Details
| Original language | English |
|---|---|
| Article number | 8335 |
| Journal | Nature Communications |
| Volume | 14 |
| Issue number | 1 |
| Publication status | Published - 14 Dec 2023 |
| Externally published | Yes |
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.
ASJC Scopus subject areas
- Chemistry(all)
- General Chemistry
- Biochemistry, Genetics and Molecular Biology(all)
- General Biochemistry,Genetics and Molecular Biology
- Physics and Astronomy(all)
- General Physics and Astronomy
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In: Nature Communications, Vol. 14, No. 1, 8335, 14.12.2023.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Molecular sensitised probe for amino acid recognition within peptide sequences
AU - Wu, Xu
AU - Borca, Bogdana
AU - Sen, Suman
AU - Koslowski, Sebastian
AU - Abb, Sabine
AU - Rosenblatt, Daniel Pablo
AU - Gallardo, Aurelio
AU - Mendieta-Moreno, Jesús I.
AU - Nachtigall, Matyas
AU - Jelinek, Pavel
AU - Rauschenbach, Stephan
AU - Kern, Klaus
AU - Schlickum, Uta
N1 - Funding information: We acknowledge funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany’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.
PY - 2023/12/14
Y1 - 2023/12/14
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85179743843&partnerID=8YFLogxK
U2 - 10.1038/s41467-023-43844-5
DO - 10.1038/s41467-023-43844-5
M3 - Article
C2 - 38097575
AN - SCOPUS:85179743843
VL - 14
JO - Nature Communications
JF - Nature Communications
SN - 2041-1723
IS - 1
M1 - 8335
ER -