Browsing by Subject "Quantum confinement"
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Item Open Access Computational modeling of quantum-confined impact ionization in Si nanocrystals embedded in SiO2(2007) Sevik, C.; Bulutay, C.Injected carriers from the contacts to delocalized bulk states of the oxide matrix via Fowler-Nordheim tunneling can give rise to quantum-confined impact ionization (QCII) of the nanocrystal (NC) valence electrons. This process is responsible for the creation of confined excitons in NCs, which is a key luminescence mechanism. For a realistic modeling of QCII in Si NCs, a number of tools are combined: ensemble Monte Carlo (EMC) charge transport, ab initio modeling for oxide matrix, pseudopotential NC electronic states together with the closed-form analytical expression for the Coulomb matrix element of the QCII. To characterize the transport properties of the embedding amorphous SiO2, ab initio band structure and density of states of the α-quartz phase of SiO2 are employed. The confined states of the Si NC are obtained by solving the atomistic pseudopotential Hamiltonian. With these ingredients, realistic modeling of the QCII process involving a SiO2 bulk state hot carrier and the NC valence electrons is provided.Item Open Access Localized plasmon-coupled semiconductor nanocrystal emitters for innovative device applications(Bilkent University, 2007) Soğancı, İbrahim MuratQuantum confinement allows for the development of novel luminescent materials such as colloidal semiconductor quantum dots for a variety of photonic applications spanning from biomedical labeling to white light generation. However, such device applications require efficient photoluminescence. To this end, in this thesis we investigate the spontaneous emission characteristics of semiconductor nanocrystal emitters under different conditions and their enhancement and controlled modification via plasmonic resonance coupling, placing metallic nanoparticles in their proximity, for innovative device applications. We first present our theoretical and experimental work on the optical characterization of nanocyrstals (e.g., CdSe, CdS, and CdSe/ZnS) including absorption/photoluminescence, time-resolved luminescence, and excitation spectra measurements. Here we demonstrate very strong electromodulation (up to 90%) of photoluminescence and absorption of such nanocrystals (nanodots and nanorods) for optical modulator applications. Second, we present our electromagnetic modeling on the optical response of metal nanoparticles using finite-difference-time-domain method. For the first time, using localized plasmons of metal nanoisland films (nano-silver) carefully spectrally and spatially tuned for optimal coupling conditions, we report very significant controlled modifications of nanocrystal emission including the peak emission wavelength shift (by 14nm), emission linewidth reduction (by 10nm with 22% FWHM reduction), photoluminescence intensity enhancement (15.1- and 21.6-fold compared to the control groups of the same nanocrystals with no plasmonic coupling and those with identical nano-silver but no dielectric spacer in the case of non-radiative energy transfer, respectively), and selectable peaking of surface-state emission at desired wavelengths. Such localized plasmonic engineering of nanocrystal emitters opens new possibilities for our lightemitting and photovoltaic devices.Item Open Access Morphological control of mesoporosity and nanoparticles within Co3O4-CuO electrospun nanofibers: quantum confinement and visible light photocatalysis performance(American Chemical Society, 2017-09) Pradhan, A. C.; Uyar, TamerThe one-dimensional (1D) mesoporous and interconnected nanoparticles (NPs) enriched composite Co3O4-CuO nanofibers (NFs) in the ratio Co:Cu = 1/4 (Co3O4-CuO NFs) composite have been synthesized by electrospinning and calcination of mixed polymeric template. Not merely the mesoporous composite Co3O4-CuO NFs but also single mesoporous Co3O4 NFs and CuO NFs have been produced for comparison. The choice of mixed polymer templates such as polyvinylpyrrolidone (PVP) and polyethylene glycol (PEG) for electrospinning is responsible for the formation of 1D mesoporous NFs. The HR-TEM result showed evolution of interconnected nanoparticles (NPs) and creation of mesoporosity in all electrospun NFs. The quantum confinement is due to NPs within NFs and has been proved by the surface-enhanced Raman scattering (SERS) study and the UV-vis-NRI diffuse reflectance spectra (DRS). The high intense photoluminescence (PL) spectra showing blue shift of all NFs also confirmed the quantum confinement phenomena. The lowering of PL spectrum after mixing of CuO in Co3O4 nanofibers framework (Co3O4-CuO NFs) proved CuO as an efficient visible light response low cost cocatalyst/charge separator. The red shifting of the band gap in composite Co3O4-CuO