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Main Authors: Cui, Jie, Zhang, Yao, Zhang, Yang, Luo, Yi, Dong, Zhen-Chao
Format: Preprint
Published: 2026
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Online Access:https://arxiv.org/abs/2603.21579
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author Cui, Jie
Zhang, Yao
Zhang, Yang
Luo, Yi
Dong, Zhen-Chao
author_facet Cui, Jie
Zhang, Yao
Zhang, Yang
Luo, Yi
Dong, Zhen-Chao
contents Determining the chemical structure for a single molecule on surface from spectroscopic data represents a challenging high-dimensional inverse problem. Tip-enhanced Raman spectroscopy (TERS) enables chemically specific imaging of single molecules with sub-nanometer spatial resolution, yet reconstructing complete molecular structures from TERS maps remains difficult owing to the ambiguous vibrational signatures and reliance on expert interpretation. Here, we introduce TERS-ABNet, a deep-learning framework that formulates single-molecule structure determination from spectroscopic images as an image-to-graph inference task. Using a "two-track" architecture, the model jointly predicts probabilistic atom and bond maps, enabling direct construction of explicit atom-bond graphs without relying on predefined chemical rules. Trained on simulated datasets, TERS-ABNet achieves about 94% atom-type classification accuracy (with a mean coordinate error of about 0.23 Å), enabling to reliably recovering molecular connectivity and fully reconstruct single-molecule structure from its TERS maps. The framework generalizes across varying spatial resolutions and structural complexity through transfer learning, and successfully reconstructs the atomic structure of a single porphyrin molecule from experimental TERS data. This work establishes a general deep-learning strategy for inferring explicit atom-bond graph representations from high-dimensional spectroscopic imaging data, providing a new pathway towards automated molecular structure determination in nanoscale characterization.
format Preprint
id arxiv_https___arxiv_org_abs_2603_21579
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle TERS-ABNet: A Deep Learning Approach for Automated Single-Molecule Structure Reconstruction with Atomic Precision from TERS Mapping
Cui, Jie
Zhang, Yao
Zhang, Yang
Luo, Yi
Dong, Zhen-Chao
Chemical Physics
Determining the chemical structure for a single molecule on surface from spectroscopic data represents a challenging high-dimensional inverse problem. Tip-enhanced Raman spectroscopy (TERS) enables chemically specific imaging of single molecules with sub-nanometer spatial resolution, yet reconstructing complete molecular structures from TERS maps remains difficult owing to the ambiguous vibrational signatures and reliance on expert interpretation. Here, we introduce TERS-ABNet, a deep-learning framework that formulates single-molecule structure determination from spectroscopic images as an image-to-graph inference task. Using a "two-track" architecture, the model jointly predicts probabilistic atom and bond maps, enabling direct construction of explicit atom-bond graphs without relying on predefined chemical rules. Trained on simulated datasets, TERS-ABNet achieves about 94% atom-type classification accuracy (with a mean coordinate error of about 0.23 Å), enabling to reliably recovering molecular connectivity and fully reconstruct single-molecule structure from its TERS maps. The framework generalizes across varying spatial resolutions and structural complexity through transfer learning, and successfully reconstructs the atomic structure of a single porphyrin molecule from experimental TERS data. This work establishes a general deep-learning strategy for inferring explicit atom-bond graph representations from high-dimensional spectroscopic imaging data, providing a new pathway towards automated molecular structure determination in nanoscale characterization.
title TERS-ABNet: A Deep Learning Approach for Automated Single-Molecule Structure Reconstruction with Atomic Precision from TERS Mapping
topic Chemical Physics
url https://arxiv.org/abs/2603.21579