Nonlinear optical approach to multiexciton relaxation dynamics in quantum dots

Vanessa M. Huxter, Gregory D. Scholes

Research output: Contribution to journalArticlepeer-review

25 Scopus citations


Unlike the majority of molecular systems quantum dots can accommodate multiple excitations, which is a particularly important attribute for potential lasing applications. We demonstrate in this work the concept of using nth order nonlinear spectroscopies in the transient grating configuration as a means of selectively exciting (n-1) 2 excitons in a semiconductor and probing the subsequent relaxation dynamics. We report a direct observation of multiparticle dynamics on ultrashort time scales through comparison of third and fifth order experiments for CdSe colloidal quantum dots. Time constants associated with multiexciton recombination and depopulation dynamics are reported. Deviation from a Poisson model for the distribution of photoexcited excitons, biexcitons, and triexcitons is also discussed.

Original languageEnglish (US)
Article number144716
JournalJournal of Chemical Physics
Issue number14
StatePublished - 2006
Externally publishedYes

All Science Journal Classification (ASJC) codes

  • General Physics and Astronomy
  • Physical and Theoretical Chemistry


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