Minimizing the Carrier Collection Loss of the Neutral-Color Transparent Crystalline-silicon Solar Modules via Hybrid Electrode Design.

Transparent solar cells can be used where conventional solar cells are inapplicable, such as, in glass windows of buildings; however, reports on modularization, which is essential for their commercialization, are scarce. Here, a novel modularization method has been proposed for the fabrication of transparent solar cells and a 100-cm2 neutral-color transparent crystalline-silicon solar module has been developed using a hybrid electrode comprising a microgrid electrode and an edge busbar electrode. The transparent solar module exhibits a power conversion efficiency (PCE) of 11.94 and 13.14% when connected in series and in parallel, respectively, with an average visible transmittance of 20%. Additionally, the module exhibits negligible losses in PCE (lower than 0.23%) in outdoor, mechanical-load, and damp-heat (at 85°C/85% RH) stability tests, indicating high stability. The transparent solar module proposes here could facilitate the commercialization of transparent solar cells.

Ionic Ir(III) complex-interfacial layer for efficient carrier collection via induced electric dipole.

The power conversion efficiency (PCE) of polymer solar cells (PSCs) has recently reached >19% through the development of photoactive materials, particularly non-fullerene acceptors. Interfacial layers (ILs) have been another essential factor in optimizing device charge extraction. In this study, we propose a series of ILs, in which ionic iridium(III) (Ir(III)) complexes of different alkali metal cations (Li+, Na+, and K+) enhance the charge collection efficiency between zinc oxide and active layers through an induced internal electric field. The anionic coordinate sphere and counter-cations of the Ir(III) complexes are distributed according to the operating voltage of the PSCs, causing electric dipoles that enhance the internal electric field and charge collection efficiency. Ion species migration in the ILs is confirmed using electrochemical impedance spectroscopy. The PCE of the PM6:Y6-based PSCs was improved from 14.0% to 15.6% by introducing an IL (Ir-K+). Furthermore, the stability of PSCs containing ionic Ir(III) complexes is enhanced significantly under ultraviolet (UV) light and AM 1.5 G one-sun irradiation owing to the intense UV absorption capacity and photo durability of the ILs. A device containing the Ir(III) complex-based ILs retained ∼60% of its initial PCE after UV irradiation, whereas the control device retained only ∼20%.

Sunlight-Activatable ROS Generator for Cell Death Using TiO2/c-Si Microwires.

Solar-driven reactive oxygen species (ROS) generation is an attractive disinfection technique for cell death and water purification. However, most photocatalysts require high stability in the water environment and the production of ROS with a sufficient amount and diffusion length to damage pathogens. Here, a ROS generation system was developed consisting of tapered crystalline silicon microwires coated with anatase titanium dioxide for a conformal junction. The system effectively absorbed >95% of sunlight over 300-1100 nm, resulting in effective ROS generation. The system was designed to produce various ROS species, but a logistic regression analysis with cellular survival data revealed that the diffusion length of the ROS is ∼9 µm, implying that the most dominant species causing cell damage is H2O2. Surprisingly, a quantitative analysis showed that only 15 min of light irradiation on the system would catalyze a local bactericidal effect comparable to the conventional germicidal level of H2O2 (∼3 mM).

Dopant-Free All-Back-Contact Si Nanohole Solar Cells Using MoOx and LiF Films.

