In this thesis, novel multi-section laser diodes based on quantum-dot material are designed and investigated which exhibit a number of advantages such as low threshold current density; temperature-insensitivity and suppress carrier diffusion due to discrete nature of density of state of quantum-dots. The spectral versatility in the range of 1.1 µm – 1.3 µm wavelengths is demonstrated through novel mode-locking regimes such as dual-wavelength mode-locking, wavelength bistability and broad tunability. Moreover, broad pulse repetition rate tuning using an external cavity configuration is presented. A high peak power of 17.7 W was generated from the quantum-dot laser as a result of the tapered geometry of the gain section of the laser has led to successful application of such device for two-photon imaging. Dual-wavelength mode-locking is demonstrated via ground (?=1180 nm) and excited (?=1263 nm) spectral bands with optical pulses from both states simultaneously in the 5-layer quantum-dot two-section diode laser. The widest spectral separation of 83 nm between the modes was achieved in a dual-wavelength mode-locked non-vibronic laser. Power and wavelength bistability are achieved in a mode-locked multi-section laser which active region incorporates non-identical QD layers grown by molecular beam epitaxy. As a result the wavelength can be electronically controlled between 1245 nm and 1290 nm by applying different voltages to the saturable absorber. Mode-locked or continuous-wave regimes are observed for both wavelengths over a 260 mA – 330 mA current ranges with average power up to 28 mW and 31 mW, respectively. In mode-locked regime, a repetition rate of 10 GHz of optical pulses as short as 4 ps is observed. Noticeable hysteresis of average power for different bias conditions is also demonstrated. The wavelength and power bistability in QD lasers are potentially suitable for flip-flop memory application. In addition, a unique mode-locked regime at expense of the reverse bias with 50 nm wavelength tuning range from 1245 nm to 1290 nm is also presented. Broad repetition rate tunability is shown from quantum-dot external cavity mode-locked 1.27 µm laser. The repetition rate from record low of 191 MHz to 1 GHz from fundamental mode-locking was achieved. Harmonic mode-locking allows further to increase tuning up to 6.8 GHz (34th-order harmonic) from 200 MHz fundamental mode-locking. High peak power of 1.5 W can be generated directly from two-section 4 mm long laser with bent waveguide at angle of 7° at 1.14 GHz repetition rate without the use of any pulse compression and optical amplifier. Stable mode-locking with an average power up to 60 mW, corresponding to 25 pJ pulse energy is also obtained at a repetition frequency of 2.4 GHz. The minimum time-bandwidth product of 1.01 is obtained with the pulse duration of 8.4 ps. Novel tapered quantum-dot lasers with a gain-guided geometry operating in a passively mode-locked regime have been investigated, using structures that incorporated either 5 or 10 quantum dot layers. The peak power of 3.6 W is achieved with pulse duration of 3.2 ps. Furthermore, the record peak power of 17.7 W and transform limited pulses of 672 fs were achieved with optimized structure. The generation of picosecond pulses with high average power of up to 209 mW was demonstrated, corresponding to 14.2 pJ pulse energy. The improved optical parameters of the tapered laser enable to achieve nonlinear images of fluorescent beads. Thus it is for the first time that QD based compact monolithic device enables to image biological samples using two-photon microscopy imaging technique.

Implementation of optical refrigeration (OR) in quantum dot (QD) materials was achieved for the first time. An OR experiment was designed and carried out in our lab and a maximum temperature drop around 0.68 K was observed in the zinc-blende crystalline CdSe/CdS (core/shell structure) QD samples under laser excitation. The cooling effect was achieved by utilizing the energy up-conversion photoluminescence (PL) of CdSe/CdS QDs with sub-band excitation. While the cooling efficiency of the system was estimated and optimized by a semi-empirical model built during this research. <div><br></div><div>This work has proved the capability of QD materials to be used as a cooling substance for OR, which significantly expanded the possible candidates for OR. The technique could have many applications, such as harvesting cooling effect from sun light with the help of metamaterials, which can produce quasi-monochromatic light. It may also be used to cool QD in optical traps, which leading may help to develop new ultra-sensitive sensors and application for quantum information science.</div>

