15 resultados para QUANTUM CHEMISTRY AND THERMOCHEMISTRY

em Cambridge University Engineering Department Publications Database


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The optical efficiency of GaN-based multiple quantum well (MQW) and light emitting diode (LED) structures grown on Si(111) substrates by metal-organic vapor phase epitaxy was measured and compared with equivalent structures on sapphire. The crystalline quality of the LED structures was comprehensively characterized using x-ray diffraction, atomic force microscopy, and plan-view transmission electron microscopy. A room temperature photoluminescence (PL) internal quantum efficiency (IQE) as high as 58% has been achieved in an InGaN/GaN MQW on Si, emitting at 460 nm. This is the highest reported PL-IQE of a c-plane GaN-based MQW on Si, and the radiative efficiency of this sample compares well with similar structures grown on sapphire. Processed LED devices on Si also show good electroluminescence (EL) performance, including a forward bias voltage of ∼3.5 V at 20 mA and a light output power of 1 mW at 45 mA from a 500 ×500 μm2 planar device without the use of any additional techniques to enhance the output coupling. The extraction efficiency of the LED devices was calculated, and the EL-IQE was then estimated to have a maximum value of 33% at a current density of 4 A cm-2, dropping to 30% at a current density of 40 A cm-2 for a planar LED device on Si emitting at 455 nm. The EL-IQE was clearly observed to increase as the structural quality of the material increased for devices on both sapphire and Si substrates. © 2011 American Institute of Physics.

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We solve the problem of steering a three-level quantum system from one eigen-state to another in minimum time and study its possible extension to the time-optimal control problem for a general n-level quantum system. For the three-level system we find all optimal controls by finding two types of symmetry in the problem: ℤ2 × S3 discrete symmetry and S1 continuous symmetry, and exploiting them to solve the problem through discrete reduction and symplectic reduction. We then study the geometry, in the same framework, which occurs in the time-optimal control of a general n-level quantum system. © 2007 IEEE.

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We solve the problem of steering a three-level quantum system from one eigen-state to another in minimum time and study its possible extension to the time-optimal control problem for a general n-level quantum system. For the three-level system we find all optimal controls by finding two types of symmetry in the problems: ℤ × S3 discrete symmetry and 51 continuous symmetry, and exploiting them to solve the problem through discrete reduction and symplectic reduction. We then study the geometry, in the same framework, which occurs in the time-optimal control of a general n-level quantum system. Copyright ©2007 Watam Press.

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InGaAs quantum dots (QDs) and nanowires have been grown on GaAs by metal-organic chemical vapour deposition on GaAs (100) and (111)B substrates, respectively. InGaAs QD lasers were fabricated and characterised. Results show ground-state lasing at about 1150 nm in devices with lengths greater than 2.5 mm. We also observed a strong influence of nanowire density on nanowire height specific to nanowires with high indium composition. This dependency was attributed to the large difference of diffusion length on (111)B surfaces between In and Ga reaction species, with In being the more mobile species. Selective area epitaxy for applications in quantum-dot optoelectronic device integration is also discussed in this paper. ©2006 IEEE.

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We review our results on integrated photonic devices fabricated using InGaAs quantum-dots. Selective-area metal organic chemical vapor deposition (MOCVD) is used to grow the active region with quantum dots emitting at different wavelengths for fabrication of the integrated devices. We will also review the structural and optical properties of III-V nanowires, and axial and radial nanowire heterostructures grown by MOCVD. In addition to binary nanowires, such as GaAs, InAs, and InP, we have demonstrated ternary InGaAs and AlGaAs nanowires. Core-shell nanowires consisting of GaAs cores with AlGaAs shells, and core-multishell nanowires with several alternating shells of AlGaAs and GaAs, exhibit strong photoluminescence. Axial segments of InGaAs have been incorporated within GaAs nanowires to form GaAs/InGaAs nanowire superlattices.

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Standard forms of density-functional theory (DFT) have good predictive power for many materials, but are not yet fully satisfactory for cluster, solid, and liquid forms of water. Recent work has stressed the importance of DFT errors in describing dispersion, but we note that errors in other parts of the energy may also contribute. We obtain information about the nature of DFT errors by using a many-body separation of the total energy into its 1-body, 2-body, and beyond-2-body components to analyze the deficiencies of the popular PBE and BLYP approximations for the energetics of water clusters and ice structures. The errors of these approximations are computed by using accurate benchmark energies from the coupled-cluster technique of molecular quantum chemistry and from quantum Monte Carlo calculations. The systems studied are isomers of the water hexamer cluster, the crystal structures Ih, II, XV, and VIII of ice, and two clusters extracted from ice VIII. For the binding energies of these systems, we use the machine-learning technique of Gaussian Approximation Potentials to correct successively for 1-body and 2-body errors of the DFT approximations. We find that even after correction for these errors, substantial beyond-2-body errors remain. The characteristics of the 2-body and beyond-2-body errors of PBE are completely different from those of BLYP, but the errors of both approximations disfavor the close approach of non-hydrogen-bonded monomers. We note the possible relevance of our findings to the understanding of liquid water.

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We show how machine learning techniques based on Bayesian inference can be used to reach new levels of realism in the computer simulation of molecular materials, focusing here on water. We train our machine-learning algorithm using accurate, correlated quantum chemistry, and predict energies and forces in molecular aggregates ranging from clusters to solid and liquid phases. The widely used electronic-structure methods based on density-functional theory (DFT) give poor accuracy for molecular materials like water, and we show how our techniques can be used to generate systematically improvable corrections to DFT. The resulting corrected DFT scheme gives remarkably accurate predictions for the relative energies of small water clusters and of different ice structures, and greatly improves the description of the structure and dynamics of liquid water.

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We report the first measurement of two-photon absorption (TPA) and self-phase modulation in an InGaAsP/InP multi-quantum-well waveguide. The TPA coefficient, β2, was found to be 60±10 cm/GW at 1.55 μm. Despite operating at 200 nm from the band edge, self-phase modulation as high as 8±2 rad was observed for 30-ps optical pulses at 3.8-W peak input power. A theoretical calculation indicates that this enhanced phase modulation is primarily due to bandfilling in the quantum wells and the free-carrier plasma effect.