J. Y. Tsao,* S. Chowdhury, M. A. Hollis,* D. Jena, N. M. Johnson, K. A. Jones, R. J. Kaplar,* S. Rajan, C. G. Van de Walle, E. Bellotti, C. L. Chua, R. Collazo, M. E. Coltrin, J. A. Cooper, K. R. Evans, S. Graham, T. A. Grotjohn, E. R. Heller, M. Higashiwaki, M. S. Islam, P. W. Juodawlkis, M. A. Khan, A. D. Koehler, J. H. Leach, U. K. Mishra, R. J. Nemanich, R. C. N. Pilawa-Podgurski, J. B. Shealy, Z. Sitar, M. J. Tadjer, A. F. Witulski, M. Wraback, and J. A. Simmons

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Ultrawide-Bandgap Semiconductors: Research Opportunities and Challenges

Ambient stability of colloidal nanocrystal quantum dots (QDs) is imperative for low-cost, high-efficiency QD photovoltaics. We synthesized air-stable, ultrasmall PbS QDs with diameter (D) down to 1.5 nm, and found an abrupt transition at D ≈ 4 nm in the air stability as the QD size was varied from 1.5 to 7.5 nm. X-ray photoemission spectroscopy measurements and density functional theory calculations reveal that the stability transition is closely associated with the shape transition of oleate-capped QDs from octahedron to cuboctahedron, driven by steric hindrance and thus size-dependent surface energy of oleate-passivated Pb-rich QD facets. This microscopic understanding of the surface chemistry on ultrasmall QDs, up to a few nanometers, should be very useful for precisely and accurately controlling physicochemical properties of colloidal QDs such as doping polarity, carrier mobility, air stability, and hot-carrier dynamics for solar cell applications.

Steric-Hindrance-Driven Shape Transition in PbS Quantum Dots: Understanding Size-Dependent Stability

The recent advances in epitaxial SiC films' growth on Si are overviewed. The basic classical methods currently used for SiC films' growth are discussed and their advantages and disadvantages are explored. The basic idea and the theoretical background for a new method of the synthesis of epitaxial SiC films on Si are given. It will be shown that the new method is significantly different from the classical techniques of thin-film growth where the evaporation of the atoms onto the substrate surface is exploited. The new method is based on the substitution of some atoms in the silicon matrix by the carbon atoms to form the molecules of silicon carbide. It will be shown that the following process of SiC nucleation happens gradually without destroying the crystalline structure of the silicon matrix, and the orientation of a grown film is imposed by the original crystalline structure of the silicon matrix (not only by the substrate surface as in conventional methods of film growth). A comparison of the new method with other epitaxy techniques will be given.The new method of solid-phase epitaxy based on the substitution of atoms and on the creation of dilatation dipoles solves one of the major problems in heteroepitaxy. It provides the synthesis of low-defective unstrained epitaxial films with a large difference between the lattice parameters of the film and the substrate without using any additional buffer layers. This method has another unique feature distinguishing it from the classical techniques of SiC films' growth—it allows the growing of SiC films of hexagonal polytypes. A new kind of phase transformation in solids owing to the chemical transformation of one substance into another will be described theoretically and revealed experimentally. This type of phase transformation, and the mechanism of a broad class of heterogeneous chemical reactions between gas and solid phases, will be illustrated by an example of the growth of SiC epitaxial layers due to the chemical interaction of CO gas with the monocrystalline silicon matrix. The discovery of this mechanism yields a new kind of template: namely, substrates with buffer transition layers for wide-gap semiconductor growth on silicon. The properties of a variety of heteroepitaxial films of wide-gap semiconductors (SiC, AlN, GaN and AlGaN) grown on a SiC/Si substrate by solid-phase epitaxy will be reported. Grown films contain no cracks and have a quality sufficient to manufacture micro- and opto-electronic devices. Also, the new abilities in the synthesis of large (150 mm diameter) low-defective SiC films on Si substrates will be demonstrated.

https://iopscience.iop.org/article/10.1088/0022-3727/47/31/313001/pdf

Theory and practice of SiC growth on Si and its applications to wide-gap semiconductor films

Temperature-dependent photoluminescence (TDPL), one of the most effective and powerful optical characterisation methods, is widely used to investigate carrier transport and localized states in semiconductor materials. Resonant excitation and non-resonant excitation are the two primary methods of researching this issue. In this study, the application ranges of the different excitation modes are confirmed by analysing the TDPL characteristics of GaN-based light-emitting diodes. For resonant excitation, the carriers are generated only in the quantum wells, and the TDPL features effectively reflect the intrinsic photoluminescence characteristics within the wells and offer certain advantages in characterising localized states and the quality of the wells. For non-resonant excitation, both the wells and barriers are excited, and the carriers that drift from the barriers can contribute to the luminescence under the driving force of the built-in field, which causes the existing equations to become inapplicable. Thus, non-resonant excitation is more suitable than resonant excitation for studying carrier transport dynamics and evaluating the internal quantum efficiency. The experimental technique described herein provides fundamental new insights into the selection of the most appropriate excitation mode for the experimental analysis of carrier transport and localized states in p-n junction devices.

http://theory.iphy.ac.cn/English/paper/srep.4.6131.pdf

Temperature-dependent photoluminescence in light-emitting diodes.

