Electron-hole quantum physics in ZnO

Abstract

This dissertation describes several new aspects of the quantum physics of electrons and holes in zinc oxide (ZnO), including a few possible applications. Zinc oxide is a II-VI semiconductor with a direct band gap in the ultraviolet. Experimental and theoretical studies have been performed, both on bulk ZnO and on ZnO nanowires. Chapter 2 presents a new technique for an ultrafast all-optical shutter, based on two-photon absorption in a ZnO crystal. This shutter can be used for luminescence experiments requiring extremely high time-resolution. Chapter 3 describes a time-resolved study on the electron-hole many-body effects in highly excited ZnO at room temperature, in particular band-filling, band-gap renormalization, and the disappearance of the exciton resonance due to screening. In Chapter 4, the quantum many-body theory developed and experimentally verified in Chapter 3, is used to explain laser action in ZnO nanowires, and compared with experimental results. In contrast to current opinion, the results indicate that excitons are not involved in the laser action. The measured emission wavelength, the laser threshold, and the spectral distance between the laser modes are shown to be excellently explained by our quantum many-body theory. Multiple scattering of light in a forest of nanowires can be employed to enhance light absorption in solar cells. Optimization of this technique requires better understanding of light diffusion in such a nanowire forest. In Chapter 5 we demonstrate a method, based on two-photon absorption, to directly measure the residence time of light in a nanowire forest, and we show that scanning electron microscope (SEM) images can be used to predict the photon mean free path. In Chapter 6 we present a new ultrafast all-optical transistor, consisting of a forest of ZnO nanowires. After excitation, laser action in this forest causes rapid recombination of the majority of the electrons and holes, limiting the amplification to 1.2 picoseconds only . This ultrafast ultraviolet transistor may have applications in all-optical computing and in pump-probe experiments. Finally, Chapter 7 presents our discovery of preformed electron-hole Cooper pairs. A ZnO crystal has been highly excited via three-photon absorption at cryogenic temperatures. A new peak appears in the measured emission spectra when the crystal is cooled below a certain temperature, and also when it is excited above a certain density. Comparison with light amplification spectra, calculated from quantum many-body theory, demonstrates that this new peak is due to amplified spontaneous emission (ASE) from preformed electron-hole Cooper pairs.