Atomic-Level Microstructure of Efficient Formamidinium-Based Perovskite Solar Cells Stabilized by 5-Ammonium Valeric Acid Iodide Revealed by Multinuclear and Two-Dimensional Solid-State NMR.

Chemical doping of inorganic-organic hybrid perovskites is an effective way of improving the performance and operational stability of perovskite solar cells (PSCs). Here we use 5-ammonium valeric acid iodide (AVAI) to chemically stabilize the structure of α-FAPbI3. Using solid-state MAS NMR, we demonstrate the atomic-level interaction between the molecular modulator and the perovskite lattice and propose a structural model of the stabilized three-dimensional structure, further aided by density functional theory (DFT) calculations. We find that one-step deposition of the perovskite in the presence of AVAI produces highly crystalline films with large, micrometer-sized grains and enhanced charge-carrier lifetimes, as probed by transient absorption spectroscopy. As a result, we achieve greatly enhanced solar cell performance for the optimized AVA-based devices with a maximum power conversion efficiency (PCE) of 18.94%. The devices retain 90% of the initial efficiency after 300 h under continuous white light illumination and maximum-power point-tracking measurement.

Impact of roughening density on the light extraction efficiency of thin-film flip-chip ultraviolet LEDs grown on SiC.

Discovering ways to increase the LED light extraction efficiency (LEE) should help create the largest performance improvement in the power of UV AlGaN LEDs. Employing surface roughening to increase the LEE of typical AlGaN UV LEDs is challenging and not well understood, yet it can be achieved easily in AlGaN LEDs grown on SiC. We fabricate thin-film UV LEDs (~294-310 nm) grown on SiC-with reflective contacts and roughened emission surface-to study and optimize KOH roughening of N-face AlN on the LEE as a function of roughened AlN pyramid size and KOH solution temperature. The LEE increased the most (2X) when the average AlN pyramid base diagonals (d) were comparable to the electroluminescence (EL) wavelength in the AlN layer (d ~λEL; 42-52 pyramids/µm2), but the LEE enhancement diminished when d was much larger than λEL (d ~5.5λEL; 2-3 pyramids/µm2). The UV LEDs had a 10 nm p-GaN contact layer, and the forward voltage was ~6 V at ~8 A/cm2, with a voltage efficiency (VE) of ~70%. The VE of the LEDs did not change after KOH roughening. This work suggests important implications to increase the LEE of AlGaN LEDs.

High-power blue superluminescent diode for high CRI lighting and high-speed visible light communication.

We demonstrated a high-power (474 mW) blue superluminescent diode (SLD) on c-plane GaN-substrate for speckle-free solid-state lighting (SSL), and high-speed visible light communication (VLC) link. The device, emitting at 442 nm, showed a large spectral bandwidth of 6.5 nm at an optical power of 105 mW. By integrating a YAG-phosphor-plate to the SLD, a CRI of 85.1 and CCT of 3392 K were measured, thus suitable for solid-state lighting. The SLD shows a relatively large 3-dB modulation bandwidth of >400 MHz, while a record high data rate of 1.45 Gigabit-per-second (Gbps) link has been achieved below forward-error correction (FEC) limit under non-return-to-zero on-off keying (NRZ-OOK) modulation scheme. Our results suggest that SLD is a promising alternative for simultaneous speckle-free white lighting and Gbps data communication dual functionalities.

Droop-free AlxGa1-xN/AlyGa1-yN quantum-disks-in-nanowires ultraviolet LED emitting at 337 nm on metal/silicon substrates.

Currently the AlGaN-based ultraviolet (UV) solid-state lighting research suffers from numerous challenges. In particular, low internal quantum efficiency, low extraction efficiency, inefficient doping, large polarization fields, and high dislocation density epitaxy constitute bottlenecks in realizing high power devices. Despite the clear advantage of quantum-confinement nanostructure, it has not been widely utilized in AlGaN-based nanowires. Here we utilize the self-assembled nanowires (NWs) with embedding quantum-disks (Qdisks) to mitigate these issues, and achieve UV emission of 337 nm at 32 A/cm2 (80 mA in 0.5 × 0.5 mm2 device), a turn-on voltage of ~5.5 V and droop-free behavior up to 120 A/cm2 of injection current. The device was grown on a titanium-coated n-type silicon substrate, to improve current injection and heat dissipation. A narrow linewidth of 11.7 nm in the electroluminescence spectrum and a strong wavefunctions overlap factor of 42% confirm strong quantum confinement within uniformly formed AlGaN/AlGaN Qdisks, verified using transmission electron microscopy (TEM). The nitride-based UV nanowires light-emitting diodes (NWs-LEDs) grown on low cost and scalable metal/silicon template substrate, offers a scalable, environment friendly and low cost solution for numerous applications, such as solid-state lighting, spectroscopy, medical science and security.

