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Title: Ultrafast fluorescent decay induced by metal-mediated dipole–dipole interaction in two-dimensional molecular aggregates

Two-dimensional molecular aggregate (2DMA), a thin sheet of strongly interacting dipole molecules self-assembled at close distance on an ordered lattice, is a fascinating fluorescent material. It is distinctively different from the conventional (single or colloidal) dye molecules and quantum dots. Here, in this paper, we verify that when a 2DMA is placed at a nanometric distance from a metallic substrate, the strong and coherent interaction between the dipoles inside the 2DMA dominates its fluorescent decay at a picosecond timescale. Our streak-camera lifetime measurement and interacting lattice–dipole calculation reveal that the metal-mediated dipole–dipole interaction shortens the fluorescent lifetime to about one-half and increases the energy dissipation rate by 10 times that expected from the noninteracting single-dipole picture. In conclusion, our finding can enrich our understanding of nanoscale energy transfer in molecular excitonic systems and may designate a unique direction for developing fast and efficient optoelectronic devices.
Authors:
 [1] ;  [1] ;  [2] ;  [1] ;  [2] ;  [3] ; ORCiD logo [4] ;  [1]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Department of Mechanical Engineering
  2. Univ. of California, Berkeley, CA (United States). Nanoscale Science and Engineering Center
  3. Northeastern Univ., Boston, MA (United States). Department of Electrical and Computer Engineering and Department of Mechanical and Industrial Engineering
  4. Univ. of California, Berkeley, CA (United States). Nanoscale Science and Engineering Center ; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Material Sciences Division; King Abdulaziz University, Jeddah (Saudi Arabia)
Publication Date:
Grant/Contract Number:
AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 114; Journal Issue: 38; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Energy Frontier Research Centers (EFRC) (United States). Light-Material Interactions in Energy Conversion (LMI)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; molecular aggregate; fluorescence; nonradiative decay; dipole–dipole interaction; surface plasmon
OSTI Identifier:
1426735

Hu, Qing, Jin, Dafei, Xiao, Jun, Nam, Sang Hoon, Liu, Xiaoze, Liu, Yongmin, Zhang, Xiang, and Fang, Nicholas X. Ultrafast fluorescent decay induced by metal-mediated dipole–dipole interaction in two-dimensional molecular aggregates. United States: N. p., Web. doi:10.1073/pnas.1703000114.
Hu, Qing, Jin, Dafei, Xiao, Jun, Nam, Sang Hoon, Liu, Xiaoze, Liu, Yongmin, Zhang, Xiang, & Fang, Nicholas X. Ultrafast fluorescent decay induced by metal-mediated dipole–dipole interaction in two-dimensional molecular aggregates. United States. doi:10.1073/pnas.1703000114.
Hu, Qing, Jin, Dafei, Xiao, Jun, Nam, Sang Hoon, Liu, Xiaoze, Liu, Yongmin, Zhang, Xiang, and Fang, Nicholas X. 2017. "Ultrafast fluorescent decay induced by metal-mediated dipole–dipole interaction in two-dimensional molecular aggregates". United States. doi:10.1073/pnas.1703000114. https://www.osti.gov/servlets/purl/1426735.
@article{osti_1426735,
title = {Ultrafast fluorescent decay induced by metal-mediated dipole–dipole interaction in two-dimensional molecular aggregates},
author = {Hu, Qing and Jin, Dafei and Xiao, Jun and Nam, Sang Hoon and Liu, Xiaoze and Liu, Yongmin and Zhang, Xiang and Fang, Nicholas X.},
abstractNote = {Two-dimensional molecular aggregate (2DMA), a thin sheet of strongly interacting dipole molecules self-assembled at close distance on an ordered lattice, is a fascinating fluorescent material. It is distinctively different from the conventional (single or colloidal) dye molecules and quantum dots. Here, in this paper, we verify that when a 2DMA is placed at a nanometric distance from a metallic substrate, the strong and coherent interaction between the dipoles inside the 2DMA dominates its fluorescent decay at a picosecond timescale. Our streak-camera lifetime measurement and interacting lattice–dipole calculation reveal that the metal-mediated dipole–dipole interaction shortens the fluorescent lifetime to about one-half and increases the energy dissipation rate by 10 times that expected from the noninteracting single-dipole picture. In conclusion, our finding can enrich our understanding of nanoscale energy transfer in molecular excitonic systems and may designate a unique direction for developing fast and efficient optoelectronic devices.},
doi = {10.1073/pnas.1703000114},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 38,
volume = 114,
place = {United States},
year = {2017},
month = {9}
}