We demonstrate novel all-back-contact Si nanohole solar cells via the simple direct deposition of molybdenum oxide (MoOx) and lithium fluoride (LiF) thin films as dopant-free and selective carrier contacts (SCCs). This approach is in contrast to conventionally used high-temperature thermal doping processes, which require multistep patterning processes to produce diffusion masks. Both MoOx and LiF thin films are inserted between the Si absorber and Al electrodes interdigitatedly at the rear cell surfaces, facilitating effective carrier collection at the MoOx/Si interface and suppressed recombination at the Si and LiF/Al electrode interface. With optimized MoOx and LiF film thickness as well as the all-back-contact design, our 1 cm(2) Si nanohole solar cells exhibit a power conversion efficiency of up to 15.4%, with an open-circuit voltage of 561 mV and a fill factor of 74.6%. In particular, because of the significant reduction in Auger/surface recombination as well as the excellent Si-nanohole light absorption, our solar cells exhibit an external quantum efficiency of 83.4% for short-wavelength light (∼400 nm), resulting in a dramatic improvement (54.6%) in the short-circuit current density (36.8 mA/cm(2)) compared to that of a planar cell (23.8 mA/cm(2)). Hence, our all-back-contact design using MoOx and LiF films formed by a simple deposition process presents a unique opportunity to develop highly efficient and low-cost nanostructured Si solar cells.

Filter-free image sensor pixels comprising silicon nanowires with selective color absorption.

The organic dye filters of conventional color image sensors achieve the red/green/blue response needed for color imaging, but have disadvantages related to durability, low absorption coefficient, and fabrication complexity. Here, we report a new paradigm for color imaging based on all-silicon nanowire devices and no filters. We fabricate pixels consisting of vertical silicon nanowires with integrated photodetectors, demonstrate that their spectral sensitivities are governed by nanowire radius, and perform color imaging. Our approach is conceptually different from filter-based methods, as absorbed light is converted to photocurrent, ultimately presenting the opportunity for very high photon efficiency.

Chromatic plasmonic polarizers for active visible color filtering and polarimetry.

Color filters are widely used in color displays, optical measurement devices, and imaging devices. Conventional color filters have usually only one fixed output color. However developing active color filters with controllable color output can lead to more compact and sophisticated color filter-based devices and applications. Recent progress in nanotechnology and new knowledge of the interaction of light with metal nanostructures allow us to capture and control light better than ever. Here we use it to fabricate active color filters, based on arrays of metallic optical nanoantennas that are tailored to interact with light at visible frequencies via excitation of localized surface plasmons. This interaction maps the polarization state of incident white light to visible color. Similarly, it converts unpolarized white light to chromatically polarized light. We experimentally demonstrate a wide range of applications including active color pixels, chromatically switchable and invisible tags, and polarization imaging based on these engineered colored metasurfaces.

Reconfigurable imaging systems using elliptical nanowires.

Materials that have subwavelength structure can add degrees of freedom to optical system design that are not possible with bulk materials. We demonstrate two lenses that are composed out of lithographically patterned arrays of elliptical cross-section silicon nanowires, which can dynamically reconfigure their imaging properties in response to the polarization of the illumination. In each element, two different focusing functions are polarization encoded into a single lens. The first nanowire lens has a different focal length for each linear polarization state, thereby realizing the front end of a nonmechanical zoom imaging system. The second nanowire lens has a different optical axis for each linear polarization state, demonstrating stereoscopic image capture from a single physical aperture.

Dramatic reduction of surface recombination by in situ surface passivation of silicon nanowires.

Nanowires have unique optical properties and are considered as important building blocks for energy harvesting applications such as solar cells. However, due to their large surface-to-volume ratios, the recombination of charge carriers through surface states reduces the carrier diffusion lengths in nanowires a few orders of magnitude, often resulting in the low efficiency (a few percent or less) of nanowire-based solar cells. Reducing the recombination by surface passivation is crucial for the realization of high-performance nanosized optoelectronic devices but remains largely unexplored. Here we show that a thin layer of amorphous silicon (a-Si) coated on a single-crystalline silicon nanowire, forming a core-shell structure in situ in the vapor-liquid-solid process, reduces the surface recombination nearly 2 orders of magnitude. Under illumination of modulated light, we measure a greater than 90-fold improvement in the photosensitivity of individual core-shell nanowires, compared to regular nanowires without shell. Simulations of the optical absorption of the nanowires indicate that the strong absorption of the a-Si shell contributes to this effect, but we conclude that the effect is mainly due to the enhanced carrier lifetime by surface passivation.