Ultrabroad linewidth orange-emitting nanowires LED for high CRI laser-based white lighting and gigahertz communications.

Group-III-nitride laser diode (LD)-based solid-state lighting device has been demonstrated to be droop-free compared to light-emitting diodes (LEDs), and highly energy-efficient compared to that of the traditional incandescent and fluorescent white light systems. The YAG:Ce3+ phosphor used in LD-based solid-state lighting, however, is associated with rapid degradation issue. An alternate phosphor/LD architecture, which is capable of sustaining high temperature, high power density, while still intensity- and bandwidth-tunable for high color-quality remained unexplored. In this paper, we present for the first time, the proof-of-concept of the generation of high-quality white light using an InGaN-based orange nanowires (NWs) LED grown on silicon, in conjunction with a blue LD, and in place of the compound-phosphor. By changing the relative intensities of the ultrabroad linewidth orange and narrow-linewidth blue components, our LED/LD device architecture achieved correlated color temperature (CCT) ranging from 3000 K to above 6000K with color rendering index (CRI) values reaching 83.1, a value unsurpassed by the YAG-phosphor/blue-LD counterpart. The white-light wireless communications was implemented using the blue LD through on-off keying (OOK) modulation to obtain a data rate of 1.06 Gbps. We therefore achieved the best of both worlds when orange-emitting NWs LED are utilized as "active-phosphor", while blue LD is used for both color mixing and optical wireless communications.

Mitigation of acyl-homoserine lactone (AHL) based bacterial quorum sensing, virulence functions, and biofilm formation by yttrium oxide core/shell nanospheres: Novel approach to combat drug resistance.

The present study evaluated the efficacy of Y2O3:Tb (core) and Y2O3:Tb@SiO2 nanospheres (core/shell NSs) against virulence functions regulated by quorum sensing (QS) and biofilm formation in pathogenic bacteria. Scanning electron microscope (SEM) images were used to study the size, shape, and morphology. The images clearly displayed spherical shaped, mono-dispersed particles with narrow size distribution and an average grain size of 110-130 nm. The chemical composition of the samples was determined by using energy dispersive X-ray (EDX) and X-ray photoelectron spectroscopy (XPS). We determined the impact of core and core/shell NSs on QS using sensor strains of Chromobacterium violaceum CVO26 and Pseudomonas aeruginosa PAO1 in a comparative study. Sub-MICs of core and core/shell NSs substantially suppressed QS-controlled violacein production in C. violaceum. Similar concentration-dependent effect of sub-MICs of synthesized core and core/shell NSs was observed in the QS-regulated virulence functions (elastase, total protease, pyocyanin production, swarming motility, and exopolysaccharide production) in PAO1. A concentration-dependent decrease (14-60%) was recorded in the biofilm forming capability of PAO1, upon treatment with core and core/shell NSs. Moreover, core/shell NSs were more effective in inhibiting biofilm at higher tested concentrations as compared to core-NSs. The synthesized NSs demonstrated significantly impaired attachment of cells to the microtiter plate indicating that NSs target biofilm inhibition at the attachment stage. Based on these results, we predict that core and core/shell NSs may be an alternative to combat the threat of drug-resistant pathogenic bacteria.

Perovskite Solar Cells Yielding Reproducible Photovoltage of 1.20 V.

