Molecular sensitised probe for amino acid recognition within peptide sequences

verfasst von: Xu Wu, Bogdana Borca, Suman Sen, Sebastian Koslowski, Sabine Abb, Daniel Pablo Rosenblatt, Aurelio Gallardo, Jesús I. Mendieta-Moreno, Matyas Nachtigall, Pavel Jelinek, Stephan Rauschenbach, Klaus Kern, Uta Schlickum
Abstract: The combination of low-temperature scanning tunnelling microscopy with a mass-selective electro-spray ion-beam deposition established the investigation of large biomolecules at nanometer and sub-nanometer scale. Due to complex architecture and conformational freedom, however, the chemical identification of building blocks of these biopolymers often relies on the presence of markers, extensive simulations, or is not possible at all. Here, we present a molecular probe-sensitisation approach addressing the identification of a specific amino acid within different peptides. A selective intermolecular interaction between the sensitiser attached at the tip-apex and the target amino acid on the surface induces an enhanced tunnelling conductance of one specific spectral feature, which can be mapped in spectroscopic imaging. Density functional theory calculations suggest a mechanism that relies on conformational changes of the sensitiser that are accompanied by local charge redistributions in the tunnelling junction, which, in turn, lower the tunnelling barrier at that specific part of the peptide.
Externe Organisation(en): Max-Planck-Institut für Festkörperforschung
Beijing Institute of Technology
Technische Universität Braunschweig
Institut de Physique des Materiaux, Bucarest-Magurele
Akademie Věd České Republiky (AV ČR)
Charles University
University of Oxford
Eidgenössische Technische Hochschule Lausanne (ETHL)
Typ: Artikel
Journal: Nature Communications
Band: 14
ISSN: 2041-1723
Publikationsdatum: 14.12.2023
Publikationsstatus: Veröffentlicht
Peer-reviewed: Ja
ASJC Scopus Sachgebiete: Chemie (insg.), Biochemie, Genetik und Molekularbiologie (insg.), Physik und Astronomie (insg.)
Elektronische Version(en): https://doi.org/10.1038/s41467-023-43844-5 (Zugang: Offen)

BibTeX

@article{a53ad7d9b54e4a56bffbed6b320d0d1a,
title = "Molecular sensitised probe for amino acid recognition within peptide sequences",
abstract = "The combination of low-temperature scanning tunnelling microscopy with a mass-selective electro-spray ion-beam deposition established the investigation of large biomolecules at nanometer and sub-nanometer scale. Due to complex architecture and conformational freedom, however, the chemical identification of building blocks of these biopolymers often relies on the presence of markers, extensive simulations, or is not possible at all. Here, we present a molecular probe-sensitisation approach addressing the identification of a specific amino acid within different peptides. A selective intermolecular interaction between the sensitiser attached at the tip-apex and the target amino acid on the surface induces an enhanced tunnelling conductance of one specific spectral feature, which can be mapped in spectroscopic imaging. Density functional theory calculations suggest a mechanism that relies on conformational changes of the sensitiser that are accompanied by local charge redistributions in the tunnelling junction, which, in turn, lower the tunnelling barrier at that specific part of the peptide.",
author = "Xu Wu and Bogdana Borca and Suman Sen and Sebastian Koslowski and Sabine Abb and Rosenblatt, {Daniel Pablo} and Aurelio Gallardo and Mendieta-Moreno, {Jes{\'u}s I.} and Matyas Nachtigall and Pavel Jelinek and Stephan Rauschenbach and Klaus Kern and Uta Schlickum",
note = "Funding information: We acknowledge funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany{\textquoteright}s Excellence Strategy-EXC-2123 QuantumFrontiers- 390837967, We acknowledge funding by the Emmy-Noether-Program of the Deutsche Forschungsgemeinschaft, B.B. acknowledge the Romanian Ministry of Research, Innovation and Digitalization for funding through UEFISCDI of the project PN-III-P2-2.1-PED-2021-0378 (contract nr. 575PED / 2022) and the Core Program PC2-PN2308020. A.G., J.M., M.N., and P.J. acknowledge financial support from the CzechNanoLab Research Infrastructure supported by MEYS CR (LM2023051), the GACR project no. 20-13692X and computational resources were provided by the e-INFRA CZ project (ID: 90254), supported by MEYS CR.",
year = "2023",
month = dec,
day = "14",
doi = "10.1038/s41467-023-43844-5",
language = "English",
volume = "14",
journal = "Nature Communications",
issn = "2041-1723",
publisher = "Nature Publishing Group",
number = "1",
}