Hierarchical Transparent Back Contacts for Bifacial CdTe PV.

A hierarchical transparent back contact leveraging an AlGaOx passivating layer, Ti3C2Tx MXene with a high work function, and a transparent cracked film lithography (CFL) templated nanogrid is demonstrated on copper-free cadmium telluride (CdTe) devices. AlGaOx improves device open-circuit voltage but reduces the fill factor when using a CFL-templated metal contact. Including a Ti3C2Tx interlayer improves the fill factor, lowers detrimental Schottky barriers, and enables metallization with CFL by providing transverse conduction into the nanogrid. The bifacial performance of an AlGaOx/Ti3C2Tx/CFL gold contact is evaluated, reaching 19.5% frontside efficiency and 2.8% backside efficiency under 1-sun illumination for a copper-free, group-V doped CdTe device. Under dual illumination, device power generation reached 200 W/m2 with 0.1 sun backside illumination.

LED-based characterization of solar cells for underwater applications.

Improved solar energy harvesting in aquatic environments would allow for superior environmental monitoring. However, developing underwater solar cells is challenging as evaluation typically requires deployment in the field or in large water tanks that can simulate aquatic light conditions. Here, we present a protocol to test underwater solar cells using a light-emitting diode (LED)-based characterization technique usable in a typical laboratory setting. We describe steps for installing and running Python code, matching LEDs to irradiance, characterizing underwater solar cells, and calculating underwater solar cell efficiency. For complete details on the use and execution of this protocol, please refer to Röhr et al.1.

Towards High-Efficiency Photon Trapping in Thin-Film Perovskite Solar Cells Using Etched Fractal Metadevices.

Reflective loss is one of the main factors contributing to power conversion efficiency limitation in thin-film perovskite solar cells. This issue has been tackled through several approaches, such as anti-reflective coatings, surface texturing, or superficial light-trapping metastructures. We report detailed simulation-based investigations on the photon trapping capabilities of a standard Methylammonium Lead Iodide (MAPbI3) solar cell, with its top layer conveniently designed as a fractal metadevice, to reach a reflection value R<0.1 in the visible domain. Our results show that, under certain architecture configurations, reflection values below 0.1 are obtained throughout the visible domain. This represents a net improvement when compared to the 0.25 reflection yielded by a reference MAPbI3 having a plane surface, under identical simulation conditions. We also present the minimum architectural requirements of the metadevice by comparing it to simpler structures of the same family and performing a comparative study. Furthermore, the designed metadevice presents low power dissipation and exhibits approximately similar behavior regardless of the incident polarization angle. As a result, the proposed system is a viable candidate for being a standard requirement in obtaining high-efficiency perovskite solar cells.

Identifying optimal photovoltaic technologies for underwater applications.

Improving solar energy collection in aquatic environments would allow for superior environmental monitoring and remote sensing, but the identification of optimal photovoltaic technologies for such applications is challenging as evaluation requires either field deployment or access to large water tanks. Here, we present a simple bench-top characterization technique that does not require direct access to water and therefore circumvents the need for field testing during initial trials of development. Employing LEDs to simulate underwater solar spectra at various depths, we compare Si and CdTe solar cells, two commercially available technologies, with GaInP cells, a technology with a wide bandgap close to ideal for underwater solar harvesting. We use this method to show that while Si cells outperform both CdTe and GaInP cells under terrestrial AM1.5G solar irradiance, CdTe and GaInP cells outperform Si cells at depths >2 m, with GaInP cells operating with underwater efficiencies approaching 54%.

Narrowing the Phase Distribution of Quasi-2D Perovskites for Stable Deep-Blue Electroluminescence.

Solution-processed quasi-2D perovskites contain multiple quantum wells with a broad width distribution. Inhomogeneity results in the charge funneling into the smallest bandgap components, which hinders deep-blue emission and accelerates Auger recombination. Here, a synthetic strategy applied to a range of quasi-2D perovskite systems is reported, that significantly narrows the quantum well dispersity. It is shown that the phase distribution in the perovskite film is significantly narrowed with controlled, simultaneous evaporation of solvent and antisolvent. Modulation of film formation kinetics of quasi-2D perovskite enables stable deep-blue electroluminescence with a peak emission wavelength of 466 nm and a narrow linewidth of 14 nm. Light emitting diodes using the perovskite film show a maximum luminance of 280 cd m-2 at an external quantum efficiency of 0.1%. This synthetic approach will serve in producing new materials widening the color gamut of next-generation displays.