Multicolored vertical silicon nanowires.

We demonstrate that vertical silicon nanowires take on a surprising variety of colors covering the entire visible spectrum, in marked contrast to the gray color of bulk silicon. This effect is readily observable by bright-field microscopy, or even to the naked eye. The reflection spectra of the nanowires each show a dip whose position depends on the nanowire radii. We compare the experimental data to the results of finite difference time domain simulations to elucidate the physical mechanisms behind the phenomena we observe. The nanowires are fabricated as arrays, but the vivid colors arise not from scattering or diffractive effects of the array, but from the guided mode properties of the individual nanowires. Each nanowire can thus define its own color, allowing for complex spatial patterning. We anticipate that the color filter effect we demonstrate could be employed in nanoscale image sensor devices.

Two GPSes in a Ball: Deciphering the Endosomal Tug-of-War Using Plasmonic Dark-Field STORM.

Live video recording of intracellular material transport is a promising means of deciphering the fascinating underlying mechanisms driving life at the molecular level. Such technology holds the key to realizing real-time observation at appropriate resolutions in three-dimensional (3D) space within living cells. Here, we report an optical microscopic method for probing endosomal dynamics with proper spatiotemporal resolution within 3D space in live cells: plasmonic dark-field STORM (pdf-STORM). We first confirmed that pdf-STORM has a spatial resolution comparable to that of scanning electron microscopy. Additionally, by observing two optical probes within a single organelle, we were able to track rotational movements and demonstrate the feasibility of using pdf-STORM to observe the angular displacements of an endosome during a "tug-of-war" over an extended period. Finally, we show various biophysical parameters of the hitherto unelucidated dynamics of endosomes-angular displacement is discontinuous and y-axis movement predominates and follows a long-tail distribution.

Polymorph-tuned synthesis of α- and ß-Bi2O3 nanowires and determination of their growth direction from polarized Raman single nanowire microscopy.

We report polymorph-tuned synthesis of α- and ß-Bi(2)O(3) nanowires and their single nanowire micro-Raman study. The single crystalline Bi(2)O(3) nanowires in different phases (α and ß) were selectively synthesized by adjusting the heating temperature of Bi precursor in a vapor transport process. No catalyst was employed. Furthermore, at an identical precursor evaporation temperature, α- and ß- phase Bi(2)O(3) nanowires were simultaneously synthesized along the temperature gradient at a substrate. The growth direction of α-Bi(2)O(3) nanowires was revealed by polarized Raman single nanowire spectra. For thin ß-Bi(2)O(3) nanowires with a very small diameter, the polarized Raman single nanowire spectrum was strongly influenced by the shape effect.

Diffusion-driven crystal structure transformation: synthesis of Heusler alloy Fe3Si nanowires.

We report fabrication of Heusler alloy Fe(3)Si nanowires by a diffusion-driven crystal structure transformation method from paramagnetic FeSi nanowires. Magnetic measurements of the Fe(3)Si nanowire ensemble show high-temperature ferromagnetic properties with T(c) >> 370 K. This methodology is also successfully applied to Co(2)Si nanowires in order to obtain metal-rich nanowires (Co) as another evidence of the structural transformation process. Our newly developed nanowire crystal transformation method would be valuable as a general method to fabricate metal-rich silicide nanowires that are otherwise difficult to synthesize.

In situ TEM observation of heterogeneous phase transition of a constrained single-crystalline Ag2Te nanowire.

