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Kang, Joohoon

Publications and source records attributed to Kang, Joohoon.

Two-Step Patterning of Scalable All-Inorganic Halide Perovskite Arrays

Halide perovskites have many important optoelectronic properties, including high emission efficiency, high absorption coefficients, color purity, and tunable emission wavelength, which makes these materials promising for optoelectronic applications. However, the inability to precisely control large-scale patterned growth of halide perovskites limits their potential toward various device applications. Here, we report a patterning method for the growth of a cesium lead halide perovskite single crystal array. Our approach consists of two steps: (1) cesium halide salt arrays patterning and (2) chemical vapor transport process to convert salt arrays into single crystal perovskite arrays. Characterizations including energy-dispersive X-ray spectroscopy and photoluminescence have been employed to confirm the chemical compositions and the optical properties of the as-synthesized perovskite arrays. This patterning method enables the patterning of single crystal cesium lead halide perovskite arrays with tunable spacing (from 2 to 20 μm) and crystal size (from 200 nm to 1.2 μm) in high production yield (almost every pixel in the array is successfully grown with converted perovskite crystals). Furthermore, our large-scale patterning method renders a platform for the study of fundamental properties and opportunities for perovskite-based optoelectronic applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Structural and spectral dynamics of single-crystalline Ruddlesden-Popper phase halide perovskite blue light-emitting diodes

Achieving perovskite-based high–color purity blue-emitting light-emitting diodes (LEDs) is still challenging. Here, we report successful synthesis of a series of blue-emissive two-dimensional Ruddlesden-Popper phase single crystals and their high–color purity blue-emitting LED demonstrations. Although this approach successfully achieves a series of bandgap emissions based on the different layer thicknesses, it still suffers from a conventional temperature-induced device degradation mechanism during high-voltage operations. To understand the underlying mechanism, we further elucidate temperature-induced device degradation by investigating the crystal structural and spectral evolution dynamics via in situ temperature-dependent single-crystal x-ray diffraction, photoluminescence (PL) characterization, and density functional theory calculation. The PL peak becomes asymmetrically broadened with a marked intensity decay, as temperature increases owing to [PbBr 6 ] 4- octahedra tilting and the organic chain disordering, which results in bandgap decrease. This study indicates that careful heat management under LED operation is a key factor to maintain the sharp and intense emission.

36 MATERIALS SCIENCE↗

Three-Dimensional Phthalocyanine Metal-Catecholates for High Electrochemical Carbon Dioxide Reduction

The synthesis of a new anionic 3D metal-catecholate framework, termed MOF-1992, is achieved by linking tetratopic cobalt phthalocyanin-2,3,9,10,16,17,23,24-octaol linkers with Fe 3 (-C 2 O 2 -) 6 (OH 2 ) 2 trimers into an extended framework of roc topology. MOF-1992 exhibits sterically accessible Co active sites together with charge transfer properties. Cathodes based on MOF-1992 and carbon black (CB) display a high coverage of electroactive sites (270 nmol cm -2 ) and a high current density (-16.5 mA cm -2 ; overpotential, -0.52 V) for the CO 2 to CO reduction reaction in water (faradaic efficiency, 80%). Finally, over the 6 h experiment, MOF-1992/CB cathodes reach turnover numbers of 5800 with turnover frequencies of 0.20 s -1 per active site.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Self-Assembly of Two-Dimensional Perovskite Nanosheet Building Blocks into Ordered Ruddlesden–Popper Perovskite Phase

The self-assembly of nanoparticles, a process whereby nanocrystal building blocks organize into even more ordered superstructures, is of great interest to nanoscience. In this work, we report the layer-by-layer assembly of 2D perovskite nanosheet building blocks. Structural analysis reveals that the assembled superlattice nanocrystals match with the layered Ruddlesden-Popper perovskite phase. This assembly proves reversible, as these superlattice nanocrystals can be reversibly exfoliated back into their building blocks via sonication. This study demonstrates the opportunity to further understand and exploit thermodynamics to increase order in a system of nanoparticles and to study emergent optical properties of a superlattice from 2D, weakly attracted, perovskite building blocks.

