Ultrafast fluorescent decay induced by metal-mediated dipole–dipole interaction in two-dimensional molecular aggregates
Abstract
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:
-
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Department of Mechanical Engineering
- Univ. of California, Berkeley, CA (United States). Nanoscale Science and Engineering Center
- Northeastern Univ., Boston, MA (United States). Department of Electrical and Computer Engineering and Department of Mechanical and Industrial Engineering
- 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:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Light-Material Interactions in Energy Conversion (LMI); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1426735
- Grant/Contract Number:
- AC02-05CH11231
- Resource 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)
- 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
Citation Formats
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., 2017.
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. https://doi.org/10.1073/pnas.1703000114
Hu, Qing, Jin, Dafei, Xiao, Jun, Nam, Sang Hoon, Liu, Xiaoze, Liu, Yongmin, Zhang, Xiang, and Fang, Nicholas X. Tue .
"Ultrafast fluorescent decay induced by metal-mediated dipole–dipole interaction in two-dimensional molecular aggregates". United States. https://doi.org/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 = {Tue Sep 05 00:00:00 EDT 2017},
month = {Tue Sep 05 00:00:00 EDT 2017}
}
Web of Science
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