Single-Molecule Vibrational Characterization of Binding Geometry Effects on Isocyanide-Metal Interactions

Fuente: arXiv
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Main Authors: Bi, Liya, Wang, Zhe, Balto, Krista, Tao, Andrea R., Pascal, Tod A., Zhang, Yanning, Figueroa, Joshua S., Li, Shaowei
Format: Preprint
Published: 2025
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author Bi, Liya
Wang, Zhe
Balto, Krista
Tao, Andrea R.
Pascal, Tod A.
Zhang, Yanning
Figueroa, Joshua S.
Li, Shaowei
author_facet Bi, Liya
Wang, Zhe
Balto, Krista
Tao, Andrea R.
Pascal, Tod A.
Zhang, Yanning
Figueroa, Joshua S.
Li, Shaowei
contents Isocyanide-metal binding is governed by sigma-donation and pi-back-bonding, which affects the energy of the isocyanide stretching mode-a characteristic probe for ligand-metal interactions. While extensive correlations exist between structure and spectroscopy in molecular isocyanide-metal systems, isocyanide interactions with metallic crystalline surfaces, where ligands often bind in various geometries, remain poorly understood. Conventional vibrational spectroscopies, such as infrared and Raman, lack the molecular-scale resolution needed to distinguish these inhomogeneous configurations. In contrast, inelastic electron tunneling spectroscopy with scanning tunneling microscopy (STM-IETS) enables direct visualization of ligand adsorption geometries and their vibrational signatures. Using STM-IETS, here we investigate a matal-adsorbed m-terphenyl isocyanie ligand and find that adsorption geometry on Cu(100) induces a significant shift in isocyanide stretching frequency, even greater than replacing Cu(100) with Ag(111). Density functional theory confirms this shift arises from atomic-scale variations in isocyanide-metal binding. This study elucidates how atomic-scale binding influences the vibrational signatures of isocyanide ligands-an often-overlooked factor in understanding isocyanide-metal interactions.
format Preprint
id arxiv_https___arxiv_org_abs_2504_03945
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Single-Molecule Vibrational Characterization of Binding Geometry Effects on Isocyanide-Metal Interactions
Bi, Liya
Wang, Zhe
Balto, Krista
Tao, Andrea R.
Pascal, Tod A.
Zhang, Yanning
Figueroa, Joshua S.
Li, Shaowei
Mesoscale and Nanoscale Physics
Isocyanide-metal binding is governed by sigma-donation and pi-back-bonding, which affects the energy of the isocyanide stretching mode-a characteristic probe for ligand-metal interactions. While extensive correlations exist between structure and spectroscopy in molecular isocyanide-metal systems, isocyanide interactions with metallic crystalline surfaces, where ligands often bind in various geometries, remain poorly understood. Conventional vibrational spectroscopies, such as infrared and Raman, lack the molecular-scale resolution needed to distinguish these inhomogeneous configurations. In contrast, inelastic electron tunneling spectroscopy with scanning tunneling microscopy (STM-IETS) enables direct visualization of ligand adsorption geometries and their vibrational signatures. Using STM-IETS, here we investigate a matal-adsorbed m-terphenyl isocyanie ligand and find that adsorption geometry on Cu(100) induces a significant shift in isocyanide stretching frequency, even greater than replacing Cu(100) with Ag(111). Density functional theory confirms this shift arises from atomic-scale variations in isocyanide-metal binding. This study elucidates how atomic-scale binding influences the vibrational signatures of isocyanide ligands-an often-overlooked factor in understanding isocyanide-metal interactions.
title Single-Molecule Vibrational Characterization of Binding Geometry Effects on Isocyanide-Metal Interactions
topic Mesoscale and Nanoscale Physics
url https://arxiv.org/abs/2504.03945