Studies various nanostructured materials have gained considerable interest within the past several decades. This novel class of materials has opened up a new realm of possibilities, both for the fundamental comprehension of matter, but also for innovative applications. The size-dependent effect observed for these systems often lies in their interaction with the surrounding environment and understanding such interactions is the pivotal point for the investigations undertaken in this thesis. Three families of nanoparticles are analyzed: semiconductor quantum dots, metallic silver nanoparticles and rare-earth oxide nanomaterials. The radical scavenging ability of cerium oxide nanoparticles (CeO2) is quite controversial since they have been labeled as both oxidizing and antioxidant species for biological systems. Here, both aqueous and organic stabilized nanoparticles are examined in straightforward systems containing only one reactive oxygen species to ensure a controlled release. The apparent absence of their direct radical scavenging ability is demonstrated despite the ease at which CeO2 nanoparticles generate stable surface Ce3+ clusters, which is used to explain the redox activity of these nanomaterials. On the contrary, CeO2 nanoparticles are shown to have an indirect scavenging effect in Fenton reactions by annihilating the reactivity of Fe2+ salts. Cadmium selenide quantum dots (CdSe QD) constitute another highly appealing family of nanocolloids in part due to their tunable, size-dependent luminescence across the visible spectrum. The effect of elemental sulfur treatment is investigated to overcome one of the main drawbacks of CdSe QD: low fluorescence quantum yield. Herein, we report a constant and reproducible quantum yield of 15%. The effect of sulfur surface treatment is also assessed following the growth of a silica shell, as well as the response towards a solution quencher (4-amino-TEMPO). The sulfur treated QD is also tested for interaction with pyronin Y, a xanthene dye that offers potential energy and electron transfer applications with the QD. Interaction with the dye molecule is compared to results obtained with untreated quantum dots, as well as CdSe/ZnS core shell examples. In another chapter of this thesis, the catalytic potential of silver nanoparticles is addressed for the grafting of polyhydrosiloxane polymer chains with various alkoxy groups. A simple one-pot synthesis is presented with silver salts and the polymer. the latter serves as a mild reducing agent and a stabilizing ligand, once silver nanoparticles are formed in-situ. We evaluate the conversion of silane into silyl ethers groups with the addition of several alcohols, whether primary, secondary or tertiary, and report the yields of grafting under the mildest conditions: room temperature, under air and atmospheric pressure.

This thesis focuses on pioneering a scalable route to fabricate quantum information devices based upon single InAs/InP quantum dots emitting in the telecommunications wavelength band around 1550 nm. Using metallic gates in combination with nanotemplate, site-selective epitaxy techniques, arrays of single quantum dots are produced and electrostatically tuned with a high degree of control over the electrical and optical properties of each individual quantum dot. Using metallic gates to apply local electric fields, the number of electrons within each quantum dot can be tuned and the nature of the optical recombination process controlled. Four electrostatic gates mounted along the sides of a square-based, pyramidal nanotemplate in combination with a flat metallic gate on the back of the InP substrate allow the application of electric fields in any direction across a single quantum dot. Using lateral fields provided by the metallic gates on the sidewalls of the pyramid and a vertical electric field able to control the charge state of the quantum dot, the exchange splitting of the exciton, trion and biexciton are measured as a function of gate voltage. A quadrupole electric field configuration is predicted to symmetrize the product of electron and hole wavefunctions within the dot, producing two degenerate exciton states from the two possible optical decay pathways of the biexciton. Building upon these capabilities, the anisotropic exchange splitting between the exciton states within the biexciton cascade is shown to be reversibly tuned through zero for the first time. We show direct control over the electron and hole wavefunction symmetry, thus enabling the entanglement of emitted photon pairs in asymmetric quantum dots. Optical spectroscopy of single InAs/InP quantum dots atop pyramidal nanotemplates in magnetic fields up to 28T is used to examine the dispersion of the s, p and d shell states. The g-factor and diamagnetic shift of the exciton and charged exciton states from over thirty single quantum dots are calculated from the spectra. The g-factor shows a generally linear dependence on dot emission energy, in agreement with previous work on this subject. A positive linear correlation between diamagnetic coefficient and g-factor is observed.

