Efficient Upper-Excited State Fluorescence in an Organic Hyperbolic Metamaterial

Yufei Shen, Yixin Yan, Alyssa N. Brigeman, Hoyeon Kim, Noel C. Giebink

Research output: Contribution to journalArticlepeer-review

11 Scopus citations


Upper-excited state emission is not usually observed from molecules owing to competition with much faster nonradiative relaxation pathways; however, it can be made more efficient by modifying the photonic density of states to enhance the radiative decay rate. Here, we show that embedding the small molecule zinc tetraphenylporphyrin (ZnTPP) in a hyperbolic metamaterial enables an ∼18-fold increase in fluorescence intensity from the second singlet excited state (S2) relative to that from the lowest singlet excited state (S1). By varying the number of periods in the HMM stack, we are able to systematically tune the ZnTPP fluorescence spectrum from red (dominated by emission from S1) to blue (dominated by emission from S2) with an instrument-limited decay lifetime <10 ps. Our results are consistent with a broadband Purcell enhancement in the radiative rate of both transitions predicted via transfer matrix modeling and point to a general opportunity to harness upper-excited states for spectrally tunable, ultrafast fluorescence via radiative decay engineering.

Original languageEnglish (US)
Pages (from-to)1693-1698
Number of pages6
JournalNano letters
Issue number3
StatePublished - Mar 14 2018

All Science Journal Classification (ASJC) codes

  • Bioengineering
  • General Chemistry
  • General Materials Science
  • Condensed Matter Physics
  • Mechanical Engineering


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