Quantum dot to quantum dot Förster resonance energy transfer: engineering materials for visual color change sensing

In this work, quantum dots (QDs) of various heterostructured compositions and shell thicknesses are used as Förster or fluorescence resonance energy transfer (FRET) donors and acceptors to optimize QD-QD FRET sensing through materials design. While several reports have highlighted the advantages of using QD-dye, rather than dye-dye, FRET in sensing applications, QD-QD FRET has lagged behind in development as a result of high background signal from direct acceptor excitation. However, in designing sensors for longitudinal studies, QD-dye sensors are limited by the photostability of the fluorescent dye. While fluorescence generally affords higher sensitivity than absorbance-based readouts, the instrumentation needed for detecting fluorescence can be expensive, motivating the development of sensors bright enough to be seen by eye or imaged with cheap consumer electronics. Harnessing the exceptional brightness of QDs, our study focuses on the development of QD-QD FRET pairs where color change is achieved for visual readout and instrument-free sensing. We demonstrate that bulk semiconductor material characteristics can be used to a priori predict and tailor the behavior of QD-QD FRET systems, and our findings show that it is possible to create QD donors that are brighter than their acceptors through concerted compositional and morphological choices in heterostructured QDs. This is significant for developing visual sensors, as we show that the most profound color change occurs when the direct acceptor emission is lower than that of the donor. Finally, the use of an optimal cadmium-free QD-QD FRET pair is presented in a pH sensor that shows a large range of pH-dependent color change with bright, instrument-free readout.