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1.
Nano Lett ; 17(3): 2021-2027, 2017 03 08.
Article in English | MEDLINE | ID: mdl-28145714

ABSTRACT

Understanding defect chemistry, particularly ion migration, and its significant effect on the surface's optical and electronic properties is one of the major challenges impeding the development of hybrid perovskite-based devices. Here, using both experimental and theoretical approaches, we demonstrated that the surface layers of the perovskite crystals may acquire a high concentration of positively charged vacancies with the complementary negatively charged halide ions pushed to the surface. This charge separation near the surface generates an electric field that can induce an increase of optical band gap in the surface layers relative to the bulk. We found that the charge separation, electric field, and the amplitude of shift in the bandgap strongly depend on the halides and organic moieties of perovskite crystals. Our findings reveal the peculiarity of surface effects that are currently limiting the applications of perovskite crystals and more importantly explain their origins, thus enabling viable surface passivation strategies to remediate them.

2.
J Phys Chem Lett ; 8(1): 137-143, 2017 Jan 05.
Article in English | MEDLINE | ID: mdl-27966364

ABSTRACT

Hybrid organic-inorganic perovskite crystals have recently become one of the most important classes of photoactive materials in the solar cell and optoelectronic communities. Albeit improvements have focused on state-of-the-art technology including various fabrication methods, device architectures, and surface passivation, progress is yet to be made in understanding the actual operational temperature on the electronic properties and the device performances. Therefore, the substantial effect of temperature on the optoelectronic properties, charge separation, charge recombination dynamics, and photoconversion efficiency are explored. The results clearly demonstrated a significant enhancement in the carrier mobility, photocurrent, charge carrier lifetime, and solar cell performance in the 60 ± 5 °C temperature range. In this temperature range, perovskite crystal exhibits a highly symmetrical relaxed cubic structure with well-aligned domains that are perpendicular to a principal axis, thereby remarkably improving the device operation. This finding provides a new key variable component and paves the way toward using perovskite crystals in highly efficient photovoltaic cells.

3.
Nano Lett ; 16(2): 1056-63, 2016 Feb 10.
Article in English | MEDLINE | ID: mdl-26745217

ABSTRACT

High-quality nitride materials grown on scalable and low-cost metallic substrates are considerably attractive for high-power light-emitters. We demonstrate here, for the first time, the high-power red (705 nm) InGaN/GaN quantum-disks (Qdisks)-in-nanowire light-emitting diodes (LEDs) self-assembled directly on metal-substrates. The LEDs exhibited a low turn-on voltage of ∼2 V without efficiency droop up to injection current of 500 mA (1.6 kA/cm(2)) at ∼5 V. This is achieved through the direct growth and optimization of high-quality nanowires on titanium (Ti) coated bulk polycrystalline-molybdenum (Mo) substrates. We performed extensive studies on the growth mechanisms, obtained high-crystal-quality nanowires, and confirmed the epitaxial relationship between the cubic titanium nitride (TiN) transition layer and the hexagonal nanowires. The growth of nanowires on all-metal stack of TiN/Ti/Mo enables simultaneous implementation of n-metal contact, reflector, and heat sink, which greatly simplifies the fabrication process of high-power light-emitters. Our work ushers in a practical platform for high-power nanowires light-emitters, providing versatile solutions for multiple cross-disciplinary applications that are greatly enhanced by leveraging on the chemical stability of nitride materials, large specific surface of nanowires, chemical lift-off ready layer structures, and reusable Mo substrates.

4.
J Phys Chem Lett ; 7(1): 137-42, 2016 Jan 07.
Article in English | MEDLINE | ID: mdl-26688008

ABSTRACT

The high optical gain and absorption of organic-inorganic hybrid perovskites have attracted attention for photonic device applications. However, owing to the sensitivity of organic moieties to solvents and temperature, device processing is challenging, particularly for patterning. Here, we report the direct patterning of perovskites using chemically gas-assisted focused-ion beam (GAFIB) etching with XeF2 and I2 precursors. We demonstrate etching enhancement in addition to controllability and marginal surface damage compared to focused-ion beam (FIB) etching without precursors. Utilizing the GAFIB etching, we fabricated a uniform and periodic submicron perovskite subwavelength grating (SWG) absorber with broadband absorption and nanoscale precision. Our results demonstrate the use of FIB as a submicron patterning tool and a means of providing surface treatment (after FIB patterning to minimize optical loss) for perovskite photonic nanostructures. The SWG absorber can be patterned on perovskite solar cells to enhance the device efficiency through increasing light trapping and absorption.

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