Fast and Reasonable Geometry Optimization of Lanthanoid Complexes with an Extended Tight Binding Quantum Chemical Method

Abstract

The recently developed tight binding electronic structure approach GFN-xTB is tested in a comprehensive and diverse lanthanoid geometry optimization benchmark containing 80 lanthanoid complexes. The results are evaluated with reference to high-quality X-ray molecular structures obtained from the Cambridge Structural Database and theoretical DFT-D3­(BJ) optimized structures for a few Pm (<i>Z</i> = 61) containing systems. The average structural heavy-atom root-mean-square deviation of GFN-xTB (0.65 Å) is smaller compared to its competitors, the Sparkle/PM6 (0.86 Å) and HF-3c (0.68 Å) quantum chemical methods. It is shown that GFN-xTB yields chemically reasonable structures, less outliers, and performs well in terms of overall computational speed compared to other low-cost methods. The good reproduction of large lanthanoid complex structures corroborates the wide applicability of the GFN-xTB approach and its value as an efficient low-cost quantum chemical method. Its main purpose is the search for energetically low-lying complex conformations in the elucidation of reaction mechanisms

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