Laterally epitaxial single crystalline Ag2Te nanowires (NWs) are synthesized on sapphire substrates by the vapor transport method. We observed the phase transitions of these Ag2Te NWs via in situ transmission electron microscopy (TEM) after covering them with Pt layers. The constrained NW shows phase transition from monoclinic to a body-centered cubic (bcc) structure near the interfaces, which is ascribed to the thermal stress caused by differences in the thermal expansion coefficients. Furthermore, we observed the nucleation and growth of bcc phase penetrating into the face-centered cubic matrix at 200 °C by high-resolution TEM in real time. Our results would provide valuable insight into how compressive stresses imposed by overlayers affect behaviors of nanodevices.

Steering epitaxial alignment of Au, Pd, and AuPd nanowire arrays by atom flux change.

We have synthesized epitaxial Au, Pd, and AuPd nanowire arrays in vertical or horizontal alignment on a c-cut sapphire substrate. We show that the vertical and horizontal nanowire arrays grow from half-octahedral seeds by the correlations of the geometry and orientation of seed crystals with those of as-grown nanowires. The alignment of nanowires can be steered by changing the atom flux. At low atom deposition flux vertical nanowires grow, while at high atom flux horizontal nanowires grow. Similar vertical/horizontal epitaxial growth is also demonstrated on SrTiO(3) substrates. This orientation-steering mechanism is visualized by molecular dynamics simulations.

Silicon Microwire Arrays with Nanoscale Spacing for Radial Junction c-Si Solar Cells with an Efficiency of 20.5.

Structural optimization of microwire arrays is important for the successful demonstration of the practical feasibility of radial junction crystalline silicon (c-Si) solar cells. In this study, we investigated an optimized design of tapered microwire (TMW) arrays to maximize the light absorption of c-Si solar cells, while minimizing the surface recombination, for simultaneously improving the open-circuit voltage and short-circuit current density (Jsc). Finite-difference time-domain simulations confirmed that controlling the spacing between the TMWs at the nanometer scale is more effective for increasing the light absorption than increasing the TMW length. The photogenerated current of a c-Si TMW array with a 200 nm spacing was calculated to be 42.90 mA/cm2, which is close to the theoretical limit of 43.37 mA/cm2 in the 300-1100 nm wavelength range. To experimentally demonstrate the TMW arrays with a nanometer-scale spacing of 200 nm, which cannot be realized by conventional photolithography, we utilized a soft lithography method based on polystyrene beads for patterning a c-Si wafer. The solar cells based on optimized TMW arrays exhibited a Jsc of 42.5 mA/cm2 and power conversion efficiency of 20.5%, which exceed those of the previously reported microwire-based radial junction solar cells.

Structure-induced ferromagnetic stabilization in free-standing hexagonal Fe(1.3)Ge nanowires.

Single-crystalline free-standing hexagonal Fe(1.3)Ge nanowires (NWs) are synthesized for the first time using a chemical vapor transport process without using any catalyst. Interestingly, Fe(1.3)Ge NWs are found to be ferromagnetic at room temperature, while bulk Fe(1.3)Ge has the lower critical temperature of 200 K. We perform first-principles density functional calculations and suggest that the observed strong ferromagnetism is attributed to the reduced distances between Fe atoms, increased number of Fe-Fe bonds, and the enhanced Fe magnetic moments. Both experimental and theoretical studies show that the magnetic moments are enhanced in the NWs, as compared to bulk Fe(1.3)Ge. We also modulate the composition ratio of as-grown iron germanide NWs by adjusting experimental conditions. It is shown that uniaxial strain on the hexagonal plane also enhances the ferromagnetic stability.

Vertical epitaxial co5 ge7 nanowire and nanobelt arrays on a thin graphitic layer for flexible field emission displays.

Vertically aligned single-crystalline Co5 Ge7 nanowire (NW) and nanobelt arrays are grown on a very thin graphite layer as well as a curved graphite layer with a good epitaxial lattice match. Co5 Ge7 NW arrays, thus grown, show very efficient field emission properties comparable to those of carbon nanotubes and may be used for flexible field emission displays in the future.

