Purely excitonic lasing in ZnO microcrystals: Temperature-induced transition between exciton-exciton and exciton-electron scattering

Since the seminal observation of room-temperature laser emission from ZnO thin films and nanowires, numerous attempts have been carried out for detailed understanding of the lasing mechanism in ZnO. In spite of the extensive efforts performed over the last decades, the origin of optical gain at room temperature is still a matter of considerable discussion. In this work, we show that a ZnO film consisting of well-packed micrometer-sized ZnO crystals exhibits purely excitonic lasing at room temperature without showing any symptoms of electron-hole plasma emission, even under optical excitation more than 25 times above the excitonic lasing threshold. The lasing mechanism is shifted from the exciton-exciton scattering to the exciton-electron scattering with increasing temperature from 3 to 150 K. The exciton-electron scattering process continues to exist with further increasing temperature from 150 to 300 K. Thus, we present distinct experimental evidence that the room-temperature excitonic lasing is achieved not by exciton-exciton scattering, as has been generally believed, but by exciton-electron scattering. We also argue that the long carrier diffusion length and the low optical loss nature of the micrometer-sized ZnO crystals, as compared to those of ZnO nanostructures, plays a key role in showing room-temperature excitonic lasing.