Charge-tunable quantum plasmons in colloidal semiconductor nanocrystals

ACS Nano
Alina M SchimpfDaniel R Gamelin

Abstract

Nanomaterials exhibiting plasmonic optical responses are impacting sensing, information processing, catalysis, solar, and photonics technologies. Recent advances have expanded the portfolio of plasmonic nanostructures into doped semiconductor nanocrystals, which allow dynamic manipulation of carrier densities. Once interpreted as intraband single-electron transitions, the infrared absorption of doped semiconductor nanocrystals is now commonly attributed to localized surface plasmon resonances and analyzed using the classical Drude model to determine carrier densities. Here, we show that the experimental plasmon resonance energies of photodoped ZnO nanocrystals with controlled sizes and carrier densities diverge from classical Drude model predictions at small sizes, revealing quantum plasmons in these nanocrystals. A Lorentz oscillator model more adequately describes the data and illustrates a closer link between plasmon resonances and single-electron transitions in semiconductors than in metals, highlighting a fundamental contrast between these two classes of plasmonic materials.

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Citations

Jan 6, 2016·Journal of the American Chemical Society·Carolyn N ValdezJames M Mayer
Aug 20, 2014·ACS Nano·Enrico Della GasperaJacek J Jasieniak
Nov 5, 2015·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·J Scott Niezgoda, Sandra J Rosenthal
Dec 10, 2014·Journal of the American Chemical Society·Alina M SchimpfDaniel R Gamelin
Aug 12, 2015·The Journal of Physical Chemistry Letters·Alina M SchimpfDaniel R Gamelin
Nov 5, 2014·The Journal of Chemical Physics·Andrew H CaldwellRichard D Robinson
Aug 12, 2015·The Journal of Physical Chemistry Letters·R Carmina MonrealS Peter Apell
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Jun 30, 2015·Accounts of Chemical Research·Alina M SchimpfDaniel R Gamelin

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