ion battery anodes under fast charging/discharging rates compared to Si nanowires. However, the induced structural defects hamper lithiation of the Si/Ge core/shell nanowire heterostructure.

Remote epitaxy enables to fabricate flexible GaN micro-LED sticker releasable from wafer., There have been rapidly increasing demands for flexible lighting apparatus, and micrometer-scale light-emitting diodes (LEDs) are regarded as one of the promising lighting sources for deformable device applications. Herein, we demonstrate a method of creating a deformable LED, based on remote heteroepitaxy of GaN microrod (MR) p-n junction arrays on c-Al2O3 wafer across graphene. The use of graphene allows the transfer of MR LED arrays onto a copper plate, and spatially separate MR arrays offer ideal device geometry suitable for deformable LED in various shapes without serious device performance degradation. Moreover, remote heteroepitaxy also allows the wafer to be reused, allowing reproducible production of MR LEDs using a single substrate without noticeable device degradation. The remote heteroepitaxial relation is determined by high-resolution scanning transmission electron microscopy, and the density functional theory simulations clarify how the remote heteroepitaxy is made possible through graphene.

Silicon photonics has been a very active area of research especially in the past two decades in order to meet the ever-increasing demand for more computational power and faster device speeds and their natural compatibility with complementary metal-oxide semiconductor. In order to develop Si as a useful photonics material, essential photonic components such as light sources, waveguides, wavelength convertors, modulators, and detectors need to be developed and integrated. However, due to the indirect electronic bandgap of Si, conventional light emission devices such as light-emitting diodes and lasers cannot be built. Therefore, there has been considerable interest in developing Si-based Raman lasers, which are nonlinear devices and require large stimulated Raman scattering (SRS) in an optical cavity. However, due to the low quantum yield of SRS in Si, Raman lasers have very large device footprints and high lasing threshold, making them unsuitable for faster, smaller, and energy-efficient devices. Here, we report strong SRS and extremely high Raman gain in Si nanowire optical cavities in the visible region with measured SRS threshold as low as 30 kW/cm2. At cavity mode resonance, light is confined into a low mode volume and high intensity electromagnetic mode inside the Si nanowire due to its high refractive index, which leads to strong SRS at low pump intensities. Electromagnetic calculations reveal greater than 6 orders of magnitude increase in Raman gain coefficient at 532 nm pump wavelength, compared to the gain value at 1.55 μm wavelength reported in literature, despite the 108 higher losses at 532 nm. Because of the high gain in such small structures, we believe that this is a significant first step in realizing a monolithically integrable nanoscale low-powered Si Raman laser.

All-optical camera, converting X-rays into visible photons, is a promising strategy for high-performance X-ray imaging detector requiring high detection efficiency and ultrafast detector response time. Zinc oxide is a suitable material for all-optical camera due to its fast radiative recombination lifetime in sub-nanosecond regime and its radiation hardness. ZnO nanostructures have been considered as proper building blocks for ultrafast detectors with spatial resolution in sub-micrometer scale. To achieve remarkable enhancement of luminescence efficiency n-type doping in ZnO has been employed. However, luminescence dynamics of doped ZnO nanostructures have not been thoroughly investigated whereas undoped ZnO nanostructures have been employed to study their luminescence dynamics. Here we report a study of luminescence dynamics of hydrogen doped ZnO nanowires obtained by hydrogen plasma treatment. Hydrogen doping in ZnO nanowires gives rise to significant increase in the near-band-edge emission of ZnO and decrease in averaged photoluminescence lifetime from 300 to 140 ps at 10 K. The effects of hydrogen doping on the luminescent characteristics of ZnO nanowires were changed by hydrogen doping process variables.

Author(s): Ro, Yun Goo; Chen, Renjie; Liu, Ren; Li, Nan; Williamson, Theodore; Yoo, Jinkyoung; Sim, Sangwan; Prasankumar, Rohit P; Dayeh, Shadi A

International audience; State-of-the-art light emitting diodes (LEDs) are made from high-purity alloys of III-V semiconductors or small molecules, but high fabrication cost and conplicated synthetic process have limited their widespread use for large area solid-state lighting applications. Here we report efficient and stable LEDs processed from solution with tunable color enabled by using phase-pure two-dimensional (2D) Ruddlesden-Popper (RP) layered perovskites with a formula (CH3(CH2)3NH3)2(CH3NH3)n-1PbnI3n+1 (n=3-5 in this report). By using controlled vertically oriented of crystal in the thin-films that facilitate efficient charge injection and transport, we obtain efficient electroluminescence with a radiance of 35 W Sr-1 cm-2 at 744 nm with an ultra-low turn-on voltage of 1V. Finally, operational stability tests suggest that phase purity is strongly correlated to stability. Phase-pure 2D perovskites exhibit >14 hours of stable operation at peak operating conditions with no droop at current-densities of several Amperes/cm2 in comparison to mixtures of 2D/3D mixture or 3D perovskites, which degrade within minutes.

