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Title: Control of Energy Flow Dynamics between Tetracene Ligands and PbS Quantum Dots by Size Tuning and Ligand Coverage

Abstract

We have prepared a series of samples with the ligand 6,13-bistri(iso-propyl)silylethynyl tetracene 2-carboxylic acid (TIPS-Tc-COOH) attached to PbS quantum dot (QD) samples of three different sizes in order to monitor and control the extent and time scales of energy flow after photoexcitation. Fast energy transfer (~1 ps) to the PbS QD occurs upon direct excitation of the ligand for all samples. The largest size QD maintains the microsecond exciton lifetime characteristic of the as-prepared oleate terminated PbS QDs. However, two smaller QD sizes with lowest exciton energies similar to or larger than the TIPS-Tc-COO- triplet energy undergo energy transfer between QD core and ligand triplet on nanosecond to microsecond timescales. For the intermediate size QDs in particular, energy can be recycled many times between ligand and core, but the triplet remains the dominant excited species at long times, living for ~3 us for fully exchanged QDs and up to 30 us for partial ligand exchange, which is revealed as a method for controlling the triplet lifetime. A unique upconverted luminescence spectrum is observed that results from annihilation of triplets after exclusive excitation of the QD core.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [1];  [2]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. Univ. of Kentucky, Lexington, KY (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1422873
Report Number(s):
NREL/JA-5900-70058
Journal ID: ISSN 1530-6984; TRN: US1801664
Grant/Contract Number:
AC36-08GO28308
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 18; Journal Issue: 2; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; energy transfer; photoluminescence; quantum dots; triplet; upconversion

Citation Formats

Kroupa, Daniel M., Arias, Dylan H., Blackburn, Jeffrey L., Carroll, Gerard M., Granger, Devin B., Anthony, John E., Beard, Matthew C., and Johnson, Justin C. Control of Energy Flow Dynamics between Tetracene Ligands and PbS Quantum Dots by Size Tuning and Ligand Coverage. United States: N. p., 2018. Web. doi:10.1021/acs.nanolett.7b04144.
Kroupa, Daniel M., Arias, Dylan H., Blackburn, Jeffrey L., Carroll, Gerard M., Granger, Devin B., Anthony, John E., Beard, Matthew C., & Johnson, Justin C. Control of Energy Flow Dynamics between Tetracene Ligands and PbS Quantum Dots by Size Tuning and Ligand Coverage. United States. doi:10.1021/acs.nanolett.7b04144.
Kroupa, Daniel M., Arias, Dylan H., Blackburn, Jeffrey L., Carroll, Gerard M., Granger, Devin B., Anthony, John E., Beard, Matthew C., and Johnson, Justin C. Wed . "Control of Energy Flow Dynamics between Tetracene Ligands and PbS Quantum Dots by Size Tuning and Ligand Coverage". United States. doi:10.1021/acs.nanolett.7b04144.
@article{osti_1422873,
title = {Control of Energy Flow Dynamics between Tetracene Ligands and PbS Quantum Dots by Size Tuning and Ligand Coverage},
author = {Kroupa, Daniel M. and Arias, Dylan H. and Blackburn, Jeffrey L. and Carroll, Gerard M. and Granger, Devin B. and Anthony, John E. and Beard, Matthew C. and Johnson, Justin C.},
abstractNote = {We have prepared a series of samples with the ligand 6,13-bistri(iso-propyl)silylethynyl tetracene 2-carboxylic acid (TIPS-Tc-COOH) attached to PbS quantum dot (QD) samples of three different sizes in order to monitor and control the extent and time scales of energy flow after photoexcitation. Fast energy transfer (~1 ps) to the PbS QD occurs upon direct excitation of the ligand for all samples. The largest size QD maintains the microsecond exciton lifetime characteristic of the as-prepared oleate terminated PbS QDs. However, two smaller QD sizes with lowest exciton energies similar to or larger than the TIPS-Tc-COO- triplet energy undergo energy transfer between QD core and ligand triplet on nanosecond to microsecond timescales. For the intermediate size QDs in particular, energy can be recycled many times between ligand and core, but the triplet remains the dominant excited species at long times, living for ~3 us for fully exchanged QDs and up to 30 us for partial ligand exchange, which is revealed as a method for controlling the triplet lifetime. A unique upconverted luminescence spectrum is observed that results from annihilation of triplets after exclusive excitation of the QD core.},
doi = {10.1021/acs.nanolett.7b04144},
journal = {Nano Letters},
number = 2,
volume = 18,
place = {United States},
year = {Wed Jan 24 00:00:00 EST 2018},
month = {Wed Jan 24 00:00:00 EST 2018}
}

Journal Article:
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