Frederick V. Mikulec

Biological applications of quantum dots

Quantum dots (QDs) are a novel class of inorganic fluorophore which are gaining widespread recognition as a result of their exceptional photophysical properties. They are rapidly being applied to existing and emerging technologies, and could have an important role in many areas. Significant challenges remain, however, which must be understood and more fully defined before they can be widely validated. This review provides on overview of QD technology, covering QD characteristics, synthesis methods, and the applications in which they have been put to use. The influence of synthesis methods on QD characteristics and their subsequent suitability to different applications is discussed, and a broad outline of the technologies into which they have been incorporated is presented, and the relative merits and weaknesses of their incorporation are evaluated. The potential for further development, and inclusion in other technologies is also discussed, and barriers restricting further progress specified, particularly with regard to the poorly understood surface chemistry of QDs, the potential for alteration of function of biological molecules when complexed with QDs, and on a larger scale the significant potential for cytotoxicity both in vitro and in vivo.

The band edge luminescence of surface modified CdSe nanocrystallites: Probing the luminescing state

We study the luminescence of surface modified CdSe nanocrystallites. There has been much speculation as to the origin of the band edge emission in these quantum confined structures. Because of their large surface to volume ratios it has been suggested that the emission originates from surface-related states. However, recent theory suggests that the band edge luminescence arises from an optically inactive fine structure state or “dark” exciton. To address this issue we modify the surface of CdSe nanocrystallites with a variety of organic and inorganic ligands. We then monitor the effect changing the surface has on the energetics of the band edge luminescence through photoluminescence and fluorescence line narrowing experiments. Our results are compared with theoretical predictions for the nonresonant and resonant luminescence. We find good agreement between experiment and theory for CdSe nanocrystallites passivated with trioctylphosphine oxide, ZnS, 4-picoline, 4-(trifluoromethyl)thiophenol, and tris(2-eth...

The Band Edge Luminescence of Surface Modified CdSe Nanocrystallites

We study the band edge luminescence of CdSe nanocrystallites to determine the origin of this emission. Previous studies have attributed the band edge emission to the recombination of photo-generated carriers trapped in localized surface states. Recently a number of “dark exciton” theories have been proposed which explain the luminescence in terms of recombination through internal core states. To address this issue we modify the surface of CdSe nanocrystallites with a number of organic/inorganic ligands and monitor the effect this has on the energetics of the resonant and non-resonant band edge luminescence. Our results for nanocrystallites passivated with trioctylphosphine oxide (TOPO), ZnS, 4-Picoline, 4-(trifluoromethyl)thiophenol, and tris(2-ethylhexyl)phosphate are in agreement with a dark exciton description of the band edge luminescence.