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Title: Strong optical response and light emission from a monolayer molecular crystal

Abstract

Excitons in two-dimensional (2D) materials are tightly bound and exhibit rich physics. So far, the optical excitations in 2D semiconductors are dominated by Wannier-Mott excitons, but molecular systems can host Frenkel excitons (FE) with unique properties. Here, we report a strong optical response in a class of monolayer molecular J-aggregates. The exciton exhibits giant oscillator strength and absorption (over 30% for monolayer) at resonance, as well as photoluminescence quantum yield in the range of 60-100%. We observe evidence of superradiance (including increased oscillator strength, bathochromic shift, reduced linewidth and lifetime) at room-temperature and more progressively towards low temperature. These unique properties only exist in monolayer owing to the large unscreened dipole interactions and suppression of charge-transfer processes. Finally, we demonstrate light-emitting devices with the monolayer J-aggregate. The intrinsic device speed could be beyond 30 GHz, which is promising for next-generation ultrafast on-chip optical communications.

Authors:
 [1];  [2];  [1]; ORCiD logo [3];  [1];  [1];  [1];  [1];  [1];  [1];  [4];  [4];  [2];  [2];  [2];  [5];  [6];  [6]; ORCiD logo [1]; ORCiD logo [1] more »;  [1];  [4];  [7];  [8]; ORCiD logo [2]; ORCiD logo [1] « less
  1. Nanjing Univ. (China)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  3. Univ. of Wisconsin, Madison, WI (United States)
  4. Univ. of California, Berkeley, CA (United States). National Science Foundation (NSF) Nanoscale Science and Engineering Center
  5. Nanjing Univ. (China); Xidian Univ., Xian (China)
  6. Southeast Univ., Nanjing (China)
  7. Chinese Univ. of Hong Kong (China)
  8. Univ. of Liverpool (United Kingdom)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
National Natural Science Foundation of China (NNSFC); Chinese Academy of Sciences (CAS); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1582356
Grant/Contract Number:  
[AC02-05CH11231; 61734003; 61521001; 61851401; 51861145202; 61861166001; 21722302; 11874199; 2015CB921600; AoE/P-03/08]
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
[ Journal Volume: 10; Journal Issue: 1]; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Molecular self-assembly; Organic–inorganic nanostructures; Two-dimensional materials

Citation Formats

Zhao, Huijuan, Zhao, Yingbo, Song, Yinxuan, Zhou, Ming, Lv, Wei, Tao, Liu, Feng, Yuzhang, Song, Biying, Ma, Yue, Zhang, Junqing, Xiao, Jun, Wang, Ying, Lien, Der-Hsien, Amani, Matin, Kim, Hyungjin, Chen, Xiaoqing, Wu, Zhangting, Ni, Zhenhua, Wang, Peng, Shi, Yi, Ma, Haibo, Zhang, Xiang, Xu, Jian-Bin, Troisi, Alessandro, Javey, Ali, and Wang, Xinran. Strong optical response and light emission from a monolayer molecular crystal. United States: N. p., 2019. Web. doi:10.1038/s41467-019-13581-9.
Zhao, Huijuan, Zhao, Yingbo, Song, Yinxuan, Zhou, Ming, Lv, Wei, Tao, Liu, Feng, Yuzhang, Song, Biying, Ma, Yue, Zhang, Junqing, Xiao, Jun, Wang, Ying, Lien, Der-Hsien, Amani, Matin, Kim, Hyungjin, Chen, Xiaoqing, Wu, Zhangting, Ni, Zhenhua, Wang, Peng, Shi, Yi, Ma, Haibo, Zhang, Xiang, Xu, Jian-Bin, Troisi, Alessandro, Javey, Ali, & Wang, Xinran. Strong optical response and light emission from a monolayer molecular crystal. United States. doi:10.1038/s41467-019-13581-9.
Zhao, Huijuan, Zhao, Yingbo, Song, Yinxuan, Zhou, Ming, Lv, Wei, Tao, Liu, Feng, Yuzhang, Song, Biying, Ma, Yue, Zhang, Junqing, Xiao, Jun, Wang, Ying, Lien, Der-Hsien, Amani, Matin, Kim, Hyungjin, Chen, Xiaoqing, Wu, Zhangting, Ni, Zhenhua, Wang, Peng, Shi, Yi, Ma, Haibo, Zhang, Xiang, Xu, Jian-Bin, Troisi, Alessandro, Javey, Ali, and Wang, Xinran. Fri . "Strong optical response and light emission from a monolayer molecular crystal". United States. doi:10.1038/s41467-019-13581-9. https://www.osti.gov/servlets/purl/1582356.
@article{osti_1582356,
title = {Strong optical response and light emission from a monolayer molecular crystal},
author = {Zhao, Huijuan and Zhao, Yingbo and Song, Yinxuan and Zhou, Ming and Lv, Wei and Tao, Liu and Feng, Yuzhang and Song, Biying and Ma, Yue and Zhang, Junqing and Xiao, Jun and Wang, Ying and Lien, Der-Hsien and Amani, Matin and Kim, Hyungjin and Chen, Xiaoqing and Wu, Zhangting and Ni, Zhenhua and Wang, Peng and Shi, Yi and Ma, Haibo and Zhang, Xiang and Xu, Jian-Bin and Troisi, Alessandro and Javey, Ali and Wang, Xinran},
abstractNote = {Excitons in two-dimensional (2D) materials are tightly bound and exhibit rich physics. So far, the optical excitations in 2D semiconductors are dominated by Wannier-Mott excitons, but molecular systems can host Frenkel excitons (FE) with unique properties. Here, we report a strong optical response in a class of monolayer molecular J-aggregates. The exciton exhibits giant oscillator strength and absorption (over 30% for monolayer) at resonance, as well as photoluminescence quantum yield in the range of 60-100%. We observe evidence of superradiance (including increased oscillator strength, bathochromic shift, reduced linewidth and lifetime) at room-temperature and more progressively towards low temperature. These unique properties only exist in monolayer owing to the large unscreened dipole interactions and suppression of charge-transfer processes. Finally, we demonstrate light-emitting devices with the monolayer J-aggregate. The intrinsic device speed could be beyond 30 GHz, which is promising for next-generation ultrafast on-chip optical communications.},
doi = {10.1038/s41467-019-13581-9},
journal = {Nature Communications},
number = [1],
volume = [10],
place = {United States},
year = {2019},
month = {12}
}

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