This paper details the design and simulation of a fault-tolerant Quantum-dot Cellular Automata (QCA) NOT gate. A version of the standard NOT gate can be constructed to take advantage to the ability to easily integrate redundant structures into a QCA design. The fault-tolerant characteristics of this inverter are analyzed with QCADesigner v2.0.3 (Windows version) simulation software. These characteristics are then compared with the characteristics of two other non-redundant styles of NOT gates. The redundant version of the gate is more robust than the standard style for the inverter. However, another simple inverter style seems to be even more than this fault-tolerant design. Both versions of the gate will need to be studied further in the future to determine which design is most practical. / Thesis (M.S.)--Wichita State University, College of Engineering, Dept. of Electrical and Computer Engineering / "July 2006." / Includes bibliographic references (leaves 31-33)

Studies various nanostructured materials have gained considerable interest within the past several decades. This novel class of materials has opened up a new realm of possibilities, both for the fundamental comprehension of matter, but also for innovative applications. The size-dependent effect observed for these systems often lies in their interaction with the surrounding environment and understanding such interactions is the pivotal point for the investigations undertaken in this thesis. Three families of nanoparticles are analyzed: semiconductor quantum dots, metallic silver nanoparticles and rare-earth oxide nanomaterials. The radical scavenging ability of cerium oxide nanoparticles (CeO2) is quite controversial since they have been labeled as both oxidizing and antioxidant species for biological systems. Here, both aqueous and organic stabilized nanoparticles are examined in straightforward systems containing only one reactive oxygen species to ensure a controlled release. The apparent absence of their direct radical scavenging ability is demonstrated despite the ease at which CeO2 nanoparticles generate stable surface Ce3+ clusters, which is used to explain the redox activity of these nanomaterials. On the contrary, CeO2 nanoparticles are shown to have an indirect scavenging effect in Fenton reactions by annihilating the reactivity of Fe2+ salts. Cadmium selenide quantum dots (CdSe QD) constitute another highly appealing family of nanocolloids in part due to their tunable, size-dependent luminescence across the visible spectrum. The effect of elemental sulfur treatment is investigated to overcome one of the main drawbacks of CdSe QD: low fluorescence quantum yield. Herein, we report a constant and reproducible quantum yield of 15%. The effect of sulfur surface treatment is also assessed following the growth of a silica shell, as well as the response towards a solution quencher (4-amino-TEMPO). The sulfur treated QD is also tested for interaction with pyronin Y, a xanthene dye that offers potential energy and electron transfer applications with the QD. Interaction with the dye molecule is compared to results obtained with untreated quantum dots, as well as CdSe/ZnS core shell examples. In another chapter of this thesis, the catalytic potential of silver nanoparticles is addressed for the grafting of polyhydrosiloxane polymer chains with various alkoxy groups. A simple one-pot synthesis is presented with silver salts and the polymer. the latter serves as a mild reducing agent and a stabilizing ligand, once silver nanoparticles are formed in-situ. We evaluate the conversion of silane into silyl ethers groups with the addition of several alcohols, whether primary, secondary or tertiary, and report the yields of grafting under the mildest conditions: room temperature, under air and atmospheric pressure.

Currently, a major challenge for solid-state spin qubit systems is achieving one-qubit operations on a timescale shorter than the spin coherence time, T2*, a goal currently two orders of magnitude away. By taking advantage of the quasi-one-dimensional structure of a nanowire and the strong spin-orbit interaction of InAs, it is estimated that π-rotations can be implemented using electric dipole spin resonance on the order of 10 ns. To this end, a procedure for the fabrication of homogeneous InAs nanowire quantum dot devices is presented herein for future investigations of solid state spin qubits as a test bed for quantum computing. Both single and double quantum dot systems are formed using local gating of InAs nanowires. Single quantum dot systems were characterized through electron transport measurements in a dilution refrigerator; in one case, the charging energy was measured to be 5.0 meV and the orbital energy was measured to be 1.5-3.5 meV. The total capacitance of the single quantum dot system was determined to be approximately 30 aF. An estimate of the quantum dot geometry resulting from confinement suggests that the quantum dot is approximately 115 nm long. The coupling energy of the double quantum dot system was measured to be approximately 4.5 meV. The electron temperature achieved with our circuitry in the dilution refrigerator is estimated to be approximately 125 mK.

