Hauke Paulsen

TL;DR: In this article, the results obtained by these methods serve as references for other electronic structure calculations that may also be applied to larger systems and allow intermolecular effects to be investigated that are important for understanding the cooperativity of spin transitions.

TL;DR: In this paper, a procedure is presented that allows us to simulate from first principles the normalized spectra of nuclear inelastic scattering (NIS) of synchrotron radiation by molecular crystals containing a M\"ossbauer isotope.

TL;DR: The vibrational entropy difference between the two isomers,DeltaS(vib), which is--together with the electronic entropy difference DeltaS(el)--the driving force for the spin-transition, has been determined from the measured and from the calculated frequencies.

TL;DR: Vibrational analysis has been performed via DFT calculations of the low-spin and high-spin state normal modes of both compounds as well as their respective infrared absorption cross sections, which are dominated by an increase of the absorption cross section upon high- spin state formation.

TL;DR: Electronic structure calculations with periodic boundary conditions have been performed that show the importance of intermolecular effects in tuning the ligand field, and thus in determining the transition temperature, and based on this qualitative analysis, an increased inductive effect of the out-of-sphere anion corresponds to a decreased SCO temperature T1/2, in agreement with the experimental results.