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At least 91 records · Page 5

Low Pressure Vapor-assisted Solution Process for Tunable Band Gap Pinhole-free Methylammonium Lead Halide Perovskite Films

Organo-lead halide perovskites have recently attracted great interest for potential applications in thin-film photovoltaics and optoelectronics. Herein, we present a protocol for the fabrication of this material via the low-pressure vapor assisted solution process (LP-VASP) method, which yields ~19% power conversion efficiency in planar heterojunction perovskite solar cells. First, we report the synthesis of methylammonium iodide (CH 3 NH 3 I) and methylammonium bromide (CH 3 NH 3 Br) from methylamine and the corresponding halide acid (HI or HBr). Then, we describe the fabrication of pinhole-free, continuous methylammonium-lead halide perovskite (CH 3 NH 3 PbX 3 with X = I, Br, Cl and their mixture) films with the LP-VASP. This process is based on two steps: i) spin-coating of a homogenous layer of lead halide precursor onto a substrate, and ii) conversion of this layer to CH 3 NH 3 PbI 3-x Br x by exposing the substrate to vapors of a mixture of CH 3 NH 3 I and CH 3 NH 3 Br at reduced pressure and 120 °C. Through slow diffusion of the methylammonium halide vapor into the lead halide precursor, we achieve slow and controlled growth of a continuous, pinhole-free perovskite film. The LP-VASP allows synthetic access to the full halide composition space in CH 3 NH 3 PbI 3-x Br x with 0 ≤ x ≤ 3. Depending on the composition of the vapor phase, the bandgap can be tuned between 1.6 eV ≤ E g ≤ 2.3 eV. In addition, by varying the composition of the halide precursor and of the vapor phase, we can also obtain CH 3 NH 3 PbI 3-x Cl x . Films obtained from the LP-VASP are reproducible, phase pure as confirmed by X-ray diffraction measurements, and show high photoluminescence quantum yield. The process does not require the use of a glovebox.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Investigation of solution-processed bismuth-niobium-oxide films

The characteristics of bismuth-niobium-oxide (BNO) films prepared using a solution process were investigated. The BNO film annealed at 550°C involving three phases: an amorphous phase, Bi₃NbO₇ fluorite microcrystals, and Nb-rich cubic pyrochlore microcrystals. The cubic pyrochlore structure, which was the main phase in this film, has not previously been reported in BNO films. The relative dielectric constant of the BNO film was approximately 140, which is much higher than that of a corresponding film prepared using a conventional vacuum sputtering process. Notably, the cubic pyrochlore microcrystals disappeared with increasing annealing temperature and were replaced with triclinic β-BiNbO₄ crystals at 590°C. The relative dielectric constant also decreased with increasing annealing temperature. Therefore, the high relative dielectric constant of the BNO film annealed at 550°C is thought to result from the BNO cubic pyrochlore structure. In addition, the BNO films annealed at 500°C contained approximately 6.5 atm.% carbon, which was lost at approximately 550°C. This result suggests that the carbon in the BNO film played an important role in the formation of the cubic pyrochlore structure.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Solids from Fuel Dissolution, Process Solutions, and Waste Evaporation

Irradiated light water reactor (LWR) fuel contains material which is insoluble in nitric acid, and process solutions are unstable with respect to precipitation of compounds insoluble in nitric acid. Accordingly, solids will be encountered during fuel reprocessing, and operations must be conducted in a way to minimize formation of additional solids and to prevent their interference with reprocessing operations.