ZnO radial p–n junction architecture has the potential for forward-leap of light-emitting diode (LED) technology in terms of higher efficacy and economical production. We report on ZnO radial p–n junction-based light emitting diodes prepared by full metalorganic chemical vapour deposition (MOCVD) with hydrogen-assisted p-type doping approach. The p-type ZnO(P) thin films were prepared by MOCVD with the precursors of dimethylzinc, tert-butanol, and tertiarybutylphosphine. Controlling the precursor flow for dopant results in the systematic change of doping concentration, Hall mobility, and electrical conductivity. Moreover, the approach of hydrogen-assisted phosphorous doping in ZnO expands the understanding of doping behaviour in ZnO. Ultraviolet and visible electroluminescence of ZnO radial p–n junction was demonstrated through a combination of position-controlled nano/microwire and crystalline p-type ZnO(P) radial shell growth on the wires. The reported research opens a pathway of realisation of production-compatible ZnO p–n junction LEDs.

The field of plasmonics has attracted considerable attention in recent years because of potential applications in various fields such as nanophotonics, photovoltaics, energy conversion, catalysis, and therapeutics. It is becoming increasing clear that intrinsic high losses associated with plasmons can be utilized to create new device concepts to harvest the generated heat. It is therefore important to design cavities, which can harvest optical excitations efficiently to generate heat. We report a highly engineered nanowire cavity, which utilizes a high dielectric silicon core with a thin plasmonic film (Au) to create an effective metallic cavity to strongly confine light, which when coupled with localized surface plasmons in the nanoparticles of the thin metal film produces exceptionally high temperatures upon laser irradiation. Raman spectroscopy of the silicon core enables precise measurements of the cavity temperature, which can reach values as high as 1000 K. The same Si-Au cavity with enhanced plasmonic activity when coupled with TiO

Semiconductor epitaxy on two-dimensional materials is beneficial for transferrable and flexible device applications. Graphene, due to the absence of permanent electric dipoles, cannot screen the electric field coming from the opposite side surface, allowing remote epitaxy for heteroepitaxy. This study demonstrates remote heteroepitaxy of ZnO microrods (MRs) on the GaN substrate across graphene layers via hydrothermal growth. Even the use of tri-layer graphene yields the remote heteroepitaxial MR arrays. Transmission electron microscopy reveals the remote heteroepitaxial relation between ZnO MRs and the GaN substrate despite the existence of graphene interlayers in between them. Density-functional theory calculations show that charge transfer along the z-direction at graphene/c-GaN possibly attract adatoms leading to remote heteroepitaxy, implying the field permeability of graphene. The ability of graphene to be released from the host substrate is exploited to exfoliate the overlayer MRs and regenerate the substrate.

Highly efficient solid-state light-emitting devices require semiconductor architectures equipped with high quantum efficiency and integratability on conductive substrates. Surface plasmon (SP)-mediated luminescence enhancement has been considered as one of the most promising solutions, because SP resonance can greatly improve the radiative recombination rate and be achieved using metal entities compatible with the electrode fabrication process. Nevertheless, metal/semiconductor heterostructures have had several fabrication-compatible issues due to metal as a potential contaminant of the semiconductor. We present here a simple fabrication scheme for a metal-lined semiconductor nanotube heterostructure, in which a metal layer is selectively formed on the inner wall of the semiconductor nanotube. The Ag-lining process in a ZnO nanotube resulted in 7.5-fold enhancement of the photoluminescence intensity at 11 K. This SP fabrication technique looks promising for highly efficient solid-state lighting based on semiconductor nanostructures without detrimental effects.

