Harnessing Atomic-Scale Thinning in Two-Dimensional Organic Molecular Crystals for In-Situ Characterization and Superior Optoelectronics

Two-dimensional organic single crystals (2D OSCs) offer high crystallinity and quantum limit properties, making them ideal for exploring unique quantum phases and developing scaled optoelectronic devices. However, accurately probing the structure-optoelectronic relationship in 2D OSCs remains challenging. Here we realize in situ optoelectronic characterization of 2D OSCs through an atomically precise thinning technique. Thinning 3D pentacene crystals to the monolayer limit induces a phase transition from Frenkel excitons to charge-transfer (CT) excitons, achieving a near-unity quantum yield (∼95.1%). In-situ electrical measurements demonstrate that this thinning improves carrier mobility and reduces threshold voltages. Utilizing 2D pentacene crystals, we construct a high-performance synapse device, showing a record paired-pulse facilitation index (PPF index ∼ 261%). This remarkable synaptic plasticity further allows us to emulate the human vision system, predicting the object trajectory with exceptional accuracy (∼99.1%). These results provide new insights into the intrinsic properties of 2D OSCs and lay the foundation for multifunctional optoelectronic applications.

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Publication Details

Journal
Nano Letters
Published
2025-05-29
DOI
https://doi.org/10.1021/acs.nanolett.5c01808
Primary Topic
Luminescence and Fluorescent Materials
Type
article
Field-Weighted Citation Impact
0.00

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article

Harnessing Atomic-Scale Thinning in Two-Dimensional Organic Molecular Crystals for In-Situ Characterization and Superior Optoelectronics

Zhixing Gan, Yuerui Lu, Rui Fang, Xueqian Sun et al.
Nano Letters
Luminescence and Fluorescent Materials
article

Harnessing Atomic-Scale Thinning in Two-Dimensional Organic Molecular Crystals for In-Situ Characterization and Superior Optoelectronics

Zhixing Gan, Yuerui Lu, Rui Fang, Xueqian Sun, Yi Shi, Youwen Liu, Kan Zhou, Sudong Yang, Yongbiao Zhai, Neng Wan, Yangyang Fu, Yichun Cui, Jiong Yang, Tong Tong, Han Yan, Fan Yang, Fuguo Tian, Hucheng Song, Linglong Zhang, Haizeng Song
article en

Abstract

Two-dimensional organic single crystals (2D OSCs) offer high crystallinity and quantum limit properties, making them ideal for exploring unique quantum phases and developing scaled optoelectronic devices. However, accurately probing the structure-optoelectronic relationship in 2D OSCs remains challenging. Here we realize in situ optoelectronic characterization of 2D OSCs through an atomically precise thinning technique. Thinning 3D pentacene crystals to the monolayer limit induces a phase transition from Frenkel excitons to charge-transfer (CT) excitons, achieving a near-unity quantum yield (∼95.1%). In-situ electrical measurements demonstrate that this thinning improves carrier mobility and reduces threshold voltages. Utilizing 2D pentacene crystals, we construct a high-performance synapse device, showing a record paired-pulse facilitation index (PPF index ∼ 261%). This remarkable synaptic plasticity further allows us to emulate the human vision system, predicting the object trajectory with exceptional accuracy (∼99.1%). These results provide new insights into the intrinsic properties of 2D OSCs and lay the foundation for multifunctional optoelectronic applications.

Nano LettersVol. 25(23)
Australian National University (AU), Nanjing Normal University (CN), Shenzhen University (CN), University of Cambridge (GB), Suzhou University of Science and Technology (CN), Numerical Method (China) (CN), National Engineering Research Center of Electromagnetic Radiation Control Materials (CN), PLA Army Engineering University (CN), Nanjing University (CN), Nanjing University of Aeronautics and Astronautics (CN)
National Natural Science Foundation of China, Science, Technology and Innovation Commission of Shenzhen Municipality, Graduate Research and Innovation Projects of Jiangsu Province
Openalex Percentile: Top 92%
Luminescence and Fluorescent Materials
DOISourceOpenAlex
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