Journal
ACS NANO
Volume 6, Issue 7, Pages 6515-6524Publisher
AMER CHEMICAL SOC
DOI: 10.1021/nn302371q
Keywords
excitation relaxation; electron-phonon couplings; phonon-bottleneck; surface effects; nanocrystals
Categories
Funding
- Center for Advanced Solar Photophysics, an Energy Frontier Research Center
- U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES)
- NDSU Advance FORWARD
- NSF [HRD-0811239, CHE-1050405]
- ND EPSCoR through NSF [EPS-0814442]
- DOE [DE-FG36-08GO88160, DEFG02-05ER15755]
- Center for Nonlinear Studies (LANL)
- U.S. DOE [DE-AC52-06NA25396]
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1050405] Funding Source: National Science Foundation
- EPSCoR
- Office Of The Director [0814442] Funding Source: National Science Foundation
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Understanding the pathways of hot exciton relaxation in photoexcited semiconductor nanocrystals, also called quantum dots (QDs), is of paramount importance in multiple energy, electronics and biological applications. An important nonradiative relaxation channel originates from the nonadiabatic (NA) coupling of electronic degrees of freedom to nuclear vibrations, which in QDs depend on the confinement effects and complicated surface chemistry. To elucidate the role of surface ligands in relaxation processes of nanocrystals, we study the dynamics of the NA exciton relaxation in Cd33Se33 semiconductor quantum dots passivated by either trimethylphosphine oxide or methylamine ligands using explicit time-dependent modeling. The large extent of hybridization between electronic states of quantum dot and ligand molecules is found to strongly facilitate exciton relaxation. Our computational results for the ligand contributions to the exciton relaxation and electronic energy-loss in small clusters are further extrapolated to larger quantum dots.
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