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Title: Influence of Nanostructure on the Exciton Dynamics of Multichromophore Donor–Acceptor Block Copolymers

Here, we explore the synthesis and photophysics of nanostructured block copolymers that mimic light-harvesting complexes. We find that the combination of a polar and electron-rich boron dipyrromethene (BODIPY) block with a nonpolar electron-poor perylene diimide (PDI) block yields a polymer that self-assembles into ordered “nanoworms”. Numerical simulations are used to determine optimal compositions to achieve robust self-assembly. Photoluminescence spectroscopy is used to probe the rich exciton dynamics in these systems. Using controls, such as homopolymers and random copolymers, we analyze the mechanisms of the photoluminescence from these polymers. With this understanding it allows us to probe in detail the photophysics of the block copolymers, including the effects of their self-assembly into nanostructures on their excited-state properties. Similar to natural systems, ordered nanostructures result in properties that are starkly different than the properties of free polymers in solution, such as enhanced rates of electronic energy transfer and elimination of excitonic emission from disordered PDI trap states.
Authors:
 [1] ;  [2] ; ORCiD logo [1] ;  [1] ;  [1] ; ORCiD logo [3] ; ORCiD logo [1]
  1. Columbia Univ., New York, NY (United States). Dept. of Chemistry
  2. Columbia Univ., New York, NY (United States). Dept. of Chemistry; Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
Publication Date:
Report Number(s):
BNL-114328-2017-JA
Journal ID: ISSN 1936-0851; KC0403020
Grant/Contract Number:
SC0012704; SC0001085; DMR-1408259
Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 11; Journal Issue: 5; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Research Org:
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); Energy Frontier Research Centers (EFRC) (United States). Re-Defining Photovoltaic Efficiency Through Molecule Scale Control (RPEMSC)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; excitonics; nanotechnology; organic electronics; photophysics; polymer chemistry; self-assembly
OSTI Identifier:
1394757

Xia, Jianlong, Busby, Erik, Sanders, Samuel N., Tung, Clarion, Cacciuto, Angelo, Sfeir, Matthew Y., and Campos, Luis M.. Influence of Nanostructure on the Exciton Dynamics of Multichromophore Donor–Acceptor Block Copolymers. United States: N. p., Web. doi:10.1021/acsnano.7b00056.
Xia, Jianlong, Busby, Erik, Sanders, Samuel N., Tung, Clarion, Cacciuto, Angelo, Sfeir, Matthew Y., & Campos, Luis M.. Influence of Nanostructure on the Exciton Dynamics of Multichromophore Donor–Acceptor Block Copolymers. United States. doi:10.1021/acsnano.7b00056.
Xia, Jianlong, Busby, Erik, Sanders, Samuel N., Tung, Clarion, Cacciuto, Angelo, Sfeir, Matthew Y., and Campos, Luis M.. 2017. "Influence of Nanostructure on the Exciton Dynamics of Multichromophore Donor–Acceptor Block Copolymers". United States. doi:10.1021/acsnano.7b00056. https://www.osti.gov/servlets/purl/1394757.
@article{osti_1394757,
title = {Influence of Nanostructure on the Exciton Dynamics of Multichromophore Donor–Acceptor Block Copolymers},
author = {Xia, Jianlong and Busby, Erik and Sanders, Samuel N. and Tung, Clarion and Cacciuto, Angelo and Sfeir, Matthew Y. and Campos, Luis M.},
abstractNote = {Here, we explore the synthesis and photophysics of nanostructured block copolymers that mimic light-harvesting complexes. We find that the combination of a polar and electron-rich boron dipyrromethene (BODIPY) block with a nonpolar electron-poor perylene diimide (PDI) block yields a polymer that self-assembles into ordered “nanoworms”. Numerical simulations are used to determine optimal compositions to achieve robust self-assembly. Photoluminescence spectroscopy is used to probe the rich exciton dynamics in these systems. Using controls, such as homopolymers and random copolymers, we analyze the mechanisms of the photoluminescence from these polymers. With this understanding it allows us to probe in detail the photophysics of the block copolymers, including the effects of their self-assembly into nanostructures on their excited-state properties. Similar to natural systems, ordered nanostructures result in properties that are starkly different than the properties of free polymers in solution, such as enhanced rates of electronic energy transfer and elimination of excitonic emission from disordered PDI trap states.},
doi = {10.1021/acsnano.7b00056},
journal = {ACS Nano},
number = 5,
volume = 11,
place = {United States},
year = {2017},
month = {3}
}