Recent success in the fabrication of axial and radial core-shell heterostructures, composed of one or more layers with different properties, on semiconductor nanowires (NWs) has enabled greater control of NW-based device operation for various applications. (1-3) However, further progress toward significant performance enhancements in a given application is hindered by the limited knowledge of carrier dynamics in these structures. In particular, the strong influence of interfaces between different layers in NWs on transport makes it especially important to understand carrier dynamics in these quasi-one-dimensional systems. Here, we use ultrafast optical microscopy (4) to directly examine carrier relaxation and diffusion in single silicon core-only and Si/SiO(2) core-shell NWs with high temporal and spatial resolution in a noncontact manner. This enables us to reveal strong coherent phonon oscillations and experimentally map electron and hole diffusion currents in individual semiconductor NWs for the first time.

Spatially resolved luminescence distributions in semiconductor heterostructures were investigated by core level excitation using hard X-ray (sub-) microbeams. Compact and mobile XEOL instruments have been developed and well adapted on the hard X-ray beamline ID22 of the European Synchrotron Radiation Facility for different wavelength collection ranges: UV-VIS and NIR. Linked by multimode optical fibers, their special designs provide precise scanning microscopy and allow easy access for multiple detection modes. Based on the hard X-ray microprobe station of ID22, details of the equipments, spectral data and representative examples are briefly described. Data collections from InAs and InGaN quantum heterostructures support the excellent performance of the optical devices. © 2011 Elsevier B.V. All rights reserved., This work was partially supported by the NANOWIRING Marie Curie ITN (EU project No. PITN-GA-2010-265073).

Integration of nanostructure lighting source arrays with well-defined emission wavelengths is of great importance for optoelectronic integrated monolithic circuitry. We report on the fabrication and optical properties of GaN-based p–n junction multishell nanotube microarrays with composition-modulated nonpolar m-plane InxGa1–xN/GaN multiple quantum wells (MQWs) integrated on c-sapphire or Si substrates. The emission wavelengths were controlled in the visible spectral range of green to violet by varying the indium mole fraction of the InxGa1–xN MQWs in the range 0.13 ≤ x ≤ 0.36. Homogeneous emission from the entire area of the nanotube LED arrays was achieved via the formation of MQWs with uniform QW widths and composition by heteroepitaxy on the well-ordered nanotube arrays. Importantly, the wavelength-invariant electroluminescence emission was observed above a turn-on of 3.0 V because both the quantum-confinement Stark effect and band filling were suppressed due to the lack of spontaneous inherent electric field in the m-plane nanotube nonpolar MQWs. The method of fabricating the multishell nanotube LED microarrays with controlled emission colors has potential applications in monolithic nonpolar photonic and optoelectronic devices on commonly used c-sapphire and Si substrates.

We report the fabrication and luminescent characteristics of GaN-based visible light-emitting diode (LED) arrays on Si substrates. For the fabrication of the LEDs, high-quality GaN/ZnO coaxial nanotube heterostructures were prepared by the heteroepitaxial growth of GaN layers on position-controlled ZnO nanotube arrays grown on 1-μm-thick crack-free GaN/Si substrates. The nanostructured LEDs were composed of GaN-based p-n homojunction with GaN/In1-xGaxN multiple quantum wells (MQWs) coaxially coated on GaN/ZnO nanotube heterostructures. The fabricated micro-LEDs emitted visible green light that originated from the MQWs of individual coaxial LEDs. In addition, the origin of the light emission was investigated by measuring cathodoluminescence and electroluminescence spectra.

Optical properties of ZnO-based single nanorods are probed by cathodoluminescence (CL) measurements at T = 5 K. We observe a variation of the ZnO near band edge CL by three orders of magnitude along the nanorod axis, accompanied by a spectral blueshift of 10-30 meV. This indicates a rather poor structural quality of the nanorod bottom part, close to the substrate. ZnO/ZnMgO quantum wells grown on top of ZnO nanorods are found to exhibit much stronger confinement effects as compared to their two-dimensional counterparts, suggesting a reduced spontaneous and piezoelectric polarization effects.

The secondary electron emission (SEE) yield of heterostructures of zinc oxide (ZnO) nanoneedles coaxially coated with aluminum nitride (AlN) or gallium nitride (GaN) has been studied using ion and X-ray beams. This paper describes experiments performed with ions (2 MeV protons and 3.6 MeV/nucleon carbon beams) and photons (synchrotron radiation at ≈1 keV). The SEE yield of the heterostructures is enhanced significantly by the intrinsic nanostructure of the ZnO nanoneedle templates as compared to the AlN and GaN thin films on silicon (Si) substrates [T.J. Vink, R.G.F.A. Verbeek, V. Elsbergen, P.K. Bachmann, Appl. Phys. Lett. 83 (2003) 2285]. One of the mechanisms responsible for SEE yield enhancement can be attributed to the larger area of the nanostructured surface.