Localizing Tungsten Single Atoms around Tungsten Nitride Nanoparticles for Efficient Oxygen Reduction Electrocatalysis in Metal-Air Batteries.

Combining isolated atomic active sites with those in nanoparticles for synergizing complex multistep catalysis is being actively pursued in the design of new electrocatalyst systems. However, these novel systems have been rarely studied due to the challenges with synthesis and analysis. Herein, a synergistically catalytic performance is demonstrated with a 0.89 V (vs reversible hydrogen electrode) onset potential in the four-step oxygen reduction reaction (ORR) by localizing tungsten single atoms around tungsten nitride nanoparticles confined into nitrogen-doped carbon (W SAs/WNNC). Through density functional theory calculations, it is shown that each of the active centers in the synergistic entity feature a specific potential-determining step in their respective reaction pathway that can be merged to optimize the intermediate steps involving scaling relations on individual active centers. Impressively, the W SAs/WNNC as the air cathode in all-solid-state Zn-air and Al-air batteries demonstrate competitive durability and reversibility, despite the acknowledged low activity of W-based catalyst toward the ORR.

In Operando Visualization and Dynamic Manipulation of Electrochemical Processes at the Electrode-Solution Interface.

Revealing the dynamic processes at the electrode-solution interface is imperative for understanding electrochemical phenomena. Most techniques have been developed to sense the electrode surface changes at the nanoscale, but provide limited information on potential-induced interfacial ion redistribution at the mesoscale. Herein, we present an in operando visualization method utilizing a microfabricated electrochemical cell combined with a laser scanning confocal microscope to observe high-resolution and fast-response interfacial processes. We report potential-induced formation and transformation of the Nernst diffusion layer, demonstrating that pulsed voltage dynamically perturbs the interface and promotes ion diffusion. This provides an additional insight into developing a dynamic manipulation method to control the electrochemical process. Our novel visualization method can easily be applied to monitor different ionic behaviors in electrochemical reactions at the mesoscale.

CO2 doping of organic interlayers for perovskite solar cells.

In perovskite solar cells, doped organic semiconductors are often used as charge-extraction interlayers situated between the photoactive layer and the electrodes. The π-conjugated small molecule 2,2',7,7'-tetrakis[N,N-di(4-methoxyphenyl)amino]-9,9-spirobifluorene (spiro-OMeTAD) is the most frequently used semiconductor in the hole-conducting layer1-6, and its electrical properties considerably affect the charge collection efficiencies of the solar cell7. To enhance the electrical conductivity of spiro-OMeTAD, lithium bis(trifluoromethane)sulfonimide (LiTFSI) is typically used in a doping process, which is conventionally initiated by exposing spiro-OMeTAD:LiTFSI blend films to air and light for several hours. This process, in which oxygen acts as the p-type dopant8-11, is time-intensive and largely depends on ambient conditions, and thus hinders the commercialization of perovskite solar cells. Here we report a fast and reproducible doping method that involves bubbling a spiro-OMeTAD:LiTFSI solution with CO2 under ultraviolet light. CO2 obtains electrons from photoexcited spiro-OMeTAD, rapidly promoting its p-type doping and resulting in the precipitation of carbonates. The CO2-treated interlayer exhibits approximately 100 times higher conductivity than a pristine film while realizing stable, high-efficiency perovskite solar cells without any post-treatments. We also show that this method can be used to dope π-conjugated polymers.

Weak polyelectrolyte-based multilayers via layer-by-layer assembly: Approaches, properties, and applications.