Campbell, D. O.↗

Epitaxially Grown Single-Crystalline SrTiO 3 Membranes Using a Solution-Processed, Amorphous SrCa 2 Al 2 O 6 Sacrificial Layer

Water-soluble sacrificial layers based on epitaxially-grown, single crystalline (Ca, Sr, Ba) 3 Al 2 O 6 layer are widely used for creating free-standing perovskite oxide membranes. However, obtaining these sacrificial layers with intricate stoichiometry remains a challenge, especially for molecular beam epitaxy (MBE). In this study, we demonstrate the hybrid MBE growth of epitaxial, single crystalline SrTiO 3 films using a solution processed, amorphous SrCa 2 Al 2 O 6 sacrificial layer onto SrTiO 3 (001) substrates. Prior to the growth, the oxygen plasma exposure was used to first create the crystalline SrCa 2 Al 2 O 6 layer with well-defined surface crystallinity. Utilizing reflection high energy electron diffraction, x-ray diffraction, and atomic force microscopy, we observe an atomic layer-by-layer growth of epitaxial, single crystalline SrTiO 3 film on the SrCa 2 Al 2 O 6 layer with atomically smooth surfaces. The SrCa 2 Al 2 O6 layer was subsequently dissolved in de-ionized water to create free-standing SrTiO3 membranes that were transferred onto a metal-coated Si wafer. Membranes created with Sr-deficiency revealed ferroelectric-like behavior measured using piezo force microscopy whereas stoichiometric films remained paraelectric-like. Furthermore, these findings underscore the viability of using ex-situ deposited amorphous SrCa2Al2O6 for epitaxial, single crystalline growth, as well as the importance of point defects in determining the ferroic properties in membranes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A Solution-Processable High-Modulus Crystalline Artificial Solid Electrolyte Interphase for Practical Lithium Metal Batteries

The solid electrolyte interphase (SEI) has been identified as a key challenge for Li metal anodes. The brittle and inhomogeneous native SEI generated by parasitic reactions between Li and liquid electrolytes can devastate battery performance; therefore, artificial SEIs (ASEIs) have been proposed as an effective strategy to replace native SEIs. Herein, as a collaboration between academia and industrial R&D teams, a multifunctional (crystalline, high modulus, and robust, Li + ion conductive, electrolyte-blocking, and solution processable) ASEI material, LiAl-FBD (where “FBD” refers to 2,2,3,3-tetra-fluoro-1,4-butanediol), for improving Li metal battery performance is designed and synthesized. The LiAl-FBD crystal structure consists of Al 3+ ions bridged by FBD 2– ligands to form anion clusters while Li + ions are loosely bound at the periphery, enabling an Li + ion conductivity of 9.4 × 10 –6 S cm –1 . Further, the fluorinated, short ligands endow LiAl-FBD with electrolyte phobicity and high modulus. The ASEI is found to prevent side reactions and extend the cycle life of Li metal electrodes. Specifically, pairing LiAl-FBD coated 50 μm thick Li with industrial 3.5 mAh cm –2 NMC811 cathode and 2.8 μL mAh –1 lean elec-trolyte, the Li metal full cells show superior cycle life compared to bare ones, achieving 250 cycles at 1 mA cm –2 .

25 ENERGY STORAGE↗

A solution-processed high performance organic solar cell using a small molecule with the thieno[3,2- b ]thiophene central unit

A solution processed acceptor–donor–acceptor (A–D–A) small molecule with thieno[3,2-b]thiophene as the central building block and 2-(1,1-dicyanomethylene)-rhodanine as the terminal unit, DRCN8TT, was designed and synthesized. The optimized power conversion efficiency (PCE) of 8.11% was achieved, which is much higher than that of its analogue molecule DRCN8T. In this work, the improved performance was ascribed to the morphology which consisted of small, highly crystalline domains that were nearly commensurate with the exiton diffusion length.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

n-Type doping of a solution processed p-type semiconductor using isoelectronic surface dopants for homojunction fabrication