High-performance photovoltaic (PV) devices require strong light absorption, low reflection and efficient photogenerated carrier collection for high quantum efficiency. Previous optical studies of vertical wires arrays have revealed that extremely efficient light absorption in the visible wavelengths is achievable. Photovoltaic studies have further advanced the wire approach by employing radial p-n junction architectures to achieve more efficient carrier collection. While radial p-n junction formation and optimized light absorption have independently been considered, PV efficiencies have further opportunities for enhancement by exploiting the radial p-n junction fabrication procedures to form arrays that simultaneously enhance both light absorption and carrier collection efficiency. Here we report a concept of morphology control to improve PV performance, light absorption and quantum efficiency of silicon radial p-i-n junction arrays. Surface energy minimization during vapor phase epitaxy is exploited to form match-head structures at the tips of the wires. The match-head structure acts as a built-in light concentrator and enhances optical absorptance and external quantum efficiencies by 30 to 40%, and PV efficiency under AM 1.5G illumination by 20% compared to cylindrical structures without match-heads. The design rules for these improvements with match-head arrays are systematically studied. This approach of process-enhanced control of three-dimensional Si morphologies provides a fab-compatible way to enhance the PV performance of Si radial p-n junction wire arrays.

Using low-temperature near-field spectroscopy, we obtained spatially and spectrally resolved photoluminescence (PL) images of individual ZnO nanorod single-quantum-well structures (SQWs) with a spatial resolution of 20 nm. We observed the dependence of the quantum confinement effect of the PL peak on the well width (L aw), from which the linewidths of near-field PL spectra of ZnO nanorod SQWs (L aw = 2.5 and 3.75 nm) were determined to be as narrow as 3 meV. However, near-field PL spectra of individual SQWs with L aw = 5.0 nm exhibited two PL peaks, presumably due to strains or defects in the ZnMgO in the nanorod SQWs. Since the exciton in a quantum structure is an ideal two-level system with long coherence times, our results provide criteria for designing nanophotonic devices.

This work was supported by NTU RGM 17/04, the National Creative Research Initiative Project, and the Center for Nanostructured Materials Technology under the 21st Century Frontier R&D Program of the Ministry of Science and Technology, Korea.

Thin high-quality gallium nitride (GaN) nanowires were synthesized by a catalytic chemical vapor deposition method. The synthesized GaN nanowires with hexagonal single-crystalline structure had thin diameters of 10-50 nm and lengths of tens of micrometers. The thin GaN nanowires revealed UV bands at 3.481 and 3.285 eV in low-temperature PL measurements due to the recombination of donor-bound excitons and donor-acceptor pairs, respectively. The blue shifts of UV bands in the low-temperature PL measurement were observed, indicating quantum confinement effects in the thin GaN nanowires which have smaller diameters than the exciton Bohr radius, 11 nm. For field emission properties of GaN nanowires, the turn-on field of GaN nanowires was 8.5 V/microm and the current density was about 0.2 mA/cm(2) at 17.5 V/microm, which is sufficient for the applications of field emission displays and vacuum microelectronic devices. Moreover, the GaN nanowires indicated stronger emission stability compared with carbon nanotubes.

The metal-semiconductor interface in self-aligned contact formation can determine the overall performance of nanoscale devices. This interfacial morphology is predicted and well researched in homogenous semiconductor nanowires (NWs) but was not pursued in heterostructured core/shell nanowires. We found here that the solid-state reactions between Ni and Ge/Si core/shell nanowires resulted in a protruded and a leading NiSiy segment into the channel. A single Ni2Ge/NiSiy to Ge/Si core/shell interface was achieved by the selective shell removal near the Ni source/drain contact areas. Using in situ transmission electron microscopy, we measured the growth rate and anisotropic strain evolution in ultra-short channels. We found elevated compressive strains near the interface between the compound contact and the NW and relatively lower strains near the center of the channel which increased exponentially below the 10 nm channel length to exceed 10% strain at ∼3 nm lengths. These compressive strains are expected to ...

