Monolayer-thick light-sensitive nanocrystal skins of oriented colloidal quantum wells

Abstract

Colloidal quantum wells (CQWs), a two-dimensional member of semiconductor nanocrystals, featuring very tight vertical quantum confinement, possess giant oscillator strengths. Also, CQWs exhibit remarkably large absorption cross-sections, thanks to their oscillator strengths combined with their laterally large geometries. Additionally, as a powerful tool of fabrication, CQWs lend themselves to be conveniently self-assembled into monolayer-thick films in a single orientation of our choice: either face-down (lying down on their large lateral surfaces and side by side leaving no large gap between them similar to a mosaic pattern) or edge-up (standing up on their thin edges and facing each other in a very dense superstructure formation of repeating chains). In this thesis, to make use of the attractive absorption properties of CQWs and leverage on our ability to construct their orientation-controlled self-assemblies, we show the first account of monolayer-thick light-sensitive nanocrystal skins (LS-NS) that employ self-oriented CQWs as their active absorptive layer. These CQW LS-NS devices operate on the principle of strong optical absorption of the monolayered assembly of CQWs and the subsequent photogenerated potential build-up across their strongly capacitive thin device for sensing in the visible to ultraviolet. Such oriented CQWs in the LS-NS device architecture yield profoundly reduced surface roughness in their monolayer-thick films, essential to high device performance. Here, specifically, we developed and demonstrated two groups of LS-NS devices: one group consisting of all face-down oriented CQWs and the other, of all edge-up ones. We systematically studied their photocharging effect, spectral sensitivity and decay times. We observed in all LS-NS devices that the spectral sensitivity complies with the first (heavy-hole) and second (light hole) excitonic peaks of the absorption of the CQWs. We also found that, as the excitation power is increased, the peak photovoltage readout increases while the sensitivity decreases. The photocharging effect was further observed as the excitation was turned off. Finally, using the edge-up orientation, we identified a profound peak photovoltage signal enhancement. These findings of the thesis indicate that the proposed LS-NS devices of the orientation-controlled CQW monolayers hold great promise for applications in photos-sensing facades over larger surfaces.