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    Surface effects of vapour-liquid-solid driven Bi surface droplets formed during molecular-beam-epitaxy of GaAsBi
    ([London] : Macmillan Publishers Limited, part of Springer Nature, 2016) Steele, J.A.; Lewis, R.A.; Horvat, J.; Nancarrow, M.J.B.; Henini, M.; Fan, D.; Mazur, Y.I.; Schmidbauer, M.; Ware, M.E.; Yu, S.-Q.; Salamo, G.J.
    Herein we investigate a (001)-oriented GaAs1−xBix/GaAs structure possessing Bi surface droplets capable of catalysing the formation of nanostructures during Bi-rich growth, through the vapour-liquid-solid mechanism. Specifically, self-aligned “nanotracks” are found to exist trailing the Bi droplets on the sample surface. Through cross-sectional high-resolution transmission electron microscopy the nanotracks are revealed to in fact be elevated above surface by the formation of a subsurface planar nanowire, a structure initiated mid-way through the molecular-beam-epitaxy growth and embedded into the epilayer, via epitaxial overgrowth. Electron microscopy studies also yield the morphological, structural and chemical properties of the nanostructures. Through a combination of Bi determination methods the compositional profile of the film is shown to be graded and inhomogeneous. Furthermore, the coherent and pure zincblende phase property of the film is detailed. Optical characterisation of features on the sample surface is carried out using polarised micro-Raman and micro-photoluminescence spectroscopies. The important light producing properties of the surface nanostructures are investigated through pump intensity-dependent micro-PL measurements, whereby relatively large local inhomogeneities are revealed to exist on the epitaxial surface for important optical parameters. We conclude that such surface effects must be considered when designing and fabricating optical devices based on GaAsBi alloys.
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    Dynamics of Broadband Lasing Cascade from a Single Dot-in-well InGaAs Microdisk
    ([London] : Macmillan Publishers Limited, part of Springer Nature, 2019) Talalaev, Vadim; Kryzhanovskaya, Natalia; Tomm, Jens W.; Rutckaia, Viktoriia; Schilling, Joerg; Zhukov, Alexey
    The development of a fast semiconductor laser is required for the realization of next-generation telecommunication applications. Since lasers operating on quantum dot ground state transitions exhibit only limited gain due to the saturation effect, we investigate lasing from excited states and compare its corresponding static and dynamic behavior to the one from the ground state. InAs quantum dots (QDs) grown in dot-in-well (DWELL) structures allowed to obtain light emission from ground and three excited states in a spectral range of 1.0–1.3 μm. This emission was coupled to whispering gallery modes (WGMs) of a 6 μm microdisk resonator and studied at room temperature by steady-state and time-resolved micro-photoluminescence. We demonstrate a cascade development of lasing arising from the ladder of quantum dot states, and compare the lasing behavior of ground and excited state emission. While the lasing threshold is being increased from the ground state to the highest excited state, the dynamic behavior is improved: turn-on times and lifetimes of WGMs become shorter paving the way towards high frequency direct driven microlasers. © 2019, The Author(s).
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    Interdot Lead Halide Excess Management in PbS Quantum Dot Solar Cells
    (Weinheim : Wiley-VCH, 2022) Albaladejo‐Siguan, Miguel; Becker‐Koch, David; Baird, Elizabeth C.; Hofstetter, Yvonne J.; Carwithen, Ben P.; Kirch, Anton; Reineke, Sebastian; Bakulin, Artem A.; Paulus, Fabian; Vaynzof, Yana
    Light-harvesting devices made from lead sulfide quantum dot (QD) absorbers are one of the many promising technologies of third-generation photovoltaics. Their simple, solution-based fabrication, together with a highly tunable and broad light absorption makes their application in newly developed solar cells, particularly promising. In order to yield devices with reduced voltage and current losses, PbS QDs need to have strategically passivated surfaces, most commonly achieved through lead iodide and bromide passivation. The interdot spacing is then predominantly filled with residual amorphous lead halide species that remain from the ligand exchange, thus hindering efficient charge transport and reducing device stability. Herein, it is demonstrated that a post-treatment by iodide-based 2-phenylethlyammonium salts and intermediate 2D perovskite formation can be used to manage the lead halide excess in the PbS QD active layer. This treatment results in improved device performance and increased shelf-life stability, demonstrating the importance of interdot spacing management in PbS QD photovoltaics.
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    Bis(stearoyl) Sulfide: A Stable, Odor-Free Sulfur Precursor for High-Efficiency Metal Sulfide Quantum Dot Photovoltaics
    (Weinheim : Wiley-VCH, 2023) Albaladejo‐Siguan, Miguel; Prudnikau, Anatol; Senina, Alina; Baird, Elizabeth C.; Hofstetter, Yvonne J.; Brunner, Julius; Shi, Juanzi; Vaynzof, Yana; Paulus, Fabian
    The synthesis of metal sulfide nanocrystals is a crucial step in the fabrication of quantum dot (QD) photovoltaics. Control over the QD size during synthesis allows for precise tuning of their optical and electronic properties, making them an appealing choice for electronic applications. This flexibility has led to the implementation of QDs in both highly-efficient single junction solar cells and other optoelectronic devices including photodetectors and transistors. Most commonly, metal sulfide QDs are synthesized using the hot-injection method utilizing a toxic, and air- and moisture-sensitive sulfur source: bis(trimethylsilyl) sulfide ((TMS)2S). Here, bis(stearoyl) sulfide (St2S) is presented as a new type of air-stable sulfur precursor for the synthesis of sulfide-based QDs, which yields uniform, pure, and stable nanocrystals. Photovoltaic devices based on these QDs are equally efficient as those fabricated by (TMS)2S but exhibit enhanced operational stability. These results highlight that St2S can be widely adopted for the synthesis of metal sulfide QDs for a range of optoelectronic applications.