Structural chemistry of molecular perovskites: towards the design of stimuli responsive behaviour Gregor Kieslich Department of Chemistry, TUM Natural School of Sciences, Technical University of Munich, Germany In the centre of my group’s research activities are dense and porous coordination polymers as a material platform. Coordination polymers such as molecular perovskites and metal-organic frameworks are framework forming materials assembled from inorganic nodes and organic linkers, providing a virtually unlimited combinatorial space for the synthesis of materials with tailor-made stimuli responsive properties of academic and technological relevance; however, this parameter space comes with a flip side: trial-and-error experiments for the synthesis of materials with targeted properties are an inefficient endeavour. Therefore, it is natural to ask: how can we efficiently harness the chemical diversity of coordination polymers? In my presentation I will show how the use of molecular building units in framework materials introduces new degrees of freedom of rotational, translational, and conformational nature that can be exploited for material design. I will discuss how understanding and controlling degrees of freedom is a fruitful approach for developing material design strategies, drawing on my group’s recent research results such as the behaviour of coordination polymers under hydrostatic pressures, [1] the introduction of new geometric degrees of freedom into molecular perovskites, [2] the discovery of a new type of polymorphism in ABX 3 perovskite coordination polymers, [3] counterintuitive material behaviour such as negative thermal expansion and uniaxial negative compressibility, [4] and the structural complexity of perovskite-type materials. [5] References 1. P. Vervoorts, J. Stebani, A. S. J. Méndez, G. Kieslich. Structural Chemistry of Metal-Organic Frameworks under Hydrostatic Pressures.ACS Materials Lett.2021, 3, 1635. 2. S. Burger, K. Hemmer, D. C. Mayer, P. Vervoorts, D. Daisenberger, J. K. Zaręba, G. Kieslich. Designing Geometric Degrees of Freedom in ReO3-Type Coordination Polymers. Adv. Funct. Mater. 2022, 32, 2205343. 3. S. Burger, S. Grover, K. T. Butler, H. L. B. Boström, R. Grau-Crespo, G. Kieslich. Tilt and Shift Polymorphism in Molecular Perovskites.Mater. Horiz.2021, 8, 2444. 4. L. Petters, S. Burger, S. Kronawitter, M. Drees, G. Kieslich. Linear Negative Thermal Expansion in Pd(acac)2.CrystEngCo mm.2021, 23, 5425. 5. S. A. Hallweger, C. Kaußler, G. Kieslich. The structural complexity of perovskites. Phys. Chem. Chem. Phys. 2022, 24, 9196.
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