Fragment-based approach for the efficient calculation of the refractive index of metal-organic frameworks

verfasst von

Marvin Treger, Carolin König, Peter Behrens, Andreas Schneider

Abstract

Increasing demands on materials in the field of optical applications require novel materials. Metal-organic frameworks (MOFs) are a prominent class of hybrid inorganic-organic materials with a modular layout. This allows the fine-tuning of their optical properties and the tailored design of optical systems. In the present theoretical study, an efficient method to calculate the refractive index (RI) of MOFs is introduced. For this purpose, the MOF is split into disjoint fragments, the linkers and the inorganic building units. The latter are disassembled until metal ions are obtained. The static polarizabilities are calculated individually using molecular density functional theory (DFT). From these, the MOF's RI is calculated. To obtain suitable polarizabilities, an exchange-correlation functional benchmark was performed first. Subsequently, this fragment-based approach was applied to a set of 24 MOFs including Zr-based MOFs and ZIFs. The calculated RI values were compared to the experimental values and validated using HSE06 hybrid functional DFT calculations with periodic boundary conditions. The examination of the MOF set revealed a speed up of the RI calculations by the fragment-based approach of up to 600 times with an estimated maximal deviation from the periodic DFT results below 4%.

Organisationseinheit(en)

AG Anorganische Festkörper- und Materialchemie
PhoenixD: Simulation, Fabrikation und Anwendung optischer Systeme
Institut für Physikalische Chemie und Elektrochemie
Institut für Anorganische Chemie

Typ

Artikel

Journal

Physical Chemistry Chemical Physics

Band

25

Seiten

19013–19023

Anzahl der Seiten

11

ISSN

1463-9076

Publikationsdatum

2023

Publikationsstatus

Veröffentlicht

Peer-reviewed

Ja

ASJC Scopus Sachgebiete

Physik und Astronomie (insg.), Physikalische und Theoretische Chemie

Elektronische Version(en)

https://doi.org/10.1039/D3CP02356G (Zugang: Offen)