Tuning the excitonic and plasmonic properties of copper chalcogenide nanocrystals

Ilka Kriegel, Chengyang Jiang, Jessica Rodríguez-Fernández, Richard D Schaller, Dmitri V. Talapin, Enrico Da Como, Jochen Feldmann

Research output: Contribution to journalArticle

272 Citations (Scopus)

Abstract

The optical properties of stoichiometric copper chalcogenide nanocrystals (NCs) are characterized by strong interband transitions in the blue part of the spectral range and a weaker absorption onset up to ∼1000 nm, with negligible absorption in the near-infrared (NIR). Oxygen exposure leads to a gradual transformation of stoichiometric copper chalcogenide NCs (namely, Cu 2-xS and Cu 2-xSe, x = 0) into their nonstoichiometric counterparts (Cu 2-xS and Cu 2-xSe, x > 0), entailing the appearance and evolution of an intense localized surface plasmon (LSP) band in the NIR. We also show that well-defined copper telluride NCs (Cu 2-xTe, x > 0) display a NIR LSP, in analogy to nonstoichiometric copper sulfide and selenide NCs. The LSP band in copper chalcogenide NCs can be tuned by actively controlling their degree of copper deficiency via oxidation and reduction experiments. We show that this controlled LSP tuning affects the excitonic transitions in the NCs, resulting in photoluminescence (PL) quenching upon oxidation and PL recovery upon subsequent reduction. Time-resolved PL spectroscopy reveals a decrease in exciton lifetime correlated to the PL quenching upon LSP evolution. Finally, we report on the dynamics of LSPs in nonstoichiometric copper chalcogenide NCs. Through pump-probe experiments, we determined the time constants for carrier-phonon scattering involved in LSP cooling. Our results demonstrate that copper chalcogenide NCs offer the unique property of holding excitons and highly tunable LSPs on demand, and hence they are envisaged as a unique platform for the evaluation of exciton/LSP interactions.

Original languageEnglish
Pages (from-to)1583-1590
Number of pages8
JournalJournal of the American Chemical Society
Volume134
Issue number3
DOIs
Publication statusPublished - Jan 25 2012

Fingerprint

Nanoparticles
Nanocrystals
Copper
Tuning
Excitons
Photoluminescence
Infrared radiation
Quenching
Phonons
Oxidation
Phonon scattering
Photoluminescence spectroscopy
Sulfides
Oxidation-Reduction
Spectrum Analysis
Optical properties
Experiments
Pumps
Oxygen
Cooling

ASJC Scopus subject areas

  • Chemistry(all)
  • Catalysis
  • Biochemistry
  • Colloid and Surface Chemistry

Cite this

Kriegel, I., Jiang, C., Rodríguez-Fernández, J., Schaller, R. D., Talapin, D. V., Da Como, E., & Feldmann, J. (2012). Tuning the excitonic and plasmonic properties of copper chalcogenide nanocrystals. Journal of the American Chemical Society, 134(3), 1583-1590. https://doi.org/10.1021/ja207798q

Tuning the excitonic and plasmonic properties of copper chalcogenide nanocrystals. / Kriegel, Ilka; Jiang, Chengyang; Rodríguez-Fernández, Jessica; Schaller, Richard D; Talapin, Dmitri V.; Da Como, Enrico; Feldmann, Jochen.

In: Journal of the American Chemical Society, Vol. 134, No. 3, 25.01.2012, p. 1583-1590.

Research output: Contribution to journalArticle

Kriegel, I, Jiang, C, Rodríguez-Fernández, J, Schaller, RD, Talapin, DV, Da Como, E & Feldmann, J 2012, 'Tuning the excitonic and plasmonic properties of copper chalcogenide nanocrystals', Journal of the American Chemical Society, vol. 134, no. 3, pp. 1583-1590. https://doi.org/10.1021/ja207798q
Kriegel, Ilka ; Jiang, Chengyang ; Rodríguez-Fernández, Jessica ; Schaller, Richard D ; Talapin, Dmitri V. ; Da Como, Enrico ; Feldmann, Jochen. / Tuning the excitonic and plasmonic properties of copper chalcogenide nanocrystals. In: Journal of the American Chemical Society. 2012 ; Vol. 134, No. 3. pp. 1583-1590.
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