In this work, an imaging tool to investigate optical inhomogeneities with site and chemical sensitivities has been integrated in a synchrotron radiation nanoprobe. Coaxial GaN/In 1-xGa xN/GaN/ZnO nanoarchitecture light emitting diode (LED) arrays are used to validate the scanning x-ray excited luminescence technique. Elemental maps and luminescence images of the hexagonal InGaN multiple quantum wells and inner deposited layers are reported with 120 nm spatial resolution. Within the experimental accuracy, the X-ray fluorescence results reveal an homogeneous distribution of the major elements involved in the pattern formation and heteroepitaxial nanotube growth. In comparison to the morphological pattern, the optical emissions from individual nanowires exhibit a striking spatial variation, indicating significant changes in the quantum confinement effects. © 2012 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim., The authors thank S. Laboure from the ESRF, for the useful help with the set-up of the beamline ID22. This work was partially supported by the NANOWIRING Marie Curie ITN (EU project No. PITN-GA-2010-265073).

New discoveries on collective processes in materials fabrication and performance are emerging in the mesoscopic size regime between the nanoscale, where atomistic effects dominate, and the macroscale, where bulk-like behavior rules. For semiconductor electronics and photonics, dimensional control of the architecture in this regime is the limiting factor for device performance. Epitaxial crystal growth is the major tool enabling simultaneous control of the dimensions and properties of such architectures. Although size-dependent effects have been studied for many small-scale systems, they have not been reported for the epitaxial growth of Si crystalline surfaces. Here, we show a strong dependence of epitaxial growth rates on size for nano to microscale radial wires and planar stripes. A model for this unexpected size-dependent vapor phase epitaxy behavior at small dimensions suggests that these effects are universal and result from an enhanced surface desorption of the silane (SiH4) growth precursor near facet edges. Introducing phosphorus or boron dopants during the silicon epitaxy further decreases the growth rates and, for phosphorus, gives rise to a critical layer thickness for single crystalline epitaxial growth. This previously unknown mesoscopic size-dependent growth effect at mesoscopic dimensions points to a new mechanism in vapor phase growth and promises greater control of advanced device geometries.

Nanostructures provide novel opportunities of studying epitaxy in nano/mesoscale and on nonplanar substrates. Epitaxial growth of silicon (Si) on the surfaces of Si nanowires along radial direction is a promising way to prepare radial p-(i)-n junction in nanoscale for optoelectronic devices. Comprehensive studies of Si radial epitaxy in micro/nanoscale reveal that morphological evolution and size-dependent radial shell growth rate for undoped and doped Si radial shells. Single crystalline Si radial p-i-n junction wire arrays were utilized to fabricate photovoltaic (PV) devices. The PV devices exhibited the photoconversion efficiency of 10%, the short-circuit current density of 39 mA/cm 2 , and the open-circuit voltage of 0.52 V, respectively.

Ultrafast optical microscopy (UOM) combines a typical optical microscope and femtosecond (fs) lasers that produce high intensity, ultrashort pulses at high repetition rates over a broad wavelength range. This enables us new types of imaging modalities, including scanning optical pump-probe microscopy, which varies the pump and probe positions relatively on the sample and ultrafast optical wide field microscopy, which is capable of rapidly acquiring wide field images at different time delays, that is measurable nearly any sample in a non-contact manner with high spatial and temporal resolution simultaneously. We directly tracked carriers in space and time throughout a NW by varying the focused position of a strong optical “pump” pulse along the Si core-shell nanowires (NWs) axis while probing the resulting changes in carrier density with a weaker “probe” pulse at one end of the NW. The resulting time-dependent dynamics reveals the influence of oxide layer encapsulation on surface state passivation in core-shell NWs, as well as the presence of strong acoustic phonon oscillations, observed here for the first time in single NWs. Time-resolved wide field images of the photoinduced changes in transmission for a patterned semiconductor thin film and a single silicon nanowire after optical excitation are also captured in real time using a two dimensional smart pixel array detector. Our experiments enable us to extract several fundamental parameters in these samples, including the diffusion current, surface recombination velocity, diffusion coefficients, and diffusion velocities, without the influence of contacts.

We have developed a new imaging method, ultrafast optical wide field microscopy, capable of rapidly acquiring wide field images of nearly any sample in a non-contact manner with high spatial and temporal resolution. Time-resolved images of the photoinduced changes in transmission for a patterned semiconductor thin film and a single silicon nanowire after optical excitation are captured using a two-dimensional smart pixel array detector. These images represent the time-dependent carrier dynamics with high sensitivity, femtosecond time resolution and sub-micrometer spatial resolution.

