Hot electron and hole dynamics in thiol-capped CdSe quantum dots revealed by 2D electronic spectroscopy

Nils Lenngren, Mohamed A. Abdellah, Kaibo Zheng, Mohammed J. Al-Marri, Donatas Zigmantas, Karel Žídek, Tõnu Pullerits

Research output: Contribution to journalArticlepeer-review

35 Citations (Scopus)


Colloidal quantum dots (QDs) have attracted interest as materials for opto-electronic applications, wherein their efficient energy use requires the understanding of carrier relaxation. In QDs capped by bifunctional thiols, used to attach the QDs to a surface, the relaxation is complicated by carrier traps. Using 2D spectroscopy at 77 K, we follow excitations in thiol-capped CdSe QDs with state specificity and high time resolution. We unambiguously identify the lowest state as an optically allowed hole trap, and identify an electron trap with excited-state absorption. The presence of traps changes the initial dynamics entirely by offering a different relaxation channel. 2D electronic spectroscopy enables us to pinpoint correlations between states and to easily separate relaxation from different starting states. We observe the direct rapid trapping of 1S3/2, 2S3/2, and 1S1/2 holes, and several competing electron relaxation processes from the 1Pe state.

Original languageEnglish
Pages (from-to)26199-26204
Number of pages6
JournalPhysical Chemistry Chemical Physics
Issue number37
Publication statusPublished - 2016
Externally publishedYes

ASJC Scopus subject areas

  • General Physics and Astronomy
  • Physical and Theoretical Chemistry


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