Layer-by-layer (LbL) assembly is a nanoscale technique with great versatility, simplicity and molecular-level processing of various nanoscopic materials. Weak polyelectrolytes have been used as major building blocks for LbL assembly providing a fundamental and versatile tool to study the underlying mechanisms and practical applications of LbL assembly due to its pH-responsive charge density and molecular conformation. Because of high-density uncompensated charges and high-chain mobility, weak polyelectrolyte exponential multilayer growth is considered one of the fastest developing areas for organized molecular films. In this article, we systematically review the current status and developments of weak polyelectrolyte-based multilayers including all-weak-polyelectrolyte multilayers, weak polyelectrolytes/other components (e.g. strong polyelectrolytes, neutral polymers, and nanoparticles) multilayers, and exponentially grown weak polyelectrolyte multilayers. Several key aspects of weak polyelectrolytes are highlighted including the pH-controllable properties, the responsiveness to environmental pH, and synergetic functions obtained from weak polyelectrolyte/other component multilayers. Throughout this review, useful applications of weak polyelectrolyte-based multilayers in drug delivery, tunable biointerfaces, nanoreactors for synthesis of nanostructures, solid state electrolytes, membrane separation, and sensors are highlighted, and promising future directions in the area of weak polyelectrolyte-based multilayer assembly such as fabrication of multi-responsive materials, adoption of unique building blocks, investigation of internal molecular-level structure and mechanism of exponentially grown multilayers, and exploration of novel biomedical and energy applications are proposed.

Electrochemical-Osmotic Process for Simultaneous Recovery of Electric Energy, Water, and Metals from Wastewater.

A highly-efficient, autonomous electrochemical-osmotic system (EOS) is developed for simultaneous recovery of electric energy, water, and metals from wastewater. We demonstrate that the system can generate a maximum electric power density of 10.5 W m-2 using a spontaneous Fe/Cu2+ galvanic cell, while simultaneously achieving copper recovery from wastewater. With an osmotic pressure difference generated by the deployed electrochemical reactions, water is osmotically extracted from the feed solution with the EOS at a water flux of 5.1 L m-2 h-1. A scaled-up EOS realizes a power density of 105.8 W per m-3 of treated water to light an LED over 24 h while also enhancing water extraction and metal recovery. The modularized EOS obtains ultrahigh (>97.5%) Faradaic efficiencies under variable operating conditions, showing excellent system stability. The EOS is also versatile: it can recover Au, Ag, and Hg from wastewaters with simultaneous electricity and water coproduction. Our study demonstrates a promising pathway for realizing multiresource recycling from wastewater by coupling electrochemical and osmosis-driven processes.

High-throughput, combinatorial synthesis of multimetallic nanoclusters.

Multimetallic nanoclusters (MMNCs) offer unique and tailorable surface chemistries that hold great potential for numerous catalytic applications. The efficient exploration of this vast chemical space necessitates an accelerated discovery pipeline that supersedes traditional "trial-and-error" experimentation while guaranteeing uniform microstructures despite compositional complexity. Herein, we report the high-throughput synthesis of an extensive series of ultrafine and homogeneous alloy MMNCs, achieved by 1) a flexible compositional design by formulation in the precursor solution phase and 2) the ultrafast synthesis of alloy MMNCs using thermal shock heating (i.e., ∼1,650 K, ∼500 ms). This approach is remarkably facile and easily accessible compared to conventional vapor-phase deposition, and the particle size and structural uniformity enable comparative studies across compositionally different MMNCs. Rapid electrochemical screening is demonstrated by using a scanning droplet cell, enabling us to discover two promising electrocatalysts, which we subsequently validated using a rotating disk setup. This demonstrated high-throughput material discovery pipeline presents a paradigm for facile and accelerated exploration of MMNCs for a broad range of applications.

Mechanically strong and electrically conductive multilayer MXene nanocomposites.

Polymer nanocomposites offer the opportunity to bridge properties of nanomaterials to the macroscale. In this work, layer-by-layer (LbL) assembly is used to demonstrate nanocomposites of 2D titanium carbide nanosheets (MXene) and clay nanoplatelets (montmorillonite) to fabricate freestanding thin films with unique multifunctional properties. These thin films can be tuned by adjusting the thickness to exhibit a tensile strength of 138 MPa-225 MPa, EMI specific shielding effectiveness normalized to thickness and density up to 24 550 dB cm2 g-1, and sheet resistance from 855 Ω sq-1-3.27 kΩ sq-1 (corresponding to a range of conductivity from 53 S m-1 to 125 S m-1). This composite is the strongest MXene-based LbL film prepared to date, in part due to the nacre-like brick-and-mortar structure. Ultra-strong, multifunctional films of this nature are desirable for many applications ranging from membranes, to structural and multifunctional composites, energy harvesting and storage, and materials for aerospace.

