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Title: Restriction-In-Motion of Surface Ligands Enhances Photoluminescence of Quantum Dots - Experiment and Theory

Journal Article · · Advanced Materials Interfaces
 [1];  [1];  [2];  [1];  [3];  [4];  [1];  [1];  [3];  [1]; ORCiD logo [1]
  1. Univ. of Connecticut, Storrs, CT (United States)
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  3. Univ. of Massachusetts, Amherst, MA (United States)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States)

Here the relationship between emission and ligand restriction of a series of ZnSe/ZnS quantum dots (QDs) encapsulated in nanoparticles is investigated systematically via experiments and quantum theory. The QDs have a ZnSe core and a ZnS shell, capped with hydrophobic ligands (triotylphosphine oxide/hexadecylamine), allowing them to be entrapped in a model biomembrane, bicelle, made of zwitterionic dipalmitoyl and dihexanoyl phosphatidylcholines and charged dipalmitoyl phosphatidylglycerol. Enhanced photoluminescence is observed upon encapsulation, depending on the QD-to-lipid ratio. Transmission electron microscopy and small-angle X-ray scattering confirm that QDs are preferably situated at the rim of bicellar discs. A simplified quantum dissipation heat-bath theory is proposed to correlate the enhancement with slower nonradiative processes caused by the restriction-in-motion (RIM) of the surface ligands. However, Fõrster resonance energy transfer due to QD aggregation counteracts the effect.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
Horizon 2020 research and innovation programme; National Institute of General Medical Sciences (NIGMS); National Institute of Health (NIH); National Science Foundation; USDOE; USDOE Office of Science (SC), Biological and Environmental Research (BER)
Grant/Contract Number:
SC0012704
OSTI ID:
1855101
Report Number(s):
BNL-222848-2022-JAAM
Journal Information:
Advanced Materials Interfaces, Journal Name: Advanced Materials Interfaces Journal Issue: 6 Vol. 9; ISSN 2196-7350
Publisher:
Wiley-VCHCopyright Statement
Country of Publication:
United States
Language:
English

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