Predicting dipole orientations in spontelectric methyl formate

  • Capturing intermolecular interactions accurately is essential for describing, e.g., morphology of molecular matter on the nanoscale. When it reveals characteristics which are not directly accessible through experiments or ab initio theories, a model here becomes eminently beneficial. In laboratory astrochemistry, the intense study of ices has led i.a. to the exploration of the spontelectric state of nanofilms. Despite its success in biophysics or biochemistry and despite its predictive power, molecular modeling has however not yet been widely deployed for solid-state astrochemistry. In this article, therefore a pertinent hitherto unaddressed problem is tackled by means of the classical molecular-dynamics method, namely the unknown distribution of relative dipole orientations in spontelectric cis-methyl formate (MF). In doing so, from ab initio data, a molecular model is derived which confirms for the first time the anomalous temperature-dependent polarization of MF. These insights thus represent a further step toward understanding spontelectric behavior. Moreover, unprecedented first-principles predictions are reported regarding the ground-state geometry of the MF trimer and tetramer. In conjunction with the study of the binding to carbonaceous substrates, these additional findings can help to exemplarily elucidate molecular ice formation in astrochemical settings.

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Author:Christian Kexel, Andrey V. Solov’yovORCiDGND
Parent Title (English):The European physical journal D
Place of publication:Berlin ; Heidelberg
Document Type:Article
Date of Publication (online):2021/03/08
Date of first Publication:2021/03/08
Publishing Institution:Universitätsbibliothek Johann Christian Senckenberg
Release Date:2022/08/24
Article Number:89
Page Number:12
First Page:1
Last Page:12
Open Access funding enabled and organized by Projekt DEAL.
The authors acknowledge the Center for Scientific Computing (CSC) Frankfurt for providing the capability to perform large-scale calculations on the FUCHS supercomputer. We also acknowledge the partial support of this work by Deutsche Forschungsgemeinschaft (No. 415716638) and by the European Commission through the RADON project within H2020-MSCA-RISE-2019 call (GA 872494). CK acknowledges partial support by European COST Action 15140.
Institut: Physik
Dewey Decimal Classification:5 Naturwissenschaften und Mathematik / 53 Physik / 530 Physik
Licence (German):License LogoCreative Commons - Namensnennung 4.0