High photovoltages and power conversion efficiencies of perovskite solar cells (PSCs) can be realized by controlling the undesired nonradiative charge carrier recombination. Here, we introduce a judicious amount of guanidinium iodide into mixed-cation and mixed-halide perovskite films to suppress the parasitic charge carrier recombination, which enabled the fabrication of >20% efficient and operationally stable PSCs yielding reproducible photovoltage as high as 1.20 V. By introducing guanidinium iodide into the perovskite precursor solution, the bandgap of the resulting absorber material changed minimally; however, the nonradiative recombination diminished considerably as revealed by time-resolved photoluminescence and electroluminescence studies. Furthermore, using capacitance-frequency measurements, we were able to correlate the hysteresis features exhibited by the PSCs with interfacial charge accumulation. This study opens up a path to realize new record efficiencies for PSCs based on guanidinium iodide doped perovskite films.

Physico-chemical properties and catalytic activity of the sol-gel prepared Ce-ion doped LaMnO3 perovskites.

Ce-doped LaMnO3 perovskite ceramics (La1-xCexMnO3) were synthesized by sol-gel based co-precipitation method and tested for the oxidation of benzyl alcohol using molecular oxygen. Benzyl alcohol conversion of ca. 25-42% was achieved with benzaldehyde as the main product. X-ray diffraction (XRD), thermogravimetric analysis (TGA), BET surface area, transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), temperature-programmed reduction (H2-TPR), temperature-programmed oxidation (O2-TPO), FT-IR and UV-vis spectroscopic techniques were used to examine the physiochemical properties. XRD analysis demonstrates the single phase crystalline high purity of the perovskite. The Ce-doped LaMnO3 perovskite demonstrated reducibility at low-temperature and higher mobility of surface O2-ion than their respective un-doped perovskite. The substitution of Ce3+ ion into the perovskite matrix improve the surface redox properties, which strongly influenced the catalytic activity of the material. The LaMnO3 perovskite exhibited considerable activity to benzyl alcohol oxidation but suffered a slow deactivation with time-on-stream. Nevertheless, the insertion of the A site metal cation with a trivalent Ce3+ metal cation led to an enhanced in catalytic performance because of atomic-scale interactions between the A and B active site. La0.95Ce0.05MnO3 catalyst demonstrated the excellent catalytic activity with a selectivity of 99% at 120 °C.

Atomic-level passivation mechanism of ammonium salts enabling highly efficient perovskite solar cells.

The high conversion efficiency has made metal halide perovskite solar cells a real breakthrough in thin film photovoltaic technology in recent years. Here, we introduce a straightforward strategy to reduce the level of electronic defects present at the interface between the perovskite film and the hole transport layer by treating the perovskite surface with different types of ammonium salts, namely ethylammonium, imidazolium and guanidinium iodide. We use a triple cation perovskite formulation containing primarily formamidinium and small amounts of cesium and methylammonium. We find that this treatment boosts the power conversion efficiency from 20.5% for the control to 22.3%, 22.1%, and 21.0% for the devices treated with ethylammonium, imidazolium and guanidinium iodide, respectively. Best performing devices showed a loss in efficiency of only 5% under full sunlight intensity with maximum power tracking for 550 h. We apply 2D- solid-state NMR to unravel the atomic-level mechanism of this passivation effect.

Direct Growth of III-Nitride Nanowire-Based Yellow Light-Emitting Diode on Amorphous Quartz Using Thin Ti Interlayer.

Consumer electronics have increasingly relied on ultra-thin glass screen due to its transparency, scalability, and cost. In particular, display technology relies on integrating light-emitting diodes with display panel as a source for backlighting. In this study, we undertook the challenge of integrating light emitters onto amorphous quartz by demonstrating the direct growth and fabrication of a III-nitride nanowire-based light-emitting diode. The proof-of-concept device exhibits a low turn-on voltage of 2.6 V, on an amorphous quartz substrate. We achieved ~ 40% transparency across the visible wavelength while maintaining electrical conductivity by employing a TiN/Ti interlayer on quartz as a translucent conducting layer. The nanowire-on-quartz LED emits a broad linewidth spectrum of light centered at true yellow color (~ 590 nm), an important wavelength bridging the green-gap in solid-state lighting technology, with significantly less strain and dislocations compared to conventional planar quantum well nitride structures. Our endeavor highlighted the feasibility of fabricating III-nitride optoelectronic device on a scalable amorphous substrate through facile growth and fabrication steps. For practical demonstration, we demonstrated tunable correlated color temperature white light, leveraging on the broadly tunable nanowire spectral characteristics across red-amber-yellow color regime.