42 ENGINEERING↗

Hybrid silicon lasers and amplifiers with 2D phosphorene film

Hybrid silicon lasers and amplifiers having resonator cavities within a silicon substrate and a two-dimensional material film on the substrate as an optical gain medium are described. The two-dimensional material film may be formed of one or more atomic layers of phosphorene (BP). The number of phosphorene layers may be adjusted to tune the emission wavelength of the hybrid devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Nanowires for Photonics

All-photonic integrated circuits are promising platforms for future systems beyond the limitation of Moore's law. Over the last several decades, one-dimensional (1D) nanowires have demonstrated great potential in photonic circuitry because of their unique 1D structure to effectively generate and tightly confine optical signals as well as easily tunable optical properties. In this Review, we categorize nanowires based on the optical properties (i.e., semiconducting, metallic, and dielectric nanowires) for their potential photonic applications (as light emitters or plasmonic and photonic waveguides). We further discuss the recent efforts in integration of nanowire-based photonic elements toward next-generation optical information processors. However, there are still several challenges remaining before the nanowires are fully utilized as photonic building blocks. In conclusion, the scientific and technical challenges and outlooks are provided to indicate the future directions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Hot Carrier and Surface Recombination Dynamics in Layered InSe Crystals

Layered indium selenide (InSe) is a van der Waals solid that has emerged as a promising material for high-performance ultrathin solar cells. The optoelectronic parameters that are critical to photoconversion efficiencies, such as hot carrier lifetime and surface recombination velocity, are however largely unexplored in InSe. Here, these key photophysical properties of layered InSe are measured with femtosecond transient reflection spectroscopy. The hot carrier cooling process is found to occur through phonon scattering. The surface recombination velocity and ambipolar diffusion coefficient are extracted from fits to the pump energy-dependent transient reflection kinetics using a free carrier diffusion model. The extracted surface recombination velocity is approximately an order of magnitude larger than that for methylammonium lead-iodide perovskites, suggesting that surface recombination is a principal source of photocarrier loss in InSe. The extracted ambipolar diffusion coefficient is consistent with previously reported values of InSe carrier mobility.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Solution-Processed Layered Gallium Telluride Thin-Film Photodetectors

Using scalable solution processing, layered gallium telluride (GaTe) nanoflake dispersions are produced in surfactant-free, low-boiling-point, water–ethanol cosolvent mixtures. During exfoliation, chemical degradation of the ambient-reactive GaTe crystals is minimized by using deoxygenated solvents in a sealed tip ultrasonication system. The structural and chemical integrity of the solution-processed GaTe nanoflakes is subsequently confirmed with a comprehensive suite of microscopic and spectroscopic analyses. Furthermore, field-effect transistors and phototransistors based on individual solution-processed GaTe nanoflakes show electronic and optoelectronic properties, respectively, that are comparable to micromechanically exfoliated GaTe. Minimal solution-processing residues from the surfactant-free, low-boiling-point cosolvent dispersion medium coupled with the high intrinsic hole doping of GaTe produces the highest electrical conductivity among solution-processed layered nanoflake thin films without post-treatment. Large-area photodetectors based on these electrically percolating thin films of solution-processed GaTe nanoflakes show a positive correlation between responsivity and illumination intensity, with a high photoconversion gain that is explained by a combination of defect-mediated optical processes and photothermal effects. Finally, overall, this study establishes solution-processed layered GaTe nanoflakes as a leading candidate for high-performance, large-area, thin-film photodetectors.

47 OTHER INSTRUMENTATION↗

Silicon-Phosphorene Nanocavity-Enhanced Optical Emission at Telecommunications Wavelengths

