4.8 Article

Spin Blockades to Relaxation of Hot Multiexcitons in Nanocrystals

Journal

JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 10, Issue 10, Pages 2341-2348

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.9b00992

Keywords

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Funding

  1. Israel Science Foundation [163/16, 914/15, 1508/14]
  2. Israel Science Foundation (ISF) [189-14]
  3. US Israel Science Foundation (BSF) [2015687]
  4. Lady Davis Fellowship Trust
  5. Raymond and Janine Bollag Post-Doctoral Fellowship Fund
  6. Marie-Sklodowska Curie action H2020-MSCA-ITN [642656]
  7. Marie Curie Actions (MSCA) [642656] Funding Source: Marie Curie Actions (MSCA)

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The conjecture that, as in bulk semiconductors, hot multiexcitons in nanocrystals cool rapidly to the lowest available energy levels is tested here by recording the effects of a single cold spectator exciton on the relaxation dynamics of a subsequently deposited hot counterpart. Results in CdSe/CdS nanodots show that a preexisting cold spectator exciton allows only half of the photoexcited electrons to relax directly to the band-edge. The rest are blocked in an excited quantum state due to conflicts in spin orientation. The latter fully relax in this sample only after similar to 25 ps as the blocked electrons spins flip, prolonging the temporal window of opportunity for harvesting the retained energy more than 100 fold! Common to all quantum-confined nanocrystals, this process will delay cooling and impact the spectroscopic signatures of hot multiexcitons in all envisioned generation scenarios. How the spin-flipping rate scales with particle size and temperature remains to be determined.

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