Experimental determination of partial charges with electron diffraction

Autor(en)

Soheil Mahmoudi, Tim Gruene, Christian Schröder, Khalil D. Ferjaoui, Erik Fröjdh, Aldo Mozzanica, Kiyofumi Takaba, Anatoliy Volkov, Julian Maisriml, Vladimir Paunović, Jeroen A. van Bokhoven, Bernhard K. Keppler

Abstrakt

Atomic partial charges, integral to understanding molecular structure, interactions and reactivity, remain an ambiguous concept lacking a precise quantum-mechanical definition^1,2. The accurate determination of atomic particle charges has far-reaching implications in fields such as chemical synthesis, applied materials science and theoretical chemistry, to name a few³. They play essential parts in molecular dynamics simulations, which can act as a computational microscope for chemical processes⁴. Until now, no general experimental method has quantified the partial charges of individual atoms in a chemical compound. Here we introduce an experimental method that assigns partial charges based on crystal structure determination through electron diffraction, applicable to any crystalline compound. Seamlessly integrated into standard electron crystallography workflows, this approach requires no specialized software or advanced expertise. Furthermore, it is not limited to specific classes of compounds. The versatility of this method is demonstrated by its application to a wide array of compounds, including the antibiotic ciprofloxacin, the amino acids histidine and tyrosine, and the inorganic zeolite ZSM-5. We refer to this new concept as ionic scattering factors modelling. It fosters a more comprehensive and precise understanding of molecular structures, providing opportunities for applications across numerous fields in the chemical and materials sciences.

Organisation(en)

Institut für Anorganische Chemie, Core Facility für Kristallstrukturanalyse, Institut für Computergestützte Biologische Chemie, Quantenoptik, Quantennanophysik und Quanteninformation

Externe Organisation(en)

Vienna Doctoral School in Chemistry, Paul Scherrer Institute, Middle Tennessee State University (MTSU), Eidgenössische Technische Hochschule Zürich

Journal

Nature

ISSN

0028-0836

DOI

https://doi.org/10.1038/s41586-025-09405-0

Publikationsdatum

2025

Peer-reviewed

Ja

ÖFOS 2012

104017 Physikalische Chemie, 104021 Strukturchemie

ASJC Scopus Sachgebiete

General

Link zum Portal

https://ucrisportal.univie.ac.at/de/publications/1477df93-9de4-41fe-beb7-087ebaf7a3a2