A Promising Carbon/g-C3 N4 Composite Negative Electrode for a Long-Life Sodium-Ion Battery.

2D graphitic carbon nitride (g-C3 N4 ) nanosheets are a promising negative electrode candidate for sodium-ion batteries (NIBs) owing to its easy scalability, low cost, chemical stability, and potentially high rate capability. However, intrinsic g-C3 N4 exhibits poor electronic conductivity, low reversible Na-storage capacity, and insufficient cyclability. DFT calculations suggest that this could be due to a large Na+ ion diffusion barrier in the innate g-C3 N4 nanosheet. A facile one-pot heating of a mixture of low-cost urea and asphalt is strategically applied to yield stacked multilayer C/g-C3 N4 composites with improved Na-storage capacity (about 2 times higher than that of g-C3 N4 , up to 254 mAh g-1 ), rate capability, and cyclability. A C/g-C3 N4 sodium-ion full cell (in which sodium rhodizonate dibasic is used as the positive electrode) demonstrates high Coulombic efficiency (ca. 99.8 %) and a negligible capacity fading over 14 000 cycles at 1 A g-1 .

Recent Advances in Metallic Glass Nanostructures: Synthesis Strategies and Electrocatalytic Applications.

Recent advances in metallic glass nanostructures (MGNs) are reported, covering a wide array of synthesis strategies, computational discovery, and design solutions that provide insight into distinct electrocatalytic applications. A brief introduction to the development and unique features of MGNs with an overview of top-down and bottom-up synthesis strategies is presented. Specifically, the morphology and structural analysis of several examples applying MGNs as electrodes are highlighted. Subsequently, a comprehensive discussion of commonly employed kinetic parameters and their connection with the unique material structures of MGNs on individual electrocatalytic reactions is made, including the hydrogen evolution reaction, oxygen reduction reaction, and alcohol (methanol or ethanol) oxidation reaction. Finally, a summary of the challenges and perspective on the future research and development relevant to MGNs as electrocatalysts is provided.

PEOz-PEDOT:PSS Composite Layer: A Route to Suppressed Hysteresis and Enhanced Open-Circuit Voltage in a Planar Perovskite Solar Cell.

The successful commercialization of perovskite solar cells (Pvs-SCs) calls for the need to find low-temperature processable interlayers with outstanding charge-transport features. In this work, we strategically blend poly(2-ethyl-2-oxazoline) (PEOz) with PEDOT:PSS as the modified hole transport layer (HTL) to achieve high-efficiency P-I-N CH3NH3PbI3 Pvs-SCs. The PEOz-PEDOT:PSS HTL exhibits enhanced features over the conventional layer including the following: (1) promoting perovskite with enlarged grain sizes to decrease the perovskite layer's recombination, (2) increasing the work function of the HTL, and (3) decreasing the noncapacitive current in Pvs-SCs. Remarkably, we demonstrate a 17.39% power conversion efficiency with very low hysteresis and high Voc values of 1.075 V for Pvs-SCs with PEOz-PEDOT:PSS.

Spray coating of the PCBM electron transport layer significantly improves the efficiency of p-i-n planar perovskite solar cells.

The p-i-n structure for perovskite solar cells has recently shown significant advantages in minimal hysteresis effects, and scalable manufacturing potential using low-temperature solution processing. However, the power conversion efficiency (PCE) of the perovskite p-i-n structure remains low mainly due to limitations using a flat electron transport layer (ETL). In this work, we demonstrate a new approach using spray coating to fabricate the [6,6]-phenyl-C(61)-butyric acid methyl ester (PCBM) ETL. By creating a rough surface, we effectively improve the light trapping properties inside the PCBM ETL. We reveal that the spray coated PCBM can form a cross-linked network, which may facilitate better charge transport and enhance extraction efficiency. By improving the contact between the perovskite film and the PCBM ETL, a reduction in the trap states is observed resulting in a PCE increase from 13% to >17%.