<p>This dissertation develops a novel application of the resonant-infrared matrix-assisted pulsed laser evaporation (RIR-MAPLE) technique toward the end goal of conjugated-polymer-based optoelectronic device fabrication. Conjugated polymers are attractive materials that are being investigated in the development of efficient optoelectronic devices due to their inexpensive material costs. Moreover, they can easily be combined with inorganic nanomaterials, such as colloidal quantum dots (CQDs), so as to realize hybrid nanocomposite-based optoelectronic devices with tunable optoelectronic characteristics and enhanced desirable features. One of the most significant challenges to the realization of optimal conjugated polymer-CQD hybrid nanocomposite-based optoelectronics has been the processes by which these materials are deposited as thin films, that is, conjugated polymer thin film processing techniques lack sufficient control so as to maintain preferred optoelectronic device behavior. More specifically, conjugated-polymer-based optoelectronics device operation and efficiency are a function of several attributes, including surface film morphology, internal polymer chain morphology, and the distribution and type of nanomaterials in the film bulk. Typical conjugated-polymer thin-film fabrication methodologies involve solution-based deposition, and the presence of the solvent has a deleterious impact, resulting in films with poor charge transport properties and subsequently poor device efficiencies. In addition, many next-generation conjugated polymer-based optoelectronics will require multi-layer device architectures, which can be difficult to achieve using traditional solution processing techniques. These issues direct the need for the development of a new polymer thin film processing technique that is less susceptible to solvent-related polymer chain morphology problems and is more capable of achieving better controlled nanocomposite thin films and multi-layer heterostructures comprising a wide range of materials. Therefore, this dissertation describes the development of a new variety of RIR-MAPLE that uses a unique target emulsion technique to address the aforementioned challenges.</p><p>The emulsion-based RIR-MAPLE technique was first developed for the controlled deposition of the conjugated polymers poly[2-methoxy-5-(2'-ethyl-hexyloxy)-1,4-phenylene vinylene] (MEH-PPV) and poly[2-methoxy-5-(2'ethylhexyloxy)-1,4-(1-cyanovinylene) phenylene] (MEH-CN-PPV) into homogenous thin films. Therein, it was identified that target composition had the most significant influence on film surface morphology, and by tuning the concentration of hydroxyl bonds in the target bulk, the laser-target absorption depth could be tuned so as to yield more or less evaporative deposition, resulting in films with tunable surface morphologies and optical behaviors.</p><p>Next, the internal morphologies of emulsion-based RIR-MAPLE-deposited MEH-PPV thin films were investigated by measuring their hole drift mobilities using the time-of-flight (TOF) photoconductivity method in the context of amorphous materials disorder models (Bässler's Gaussian Disorder model and the Correlated Disorder model) in order to provide a quantitative measure of polymer chain packing. The polymer chain packing of the RIR-MAPLE-deposited films was demonstrated to be superior and more conducive to charge transport in comparison to spin-cast and drop-cast MEH-PPV films, yielding enhanced hole mobilities.</p><p>The emulsion-based RIR-MAPLE technique was also developed for the deposition of different classes of inorganic nanoparticles, namely un-encapsulated nanoparticles and ligand-encapsulated nanoparticles. These different classes of nanoparticles were identified to have different film growth regimes, such that either rough or smooth films were obtained, respectively. The ligand-encapsulated nanoparticles were then co-deposited with MEH-PPV as conjugated polymer-CQD hybrid nanocomposites, wherein the distributions of the constituent materials in the film bulk were identified to be tunable, from homogeneous to highly clustered. The RIR-MAPLE deposition regime determined the said distributions, that is, if the polymer and CQDs were sequentially deposited from a sectioned target or simultaneously deposited from a single target, respectively. The homogeneous conjugated polymer-CQD nanocomposites were also investigated in terms of their charge transport properties using the TOF photoconductivity technique, where it was identified that despite the enhanced dispersion of CQDs in the film bulk, the presence of a high concentration of CQDs degraded hole drift mobility, which indicates that special considerations must be taken when incorporating CQDs into conjugated-polymer-based nanocomposite optoelectronics.</p><p>Finally, the unique capability of RIR-MAPLE to enable novel conjugated polymer-based optical heterostructures and optoelectronic devices was evaluated by the successful demonstration of a conjugated polymer-based distributed Bragg reflector (DBR), a plasmonic absorption enhancement layer, and a conjugated polymer-based photovoltaic solar cell featuring a novel electron-transporting layer. These optical heterostructures and optoelectronic devices demonstrate that all of the constituent polymer and nanocomposite layers have controllable thicknesses and abrupt interfaces, thereby confirming the capability of RIR-MAPLE to achieve multi-layer, conjugated polymer-based heterostructures and device architectures that are appropriate for enhancing specific desired optical behaviors and optoelectronic device efficiencies.</p> / Dissertation