Seawater-Mediated Solar-to-Sodium Conversion by Bismuth Vanadate Photoanode- Photovoltaic Tandem Cell: Solar Rechargeable Seawater Battery.

Conversion of sunlight to chemical energy based on photoelectrochemical (PEC) processes has been considered as a promising strategy for solar energy harvesting. Here, we propose a novel platform that converts solar energy into sodium (Na) as a solid-state solar fuel via the PEC oxidation of natural seawater, for which a Na ion-selective ceramic membrane is employed together with photoelectrode (PE)-photovoltaic (PV) tandem cell. Using an elaborately modified bismuth vanadate-based PE in tandem with crystalline silicon PV, we demonstrate unassisted solar-to-Na conversion (equivalent to solar charge of seawater battery) with an unprecedentedly high efficiency of 8% (expected operating point under 1 sun) and measured operation efficiency of 5.7% (0.2 sun) and long-term stability, suggesting a new benchmark for low-cost, efficient, and scalable solid solar fuel production. The sodium turns easily into electricity on demand making the device a nature-friendly, monolithic solar rechargeable seawater battery.

Phosphorescent Energy Downshifting for Diminishing Surface Recombination in Silicon Nanowire Solar Cells.

Molecularly engineered Ir(III) complexes can transfer energy from short-wavelength photons (λ < 450 nm) to photons of longer wavelength (λ > 500 nm), which can enhance the otherwise low internal quantum efficiency (IQE) of crystalline Si (c-Si) nanowire solar cells (NWSCs) in the short-wavelength region. Herein, we demonstrate a phosphorescent energy downshifting system using Ir(III) complexes at short wavelengths (300-450 nm) to diminish the severe surface recombination that occurs in c-Si NWSCs. The developed Ir(III) complexes can be considered promising energy converters because they exhibit superior intrinsic properties such as a high quantum yield, a large Stokes shift, a long exciton diffusion length in crystalline film, and a reproducible synthetic procedure. Using the developed Ir(III) complexes, highly crystalline energy downshifting layers were fabricated by ultrasonic spray deposition to enhance the photoluminescence efficiency by increasing the radiative decay. With the optimized energy downshifting layer, our 1 cm2 c-Si NWSCs with Ir(III) complexes exhibited a higher IQE value for short-wavelength light (300-450 nm) compared with that of bare Si NWSCs without Ir(III) complexes, resulting in a notable increase in the short-circuit current density (from 34.4 mA·cm-2 to 36.5 mA·cm-2).

Embedded Metal Electrode for Organic-Inorganic Hybrid Nanowire Solar Cells.

We demonstrate here an embedded metal electrode for highly efficient organic-inorganic hybrid nanowire solar cells. The electrode proposed here is an effective alternative to the conventional bus and finger electrode which leads to a localized short circuit at a direct Si/metal contact and has a poor collection efficiency due to a nonoptimized electrode design. In our design, a Ag/SiO2 electrode is embedded into a Si substrate while being positioned between Si nanowire arrays underneath poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS), facilitating suppressed recombination at the Si/Ag interface and notable improvements in the fabrication reproducibility. With an optimized microgrid electrode, our 1 cm2 hybrid solar cells exhibit a power conversion efficiency of up to 16.1% with an open-circuit voltage of 607 mV and a short circuit current density of 34.0 mA/cm2. This power conversion efficiency is more than twice as high as that of solar cells using a conventional electrode (8.0%). The microgrid electrode significantly minimizes the optical and electrical losses. This reproducibly yields a superior quantum efficiency of 99% at the main solar spectrum wavelength of 600 nm. In particular, our solar cells exhibit a significant increase in the fill factor of 78.3% compared to that of a conventional electrode (61.4%); this is because of the drastic reduction in the metal/contact resistance of the 1 µm-thick Ag electrode. Hence, the use of our embedded microgrid electrode in the construction of an ideal carrier collection path presents an opportunity in the development of highly efficient organic-inorganic hybrid solar cells.