An understanding of non-equilibrium carrier dynamics in silicon (Si) nanowires (NWs) and NW heterostructures is very important due to their many nanophotonic and nanoelectronics applications. Here, we describe the first measurements of ultrafast carrier dynamics and diffusion in single heterostructured Si nanowires, obtained using ultrafast optical microscopy. By isolating individual nanowires, we avoid complications resulting from the broad size and alignment distribution in nanowire ensembles, allowing us to directly probe ultrafast carrier dynamics in these quasi-one-dimensional systems. Spatially-resolved pump-probe spectroscopy demonstrates the influence of surface-mediated mechanisms on carrier dynamics in a single NW, while polarization-resolved femtosecond pump-probe spectroscopy reveals a clear anisotropy in carrier lifetimes measured parallel and perpendicular to the NW axis, due to density-dependent Auger recombination. Furthermore, separating the pump and probe spots along the NW axis enabled us to track space and time dependent carrier diffusion in radial and axial NW heterostructures. These results enable us to reveal the influence of radial and axial interfaces on carrier dynamics and charge transport in these quasi-one-dimensional nanosystems, which can then be used to tailor carrier relaxation in a single nanowire heterostructure for a given application.

Two different approaches to realize high-performance silicon nanowire solar cell on low-cost substrates will be presented. Study on Si nanopillars fabricated by deep reactive ion etching followed by epitaxial growth of electrically doped radial shell showed morphological effect on optical absorption, geometrical effect on external quantum efficiency and on device efficiency. Especially optical absorption properties of Si radial p-i-n junction arrays were investigated by both theoretical calculation with finite domain time difference method and absorbance measurements. Photovoltaic cell based on single crystalline Si nanopillar arrays demonstrated efficiency of higher than 10%. Additionally, randomly oriented Si radial p-i-n junction arrays were grown on stainless steel substrate. Si radial p-i-n junction photovoltaic device showed >3.5% efficiency.

Nanowires (NWs) consisting of P-doped Si/B-doped Ge axial heterojunctions were grown via vapor-liquid-solid synthesis using a combination of Au and AuGa catalyst particles. Off-axis electron holography (EH) was used to measure the electrostatic potential profile across the junction resulting from electrically active dopants, and atom-probe tomography (APT) was used to map total dopant concentration profiles. A comparison of the electrostatic potential profile measured from EH with simulations that were based on the APT results indicates that Ga atoms unintentionally introduced during AuGa catalyst growth were mostly electronically inactive. This finding was also corroborated by in situ electron-holography biasing experiments. Electronic band structure simulations guided by the experimental results helped to provide a much better explanation of the NW electrical behavior. Overall, this work demonstrates that the combination of EH, APT, in situ biasing, and simulations allows a more complete understanding of NW electrical properties to be developed.

Excitonic phenomena, such as excitonic absorption and emission, have been used in many photonic and optoelectronic semiconductor device applications. As the sizes of these nanoscale materials have approached to exciton diffusion lengths in semiconductors, a fundamental understanding of exciton transport in semiconductors has become imperative. We present exciton transport in a single MgZnO nanorod in the spatiotemporal regime with several nanometer-scale spatial resolution and several tens of picosecond temporal resolution. This study was performed using temperature-dependent cathodoluminescence and time-resolved photoluminescence spectroscopies. The exciton diffusion length in the MgZnO nanorod decreased from 100 to 70 nm with increasing temperature in the range of 5 and 80 K. The results obtained for the temperature dependence of exciton diffusion length and luminescence lifetime revealed that the dominant exciton scattering mechanism in MgZnO nanorod is exciton-phonon assisted piezoelectric field scattering.

We map space-and-time-dependent carrier dynamics in single silicon nanowires firstly, using ultrafast optical microscopy. This enables us to directly measure acoustic phonon oscillations and carrier velocities in Si and Si/SiO 2 core-shell nanowires.

This chapter discusses studies of semiconducting nanowire arrays for solar cells. The concept of 3D nanowire architectures for photovoltaic light harvesting to effectively decouple light absorption and carrier separation is presented. The available literature on semiconductor nanowire solar cell studies is summarized. Optical and electronic aspects specific to nanowires are discussed to illustrate the basic principles. Finally, issues related to integration for solar cell applications are highlighted.