The p-n junction is one of the fundamental requirements for a practical semiconductor-based electronic device. Designing a heterojunction comprising of dissimilar p-type and n-type semiconductors calls for careful energy level considerations, both when selecting the semiconductor materials as well as the metal contacts. A homojunction based on a single semiconductor simplifies this task, as energy levels of the p-type and n-type materials are already fairly similar, allowing for easier selection of contacts. Traditionally, homojunctions rely on doping of a bulk semiconductor to achieve p- and n-type transport through controlled addition of aliovalent dopants via energy-intensive processes such as ion implantation or thermal annealing. Exact control of doping in nanocrystalline semiconductors is significantly more challenging, due to self-purification effects. However, owing to their large surface areas, surface moieties can be utilized to both dope the nanostructures as well as tune their energy levels. Here, we present a facile technique based on an isoelectronic surface dopant in order to achieve p- and n-type materials based on the same semiconductor. We show that thin p-type colloidal Bi 2 Te 3 nanowires can be switched to n-type through surface functionalization, thus increasing the availability of new nanocrystalline solution-processable p-n homojunctions.

42 ENGINEERING↗

Suppression of dark current through barrier engineer for solution-processed colloidal quantum-dots infrared photodetectors

In an attempt to suppress the dark current, the barrier layer engineer for solution-processed PbSe colloidal quantum-dot (CQD) photodetectors has been investigated in the present study. It was found that the dark current can be significantly suppressed by implementing two types of carrier blocking layers, namely, hole blocking layer and electron blocking layer, sandwiched in between two active PbSe CQD layers. Meanwhile no adverse impact has been observed for the photo current. Our study suggests that this improvement resides on the transport pathway created via carrier recombination at intermediate layer, which provides wide implications for the suppression of dark current for infrared photodetectors.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Oxidation-resistant, solution-processed plasmonic Ni nanochain-SiO{sub x} (x < 2) selective solar thermal absorbers

Metal oxidation at high temperatures has long been a challenge in cermet solar thermal absorbers, which impedes the development of atmospherically stable, high-temperature, high-performance concentrated solar power (CSP) systems. In this work, we demonstrate solution-processed Ni nanochain-SiO{sub x} (x < 2) and Ni nanochain-SiO{sub 2} selective solar thermal absorbers that exhibit a strong anti-oxidation behavior up to 600 °C in air. The thermal stability is far superior to previously reported Ni nanoparticle-Al{sub 2}O{sub 3} selective solar thermal absorbers, which readily oxidize at 450 °C. The SiO{sub x} (x < 2) and SiO{sub 2} matrices are derived from hydrogen silsesquioxane and tetraethyl orthosilicate precursors, respectively, which comprise Si-O cage-like structures and Si-O networks. Fourier transform infrared spectroscopy shows that the dissociation of Si-O cage-like structures and Si-O networks at high temperatures have enabled the formation of new bonds at the Ni/SiO{sub x} interface to passivate the surface of Ni nanoparticles and prevent oxidation. X-ray photoelectron spectroscopy and Raman spectroscopy demonstrate that the excess Si in the SiO{sub x} (x < 2) matrices reacts with Ni nanostructures to form silicides at the interfaces, which further improves the anti-oxidation properties. As a result, Ni-SiO{sub x} (x < 2) systems demonstrate better anti-oxidation performance than Ni-SiO{sub 2} systems. This oxidation-resistant Ni nanochain-SiO{sub x} (x < 2) cermet coating also exhibits excellent high-temperature optical performance, with a high solar absorptance of ∼90% and a low emittance ∼18% measured at 300 °C. These results open the door towards atmospheric stable, high temperature, high-performance solar selective absorber coatings processed by low-cost solution-chemical methods for future generations of CSP systems.

36 MATERIALS SCIENCE↗

P‐23: Enhancement in the Mobility and the Stability of Solution‐Processed Zinc‐Tin Oxide Thin‐Film Transistors Using Alkali Metal Superoxide

We have studied how to improve the mobility and stability of solution processed zinc‐tin oxide thin‐film transistors (ZTO TFTs) simultaneously using multifunctional potassium superoxide precursor. Potassium cations in the potassium superoxide precursor acts as a shallow donor in the ZTO thin film to improve the carrier concentration (electron), which allows the potassium‐doped ZTO TFT to exhibit high mobility. Then, the anion of the precursor exists as a superoxide radical, and it showed the effect of reducing the oxygen vacancy in the process of forming the oxide thin film Consequently, potassium‐doped ZTO TFT using potassium superoxide precursor exhibited improved mobility and stability, showing an increase in the mobility from 5.11 to 8.36 cm 2 /Vs and a decrease in the threshold voltage shift from 4.65 to 3.36 V under a negative bias temperature illumination stress test conducted over 5,000 sec..