Generating and amplifying light in silicon (Si) continues to attract significant attention due to the possibility of integrating optical and electronic components in a single material platform. Unfortunately, silicon is an indirect band gap material and therefore an inefficient emitter of light. With the rise of integrated photonics, the search for silicon-based light sources has evolved from a scientific quest to a major technological bottleneck for scalable, CMOS-compatible, light sources. Recently, emerging two-dimensional materials have opened the prospect of tailoring material properties based on atomic layers. Few-layer phosphorene, which is isolated through exfoliation from black phosphorus (BP), is a great candidate to partner with silicon due to its layer-tunable direct band gap in the near-infrared where silicon is transparent. Here we demonstrate a hybrid silicon optical emitter composed of few-layer phosphorene nanomaterial flakes coupled to silicon photonic crystal resonators. We show single-mode emission in the telecommunications band of 1.55 μm ($E_g$ = 0.8 eV) under continuous wave optical excitation at room temperature. The solution-processed few-layer BP flakes enable tunable emission across a broad range of wavelengths and the simultaneous creation of multiple devices. Our work highlights the versatility of the Si-BP material platform for creating optically active devices in integrated silicon chips.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Revealing the Effects of Electrode Crystallographic Orientation on Battery Electrochemistry via the Anisotropic Lithiation and Sodiation of ReS 2

Practical application of electrochemical water splitting demands durable, efficient, and non-noble metal catalysts for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Herein, we report a new hydrogen evolution nanowire electrocatalyst, consisting of S-doped CoWP nanoparticles embedded in S- and N-doped carbon matrix (S-CoWP@(S,N)-C), which is in situ transformed from Hofmann-type (Co, W)-based metal–organic framework (MOF) nanowires. Because of S and N doping to the carbon matrix and the S doping to CoWP nanoparticles, the obtained S-CoWP@(S,N)-C catalyst reaches a current density of -10 mA cm –2 at -35 and -67 mV (vs RHE) in acidic and alkaline electrolytes, respectively. Powered by a lead halide perovskite solar cell, an unassisted two-electrode solar water-splitting device using MOF-derived S-CoWP@(S,N)-C HER electrocatalysts and S-CoW@(S,N)-C OER electrocatalysts displays a solar-to-hydrogen conversion efficiency of 10.98%. Our method is highly applicable for developing robust electrocatalysts toward efficient and low-cost solar-driven water splitting.

25 ENERGY STORAGE↗

Anhydrous Liquid-Phase Exfoliation of Pristine Electrochemically Active GeS Nanosheets

Germanium sulfide (GeS) is an emerging layered material with high promise in its two-dimensional (2D) exfoliated form for energy storage applications. While liquid-phase exfoliation (LPE) has been utilized for the low-cost, scalable production of related 2D materials, it has not yet been demonstrated for GeS nanosheets due to its chemical instability in ambient conditions. Here, GeS LPE is achieved in anhydrous N-methyl-2-pyrrolidone using a customized sealed-tip sonication system, yielding sub-10 nm thick GeS nanosheets that are structurally pristine with minimal chemical degradation as revealed by atomic force microscopy, Raman spectroscopy, X-ray photoelectron spectroscopy, and transmission electron microscopy. Lithium-ion battery anodes based on these high-quality GeS nanosheets possess superlative electrochemical performance including high cycling stability over 1000 cycles and high rate capability in excess of 10 A g –1 . Finally, overall, this work establishes a scalable LPE pathway for the production of pristine electrochemically active GeS nanosheets that are well-suited for high-power lithium-ion battery applications.

25 ENERGY STORAGE↗

Layer-by-Layer Sorting of Rhenium Disulfide via High-Density Isopycnic Density Gradient Ultracentrifugation

Isopycnic density gradient ultracentrifugation (iDGU) has been widely applied to sort nanomaterials by their physical and electronic structure. Yet, the commonly used density-gradient medium iodixanol has a finite maximum buoyant density that prevents the use of iDGU for high-density nanomaterials. Here, we overcome this limit by adding cesium chloride (CsCl) to iodixanol, thus increasing its maximum buoyant density to the point where the high-density two-dimensional nanomaterial rhenium disulfide (ReS 2 ) can be sorted in a layer-by-layer manner with iDGU. The resulting aqueous ReS 2 dispersions show photoluminescence at ~1.5 eV, which is consistent with its direct bandgap semiconductor electronic structure. Moreover, photocurrent measurements on thin films formed from solution-processed ReS 2 show a spectral response that is consistent with optical absorbance and photoluminescence data. In addition to offering a pathway for effective solution processing of ReS 2 , this work establishes a general methodology for sorting high-density nanomaterials via iDGU.

36 MATERIALS SCIENCE↗