Please use this identifier to cite or link to this item:
http://hdl.handle.net/2445/185365
Title: | Accurate calculation of spin-state energy gaps in Fe(iii) spin-crossover systems using density functional methods |
Author: | Vidal, Daniel Cirera Fernández, Jordi Ribas Ariño, Jordi |
Keywords: | Teoria del funcional de densitat Energia Òxid de ferro Density functionals Energy Ferric oxide |
Issue Date: | 21-Dec-2021 |
Publisher: | Royal Society of Chemistry |
Abstract: | Fe(III) complexes are receiving ever-increasing attention as spin crossover (SCO) systems because they are usually air stable, as opposed to Fe(II) complexes, which are prone to oxidation. Here, we present the first systematic study exclusively devoted to assess the accuracy of several exchange-correlation functionals when it comes to predicting the energy gap between the high-spin (S = 5/2) and the low-spin (S = 1/2) states of Fe(III) complexes. Using a dataset of 24 different Fe(III) hexacoordinated complexes, it is demonstrated that the B3LYP* functional is an excellent choice not only for predicting spin-state energy gaps for Fe(III) complexes undergoing spin-transitions but also for discriminating Fe(III) complexes that are either low- or high-spin in the whole range of temperatures. Our benchmark study has led to the identification of a very versatile Fe(III) compound whose SCO properties can be engineered upon changing a single axial ligand. Overall, this work demonstrates that B3LYP* is a reliable functional for screening new spin-crossover systems with tailored properties. |
Note: | Versió postprint del document publicat a: https://doi.org/10.1039/d1dt03335b |
It is part of: | Dalton Transactions, 2021, vol. 50, num. 47, p. 17635-17642 |
URI: | http://hdl.handle.net/2445/185365 |
Related resource: | https://doi.org/10.1039/d1dt03335b |
ISSN: | 1477-9226 |
Appears in Collections: | Articles publicats en revistes (Institut de Química Teòrica i Computacional (IQTCUB)) Articles publicats en revistes (Ciència dels Materials i Química Física) |
Files in This Item:
File | Description | Size | Format | |
---|---|---|---|---|
717123.pdf | 3.01 MB | Adobe PDF | View/Open |
Items in DSpace are protected by copyright, with all rights reserved, unless otherwise indicated.