Jung, Tae Soo↗

A Low-Temperature, Solution-Processable Organic Electron-Transporting Layer Based on Planar Coronene for High-performance Conventional Perovskite Solar Cells

A low-temperature, solution-processable organic electron-transporting material (ETM) is successfully developed for efficient conventional n-i-p perovskite solar cells (PVSCs). This ETM can show a high efficiency over 17% on rigid device and 14.2% on flexible PVSC. Lastly, to the best of our knowledge, this efficiency is among the highest values reported for flexible n-i-p PVSCs with negligible hysteresis thus far.

14 SOLAR ENERGY↗

Solution-processed BiI 3 thin films for photovoltaic applications: Improved carrier collection via solvent annealing

Here, we report all-inorganic solar cells based on solution-processed BiI 3 . Two-electron donor solvents such as tetrahydrofuran and dimethylformamide were found to form adducts with BiI 3 , which make them highly soluble in these solvents. BiI 3 thin films were deposited by spin-coating. Solvent annealing BiI 3 thin films at relatively low temperatures (≤100 °C) resulted in increased grain size and crystallographic reorientation of grains within the films. The BiI3 films were stable against oxidation for several months and could withstand several hours of annealing in air at temperatures below 150 °C without degradation. Surface oxidation was found to improve photovoltaic device performance due to the formation of a BiOI layer at the BiI 3 surface which facilitated hole extraction. Nonoptimized BiI 3 solar cells achieved the highest power conversion efficiencies of 1.0%, demonstrating the potential of BiI 3 as a nontoxic, air-stable metal-halide absorber material for photovoltaic applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Room-temperature, solution-processable organic electron extraction layer for high-performance planar heterojunction perovskite solar cells

Here in this work, we describe a room-temperature, solution-processable organic electron extraction layer (EEL) for high-performance planar heterojunction perovskite solar cells (PHJ PVSCs). This EEL is composed of a bilayered fulleropyrrolidinium iodide (FPI)-polyethyleneimine (PEIE) and PC 61 BM, which yields a promising power conversion efficiency (PCE) of 15.7% with insignificant hysteresis. We reveal that PC 61 BM can serve as a surface modifier of FPI-PEIE to simultaneously facilitate the crystallization of perovskite and the charge extraction at FPI-PEIE/CH 3 NH 3 PbI 3 interface. Furthermore, the FPI-PEIE can also tune the work function of ITO and dope PC 61 BM to promote the efficient electron transport between ITO and PC 61 BM. Based on the advantages of room-temperature processability and decent electrical property of FPI-PEIE/PC 61 BM EEL, a high-performance flexible PVSC with a PCE ~10% is eventually demonstrated. Lastly, this study shows the potential of low-temperature processed organic EEL to replace transition metal oxide-based interlayers for highly printing compatible PVSCs with high-performance.

