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

Ultrafast fluorescent decay induced by metal-mediated dipole–dipole interaction in two-dimensional molecular aggregates
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二维分子聚集体中金属介导的偶极-偶极相互作用诱导的超快荧光衰减

DOI:
10.1073/pnas.1703000114
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发表时间:
2017
期刊:
Proceedings of the National Academy of Sciences
影响因子:
--
通讯作者:
Fang, Nicholas X.
Fang, Nicholas X.
中科院分区:
--
文献类型:
--
作者:
Hu, Qing;Jin, Dafei;Xiao, Jun;Nam, Sang Hoon;Liu, Xiaoze;Liu, Yongmin;Zhang, Xiang;Fang, Nicholas X.

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二维分子聚集体(2DMA)是一种在有序晶格上近距离自组装的强相互作用的偶极子分子薄片,是一种令人着迷的荧光材料。它与传统的(单一或胶体)染料分子和量子点明显不同。在本文中,我们验证了当2DMA与金属衬底放置在纳米距离时,2DMA内部偶极子之间的强相干相互作用主导了其在皮秒时间尺度上的荧光衰减。我们的条纹相机寿命测量和相互作用的晶格偶极子计算表明,金属介导的偶极子-偶极子相互作用将荧光寿命缩短到大约一半,并将能量耗散率提高到非相互作用的单偶极子图像的10倍。这一发现丰富了我们对分子激子系统中纳米尺度能量传递的认识,并为开发快速高效的光电器件指明了一个独特的方向。
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. 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. 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.
吸附在溴化银 (I) 和二氧化硅上的 J-聚集体具有短且与激发无关的荧光寿命
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