Three-Phase Morphology Evolution in Sequentially Solution-Processed Polymer Photodetector: Toward Low Dark Current and High Photodetectivity.

Sequentially solution-processed polymer photodetectors (SSP PPDs) based on poly(3-hexylthiophene-2,5-diyl) (P3HT)/[6,6]-phenyl C71-butyric acid methyl ester (PC71BM) are fabricated by depositing the top layers of PC71BM from an appropriate cosolvent of 2-chlorophenol (2-CP)/o-dichlorobenzene (ODCB) onto the predeposited bottom layers of P3HT. By adjusting the ratio of 2-CP/ODCB in the top PC71BM layers, the resulting SSP PPD shows a decreased dark current and an increased photocurrent, leading to a maximum detectivity of 1.23 × 1012 Jones at a wavelength of 550 nm. This value is 5.3-fold higher than that of the conventional bulk heterojunction PPD. Morphology studies reveal that the PC71BM partially penetrates the predeposited P3HT layer during the spin-coating process, resulting in an optimal three-phase morphology with one well-mixed interdiffusion P3HT/PC71BM phase in the middle of the bulk and two pure phases of P3HT and PC71BM at the two electrode sides. We show that the pure phases form high Schottky barriers (>2.0 eV) at the active layer/electrodes interface and efficiently block unfavorable reverse charge carrier injection by significantly decreasing the dark current. The interdiffussion phase enlarges the donor-acceptor interfacial area leading to a large photocurrent. We also reveal that the improved performance of SSP PPDs is also due to the enhanced optical absorption, improved P3HT crystallinity, increased charge carrier mobilities, and suppressed bimolecular recombination.

Nanopatterned Bulk Metallic Glass Biosensors.

Nanopatterning as a surface area enhancement method has the potential to increase signal and sensitivity of biosensors. Platinum-based bulk metallic glass (Pt-BMG) is a biocompatible material with electrical properties conducive for biosensor electrode applications, which can be processed in air at comparably low temperatures to produce nonrandom topography at the nanoscale. Work presented here employs nanopatterned Pt-BMG electrodes functionalized with glucose oxidase enzyme to explore the impact of nonrandom and highly reproducible nanoscale surface area enhancement on glucose biosensor performance. Electrochemical measurements including cyclic voltammetry (CV) and amperometric voltammetry (AV) were completed to compare the performance of 200 nm Pt-BMG electrodes vs Flat Pt-BMG control electrodes. Glucose dosing response was studied in a range of 2 mM to 10 mM. Effective current density dynamic range for the 200 nm Pt-BMG was 10-12 times greater than that of the Flat BMG control. Nanopatterned electrode sensitivity was measured to be 3.28 µA/cm2/mM, which was also an order of magnitude greater than the flat electrode. These results suggest that nonrandom nanotopography is a scalable and customizable engineering tool which can be integrated with Pt-BMGs to produce biocompatible biosensors with enhanced signal and sensitivity.

Charge Transfer from Carbon Nanotubes to Silicon in Flexible Carbon Nanotube/Silicon Solar Cells.

Mechanical fragility and insufficient light absorption are two major challenges for thin flexible crystalline Si-based solar cells. Flexible hybrid single-walled carbon nanotube (SWNT)/Si solar cells are demonstrated by applying scalable room-temperature processes for the fabrication of solar-cell components (e.g., preparation of SWNT thin films and SWNT/Si p-n junctions). The flexible SWNT/Si solar cells present an intrinsic efficiency ≈7.5% without any additional light-trapping structures. By using these solar cells as model systems, the charge transport mechanisms at the SWNT/Si interface are investigated using femtosecond transient absorption. Although primary photon absorption occurs in Si, transient absorption measurements show that SWNTs also generate and inject excited charge carriers to Si. Such effects can be tuned by controlling the thickness of the SWNTs. Findings from this study could open a new pathway for designing and improving the efficiency of photocarrier generation and absorption for high-performance ultrathin hybrid SWNT/Si solar cells.