Plasmon-Enhanced Exciton Delocalization in Squaraine-Type Molecular Aggregates

Quenzel, Thomas1,2; Timmer, Daniel1,2; Gittinger, Moritz1,2; Zablocki, Jennifer3; Zheng, Fulu4; Schiek, Manuela1,2,5; Lutzen, Arne3; Frauenheim, Thomas4,6,7; Tretiak, Sergei8; Silies, Martin1,2,9; Zhong, Jin-Hui1,2,10; De Sio, Antonietta1,2; Lienau, Christoph1,2,5

2022-03-22

10.1021/acsnano.1c11398

ACS Nano   影响因子和分区

1936-0851

1936-086X

Enlarging exciton coherence lengths in molecular aggregates is critical for enhancing the collective optical and transport properties of molecular thin film nanostructures or devices. We demonstrate that the exciton coherence length of squaraine aggregates can be increased from 10 to 24 molecular units at room temperature when preparing the aggregated thin film on a metallic rather than a dielectric substrate. Two-dimensional electronic spectroscopy measurements reveal a much lower degree of inhomogeneous line broadening for aggregates on a gold film, pointing to a reduced disorder. The result is corroborated by simulations based on a Frenkel exciton model including exciton-plasmon coupling effects. The simulation shows that localized, energetically nearly resonant excitons on spatially well separated segments can be radiatively coupled via delocalized surface plasmon polariton modes at a planar molecule-gold interface. Such plasmon-enhanced delocalization of the exciton wave function is of high importance for improving the coherent transport properties of molecular aggregates on the nanoscale. Additionally, it may help tailor the collective optical response of organic materials for quantum optical applications.

molecular aggregates excitons wave function delocalization two-dimensional electronic spectroscopy squaraine surface plasmon polariton

SCI ; EI

英语

NI论文

通讯

Deutsche Forschungsgemeinschaft within the Priority Program Tailored Disorder["SPP1839","SFB1372","INST 184/163-1","INST 184/164-1","Li 580/16-1","DE 3578/3-1"] ; Deutsche Forschungsgemeinschaft within Graduate School "Molecular Basis of Sensory Biology"[RTG 1885] ; Deutsche Forschungsgemeinschaft within Graduate School "Template-designed organic electronics (TIDE)"[GRK 2591] ; BMBF[FKZ: 13N13637]

Chemistry ; Science & Technology - Other Topics ; Materials Science

Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary

WOS:000780214300109

AMER CHEMICAL SOC

Web of Science

1.Carl von Ossietzky Univ Oldenburg, Inst Phys, D-26129 Oldenburg, Germany
2.Carl von Ossietzky Univ Oldenburg, Ctr Interface Sci, D-26129 Oldenburg, Germany
3.Univ Bonn, Kekule Inst Organ Chem & Biochem, D-53121 Bonn, Germany
4.Univ Bremen, Bremen Ctr Computat Mat Sci, D-28359 Bremen, Germany
5.Carl von Ossietzky Univ Oldenburg, Forschungszentrum Neurosensor, D-26111 Oldenburg, Germany
6.Beijing Computat Sci Res Ctr CSRC, Beijing 100193, Peoples R China
7.Shenzhen Computat Sci & Appl Res CSAR Inst, Shenzhen 518110, Peoples R China
8.Los Alamos Natl Lab, Theoret Div, Los Alamos, NM 87545 USA
9.Univ Appl Sci, Inst Lasers & Opt, D-26723 Emden, Germany
10.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Guangdong, Peoples R China

Quenzel, Thomas,Timmer, Daniel,Gittinger, Moritz,et al. Plasmon-Enhanced Exciton Delocalization in Squaraine-Type Molecular Aggregates[J]. ACS Nano,2022,16(3).

Quenzel, Thomas.,Timmer, Daniel.,Gittinger, Moritz.,Zablocki, Jennifer.,Zheng, Fulu.,...&Lienau, Christoph.(2022).Plasmon-Enhanced Exciton Delocalization in Squaraine-Type Molecular Aggregates.ACS Nano,16(3).

Quenzel, Thomas,et al."Plasmon-Enhanced Exciton Delocalization in Squaraine-Type Molecular Aggregates".ACS Nano 16.3(2022).