14 SOLAR ENERGY↗

Solution-processed PCDTBT capped low-voltage InGaZnO{sub x} thin film phototransistors for visible-light detection

The effects of visible-light detection based on solution processed poly[N-9′′-hepta-decanyl-2,7-carbazole-alt-5,5-(4′,7′-di-2-thienyl-2′,1′, 3′benzothiadiazole) (PCDTBT) capped InGaZnOx (IGZO) phototransistors with Al{sub 2}O{sub x} serving as gate dielectric are investigated in this paper. The high-k dielectric is used to lower the device operating voltage down to 2 V. Photons emitted from laser sources with the wavelengths (λ) of 532 nm and 635 nm are absorbed through the layer of PCDTBT to generate electron-hole-pairs (EHPs). After the separation of EHPs, electrons are injected into IGZO layer through the p-n junction formed between the IGZO (n-type semiconductor) and the PCDTBT (p-type semiconductor). The photo-generated carriers boost the drain current of the transistors as well as bring about the negative threshold voltage shift. Significant enhanced detection performance is achieved under the laser wavelength of 532 nm. The highest photoresponsivity reaches up to 20 A/W, while the photoresponse rise time comes to 10 ms and the fall time comes to approximate 76 ms, which is much faster than trap assisted IGZO visible light detection. The fabricated phototransistors favor the application of visible-light detectors and/or optical switches.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Light-induced hysteresis and recovery behaviors in photochemically activated solution-processed metal-oxide thin-film transistors

In this report, photo-induced hysteresis, threshold voltage (V{sub T}) shift, and recovery behaviors in photochemically activated solution-processed indium-gallium-zinc oxide (IGZO) thin-film transistors (TFTs) are investigated. It was observed that a white light illumination caused negative V{sub T} shift along with creation of clockwise hysteresis in electrical characteristics which can be attributed to photo-generated doubly ionized oxygen vacancies at the semiconductor/gate dielectric interface. More importantly, the photochemically activated IGZO TFTs showed much reduced overall V{sub T} shift compared to thermally annealed TFTs. Reduced number of donor-like interface states creation under light illumination and more facile neutralization of ionized oxygen vacancies by electron capture under positive gate potential are claimed to be the origin of the less V{sub T} shift in photochemically activated TFTs.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

White top-emitting organic light-emitting diodes with solution-processed nano-particle scattering layers

A random scattering approach to enhance light extraction in white top-emitting organic light-emitting diodes (OLEDs) is reported. Through solution processing from fluorinated solvents, a nano-particle scattering layer (NPSL) can be deposited directly on top of small molecule OLEDs without affecting their electrical performance. The scattering length for light inside the NPSL is determined from transmission measurements and found to be in agreement with Mie scattering theory. Furthermore, the dependence of the light outcoupling enhancement on electron transport layer thickness is studied. Depending on the electron transport layer thickness, the NPSL enhances the external quantum efficiency of the investigated white OLEDs by between 1.5 and 2.3-fold. For a device structure that has been optimized prior to application of the NPSL, the maximum external quantum efficiency is improved from 4.7% to 7.4% (1.6-fold improvement). In addition, the scattering layer strongly reduces the undesired shift in emission color with viewing angle.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Low cost and solution processible sandwiched CH3NH3PbI3-xClx based photodetector

Highlights: • High quality CH{sub 3}NH{sub 3}PbI{sub 3-x}Cl{sub x} thin film is synthesized using low temperature solution processible spin coating technique. • Perovskite based Metal-semiconductor-metal (MSM) photodetector is demonstrated without hole or electron transporting materials or noble metals. • Low cost & simple structured perovskite device exhibits good transient response, responsivity and detectivity. - Abstract: The CH{sub 3}NH{sub 3}PbI{sub 3-x}Cl{sub x} has been emerged as one of the most promising materials for the photodetector based applications. In recent years, many device structures consisting of hole transporting material, electron transporting material, conducting polymers and noble metals as contact electrodes have been investigated which escort to the increased cost and complexity in the fabrication process. Hence, it is essential to explore low cost, simple processed and high-performance photodetectors. The effect of applied external bias on photodetector has been examined in order to investigate performance. It is important to mention that because of the ion migration phenomenon taking place across the junction at higher bias, an unsaturated photocurrent has been observed during ON time of the photoresponse which may be scope of study for furtherance in low cost and highly stable photodetector. Responsivity and detectivity has been increased by 40 and 32 times at 1.2 V. Similarly, LDR is increased by 8 times.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