Journal
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Volume 18, Issue 37, Pages 26199-26204Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c6cp04190f
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Funding
- Swedish Research Council (VR)
- Knut and Alice Wallenberg Foundation
- Swedish Energy Agency
- NPRP grant from the Qatar National Research Fund [NPRP7-227-1-034]
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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 1S(3/2), 2S(3/2), and 1S(1/2) holes, and several competing electron relaxation processes from the 1P(e) state.
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