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Title: Temperature-controlled metal/ligand stoichiometric ratio in Ag-TCNE coordination networks

Abstract

The deposition of tetracyanoethylene (TCNE) on Ag(111), both at Room Temperature (RT, 300 K) and low temperatures (150 K), leads to the formation of coordination networks involving silver adatoms, as revealed by Variable-Temperature Scanning Tunneling Microscopy. Our results indicate that TCNE molecules etch away material from the step edges and possibly also from the terraces, which facilitates the formation of the observed coordination networks. Moreover, such process is temperature dependent, which allows for different stoichiometric ratios between Ag and TCNE just by adjusting the deposition temperature. X-ray Photoelectron Spectroscopy and Density Functional Theory calculations reveal that charge-transfer from the surface to the molecule and the concomitant geometrical distortions at both sides of the organic/inorganic interface might facilitate the extraction of silver atoms from the step-edges and, thus, its incorporation into the observed TCNE coordination networks.

Authors:
 [1];  [2];  [3];  [2];  [4];  [2];  [4]; ;  [1];  [4]
  1. Departamento de Física de la Materia Condensada, Universidad Autónoma de Madrid, Cantoblanco, 28049 Madrid (Spain)
  2. IMDEA Nanoscience, c\Faraday 9, Campus de Cantoblanco, 28049 Madrid (Spain)
  3. Departamento de Química Orgánica, Facultad de Ciencias Químicas, Universidad Complutense de Madrid, Ciudad Universitaria s/n, Madrid (Spain)
  4. (Spain)
Publication Date:
OSTI Identifier:
22415487
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 142; Journal Issue: 10; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ATOMS; DENSITY FUNCTIONAL METHOD; DEPOSITION; EXTRACTION; INTERFACES; LIGANDS; MOLECULES; PROPIOLONITRILE; SCANNING TUNNELING MICROSCOPY; SILVER; STOICHIOMETRY; SURFACES; TEMPERATURE DEPENDENCE; X-RAY PHOTOELECTRON SPECTROSCOPY

Citation Formats

Rodríguez-Fernández, Jonathan, Lauwaet, Koen, Herranz, Maria Ángeles, Martín, Nazario, Departamento de Química Orgánica, Facultad de Ciencias Químicas, Universidad Complutense de Madrid, Ciudad Universitaria s/n, Madrid, Gallego, José María, Instituto de Ciencia de Materiales de Madrid, ICMM, CSIC, Sor Juana Inés de la Cruz s\n, 28049 Madrid, Miranda, Rodolfo, Otero, Roberto, and IMDEA Nanoscience, c\Faraday 9, Campus de Cantoblanco, 28049 Madrid. Temperature-controlled metal/ligand stoichiometric ratio in Ag-TCNE coordination networks. United States: N. p., 2015. Web. doi:10.1063/1.4913326.
Rodríguez-Fernández, Jonathan, Lauwaet, Koen, Herranz, Maria Ángeles, Martín, Nazario, Departamento de Química Orgánica, Facultad de Ciencias Químicas, Universidad Complutense de Madrid, Ciudad Universitaria s/n, Madrid, Gallego, José María, Instituto de Ciencia de Materiales de Madrid, ICMM, CSIC, Sor Juana Inés de la Cruz s\n, 28049 Madrid, Miranda, Rodolfo, Otero, Roberto, & IMDEA Nanoscience, c\Faraday 9, Campus de Cantoblanco, 28049 Madrid. Temperature-controlled metal/ligand stoichiometric ratio in Ag-TCNE coordination networks. United States. doi:10.1063/1.4913326.
Rodríguez-Fernández, Jonathan, Lauwaet, Koen, Herranz, Maria Ángeles, Martín, Nazario, Departamento de Química Orgánica, Facultad de Ciencias Químicas, Universidad Complutense de Madrid, Ciudad Universitaria s/n, Madrid, Gallego, José María, Instituto de Ciencia de Materiales de Madrid, ICMM, CSIC, Sor Juana Inés de la Cruz s\n, 28049 Madrid, Miranda, Rodolfo, Otero, Roberto, and IMDEA Nanoscience, c\Faraday 9, Campus de Cantoblanco, 28049 Madrid. Sat . "Temperature-controlled metal/ligand stoichiometric ratio in Ag-TCNE coordination networks". United States. doi:10.1063/1.4913326.
@article{osti_22415487,
title = {Temperature-controlled metal/ligand stoichiometric ratio in Ag-TCNE coordination networks},
author = {Rodríguez-Fernández, Jonathan and Lauwaet, Koen and Herranz, Maria Ángeles and Martín, Nazario and Departamento de Química Orgánica, Facultad de Ciencias Químicas, Universidad Complutense de Madrid, Ciudad Universitaria s/n, Madrid and Gallego, José María and Instituto de Ciencia de Materiales de Madrid, ICMM, CSIC, Sor Juana Inés de la Cruz s\n, 28049 Madrid and Miranda, Rodolfo and Otero, Roberto and IMDEA Nanoscience, c\Faraday 9, Campus de Cantoblanco, 28049 Madrid},
abstractNote = {The deposition of tetracyanoethylene (TCNE) on Ag(111), both at Room Temperature (RT, 300 K) and low temperatures (150 K), leads to the formation of coordination networks involving silver adatoms, as revealed by Variable-Temperature Scanning Tunneling Microscopy. Our results indicate that TCNE molecules etch away material from the step edges and possibly also from the terraces, which facilitates the formation of the observed coordination networks. Moreover, such process is temperature dependent, which allows for different stoichiometric ratios between Ag and TCNE just by adjusting the deposition temperature. X-ray Photoelectron Spectroscopy and Density Functional Theory calculations reveal that charge-transfer from the surface to the molecule and the concomitant geometrical distortions at both sides of the organic/inorganic interface might facilitate the extraction of silver atoms from the step-edges and, thus, its incorporation into the observed TCNE coordination networks.},
doi = {10.1063/1.4913326},
journal = {Journal of Chemical Physics},
number = 10,
volume = 142,
place = {United States},
year = {Sat Mar 14 00:00:00 EDT 2015},
month = {Sat Mar 14 00:00:00 EDT 2015}
}