The purpose of this thesis is to fabricate 12-layer In0.75Ga0.25As quantum dot-in-a-well (In0.1Ga0.9As) structures grown by molecular-beam epitaxy (MBE) on GaAs substrate, and analyze the optical properties of laser devices for optical fiber communication systems. For the laser structures, larger Al content AlGaAs cladding layer enhance the optical confinement, but encounter much challenges to improve the quality. After we simulate and fabricate different Al content laser structures, we find the best cladding layer composition - Al0.2Ga0.8As which performs a best material gain. In the active layer, 12 layers In0.75Ga0.25As quantum dots (QDs) and QDs in a well (DWell) structure, and DWell with Be-doping in the well structure are included in this study. The well structure slows down the hot carriers speed and Be-doping decrease the carrier life time and increases the electron-hole pair recombination rate. We increase the QDs deposition coverage to move the emission wavelength to 1.3£gm, but the high temperature cladding layer growth process indirectly anneal the QDs and result in the emission wavelength blue shift to 1.24£gm. In the laser fabrication, to transport the light wave in smaller dispersion loss single mode waveguide, wet etching photolithography processes are adapted in this study to fabricate 2£gm width ridge waveguide. The as-cleaved facets are used as Fabry-Perot laser mirrors in ridge waveguide lasers. Finally, the current density of QD Laser(C528) lasing in CW mode is 581A/cm2, slope efficiency of 510mW/A and maximum power/facet of 65mW are obtained.Then the current density of DWELL+PD Laser(C540) lasing in CW mode is 880A/cm2, slope efficiency of 430mW/A and maximum power/facet of 34mW are obtained.

Nanocrystal has non-negligible ratio of the surface atoms. The photophysics of the nanocrystal is strongly influenced by the surface states.There are two surface-related phenomena: the on-off blinking and the red-emission. On-off blinking is a phenomenon commonly observed in thesingle emitters, such as dye molecules and semiconductor quantum dots (QD).In the QD, the charged state caused by the charge transferring from the core to the surface states explains the off-state. Another surface-related phenomenon is the red-emission, which is the emission from the low-lying surface trapped states. This thesis investigates the correlation between the on-off blinking and the red-emissions of the semiconductor nanocrystals. CdSe/ZnS core/shell colloidal nanocrystals with 2.1nm in diameter and emission peak at 515nm were examined. PL spectrum in the solution indicates that besides the band-edge emission, there is a broadband emission spanning the wavelength range of 590 ¡V 800 nm, which is called the red-emission. The lifetime of the band-edge emission is about 20ns, and that of the red-emission is about 200ns. Since they are with different fluorescence lifetime, the band-edge emission and the red-emission are from distinct emission species. Emission intensity from individual QDs of the band-edge emission and the red-emission are recorded by an imaging CCD. Most QDs exhibit band-edge emission. Only few QDs show the red-emission. Both emissions exhibit clear on-off blinking, indicating the two phenomena are with different mechanism.Moreover, the band-edge emission and the red-emission are mutual exclusive.None QDs exhibit both emissions. This indicates the tiny structure difference from one QD particle to another QD particle resulting in a dramatic different of the excitation energy relaxation pathway.