Exploring nanoscience confronts novel demands on the understanding of nanomaterial properties. To fulfill the demands, characterization methods for nanostructures should be sensitive to small amount of materials and have high resolution. Luminescence spectroscopy and microscopy can satisfy the requirements of nanoscale characterization although those have been used in semiconductors research for several decades. This chapter concentrates on the study of optical properties and related phenomena in semiconductor one-dimensional nanostructures using luminescence characterizations.

This proceeding summarizes the materials preparation of position-controlled ZnO-based nanorod heterostructures and fabrication of vertically-aligned wide band gap semiconductor nanorod light-emitting devices. Especially the fabrication of GaN/In x Ga 1-x N/GaN/ZnO nanorod heterostructured visible-light-emitter arrays on sapphire and Si substrates, representing important progress in the field of nanoheteroepitaxy and photonic devices in nanoscale, are reported. Particularly, position-controlled vertical nanostructure arrays make those possible to prepare high-quality material systems without stress or strain accumulation and to fabricate high-performance light-emitting devices (LEDs) with a three-dimensional device configuration. Our method based on nanoheteroepitaxy and position-controlled nanodevice integration for fabricating GaN-based micro-LED arrays constitutes a promising strategy for resolving the issues of conventional GaN LEDs and fabricating high-performance LEDs on various substrates for potential optoelectronic integrated circuits and solid-state lighting applications.

The superradiance had been predicted by Dicke in 1954 theoretically [1] and observed in atomic and molecular systems experimentally [2]. In the recent experiments, the superradiance and superfluorescence by nano-structures of solid-state materials such as an ensemble of quantum dots were observed [3, 4]. The superradiance by solid-state materials has advantage for the application of devices as compared with that by other materials such as atoms and molecules. Our group also observed the superradiant behaviour of emissions from a semiconductor nano-rod as shown in Fig. 1 (a). This sample is a nano-array of quantum-well dots (QWDs) with the width of 3.25 nm and barrier layers with the width of 9 nm. The diameter of the rod is 80 nm. The number of QWDs is about ten. In order to clarify the mechanism of the new type of superradiance by solid-state materials, we constructed the full-quantum-mechanical theory of superradiance [5], in which theory, the fundamental equations of the superradiant photoluminescence were derived by the scheme of the semiconductor luminescence equations [6]. The important development of our theory is an introduction of a correlation between polarizations via a radiation field which is the origin of superradiance. Here we will clarify the characteristics of superradiant emissions from the nano-array of QWDs and prove that the superradiance by our sample of the nano-rod can be realized theoretically.

We report nanophotonic energy up-conversion operation in ZnO nanorod double-quantum-well structures assisted by the optical absorption of phonons via an optical near-field.

ZnO/Zn0.8Mg0.2O coaxial nanorod heterostructures were prepared by employing catalyst-free metal-organic vapor-phase epitaxy, and their structural and photoluminescent (PL) properties were investigated using transmission electron microscopy (TEM) and temperature-dependent PL spectroscopy. TEM images show that ZnO/Zn0.8Mg0.2O layers were epitaxially grown on the entire surfaces of the ZnO nanorods and the ZnO nanorod diameters as a core material were as small as 9 +/- 2 nm. A dominant PL peak was observed at 3.316 eV, from room-temperature PL spectra of ZnO/Zn0.8Mg0.2O coaxial nanorod heterostructures with ZnO core diameters of 9 nm, indicating a PL blue shift of 30 meV, which resulted from a quantum confinement effect along the radial direction in ZnO nanorods. Furthermore, temperature-dependent PL properties of the coaxial nanorod heterostructures were investigated, showing much higher PL intensity for the coaxial nanorod heterostructures than that of bare ZnO nanorods at room temperature. The origin of the enhanced PL intensity and reduced thermal quenching for the coaxial nanorod heterostructures is also discussed.

We report on fabrications and characteristics of high performance ZnO nanorod nanodevices including Schottky diodes, metal-oxide-semiconductor field-effect transistors (MOSFETs), metal-semiconductor field-effect transistors (MESFETs) and logic gate devices. Electrical characteristics of several ZnO nanorod MOSFETs are compared in this proceeding. In particular, after coating polymer thin films on ZnO nanorod surfaces, the nanorod MOSFETs exhibited much improved field effect transistor characteristics including field effect electron mobility as high as 3000 cm 2 /Vs. In addition, ZnO nanorod Schottky diodes and MESFETs were fabricated using Au/ZnO Schottky contacts without any specific oxide etching process. These devices have been used for realization of ZnO nanorod logic gates.