Nonpolar and semipolar III-nitride-based blue and green light-emitting diodes (LEDs) have been extensively investigated as potential replacements for current polar c-plane LEDs. High-power and low-efficiency-droop blue LEDs have been demonstrated on nonpolar and semipolar planes III-nitride due to the advantages of eliminated or reduced polarization-related electric field and homoepitaxial growth. Semipolar (202¯1) and (202¯1¯) LEDs have contributed to bridging “green gap” (low efficiency in green spectral region) by incorporating high indium compositions, reducing polarization effects, and suppressing defects. Other properties, such as low thermal droop, narrow spectral linewidth, small wavelength shift, and polarized emission, have also been reported for nonpolar and semipolar LEDs. In this paper we review the theoretical background, device performance, material properties, and physical mechanisms for nonpolar and semipolar III-nitride semiconductors and associated blue and green LEDs. The latest progress on topics including efficiency droop, thermal droop, green-gap, and three-dimensional nanostructures is detailed. Future challenges, potential solutions, and applications will also be covered.

Toward ultimate efficiency: progress and prospects on planar and 3D nanostructured nonpolar and semipolar InGaN light-emitting diodes

Electrically driven quantum dot, wire, and well hybrid light-emitting diodes are demonstrated by using nanometer-sized pyramid structures of GaN. InGaN quantum dots, wires, and wells are formed at the tops, edges, and sidewalls of pyramids, respectively. The hybrid light-emitting diodes containing low-dimensional quantum structures are good candidates for broad-band highly efficient visible lighting sources.

Electrically Driven Quantum Dot/Wire/Well Hybrid Light-Emitting Diodes

We report the formation mechanism and the characteristics of catalyst-free and mask-free heteroepitaxial GaN submicrometer- and micrometer-sized rods (SMRs) under biaxial strain grown on Si(111) substrates by metal–organic chemical vapor deposition. We found that the GaN SMRs on Si(111) substrates were subject to strong tensile strain on their N-terminated top (0001) GaN surface due to the lattice mismatch between GaN and Si. Our calculations based on the density functional theory showed that the (0001) GaN surface energy increased (decreased) monotonically with increasing tensile (compressive) strain, resulting in a faster GaN growth rate of the tensile-strained top (0001) surface of GaN SMRs than that of the compressive-strained one. We experimentally verified this result by comparing GaN on Si(111) substrates with tensile strain and on 6H-SiC substrates with compressive strain. In addition, we confirmed that the vertical growth rate of GaN SMRs could be controlled by adjusting growth conditions, esp...

Growth Mechanism of Catalyst-Free and Mask-Free Heteroepitaxial GaN Submicrometer- and Micrometer-Sized Rods under Biaxial Strain: Variation of Surface Energy and Adatom Kinetics

A dislocation-eliminating chemical control method for high-quality GaN nanostructures together with various types of InGaN quantum well structures are demonstrated using a chemical vapor-phase etching technique. Unlike chemical wet etching, chemical vapor-phase etching could efficiently control the GaN and form various shapes of dislocation-free and strain-relaxed GaN nanostructures. The chemically controlled GaN nanostructures showed improved crystal quality due to the selective etching of defects and revealed various facets with reduced residual strain via the facet-selective etching mechanism. These structural properties derived excellent optical performance of the GaN nanostructures. The chemical vapor-phase etching method also showed possibilities of the fascinating applications for high-efficiency InGaN quantum well structures, such as InGaN quantum well layer on void embedded GaN layer, InGaN quantum well embedded GaN nanostructure, and InGaN/GaN core/shell nanostructure.

Dislocation-Eliminating Chemical Control Method for High-Efficiency GaN-Based Light Emitting Nanostructures

Ultrashort carrier lifetime of vapor–liquid–solid-grown GaN/InGaN multi-quantum-well coaxial nanorods

We report the measurement of the (r13, r33) Pockels electro-optic coefficients in a GaN thin film grown on a Si(111) substrate. The converse piezoelectric (d33) and electro-absorptive coefficients are simultaneously determined. Single crystalline GaN epitaxial layers were grown with a AlGaN buffer layer by metal organic chemical vapor deposition, and their structural and optical properties were systematically investigated. The electro-optic, converse piezoelectric, and electro-absorptive coefficients of the GaN layer are determined using an original method. A semi-transparent gold electrode is deposited on the top of the GaN layer, and an alternating voltage is applied between top and bottom electrodes. The coefficients are simultaneously and analytically determined from the measurement of the electric-field-induced variation ΔR(θ) in the reflectivity of the Au/GaN/buffer/Si stack, versus incident angle and light polarization. The method also enables to determine the GaN layer polarity. The results obtained for a Ga-face [0001] GaN layer when using a modulation frequency of 230 Hz are for the electro-optic coefficients r13 = +1.00 ± 0.02 pm/V, r33 = +1.60 ± 0.05 pm/V at 633 nm, and for the converse piezoelectric coefficient d33 = +4.59 ± 0.03 pm/V. The value measured for the electro-absorptive variation at 633 nm is Δko/ΔE = +0.77 ± 0.05 pm/V.

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Suk-Min Ko

Papers

Electrically Driven Quantum Dot/Wire/Well Hybrid Light-Emitting Diodes

Growth Mechanism of Catalyst-Free and Mask-Free Heteroepitaxial GaN Submicrometer- and Micrometer-Sized Rods under Biaxial Strain: Variation of Surface Energy and Adatom Kinetics

Dislocation-Eliminating Chemical Control Method for High-Efficiency GaN-Based Light Emitting Nanostructures

Ultrashort carrier lifetime of vapor–liquid–solid-grown GaN/InGaN multi-quantum-well coaxial nanorods

Electro-optic and converse-piezoelectric properties of epitaxial GaN grown on silicon by metal-organic chemical vapor deposition