Metal-organic frameworks (MOFs) that exhibit spin-crossover behavior have attracted much interest because of their potential technological applications. A key parameter that characterizes these materials is the transition temperature, defined as the temperature with equal populations of low-spin and high-spin species. A number of studies have been devoted to [Fe(pz)Pt(CN)4] since its transition temperature is near room temperature. Furthermore, it was experimentally reported that the transition temperature of [Fe(pz)Pt(CN)4] can be controlled by the adsorption of guest molecules [1]. We have recently developed a novel hybrid Monte Carlo/molecular dynamics (MC/MD) method that enables the calculation of the transition temperature in MOFs with high accuracy [2]. In this study, we report on MC/MD simulations aimed at characterizing the spin-crossover properties of [Fe(pz)Pt(CN)4] upon adsorption of chemically and structurally different guest molecules. The calculated transition temperatures for the different guest molecules are in excellent agreement with the available experimental data. This has allowed us to develop a molecular-level picture of spin-crossover behavior in [Fe(pz)Pt(CN)4] [3,4] and to determine the physical mechanisms responsible for the stabilization of the LS state [5]. Besides providing a theoretical analysis of experimental data reported in the literature, we will demonstrate that the variation of the spin-crossover temperature of [Fe(pz)Pt(CN)4] upon guest adsorption can be used to detect toxic gases.<br/>

Molecular mechanisms of spin crossover in the {Fe(pz)[Pt(CN)4]} MOF upon guest adsorption

253rd National Meeting (2017)

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