Giant defect emission enhancement from ZnO nanowires through desulfurization process.

Zinc oxide (ZnO) is a stable, direct bandgap semiconductor emitting in the UV with a multitude of technical applications. It is well known that ZnO emission can be shifted into the green for visible light applications through the introduction of defects. However, generating consistent and efficient green emission through this process is challenging, particularly given that the chemical or atomic origin of the green emission in ZnO is still under debate. In this work we present a new method, for which we coin term desulfurization, for creating green emitting ZnO with significantly enhanced quantum efficiency. Solution grown ZnO nanowires are partially converted to ZnS, then desulfurized back to ZnO, resulting in a highly controlled concentration of oxygen defects as determined by X-ray photoelectron spectroscopy and electron paramagnetic resonance. Using this controlled placement of oxygen vacancies we observe a greater than 40-fold enhancement of integrated emission intensity and explore the nature of this enhancement through low temperature photoluminescence experiments

Dynamics of coherence, localization and excitation transfer in disordered nanorings

Self-assembled supramolecular aggregates are excellent candidates for the design of efficient excitation transport devices. Both artificially prepared and natural photosynthetic aggregates in plants and bacteria present an important degree of disorder that is supposed to hinder excitation transport. Besides, molecular excitations couple to nuclear motion affecting excitation transport in a variety of ways. We present an exhaustive study of exciton dynamics in disordered nanorings with long-range interactions under the influence of a phonon bath and take the LH2 system of purple bacteria as a model. Nuclear motion is explicitly taken into account by employing the Davydov ansatz description of the polaron and quantum dynamics are obtained using a time-dependent variational method. We reveal an optimal exciton-phonon coupling that suppresses disorder-induced localization and facilitate excitation de-trapping. This excitation transfer enhancement, mediated by environmental phonons, is attributed to energy relaxation toward extended, low-energy excitons provided by the precise LH2 geometry with anti-parallel dipoles and long-range interactions. An analysis of localization and spectral statistics is followed by dynamical measures of coherence and localization, transfer efficiency and superradiance. Linear absorption, 2D photon-echo spectra and diffusion measures of the exciton are examined to monitor the diffusive behavior as a function of the strengths of disorder and exciton-phonon coupling.Comment: 18 pages, 13 figure

Ultrafast polariton-phonon dynamics of strongly coupled quantum dot-nanocavity systems

We investigate the influence of exciton-phonon coupling on the dynamics of a strongly coupled quantum dot-photonic crystal cavity system and explore the effects of this interaction on different schemes for non-classical light generation. By performing time-resolved measurements, we map out the detuning-dependent polariton lifetime and extract the spectrum of the polariton-to-phonon coupling with unprecedented precision. Photon-blockade experiments for different pulse-length and detuning conditions (supported by quantum optical simulations) reveal that achieving high-fidelity photon blockade requires an intricate understanding of the phonons' influence on the system dynamics. Finally, we achieve direct coherent control of the polariton states of a strongly coupled system and demonstrate that their efficient coupling to phonons can be exploited for novel concepts in high-fidelity single photon generation

NONRADIATIVE-TRANSITIONS IN SEMICONDUCTORS

Non-radiative transitions affect many aspects of semiconductor performance. Normally they reduce device efficiency by suppressing luminescence, creating defects, reducing carrier lifetimes, or enhancing diffusion during operation. The present review surveys both the theoretical and practical understanding of non-radiative transitions. It includes general theoretical results and the associated ideas, with the emphasis on phonon-induced and defect Auger processes. Most of the purely formal aspects are omitted, but the points of principle where uncertainties remain are discussed. The review also covers the relation between basic theoretical studies and practical applied work on device degradation. This includes a description of the atomic processes involved in the more important mechanism of device deterioration and the theoretical understanding of the mechanism of these underlying processes. Finally, there is a survey of models proposed for 'killer' centres