NFs is due to the internal charge transfer between Co2+ to Co3+ and Cu2+, proved by UV-vis absorption spectroscopy. Creation of oxygen vacancies by mixing of CuO and Co3O4 also prevents the electron-hole recombination and enhances the photocatalytic activity in composite Co3O4-CuO NFs. The photocurrent density, Mott-Schottky (MS), and electrochemical impedance spectroscopy (EIS) studies of all NFs favor the high photocatalytic performance. The mesoporous composite Co3O4-CuO NFs exhibits high photocatalytic activity toward phenolic compounds degradation as compared to the other two NFs (Co3O4 NFs and CuO NFs). The kinetic study of phenolic compounds followed first order rate equation. The high photocatalytic activity of composite Co3O4-CuO NFs is attributed to the formation of mesoporosity and interconnected NPs within NFs framework, quantum confinement, extended light absorption property, internal charge transfer, and effective photogenerated charge separations.Item Open Access Quantum size effect on the phonon-induced Zeeman splitting in a GaAs quantum dot with Gaussian and parabolic confining potentials(Elsevier B.V., 2008) Mukhopadhyaya, S.; Boyacioglu, B.; Saglam, M.; Chatterjee, A.The Zeeman splitting of the ground and the first excited level of a Gaussian GaAs quantum dot is studied in the presence of electron-longitudinal-optical (LO)-phonon interaction incorporating the spin of the electron and is compared with the case of a parabolic dot. It is shown that the Zeeman splitting is suppressed because of the polaronic interaction and becomes strongly size dependent, but the parabolic confinement overestimates this Zeeman suppression. It is also shown that although the energy levels are split because of the spin-field interaction, the cyclotron frequencies and the Zeeman lines are independent of the electron spin in the dipole transition. © 2008 Elsevier B.V. All rights reserved.Item Open Access The role of the interface in germanium quantum dots: when not only size matters for quantum confinement effects(Royal Society of Chemistry, 2015) Cosentino, S.; Mio, A. M.; Barbagiovanni, E. G.; Raciti, R.; Bahariqushchi, R.; Miritello, M.; Nicotra, G.; Aydınlı, Atilla; Spinella, C.; Terrasi, A.; Mirabella, S.Quantum confinement (QC) typically assumes a sharp interface between a nanostructure and its environment, leading to an abrupt change in the potential for confined electrons and holes. When the interface is not ideally sharp and clean, significant deviations from the QC rule appear and other parameters beyond the nanostructure size play a considerable role. In this work we elucidate the role of the interface on QC in Ge quantum dots (QDs) synthesized by rf-magnetron sputtering or plasma enhanced chemical vapor deposition (PECVD). Through a detailed electron energy loss spectroscopy (EELS) analysis we investigated the structural and chemical properties of QD interfaces. PECVD QDs exhibit a sharper interface compared to sputter ones, which also evidences a larger contribution of mixed Ge-oxide states. Such a difference strongly modifies the QC strength, as experimentally verified by light absorption spectroscopy. A large size-tuning of the optical bandgap and an increase in the oscillator strength occur when the interface is sharp. A spatially dependent effective mass (SPDEM) model is employed to account for the interface difference between Ge QDs, pointing out a larger reduction in the exciton effective mass in the sharper interface case. These results add new insights into the role of interfaces on confined systems, and open the route for reliable exploitation of QC effects. © The Royal Society of Chemistry.Item Open Access Ultrahigh green and red optical gain cross sections from solutions of colloidal quantum well heterostructures(American Chemical Society, 2021-03-11) Delikanli, Savaş; Erdem, Onur; Işık, Furkan; Dehghanpour Baruj, Hamed; Shabani, Farzan; Yağcı, Hüseyin Bilge; Durmuşoğlu, E. G.; Demir, Hilmi VolkanWe demonstrate amplified spontaneous emission (ASE) in solution with ultralow thresholds of 30 μJ/cm2 in red and of 44 μJ/cm2 in green from engineered colloidal quantum well (CQW) heterostructures. For this purpose, CdSe/CdS core/crown CQWs, designed to hit the green region, and CdSe/CdS@CdxZn1–xS core/crown@gradient-alloyed shell CQWs, further tuned to reach the red region by shell alloying, were employed to achieve high-performance ASE in the visible range. The net modal gain of these CQWs reaches 530 cm–1 for the green and 201 cm–1 for the red, 2–3 orders of magnitude larger than those of colloidal quantum dots (QDs) in solution. To explain the root cause for ultrahigh gain coefficient in solution, we show for the first time that the gain cross sections of these CQWs is ≥3.3 × 10–14 cm2 in the green and ≥1.3 × 10–14 cm2 in the red, which are two orders of magnitude larger compared to those of CQDs.