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

Hu, Qing; Jin, Dafei; Xiao, Jun; Nam, Sang Hoon; Liu, Xiaoze; Liu, Yongmin; Zhang, Xiang; Fang, Nicholas X.

doi:10.1073/pnas.1703000114

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

Journal Article · Tue Sep 05 04:00:00 EDT 2017 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.1703000114· OSTI ID:1426735

Hu, Qing ^[1]; Jin, Dafei ^[1]; Xiao, Jun ^[2]; Nam, Sang Hoon ^[1]; Liu, Xiaoze ^[2]; Liu, Yongmin ^[3]; ^[4]; Fang, Nicholas X. ^[1]

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)

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.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Light-Material Interactions in Energy Conversion (LMI); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1426735

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 38 Vol. 114; ISSN 0027-8424

Publisher:: National Academy of Sciences, Washington, DC (United States)Copyright Statement

Country of Publication:: United States

Language:: English

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