5 years ago

Electronic and Optical Properties of Methylated Adamantanes

Electronic and Optical Properties of Methylated Adamantanes
Robert Richter, Torbjörn Rander, Andre Knecht, Thomas Möller, David Wolter, Andrea Merli, Tobias Bischoff
Recent theoretical work has identified functionalized diamondoids as promising candidates for the tailoring of fluorescent nanomaterials. However, experiments confirming that optical gap tuning can be achieved through functionalization have, up until now, found only systems where fluorescence is quenched. We address this shortcoming by investigating a series of methylated adamantanes. For the first time, a class of functionalized diamondoids is shown to fluoresce in the gas phase. In order to understand the evolution of the optical and electronic structure properties with degree of functionalization, photoelectron spectroscopy was used to map the occupied valence electronic structure, while absorption and fluorescence spectroscopies yielded information about the unoccupied electronic structure and postexcitation relaxation behavior. The resulting spectra were modeled by (time-dependent) density functional theory. These results show that it is possible to overcome fluorescence quenching when functionalizing diamondoids and represent a significant step toward tailoring the electronic structure of these and other semiconductor particles in a manner suitable to applications.

Publisher URL: http://dx.doi.org/10.1021/jacs.7b05150

DOI: 10.1021/jacs.7b05150

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