Spin Blockades to Relaxation of Hot Multiexcitons in Nanocrystals.

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ID: 72208
2019
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Abstract
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 ∼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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ghosh2019spinthe Use this key to autocite in the manuscript while using SciMatic Manuscript Manager or Thesis Manager
Authors Ghosh, Tufan;Dehnel, Joanna;Fabian, Marcel;Lifshitz, Efrat;Baer, Roi;Ruhman, Sanford;
Journal The journal of physical chemistry letters
Year 2019
DOI
10.1021/acs.jpclett.9b00992
URL
Keywords
cognition depression mental health audience spectator

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