A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
Magnetically induced currents and aromaticity in ligand-stabilized Au and AuPt superatoms (2021)

López-Estrada, O., Zuniga-Gutierrez, B., Selenius, E., Malola, S., & Häkkinen, H. (2021). Magnetically induced currents and aromaticity in ligand-stabilized Au and AuPt superatoms. Nature Communications, 12, Article 2477. https://doi.org/10.1038/s41467-021-22715-x

JYU-tekijät tai -toimittajat

Julkaisun tiedot

Julkaisun kaikki tekijät tai toimittajat: López-Estrada, Omar; Zuniga-Gutierrez, Bernardo; Selenius, Elli; Malola, Sami; Häkkinen, Hannu

Lehti tai sarja: Nature Communications

eISSN: 2041-1723

Julkaisuvuosi: 2021

Ilmestymispäivä: 30.04.2021

Volyymi: 12

Artikkelinumero: 2477

Kustantaja: Nature Publishing Group

Julkaisumaa: Britannia

Julkaisun kieli: englanti

DOI: https://doi.org/10.1038/s41467-021-22715-x

Julkaisun avoin saatavuus: Avoimesti saatavilla

Julkaisukanavan avoin saatavuus: Kokonaan avoin julkaisukanava

Julkaisu on rinnakkaistallennettu (JYX): https://jyx.jyu.fi/handle/123456789/75282

Lisätietoja: Author Correction. Nat Commun 13, 506 (2022). https://doi.org/10.1038/s41467-022-28053-w

Tiivistelmä

Understanding magnetically induced currents (MICs) in aromatic or metallic nanostructures is crucial for interpreting local magnetic shielding and NMR data. Direct measurements of the induced currents have been successful only in a few planar molecules but their indirect effects are seen in NMR shifts of probe nuclei. Here, we have implemented a numerically efficient method to calculate gauge-including MICs in the formalism of auxiliary density functional theory. We analyze the currents in two experimentally synthesized gold-based, hydrogen-containing ligand-stabilized nanoclusters [HAu9(PPh3)8]2+ and [PtHAu8(PPh3)8]+. Both clusters have a similar octet configuration of Au(6s)-derived delocalized “superatomic” electrons. Surprisingly, Pt-doping in gold increases the diatropic response of the superatomic electrons to an external magnetic field and enhances the aromaticity of [PtHAu8(PPh3)8]+. This is manifested by a stronger shielding of the hydrogen proton in the metal core of the cluster as compared to [HAu9(PPh3)8]2+, causing a significant upfield shift in agreement with experimental proton NMR data measured for these two clusters. Our method allows the determination of local magnetic shielding properties for any component in large 3D nanostructures, opening the door for detailed interpretation of complex NMR spectra.

YSO-asiasanat: nanohiukkaset; sähkövirta; laskennallinen kemia; tiheysfunktionaaliteoria

Vapaat asiasanat: computational chemistry; method development; nanoparticles

Liittyvät organisaatiot

Hankkeet, joissa julkaisu on tehty

OKM-raportointi: Kyllä

Raportointivuosi: 2021

JUFO-taso: 3